EP4705421A2 - Upcycling of polyethylene and polypropylene and their mixtures to high-value surfactants - Google Patents

Abstract

Herein, a method for controlling the thermolysis products molar mass using a coolant fluid (e.g., water) to modulate the final products' condensation temperatures. With this strategy, the thermolysis of polyethylene (PE) and polypropylene (PP) is tailored to generate liquid oil, without any catalysts or additives. Subsequent addition of sulfuric acid across the alkenyl groups, followed by the neutralization with sodium hydroxide affords sulfate detergents with excellent foaming behavior.

Description

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--- °°,,°°,,°°,,°°,,°,°,°,°,°,°,°,°,°, .n °,°,°,rn rn wnnwmrr ° m°,°, r°mrr ° °,° °,° °, mrr ° ,°.n°m°,° °.nm , r ° °, ° °,r ° ,°.r mrr ° °,rn nnmr mrm,n vn.nrxm, nrnnrnm.mnnnrn:nrm mrn mmnrrnnr mrrnr mxrnnrr-rnmrnr mrnrrnr mrnr mrrnrn nr mr r r rnmnnr. vvnr n rm .rxm,nr mnnn nr nrmnr mr.nm , v nr nrn mn nm . rvnm , mr r nmn nn w r n v n w mxr v . r nmnn m mr wnrn nvr rm rnvrnn mxr , mnm rr m . r nn mrn mxr ,rrn m rrm r mnn mn vr nnn mr w ..,,, r,rm rr.nm , r nm rm r,rm ,,,,,, ,rrm r.nm , r nm ,, ,,,,,,,,,,,,,,,,,,,,,,,,,,,,,,,,,,,,,,, ,,,,,,,,,,,,,,r r.,,,,,,,,,, mxrn wmx , vn nnnr.mnmmn n w,nnnnrrv m w v m mxr wx.nm ,r vn mmn n nmnr. wrr n w m rn v . w nxm, nn nwnnnr n v nn r nn nrrn n nnrnr rrw nn v n n nn nr n v n ,mn mxnrrn wxr rv mmn n v n nr nr.nn vn wrn, nnr. n vmn w nnnr rv r r n.nmn r, - --- nrnnrr.rxmrn, vnn.rnnnr,n,,nr, w v r ,, ,,rnmnwn n v .,n, , , nrv rmrrrnn v .rxm, nr r znn v rn rr z nnrnrvnr m v r mrr wn n vn.r w nxm, m v rn v v m n v mrrwrn m v r n v .rxmr,r m m v . mxr wx n v n mmn n nxnrr wxnn v n w wxr , rn mxr w n wxm nnr. nnr rr, mmn nn r nn nrrn nnr rwrwnnn v n n nn nr nn wx, nnrn n rvmrr n m mxr v n mrr n m mxr wx mmn nwn m mxr wx n r nnrrr . mrr n nnrnn , ,n,v,r nnr.nm , nr, -n- m, nnr,mr,rr, nm ,,rzn ,x -n- r vrnr.n nr n nnrmr r n.rxm, r n mmn n nnr. nnr r rm v , v n rm v .n rmvrm nnrr rmvnn nnr.nmm,, r r r n nw nr nn rnr n nnr mvrm nnr, , rnm , w.r, , mnr, r ,r mnn xm., r nnrnnr n r nrr.r v n rn v rmnrnrrrn wn rn xmn, r mrr rnmrrn . vrxmrn,nr. w n n rn r rn, rn n nv.nmmrr,.n w nxm, rm nnrr mrnrmrr -° °.nm , °° °, -° °, -r° -°°, -°°, -°°, -°°, -°°, -°°°, - - --- °°,, - -°° °°,° -, -°°°,° -,° -°°°, -° °, -° °, -° ° °.nm , nnrm , -° °,° °,° °, -°, -°, - rr -°, -°, -°, -°, -°, -°, -°°,, - -°°,, - -°, -°, -°, -°, -°, -°, -°, -°, °, -°, -°, -°, -°, -°°, -°, -°, -°, -°, -°, -°, -°, -°, - °,°,°,°,°,°,°,, -°°,, -°°,, -°°, -°,°,°,°,°,°, °,°,°,°, ,°,°,°,°,°,°, °,°, °,°,°,°,°,°,°,°,°, °,°,°°,,r°°,r°n, rn°,w°,nn°w,m°,rr°,°.,°,°, mr wnrmrn, r mrrrn. mrrrnn vn v n w nnnnr.r.rnxm, m v wnm ,rr,,,,, m ,rrw mrrrn. wnnwnn ,,,r mrrrn.mrrrn n r mrr.nmnnmrrwnr rmrrn mrrnnnrmrr ,°m,rr rn wn v °,°,°,°°,,°°,,°° °,°,°,°,°, °,°,°, ,,°°,,°,°°,,r°n,m°,n°n,r°.,n°m, °,,rmr°r rn wn v n nnrr ° ,°. nm , mx,r rnrv rrrn wx,, ,r rvmnrmnnr.nxr m r rnn rrn mnn r r.nr wxnrnrnnr m. rn r rnn rrnrv r m m r rm n n. rrnn r . r n mmnnr rrnnrnrrrnnn n n. rm n rvrm nn m r nn rx rrn r .nm , mnxrm wnxnn r rnr nn vr rnnn , wrn mxrr mr wmxr wn - --- nr wnrvr r mnnnr rnrx,zrn.nm. , wx r rnnr rnmn mn,. mrr rrrrnnrrrn r mrn, w r n r w vr rn r mn, ,mr rn .xm rnrrrnnn r n, ,r 3•rr₂,₃•mrrn,n wr rn nm₃,rn₃•n,-₂₆,. rnrx. r x r ,rxm, r nm .,n , wx,,r mnnr nr n w r r rrx m.nn r mnn r,x wxzn,,r,m wnx,n,r mnnr n rn xz , wx,,r r r r r rrx. n r rn mnnr w r r nn rz. nn rmn n n,r mz.rr rnrrn nrz.nm , wnr n r nx mmxr, n n.xnmrn.xmrvnrnn ⁺, nr +z ,r₄z⁺n ,²⁺,r²⁺n r ,n²⁺rrn nnnn nmrn r nrnn mrxr mrx. nnn r rm , m r rnrrn rnn, w rr nrrnr rrnr m r rn. r rrn,rxm,nn nnr mrr nrnrm rnnr rnnnrnnrn.nnr,nrnnnnnrn nr r..,rrnr m r rnmr rrnrn .rnnn rr rn, rn rrn, w mrrn r n ,rm ,nrnr,nnrnvrn. .nrn mn r₂rn . nn nm, m, r r rnm, rm, n. r xm, n nm, - --- mr,rr-rr-n, nnnr'nm,,rr' , n r m r rx nr ,nn n. ,nm rx, m rrm rrnrnn r-x- r.nm nmnnr.rxm, wx,, , x m r rnnr rx n. r mnnr r rx mxr wx,, ,nm , mnn m r.rx r mrmnrnrrnnr rnmnn r r mnr nr nn r . mnnm rmnr rnnr,n vmr, w.x,n,r ,r mnnr x m , ,rxm,nn nrnrrn.n mx wnnrmnr w vx,,r ,mrr wmx,n,nr,rx xn x rmx wnnr n v . mnnr mnnnmn rw, n n n rm rnv m w r mnnr n rnr n r w r n. nr rnr rm, nnmmn nr, rrn rvnvnrn mnn n nrnrnn wn rz mrnnvrn nx xr n r rmnn r “”n.n “n,” rn, mnnr mr wn n rn nmr mnnnnvnnnr n nn m. “”n “n” “”r n rn m . r r nrrr nnr nnr n r r rr nxnr w rn m v nrrr nn n nn n nmmn nmrn,, n.mn,rrmn,nnrnmn,n vn mr r m rrr,nr, rn-nmm-nrn rr nrmnrr. nnr mn r rnn rrrm mrrn, vn nmn,,nr .mnmrn r nr - --- mnrrmrn nmnnvnn,r mmr v wr, n m rrn,.... wr ,,rrr,,rrrr rr. m nr ,,,r,-, ,,r,- .xm - n , rr m rmn ,vn n. wrm “ ” mn rmn, n,- , nr,- r rn,rn, x,- n,- n,,-rr- x, n,- n,r- n,rx,-,mnn,- n,- mn,- x-rnm ,x,rx,rn - xmn, n,- xrnmn,- xmn,- rn,rn,r- nmn,r rn r n m rrmn,- - x ,x,rx,rn n n. r,rm,rvmn,r m,nn nnr .., mrnnr,nrrrm n,.., r n,.,-n n,rx, x,rx,r n mmn, mnn . vnr n n x,.., , vnr. rn mnr vrnn, rmn “n,” “rxm,” “r ,”n “ n” mn r n mr xrn v. r, v rv vn r r rm n,rmr,n rn n nr mn,z, m rxm nrrrr rr r nn n n x, rnn mr, r, r n rn,nvrn r, v, mrmnrrrn ,n r rnwn n r vn rn rrr r n.nmrmn, v rv nr , rn,nn rn rmn.n , nr vrnn rw “ ”n “r ” mn nmn v n rrnrrnr “rn,r”r “.nrxmnr,,nmn,z,rm n,rmr . nr wr “ ,”r “r ” w rr nxr nv v, rmr ” “rxm,”r “r ” r rw. n nv v ,n , wrn nrn w wrnmr.nmnn rnn, wn nmw mr - --- mrnn wnmrn mnrxmn. vr wr r r wrnvr n nnmnnrnn r. mn nnrr.rnr wxn,nr nn,nn:mnnnmrr rm n mmn n w nnrrv m ,n v n nnr, wrn mxr wxnr r mrrvrr nn rn mrr v r mrrr nrrmmrnv mn mxnnr w vxnrr n.r . m rn nn - wrn rn mrr r v mn. n r ° °r mn vr r rm. m mn rn mnnn,rm - mn wrn r mnr,rmrm rm. mn mr,rmrn mnn. rn,rm -r w,rn nr m . m rn nn - wrrrm r. v n n m v r nm rrnr mrr z ° °r m nr . m rrn n n. r nn r n, nnnr n mr rm nn w r n v n ,n mnnrn m mxr w mmn n w nnr rv w r n v xrn nrrr mnrrnnn wr,r wnrnmnrn r.nmn nn w r n v rv mxr wxnr . r m,rm rnr,nrmn r- wrn r nmrm . m rn nn ,r-rm wr r. ° ° n r mrr °. m . °,°rn°,n°n ° - wrn r mrr °,° ,° °,° °,° . m °. ° °.rn nn - wrn r mrr - --- °. m°,r r°n n°,n ° - wrn r mrr . m rn nn -°,r ° °. mn wrn mrx nnr.r. mn rn nn - wrn mrx rn.. m v r.n nn - wrnnr nrnr xn. mmx wrnn nn - wrn mrx rm.x m wnnrrnnr nnnn v .- wrn mrx m. m rn n vn. - wrn v rm.r r mrr. nnrnrnnn r n-, wrn mr r n,nr n, rn n,nr . m rn nnnmnn-r.rm r nn -n n, wrn mr - w-n n,n .n rx mrn mrxnr wnn. xnrm -. wrn ww. r mnn mxr. m wrn nrvn mxr - rrrn. xnm.xn . mrx rn wnnrv -rr mxrnrnrn. mxr .mr m mxrrn wxnrnm - w,rrnr m nvrnrm , m ,r . m rrrm . w n nn - wrnmrr rn °.n v n nnrr ° °,r ° -.° m °.rn nn - wrn r mrr m.r mr -°rn°,n -n° °, -- w°rn°, -n°n°rr°, - - --- °° °°°, -° °, -° °, -° °, -°° °, - °, -° , -°,° -°°,° -° °, -° °, -° °, -° ° ° , -° °, -° °,° °,° °, rz.r m. rn nn - wrn nnrn vn.r m. wrrnrn nn - wrn w rrn w, mn mxr wxnr w,w, .r m n w mxr wxnr. n r rn nn - wrn m rrn m. m r mnxrn wnxnr.- wrn mxr .xr m rn. n nn - wrn mxr wxnr mnnnn rrnn - n r , r r.n mr. nnnrnrnnrrn,- wrn mxr wxnr r r rrn,rmnn nr.. z m rn nn - wrn m rrn n. mn. mrxrn nn - wrn nrznn . m r mrx. r n rn nn - wrn nnrn mnn,r.n wrn wr, , mnr, r ,r rr.r mn rrnrrnn - wrn wxnr r rx. m rn n.n - wrn mnn rx. m r mnxrnn . - wrn mnn . m mnnr r. rm r nnnnn - wrn rx . m rn -- rx nmnnr.n wx wnvr rnnnnn - wrn, w mxrnr m wxxr - --- r. n wnvr rnnn , xmwrvnmr rn r,nnr, w nnnnn w r n rr r wnnxmr.n rrnnrxn r,r nnnm rn r rn.n n nn vr rnv, m n, nrr, rn r.rv nn vnn wn rn ..,mn, m nr r w r nmrn rwm,rrrr,.r, wm,rrmrrnrvn n r.n rr r nr n °r mnmrr,n xx -m --r.v , , rnn,nn,r w rnnvrr n,nvrnnm,nnnnmrn,.n rr n r nmrn r r .., r r w ,rr, rv r rr.nvrn n,rnn w n -v,-v n w m rnvrn n m m.rn n rr wnvr nn n r n nr nvrn rn n n r mx ~-. r n nrn nn,r rnr .rm, rrrrn-r nnrm ,rnn rnrn r r nrr n. nmx n-r r n rx nvr mnn r n n, wxr rmnm nn , vr rn n n. -nmr ^- nr mr n wxn r vmrn,nnnn.vnnrrnnvrn w r -nv r-mr- r n,m,nn,m n,mn,n wrrmn. mr nn -nmmr w nnnr-v mr, v..,nnvnrvnn nrnrxnvr - --- nmrrrn.¹².^9-1r¹vrm, nrmn wn,wvrm,r n rn rv n v n- n .r nr w n ,.., nn. n, r-n n- r-m nrn rx n rmzn r nvrrm¹³-n n¹⁴ n - nmrv vwrr m nm- n , r v,nr r n v rnnnnmmrz .¹⁵n nvr nm rnr r v nnrzn n . nrn n- n -v n , nvrn nr. rnrn n n r n nnmn,rnr v mr mn..,mr .m v .., rn , wx,n r rrm mn nrrnn,nrnr r mrm vrn nn r ,¹⁶ nn w n rn rn n r n m rrn n. r nnvmrvn nn n mrr n nr n^®> r n m,nr.¹⁷rmnmn,r nvnr m rn rrm r n wrnxn r r n r ¹⁸-n n rrr r nnn, rn nr 2n r. rn, mzn vrrn mnmr r- m-rr r rnrn.r¹⁹,nrnv rrr -,nmrn- rn m mnr-,nn m w nrn-nrrrv₂,m₂,n, n nr-mr-vm n,nrr nrnrm rn rn r w n r n rn w vnnvrn. r n nn rnr rnn-mrr rm m n v . . mr vr rn nmr ~-nrm rrr rrr rrnn r rw “n” vrz wxn xz nnn m wr m nv .. nrm r r n nvrn -nnvrnmn- rnn v n . nnm. nnnrnn n w nnvrnmn nn nrnnn,n n nnr.m mxnr xm w v ..,rrn nr mmr rn rn nr rnm..¹⁰, w v r mr v n m r - --- r w~ m wnr mn m- n rz r r nn n m r rn ~₂, ℃ v ₂n₂,rr. r n w mn. mr “m” . r,n nn vrr z ~ ℃r wx. wx wrnn n n zrn rrmr,n nrrmnn rrrrn. wx rm r rvnnrr v --wx,rr-r-w nn₂-₂-wx, ,₂x.₂-,- x wr w., w.,n w. . n , ,n , r v.nnrxrmn w mrrrnnr ..rn nmr nrm wx wr r-nrrn n w -,.rmr-m rmr w rrz wxm n n w,,wn mn wx w mnrr rrn~ w. w mrn. n.mrrmr. , rvn nn²⁰n rn ,--wxn-r- mr r nnw r r.n --wx.₂--wx wxx - n m rnn mr 2-wx₂.,n nn mr-r-wrxrwrrnnnrnw²n 1rvr mrr rn wmn- ~ r r n xn-nnn r,rn rn n rr,¹⁴ r^{, 22, 23}. r-r-wx wrnrnw rrzn -rwnrmr n rn . rr, nrr - nrm r r-wx w n . -mrr rmnrmr rv x m r w mnr w rn wnx .n. - nn rrnn> ,²⁴m rrr m nznn w-v n wm nz v rn. r m--wxrnmr--- w vr wx vr mznr nr n , r v₂.nwx . nm nmr_nv ~r _nnn ~ w ,vrrrn_wn mnrv wr rn n-m₂-wrx ~ wr. -n₂-rwx,nv-r-wxr wnr nm_w rrrr--rwzx w n ~r m_n ~ n_w ~ . rr nn rnxrmr mn .n,rr n nnr rnnnrnrnm nrm , nv wxrr. -rn rnnnn¹r r.nnn.,¹³-₂-wxnn--wx,n mwnnrrnmrnr - --- nn,¹³ , - . rn ₂ xz --wxnr nrn n nn wnxr w. nn. vmvnrn-mn r n r ²⁵ ℃^{, 26}. wrn vn₂xzn₄- r r nrnx n, r rn n r rv. w.x,r w m ,wn n -xrvn w rx mvrnr nnr,nr z xz rnnrnr rn n rn m.²n⁷ wnnn r n--wnrw, wn rnnx, rn v n ₂xr--wx.--wxw rn vrn -₂-wx. r , x n¹³--wx -,rrnnnr rnnnrnn r . n, mnn mnrr n mnr r, n,nrx . wr mrrxrn, w w wrnm n r w. x nn ¹³ vr n r n n n n ., . n n w -r-z w w r,rrzn ,wn--rm.rr wrxnnrnnn mnrr vnm, wr nnr .. r . rn .¹ xn rr ww nmr , --.n.,n n n rx n-r. . n wxrmn rrn v,vnnrnr m m mnrx . ~ m r r nnrn, vnvrnn,nr.,rrnr wn --nrmr --wx,n₂r-r-_{2 2 2 2}wx, v r₂ v . wx w wx w., w.,n w., r ..nn ,,x.-,-,n, w mmn n nr n r n w mx rmn n r,mnn n r r n n v w nnvn mr nm rv. rr, wr mm r₂n rm rr.- n -rv wx nmr n wr m m rrnnr n- .. rn n,n,nn wr mnn+ n rn - ,n r rmr r n mnm n. nnrnn nmnn r nrnm -rr-wxrnmrwr w n rm nrmnzn.w..mrrrrnv, - --- rnr,²⁸-r₂-wxwn-r-w mxr wrr-rrrzrn- nr- - . , r n,--wxn -r-wx wrrm n x n. nrn n ₂.,,n . rmr m rmn n w mnr rn,vn rr nn rrm rmn n w-m-- rmn n wr n ,v n .¹³n,m mnrrmnrn m n ¹rn mrrr.mn. m rnr wr xrmnn wnn.-r-wxnn n, ,n r m-nr x-n ., n rn wmr -₂-wx. r rv wx, n -₂-wxn-r-wx w n n ~. ℃rvrrnrr.x-₂-nwxx n w wrn-r-wx, w wnr , .. rn - , x n r wr rr,zn n-rn, .. r n -r- r rn n n--. rnwn nr rr n w rnrn ,n n -rxr rmnrr.-r-xrnn . , n rn r v m r mn m m , n rx r nv rn . n r rnn mxrn wx w.n, w nvrn, nrn , w., n wx n.., wx w wr., ,vnnvr nm ₂ r n-nnn r . m . n . vn r v ,rnnnn r .nr,²⁹nn mn n r .¹⁶n nn r rrn rn mrn vn n m r , n r n nnnnr rn^30,r ³¹nn r. n_"r_" ^^^! n v ^- mn ^^^! ^=v. nr r ^^^! =.m.rmnm,nrm _"# mn ^- n rm.nmvvrmr.nrr xnrmn,n nnrm n ^-n ,n r mvr nnnrn rnr n r nv r ^^_"",% =.mn ^^n = -. m ^^ =. mn ^^ _{&&' "",%&&'} ^_""v_,r_&' =r.._"n_#,%&& mn_' nr ^^n_"",&' =m _"#,%&&' ^=. m.wvr, ^ -.rrm ^^_"#,_,&' =.nmvnv ^^_"r_#, ^_&'- ^= -.n - --- mv. mn rmn mrn rnnn. ^-.³²n wr r n r nr n rn nn ^- nw wrvn rmnrm ^ n mrr .nnr, n xrmnnm- nn mvr.vrrnvnrnnrm ^- nr wn w mrr r w w rr, wr n rm nnrm r ~r –mr ~r ..²v^{0, 33-40}, w rm r r nr> rnr wr rr vr nr rnm n n n r rm n nr . r r w mrr-rn v w rn n,nn,rww x nr . w mr v vrn , r nrmrnr r w zn.n n rnnnnm mvr w , rrnn v,mr-mn mv mrr vm w m rmnv. nn-r- nrrnn nmrrr w-rxn rnr m nrn m .n wxrrx, r ,¹⁹ r r xnn rr nxnv n nn.rmrn, r n rrnn r n r w r-n- mxr, rmvn n v r- m wnr-mmrv . r n w r mn vr rn m ⁴¹.^-43 nn r n -v -mr-vm rnnr w . nrr r n n nrm nzr, r n - nm. mn n w nr rn r x >.nr rwnzn ,,.m, wnrr,.,rmn-xm-nr w,.r r rmmr ₆₆ rr,n.₇n_{8 810} 4^{4, 4} rv.nrn wnr xm w-rnnzrz rwrn mnr rrn rrr.z⁵.r n w n n - ---nrmnn r mrnm mr n wrrrmn w - mnn, n nm xnzmn.. wrm.nwn.mrm n r n : rnrmr wr nrnrm. ° rmv m mn^-1 nnnw m nw . mn m m mnn^{-1 -1} mnvnm , : mmnvnnn mm. m °n mnnvnm ° mn^-1 ° mnvvnnnnmm. m ° w rmrv-m rrmrn rm-n.n wrrrrmn n . rn w rrm n m m r w nn. rnrnmr n m rn nrrnvnvrn nrmr mrnr r wn ˚. znn -¹r vnr w r wxrrm n n. rrzn --wx nm r n r n ₂ wrn n r -xn wr vn r znnz.n r n-rv wx,xz wx,n rn r m n rrnn rwn. rn xrmn w rn rn nmn r vn, w rxrnrmrmn,rrnvn rmr z rrrnrmnrr r w,rnrmz rnmnrmmn . rnmr - m r ^–1 rrn r n m^-1 m n rn – m w n ® w rxn. rmrnr w..rmn n rmmnmr ^TM - --- mrmn r wrrrm wnrnrrmrmnnw- m rmr nrmn. r °n n mm mnm m n mmrn:z. mz rrnr m nzn m r - w rrmn n mnvnr- w,rmm- wn mr- nvnmrr °. z. w r w mnn mn mmmrmnm wr vn : wr: nr nnn mmnm rm n vn : rn: nr nnn m w m, mxn wnr rnn:nn:..mrm wrr.rn xn,nn wn nznwn n m n nn vn m. wr r r m n m rn - mzn nm ..nz rnr n nznr w rn n v .nn w nrrm . zn w:.mn, n w:.mn,n r °, vnmrr : °,rn r:mrr: : ° w :.mn, mrr: °, n . rr n w nn₂₂ mxr r w,n r nn₂nr ..mrr r. r ~ m w m- n rz r r r r r r w w rz n w rn rr-rn. nx m wn rn,r wm. n w w rn m n r mn w mxr n wrn n ., . r r rv n nrr ₂ .mn , nn n wr wr vn n wr rr w mnrr n: n r rn r v. r n w vr-rrzn rrz r r, r ~ ℃ rr ~r m wn ., w.~₂n ℃r mwn, wnr nrrnnmrrnr mm r mrn r rr “m”., . “m” rn nrnnmr..rmn. r rm m w rnrmmnrx m mnr.r n rwrz w, . r wr w r r m w , . n,n r n w ,rn, rnr rnrrr w wn nwn wr r nmr rmmrmr.rr. - --- n n n. m mnnnn rw w...x .n xrmn, m wx r rn w r w r wx m wrrnrr nr r. nnwr w n r r r ~ m. .mrr w ℃,n r nr r .. wxn rx n, xzr wr n nn. n nrrn,, ~n m.n nm mnxr wn rnrxr mnnrnrr rmn . n ~nnnr , w r r, n n. wr nr nn wrr w wrn v r ~. m rr n n . w rn wm nvr . wr xrrmrnz mn . m r.mw n r n nr w r. n.rrmrrrnm rr wz rnrr w rnr nrnn rmrn... mrr r r m w ~ ℃ r,. wxnn n.rz wx w w mr r nnn n. n r w w n r r wrxnn r rn , r r,n n r .rwr, m xn w n r w r rxn. rxnxn, wx rn r rrx wn. wr rxn,. wxxnn wrn wrr rnr n m,w vn rmv n rr rr r-w xn₀n rr vrr ℃, mr.n r rr v mn wrnrmw w vxmr₁-zm₀.vrn. n m m1 w rrmm.rr. nvrzrn. rr rr w rnn, rmnr w rn₂ - n -n.. nn rrr wr wmrm mn n,rrnrrzrnn n v. w:rn-,rv wxm, n mnn wr,mnrnnm-nrn - --- vn,-rv wxnvnmwxmrn n rvmmrr.nr r rrzn r wx n.r - rrnn xn, wxv wrmrvr.n xn r mm.vn --wxn xn w nnnrn wr r . v. ₂ w,n rr ℃n rmn nmrnvr _nn w vr m r w _w wx wr ^^{^} _* ^{= ^} _^^ ^{^}n +^{+ =} _* ^*, _^ ^{^} _^^ ^{^} _{^ ^} ^{^} _^ ^{^} _^^ ⁺ ₊ ^{=* *, ^^ ^ ^^^++} wr ^^₊n ^^₊ -.m nnrnn.n rn rr ² ^_{^* =} ^{^} _^^ ^{^+} ₌ ^{, ^^ ×} _{* ^} ^{^} _^ ^{^} ₊ * ⁺ _× ^{× ^^ ^^+} wrm ^^₊ nnn rn rrn nrmr.-.. n.zxn n v n -.n . wxrxrn wn mnr n rnnx ^^ ^^ r n - , wxr wrv n r x n vr,nxnnnn wx ~ mnnr w.. rw. rnnx w mn wrn nr mmrrn . . ^^ ^ ^/0 nn_./0 m¹.nrn ^ = wr r - --- rmn. n m rn m. nmnr nrn -rv wr mrnr, :, n w z v -.nr n -, wrx n nn nzn r v wr m n , m rvn n. ^_^ ^{^^'02} nn r r m . r nm r _{^^ =^ ^^34 ×} m r w mrx rmnmrvr nnnrrmnrw nn r n r n, r rnr mrzn,n nmrnnr mnmn.rnnn r rnr , - n r n rmr rmr - nrv nnrrmnn.rrnr,n rmnmnn . vn r n. nrmn . ^- nn m n vr mrr w ^{4, 5}n m rnrrmnnrr nn n .nrmn v n_{1 9} nm n . r rmn v m , n ^{mr x} _{1 9} n r m n m^r’^rw. rm w n n v vr ^^r ^ _{= ^^} ⁿ _^^ wr ^^ _{" + ^^ ^^ + ^^} n ^{nnr v} wr _{^^ × ^^, + ^^ + ^^ × ^^, + ^^5} n nn mⁿr nmr r nn. n _{^^ ×} ⁿ _^^, ^{n n} ₊ ^{r r} _{^^ × ^} ^{v v} _{^ + ^^ × ^^6 + ^} ^r _{^ + ^^ × ^^, + ^^ × ^^ + ^^ × ^^6 + ^^ ^^ × ^} ^{n rv rm r ^- n} n nnr v _{^, +}n _{^^ + ^}r_^&v _{+ ^^7}rm r ^- n - --- n ^nnr ^^ ^v × ^^_, + ^^ × ^^ + ^^ × ^^₆ + ^^ + ^^₈ + ^^_{7 ^^ − ×} ^{mr r rvrm r ^- n n nnr v m} _{^^, +} ^{r r} _{^^ + ^^% ^^ − × ^^, + ^^ − × ^^ + ^^ − ×} ^r _^^ ^v _{6 +} ^r _^^ ^m _{+ ^^} ^{r ^- n} r rmnmrmr ₅ . wrmmrzn . n- r w n r vv m.⁶ ^-nnnr - m r n. rn ,, nrrn rrnnnn r nrn r n, m r n_{1 2}n₃rmnr r xrnnmrr n vnnrmrn r v .nnr mn.r- m nr _a wr n n . rmr wrnr mnr n r nr n, n n v vnnr. w mrr rn – , nnr v r v v rr-x_Eamrn m m,n nn .⁶mrvnn nn r _lgA mrn. . nv n _e wnmr mn n r-xnn r. . v.nrnnnrn r rnzn66n r-xrnn m₈₁₀n. r m nzn₆r₆n-xn₈₁₀ wr mr nnxrn rr vn₆₆r₈₁₀, ~ mnnxrn rn v₃n wr r mr nnn n.r n ₃ wr nmm, mxrrr wzr w n.wrnnnrrnr₆ mxnn. mxnr r vn wr . mn. m, r v₆.₈₁₀ nnr.n nr n r rr n wnx n w . nnxrn rrn m . r rnz r rmn r vn wr z x n₆₆n-xn₈₁₀n nr n r vrnn r wrrn. m r nn v wr w n wrm ℃rrm mrnn v.mm rrz w vn n vr n. mxr wr nnrnm wr rmn n . zn. nr' m ^{^^ =91:!;<=*> × ^^ ^^ 2 × ^} - --- ^^{^ ?@=*1 ^ wr ^^ n} _{./. ^^91:!;<=*> .2} ^× _{^^=*=12 × ^^ ^^91:!;<=} ^./. _{mr m ^^} ⁶⁶ _r ⁿ _*> ^-xn _n ⁸ _v ¹⁰ _{r r ^^ n} ^@= _m ^{*12 66 810} n _{66 810=*=12 r r , r} mn, r v ^^ m -nxr n. -rv wx r r rn x. nnrn nr n nnrnn--wxr rm ~ mm ~.n mmvrnr-rx.n,nn mmm zrr,r .n.n-r-wxnrwnmr r nrm ~ mm ~. nrn nrn rvr ~ mm r rmn m n. n nnnrnr m r w r n: nnrnzrnn.xm mvnrmrnnn n wx n-r x n rn⁷- rx,⁸r r n r n,^{7, 9} nnnnmrrznn mrr w rmn n, rmrnrm v nrmn~ r n v . m r w nrmn -- nrmrmn, n ~ w rr _n ~ n_w ~ n-r- _n ~ nrn nmnvr<n> n - .n rrnr rnn , mrz r n xnm mnnn n n r n m mnr.rr, nnxz wnrrmx ,n rrxn-n nmnnrr-.-wxn,n wx, n nnnrn~ mm, -r- .rr, n wrn rmrn rmn . nrmrn vr nx n,n r x n w .rnrrrnrrxrn.n r. - --- c nn n ^{a b}rrn wrx ^c rnzrn, n,n xn. ,r w v. , r r nrm , ,n ^{d e}r r wv.nrm ,nvrrm v. ^fr n n wr nrm mm mr, vr r rn n.- w nrm ^gvrnrmm , w,r , ,nnzr. .rm rnmrrrnnnr,nrvnrxrmn ^v .. x x x x vv^{a b} 2 - --- - - r - - - - - ₂ ^{a b}xxn v wm r w nr ₂ nrw r. .vr m rn w w - wnx m-rvr wxnnnn .n. - --- 2 ^c wr r.nn n nnr nrmnn. xmr . v x w ^bx. nmnr w. n ℃ wnrw r ~ m,vn w . =nnrnn wx,xz wx,n . x = - --- a ₂ . ⁰ ₁ ^. p _n - --- ^{b c} ‘-’n ‘-’ wr xz wxn nrm wxx n. ^d- w m r x n. ^e- m w mnnrnr xn wnr. rmn n . .nnr nrmn v m -r , ,n . rnxnrrrnmrmnr-r nn,,n mr r 298 K.⁵ . ^^ /mol K rou lael _{^^, ^^ ^^ ^^} ∆ ^^ ^{^^} ∆ ^^ ^{^^} 600 800 K . ^ - --- 2 -. -. ^armnrnm ’w. ^^ _{^^, ^^ ^^ ^^} w .rmnm. rmr ^- nn n rnmrr. ^{^^ ^^ . . . . . .} ^_^ ^{^ ^} ^_^ ^{^^ ^^ ^^} ^_{^ ^^ ^^ ^^ ^^} ^. . _. ^. -_. ^. . _-. ^. -_. rnmr.rr v v r ^- n r nnn rmr v - --- b _{a a} . x - m . rr, nnmnmmrvn v w n,n mnmn m m n.rrn, r r w nrn rm r ’ mr m n n rr m r n ’.., wr mr m r n n,n n r n m °rr. wn r , rm n rn -, w w r nr w rrnnn mxr r wnr r v. , rm ,n r wx.n n nnrn n -nr nn nrzn w, mn r r nr n ,w vrvn rmmrr.mrx, r, nrrn wn-rxrmnmnn mn..,rnnrnnnr nrrn n w rrm. v- rrmnr,¹¹nrr-rnx mr,n¹².nr znn-, rr.,⁷nv m - --- z ¹m 4rnvr r rrnrm ° wn..⁷nr n z m rn wr n .xnr nvrv nrvnn,nnn m r,mn rrnn.¹³n- rm r n.¹⁵rm rn n n rnn -rz- r nmn rrnnn nvr vwrnrnrrnnrnrnrm . wxn₂ n vr rrn. , wrn ,r rnrr r, r nn --wx nmr rn .¹¹ wnwrr n r xnv mr nrrrn, rn-m nnr rn rr v rrn, m r m r ₂m₂.¹⁶n nwrrn n₂ n m₂r nrrwr rnrmrr .nr, v m rn mx , v rr,nmm n r nm n .rr, mn n-r r r --wx rn nrm r nnn-.nrnnm r,wrnnrrxnnnmrnrr.¹mrn, zrnnr m 1n rrnmnrn,,nnrm r-rrvnrnr.⁷ , rnnn n.^8-21 mnnrr, r v rn r rrn nv n, n rrr. m n rrrmnrvnn mrr-rnrm rrm wx,w x n nr .²² rm r mr m nvr,rn nm m n mrrrn, n v n.mn wr n nr wx .rrmr, n v w nr rrn rv w mr v,n nrm n-r r , w nrzn.nr n rnr r rmn w rm r r nmnr m mrrrnnnr mrr-rnrm vr , vn,nr rr. rn-rvnrrrrmw- w - --- nnrrnrmn rn rnn.nnmrrrrn-rnnrmnn, rn nr n r r m , wrm mrr n r r n rnr .n n rnn n mrn n,n w nn r mr m, nrnnnn r . nr r n z nnm nnnnxnnnnn r n, n’rv rr,²²nn nnn zn.n nrn rm nrm wrr nn r r r rn xrn mrr n..nnr r . rvn rn r nr n , wr rmr m rn nmr n nr rm rn. =-rv °nn =, ° w_w,n. rm-m wrrr w rm nn . r n r nr w. wxn nrnn r r . r nnr rrn .,. rmrn znnn xn rv nm r nnr ~. mn m wxn rv.nnr,wn wrr r r ,vn . r zn . r. r n rn,mrr ~ °n w. n r r . , r °r.nn, wr rn r nnn, mnn wr nm,vn r r- nr . r rv.rrrrzn rm r-n rv r rrrnnrrn wrn n,n wn m nnrnnrnm rnrnnrm.r nr r rmrnnmnrr- r rnn.nnn.r²m³ , r, wx w w. m n wx = ° rv mrm n, xnr = ° mnn.n n n wx, rm rrn nn n r nn mnrn,--n,nnn ~ w. r w n vrz rrn w..wrm, -° m,rn rx- nmnn.n v . , r r --wx v n r mr n nv nrvrnn r nr r nm =- °.nnr, -° r n n mn nn r n rrn “rx w”. n, - --- v mnrrzr r mr wrr ~n °nn °mnnr w r.vrwnxmn rrr rvnn rrn-rvnn. n rwnrmrvzn rrn rv mn - vwr-nn . m. -rm = ° mnr n wx. m -nn nn. mnrn nmr vwrrmn nn . m nxrnnvn . r nn n rm rmn nrm- n, w rn r n- , w w nmrvr mrn. nr r vr mr w m ~ m nn x . n . , n - rrn rm n m rn rrn,nn n rn n v n.n nrr, rm = ° r nwr- r r - nvn rv rr r nm rr m . nrvnrzn mx n.m wr ,n wx w r mrnnr wnr =m °nrw rn nrn °,rm mr mnr w ., m, . rv ²⁴ mr mrr ., m “ r °mrrmr nnr . m ,-m-- nn rn .”, ̶mrrr wmnnv₉rn w rrrnrv, r .²⁵r^-26 rn w.rr n,rr . wrmr m mn,nn-- rnnn,n-m--nn . rn w n r nn n -.n n, n wx w rm r rr rrn . nrm nrrwrr r nn , m r mr m.n. n, n- r v vr r nn ~ vn,wnnvr mr m ~ mr wx mrrmrnrn r .. r, r r vrn mr rmn, xnnnnn nn nrm . n wxr nr rn ^^_./. - w n r. mm r- nn = °. mm r--° v. rmnm wx-°r,n-nr. r nrrm ^^_./.nw-nnn m mrmn - --- vrnnnrrnn.²⁷nrrr,, vnr nnrnrv r mrvn r .nrn, m nn- m n ¹ mr m rm rn nrn n n. wrm -n. w nnn rmnn -n, m ,..rrmr,- n m-- n ,, nn nrmrmrrn ,- nrn w -rv-m, mn-r-nr,,nn,n,-,rm,--nnn .. n rm ,n nmnrm -rm xn, wr n m .n , nn n mrr r m rmnn . . r rm nvrrn-wr mxr wn v-mxr mxr, mnnmrrrm. rm n vrrnrmn . mxrrnrn w m n.²⁸ mxr r wrm r mr n n m w. mmr r,. m , w. mnnnr,wrm nn. wnx w. w rrnr wx = °, wr r nnn . w nnr r nnn r . r. nr = = ° °rn wr. ~ mr n w mr n,nnrnn--nn w. r .. n n mrrm ,r w wn mnvr n r r n w mr m r r n m nnrn mrr rvnn znr .. rvnrr r n- w . n~ mr mxr-rv wxn ~ mr .n nrrnnr w mnnr rr n rm . nnn,n,n nrm rm mnn, m-rmnnmn rmn n wr -,nnn w nr .,r ,,,,,n.rvr, rnrm xnn m..mn m rnn , ,,-n rn. nr x,r w x nrr vr-n mxxn vrrmn n .n rn, rmn rm .r. rmnnrn,nnrn = °rnvwr.--nnnw wx¹rm- - --- nrn r rnn r n n r n-r nrn. n-n,n-r rnn rrnrnnrr.nnnzrnr , ,n rnr vnr mnn mr vrn , nr n w vrzn, n rm wrn .. r n r r, n wr r w nn vr n rnnw . . rn wr n nrz wr r rmr rn nr n rn .. n_{2 4} - nvr x-n, n.rmnn ¹ vn. rn n .-. m r rvnv . w nw rnn .n. m— rnn wn.nnn.-nrvnv ¹-¹r³ , r v—.wr.nrrrr - rnn,rr, mnrnr mn rnn.n mnmn . wwrvrn,n nr n rnnn mn nrrnrmrnnn rn nrrrn r .n mrznrr,²⁹rnrm -n -n rrnn r n r n v wvr, nr nrn nr . m n r,. rm wr n n .vnn mx rr r rm nrzn w n r ~ rr,rrrrn wr rnrr wrnv n vr nrm zn. w n rn rmn w w r nnrnn n . r. rmn w r r rn , n mr n n r r wnrnrn rnnrm . n r r. r ,n -rn, wrnn rn rrmr wnnrn r.nn.nrrn-,-. ...rn w rr w mr mxn nrr nnmrvr w r vr nrnwn rn’ mn- nn-, mrmnr-n,n-rm. rrv mnnrnn mx rnrmrnnx wr.³⁰ -n-vrn,,nnrrrnm n , wnnrrrn -. - --- , w.v.vr , w w mnn w w n m n-n.. r-mrvmrnr.-rnrnx x wnnmnmvrrvn r . , w.nnr,-nnn rn n nr rmn m r³.,^{nd rd}w,rm mn xrr rn n.¹n , w-m r -rnn rrmnrrmnr mxn.³²rrnrmrr,nnnxvnr wn nv mn wrnrn n, vm ..,r n rnrr rmn m n w-rv rn,³ rnmr. mrn, wrrrmn wrwn-nw rr mrxr w rr m. w.r³rnm n . n -n-rn w nnrn. m mxr . m nm n , r v.mr , -rmnr m r r m nrrmn mr r -rn, rn nr rnnrnnr mx n w n n m r. rn, xnmnn. m mx w w xn, w rrrrr r r rnrrnr n’ . w vrw. nrnnrrnnnnxm wr, nrr nmrnnnr m.-rn r n rn n wnr, r n. mm r m rnn n r-wr m,..-rn rn_CMC =. mm, = nnrwn mznrrn mnnmrnn_Cn =.w mm,rn =nnr mn,n. r,n, n n rr n r_MCn r n.³⁴ m nn n. m wm.r n mxrrrr v n _C,_MCr -rn . , rnr -rn. x rnnnrvr =m mx w nnn w. rn . , w CMC. rv w mnr w r- mnmr r’ r “mrm³⁵r".mr mxr-rvrnr,n mrmv w > n wnnrn. r,rn r rrrrmnvn - --- rrnr vm-rnwnrrzm r r wn.n znn n v r r rr n .,rn. rnn -r rrn vnn rrnr ^36-37n mn, nrrm rn nnrmxrnnnrmrn-vnrrn . nr rrrnnnmnrm v vn- m.^38-39rvr, rv m rm rm ⁴⁰nrn w v r, w n rr zmrr wr °. nn mrv rm nrnn rrnr wn n m vm . n rn.⁴¹ nrwrn, n rm n rm n,n n n rvn rnrmn mn ~ m n.⁴² r-r wwxnr nn -rv n xvn n r n. , - w nn wr nvr rmr r rrn, ,.v ₃ mxr . rrmnr r n n n rn,rn nnrr-rr-nn. r nvv mr x ,nn-r rrvnn m n nrnvrnmnr rmn r n nrn nrm.mn m m nr, zwnn w rrrn vr rr nr rn n . m rnm nrz n.., wr v. m n mrrrnn nrmn v vr mr m nrm rrnrn nr n rm n wx. rr vrz wr , n v-r wm rr w rnn nrn n-vrnr.mrm, w, wxnrn vn rrnm. r . r nzn ,.,mr rr,n., r m-rr, wrnr,xn₆₆ n. w rmr,r n.mrxmr, - --- wm,nnnr,n nr wr n n r,.n r nr.r,mrvrzn. mmr^®r wr w rr ✕ r wrvrznwrn mn vrzrr mn mn,nrmnrrm . --n r. mn w rr n r rmr w wnnn wrn m x:. mm x.mn mnzn r . ° rmrr, ° mmnw r, mmnn nrmrr, mnmrr, ° n mnmrr, ° rm r, °mnn n-mn.n,-. .nrn w wrrrrnm n rm m n .m. wn rnnnn w- mn m, m.., wn nrm.: ° r r n : rv nnw::w: mmn n n mmn mnvnm: mmnnnm:m.: m °n mnnvvnm : °mn .nrnnrmn:m. ° . : : ° n-.n-: - m °r w rrm n - mrr rrn w r . mmmrn °r wx w m w r . mmnn w ,,-rrnzn n,, r wn rrvnx r. m rrm n mn n- wnrr.r, xmr rrn wmn - --- mmn . mm.,.n x. xm. ,- x . mm.. xm . mm.. x -.- m m wr vn v nmnnrn ~. mmnrr r mn. n w r r .mrn rnn v. m wn nn wr . x mmmnn mrn: m x , m x , m x n n , r, rmrr w.nrr mn m. mnn- r mrnrrrn nmm,-rn r-r, n - nm,n nm ¹³rmxr.rr w¹ n nx. .rmnr w wrrr rrmr nnr nzzrnrnvnrrm. rmrrmnn wrn n¹³ zrrvn rn wrr rrmxn n n. xrmnr n n zrnrvn rxnrn n.- wr n,n znnrmn . mr w rxnm , rmmw .n nnr nn mrmn wrn rrmnrrnr mn wnr vmwn ~m,r.rn r nx,nrmn r wr ~.r nn mrmn wrv nnnr nm ~ ,rr r m w r vm rm ,n rnm ~. n ,.r m- nvrzrz r rrnzr,. w mm nrrnr z,. mm wr rn, mrr w w rm r, °r mn.r m r r w ~ °,n °mn rnmrr rn rmmrr wrr r m w ~ °. mm, znmr wr wrr n r rr .r mn, r n rr.z ~ °n ~ °, r v. rm r n w rnnmnn, nrm. wnx w n xnw m ,rnr v, wxr rm r r w -n - n w rmn .rn rn, m w w n °,nrr m mn-nrr-m vr w wr rrr.w w wrrn.nr mn, v - --- n. mnnr wrnrrr rnm.mrrr mnn nrz w n nnvr nmn rn n wr m wr. m,✕. mn xn w wn r n w m xn w r n mnmxr wrrrnvr-24,rnrznrn.n rr v,n xnn r rn n, mr vm m mv r rn v °. m w mnr x nnrnnr mr z rrnv¹r nnn n rmn r r wvr nx .n nnm n² m, vnr n rnrrrrmrm . n n, m nvrnmnn m v n w rnn rnnnmrn.n nr vmr nrnm rnnrrnnrn.³m^-4n r, rrnvrrn rnrrrnnrrn r.nnw r rr n rw mr nr nr rm n rr nr,rnv rnv rnn nr .wvr, n mrv n n r r , nw r rnn w v nnxnvn r r nn .rnz r-wr w nr n rrm.rr. w nnrr nrrvn.nnvr,nnr nn_w rnnn .mrn, n’mrr nrn r v r n wr mrr wn °n °n r wxr . rmnn r,mnn n rrxn v m r r znr n , nv w n .rr,n rrm r rn nrvr r r nnr n r xr nnrn nr n mr mn. wx wv ¹ 6m₆nn nnnnwnmn r . r nn₆₆ : nrn nr, nnnr₆₆n ^^_./. w,,rmn. nn _{^^ =} ^{^} _^ ^{^} _^ ^{^^} _^ ^{^} _^ ^{^} _^^ - --- w mrrn ^^_:!; ^ r_<=*> ^_M=Nr =nz m ^^nn rvn ^ nrn^z_:!; nn_<=*> r ^^_M=N12 mr nv n m rm6r6 ^^r₆₆n ^^^n m nmvrn rnnn₁₂nr ^^₌ =rrmn n n ^^ m_=*=12 m.n mr,n wrmx.rmnz_*=12 x rnrnnnrn nr nn xn n n ^^_./. r vrn n nrr mrnr w rm nn. n nr wn,n v znrz =r °rn wrxn mrm nnnn m r r r nn =.-.°.vn , m nn.rn m r r = - ° wr nv r r nn.mnnnr mm wrrn.nnz. r w nv w nnr m n2n4 r rr24 n. rn rn wr nrz n rm rn. n, rnmnrnn w wnxn.- nrmnnnxrnrmxr wn rrn wn ~ rn .-. r m r rm nrv ₇rn₂₆ , nr rn .rrn v w n rnnrmn. m r r nrmrv rrn wr^a. ,r rrn m_{2 2 2}nn rn n m r °.,r, _11-24 ¹r⁶n 2-₇₂ -_{3 2}n₃ °,- _6-36 ¹⁵ rrrmn ₂- °r,, _5-21 ¹¹ , rmnrrmr- n zn °:,- _7-26 wr - --- znr- ^arn nmr r °,m v w¹.nnrnnrrn nnrnnnr mrm.r . nnrn wr nn- .nr m- wrrrzznrmrmn mrr m .nrm w . wr.rrrm m nr-rz.n m n r nxrmn. nmr nw. rn mwrnrnnr, rrmrn rrnn nmrnrr - --- rn rrnrnn nr mr wn nmr rrn. rn mmm rnnw rnrrmn.rxmr, n. rnrnr nmrn "^1-2." rr m nr mnrnnnnnn wn w nrnr n r n nrrnnrr rrn n . n nnv n nrr rvr nr n wr rrn xr m m n n. nrrn nn nxn nxr r mr r n nn nxr nnn nnrm nn n.nnn n n rnn nn n n xr r rnn mnn m.rrmr,nnrrn r rrnnnnnrmn xnr nn wnn nnnn nnmrnrn nrnrnnxn nn r mn nr nnmnmnn n nm. rnr rr nrnr n n n vr rr r.rr, nrv n n n m n rnrm xnnn nrm. nr,v.m,..w,..,r n,,n vr m. n,n , , . rn .m.rnrr,..rnr,.. m,..,n rnnrn w,.vr w nmn. , ,-. r ,. r,., r n: n n rn. . n n : n , , - nn,v.rn,. wn,.r,n.,., nrmnn.rnnvrn nnn mnvw mnm ,..nr,, . rvr- vn,m.rz.n,..,.mn r, rm,-.rm - --- v rn,..n. ,..,r m,.. n,..,wr mr n-n nn,.r,.r..nn,, ,-. ..r . r,.v,.. n,.. r, r n,.,r vn n r rn n nmm mr n.,n,., . n, n-,r.. rn,.,r.m :mm, ,nn- m n,. nmm,.,.r ,.nn, . .. z-nz,.. r,.. nn,...,...,.,n,.m rrr, rn m v v - z n .rn m r x nnr ,.n,.nr,n.,m. , , -. r n nnz,..r,.. ,.,., n mn nn ,rn w, -v. m.r n mmrnn,.rmn,x.-.n,.vr,r. n,r.n, n.r, x.nr nn ,.,.,, n,rm, -. .r mr.r rn.:wr, .. r n n rr,. n,. n,., nn v , , . n n wxnr m nn.n vn . -mr,n.,..n,,..., r,n..n,n. ,.. n,.. r, rn rmzn.n , ,n-n rm nm n,..nn,. ,..n,.-,. v,. ,. ,. , ..,. mr,.. n w n rm ..rw,.., nrn w r ,. ,r.rnrm.nn , , -. nnnn rmr n,.,w r rrn n nr rmnm mxr nr w -rrm- mr mn.vrnrrn rn , ,-. rvw.rn nnv,rn.mn,.,mrnnrrnn,w,n-. n : - --- .rm,..,r, x,-n -n n.rn m nr,.n,. r . wn,..rr,..n,. nw,,...., r,r. r,.. rr,. rn-mnnrmn n-rnn v n , , v nw r n r rn.m r--v. mrrnrz,.r. n,.m.nrmrn-rvr,.. nnr,.., n mrnm.,n.rrv,n.n,rnrmmrr nr ,r n,n- .m r wxnnn..rr n rr nrn xnnn w..rn mr nnw-n n -m,.. ,.,x vrr n , , - . .nr nnrn mr r m, r, rnn ,.nn,.. r,..rrnn -.. n,..mm, ,.nnn,. n, mr,.. w,....rr,n,.,. rnr,n.-.r,. ,.. r . nr n nn - rrv,. v , , -. m ,.v,.,rrzn nr wxr - ,m.nr.rn rmr , ,-.n r rmnr, , mr r,., .x n rm .nr nnrn r,,.,-,. nrm .. rn,., x n rrn.. nn.rn.rrx n r m n.r n vn,..mrnrn,. n , ,-..rnnr,..r,. ,...mnrz,,... n,.. r,.. ,... nr,.. ,.r,. wr,..,..,n.r.m,m.n.nv,. ,.. m,..,x w vrz - v,x nn nnn.n , ,-n.r nmm - --- n.zrn,. r,.r,. ,.nz,.,-rnrr nnn,.. r,.. , ,-. rmnmrr , v r mn rrr. r n,..r.w rn m , ,-. m n,..,rrnrr r v .n rn- ,,.n.rm,n.r.,..r,n..,r.,. r r,. nnnr r nn rn,..,r-x - n r n: mn vnnr n r n rnr,r..m nrnnn,.mrnnn, .,.,- rnw. nr,.,n n rm ,-. n r , nrn,. rrn,..vrr,.,v nr rn r n . r.rn n n r , ,- ,. n,. r,.. r,.., mrnn , -nr :r r n m.m m , n. r ,r..n..mn,r.. n,..., mr r n—r:rm mrm,....rm,n.nrmn,.,,r,-.r n:. rn n,mnn r n r n.rn n n nn,,.-. r rn,..rnrn,r.,x, rm r nr r,. zr,. z,.rx ,-. m nn nn r - ,. ,.,r n r.nr nnrn mr rn nn n ,.wr,., rzn , , - . r,nrvnn n ,, n w wr . vn,,...xvnznrnx nrr- rn..rn. ,,.. - --- n,,....r,n.n,,...,xrnr . , . ., . r ,... ,. n,. n, nn.nvnxn r rm rnn n r ,.r rn-nr,.,n.,. rr,.. n,.n,., n rn nr.nmn nr m n nn x r r , , - .nn,..r,.. .nvn m,xmrnnz mxnr.nr rnmrrrm,n, - nzrnnn,.r r.n,.r.rm ,..,r n rmr m -. m m rrr.n mr , ,.nz,.n,n.,n.m,,...,nm,.rnnn,m. ,r.rmrnz,m.nnzm, n nzn rmrr n r r rr n m , , - n.n nn,.. ,.. rmnmr ., v r mn rrr. n,..rwr. rn m , ,-. mr ,nn,r.m,.,..rrr,n..r,r. r v .n nr r,.. nnrn,..n r,. r r,.rn,..,rn- xnn - n r n: mn vnnr nr- n,.,r.m m , ,-. r,.. ,n.,mrzmnr.znnrn mmnrz.n, -. rx-n mrzn . rvrnn mrnm , ,-.,n rx.rn nnrrn,..mr,.,.,r,m-m.rzn r rn .nr - --- r n rn,.rnn,.rnn,. wr,.,n n rm ,- r nn n.rn n n r ,rnnnr.,r.mwr ,n.nrn,-.mr,., nmrn-n , - n n.rm , r n,. r..n..mn,r..rn,n.n.., mr, r,n—-r:rm mrm,....m,.rmn . .r , ,- ,.,r r n..n. mrr-vrz,... ,.. rmn-vr,.. nnr,.., n nr.nnrrnnmn rr r ,. n,. nrn mr r , , - . nr r,.. r,.., mrnn , - :r r n m.m m , nr. n,. rrn,r...rnvrr,n.,vnnr rrn ,r n . ,- nn,.r rn,..rnrn,r.,x, ,rm- r nr r,. zr,. z,.rx,. . m nn nn r -n n,n.,r n r.nr nnrn mr r , , -n r,n,r.vwnrn,., rzn n w .wr . x n ,,-. .n,.,..m.m,nn.,.n,...rr,r.,.rrrnn,,..nnn,.n,... w,. rr, . ,.. mr,. . ,.vrnn,nr n ,, -. . r,.vn,..nnr,,nmnr,m.,r.zn ,,-. - --- ,.-,. nr,.n,. ,.. n,mmn nr nvrnmn n..mn. nr,r,n,.n,...n ,..r,nr nvrnn .. nrn,,...wm,,- .rrn. nn,.mnrn ,, -. r ..r,nn,, ,.zr,rn n n .z .-m.r,.-. n,.rn .n,.rm, ,nnr,., . - .rmnn,.mnn,nr ,, ,,.-,. mr,. ,. ,.rnz,.r,nr mmn.n,.. ,... r ,.,.-.,. n, r ...,., ,n.,, ..rr. ,.r.r,.nw,n,...rnm,n,.n.vr,n.,, ... m, n mr nnrn mn- v, .m,..nn,.,.. ,,-. :nvrnmn .r,.. ,.. , ..,.,n,,.r.rr,. n,. n, n vn ,,.. . .r,n.nnn,,...,w.n.,.rn,.n,.,.. n,..mm, w, . ,. rr,. r,.n,.. rn..rr,,.rnr, ,,-. m . v,.nw,..m,nn nr .. n,..:..,n.,rn,r., ,n,nvr, ,. -. n ,, nmnn m .nnm,-.. .,.,.n,,r n rn ,, -. ,.,.,.n,.,.r..n,.n,,.,,-... n r,.,. - --- r .v.,...rn,,.....mn,,...nv,..z,..r,.... rn vr,..n,..r, rn ,...,n m.r.,.n, ,nz, n,-..n,,.,n-,. ,.nr,..rrr,. :n.vrn w,.rrn,n. ,nn . r , r,n.n-r w .m,..n,.n,. ,.r . rn rnn ,.,.m,nrnn ,,. ,r.m,r,,m-.nnrnnr n:r nn n ..-. - ,.r ,.x,rn n n r ,, ..,r,..wr,nr,.r,wn,r.vnn n ,,-. r,rn r n nmnrr,,.r,nzn-r,..mrr,..wr,..r ,.,..mn n,..m,.mz,.n,. n, .. nn,..n,n ,., . . ,. r,.rn,m m ,,- .,n,,.,.n, nr : m nnnrn ..,,..,.,.. n,,..nn,nmr ,, - . . ,.n,rn r ,,-.r .,m,rn....nmr,..,nmr,.. ,..,..rm, ..rrn,..rnn,..rrrnnn,nrn,,n-. ,, mr r .-. ,,rm,-..,. rnn,nr nnrn mr - --- m ,.,n-,... r,.n,.nz,.. rm,..rw, ...nm,n.,vrn,.rr, vw ,,-. . n nr r n n ,,- ,,..nw,.nr,.. m,rn n n r .-..r:nvnr,nm.n.rm,v,-..,nr ,.. vv,..r, .. r,..rrn, -. .:.rv,.nn,.n nmr m nnrn,. x z,vr, ,.-. ... ,r.,n rn r, . m .n mr,.n,.n,.n,..n,nnn ..mn, r n nrn r .:..mr,.nnn, . m.m,r., mrrn,,..,m.m-. . ,. n,n r,., . mr xmmr,zrrn mmnn,vn-. rrrnr rrnnrnnrr rn rr. wn vrnrnn mnnr mm m v-r r. m nn vr rnrn r.n nrnn n rn wn w r nrn rnnnnxm wnnrm.xmrn,

Claims

- --- .m: mnrmrnr wxnrr rmn-rvr mrn: n,n m m r nn r n, nnrrv nmn mrx,n v n mmn n w nnrr nrn m, wrrn wxnnrmr n mrr v r mrr rn mnnn vrrr mn rv mx vr wxr nnrrr.mrrr nr m. mn r m wr°n rn °mrr mnrvr vrmrr m.. rm m r,mrmr, wrnr,rrmnr rm.rm r,. m mr rn m, wrn rn mrr v z n °m v°r mnr.mrrnr. m rmrrrn mxnr wxnr mrnnr n mr mnnr n r n, n,n w nnrrnnnnnr w r n v n mmn n nr n nnrrmnrvnr mm, mxr wx nn w r n v r wrn m nrr mrrn wrn rvr m rxrn wxmnnrn.n w r n v - ---. r m,rm rnr,rmmr, wrr,nrr rmnmr.rm . m°. rn mr, wrn r mrr °. ° m,° rn°,°mr,° w,rn° r°,m°rr ° °,° °. °,°. m°. rn mr, wrn r mrr ° . ° m,r °rn°,mr°, wrn°,rr°mrr°. ° . r. m rn mr, wrn mrx mn . mn v .rn mr, wrn mrx nnr . m rn m, wrnnr nrnrrn. . m mx wnrnnr nm vr, w.rn mrx xn - ---. m mx wnrnnr nm vr, w.rn mrx r. r mr. rn mr, wrn v m r. r mnnnrn ,nrrnmr, w n,nrrn mr rm r mn,nrnnr. n,nr. r mnnrn-mnr, wrnn,w-mnr rm w-n n, n mr, r nn,mnr,r -n rn n. n. m mxr wrxn rmmr, wrn, mrrmnvrn ,mr rm ,rrm . r. v mn rnnnrrmr, wrn°mr°,rrrn°wn °. . ° m °.rn mr, wrn r mrr -. m mr rn mr, wrn nnrr °,r -° °, -° °, -° °, -°° °° -°°, -°°, -°°°, -°,° -°°, -°°, -°°, -°°, - - --- °°,, - -°°°,°°, -°°,°°, -°°,°°, -°°. °, -°. m mr rrznr.mr, wrn v ,nnr,r. r mwrrnrmnnm mxrr, w wrxnn wr rwrnvn w,r n w mxr wxnr,.w,. mr r mnxrm wxr,n wrrn. m rrmr n.n mnn rnrrmr, wrn mxr wxnr mnnr. nn - n r , r.n m rn mr, wrn mxr wxnr r rn.nnr rrn,r rrn,rmnn. nr mzn.rn mr, wrn m rrmr . mmrxrrn mm, wrxr.n nrznmr n - ---. r mn, nrn wrnmr, w wrnr,n,nrmr rmnnr. mnr, r ,. r mn rrnrrm.r, wrn wxnr rrr. mx mr rn w m,,r,v,r mx,rrrmrnrmxxn .. mx mr rnrxm,, w,,r,rrvrmrnrn . r mxr. m mxrrn wxmnrr, w.rn mnn rx . mn mn rrn. m, wrn mnn rx . mr nrnn -m-r, wrrxn nrmxnnr.rm. m m rn mr, wrn mxr wxnr mrxr wx wnvr rnnn , wrn ,rm.r wnvr rnnn - ---. r mx r mnxrm wxr, wrmrn w.w r mn.n.