CA2039135A1 - Polyester, polycarbonate and/or polyphenylene ether with polyorgano-siloxane/polyvinyl-based graft (meth) acrylate polymers - Google Patents

Abstract

337-2181 (8CT-4905) ABSTRACT OF THE DISCLOSURE
Polyphasic resin blends and particularly polycarbonate/polyester blends, are prepared with modifiers comprising combinations of polyorganosiloxane/
polyvinyl-based graft copolymer(s), polyorganosiloxane based graft copolymer 5) and/or diene rubber-based graft copolymer(s), imparting a wide range of physical properties to the blend.

Description

2~39~3~ `
-- -2- 337-2181 ( BCT-4905 ) . . . , , . .
n~o ~ n_rrol~
Thi~ sention relate~ to thermoplastic resins oomprising a polycarbonate re3in alone or polypha~ic 30 r~in mixture~ of polycarbona~ce re~in with a saturated polye3ter re~in and/or an ela~to~er, comprl~ g a poly ~ ethere3ter ) elasto~er or a poly t eth~r imide e~ter ) , ela~tomer or bo~h and/or a polyphenylene ether re~in, and a modifier ~ompo~ition compri~ing two multi-~tage 35 graft polymer compo~ition~ in combina~ion.

. .
, ~ ,~
.
:: :
': ' ', .

.
;.

~03~

-3- 337-2181 (8CT-4905) An-~O O' 1-- IW~-OII
Polycarbonate re~in compositions and blends with other thermoplastic resins are widely used because of their excellent properties.
There have been many attempts in the ar~ to provide polyorganosiloxane-based graft polymers which may be u eful as impac~ strength modifiers for thermoplastic resinsO See, for example, U.S. Pa~ent No.
2,891,920 (J.F. ~yde, e~ al.); and O. Graiver, et al~, Rubber Chem. Tech., 56 (5), 918 (1983).
U.S. Patent No. 3,898,300 states that a poly-organosiloxane-based graft copolymer for improving the impact strength of styrene ~S)/acrylonitrile (AN) resin i3 formed by graftin~ S/AN comonomers in an emulsion system on~o the vinylsiloxane or allylsiloxane containing silicone substrate. ~S. Paten~ No. 4,071,577 describes a similar approach by using a mercaptosiloxane in place o~ vinyl-group containing siloxane3. ~uropean Patent Application No7 0,166,900 reports further improvement of polysiloxane~-based graft polymers and increased S/AN
impact strength by u3ing acryloxy-functionali~ed siloxane as the graft-linking agent.
Relevant for its broad teachi~gs is BASF's U.K. Patent No. 1,590,549 which describe~ the use of a polyorganosiloxane-ba ed graft copolymer in various t~ermopla~tic co~positions. Poor compatibility is ob~erved with these composit~ons. Slmilarly, European Patent Applicatlon No. 249,364 describes the use of a polyorgano~iloxane-based gra~t copolymer in polycarbonate re~in compo~itions and mixtures thPreof with~a saturated polye~ter and/or a polyester ela~tomer. The modifier therein ha~ relatively poor rubber integri~y aQd incompatibility with the resin as well.
The use of a die~e or acrylic rubber-based modifier in thermoplastic resin3 ha~ become a co~mon .. . . . ..

~)39~3~

-4- 337-2181 (8CT-4905) practice in the ar~. The selection of either material depends largely on the end use purposes such as weatherability or low temperature impac~ resistance.
Uniform color appearance of molded parts is a benefit which is gained by using a diene-based modif ier over acrylics. However, ~he unsaturated moieties of the diene rubber restric~ i~s outdoor use to ~ome extent due ~o its tendency to oxidize and to yellow.
None of the references disclose the in-situ co-homopolymerization o~ vinyl monomers in the presence of siloxanes in an emulsion system, as described hereinbelow. The present invention is also directed to the use of graft polymers provided by subsequent graft polymerization of vinyl monomers (eOg. polymethyl (meth)acryla~e, polystyrene or styrene/acrylonitrile copolymer~ in the presence of such a co-homopolymerized polyorganosiloxane/vinyl-based substrate.
Surprisingly, i~ has been found ~hat partial replacement of the oxidation or ozone sen~itive rubber by a silicone-based rubber affect~ more improvements t such a~ low temperature ductility, low glo~s, and impact and discoloring re~is~anoe against thermal agins on the blend~ described hereinafter. Unexpectedly, it is now possible to prepare low gloss polycarbonate and polyester blend.Q having both excellent low temperature recistance and discoloration resistance by the addition of an effective amount of a silicone-ba~ed impact modifier to a diene-based modi~ier.
Mention i~ al~o made to European Patent Application No. 0,260,558 which discloses a combination of a silicone-based modif ier with an alkylacryla~e-based modifier. The pa entee, however, make no mention of the use of a diene-baced impact modifier.
Additionally, it is de~cribed in S.Y. Hobbs et 3S al, Polymer Bulletin, 17, 341 (19~7) and S.Y~ Hobbs et ~3~3~i -5- 337 2181 (8CT-4905~

al, Jousnal of Material Science, 23, 1219 (198a) that in polycarbonate/saturated polyester resin blends, typical core-shell type modifiers such as Acryloid RM-330 (poly-bu~ylacrylate core-methyl methacrylate shell, ~ohm and ~aas Company) or KM-653 (poly~utadiene core-styrene/methyl methacrylate polymer shell~ Rohm and Haas Company) segre-gate completely in the polycarbonate phase leaYing the less ductile saturated polyester pha~e without any modifier.
There is evidence that in blends or mixtures comprised of two different resin~, modification of both phases can significantly improve low temperature toughne~s.
Van der Meer, in Dutch Patent Application Nos. 8600166 and 86202388O4 filed on January 12, 1986 and on December 30, 1986, respectively, and Van der ~eer and ~obbs in commonly owned copending U.S. Patent Application Serial NoO 07/007,268 filed on JanuaLy 27~ 1987, attorney's docke no. 335-2019 (8CB-10,306) have demonstrated this in polyphenylene ether (PPE)/polyamide ~nylon) blends where Kraton~ rubber (~tyrene butadiene-~tyrene AB~ block copolym~r, Shell Chemi~al Co~pany) wa~ used ~o modify the PPE pha~e and maleic anhydride func~ionalized EPDM (ethylene-propylene-nonconjugated diene monomer polymer) rubber wa used to modify the nylon phase.
~ ASF's 6erman Patent No. 3521956 discloses the modificatian of the poly(butylene terephthalate) (P~T~ phase of a PBT/PC polyphasic blend through the incorporation of olefin polymers tha~ contain epoxy groups. The effectiveness of this method, however, depends on the ability to establish sufficient gra~ting of PBT o~ the epoxy groups of the ole~in polymers during compounding in an extruder. The fact that both mixing and grafting chemistry mu5t take place simulta-neously places high demands on the compou~ding process, and therefore, the succe3s of the 3ASF method has been limited.
It has been surprisingly found ~hat migration of multi Rtage graft polymer modi~ier~ can be induced to segregate different modi~ier~ into the di~erent phase~

~Q~9~3~a -6- 337-21~1 [8CT-4905) of polyphasic PC~PBT containing blends or mix~ures of the same with poly(etherester) elastomer, poly(ether-imide e~ter) elastomer and/or polyphenylene ether resins by va~ying the amount of (me~h)acrylonitrile in the S outermost stage of the modifiers. Therefore~ two or more different modi~iers, each with a different amount of (me~h)acryl~nitrile in th~ outelmost stage can be combined to yield a desired distribution of modifier in the PC phase and in th~ PBT phase resulting in optimum toughness of the polyphasic blend. Such blends particularly exhibit superior low tempera~ure toughnes.
when compared with those formulated with modifiers residing in only one phase of the blend.

FIG. 1 i~ a trans~is3ion elPctron micrograph of a polyphasic blend o~ PG, PaT, a polyorganosiloxane/-polyvinyl-based graft copolymer mcdifier (CSi~) (Silicone (Si)/Polystyrene (PS)Methyl methacrylate (MMA) wt. ratio of 70:30, S1/PS wt. ratio o~ 95:5) and a CSiM modifier (tSi~PS)-S/A~ wt. ratio of 70 30, Si/PS
wt. ratio of 95:5, S/AN wt. ra~io of 75:25, stained with OSO4 and Ru04~ showing ~he complete segregation of CSiM
modifier ((Si/PS)-MMA) in the PC phase and CSiM modifier (~Si/PS)-S/A~, S/A~ wt. ratio of 75:25) in the P~T
phase.
FIG. 2 is a transmisRion electron micrograph of a polyphasic blend of PC, PBT, and CSiM modifi~r ((5i/PS)-S/AN wt. ratio of 70:30, Si/PS wt. ra~io of 95:5, S/AN wt. ratio of 75:25), stained with OsO4 and Ru04, showing complete segregation of the modifier in the PBT phase.
FIG. 3 is a transmission electron micrograph of a polyphasic blend of PC, PBT, and CSiM modifier ((Si/PS)-MMA wt. ra~io of 70:30, Si/PS wt. ratio of ~2~3~3~35 -7- 337~2181 (8CT-4905 95~5), stained with OSO4 and RuO~, showing complete segregation of the modifier in the PC phase.
FIG. 4 is a transmission electron micrograph of a polyphasic blend of PC, P~T, and CSiM modifier ((Si/PS)-MMA/AN w~. ratio of 70030, 5i/P~ wt. ratio of 95:5, MMA/AN wt. ratio of 75:253, stained with OsO4 and Ru04, showing complete cegregation of the modifier in the P~T phase.
FIG. 5 is a ~ransmi~sion electron micrograph o~ a polyphasic blend of PC, PBT, and CSi~ modifier ((Si/PS)-MMA/AN wt. ratio of 70:30, Si/PS wt. ratio of 95:5, MMA/AM wt. ratio of 95 5), stained with OSO4 and Ru04, showiny the complete segreyation of the modifier in the PC phase.
FIG. 6 is a tran~mis~ion electron ~icrograph o~ a polyphasic blend of PC, PBT, butadiene rubber sub~trate~S/MM~ outermo~t stage ~odifier, and high rubber graf~ ABS modifier (A B-S wt. ra~io of 7.5:70:22.5), ~tained with OSO4 and Ru04, ehowing segregation of the bu~adiene rubber subs~rate S~MMA outermo~t stage ~odifier in th~ PC phase and the ABS modifier in the PBT phase.
~IG. 7 i~ a tran~missio~ electron micrograph of a polyph~sic blend of PC, PBT and a butadie~e rubber substrate-S/MMA outermost stage modifier, s~ained with 9S04 and Ru04, showing ~he segregation o~ the modifier in the PC phaseO

S~n~R~ OF TEB I~YE~TIO~
A~cording to the pre~ent invention, there are provided polyphasic resin compo~itions comprising a mixture (A-l~ comprising (i) a polycarbonate resin phase and (ii) a saturated polye~ter re~in phase~ a ~ixture (A-2) compri~in~ (i) a polycarbonate re~in phase, (ii~ a saturated polyester re~in phase, (iii) a poly(ether imide) ela~tomer pha~e~ (iv~ a poly(etherimide ester~
elastom~r phase, (v) a polyphenylene ~ther re~in phase, 2t~3~5 -8- 337-2181 (3CT-4905) or a mixkure of (i), (ii) and any o~ (iii), (iv) and (v); or a mixture (A-3) o~ (A-lj and (A 2); and an effec~ive amoun~ of a modi~ier composition (B) comprising, in combination, (1) a multi-stage graft polymer composition comprising (a) as a first stage, (i) an organofiiloxane polymer, unitæ
derived from a cross-linking agent or ag~nts and optionally units which serve a a grat-linking agent or agents;
(ii) a polymeric substrate comprised of units of a di~ne rubber and op~cionally units derived from a cross-linking agent or agents; or (iii) a polymeric co-homopolymerized sub~trate comprising of, in combination, an organosiloxane polymer; at lea t one vinyl-ba3ed polymer; and optionally units derived from a cross~linking agent or agent~, units which serve a~ a graft li~king agent or agen~s, units derived from a cross-linking agen~ or agents and unit~ from the same or d$fferent agent or agents which serve as a graft-linking agent or agents or a mixtur~ of any of the for~going; and (b) at lea~t one subse~uent stage or stages g~a~t polymerized in the presence of any previous stages and which i3 comprised of a vinyl-based polymer or a cro~-linked vinyl-ba ed polymer, the outermost stage o which contains from zero to no ~ore than an amount of polymerized or copolymerized ~eth)acrylonitrile unit~
3~ which will induce migration of multi-qtage composition (1) into said polLycarbonate re~in phase; and (2) a multi-~tage graft polymer composition compr i5 ing (a) as a first sta~e, (i) an organosiloxane polymer, uni~s ~3~ 5 ~9- 337-2181 (8CT-4905) deriYed from a cross-linking agent or agent.~ and optionally units which serve as a graf~-linking agent or agents;
(ii) a polymeric substrate comprised of units of a diene rubber and op~ionally unit3 derived from a cross-linking agent or agents; or ~iii) a polymeric co-homopolymerized substrate comprised of, in combination, an organosiloxane polymer; at least one vinyl-based polym~r; and optionally units derived fro~ a cross~linking agent or agents, units which serve a-~ a graft-linking agent or agents, units derived from a cross-linking agent or agents and units from the same or different agent or agents which serve as a gra~t-linking agent or agents or a mix~ure of any of the foregoing; and ( b ) ak least one subsequen'c stage or stages graft polymerized in the pre~ence of any previDus stage and which is comprised of a vinyl-based polymer or a cross-linked vinyl-based polym~r, the outermo$t staqa having a content of a polymerized or copolymerized (~eth~acrylonitrile units at lea~t sufficient to induce migration of multi-stage composition (2) into said saturated polye~ter re~in pha~e.
Also conte~plat2d by the invention is a ~S composition as defined ahove, but where the modifier composi~ion (8) additionally comprise~ a ~hird componen~
(3) which i3 different than both (1) and (2) and which comprises ~a) a~ a first stage ~i) an organosiloxane polymer, units derived from a cros3-linking agent or agents and optionally unit.~ which ~erYe a~ a graft-linking agent or agentst (ii) a polymeric substrate comprised of units of a diene rubber and optionally units derived ~C~39~5 -10- 337~2181 (8CT-4gO5) frsm a cross-linking agent or agents, or (iii) a polymeric co-homopolymerized substrate compri~ed of, in combination/ an organosiloxane polymer; at least one vinyl-ba~ed polymer; and op~ionally units derived from a cross-linking agent or agents~ units which serve a5 a graft-linking agen~ or agents, units derived from a cross-linking agent or agents and u~its from the same or different a~ent or agen~Q which serve a-~ a graft-linking agent o~ agents or a mixture o~ any of the foregoing; and (b) at least one subsequent stage or stages graft polymerized in the presence of any previous stages and which is comprised of a vinyl-based polymer or a cro~s-linked vinyl-based polymer.
lS Further conte~plated by the invention are composition~ as abo~e defined wherein su,b~equent s~age-~
(l)(b) comprise (b)(i) a ~econd stage compri ing at least one vinyl poly~er and optionally units derived ro~ a cross-linking agen~ or agent~, units which ~erve 23 as a g~aft-linking agent or agents, unit~ derived from a cros~-linking agent or agents and units from the sam2 or different a~ent or agents which serve a~ a graft-linking agent or agent~ or a mixture of any o the oregoing;
and (b)(ii) a third stage comprising at least one ~S vinyl-based polymer or cro~s-linked vinyl-based polymer which is the ~ame or differen~ than (b)~i) and which contains from zero ~o no more than n amount of polymerized or copolymerized (meth)acrylonitrile which will induce migration of the multi-~tage compo~ition (1) into th~ polycarbonate re~in pha~e.
Additionally~ co~position~ wherein ~ubsequent ~tage~ ~2~(b) compri~e (b)(i~ a ~econd stage comprising at least one vinyl-polymer and optionally unlt~ derived fro~ a cross-linking agent or agent , units which serve as a graf~-linking agent or agent , unit~ derived from a ... ... . . . .. ... . .. . . .. .....

~3~35 ~ 337-2181 (8CT-4905) cross-linking agent or agents and units from the ~ame or different agent or agents which serve as a graft-linking agent or agents, or a mixture of any of the foregoing;
and (b)(ii) a third seage comprising at le~8t one vinyl-based polymer which is the sam~ as or different than (b)(i), and which has a content of polymerized or copolymeri~ed (meth)acrylonitrile uni~s at leas~
sufficient to induce migra~ion of multi-stage composition (2) into the saturated polyester reQin phase; and composition~ wherein both subsequent s~ages (l)(b) a~d (2)(b) comprise two stages, (l)(b)(i) and (l)(b)(ii), and (2)(b)(i) and (2)(b)(ii) correspondingly, as described immediately above are proposed.
Another preferred embodiment of the present 1~ invention en~ompasse~ a polyphasic resin compo~ition compri~ing a mixture (A-l) comprising ~i~ a polycarbonate resin phas~ and (ii) a ~aturated polye~ter re~in phases a~d an effective amount of a modifier compo~ition (B) comprising, in combination, I
(13 a multi-stage polyorgano~iloxane/polyvinyl-based graft polymer composition comprising (a) a~ a first stage, a polymeric co-homo-polymerized substrale compri~ed of, in combination, an organosiloxane polymer; a~ lea~t one vinyl-based polymer and optionally unit~ derived from a cross-linking agent or agents, units which ~er~e a~ a graft-linking agen~ or agents! units derived from a cros~-linking agent or agents and units fro~ the same or different agent or agene~ which serve as a graft-linkiny agent or agents, or a mixture of any of the oregoiny7 and (b) ae least one subsequent stage or stages graft polymerized in the presence of any previou~ stage~
and which i~ comprised of a vi~yl-based polymer or a cros~-linked vinyl-baqed polymar, the ou~er~ost ~tage of -12- 337-2181 (8CT-4905) which contains from zero to more ~han an a~ount of polymerized or copolymerized ~meth)acrylonl~rlle uni~s which will induce migration of multi-stage composition (1) into the polycarbonate re in phase; and (2) a multi-stage polyorganosiloxane/polyvinyl-based graft poly~er composition comprising (a) as a first s~age~ a polymeric co-homo-polymerized substrate, wbich may be the same as or di~ferent than (l~(a)~ comprised of, in combina~ion, an organosiloxane polymer; a~ le~st one vinyl-based polymer; and optionally uni~s derived from a cross-linking agent or agents, units which serve as a graft-linking agent or agents, units derived from a cro~s-linking agent or agents and uni~s from the sam~ or di~ferent lS agent or agent~ which serve a graf~-linking agent or agents, or a mix~ure of any of ~h~ foregoing; and ~b) at least one sub~equent s~age or stages graft polymerized in the presence of any previous stages and which i8 comprised of a vinyl-ba~ed polymer or a cross-linked vinyl-based polymer, the outermost stage having a content of polymerized or copolymerized (meth)-acrylonitrile units at lea~t suff$cient to induce migration of multi-~tage compo~ition ~2) into the saturated polye~ter resin phaseO
2S A preferred feature o~ the embodiment contemplates subsequent stage (1) (b) comprising (b)(i) a second stage comprising at least one vinyl polymer and optionally unit~ derived rom a cros~-linking a~en~ or ag~nt~, uni~s which serve as a graf~-linking agent or agents, units derived from a cross-linking agent or agents and units from the ~ame or differen~ agent or agents which serve a~ a graft-linking agent or agents or a mixture of any o~ the foregoing; and (b)~ii) a third stage compri~ing at lea~t one vinyl-b~ed poly~er or cros~linked vinyl-based polymer which is the ~ame a3 or 3~35 -13- 337-2181 (8CT-4905) differen~ than (b)(i) and which contains from zero to no more than an amount of polymerized or copolymerized tmeth)acrylonitrile units which will induce migration of multi-stage composition (1~ into the polycarbonate re~in pha~e.
5ub~equent stage (2)(b) oomprising (b)(i) a ~econd stage comprising at least one vinyl polymer an~
optionally units derived ~rom A croq~-linking agent or ayents, units which serve as a graft-linking agent or agents, units derived from a cross-linking agent or agents and units from the same or different agent or agents which serve as a graft~linking agent or agents~
or a mixture of any of the foregoing; and (b)(ii~ a third s~age comprising at least one vinyl-based polymer or a cro~s~linked vinyl-based polymer which i~ the same as or different than (b)(i) and which ha~ a content o~
polymerized or copolymerized ~me~h)acrylonitsile units at lea~t suf~icient to induce migration of multi-stage compo~ition (2) into ~he sa~urated palyester resin pha~e i-~ also contemplated as are compo~ition~ wherein both (l)(b) and (2)(b) comprise two ~tageg, (l~(b)(i) and (l)(b)(ii), and (2)(b)(i) and (2)(b)(ii), corre~pondingly, a-~ de~cribed immediately above.
The invention also provide~ a proce~s for producing a polyphasic re in composition comprising the s~ep3 of:
~ i) providing two first s~age substra~e~
independantly by the concurrent co-homopolymerization of an organosiloxane, one or more vinyl-based monomers, and optionally units derived from a cro~s-linking agent or agents, uni~s which serve a~ a gra~t-linking agent or agents, units derived fro~ a cro~3-linking agent or agents and unit~ from the same or dlf~erent agen~ or agents which serve a~ a yraft-linking agent or agents, or a mixture of any of the foregoing;

~39~3~
-14- 337-2181 (8CT-4905) tii) independently neutralizing each of the two reaction masses of the foregoing polymerization step to a pH of at leas~ about 6~5 to provide a neutralized polyorganosiloxane/polyvinyl~based substrate latex;
(iii) graft polymerizing to one of the first stage sub-strates at least one vinyl based monomer or a vinyl-ba~ed monomer and a cross-linker, said monomers being selected to provide that ~he outermos~ stage contain~ from zero to no more than an amoun of polymerized or copolymerized tmeth)acrylonitrile which will induce migration of the resultant multi-stage composition into the polycarbonate re~in phase of a polycarbonate re~in phase/saturated polyester resin phase mixture:
lS (iv) graft polymerizing to the remaining first ~tage substrate a vinyl-based monomer or a vinyl~based monomer and a cross-linker, said monomers being selected to provide that the ou~ermost stage ha~ a content of polymerized or copolymerized (meth~acrylonitrile units at least suf~icient to induce migration of th~ resultant multistage composition into the sa~urated polyester re3in phase of a polycarbonate re3in phas~/saturated polyester re~in phase mixture;
(v) isolating the two multi-~tage organo-siloxane/vinyl-based graft polymers to provide poly-organosiloxane~polyvinyl-based modifiers for thermoplastic resin.~;
(vi) combining independent modifying amoun~s of the two polyorganosiloxane/polyvinyl-ba~ed modifiers with a polypha~ic resin mixture.
Processes also are defined wherein in step (i) only one first stage subs~rate i8 provided and that substrate is subsequen~y divid0d into two poritions;
wherein graft polymerization s~ep (iii) is carried out in two successive stages co~prising (l) graf~ polymerizing ,~, , , ~ O 3 ~
-15 337-2181 (8C~-4gO5) at least one vinyl-based monomer; or vinyl-based monomer in admixture with a cross-linker, a graft-linker, or a cross- and graft-linker or a mixtuze of any o~ the foregoing to produce a second stage polymer or cross-linked polymer on the substra~e and ~hereafter, (2)graft polymerizing at least one vinyl-based monomer, or a vinyl-based monomer and a cross-linker, which i5 the same as or different ~han ~hat u ed in stage (l) to produce a third stage of polymer on the second s age, said monomers being selected to provide that the outermost stage contains from zero ~o no more than an amount of polymerized or copolymerized (meth)acrylonitrile units which will induce migration of the resultant multi-~tage composition into the polycarbonate re~in phase of a polycarbonate resin pha~e/saturated polyester resin phase mixtur~;
wherein step (iv~ is carried out in two ~uccessive stages comprising: (1) graft polymerizing at least one vinyl-based monomer; or vinyl-ba~ed monomer in admixture with a cross-linker, a graft-linker or a cross-and graft-linker or a mix~ure of any o~ the foregoing to produce a second stage polymer or cross-linked polymer on said substrate; and therea~ter, (2~ graft polymerizing at least one vinyl-based monomer or a vinyl-based monomer and a cro~s-llnker which is the sa~e or different than that used in stage (11 to produce a third stage polymer on the second stage, said monomer being selected to provide that the outermo~t stage has a content of polymerized or copolymerized (meth)acrylonitrile units at least ufficient to induce migration o~ the resultant multi-~tage co~po~ition into the saturated polye~ter re~in phase of a polycarbonate re~in phase/saturated polyester resin phase mixture; and wherein both step~ (iii~ and (iv) are carried 5 out in two stages as de~cribed immediately above.

X~3~35 -16- 337-2181 (8CT-4905) Also contemplated in another a~pect of the invention are compositions comprising a polycarbonate resin (A); a mix~ure (A-l) comprising (i) a polycarbonate re~in and (ii) a sa~ura~ed polyester re~in; a mixture (A-2) compri~ing (i) a polycarbonate resin, and (iii) a poly(etheres~er) elastomer or (iv) a poly(etherimide e~t~r) elastom2r or a mixture of (iii) and liv); a mix~ure (A 3) comprising li) a polycarbonate resin, (ii) a saturated polyester resin and (iii) a poly(etherester) elastomer, (iv) a poly(etheri~ide) elastomer or a mix~ure of (iii~ and (iv); or a mix~ure (A 4) of any of the foregoiing; and an ef ective amount of a modifier composition (B) comprising, in combina~ion, ~1) a multi-stage polyorganosiloxane-based g~aft polymer composition (GSim) comprising ~a) as a first stage, a~ organociloxane polymer r units derived frum a cross-linking agent or agents and optionally uni~s which serve a~ a graf~-linking agent or agents; and (b) at least one subsequent stage or stages graft polymerized in the presence of any previous stages and which is comprised of a vinyl-based polymer or a cross~ ked vinyl-ba~ed polymer and ~2) a diene rubber-based graft copolymer composition compri~in~
~a~ as a first stage, a polymer substrate comprised of units of a diene rubber and optionally unit~ derived from a cross-linking agent or agents; and (b) at lea.~ o~e ~ubsequent stage graf~
polymerized in the presence of any previous stages and which is comprised of a vinyl-based polymer or a cross~
linked vinyl-ba~ed polymer, the weight ratio of (1) to (2) being from 1 to 9:9 to 1.

~3~3~
-17- 337-2181 (8CT-49053 Also contemplated in the preferred feature is a composi~ion wherein first stage (l)(a) is replaced by first stage (l)~a) which comprises a polymeric co-homopolymerized substrate comprised o , in co~bination, an organosiloxane polymer; a~ least one vinyl-based polymer; and optionally units derived from a cro~-linking agent or agents, unit~ which serve as a graft-linking agent or agents, units derived from a cross-linking agent or agents and units from the same or different agent or agents which serve as a yraf~-linking agent or agents or a mixture of any of the foregoing.
Additionally, envisioned in thi~ preferred feature are subsequen~ stages in components (1) and ( 2 comprisiny:
(b)(i) a second stage comprising at least one vinyl polymer and optionally unit~ derived from a cro~s-linking agent or agents, unit~ which s~rve as a graft-linking agent or agents, units derived from a cross-linking agent or agents a~d u~it~ fro~ the same agent or agen~s which serve as a graf~-linking agent or agents, or a mix~ure of any of the foregoing; and (b)~ii) a third stage co~prising at least one vinyl-based polymer or a cross linked vinyl~based eolymer which is the same or d~fferent tha~ (b)(i).

Polycarbona~e resins (A) or (i), sui~able for use in thi~ invention, can comprise non-aromatic a~ well as aromatic form~. With respect to aromatic polycarbonate resins, the~e can be made by those skilled in thi~ art or can be obtained from a va~ie~y of comm~rcial sources.
They may be prepared by reacting a dihydro~y compound such a~ a dihydric phenol and/or a polyhydroxy compound with a carbonate precursor, such a~ phosgene, a haloformate or a carbonate e~ter such as a diester of ~)3~35 ~ 337-2181 (~CT-4905) carbonic acid. Typically, they will have recurring structural units of the formula:

11 ~
~ O - A - O - C ~

wherein A is a divalent aromatic radical of the dihydric phenol e~ployed in the polymer produc~ng reaction.
Preferably, ~he aromatic carbonate polymers have an intrinsic viscosity ranging from 0.30 to 1~0 dl/g ~easured in me~hylene chloride at 25C~. 8y dihydric phenols is mean~ mononuclear or polynuclear aromatic compounds containing ~wo hydroxy radicals, each of which is attached to a carbon atom of an aromatic nucleus.
Typically, dihydric phenols include 2~2-bis-(4 hydroxy-phenyl)propane; 2,2-bi~-(3,5-dimethyl 4 hydroxyphenyl)-propanes 4,4'-di hydroxydiphenyl ether; bis(2-hydroxy-phenyl1methane, mixture3 thereof and the like. The preferred aroma~ic carbonate polymer for component (A) or (i) i~ a homopolymer derived from 2,2-bi~(4-hydroxy-phenyl~propane(bisphenol-A~.
Poly(ester carbonates) for use in the inveneion are known and can be obtained commercially.
Generally, they ar~ copolyester~ comprising recurring carbonate group~:

~ O - C - O
carboxylate groups ~ C ~

and aromatic carbocyclic group~ in the linear polymer .. .. . . . .

2~ L35 -19 337W21al (8CT-4905) chain, in which a~ least some o~ the carboxylate groups and at lea3t some of the carbona~e groups are bonded directly to ring carbon atoms of the aromatic carbocyclic groups. The~e poly(ester carbonate~ in general, are prepared by reacting a difunctional carboxylic acid such as phthalic acid, issphthalic acid, terephthalic acid~ homophthalic acid, o-, m-, and p-phenylenediacetic acid the polynuclear aromatic acids~ such a~ diphenic acid, l,4-naph~halic acid; mixture~ o~ any of the foregoing, and the like, with a dihydric phenol and a carbonate precursor, of the types deQcribed above. ~ ~
particularly useful poly(ester carbonate) i~ derived fro~
bisphenol-A, isophthalic acid, terephthalic acid, or a mixture of isophthalic acid and terephthalic acid, or the reactive derivatives of ~hese acids such as terephthaloyl dichloride, or a mixture thereof, and phosgene. The molar proportion~ o dihydroxy diaryl unit~ to benzenedicarboxylate units to carbonate unit~
can range from 1 0.30-0.80 0O70O0.20 and the molar range of terephthalate units to i~ophthalate units can ran~e from 9:1 to 2:8 in this preferred family of resins.
The aromatic dihydric phenol sulfone polymer re-nins useful in component~ (A) and (i) are a family of resins which can be made by those skilled in this art.
For example, homopolymer~ o~ dihydric phenol, and a dihydroxydiphenyl sulfone and a carbonate precursor can be prepared a~ well a~ copolymers of a dihydric phenol and a carbonate precursor can be made accordinq to the description in Schnell, et al~, U.S. Patent No.
3,271,367. A preferred ~aterial is made by polymerizing bis-~3,5-dimethyl-4-hydroxyphenyl) 5ul fone, alone, or especially in combination with bisphenol-A with phosgene or a phosgene precursor, in accordance with the de~cription in Fox, U.S. Patent No. 3,737,409.
E~pecially preferred is a copolymer made by reactin~ 40 ~33~
-20- 337-2181 (8CT-4905) to 99 wei~ht percen~ of ~he sulfone, 1 to 60 weight percent of the bisphenol with pho~gene.
Polyesters (iii) suitable for use herein may be saturated or unsa~urated or polyester ela~tomers and S are generally derived from an aliphatic or cycloaliphatic diol, or mix~ures thereof, containing fro~ 2 to about 10 carbon atom~ and at lea~t one aromatic dicarboxylic acid. Preferred saturated polye~ter resins comprise the reaction produc~ of a dicarboxylic acid or a chemical equivalent thereof and a diol. Preferred polyesters are derived from an aliphatic diol and an aromatic dicarboxylic acid and have repeated units of the following general formulas ~ t CH2 ~ O - C ~ ,C -wherein n i~ an integer of from 2 to 4~
The most preferred poly~ter~ ar~ poly~ethylene terephthalate~ and poly(l,4-butylene ~erephthalate).
Also contemplated herein are ~he abov~
polyesters with minor amounts, e.g., from 0.5 to about 2 percent by weight, of units d~rived from aliph3tic acid and/or aliphatic polyol~ to form copolye~ters. The aliphatic polyol~ include glycol~, ~uch as poly(ethylene glycol). All such polye ters can be made ~ollowing the teaching3 of, for example, U.S. Patent Nos. 2,465,319 and 3,047,539.
The polye~ters which are derived from a cycloaliphatic diol and an aro~atic dicarboxylic acid aee prepared, for example, by conden~inq either the cis-or trans-isomer (or mix ure3 thereof) of, for example, 1,4-cyclohexanedimethanol with an aromatic dicarboxylic ~339~.3.~

-21- 337-2181 (8CT-4905) ac~d as to produce a polye~ter having recurring units of ~he following formula:

r~ o o 11 il ~ ~ C~2 ~ - C~2 ~ - C - R - C -wherein the cyclohexane ring is selected from the cis-and tran~-isomers thereof and R represents an aryl radical containing 6 to 20 carbon atom~ and which is the decarboxylated re~idue derived from an aromatic dicarboxylic acid.
~xamples of aro~atic dicarboxylic acids represen~ed by the decarboxylated residue R are isophthalic or terephthalic acid, 1,2-di(p-carboxyphenyl) ethane, 4,4'-dicarboxydiphenyl ether, etc., and mixture~
of these. All o~ the~e acids contain at least one aromatic nucleus. Acids containing fu~ed ring~ can al~o be pre ent, ~uch as in 1~4- or 1,5-naphthalenedicarboxylic acid-q. The preferred dicarboxylic acid~ are terephthalic acid or a mixture of terephthalic and isophthalic acid~.
Another pre~erred polye~ter may be derived from the reaction of either the cis- or trans-i~omer (or a mixture thereof1 of 1,4-cyclchexanedimethanol with a ~ixture of isophthalic and terephthalic acids. Such a polye~ter would have repeating units of the formula:

~ - C~ 2 ~ ~ C~
Still another preerred polye~ter i~ a copoly-e ter derived from a cyclohexanedimethanol, an alkylene glycol and an aroma~ic dicarboxylic acid. The e copolye~ters are prepared by condensing eithe the Ci3-or trans-isomer (or mixture~ thereo~) o~, for example, ~391~5 -22- 337-2181 (8CT-4905) 1~4-cyclohexanedime~hanol and an alkylene glycol with an aromatic dica boxylic acid so as to produce a copolyes~er having units of ~he following formula:

~ 0 - CH~ ~ C~2 ~ C - R - C

11 \
t ~ C~2~ - c ~ ct Y
wherein the cyclohexane ring is selec~ed from the cis-and trans-isomers th~reof, R is as previously defined, n is an integer of 2 to 4, the x units comprise from about 10 to about 90 percent by weight and the y uni~s comprise from abou~ 90 to ahou~ 10 pe~cen~ by weight.
Such a preferred copolyestPr may be derived from the reaction of either the ci~- or trans-isomer (or mixture8 thereof3 of 1,4-cyclohexaQedime~hanol and ethylene glycol with terephthalic acid in a molar ratio of 1:2:~. These copolyesters have repeating units of the following formula:

~ ~ C~2~} C~2 ~ ~ 11 ~11 ~
x ~O~C~2~0 - 11~" ~

wherein x and y are as previously defined.
The polye~ter~ de~cribed herein are either commercially available or can be produced by methods ;~0~3~
-23- 337-2181 (8CT-4905) well known in ~he art, such as those set forth in, for example, U~S. Patent No. 2,901,466.
The polyesters used herein have an intrinsic viscosity of from about 0.4 to abou~ 2.0 dl/g as measured in a 60:40 phenol:te~rachloroethane mix~ure or similar solvent at 23~-30C.
Polyester elastomers preferably comprise a block copolymer consisting of (1) polyester segments and (2) polyether or poly~etherimide) segmen~q~ Preferred are polyester segmen~s comprising poly(l,4-butylene terephthalate) and polyether or poly(etherimide) segments comprising a polyalkylene ether glyool, or an imide acid capped polyalkylene ether diamine, or a mixture o~ such segments.
The poly(etherester) elastomer (iii) for use aq a component in the invention i~ a block copolymer consisting o~ polyester cegments and polyether segments having molecular weights of 400 to 20,000. The polyester segment con~ists o~ a polye~ter obtained by condensation of an aromatic dicarboxylic acid with an alkylene glycol. Examples of this segment are as cited above in the case of the saturated polyester~ Preferred examples of this segment are poly(l,4-butylene terephthalate) and poly(ethylene terephthalate). On the other hand, the polyether segment consists of a polyalkylene ether glycol, e.g. poly(ethylene oxide~
glycol, poly(tetramethylene oxide) glycol, poly(propylene oxide) glycol, or a mixture thereof; an alipha~ic polye~ter, e.g. a polya~ter re~ul~ing from the reac~ion of an aliphatic dicarboxylic acid of 2 to 12 carbon atoms with an aliphatic glycol of 2 ~o 10 carbon atom , more specifically, polyethylene adipate, polyte~ra-methylene adipate, polyethylene sebacate, polyneopentyl sebacate, polyhexamethylene azelate, or poly-~-caprolactone.
The content of the polyether segment in the poly(ether-~1~39~3~
-24- 337-2181 ~aCT-~905) e~er~ elas~omer is pre~erably from 2 to 80 percent by weightO
The poly(etherimide ester) ela~tomers (iv) used herein may be prepared from one or more diols, one or more dicarboxylic aoids and one or more high molecular weigh~c polyoxyalkylene dlimide diacids.
Preparation of such mateeial~ is described in de~ail in UOS. Patent No. 4,556,705 o R.J. McCready, i~sued December 3, 1985 and hereby incorporated by reference.
The poly(etherimide ester) elastomer~ used herein may be prepared by conventional processes, such a~ esterification and condensation reac~ions for the production of polyesters, to provide rando~ or block copolymers. Thus, poly(etherimide e~ers) may be 15 generally charac:terized as the reaction product of the aforementioned diols and acids~
~ he polyphenylene ether resin (v) in the invention i-~ a hamopoly~er or copolymer repre~ented by the formula ~ ~

wherein Ql through Q4 are selec~ed independently of each other ~rom the group con~isting of hydrogen and hydrocarbon radical.~ and m denotes a num~er of 30 or more.
Examples of such polyphenylene ether re~ins include poly~2,6-dimethyl-1,4-phenylene~ether, poly(2,6-diethyl-1,4 phenylene)ether, poly(2~6-dipropyl~1,4-phenylene)e~her, poly(2-methyl-6-ethyl-1,4-phenylene)~
ether~ poly(2-methyl 6-propyl-1j4 phenylene)ether, 3913~

-25- 337-2181 (8CT-4905) poly(2-ethyl-6-propy~ 4-phenylene)ether~ copolymer of (2,6-dimethyl~1,4-phenylene)ether with (2~3,6-trimethyl-1,4~phenylene)ether, copolymer of (2,6-diethy1-1,4-phenylene)ether with (2,3,6-trimethyl~1,4-phenylene)ether, and copolymer of (2,6-dimethyl-1,4-phenylene)ether with (2,3,6-triethyl-1~4-phenylene)ether~ Of these polymers, preferred are poly(2,6-dimethyl-1,4-phenylene)ether and a copolymer of (2,6-dimethyl-1,4-phenylene)ether with (2,3,6-trimethyl-1,4-phenylene)e~her. Particularly preferred is a poly(2,6 dimethyl-1,4-phenylene)ether resin. There is no particular restriction on the polymerization degree of the polyphenylene ether resin used in the invention, but it is preferable to use the re~in having a reduced viscosity of 0.3 to 0.7 dl/g measured in chloroform at 25C. Resins having a les reduced viscosity than 0.3 dl/g tend to exhibit low heat stability while reqin having a reduced viscosity exceeding 0.7 dl/g ~end to have inferior moldabilityO
A preferred composition comprises a mixture (A-l~ comprising (i) a polyca bonate resin and (ii~ a sa~urated polyester resin.
The multi-stage polyorganosiloxane-based gra~t polymers may be prepared with or without the incorporation of a vinyl-based polymer. Where incorporation of the vinyl-based polymer is desired, the process is generally described hereinbelow by a co-ho~opolymerization proce~s.
Co-homopolymerization reer~ to a polymerization step where two distinct polymerization mechani~ms are effected concurrently, including simultaneously. In particular, the first stage co-hompolymerization may encompa3s a siloxane polymerization (e.g., ring opening and condensation mechanism) in conjunction with a concurren vinyl polymerization. The discrete mechanism-~ are not seen as competing with each o~her, ~ 3 S
-~6- 337-2181 (8CT-4905) but rather, two homopolymer~ are concurrently produced each retaining its own structure.
The co-homopolymerization process may provide two discrete networks rather than a random copolymer.
While not intending to be bound by any theory, it is possible that the network(s~ comprises two or more distinct interpenetrating polymer phases, which provide the additional strength needed in the polyorganosiloxane~
This is evidenced by the two distinct glas~ transition temperatures which can be detected by differential scanning calorimetry. Preferably, the product of the co-homopolymerization process is rubbery instead of a resin-like powder.
Subsequen~ to the co-homopolymerization of the siloxanes and vinyl-based monomers of the first step, at least one additional graft polymeri~ation proces~ is utilized to achieve the multi-stage polyorgano~iloxane~-polyvinyl-based graft polymers of the pre3ent invention.
The subsequent graf~ polymeriza~ion is pre~erably of at lea~t one vinyl~based type monomer~ It has been found that a styrene/acrylonitrile copolymer, an alkyl(meth)acrylate polymer or alkyl(meth)acrylate/
acrylonitrile copolymer is particularly ef~ective as the se~ond s~age graft polymer or copolymer, or as the outermost stage when in~ermediary stages are optionally utilized, and when two modifier compositions are utilized in combina~ion.
The foregoing polyorganosiloxane/polyvinyl-based graft poly~er can be isolated and utilized, for example, as an impact i~proving agent for thermoplasti~ resins as `-will be discusssd in detail below~
~ dditional cross-linking and/or graft-linking agent can be utilized in this initial stage to provide co-homopolymerized network~ f rom both polymeric con3tituent5 which provide greater rubber integrity.
-20391;~5 -27- 337-2181 (8CT-4905) The firs~ stage rubbery subs~rake is provided by a series of sequential pzocessing stepsO In a premixing step the ingredients required for the reaction of the organosiloxane(s~ and optional vinyl-ba~ed monomer(s) aEe premixed with water and suitable cross-linker(s), graft-linker(s), initia~or(s) and surfactant(s).
The premixed ingredients are homogenized by conventional means. The reactions may begin a~ this early s~age o~
the process but these reactions are generally slow at room temperature. The homogenized reactants may be directed to a reaotor vessel, typically stainless steel or glass flasks, under a nitrogen blanket. ~eat is applied to facilitate the reaction. For typical 5 to S0 gallon stainles~ steel reactors, a 3 to 6 hour residence time at 75 to 90 degree~ centigrada is adequate to complete the co-homopolymeriza~ion. Cooling for 2 to 6 hours will typically reduce ~he temperature to at least room temperature where the reaction mas~ can be held for 3 ~o 72 hours. Cooling to lower temperatures ~e.g~ 5 degrees centigrade) may sometime~ be pre~erred ~ince this may enhance the properties of the newly formed polyorganosiloxane/polyvinyl-ba~ed substrate.
Cooling to room tempera~ure or lower allows the polyorganosiloxane portion ~o build molecular weight, thereby miniMizing the ex~ractable silicone rubber fragmen~s and optimizing physical properties of the product for certain application~. Generally, lower temperature~ are pre~erred when it is desired ~o optimize the elasticity of the formed polyorganosiloxane/
polyvinyl-based sub~trate.
The initiator for the siloxane componen~ can be any ionic ring opening type initiator when cyclic siloxanes are utilized, such a3 alkylarylsul~onic acids, alkyldiaryldisulfonic acids, alkyl~ulfonic acids, and the like. The best suited example is dodecylben2enesulfonic ;~1)3~3~
2~- 337-2181 (8CT-4905) acid which can act as an initiator and at the same time as an emulsifier. In some cases, ~he joint use of a metal salt of an a~orementioned sulfonic acid is also preferred.
The initiator for the optional styrenic or other vinyl-based monomers in ~he co-homopolymerization proce~s can be any organic soluble radical initia~or, such as azobisisobutyronitrile ~AIBN) and the organic peroxides, e.g. benzoyl peroxide, dichlorobenzoyl peroxide, and tert-butyl perbenzoate~ Also suitable are water-soluble radical initiators such as the persulfates.
Although it is possible to charge this type of initia~or at the beginning of the process, it is preferred that it be charged continuously or incremen~ally during the co-homopolymerization period. Since persulfate is less stable in the acid conditions of the siloxane polymerization, it is preferred that the persulfate be added over time to keep the vinyl polymerization running. Particle size, p~ and total solids measurements can be readily monitored at this stage of the process.
A latex rubber emulsion prepared as described above will generally contain particle~ having an average diameter of lO0 to 800 nanometers and preferably lS0 ts 400 nanometers. The particle size is particularly influenced by the homogenization pressure (and the number of passes through the homogenizer~ and the composition of the reaction ingredients. A pressure range of 2000 to 12000 psi i~ typical, and 3000 to 9000 psi is preferred~ Multiple passes through the homogenizer may be preferred, but on a large scale, a ~ingle pass may be mo t practical.
The foregoing reaceion steps mus~ be followed by a suitable neutralization process to provide the products of the invention. The main object of the neu~ralization is to quench the siloxane polymerization.

3~
29~ 337-2181 (8CT-4905) This is accomplished by adding a caustic solution such as sodium hydroxide, potassium hydroxide, pota~ium or sodium carbona~e, sodium hydrogen carbonate, triethanol-amine or triethylamine. The p~ of the reaction solution may be raised ~rom a level o~ 1 ~o 3 to a p~ of at least 6.5, and preferably 7 to 9.
It is often de~irable to add addi ional soap or sur~actant to the emulsion formed at the end of the firs~ stage, prior to the neutralization step.
Additional ~urfac~ant tend~ to facilitate avoidance o~
premature agglomeration or flocculation of the co-homopolymerized rubber in the quench step.
The foregoing co-homopolymerization proce~s provides a rubbery network composed o~ a polyorgano siloxane/polyvinyl-based sub~trate. Thi~ substrate is the fir~t stage of ~he gzaft polymer of the present invention. Optionally, a fir~t ~tage comprising an organosiloxane polymer with units derived from a cross-linking aqent or agents and optionally units which serve as a graft-linking a~en~ or agen~s may be employed. Th~
organosiloxane polymer can be prepared in a manner according to th~ prior art, e.g. European Patent Application NoO 0,166,900. Also contemplated are mixture~ of the co-ho~opolymerized sub3trate with silicone sub~rates.
~he next stage involves the graft polymeri~ation o addi~ional vinyl-func~ional moietie~ onto graft ~i$e~
provided by the rubbery subs rate particles on the latex ormed in the first s~age.
The grafted polymers will preferably be the product o~ a vinyl polymerization process. Suitable vinyl monomers for qraft polymerization include, withou~
limita~ion, alkenyl aromatic compounds such a~ styrene, divinylbenzene, alpha-methylstyrene, vinyl toluene, halogenated styrene and the like~ methacrylates such as ~33~
-30- 337-2181 (8CT-4905) methyl methacrylate and 2-ethylhexyl methacrylate;
acrylates such as acrylic acid, methyl acrylate, ethyl acrylate and butyl acrylate; vinyl cyanide compounds such as acrylonitrile and methacrylonitrile; 012fins such as ethylene, propylene, butadiene, isoprene, and ehloroprene; other vinyl compounds such as acrylamide~, N-(mono or di-substitutedjalkyl acrylamide~, vinyl acetate, vinyl chloride, vinyl alkyl ethers, allyl (meth)acrylate, triallyl isocyannurate~ ethylene dimethacrylate, diallyl maleate, maleic a~hydride;
maleimide compounds such as maleimide, and N-phenyl (or alkyl) maleimide; and mixture of these monomersO
Preferred vinyl based polymers of subsequent stages (l)(b) and (2)(b) in the organosiloxane-based or the organosiloxane/vinyl-based poly~ers comprise at lea~t one selected from the group consis~ing of alkenyl aromatic compounds, (meth)acryla~e co~pound~, vinyl cyanide compounds, maleimide compound~ and acrylamide compounds. ~specially preferred are polystyrene, poly~me~hyl methacryla~e), styrene/acryloni~rile copolymer, styrene/methyl methacrylate copolymer and methyl methacrylate/acrylonitrile copolymer.
The vinyl polymerization is accomplished in an emulsion; therefore, water-soluble initiators are suitable, e.g. potas~ium persulfate, sodium persulfate and ammonium persulfateO It i~ practical to add the initiator at the beginning of this step, prior to charging the vinyl monomer for the second s~age polymerization. Other Redox initiator sy~tems, such a~
cumene hydroperoxide/~errous sulfa~e/glucose/sodiu~
pyrophosphate, can also be utilized at thi~ stage as well a~ other organic peroxides.
Sequential multi-stage polymerization proces~eq Oe this type are someti~es referred to as core-shell processe~. rt i~ preferred, however, to -31- 337-2181 (8CT-4905) describe them as multi-stage graft polymerization processes wherein the ini~ial stage provides a co-homopolymerized organosiloxane/vinyl-based substrateO
This substrate may have sufficient grafting site~ for a second or subsequent stage to be grafted thereto.
Grafted polystyrene, poly(me~h)acrylate, styrene/-acrylonitrile copolymer, methyl me~hacrylate/-acrylonitrile copolymer or styrene/divinylbenzene copolymer as the outermost stage is preferred, yet many other intermediary stage~ such as a butyl acrylate stage are also contemplated. Furthermore, the grafting of additional stages of the same or different kinds is also possible.
The organosiloxanes useful in the first stage of the composition are any of those known to produce silicone elastomers and may include those which are hydroxy-, vinyl-, hydride- or mercapto- end capped linear organosiloxane oligomersO
The polyorganosiloxanes will be comprise~
primarily of units o~ the forNula nsio(4-n~/2 wherein R is hydrogen or a monovalent hydrocarbon radical of about 1 to 16 carbon atoms and n is 0, 1 or 2.
Preferred among the organosiloxanes are those in cyclic form having three or more siloxane units, and most preferred are those having three ~o six units.
Such organosiloxanes include, without limitation, for example, hexamethylcyclotrisilo~ane, octame~hylcyclo-tetrasiloxane, decamethylcyclopentasiloxane, dodeca-methylcyclohexa~iloxane, trimethyltriphenylcyclotri-siloxane, tetramethyltetraphenylcyclotetrasilaxane, tetramethyltetravinylcyclotetrasiloxane and octaphenylcyclotetrasiloxaneO These or similar organosiloxane~ may be used alone or in combina~ion.

9~35 -32~ 337-2181 (8CT-4905) The vinyl-based monomers useful in conjunction with the co-homopolymerization of organosiloxanes in the first stage are preferred to be alkenyl aromatic compound~ such a~ styrene, divinylbenzene, alpha-methyl-styrene, vinyl toluene, vinyl naphthalene, vinyl anthracene,and halogenated styrene or its derivatives. Other suitable vinyl-based monomers include acrylic acids and acrylate~ such as methyl~, ethyl-, alkyl-, or bu~yl-acrylate; methacrylate~ such a3 methyl methacrylate, or 2-ethylhexyl methacrylate; vinyl cyanide3 such as acrylo-nitrile, and methacrylonitrile, olefin~ such a~ ethylene, propylene, butadiene, isoprene, and chloroprene; and other vinyl compounds su~h as vinyl imidazole, 5-vinyl-2-norbornene, vinyl pyridine, vinyl pyrrolidinone, vinyl acetate, vinyl alkyl ethers, vinyl chloridei vinyl furan, N-vinylcarbazole, allyl (me~h)acrylate, triallyl isocyanurate, ethylene di(m~th)arylate, butylene di(meth)acrylate, diallyl maleate, and maleic anhydride;
maleimide compounds such a~ maleimide, and N-phenyl (or alkyl) maleimide~; acrylamides; N-(mono or disubstituted) acrylamides, and mixtures of any of these monomers. In general, any rubbery or glassy vinyl type monomer may be used which can be mixable with the organosiloxane.
. Preferred vinyl-ba ed polymer components of the first stage substrate of the polyorganosiloxane/-polyvinyl-based graft copoly~er compri~e pri~arily alkenyl aromatic units, (meth)acrylate units or mix~ures thereof. E~pecially preferred i~ poly~tyrene.
Typically, the vinyl-ba~ed component of the first stage co-homopolymer will be present in an amount of approximately 3 to 97 weight percent and correspondingly the organosiloxane component will be present in an amount of approximately 97 to 3 weight percent. Preferably, the vinyl-ba~ed component will ~3~ 5 -33- 337-2181 (8CT-4905) comprise approximately S to 45 weight percent of ~he first stage of the co-homopolymerized substrate.
The cros -linker composition u~ed in conjunc~ion with ~he organosiloxane component of the presen~ compositions can have the general formula:
R n ~ Si(ORl)4 n wherein n is 0, 1 or 2, preferably 0 or 1, and each independently represents hydrogen sr a monovalent hydrocarbon radical selected from among alkyl or aryl radicals having 1 to 1~ carbon atom~ preferably methyl, ethyl and phenyl. R~ can be the same as Rl or can be a vinyl, alkenyl, thio, or (meth)acrylo~y alkyl functional radical. When R2 is a vinyl, alkenyl, thio or acryloxy alkyl radical and n i 1, the cro~s-linker compound can also act as a graft-linker.
A preferred cross linker compound is te~ra-ethoxysilane. A co~bination cross~linking and graft-linking compound is vinyltriethoxysilane. Another suitable choice is gamma-me~hacryloxypropyl~rimethoxy-silane.
The multi-stage polyorganosiloxane/polyvinyl-based graft product of the present invention can be isolated by conventional mean~ such as hot solution coagulation. For exampl~, an electrolytic solution of about O.S to 5 percent aluminum sulfate or magnesium sulfate in water can be prepared and heated to about 75 to 95C. When the latex is added, with agi~ation, the graft product will precipitate and can be held at an elevated temperature for about 10 minutes whereupon it may be filter washed. Commerical latex isolation technique3 such as spray dryers may also be utilized.
The diene rubber-based graft polymer compositions comprise a first stage subs~rate of units -3~- 337-2181 (8CT-4905) derived from a diene rubber and optionally units derived from a cross-linking agent or agents. Diene~ are generally classified as hydrocarbon-based molecules having at least two conjugated double bond~. Other examples of diene rubbers are styrene/butadiene rubber, acrylonitrile~butadien~, isoprene rubber, chloroprene rubber or 1,3-dimethylbutadiene rubber~
Vinyl-based polymers useful in the subsequent stage~ of the diene rubber-based graft copolymer are selected ~rom alkenyl aromatic compound-~, (meth)acrylate compounds, vinyl cyanide compounds and acrylamide compounds.
Alkenyl aromatic polymer re~ins useful as component tb) are, in general~ those having at least 25 percent o~ their units derived fro~ a mono~er having the formula CRl =C~R2 R5 ~

wherein Rl and R2 are selected from the group consisting of lower alkyl or alkenyl groups of fro~ 1 to 6 carbon atom~ and hydrogen; R3 and R4 are selested from the group consisting of chloro; bromo, hydrog~n and lower alkyl of from 1 to 6 carbon atom~; R5 and R6 ire selected from the group consisting of hydrogen and lower alkyl and alkenyl groups of from 1 to 6 carbon~ or RS
2S and R6 may be concatenated together with hydrocarbyl group~ to ~or~ a naphthyl group.
Materials that may be copolymeri~ed with ~he units of the alkenyl aromatic monomer include tho~e having the general formula:

, ~6~3~3~L35 -35 337-2181 (8CT-4905) R7 - C~ = C-~ C~2~ R

wherein R7 and R8 represent a subs~ituent selec~ed from the group consisting of hydrogen, halogen, an alkyl group of 1-4 carbon atom~ carboalkoxy or R7 and R8 taken together represent an anhydride linkage (-COOOC-), and R is hydrogen, vinyl, an alkyl or alkenyl group having 1 to 12 carbon atom~, cycloalkyl, carboalkoxy, alkoxy-alkyl, alkyl carboxyl, ketoxy, halogen~ carboxy, cyano or pyridyl and n is 0 or a whole number between 1 and 9.
~ Meth)acrylates are generally produced in a two-~ep proce~3 wherein an acetone is reacted with a hydrogen cyanide to form an acetone cyanohydrin which is then heated in the presence of an alcohol to produce the (meth)acrylate. Preferred (meth~acrylates are methyl acrylate, ethyl acrylate, butyl acrylate and methyl me~hacrylate.
Vinyl cya~ides useful ln the practice of th0 present inventio~ are comprised of the following general formula CN
C~2 ' CRl wherein Rl is an alkyl group o~ from 1 to 6 carbon atom~.
Acrylamide~ are well known in the art and generally comrpise hydrocarbon3 having a group comprising the following general formula C~2 = C~ - C ~ ~2 ~ .; ., . .,, ~ . . . .
.

~)3~
-36- 337-2188 (8CT-4905) Preferred embodiments of the diene rubber-based graft poly~er are a first stage ~a)(ii) compri~ing units of a polybutadiene rubber and subsequent stage or stages (b) comprising poly(methyl methacrylate), me~hyl methacrylate/styrene copolymer or methyl methacrylate/
acrylonitrile copolymer.
The thermoplastic resin composition may also contain an effective amount of any suitable additives such as addition rubbers, polymers, fillers, pigments, waxes, lubricants, proces~ing assis~ant~, dyes, antioxidan~s, heat stabilizers, ultraviolet light absorber and mold release agents.
The reinforcing filler can be comprised of any organic or inorganic filler in~luding but not limited to ~lass fiber, carbon fiber, aramid fiber, metallic fiber~
whisker, glass beads, glas~ flakes, calcium carbonate, talc, mica, aluminum oxide, magnesium hydroxide, boron extrude, beryllium oxide, calcium silicate, clay or metal powder.
Platinum compounds are often utilized in conjunction wi~h polyorganosiloxane Gompositions in order to enhance the flame re~ardance of the latter.
Platinum complexes are also used a~ cataly~ts in certain hydrosilation processes although such catalysts are not necessary for the practice o~ the prese~t invention. A~
flame retarding additive~, however, there may be utilized the reaction product of chloroplatinic acid and organosilicon compounds a~ described in U.S. Patent No.
3,220,972. Another platinum compound is seen in U.S.
Patent No. 3 "75,452 de~cribing platinum-containing polyorganosiloxanes. Other fire retardants are compounds based on elemen~ary red phosphorous compounds, other phosphorou~ compounds, halogen~, antimony oxide~, iron oxides, zinc oxides and the likeO

~)39~
37- 337-2181 (8CT-490~) Preferably, component A, A-l, A~2, A-3 or A-4 comprise3 from 1 to 99 parts by weight and component B
co~prises from 99 to 1 part by weight per 100 parts by weight of A, A-l, A-2, A 3 or A-4 and B combined.
S Modifier composition (B) is comprised of from 1 to 99 part~ by weight of componen~ (1) and from 99 to 1 part by weight of component (2) based upon 100 parts by weight of tB).
When the polyphasic resin composition comprises the preferred embodi~en~ of mixture (~
comprising (i) a polycarbonate resin phase and (ii) a saturated polyester re3i~ pha~e and modifier composition (B) compri5ing two polyorganosiloxane/polyvinyl-based graft polymers, in combination, component (Aol) pre~erably co~prise~ from about 99 to about 37 parts by weight and component (B) comprises from about 1 to about 63 part~ by weight per 100 parts by weight of (A-l) and (B) tog~the~.
In general, the first stage comprising the polyorganosiloxane-based polymer subs~rate, ~he diene rubber-ba~ed polymer subctrate or the co-homopolymerized polyorganosiloxane/polyvinyl-ba~ed substrate each will independently comprise approximately 5 to 95 weight percent of the correponding to~al graft polymer ba~ed upon the weight of the first stage and the subsequent stage or stages taken together. Pr~ferably the first stage will comprise approximately 30 to 90 weight percent on the same ba~is. Correspondingly, the subsequent stage~, comprising the additional grafted vinyl polymers, will comprise approximately 95 to 5 weight percent and preferably approximately 70 to 10 weight percent on the same basis. In the multi-stage systems, preferably9 the ratio o~ fir~t s~age substrate (l)(a) and/or (2)(a) to second stage polymer (b)~

10:90 to 90:10 and the amoun~ of third stage polymer 3~3~

-38- 337-2181 (8CT-4905) (b)(ii) co~prises ~rom about 10 to about 90 parts by weight of (l)(a) and/or (2)~a), (b)(i) and (b)(iij combined~
Subsequent stages (l)(b) and 12)(b) may differ in the selection of monomeric units which comprise the polymers or may di~fer in the ratio of ~he same monomeric units in each of ~he sub~equent stages to each other which comprise the polymer~.
The amount of polymerized or copolymerized (meth3acrylonitrile units in the outermost stage of each of the component~, (1) and (2) of modifier composition (B) based upon the weight o~ the corresponding outermost stage will determine into which phase of the resin blend the particular graft polymer will be induced to migrate lS and finally to segregate. For example, in a modified (PC)/(PBT) blend, it is believed that such segregation i3 dictated by the interfacial energy variation~ ~etween the modifiers and the resins comprising the blend, with ~he co~ponents having outermo~t stages wi~h higher levels of polymerized or copolymerized (meth)acrylonitrile migrating to the more brit~le PBT ph~se and the components havins outermost stages with either no or low levels of tmeth)acrylonitrile migrating to the PC phase.
Therefore, by varying the a~ount of polymerized or copolymerized (meth)acrylonitrile in the outermost ~tage of the components of a multi-component modifier, portions of the modifier can be distributed in each phase of the blend re~ulting in two or more phases of the blend being simultaneously modified. As a result, improved impact modi~cation and particularly superior low temperature toughness and lower ductile/brittle transition of multi-phase blends is aocompli~hed by this dual-phase modifica~ion aR compared to blends having modifiers in only one resin phase. Additionally, the X~3~35 _39- 337-2181 (8CT-49n5) proce~sing difficultie~ associated with melt gra~ing chemistry are eliminated.
Preferably, the content of polymerized or copolymerized (meth)acrylonitrile units in ~he outermost stage of multi-stage composition (1) range~ from 0 ~o les~ than about 20 percent by weight of that outermost stage, and the content of polymerized or copolymerized (meth)acrylonitrile uni~s in the outermost stage of multi-stage compositlon (2) range~ upwardly from greater than abou~ 20 percent by weight of that outermost stage.
Most preferably, the conten~ of polymerized or copolymerized (meth)acrylonitrile units in the outermost stage of multi-stage oomposition (1) rangas from 0 to about 5 percent by weight of that outermost stage, and the content of polymerized or copolymeri~ed (me~h)-acrylonitrile units in the outermost ~tage of mul~i-stage composition (2) ranges upwardly from greater than about 25 percent by weight of that outermo~t stage.
It is believed that in a polypha~ic re~in composition comprised of (A~ i) a polycarbona~e resin phase and (ii) a saturated polye~ter resin phase, incorporation of a major fraction of the modi~ier in the more brittle PBT phase is important in aehieving maxi~um low temperature toughness.

D~SCRIPT~O~ OF T~ PREF2RR~D ~BODI~ENTS
~he following examples illustrate the invention without-limita~ion. All part~ are given by weight unle~s otherwise indicated. Impact strengths are reported as notched Izod (NI) according to ASTM D-256 at room temperature (23C) unle~s otherwise ~pecifled and as Charpy NI in a falling weight test~ Weld line strenqth (DG) i~ measured on one-eighth inch unno~ched Izod bars molded in a double-ga~ed mold. Ten~ile propertie~ are measured by ~STM D-638 as Tensile Yield Strength, Tensile Break Strength, Tensile Modulus, ~39~ 5 -40- 337-2181 ~8CT-4905) Elongation at Yield and Elongation at Break. 5urface gloss, 60, is measured by ASTM D-523 7 and Delta Yellowness Index is measuced by yellowne s index increase after aging for 96 hours at 125C.
A single slash is used between monomers of a single stage, and a double slash or a hyphen is used as a shorthand method of indicating separa~ion between stages. The first stage to be polymerized is written first before the double slash or hyphen, and subsequent ~tages are written subsequently.

~A~PLX 1 A well mixed dry blend of 50 parts of polycarbona~e (Lexan~ 141), 40 par~ of saturated polye~ter (Valox- 315), 0.9 part of a s~abilizer package, 2.5 parts of a CSiM modifier ((~i/P5)-MMA wt.
ratio of 70:30, 5i/PS wt. ra~io of 95:5) and 7,5 parts o~ a C5iM modifier ((Si/PS)-S/AN w~. ra~io of 70:30, Si/PS wt. ratio of ~5:5, S/A~ w~. ratio o~ 75:25) is extruded on a Welding Engineers twin screw extruder operating at 400 rpm (65 gm/min) with barrel zones se~
at 250, 375, 510 r 510 ~ 510 and 510Fo Tensile and notched Izod bars are molded in a Boy injection molding machine at 280C. A sample is also thermally aged at 120C for 168 ho~rs. Tests on both aged and non-aged sample~ are conducted according to the above methods.
Segregation o the two CSiM modi~ier~ i~ illustrated in FIG. 1. The C9iM modi~ier ((Si/PS)-MMA wt. ratio of 70:30~ S~PS wt. ratio of 95:5~ (5) appears a~ separate particles in the polycarbonate (1) phase of the PC(l)/PBT(3) blend, and the CSiM modifier ((8i/PS)-S/AN
wt. ratio of 70~30, SijPS wt. ra'~io of 95:5, S~AN wt.
ratio of 75:25) (7) appears in the PBT (3) phase o~ the PC(l)/P8T~3) blend of the non-aged sample. Properties are summarized in Table 1.

~3~3~35 -41- 337-2181 (8CT 4905) CO~ARA~
The procedure of Example 1 i~ followed substituting a dry blend of 50 parts of polycarbonate (Lexan 1~13, 40 parts of sa~urated polyester (Yalox 315), 0.9 part o~ a stabilizer package and 10 par~s of a CSiM modifier ((Si/PS~-S/AN wt. ratio of 70~30 7 Si/PS
Wto ratio o~ 95.5, S~A~ Wto ratio of 75:253. FI~. 2 illustrates the complete segr~gation of the CSiM
modifier ((Si/PS)-S/AN wt. ratio of 70 30, Si/PS wt.
ratio of 95:5, S/AN wt. ratio of 7S:25) t7) in the PBT(3) phase of the PC(1)/PBT(3) blend of the non-aged sample. Properties are summarized in Table 1.

co~
The procedure of Example 1 i~ followed substituting a dry blend of 50 parts of polycarbo~ate (hexan- 141), 40 parts of sa~urated polyester (Valox 315), 0.9 part of a stabilizer packa~e, and 10 parts of a CSi~ modifier ((Si/PS)-~A wt. ratio of 70:30, Si/P5 wt. ratio of 95:5). Thermal aging is carried out at ~0 90C for 96 hours. FIG~ 3 illustrate3 the compl~te seqregation of the CSiM modi~ier ((Si/PS~-M~A, wt. ratio of 70:30, Si/PS wt. ratio of 95:5) (5) in the PC(l) phase of the PC~l)/PBT(31 blend of the non-aged sampl2.
Properties are summarized in Table 1.

ISD~LI~ 2 T~e procedure of Example 1 i5 followed substi~uting a dry blend of 50 parts of polycarbonate (Lexan 141), 40 part~ of ~aturated polyester (Valox 315), 0.9 part of a stabilizer package, 7.5 parts of a CSiM modifier ((Si/PS)-MM~/A~ wt. ratio of 70:30, SiJP5 wt. ratio of 95:5, M~A/AN wt. ratio of 75:25) and 2.5 parts of a CSiM modifier ((Si/PS)~MMA Wto ratio o 70:30, Si/PS wt. ratio of 95:5~. Properties are summarized in Table 1.

3~
-42- 337~2181 (8CT-4905) ~PAaATrV~ ~a~P~ 2~*
__ ~__ The procedure of Example 1 is followed sub~tituting a dry blend of 50 parts of polycarbonate (Lexan~ 141), 40 parts of satura~ed polyester (Valox-315), Q.9 par~ of a stabilizez package, and 10 parts of a CSiM ((Si/PS)-M~A/AN Wto ratio of 70:30, Si/PS wt.
ratio of 9;:5, MMA/AN wt. ratio of 75:25). FIG. 4 illustrates ~he comple~e segregation of the CSiM
modifier ((5i/P~)MMA/AN wt. ratio of 70:30, Si/PS w~
ratio of 95:5, MMA/AN wt. ratio of 75:25) i~ the PBT(3) phase of the PC(l)/PB~(3) blend of the non-aged sa~ple.
Propertie~ are summarized in ~able 1.

~ ~ L~ 3 The procedure of ~xample 1 is followed substituting a dry blend of 50 parts of polycarbonate (Lexan~ 141), 40 parts of saturat~d polye~er (Yalo~
315), 0.9 part of a stabilizer package, 7.5 parts of a CSiM modifier ((Si/PS)-M~A/~N wt. ratio of 7n:30, Si/PS
wt. ratio of 95:5, MMA/~N wt- ratio of 75:25) and 2O5 parts of a CSiM modifier ~(S1/PS)-M~/AN wt. ratio of 70:30, Si/PS wt. ratio of 95:5, M~A/A~ wt. ratio of 95:5). Prop~rtie~ are su~marized in Table 1.

CO ARATIVB ~ PL~ 3A*
The procedure of Example 1 i~ followed substituting a dry blend of 50 parts of polycarbonate lLexan 141), 40 parts of saturated polyester (Valox-315), 0.9 part of a stabilizer package, and 10 parts of a CSiN (~Si/PS)-M~h/~N wt. ratio of 70:30~ Si~PS wt.
ratio o~ 95:5, MMA/AN wt. ratio of 95:5). FIG. 5 illustrate~ the co~plete segregation of the CSiM
~odifier ((Si/PS)MMA/AN wt. ratio of 70:30, Si/P~ wt.
ratio of 95:5, M~A~l wt. ratio of 95:5~ (ll) in the PC~l) phase of the PC(l)/PBT(3) blend of ~he non-aged sample. Properties are sum~arized in Table 1.

':

3~5 -43- 337-2181 (8CT-4905) Inspection of Table 1 below shows that the polyphasic resin blends of Examples 1, 2 and 3, which have CSiM modifier in both re~in phases, have significantly lower ductile/bri~tle transition, i.e.
-~5C, than Comparative Examples lA*, 1~*, 2A* and 3~*
which have modifier in only one resin phase. The dual-phase modified blend~ achieve optimum levels of toughening, particularly at low temperature , as is seen by the impact s~rengths of Example~ 1, 2 and 3 when compared wi~h the Comparative Examples a~ ~30C and lowerO The incorporation of a major portion of the impact modifier in the more brittle P8T phase appears to be ~mportant in achieving maximum low temperature toughness, again as illustrated by E~amples 1, 2 and 3.
Figure~ 1, 3 and 5 show that when li~tle or no (meth)-acrylonitrile units are present in the ou~ermost stage of a component tha~ the modifier compon*nt segregates in the polycarbonate pha~e of the PC/PBT blend~ Figures 1, 2 and 4 show that when higher amounts, such as at least 25 percent by weight, of (me~h)acrylonitrile units are pre~ent in the outermost stage of the modifier component, the modifier component segregates in the PBT
phase of the PC/P3T blend.

~1[33~35 _~4_ 337-2181 (8C~-490S) 1 o c~ a~ o 0 ^ r~ ~ O

~1 o cn u~ ~ o o U~ ~ I I s ~ n o I 1~ a~ c o ~ I
_, _ t~
. ~ 1 o o ~ o a~ ~ o u~

æ
z u~ ~

ml o o ~ O ~ o _ _ _ t- _ ~
~~ o o al o '~
Z ~ u~ ~r . ,~ I I I ~ I ~ ~ I ~ u~ I r~ 1` ~ o ~2 O ~ _ U~
~e o P~
r~ O O a~

u u c~
a. -- O ~ O .~ _ O ~ _ O
- ~ o u o ~ o ~ ~ c~ o ~ o ~ ~ ~ ~ 9 0 ~ ~ ~ ~ 9 r~7 .C ~ o ~ o ~ _I ~ ~ o ~ o ~ ~
c ~ ~ ~ 0 .8 ~U N e ~
ILI ~ ~ 0 J Ll ~ ~3 i V ~ U U U ~ Ll aa U ~ s ,~ ~ ~n o In ~ U~
~1 O O ~ U~
P~U t.~ U i'~

~1)3~35 -45~ 337-2181 (8CT-4905) TABLE 1 (Cont'd) :~ r A - Lexan~ 141, poly(bisphenol-~ carbonate), General Electric Company B - Valox~ 315, poly(l,4-butylene ~erephthalate), General Electric Company C - (Si/PS)-S/AN wt. ratio of 70:30, Si/PS wt~ ratio o~
95:5, 5/AN wt. ratio of 75:25 D - (Si~PS)-M~A wt. ratio of 70:30, Si/PS wt. ratio of 9s:5 - (Si/PS~-MMA/AN wt. ratio of 70:30, 5i/PS wt. ratio of 95:5, MMA/AN wt. ratio of 95:5 F - (Si/PS)-MMA/AN wt. ratio o~ 70O30~ Si/PS wt. ratio of 95.5, M~A/AN w~. ratio o 75~25 ;~3~3~
46- 337-2181 (8CT-4905) ~r~KP~B ~
A dry blend of 50 par~s of polycarbo~a~e (Lexan~ 141), 40 parts of saturate~ polye~ter .(Valox 315), 0.9 part of a stabilizer package, 5 parts of a butadiene rubber substrate~S~MMA outermost stage modifier (Acryloid ~-653) and 5 parts of a high rubber graft ABS modifier (A-B-S wt. ratio of 7.5:70:~2.5 - U.S.
Pa~ent No. 4,753,986) i5 compounded via a ~ingle pas~
extrusion process at 500F on a Welding Engineers twin screw e~truder, pelletized, and molded. Segregation of these two modifiers is illustrated in FIG. 6. The ~M-653 (13) modifier with no acrylonitrile in the outermost stage appears in the PC(l) phase and the ABS
modifier (15) appears in the PBT ~3) phase of the PC(l)/PBT(3) blend.

C} ~
The procedure of Example 4 i~ followed substituting a dry blend of 15 part~ of polycarbonate (Lexan- 141), 70 parts of saturated polyester (Valox~
315), 0.9 part of a ~tabilizer packag~, a~d 15 parts of a butadiene rubber substrate-S/MMA outer~o~t stage modi~ier (Acryloid~ 653). FIG. 7 illustrates the segregation of the modifier (13) in th~ PC(ll of the PC(l)/PBT(3) blend.

~SA~L~ 5 .
The procedure of Example 1 is followed ~ub~tituting a dry blend of 5U parts of polycarbonate resin tLex~n- 141~ 40 part~ of saturat~d polye~ter re~in (Valox~ 315), 2.5 parS~ of a CSiM modifier (tSi/PS)-MMA wt. ra~io of 70:30 7 Si/PS wt. ratio of 95:5) and 7.5 parts of a CSiM modifier ((Si/PS)-S/AN wt.
ratio of 70:30, Si/PS wt. ra~io of g5:5, 9/AN wt. ratio of 75:25). A composi~ion will be formed in accordance with the appended claims.

, ;~ ' , -47- 337-2181 (8CT-4905 ~A~P~ 6 The procedure of Example 1 i~ followed substituting a dry blend of 50 parts of polycarbonate re3in (Lexan~ 141), 40 parts of sa~urated polye~ter resin (Valox~ 315), 7.5 parts of a CSiM modifier ((Si/P5)-MMA/AN wt. ratio of 70:30, Si/PS wt. ratio of 95:5, MMA/~ wt. ratio of 75:25) and 2~5 parts of a CSi~
modifier ((Si/PS)-MMA w~. ratio of 70:30, Si/PS wt.
ratio of 95:5). A co~position will be for~ed in accordance with the appended claim~.

e~anPLe 7 The procedure of Example 1 is followed ~ubstituting a dry blend of 50 parts of polycarbonate resin (Lexan- 141), 40 part3 of saturated polyester lS resin (Valox 315), 7.5 parts of a CSiM modifier ((Si/PS)-MM~/~N wt. ratio of 70:30, Si/PS wt. ratio of 95:5, MMA/A~ wt. ratio of 75:25) and 2.5 parts of a CSiM
modifier ~(Si/PS)-M~A/~N w~. ratio of 70:30, Si/PS w~.
ra~io of 95:5~ MMA/A~ wt. ratio of 9S:5). A co~position will be formed in accordance with the append~d claims.

The procedure of Example 1 is followed substitu~ing a dry blend of 45 parts of saturated polye~ter re~in (Valox~ 315), 30 parts of polyphenylene ether resin (PPE) (vacuum vented, 14 parts of poly-carbonate re~in (HILEX~, poly~bi~phenol-A carbonate), General Electric Company), 2.5 parts of a CSiM modifier ~(Sl/PS)-MMA wt. ratio of 70:30, Si~PS wt~ ratio of 95:5) and 7.5 parts of a CSi~ modifier ~(Si/~5)-S/~N wt.
ratio of 70:30, Si/PS wto ratio of 95:5, S/AN wt. ratio of 75:25). A composition will be ~or~ed in accordance with th~ appended claimQ.

~3~ 5 -~8- 337 2181 (8CT-4905 ex~e 9 The procedure of ~xample 1 is followed substituting a dry blend of 46 parts o saturated polyester resin (Valox 315) 9 30 parts of polyphenylene ether re~in (vacuum vented), 14 parts of polycarbonate resin (~I~EXQ), 7.5 parts of a C~i~ modifier ((Si/PS)-MMA/AN wt. ratio of 70:30, Si/PS wt~ ratio of 95:5, MMA/AN wto ratio of 75:25) and 2.5 parts of CSiM
modifier ((Si/P~)-MMA wt. ratio of 70:30, Si/PS wt.
ratio of 95:5). A composition will be formed in accordance with the appended claim~. -~a~pL~ 10 The procedure of Example 1 i~ followed substituting a dry blend of 46 parts of saturated polye~ter re~in (Valox~ 315), 30 parts of polyphenylene ether resin (vacuum vented~, 14 parts of polycarbonate resin (~ILEX~)~ 7.5 parts of a CSiM modifier ((Si/PS)-M~A/AN wt. ratio of 70:30, Si/P5 Wto ratio of 95:5, MMA/AN w~. ratio o~ 75:25) and 2.5 pa~tR of a CSiM
modifier ((Si/PS)-MMA/AN wt. ra~io of 70~30, Si/PS wt.
ratio of 95:5, MMA/AN w~. ratio of 95:5). A composition will be formed in accordance wi~h the appended claims.

PROCED~R~ A
Genera~ Procedure ~or Sili~one Graft Copolymer (GSiM) Synthesis (Si-S~AN wt. ratio of 72:28, S/AN wt. r~tio of 75:25) To deionized water, 400 par~s, containing 1.33 parts of dodecylbenzenesulfonic acid dissolved therein, i~ added a mixture comprising 90 parts o~ octamethyl-cyclote~rasiloxane, 5 part~ of tetravinyltetramethyl-cyclotetrasiloxane, 5.5 parts of vinyltriethoxy3ilane, 1.7 parts of tetrae~hoxysilane, 1043 parts of gamma-methacryloxypropyltrimethoxysila~e, 0.67 part of divinylbenzene and 0.093 part of a platinum catalyst ;;
.

3~

-49- 337-2181 (8C~-~905) (Silicone Product No. 88034). The emulsion is homogenized by passing twice through a homogenizer at a pressure of 7600 to 8600 psi. The emulsion is then stored for 5 hours at 75C and cooled for 13 hours overnight. The silicone emulsion is then neutralized to p~ 7.S by adding 5 parts of 15 percent aqueous potassium carbonate solution. The silicone rubber ha~ a yield of about 83.5 percen~, a gel content of about 71.3 percent and a 14.6 degree of swelling. The ~ol fraction possesses a Mw/Mn of 48,600/19,700 mea~ured by gel permeation chromatography against polystyrene standards.
To the core latex is then graft polymerized a 75/25 mixture of styrene/acrylonitrile for 6 hours at 75C
which is persulfate initiated. The polymer~ are then lS isolated by coagulation and vacuum dried at 65C
resulting in a silicone-3tyrene/acrylonitrile weight ratio of 72:28 ba~ed on ~inal conversion. The S/A~
graft efficiency is 25 percent~

P~DC8DoR~ B
General Procedure for Silioone/Polys~yrene Gr a f t Copolymer (CSiM) Synthesis ((Sl/PS)-S/AN wt. ratio of 70:30, 5/AN wt ratio of 75 25) To 40Q parts of deionized water containing 1.33 parts o~ dodecylbenzene~ulfonic acid dissolved ~harein is admixed an organic mixture comprising 90 parts of oc~amethylcyclotetrasiloxane, 10 parts of tetravinyltetramethylcyclotetra~iloxane, 1.7 part~ of tetraethoxy~ilane, 1.43 par~s of gamma~methacryloxypropyl-trimethoxy~ilane, O.C97 part o~ a platinum catalyst 301ution, 33.3 parts of styrene and 0.67 part of divinylbenzene. The mixture is stirred and ~hen homogenized twice under an impinging pre~sure of about 8000 psi. ~he crude emul~ion is then polymerized at 75C for 6 hours followed by overnight cooling down to ~039~
-50- 337 2181 (8CT-4905) room temperature. A potassium persulfate solution (0.17 part in 8.17 parts deionized waterJ i~ added over the first four hours at 75C as a styrene polymerization initiator. The silicone/polystyrene substrate emulsion is then quenched by neutralization from p~ 1.7 to 8.1 _ following an optional addition of 0.67 part of GAFAC
RE610 which is predissolved in 6 parts o~ deionized water. The silicone/polystyrene rubber ha~ a polymerization yield of 87.3 percent, a mean diameter of 230 nm, a gel content of 78 percent and 13.6 degree of swelling. To the substra~e latex is grafted polymerized a 75/25 S~AN mixture for a total of 6 hours at 75C
u~ing potassium persulfate a~ the initiator. The substrate to S/AN weight ratio is 70:30, and the second stage graft efficiency is measured at 60 percent usin~
methyl ethyl ketone Soxhlet extraction.

PRCClCDaR~ C
CSiM ((Si/BA)-S/AN wt. ratio of 70:30, S/AN wt. ratio of 75lZ5~ Slo~he~i~
Procedure B i~ ~ollowed substituting butyl acrylate (3A~ for styrene a^~ the vinyl-based polymer component of the substrate latex.

PROC~D~ D
General Procedure for Sllicone/Polystyrene-BA-S/AN Grat Copolymer (CSiM) Synthe~is ((Si/PS)-BA-S/AN wt. ratio of 35:3~:30, S/AN wt. ratio of 75:25) rhe procedure of Procedure B i3 repeated to produce the silicone/polystyrene first stage substrate.
~owever, at the second stage, to the silicone/polystyrene latex is added one stream containing butyl acrylate, butylene glycol diacrylate, diallyl maleate, deionized water and sodiu~ dodecylbenzene sulfonate concurrently with another aqueous strea~ consi~ting of a water-soluble X [)3~35 -51- 337-2181 (8GT-4905) initiator over a period o~ 1 to 3 hours at 75C. The butyl acrylate to ~he dry silicone/polystyrene subs~rate weight ratio is aimed a~ 35s35. The S/AN graf~ing procedure of Procedure B is then repeated as are the isolation steps.

PROCZ W R~ ~

Procedure ~ i5 followed substituting poly-styrene for ~tyrene/acrylonitrile copolym~r a~ the graft stage.

PPOC~DU B ~

Procedure B i~ followed sub~tituting poly-(~ethyl methacrylatej for styrene/acrylonitrile copolymer as th~ grat stage.

A dry blend of 39 parts of a ~aturated polyester resin (poly(1,4-butylene ~erephthalate), P~, Yalox 315, General ~lectric Company), 45O75 parts o~ a polycarbonate re~in (poly(bisphenoloA carbonate~, Lexan~
141, General Blectric Company), 7 parts o~ a GSiM
modifier (Si-S/AN wt. ratio of 72:2B, 5/AN wt. ratio of 7S:25) prepared by the method of Procedure A, 7 parts of a butadiene rubber subs~rate-S/M~A outermo~t stage modifier ~Acryloid- RH-653, Rohm and ~aa~ Company) and 1.25 par~s of a stabilizer package are tumble mixed to give a homogeneous powdsr dispersion within the pellets.
The blend is then fed into a Werner Pfleiderer 30 mm twin screw extruder und~r the following conditionss 2~33~ 5 -5~- 337-2181 (8CT-4905) Screw Speed 200 ~pm Throughput Rate 20 lb/hr zone 1 195C
zone 2 210C
zone 3-5, die 230-250G.

The extrudate is pelletized, dried at 140F
and then Lnjection molded on a 75 ton Newbury molding mashine. A sample is then ~hermally aged at 125C for 96 hours. ~ests on both aged a~d non-aged samples are conducted~ Propertie~ are summarized in Table 2.

conpA2~TIv~ E~A~PL~ llA~
The procedure of Example 11 i5 followed substituting a dry blend of 39 parts of ~aturated polyester (Valox 315), 45.75 parts of polycarbonate (Le~an~ 141), 14 parts of a butadiene rubber subs~ra~e-S/M~A outermost stage modifier (Acryloid R~ 653), and 1.25 parts o~ a stabilizer package. Propertie~ are summarized in Table 2.

co~pa~ATIvE B8aNpL~ llB~
The procedure of Example 11 i~ followed substituting a dry blend of 39 parts of saturated polye~ter (Valox0 315~, 45.75 par~s of polycarbonate (Lexan~ 141), 14 parts of a GSiM modifier (~i-S/AN wt.
ratio of 72:28, S/AN wt. ratio o 75:25) prepared by the method of Procedure A and 1.25 parts of a stabilizer package. Properties are summarized in Table 2.

~ clearly demon~trated fro~ Table 2 below, only the example containing bo~h the diene-ba~ed modifier and the G5iM modifier in combination ~Example 11) exhibit~ uniformly good phy~ical propertie , possessing good impact re~istance, low temperature - . :

;. .

~3~

-53- 337-2181 (8CT-4905) ductility, tensile strength, de~irably low gloss, and re~istance ~o yellowing and property 108~ because of thermal aging. The blend containing only the diene-based modifier (Comparative Example 11~*) while exhibiting good strength related characteristics, exhibits poor resistance to yellowing and ha~ a high gloss. The blend containing only the GSiM modifier, (ComparatiYe Example llB*) doe~ not exhibit good low temperature ductility in the blends, ha~ poor thermal stability, and is inferior to the blend combina~ion (Example 111 in most other respects a-~ well.

~03913~
~54 337-2181 (8CT-4905) ~BLB 2 POLY~ST~/POLYCARBO~T~ G5i~ ~ODIFI~ BL~DS
~a~ple 11 11~ llB~
C01a~08itio!1 Polyester Resin A 39 39 39 Polycarbonate Resin B 45.75 45.754S.75 ~-653 C 7 14 GSiM D 7 _ 14 Stabilizess 1~25 1.251~25 Propertie~
60 Gloss, ~ 62.3 96.0 68.3 NI @ R.T. (ft-lbs/in) .125~
Non-Aged Sample 12.6 12.1 11,4 Thermally Aged Sample 11-0 10.8 3O0 Retention, % 87~3 89.3 26.3 Delta Yellow Index 5.5 18~9 4.9 Cbarpy NI, (ft-lbs/in) R.~. - 8.1 10C - - 6.1 0C ~.1 8.8 2.8 -10C 7.6 8.0 2.9 -20C 5.1 3.1 -30C 2.7 2.9 2.0 Tensile Strength Yield, Kpsi 6.7 8.1 6.9 Break 5.6 6.6 6.1 Tensile Modulus Rpsi 14.9 15.5 14.4 Elongation, %
Yield 7.3 8.6 7.9 Break 42 169 ~9 A - Valox- 315, poly(l,4-butylene terephthalate), General Electric Company B - Lexan- 141, poly(bisphenol-A carbonate), General Electric Company C - Acryloid- KM-653, butadiene rubber substrate-S/MMA
outermost stage, Roh~ and Haas Co~pany D - 5i-S/~N wt. ra~io of 72:28, S/AN wt. ratio o 75:25, Procedure A

~ 3 5 -55- 337-2181 (8CT 49053 ~ P~ 12 The procedure of Example 11 is followed sub~tituti~g a dry blend of 39 parts (780 gram~) of saturated polye~tel (Valox9 315), 44.75 par~s (895 gram~) of polycarbonate (Lexan9 141)~ 1 part (20 grams) of polycarbonate (Lexan M~4545, poly(bisphenol-A
carbonate), General Elec~ric Company), 3.5 par~s (70 grams) of a butadiene rubber substrate-S~MMA outermost stage modifi~r (Acryloid~ RM-653), 10~5 parts (21U
grams) of a CSi~ modifier ((Si/PS)-S/AN w~. ratio o 70s30, S/AN wt- ratio of 75:25~ prepared by the method of Procedure B, 1 part (20 gram~ of red coloran (Red 624) and 1025 parts (25 gram~) of a stabilizer package.
Properties are ~ummarized in Table 3.

CO~ ~
The procedure of Example 11 i~ followed substitu~ing a dry blend of 39 par~s (780 gram~) o~
saturated polyestar (Valoxa 315~, 4~.75 parts (895 grams) of polycarbonate (Le~an~ 141), 1 part (20 grams) of polycarbonate (Lexan~ ML4545), 14 parts (280 gram~) I
of a butadiene rubber substrate-S~MMA outer~o~t stage modifier (acryloid ~M-653), 1 part (20 gram~) of red colorant ~Red 624) and 1.25 parts (25 gram~) of a stabilizer package. Properties are summarized i~ Table 3.

CO~PaR~IY~ ~AXP~ 12B~
The procedure of Example 11 is followed ~ub~tituting a dry blend of 39 part (780 grams) of saturated polyester (Valox~ 315~, 4~75 par~s (895 grams) of polycarbonate (Lexan4 141), 1 part (20 gram ) of polycarbonate (Lexan~ ML4545), 14 part3 (280 gram~) of a CSi~ modifier ((Si/PS)-S/AN wt. ratio of 70:30, S/AN wt. ratio of 75:25) prepared by the method of Procedure B, 1 part (20 gram~) of red colorant (Red 21~39~35 ~56- 337-2181 (8CT-4905) 624) and 1~25 parts (25 gram~1 o~ a stabilizer paekage.
Proper~ies are summarized in Table 3.

~ PLe 13 The procedure of Example 11 is followed substituting a dry blend of 39 par~ (780 grams) of saturated polye~ter (Valox~ 315), 44.75 parts (895 grams) of polycarbonate (Lexan~ 141), 1 part (2C grams) of polycarbonate (Lexan~ M~4545), 7 parts (140 grams) of a butadiene rubber substrate-S/~M~ outermost stage modi~iar (Acryloid- RM-653], 7 parts (140 gram~) of a CSiM modifier ~(Si/PS)-S/AN wt. ratio of 70:30, S/AN wt. ratio of 75:25) prepared by the method of Procedure B, 1 part (20 grams) of red colorant (Red 624) and 1.25 parts (25 grams) of a ~tabilizer package. Properties ar~
sum~arized in Table 3.

~PIi~
The procedure of Example ll i8 followe~
substituting a dry blend of 39 parts ( 780 grams ) of saturated polyester (Valox- 315); 44.75 parts (895 grams) of polycarbonate (Lexan- 141), 1 part (20 grams) of polycarbo~ate (Lexan~ M~4545), 10~5 parts (210 grams) of a butadiene rubber substrate-5/MMA outermost stage modifier (Acryloid~ K~-653), 3.5 parts (70 grams) of a CSiM modifier ((Si/PS)-S/~N wt~ ratio of 70:30, S/A~ wt.
ra~io of 75:25) prepared by the method of Procedure B, 1 part (20 gra~) of red colorant (Red 624) and 1.25 parts (25 gra~) of a stabilizer package. Properties are summarized in Table 3.

A~ can be ~een from Table 3 below, the samples containing the combi~ed modi~iers exhibit good impac~
resi~tance, appearance and low gloss characteris~cic~.
Comparative Example 12A* containing no C5~1~t, while Z~3~5 -57- 337-2181 ( 8CT-4905 ~

exhibiting good strength characteris~ics, is glo~sy and thu~ not useful in de~3ired losq gloss applications.

.
~, : . . .
.

5~- 337-2181 (8CT-4905) T~BL~ 3 RED PI~ T~D BL~DS
__ __ Esa~ples 1~ 12A~ 12B~ 13 1~
Polyester A 3~ 39 3~ 39 39 wt% (gms) (780) (780) (780) (780) (780~
Polycarbonate B 44O7S 44.75 44 75 44.75 44.75 w~ (gms) (895) (895) ~895) (~95) (~95) Polycarbonate C
wt~ (gms~ (20) (20) (20) (20) (20) RM-65~ D 3 5 14 7 10.5 wt~ (gms) (70) (280) (140~ (21n) CSiM E 10.5 - 14 7 3,5~
wt~ (gms) (210) (280) (140) (7o) Red Colorant F
wt~ (gms) (20) (20) (20) (20) (20) S~abilizers 1.25 1.25 1O25 1.25 1.25 wt~ (g~s) ~25) (25) (~5) (25) ~2~) ProFerties DG, ft-lbs/in 20.0 32.2 13.7 24.3 28.6 NI @ R.T., ft-lb3/in .125~
Non-Aged Sample13.9 14.1 12.2 13.3 14.4 Thermally Aged Sample 9.8 12.0 2O9 lI.1 12.3 % Retention 70.5 85~1 23.8 83.5 85.4 Color AppearanceDull Good Dull Good Good 60 Gloss 3593 94.2 27.2 50.7 70r7 A - Valox- 315t poly(l,4-bu~ylene terephthalate), General Electric Company a - Lexan- 141, polytbisphenol-A c~rbonate), General Electric Company C - Lexan- M~454S, poly(b~sphenol-A carbonate), General Elec~ric Company D - Acryloid- KM-653, butadiene rubber substrate-S/MM~ outermos~
stage, Rohm and ~aa3 Company E - tSi/PS)-S/AN wt. ra~io of 70:33, S/~N wt. ra~io of 75:~5, Procedure 3 F - Red 624 -59- 337-2181 (8CT-4905) s The procedure of Example 12 is followed sub~ti~uting the CSiM modifier ((5i/BA~-S/AN wt. ratio Of 70 30 ~ S/AN wto ratio o~ 75O25) prepared by the method of Procedure C ~or ~he CSiM modifier prepared by the method o~ Procedure B. A composition will be formed in accordance with the appended claims, e~pL~ 1~
The procedure of ~xample 12 is follow~d substituting the CSiM modifier ((Si/P5~-~A-S/~N wt.
ratio of 35:35:30, S/AN wt~ ratio of 75:25) prepared by the method of Procedure D for the CSi~ modifier prepa~ed by the method o~ Procedure B~ A compo~ition will be formed in accordance with the appended claims.

~ A~L~S 17-19 Example 12 i~ repeat~d three time~ adding - re~pectively an effective amount of red pho~phorous flame retardant, an effectiv~ amount of glas~ fiber and an effective amount o~ both red pho~phorous and glas~
fiber. Compositions will be ~ormed in accordance with the appended claims.

~PI.~ 20 The procedure of ~xample 12 i8 ~ollowed sub3tituting the CSiM modi~ier ((Si/PS)-PS wt. ratio of 70:30) prepared by the method of Procedu~e ~ for the CSiM modifi~r prepared by the method of Procedure B.
composition will b~ formed i~ accordanc~ with the appended claims.

~S~P~ 2l The procedure of Example 12 i8 followed substituting the C5i~ modifier (Si/PS-MMA wt. ratio of 70:30) prepared by the method of Procedure F for the ~3~35 -60- 337-2181 (8CT-4905) C5iM prepared by the me~hod of Procedure s. A
composition will be formed in accordance wi~h the appended claim~.

~A~PL~ 22 ~he procedure of 2xample 11 is followed, except dry blending is performed with no polye~ter re~in. A composition will be formed in accordance with the appended claims.

In the foregoing examples, the degree o~ ~
swelling can be determined in the ~ollowing fashion:
A prepared polyorganosiloxane ba ed latex i5 ' coagulated by adding it to about four times it~ volume of methanol and water (lsl volume ratio) containing 1 wt. percent MgSO4. ~he precipita~ed rubber i~ washed and vacuum-dried a~ 70C overnight. ~pproximately 1 g of the dry silicone-based rubber i~ immer~ed in 100 ml of toluene for 20 ~o 24 hour~ at ambient temperature and allowed to swell. The exce3~ tolu~ne is separated by decantation. The swelled polymer i~ vacuum-dried at 60C overnight, and the re8ulting polymer i~ weighedO
The degree o swelling is calculated a~: DS ~ ((weight of swelled polymer) - (weight of dry polymer)) divided by (weight of dry polymer).
Graft Efficiency can be determined by weighing dry multi-stage polyorgano~ilo~ane-~a~ed graft polymer in a weighed thimble which i~ Soxhlet extracted by acetone for 20 to 22 hours. After vacuu~ drying, the re~idue of the extraction is weighed. The graft efficiency is calculated a~: G~ (~) = t(weight of grafted monomer(s) x 100) divided by ~weigh~ of total monomer( 8 ) polymerized).
All patent~, applications, publications and t~st method~ mentioned above are hereby incorporated by ref~rence.

.

~ ~t~
-61- 337-2181 (8CT-4905) Many variations of the present invention will ~ugge~t them~elves to those skilled in this art in light of ~he above, detailed description. For example, the aromatic polycarbonate can be replaced in whole or in part wi~h a polye~ter carbonate containing units derived from bisphenol-~, phosgene and t~rephthaloyl chloride and/or isophthaloyl chloride. The aromatic polycarbonate can be replaced in whole or in part by a polycarbonate containing units of bis(3,5-dimethyl-4-hydroxy phenyl~-~ulfone, alone or combined with bi~phenol-A. ~he poly(ethylene terephthalate) can be replaced in whole or in part by poly(l,4-bu~ylene terephthalate~ or by a polyester derived from 1,4 cyclohexanedimethanol alone or combined with ethylene glycol and terephthalic acid and/or isophthalic acid. Pla inum complexes may be employed as catalysts in the hydro~ilation process.
Additionally, modifiers tB) compriQi~g four or more component co~bination~ can be designed such a-q two different CSiM's, a GSi~ and a diene rubber-based graft copolymer; two diffe~ent CSiM's and two differen~ diene rubber-based graft copolymers; two different CSiM9s and two different GSiM'ss three differen~ CSiM's a~d a GSiMt three different GSiM's and a CSiM two different diene rubber-ba~ed graft copolymers, a GSiM and a CSi~;
and the like. All such modifications are within t~e ull intended scope of the appended claims.

Claims (130)

1. A polyphasic resin composition comprising a mixture (A-1) comprising (i) a polycarbonate resin phase and (ii) a saturated polyester resin phase; a mixture (A-2) comprising (i) a polycarbonate resin phase, (ii) a saturated polyester resin phase, (iii) a poly(etherester) elastomer phase; (iv) a poly(etherimide ester) elastomer phase, (v) a polyphenylene ether resin phase or a mixture of (i), (ii) and any of (iii), (iv) and (v); or a mixture (A-3) of (A-1) and (A-2); and an effective amount of a modifier composition (B) comprising, in combination, (1) a multi stage graft polymer composition comprising (a) as a first stage, (i) an organosiloxane polymer, units derived from a cross-linking agent or agents and optionally units which serve as a graft-linking agent or agents;
( ii) a polymeric substrate comprised of units of a diene rubber and optionally units derived from a cross-linking agent or agents; or (iii) a polymeric co-homopolymerized substrate comprised of, in combination, an organosiloxane polymer; at least one vinyl-based polymer; and optionally units derived from a cross-linking agent or agents, units which serve as a graft-linking agent or agents, units derived from a cross-linking agent or agents and units from the same or different agent or agents which serve as a graft linking agent or agents or a mixture of any of the foregoing; and (b) at least one subsequent stage or stages graft polymerized in the presence of any previous stages and which is comprised of a vinyl-based polymer or a cross-linked vinyl-based polymer, the outermost stage of -63- 337-2181 (8CT-4905) which contains from zero to no more than an amount of polymerized or copolymerized (meth)acrylonitrile units which will induce migration of multi-stage composition (1) into said polycarbonate resin phase; and (2) a multi-stage graft polymer composition, comprising (a) as a first stage, (i) an organosiloxane polymer, units derived from a cross-linking agent or agents and optionally units which serve as a graft-linking agent or agents;
(ii) a polymeric substrate comprised of units of a diene rubber and optionally units derived from a cross linking agent or agents; or (iii) a polymeric co-homopolymerized substrate comprised of, in combination, an organosiloxane polymer; at least one vinyl-based polymer; and optionally units derived from a cross-linking agent or agents, units which serve as a graft-linking agent or agents, units derived from a cross-linking agent or agents and units from the same or different agent or agents which serve as a graft-linking agent or agents or a mixture of any of the foregoing; and (b) at least one subsequent stage or stages graft polymerized in the presence of any previous stages and which is comprised of a vinyl-based polymer or a cross-linked vinyl-based polymer, the outermost stage having a content of polymerized or copolymerized (meth)acrylonitrile units at least sufficient to induce migration of multi-stage composition (2) into said saturated polyester resin phase.

-64- 337-2181 (8CT-4905)

2. A composition as defined in Claim 1 wherein said content of polymerized or copolymerized (meth)acrylonitrile units in the outermost stage of multi-stage composition (1) ranges from 0 to less than about 20 percent by weight of said outermost stage and said content of polymerized or copolymerized (meth)-acrylonitrile units in the outermost stage of multi-stage composition (2) ranges upwardly from greater than about 20 percent by weight of said outermost stage.

3. A composition as defined in Claim 2 wherein said content of polymerized or copolymerized (meth)acrylonitrile units in the outermost stage of multi-stage composition (1) ranges from 0 to about 5 percent by weight of said outermost stage and said content of polymerized or copolymerized (meth)-acrylonitrile units in the outermost stage of multi stage composition (2) ranges upwardly from greater than about 25 percent by weight of said outermost stage.

-65- 337-2181 (8CT-4905)

4. A composition as defined in Claim 1 which also includes a multi-stage graft polymer composition (3) which is different than both (1) and (2) and comprises (a) as a first stage, (i) an organosiloxane polymer, units derived from a cross-linking agent or agents and optionally units which serve as a graft-linking agent or agents;
(ii) a polymeric substrate comprised of units of a diene rubber and optionally units derived from a cross-linking agent or agents; or (iii) a polymeric co-homopolymerized substrate comprised of, in combination, an organosiloxane polymer; at least one vinyl-based polymer; and optionally units derived from a cross-linking agent or agents, units which serve as a graft-linking agent or agents, units derived from a cross-linking agent or agents and units from the same or different agent or agents which serve as a graft-linking agent or agents or a mixture of any of the foregoing; and (b) at least one subsequent stage or stages graft polymerized in the presence of any previous stages and which is comprised of a vinyl-based polymer or a cross-linked vinyl-based polymer.

5. A composition as defined in Claim 1 wherein component A-1, A-2 or A-3 comprises from 1 to 99 parts by weight and component B comprises from 99 to 1 part by weight per 100 parts by weight of A-1, A-2 or A-3 and B combined.

-66- 337-2181 (8CT-4905)

6. A composition as defined in Claim 1 wherein said first stage substrate (1)(a) and (2)(a) each independently comprise approximately 5 to 95 weight percent of the total corresponding graft polymer composition (1) and (2) based upon the weight of said first stage and any subsequent graft stage taken together.

7. A composition as defined in Claim 1 wherein said first stages (1)(a) and (2)(a) each independently comprise approximately 30 to 90 weight percent of the total weight of each corresponding graft polymer composition (1) and (2).

8. A composition as defined in Claim 1 wherein in said polymers (1) and (2), at least one of said first stage substrates (1) (a) (iii) and (2) (a) (iii) independently are comprised of approximately 3 to 97 weight percent organosiloxane-based polymer and correspondingly about 97 to 3 weight percent vinyl-based polymer.

9. A composition as defined in Claim 8 wherein at least one of said first stage substrates (1)(a)(iii) and (2)(a)(iii) independently are comprised of approximately 5 to 45 weight percent vinyl-based polymer.

10. A composition as defined in Claim 1 wherein said organosiloxane polymers (1)(a)(i), (1)(a)(iii), (2)(a)(i) and (2)(a)(iii) independently are comprised primarily of units of the formula RnSiO(4-n)/2 wherein R is hydrogen or a monovalent hydrocarbon radical of about 1 to 16 carbon atoms and n is 0, 1 or 2.

67- 337-2181 (8CT-4905)

11. A composition as defined in Claim 1 wherein in said co-homopolymers (1)(a)(iii)/1(b) and (2)(a)(iii)/(2)(b), the vinyl-based polymer component of said first stage substrate (1)(a)(iii) and (2)(a)(iii) are independently comprised primarily of alkenyl aromatic units, (meth)acrylate units or a mixture thereof.

12. A composition as defined in Claim 11 wherein at least one of said vinyl-based polymer components comprises polystyrene.

13. A composition as defined in Claim 1 wherein said vinyl-based polymer in the subsequent stage or stages (1)(b) and (2)(b) independently comprise at least one selected from the group consisting of alkenyl aromatic compounds, (meth)acrylate compounds, vinyl cyanide compounds, maleimide compounds, and acrylamide compounds.

14. A composition as defined in Claim 13 wherein said vinyl-based polymers are independently selected from the group consisting of polystyrene, styrene/acrylonitrile copolymer, poly(methyl meth-acrylate), methyl methacrylate/acrylonitrile copolymer and styrene/methyl methacrylate polymer.

-68- 337-2181 (8CT-4905)

15. A composition as defined in Claim 1 wherein subsequent stages (1) (b) comprise (b) (i) a second stage comprising at least one vinyl polymer and optionally units derived from a cross-linkig agent or agents, units which serve as a graft-linking agent or agents, units derived from a cross-linking agent or agents and units from the same or different agent or agents which serve as a graft-linking agent or agents, or a mixture of any of the foregoing; and (b) (ii) a third stage comprising at least one vinyl based polymer or cross-linked vinyl-based polymer which is the same or different that (b) (i) , and which contains from zero to no more than an amount o polymerized or copolymerized (meth)acrylonitrile which will induce migration of multi-stage composition (1) into said polycarbonate resin phase; or subsequent stages (2)(b) comprise (b)(i) a second stage comprising at least one vinyl polymer and optionally units derived from a cross-linking agent or agents, units which serve as a graft-liniking agent or agents, units derived from a cross-linking agent or agents and units from the same or different agent or agents which serve as a graft-linking agent or agents, or a mixture of any of the forgegoing; and (b)(ii) a third stage comprising at least one vinyl-based polymer or cross-linked -69- 337-2181 (8CT-4905) vinyl-based polymer which is the same or different than (b)(i), and which has a content of polymerized or copolymerized (meth)acrylonitrile units at least sufficient to induce migration of multi-stage composition (2) into said saturated polyester resin phase; or subsequent stages (1)(b) comprise said (1)(b)(i) and said (1)(b)(ii) stages and subsequent stages (2)(b) comprise said (2)(b)(i) and said (2)(b)(ii) stages.

16. A composition as defined in Claim 15 wherein the ratio of first stage substrates (1)(a) and (2)(a), to corresponding second stage polymer (1)(b)(i) and (2)(b)(i) independently are 10:90 to 90:10 and the amount of corresponding third stage polymers (1)(b)(ii) and (2)(b)(ii), independently comprise from about 10 to about 90 parts by weight per 100 parts by weight of corresponding (1)(a), (1)(b)(i) and (1)(b)(ii) combined or (2)(a), (2)(b)(i) and (2)(b)(ii) combined.

17. A composition as defined in Claim 1 wherein said polycarbonate resin (i) comprises poly(bisphenol-A carbonate).

18. A composition as defined in Claim 1 wherein said saturated polyester resin (ii) comprises the reaction product of a dicarboxylic acid or chemical equivalent thereof and a diol.

19. A composition as defined in Claim 18 wherein said saturated polyester resin (ii) comprises poly(1,4 butylene terephthalate).

-70- 337-2181 (8CT-4905)

20. A composition as defined in Claim 1 wherein said poly(etherester) elastomer (iii) comprises a block copolymer consisting of (1) polyester segments and (2) polyether segments.

21. A composition as defined in Claim 1 wherein said poly(etherimide ester) elastomer (iv) comprises a block copolymer consisting of (1) polyester segments and (2) poly(etherimide) segments.

22. A composition as defined in Claim 20 wherein said polyester segments comprise poly(1,4-butylene terephthalate) and said polyether or poly(etherimide) segments comprise a polyalkylene ether glycol or an imide acid capped polyalkylene ether diamine, or a mixture of such segments.

23. A composition as defined in Claim 21 wherein said polyester segments comprise poly(1,4 butylene terephthalate) and said polyether or poly(etherimide) segments comprise a polyalkylene ether glycol or an imide acid capped polyalkylene ether diamine, or a mixture of such segments.

24. A composition as defined in Claim 1 wherein said poly(etherimide ester) elastomer (iv) is the reaction product of (a) one or more low molecular weight diols, (b) one or more dicarboxylic acids, and (c) one or more polyoxyalkylene diimide diacids.

-71- 337-2181 (8CT-4905)

25. A composition as defined in Claim 24 wherein said polyoxyalkylene diimide diacid is derived from trimellitic anhydride and a polyoxyalkylene diamine selected from the group consisting of polypropylene oxide diamine and a copoly(ethylene oxide/propylene oxide diamine having predominantly polyethylene oxide in the backbone.

26. A composition as defined in Claim 1 wherein said polyphenylene ether resin (iv) comprises poly(2,6-dimethyl-1,4-phenylene)ether, a copolymer of (2,6-dimethyl-1,4-phenylene)ether with (2,3,6-trimethyl-1,4-phenylene)ether or a mixture thereof.

27. A composition as defined in Claim 1 which also includes (C) an effective amount of a flame retardant agent.

28. A composition as defined in Claim 15 which also includes (C) an effective amount o a flame retardant agent.

29. A composition as defined in Claim 1 which also includes (D) an effective amount of a reinforcing filler.

30. A composition as defined in Claim 15 which also includes (D) an effective amount of a reinforcing filler.

-72- 337-2181 (8CT-4905)

31. A composition a defined in Claim 1 which also includes (C) an effective amount of flame retardant agent; and (D) an effective amount of a reinforcing filler.

32. A composition as defined in Claim 15 which also includes (C) an effective amount of flame retardant agent; and (D) an effective amount of a reinforcing filler.

33. An article folded from a composition as defined in Claim 1.

34. An article molded from a composition as defined in Claim 15.

35. An article extruded from a composition as defined in Claim 1.

36. An article extruded from a composition as defined in Claim 15.

37. An article thermoformed from a composition as defined in Claim 1.

38. An article thermoformed from a composition as defined in Claim 15.

73- 337-2181 (8CT-4905)

39. A polyphasic resin composition comprising a mixture (A-1) comprising (i) a polycarbonate resin phase and (ii) a saturated polyester resin phase; and an effective amount of a modifier composition (B) comprising, in combination, (1) a multi-stage polyorganosiloxane/polyvinyl-based graft polymer composition comprising (a) a a first stage, a polymeric co-homo-polymerized substrate comprised of, in combination, an organosiloxane polymer; at least one vinyl-based polymer; and optionally units derived from a cross-linking agent or agents, units which serve as a graft-linking agent or agents, units derived from a cross-linking agent or agents and units from the same or different agent or agents which serve as a graft-linking agent or agents or a mixture of any of the froegoing;
and (b) at least one subsequent stage or stages graft polymerized in the presence of any previous stages and which is comprised of a vinyl-based polymer or a cross-linked vinyl-based polymer, the outermost stage of which contains from zero to no more than an amount of polymerized or copolymerized (meth)acrylonitrile units, which will induce migration of multi-stage composition (1) into said polycarbonate resin phase; and (2) a multi-stage polyorganosiloxane/polyvinyl-based graft polymer composition comprising:
(a) as a first stage, a polymeric co-homo-polymerized substrate, which may be the same as or different than (1)(a), comprised of, in combination, an organosiloxane polymer; at least one vinyl-based polymer; and optionally units derived from a cross-linking agent or agents, units which serve as a graft-linking agent or agents, units derived from a cross-linking agent or agents and units from the same or -74- 337-2181 (8CT-4905) different agent or agents which serve as a graft-linking agent or agents or a mixture of any of the foregoing;
and (b) at least one subsequent stage or stages graft polymerized in the presence of any previous stages and which is comprised of a vinyl-based polymer or a cross-linked vinyl-based polymer, the outermost stage having a content of polymerized or copolymerized (meth)-acrylonitrile units at least sufficient to induce migration of multi-stage composition (2) into said saturated polyester resin phase.

40. A composition as defined in Claim 39 wherein said content of polymerized or copolymerized (meth)acrylonitrile units in the outermost stage of multi-stage composition (1) ranges from 0 to less than about 20 percent by weight of said outermost stage and said content of polymerized or copolymerized (meth)-acrylonitrile units in the outermost stage of multi-stage composition (2) ranges upwardly from greater than about 20 percent by weight of said outermost stage.

41. A composition as defined in Claim 39 wherein said content of polymerized or copolymerized (meth)acrylonitrile units in the outermost stage of multi-stage composition (1) ranges from 0 to about 5 percent by weight of said outermost stage and said content of polymerized or copolymerized (meth)-acrylonitrile units in the outermost stage of multi-stage composition (2) ranges upwardly from greater than about 25 percent by weight of said outermost stage.

-75- 337-2181 (8CT-4905)

42. A composition as defined in Claim 39 wherein component (A-1) comprises from about 1 to about 99 parts by weight and component (B) comprises from about 99 to about 1 part by weight per 100 parts by weight of (A-1) and (B) together.

43. A composition as defined in Claim 39 wherein component (A-1) comprises from about 99 to about 37 parts by weight and component (B) comprises from about 1 to about 63 parts by weight per 100 parts by weight of (A-1) and (B) together.

44. A composition as defined in Claim 39 wherein component (1) comprises from about 1 to about 99 parts by weight and component (2) comprises from about 99 to about 1 part by weight per 100 parts by weight of (B).

45. A composition as defined in Claim 44 wherein component (1) comprises from about 75 to about 99 parts by weight and component (2) comprises from about 1 to about 25 parts by weight par 100 parts by weight of (B).

46. A composition as defined in Claim 39 wherein said organosiloxane/vinyl co-homopolymer first stage substrate (1)(a) comprises approximately 5 to 95 weight percent of the total graft polymer composition (1) based upon the weight of said first stage and any subsequent graft stages (1)(b) taken together.

-76- 337-2181 (8CT-4905)

47. A composition as defined in Claim 39 wherein said organosiloxane/vinyl co-homopolymer first stage substrate (2)(a) comprises approximately 5 to 95 weight percent of the total graft polymer composition (2) based upon the weight of said first stage and any subsequent graft stages (2)(b) taken together.

48. A composition as defined in Claim 46 wherein said first stage substrate (1)(a) comprises approximately 30 to 90 weight percent of the total graft polymer composition (1).

49. A composition as defined in Claim 47 wherein said first stage substrate (2)(a) comprises approximately 30 to 90 weight percent of the total graft polymer composition (2).

50. A composition as defined in Claim 39 wherein said first stage substrates (1)(a) and (2)(a) are independently comprised of approximately 3 to 97 weight percent organosiloxane-based polymer and correspondingly approximately 97 to 3 weight percent vinyl-based polymer.

51. A composition as defined in Claim 39 wherein said first stage substrates (1)(a) and (2)(a) are independently comprised of approximately 5 to 45 weight percent vinyl-based polymer.

-77- 337-2181 (8CT-4905)

52. A composition as defined in Claim 39 wherein said organosiloxane polymer in first stages (1)(a) and (2)(a) are independently comprised primarily of units of the formula RnSiO(4-n)/2 wherein R is hydrogen or a monovalent hydrocarbon radical of about 1 to 16 carbon atoms and n is 0, 1 or 2.

53. A composition as defined in Claim 39 wherein said vinyl-based polymer components o said first stage substrates (1)(a) and (2)(a) independently are comprised primarily of the same or different alkenyl aromatic units, (meth)acrylate units or a mixture thereof.

54. A composition as defined in Claim 53 wherein at least one of said vinyl-based polymer components comprises polystyrene.

55. A composition as defined in Claim 53 wherein in addition to alkenyl aromatic units, at least one of said vinyl-based polymer components also includes divinylbenzene units.

56. A composition as defined in Claim 55 wherein at least one of said vinyl-based polymer components comprises styrene/divinylbenzene copolymer.

-78- 337-2181 (8CT-4905)

57. A composition as defined in Claim 39 wherein said vinyl-based polymer or cross-linked vinyl based polymer in any subsequent stage (1)(b) comprises at least one of selected from the group consisting of alkenyl aromatic compounds, (meth)acrylate compounds, vinyl cyanide compounds, maleimide compounds, acrylamide compounds, or any combination of the foregoing compounds.

58. A composition as defined in Claim 57 wherein said polymer is selected from the group consisting of polystyrene, methyl methacrylate, styrene/divinylbenzene copolymer, styrene/acrylontrile copolymer, methyl methacrylate/acrylonitrile copolymer, styrene/methyl methacrylate copolymer and styrene/
acrylonitrile/divinylbenzene terpolymer.

59. A composition as defined in Claim 39 wherein said polymer in any subsequent stage (2)(b) comprises at least one selected from the group consisting of alkenyl aromatic/acrylonitrile copolymer, methyl meth(acrylate)/acrylonitrile copolymer, maleimide/acrylonitrile copolymer and acrylamide/-acrylonitrile copolymer.

60. A composition as defined in Claim 59 wherein said polymer is selected from the group consisting of styrene/acrylonitrile copolymer and methyl methacrylate/acrylonitrile copolymer.

-79- 337-2181 (8CT-4905)

61. A composition as defined in Claim 39 wherein said subsequent stages (1)(b) comprise (b)(i) a second stage comprising at least one vinyl polymer and optionally units derived from a cross-linking agent or agents, units which serve as a graft-linking agent or agent, units derived from a cross-linking agent or agents and units from the same or different agent or agents which serve as a graft-linking agent or agents, or a mixture of any of the foregoing; and (b)(ii) a third s age comprising at least one vinyl-based polymer or cross-linked vinyl-based polymer which is the same or different than (b)(i) and which contains from zero to no more than an amount of polymerized or copolymerized (meth)acrylonitrile units which will induce migration of multi-stage composition (1) into said polycarbonate resin phase; or subsequent stages (2)(b) comprise (b)(i) a second stage comprising at least one vinyl polymer and optionally units derived from a cross-linking agent or agents, unit which serve as a graft-linking agent or agents, units derived from a cross-linking agent or agents and units from the same or different agent or agents which serve as a graft-linking agent or agents, or a mixture of any of the foregoing; and (b)(ii) a third stage comprising at least one vinyl-based polymer or a cross-linked -80- 337-2181 (8CT-4905) vinyl-based polymer which is the same or different than (b)(i) and which has a content of polymerized or copolymerized (meth)acrylonitrile units at least sufficient to induce migration of multi-stage composition (2) into said saturated polyester resin phase; or subsequent stages (1)(b) comprise said (1)(b)(i) and said (1)(b)(ii) stages and subsequent stages (2)(b) comprise said (2)(b)(i) and said (2)(b)(ii) stages.

62. A composition as defined in Claim 61 wherein the ratio of first stage substrate (1)(a) to second stage polymer (1)(b)(i) is 10:90 to 90:10 and the amount of third stage polymer (1)(b)(ii) comprises from about 10 to about 90 parts by weight per 100 parts by weight of (1)(a), (1)(b)(i) and (1)(b)(ii) combined; and the ratio of first stage substrate (2)(a) to second stage polymer (2)(b)(i) is 10:90 to 90:10 and the amount of third stage polymer (2)(b)(ii) comprises from about 10 to about 90 parts by weight per 100 parts by weight of (2)(a), (2)(b)(i) and (2)(b)(ii) combined.

63. A composition as defined in Claim 39 wherein said polycarbonate resin phase (A-1)(i) comprises the reaction product of (1) a dihydroxydiaryl-alkane, (2) a polyhydroxypolyarylalkane, or a mixture of (1) and (2), and (3) either (a) phosgene or (b) a diester of carbonic acid.

-81- 337-2131 (8CT-4905)

64. A composition as defined in Claim 61 wherein said polycarbonate resin phase (A-1)(i) comprises the reaction product of (1) a dihydroxydiaryl-alkane, (2) a polyhydroxypolyarylalkane, or a mixture of (1) and (2), and (3) either (a) phosgene or (b) a diester of carbonic acid.

65. A composition as defined in Claim 63 wherein said polycarbonate resin phase comprises a poly-(bisphenol-A carbonate) resin phase.

66. A composition as defined in Claim 64 wherein said polycarbonate resin phase comprises a poly-(bisphenol-A carbonate) resin phase.

67. A composition as defined in Claim 39 wherein said saturated polyester resin phase (A-1) (ii) comprises the reaction product of a dicarboxylic acid and a glycol.

68. A composition as defined in Claim 61 wherein said saturated polyester resin phase (A-1)(ii) comprises the reaction product of a dicarboxylic acid and a glycol.

69. A composition as defined in Claim 67 wherein said saturated polyester resin phase (A-1)(ii) comprises a poly(1,4-butylene terephthalate) resin phase.

70. A composition as defined in Claim 68 wherein said saturated polyester resin phase (A-1)(ii) comprises a poly(1,4-butylene terephthalate) resin phase.

-82- 337-2181 (8CT-4905)

71. A composition as defined in Claim 39 wherein said resin mixture (A-1) comprises (i) a poly(bisphenol-A carbonate) resin phase and (ii) a poly(1,4-butylene terephthalate) resin phase.

72. A composition as defined in Claim 61 wherein said resin mixture (A-1) comprises (i) a poly(bisphenol-A carbonate) resin phase and (ii) a poly(1,4-butylene terephthalate) resin phase.

73. A composition as defined in Claim 39 which also includes (D) an effective amount of a flame retardant agent.

74. A composition as defined in Claim 61 which also includes (D) an effective amount of a flame retardant agent.

75. A composition as defined in Claim 39 which also includes (E) an effective amount of a reinforcing filler.

76. A composition as defined in Claim 61 which also includes (E) an effective amount of a reinforcing filler.

77. A composition as defined in Claim 39 which also includes (D) an effective amount of a flame retardant agent; and (E) an effective amount of a reinforcing filler.

-83- 337-2181 (8CT-4905)

78. A composition as defined in Claim 61 which also includes (D) an effective amount of a flame retardant agent; and (E) an effective amount of a reinforcing filler.

79. An article molded from a composition as defined in Claim 39.

80. An article molded from a composition as defined in Claim 61.

81. An article extruded from a composition as defined in Claim 39.

82. An article extruded from a composition as defined in Claim 61.

83. An article thermoformed from a composition as defined in Claim 39.

84. An article thermoformed from a composition as defined in Claim 61.

-84- 337-2181 (8CT-4905)

85. A process for producing a polyphasic resin composition comprising the steps of (i) providing two first stage substrates independently by the concurrent co-homopolymerization of (1) an organosiloxane and one or more vinyl-based monomers;
(2) an organosiloxane, one or more vinyl-based monomers, and units which are derived from a cross-linking agent or agents;
(3) an organosiloxane, one or more vinyl-based monomers, and units which serve as a graft-linking agent or agents;
(4) an organosiloxane, one or more vinyl-based monomers, units which are derived from at least one cross-linking agent or agents and units of the same or different agent or agents which serve as a graft-linking agent or agents; or (5) a mixture of any of (1), (2), (3) or (4);
(ii) independently neutralizing each of the two reaction masses of the foregoing polymerization step to a pH of at least about 6.5 to provide a neutralized polyorganosiloxane/polyvinyl-based substrate latex;
(iii) graft polymerizing to one of said first stage substrates at least one vinyl-based monomer or a vinyl-based monomer and a cross-linker, said monomers being selected to provide that the outermost stage contains from zero to no more than an amount of polymerized or copolymerized (meth)acrylonitrile which will induce migration of the resultant multi-stage composition into the polycarbonate phase of a polycarbonate resin phase/saturated polyester resin phase mixture;
(iv) graft polymerizing to the remaining of said two first stage substrates a vinyl-based monomer or -85- 337-2181 (8CT-4905) vinyl-based monomer and cross-linker, said monomers being selected to provide that the outermost stage has a content of polymerized or copolymerized (meth)acrylonitrile units at least sufficient to induce migration of the resultant multistage composition into the saturated polyester resin phase of a polycarbonate resin phase/saturated polyester resin phase mixture;
(v) isolating said two multi-stage organo-siloxane/vinyl-based graft polymers to provide two poly-organosiloxane/polyvinyl-based modifiers for thermoplastic resins;
(vi) combining independent modifying amounts of said two polyorganosiloxane/polyvinyl-based modifier with a polyphasic resin mixture.

86. A process as defined in Claim 85 wherein in step (i), only one first stage substrate is provided and is subsequently divided into two independent portions to provide two first stage substrates.

87. A process as defined in Claim 85 wherein in step (i) only one first stage substrate is provided and in step (ii) the first stage substrate of step (i) is neutralized to a pH of at least about 6.5 and is then divided into two independent portions to provide two first stage substrates.

-86- 337-2181 (8CT-4905)

88. A process as defined in Claim 85 wherein the graft polymerization step (iii) is carried out in two successive stages comprising:
(1) graft polymerizing at least one vinyl-based monomer; or vinyl-based monomer in admixture with a cross-linker, a graft-linker or a cross- and graft-linker or a mixture of any of the foregoing to produce a second stage polymer or cross-linked polymer on said substrate and thereafter, (2) graft polymerizing at least one vinyl-based monomer or a vinyl-based monomer and a cross-linker which is the same as or different than that used in stage (1), to produce a third stage of polymer on said second stage, said monomers being selected to provide that the outermost stage contains from zero to no more than an amount of polymerized or copolymerized (meth)-acrylonitrile which will induce migration of the resultant multi-stage composition into the polycarbonate phase of a polycarbonate resin phase/saturated polyester resin phase mixture.

-87- 337-2181 (8CT-4905)

89. A process as defined in Claim 85 wherein the graft polymerization step (iv) is carried out in two successive stages comprising:
(1) graft polymerizing at least one vinyl-based monomer; or vinyl-based monomer in admixture with a cross-linker, a graft-linker or a cross- and graft linker or a mixture of any of the foregoing to produce a second stage polymer or cross-linked polymer on said substrate, and thereafter, (2) graft polymerizing at least one vinyl-based monomer or a vinyl-based monomer and a cross linker which is the same as or different than that used in stage (1), to produce a third stage of polymer on said second stage, said monomers being selected to provide that the outermost stage has a content of polymerized or copolymerized (meth)acrylonitrile units at least sufficient to induce migration of the resultant multi-stage composition into the saturated polyester resin phase of a polycarbonate resin phase/saturated polyester resin phase mixture.

-88- 337-2181 (8CT-4905)

90. A process as defined in Claim 85 wherein the graft polymerization step (iii) is carried out in the successive stages comprising:
(1) graft polymerizing at least one vinyl-based monomer; or vinyl-based monomer in admixture with a cross-linker, a graft-linker or a crossand graft-linker or a mixture of any of the foregoing to produce a second stage polymer or cross-linked polymer on said substrate, and thereafter;
(2) graft polymerizing at least one vinyl-based monomer or a vinyl-based monomer and a cross-linker which is the same as or different than that used in stage (1), to produce a third stage polymer of said second stage, said monomer being selected to provide that the outermost stage contains from zero to no more than an amount of polymerized or copolymerized (meth)-acrylonitrile which will induce migration of the resultant multi-stage composition into the polycarbonate phase of a polycarbonate resin phase/saturated polyester resin phase mixture; and the graft polymerization step (iv) is carried out in the successive stages comprising:
(1) graft polymerizing at least one vinyl-based monomer; or vinyl-based monomer in admixture with a cross-linker, a graft-linker or a cross- and graft linker or a mixture of any of the foregoing to produce a second stage polymer or cross-linked polymer on said substrate, and thereafter;
(2) graft polymerizing at least one vinyl-based monomer; or a vinyl-based monomer and a cross-linker which is the same as or different than that used in stage (1), to produce a third stage of polymer on said second stage, said monomers being selected to provide that the outermost stage has a content of polymerized or copolymerized (meth)acrylonitrile units at least -89- 337-2181 (8CT-4905) sufficient to induce migration of the resultant multi-stage composition into the saturated polyester resin phase of a polycarbonate resin/saturated polyester resin mixture.

91. A process as defined in Claim 85 wherein step (iv) is performed before step (iii).

92. A process as defined in Claim 85 wherein said polyphasic resin comprises a mixture of a polycarbonate resin phase and a saturated polyester resin phase.

93. A process as defined in Claim 88 wherein said polyphasic resin comprises a mixture of a polycarbonate resin phase and a saturated polyester resin phase.

94. A process as defined in Claim 89 wherein said polyphasic resin comprises a mixture of a polycarbonate resin phase and a saturated polyester resin phase.

95. A process as defined in Claim 90 wherein said polyphasic resin comprises a mixture of a polycarbonate resin phase and a saturated polyester resin phase.

-90- 337-2181 (8CT-4905)

96. A composition comprising a polycarbonate resin (A); a mixture (A-1) comprising (i) a polycarbonate resin and (ii) a saturated polyester resins; a mixture (A-2) comprising (i) a polycarbonate resin and (iii) a poly(etherester) elastomer, or (iv) a poly(etherimide ester) elastomer or a mixture of (iii) and (iv); a mixture (A-3) comprising (i) a polycarbonate resin, (ii) a saturated polyester resin and (iii) a poly(etherester) elastomer, or (iv) a poly(etherimide ester) elastomer or a mixture of (iii) and (iv); or a mixture (A-4) of any of the foregoing; and an effective amount of a modifier composition (B) comprising, in combination, (1) a multi-stage polyorganosiloxane-based graft polymer composition comprising (a)(i) as a first stage, an organosiloxane polymer, units derived from a cross-linking agent or agents and optionally units which serve as a graft-linking agent or agents; and (b) at least one subsequent stage or stages graft polymerized in the presence of any previous stages and which is comprised of a vinyl-based polymer or a cross-linked vinyl based polymer; and (2) a diene rubber-based graft copolymer composition comprising (a) (ii) as a first stage, a polymeric substrate comprised of units of a diene rubber and optionally units derived from a cross-linking agent or agents; and (b) at least one subsequent stage graft polymerized in the presence of any previous stages and which is comprised of a vinyl-based polymer or a cross-linked vinyl-based polymer, the weight ratio of (1) to (2) being from 1 to 9: 9 to 1; or -91- 337-2181 (8CT-4905) (1) a multi-stage polyorganosiloxane/polyvinyl-based graft polymer composition comprising, (a)(iii) as a first stage, a polymeric co homopolymerized substrate comprised of, in combination, an organosiloxane polymer; at least one vinyl-based polymer; and optionally units derived from a cross-linking agent or agents, units which serve as a graft-linking agent or agents, units derived from a cross-linking agent or agents and units from the same or different agent or agents which serve as a graft-linking agent or agents or a mixture of any of the foregoing;
and (b) at least one subsequent stage or stages graft polymerized in the presence of any previous stages and which is comprised of a vinyl-based polymer or a cross-linked vinyl-based polymer; and (2) a diene rubber-based graft copolymer composition comprising (a)(ii) as a first stage, a polymeric substrate comprised of units of a diene rubber and optionally units derived from a cross-linking agent or agents; and (b) at least one subsequent stage graft polymerized in the presence of any previous stages and which is comprised of a vinyl-based polymer or a cross-linked vinyl-based polymer, the weight ratio of (1) to (2) being from 1 to 9:9 to 1.

97. A composition as defined in Claim 96 wherein mixture (A-1) comprises (i) a polycarbonate resin and (ii) a saturated polyester resin.

-92- 337-2181 (8CT-4905)

98. A composition as defined in Claim 96 wherein component (A), (A-1), (A-2), (A-3) or (A-4) comprises from 1 to 99 parts by weight and component (B) comprises from 99 to 1 part by weight per 100 parts by weight of (A), (A-1), (A-2), (A-3) or (A-4) and (B) combined.

99. A composition as defined in Claim 96 wherein said first stages (a) in (1) and (2) comprise approximately 5 to 95 weight percent of the total graft polymer composition based upon the weight of said first stage and any subsequent graft stages taken together.

100. A composition as defined in Claim 99 wherein said first stages (a) comprise approximately 30 to 90 weight percent of the total weight of each graft polymer composition.

101. A composition as defined in Claim 96 wherein in said composition (1) said first stage substrate (a)(iii) is comprised of approximately 3 to 97 weight percent organosiloxane-based polymer and correspondingly about 97 to 3 weight percent vinyl-based polymer.

102. A composition as defined in Claim 101 wherein said first stage substrate, (1)(a), is comprised of approximately 5 to 45 weight percent vinyl-based polymer.

-93- 337-2181 (8CT-4905)

103. A composition as defined in Claim 96 wherein said organosiloxane polymer is comprised primarily of units of the formula RnSiO(4-n)/2 wherein R is hydrogen or a monovalent hydrocarbon radical of about 1 to 16 carbon atoms and n is 0, 1 or 2.

104. A composition as defined in Claim 96 wherein the vinyl-based polymer component of said first stage substrate (1)(a)(iii) is comprised primarily of alkenyl aromatic units, (meth)acrylate units or a mixture thereof.

105. A composition as defined in Claim 104 wherein said vinyl-based polymer component comprises polystyrene.

106. A composition as defined in Claim 96 wherein said vinyl-based polymer in the subsequent stage or stages (1)(b) and (2)(b) comprise at least one selected from the group consisting of alkenyl aromatic compounds, (meth)acrylate compounds, vinyl cyanide compounds, maleimide compounds, and acrylamide compounds.

107. A composition as defined in Claim 106 wherein said vinyl-based polymer is selected from the group consisting of polystyrene, styrene/acrylonitrile copolymer, poly(methyl methacrylate) and styrene/methyl methacrylate copolymer.

-94- 337-2181 (8CT-4905)

108. A composition as defined in Claim 96 wherein said first stage substrate (2)(a) comprises units of a polybutadiene rubber.

109. A composition as defined in Claim 108 wherein said subsequent stage or stages (2)(b) comprise poly(methyl methacrylate), a methyl methacrylate/styrene copolymer or a styrene/acrylonitrile copolymer.

110. A composition as defined in Claim 96 wherein said subsequent stages in components (1) and (2) comprise (b)(i) a second stage comprising at least one vinyl polymer and optionally units derived from a cross-linking agent or agents, units which serve as a graft-linking agent or agents, units derived from a cross-linking agent or agents and units from the same agent or agents which serve as a graft-linking agent or agents, or a mixture of any of the foregoing; and (b)(ii) a third stage comprising at least one vinyl-based polymer or cross-linked vinyl-based polymer which is the same or different than (b)(i).

111. A composition as defined in Claim 110 wherein the ratio of first substrate (1)(a) and (2)(a) to second stage polymer (b)(i) is 10:90 to 90:10 and the amount of third stage polymer (b)(ii) comprises from about 10 to about 90 parts by weight per 100 parts by weight of (1)(a), (2)(a), (b)(i), and (b)(ii) combined.

-95- 337-2181 (8CT-4905)

112. A composition as defined in Claim 110 wherein in (1) subsequent stage (b)(i) comprises a cross-linked butyl acrylate polymer and subsequent stage (b)(ii) comprises a styrene/acrylonitrile copolymer.

113. A composition a defined in Claim 96 wherein said polycarbonate resin (A) comprises poly(bisphenol-A carbonate).

114. A composition as defined in Claim 96 wherein said saturated polyester resin (ii) comprises the reaction product of a dicarboxylic acid or chemical equivalent thereof and a diol.

115. A composition as defined in Claim 114 wherein said saturated polyester resin (ii) comprises poly(1,4-butylene terephthalate).

116. A composition as defined in Claim 96 wherein said poly(etherester) elastomer (iii), poly(etherimide ester) elastomer (iv) or mixture of (iii) and (iv), comprises a block copolymer consisting of (1) polyester segment and (2) polyether or poly(etherimide) segments.

117. A composition as defined in Claim 116 wherein said polyester segments comprise poly(1,4-butylene terephthalate) and said polyether or poly(etherimide) segments comprise a polyalkylene ether glycol or an imide acid capped polyalkylene ether diamine, or a mixture of such segments.

118. A composition as defined in Claim 96 which also includes (C) an effective amount of a flame retardant agent.

-96- 337-2181 (8CT-4905)

119. A composition as defined in Claim 96 which also includes (D) an effective amount of a reinforcing filler.

120. A composition as defined in Claim 96 which also includes (C) an effective amount of flame retardant agent; and (D) an effective amount of a reinforcing filler.

121. An article molded from a composition as defined in Claim 87.

122. An article extruded from a composition as defined in Claim 87.

123. An article thermoformed from a composition as defined in Claim 87.

124. A composition as defined in Claim 110 which also includes (C) an effective amount of a flame retardant agent.

125. A composition as defined in Claim 110 which also includes (D) an effective amount of a reinforcing filler.

-97- 337-2181 (8CT-4905)

126. A composition as defined in Claim 114 which also includes (C) an effective amount of a flame retardant agent; and (D) an effective amount of a reinforcing filler.

127. An article molded from a composition as defined in Claim 110.

128. An article extruded from a composition as defined in Claim 110.

129. An article thermoformed from a composition as defined in Claim 110.

130. The invention as defined in any of the preceding claims including any further features of novelty disclosed.