CA2005833A1 - Fuel briquettes with combustion inhibitor and method of making same - Google Patents
Fuel briquettes with combustion inhibitor and method of making sameInfo
- Publication number
- CA2005833A1 CA2005833A1 CA002005833A CA2005833A CA2005833A1 CA 2005833 A1 CA2005833 A1 CA 2005833A1 CA 002005833 A CA002005833 A CA 002005833A CA 2005833 A CA2005833 A CA 2005833A CA 2005833 A1 CA2005833 A1 CA 2005833A1
- Authority
- CA
- Canada
- Prior art keywords
- binder
- composition
- combustion inhibitor
- weight
- fuel
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
- Abandoned
Links
- 239000000446 fuel Substances 0.000 title claims abstract description 29
- 238000002485 combustion reaction Methods 0.000 title claims abstract description 20
- 239000003112 inhibitor Substances 0.000 title claims abstract description 15
- 238000004519 manufacturing process Methods 0.000 title claims 2
- 239000000203 mixture Substances 0.000 claims abstract description 25
- 239000011230 binding agent Substances 0.000 claims abstract description 20
- 239000004484 Briquette Substances 0.000 claims abstract description 16
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims abstract description 13
- 229910052799 carbon Inorganic materials 0.000 claims abstract description 13
- 239000003245 coal Substances 0.000 claims abstract description 13
- VTYYLEPIZMXCLO-UHFFFAOYSA-L Calcium carbonate Chemical compound [Ca+2].[O-]C([O-])=O VTYYLEPIZMXCLO-UHFFFAOYSA-L 0.000 claims abstract description 12
- 239000002006 petroleum coke Substances 0.000 claims abstract description 10
- 229910000019 calcium carbonate Inorganic materials 0.000 claims abstract description 6
- 229910000514 dolomite Inorganic materials 0.000 claims abstract description 6
- 239000010459 dolomite Substances 0.000 claims abstract description 6
- 239000000470 constituent Substances 0.000 claims abstract description 3
- 238000000034 method Methods 0.000 claims description 9
- 238000010438 heat treatment Methods 0.000 claims description 7
- 238000000465 moulding Methods 0.000 claims description 2
- LSNNMFCWUKXFEE-UHFFFAOYSA-N Sulfurous acid Chemical group OS(O)=O LSNNMFCWUKXFEE-UHFFFAOYSA-N 0.000 claims 2
- 230000001427 coherent effect Effects 0.000 claims 2
- 239000002699 waste material Substances 0.000 claims 2
- 238000006243 chemical reaction Methods 0.000 claims 1
- 230000035876 healing Effects 0.000 claims 1
- 238000007654 immersion Methods 0.000 claims 1
- 239000000126 substance Substances 0.000 claims 1
- 239000003039 volatile agent Substances 0.000 claims 1
- 239000000571 coke Substances 0.000 description 7
- 150000002500 ions Chemical class 0.000 description 7
- BVKZGUZCCUSVTD-UHFFFAOYSA-L Carbonate Chemical compound [O-]C([O-])=O BVKZGUZCCUSVTD-UHFFFAOYSA-L 0.000 description 4
- 239000003208 petroleum Substances 0.000 description 3
- 241000905957 Channa melasoma Species 0.000 description 2
- 239000002956 ash Substances 0.000 description 2
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 2
- 230000015572 biosynthetic process Effects 0.000 description 2
- 150000001875 compounds Chemical class 0.000 description 2
- 229910052760 oxygen Inorganic materials 0.000 description 2
- 239000001301 oxygen Substances 0.000 description 2
- 241000370685 Arge Species 0.000 description 1
- 101100481176 Bacillus subtilis (strain 168) thiE gene Proteins 0.000 description 1
- OYPRJOBELJOOCE-UHFFFAOYSA-N Calcium Chemical compound [Ca] OYPRJOBELJOOCE-UHFFFAOYSA-N 0.000 description 1
- 241000736839 Chara Species 0.000 description 1
- 241000518994 Conta Species 0.000 description 1
- 101100494344 Desulfobacterium autotrophicum (strain ATCC 43914 / DSM 3382 / HRM2) bzaF gene Proteins 0.000 description 1
- FYYHWMGAXLPEAU-UHFFFAOYSA-N Magnesium Chemical compound [Mg] FYYHWMGAXLPEAU-UHFFFAOYSA-N 0.000 description 1
- 101100270435 Mus musculus Arhgef12 gene Proteins 0.000 description 1
- 208000003251 Pruritus Diseases 0.000 description 1
- 235000013405 beer Nutrition 0.000 description 1
- 229910052791 calcium Inorganic materials 0.000 description 1
- 239000011575 calcium Substances 0.000 description 1
- 239000003795 chemical substances by application Substances 0.000 description 1
- YZIYKJHYYHPJIB-UUPCJSQJSA-N chlorhexidine gluconate Chemical compound OC[C@@H](O)[C@@H](O)[C@H](O)[C@@H](O)C(O)=O.OC[C@@H](O)[C@@H](O)[C@H](O)[C@@H](O)C(O)=O.C1=CC(Cl)=CC=C1NC(=N)NC(=N)NCCCCCCNC(=N)NC(=N)NC1=CC=C(Cl)C=C1 YZIYKJHYYHPJIB-UUPCJSQJSA-N 0.000 description 1
- 239000010883 coal ash Substances 0.000 description 1
- 238000010586 diagram Methods 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 239000003334 fuel briquet Substances 0.000 description 1
- 229930195733 hydrocarbon Natural products 0.000 description 1
- 150000002430 hydrocarbons Chemical class 0.000 description 1
- 229910052749 magnesium Inorganic materials 0.000 description 1
- 239000011777 magnesium Substances 0.000 description 1
- VZGDMQKNWNREIO-UHFFFAOYSA-N tetrachloromethane Chemical compound ClC(Cl)(Cl)Cl VZGDMQKNWNREIO-UHFFFAOYSA-N 0.000 description 1
- 101150029215 thiC gene Proteins 0.000 description 1
- 210000005239 tubule Anatomy 0.000 description 1
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 1
Classifications
-
- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10L—FUELS NOT OTHERWISE PROVIDED FOR; NATURAL GAS; SYNTHETIC NATURAL GAS OBTAINED BY PROCESSES NOT COVERED BY SUBCLASSES C10G, C10K; LIQUEFIED PETROLEUM GAS; ADDING MATERIALS TO FUELS OR FIRES TO REDUCE SMOKE OR UNDESIRABLE DEPOSITS OR TO FACILITATE SOOT REMOVAL; FIRELIGHTERS
- C10L5/00—Solid fuels
- C10L5/02—Solid fuels such as briquettes consisting mainly of carbonaceous materials of mineral or non-mineral origin
- C10L5/06—Methods of shaping, e.g. pelletizing or briquetting
- C10L5/10—Methods of shaping, e.g. pelletizing or briquetting with the aid of binders, e.g. pretreated binders
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E50/00—Technologies for the production of fuel of non-fossil origin
- Y02E50/30—Fuel from waste, e.g. synthetic alcohol or diesel
Landscapes
- Chemical & Material Sciences (AREA)
- Life Sciences & Earth Sciences (AREA)
- Environmental & Geological Engineering (AREA)
- General Life Sciences & Earth Sciences (AREA)
- Geochemistry & Mineralogy (AREA)
- Geology (AREA)
- Oil, Petroleum & Natural Gas (AREA)
- Organic Chemistry (AREA)
- Solid Fuels And Fuel-Associated Substances (AREA)
- Fuel Cell (AREA)
- Inert Electrodes (AREA)
- Battery Electrode And Active Subsutance (AREA)
- Telephone Function (AREA)
- Solid-Fuel Combustion (AREA)
- Liquid Carbonaceous Fuels (AREA)
- Coke Industry (AREA)
Abstract
ABSTRACT OF THE DISCLOSURE
Fuel briquettes comprising a fine-grain carbon carrier consisting of petroleum coke or a mixture of mainly petroleum coke and coal (preferably non-caking coal) with a binder and with a fine-grain combustion inhibitor mixed therein in the form of calcium carbonate and/or dolomite, which has been added to the initial fuel briquette mixture in a quantity in excess of 2%
by weight, volatile constituents being eliminated from the fuel briquette.
Fuel briquettes comprising a fine-grain carbon carrier consisting of petroleum coke or a mixture of mainly petroleum coke and coal (preferably non-caking coal) with a binder and with a fine-grain combustion inhibitor mixed therein in the form of calcium carbonate and/or dolomite, which has been added to the initial fuel briquette mixture in a quantity in excess of 2%
by weight, volatile constituents being eliminated from the fuel briquette.
Description
29~S833 BRIQ~ 'ES WIq~I COMBt~STION I~HIBI~irOR AND ~OD OF M~XING SAl~E
CIF~AT:lON
The lrlv~ntion ~late~ to fuel bxiqu~3tte~ c~omprl~lng a, ~ine,--graln c~rbon earrier ~onsi6ting oC petroll2um coke or a ~ixt;u:re o~ mainly petr~le~ cok~ and oc,al, prefera~ly non-ca~ing co~,l., with a b~nder. ~h~ term "fuel briquet~es" denote~ brir~ette~ of the kind used for heat generati.on in domes.tia fires, central heating boi1er6 r thermal power 6tations an~ the like.
E~R~R~ 5~T~ 3~LON
Fuel briquette~ in whioh the fi.ne-grain carbon ca~rier i~
petrole~m co~e or mainly petroleu~ coke generate excessive temperatures on ao~nbustion whi~h clamage the combu~tion equipment.
They have inadequate ~tr~ength and readily d~lntec3rate ~ur~nc~
handling and combu~tion~
FU~ iqut~tte~ o~ this kin~ generelte ~xt,~6siv~ ~emperatures on combu~tion and ~e~t~oy the combustion eg~ipment from the simple ~urnat,e to the heating boiler. Petrolt~um coke frequently oontains a conslderable amount of sul~ur, e~g~ in quantities o~
0.8 to 5% or more. The same applaes to the binde:r, parti~larly in the ~ase of pitch.
[ 1 ;~OOS~333 Fuel ~rique~tes conta~ning petroleu~.n ~oke or main}y petroleum coke as t:he ~ine-grain c~rbon carrier ther1~0re ~ene~ate exeessiv~ amount~ of ~ulfur dioxid,3 i~na, for other reasons, nitric oxides a~. well.
The l~ttex also appl ~ es to briquette~ o:E ~he above-d~cr~.~)ed ¢omp~ition (U.~:. Patent 2,036,642) whl~h, in order to i.ncrease the ~trength, ~re manu~actured by mean~3 of a special binder mixtu~e whiah also contaLns caloiu~ hyl1roz:lde ~s a binder in ~
quantlty o~ a~o~ 2~ by weight. ~n thi~s ca!;e the in$~ial. mixt:ure i~ heat-trealted at a~ou~ 250-C in ~he unmo:lded ~tate and is molded i~to the ~inal ~uel briquettes nf~er ~ooling.
In pr2,ctice, ~uel bri~uettes col1talning ~ine-grain hi.gh-a.sh ~on~ont c:oal a~ caxbon carr~er hav,~3 ~e-~n disclosed experimental-ly wlth addition~ of ~ine-graln calcium carbona~e a~ desul~urlz-ation agent, due conside~ation be$ng g:Lven to sto$chiometrlcaspects. TherQ 3~e no pxoblem~ as~cciated with th~ ¢om~ustion temperat~res oacUrring with such fuel briqllettes, ~u~h temperat~res be~ng aete~tnined by the coal ash ~ontent. The regulred de5ulfurization ~5 unsat~ ac1:ory ~nd ~orreYponding ~0 2uel bri~uettes hav~ ound little use :in practice.
5~JE.~'S OF ~H~ YX~TIO~
An o~eot of tha invention ~8 to provide ~uel bri~uetteq ¢ontainlng petroleum co~e or mainly petroleum coXe whlch wlll burn in z. co~txo1led fashion involving no pro~le~s for the combus~ion appllance.
~ nother ob~e~t o~ the inven~ion is 1;o pr.ov~de an improved metho~ of` maXlng fuel ~riguettes.
~ 2 J
17~44 S~MMA~ OF TH~ INVE~IO~~
To this end, the invention relates to i.uel bric~ettes com3-,ri~-ing a ~ine-gxaill c~lrbon aar~ie~ ca,nsistLn5~ of petroleum coke o~
~ mixtur~3 o~ ma~nly petroleu~ c:oke and coal (preferably non-c~ak-5 lng coal~ wi~h ~ ~i.nder and wlt;h a ~ine-gxain COmbUStiOll inhlbitor m~xed therein in the fo~ of calc~um carbonate an~for dolomite~ whi~h has~ beer~ ~dded to the init:ial fuel briquette mix~ure in a quan~i.ty in ex~e~ of 2~ ~y weight, volati:Le ~on&tl~u-~nts ~elnq elimi.nated Pro~ the fruel briquette.
Th~ term volatile ~ons~t~ents denote~ ~ate~ vApor, ~snd ~l~o hydroc~rbon~. Test~ hâve Bhowrl that vol3t:ile con~tituento are libe~ated at ev~n ~ery 3.ow temperatures. ~he volatlle const;Ltu-e~t~ ori~3inate ~om the inltial mi~ture, ~.g., from the binder.
The heat treatment i5 eP~ected neverthele~;s even i~ there are no volat~le constituents present.
A 6at:l6faatory heat treatmerlt is obtained even at te~npera~
tures of littlo ovor 100-C. The temperatures o~ t,he ~eat tr~at-ment 6hould not ~xc~eed 500'~.
In th~æ ~uel bric~ettes aa¢ordlng t~ the t nvention, the ~alaium aar~onat:e 2Ind~0r the dolo~ite ~ulI111 a new fun~tio~, i.e. thal; o~ a ao~ ustic~n inhi~itGr. The addition of calciu~
carbonatl3 and~or dolomi~e has ~een mixed lnto the initial mixture Ln a quan~ity suffi~ient ~or this puxpose and w:ith ~
flneness sufflc:ient; ~or this purpose. ~uring the heat-~rea~ment the fue~ briquett~si unde~go hardening. They do not dis~ntegrate on handl lng .
In ad~ition, ~hey ret:ain th~ir shape ~ufflcient:ly du~ing combus~$on, even when bllrning ~way.
[ 3 ~
20058~3 Conse~uently, durlng combust:ioni of the fuel bri.quettes aocording to th~ inventi>on a calcium-contcl~n~ng a~;h laye~ o~
adequa~e th~eknessi continually forms around the lr,,dividual brlquett~es and enclo~es tho un~urn.ed cor~ like a closed she:ll as it were, ~o~m~ ~ dlffuGi.on bar~ler to the oxygen requir~3d ~or combustion o~ the car~on ca~ri~r and allows oxygen to pZ16S only ln a quanti~y 6uch that the~e are no distur~ingly high tempexatt~xes. The ~uantity of co~bustion ~nhibitor ~ixed into the product is adjusted in thiC way.
3ur~nc3 bu~ning, ao ths d~amet~r of th~ unburned core decrea~es the ash layer .become~ thicker an~ mor~ ota~l~ as ~l ~hell, BO that no ~sturbingly high te~per,~tures occur duxirlcJ
the entire combu~t1on of the fuel ~risuet~.~s accordin~ to the invention~ On the othe~ hand, the tem~er~tures are adequate for desul~uri.zatlon, calc1um ~ulfite o:r c~lcium ~ulfate, or magnesium ~ulf~te or m~g~eslum ~ul~ate ~or~ing and going int:o the ash. A~ording~ to the ~nvention, ther~efore, it ~8 ~lso possible to use petroleu~ cok- having a hil~h 6ulfur content.
Thei degree of desul~uri~tlon tS a's much a.s 80~ and moxe.
There are nu~erous possibil~ties of development withln the inventlon. A prefe~rred embodi~ent of the invention whic:h i~;
particularly lmport;ant econom$~ally, s~nce ~arge quantit:ies of petroleuT~ coke and pitch, are forme~ in pet;roleum di~tillation, is chara~terized in that. the carbon carrier consists of petroleur~ aoXe and the combustton inhibito~ has been added to the initial mixkure~ ln a quantity in exce~ of 3% by welght.
Fuel briquett;es aocord~ng to the invention have prov~d ~atis~actory ~n wh~.ch the bi~der i~ a bitLlminous bri~ue~.tin~
XC~OS83;~
~lhder, e.g. pitch, W~iCh has ~een added to the ini.tial l~ixture in a quantlty of 5 l:o 10~ by weight;, pre~era~ly ln a guantity o~
abou~ 8% by ~eight.
Also satisfa~ory are ~uel brl~uettes in wh$ch t.he binder :Ls ~u~ltQ w.~ste li~uor, which ha~ beeln ad~ed to the lnitla:l mlxture in a quantity o~ ~ to 10~ by weight., prefera~ly in a quant~ty of a~out 6~ by we~ght. Ot~er bind~r~ c~n b~3 used according to 1;he inventlon. The c:o~ustion inhibitor i~ preferably solely ca~cium carbonate. The grai.n ~iz:e of th~
carbon carrler in the fuel ~riq~lettes according to ~h~ invent;lon 3hould not be exc~sC~ive but ~s usually belc~w 3 mm. Some larg~3r q~n-slze component:s do not ha~e an adver~:e ef~ect. Th~. graln ~iz~ of th~ oombusti.on inh$b~to~ should ~e 60 ad~u~ted aR to give the ef~ects desc~ d. A graln ~ize o~ le~s than 1 mm i~
there~ore advantage,ously used.
~ he fuel bri~let~es aooxding to the invent~on can be manu~actured in vari,ous ways us~.ng convQntional br~quettlng technology ald~. More particul~rly, brlqu~tting presse~ can ~)e used. ~h13 subject o~ the~ ~nvent,ion i8 alsc~ a process for productlon of ~uel briguettes of' the compo~;ltion indicated, wherein the ~ne~grzlin c~,r~oh cz,rrier, the binder and the ine-grain CombUE;t~ on ~nhib~tor a~e mixed and pre~orms a~e mo].ded ~rom the mixture an~l wherein by a heat trez\tment of a tempere~ure below the ~eaction t:emper2ture o~ the combustion 25 inh~ bitor the pr~3for~s are hardened and any volatile con~tltuents present are ~uff~Lciently comp~et.ely eliminated. Hydrocarbons ~re also liberated even ~t 300'C. W~ter vapor is el~minated too at tempe~a~ul-es a~ove l.Q0-C i~ thQ pre~orm~ co~tain water.
~ 5 ]
CIF~AT:lON
The lrlv~ntion ~late~ to fuel bxiqu~3tte~ c~omprl~lng a, ~ine,--graln c~rbon earrier ~onsi6ting oC petroll2um coke or a ~ixt;u:re o~ mainly petr~le~ cok~ and oc,al, prefera~ly non-ca~ing co~,l., with a b~nder. ~h~ term "fuel briquet~es" denote~ brir~ette~ of the kind used for heat generati.on in domes.tia fires, central heating boi1er6 r thermal power 6tations an~ the like.
E~R~R~ 5~T~ 3~LON
Fuel briquette~ in whioh the fi.ne-grain carbon ca~rier i~
petrole~m co~e or mainly petroleu~ coke generate excessive temperatures on ao~nbustion whi~h clamage the combu~tion equipment.
They have inadequate ~tr~ength and readily d~lntec3rate ~ur~nc~
handling and combu~tion~
FU~ iqut~tte~ o~ this kin~ generelte ~xt,~6siv~ ~emperatures on combu~tion and ~e~t~oy the combustion eg~ipment from the simple ~urnat,e to the heating boiler. Petrolt~um coke frequently oontains a conslderable amount of sul~ur, e~g~ in quantities o~
0.8 to 5% or more. The same applaes to the binde:r, parti~larly in the ~ase of pitch.
[ 1 ;~OOS~333 Fuel ~rique~tes conta~ning petroleu~.n ~oke or main}y petroleum coke as t:he ~ine-grain c~rbon carrier ther1~0re ~ene~ate exeessiv~ amount~ of ~ulfur dioxid,3 i~na, for other reasons, nitric oxides a~. well.
The l~ttex also appl ~ es to briquette~ o:E ~he above-d~cr~.~)ed ¢omp~ition (U.~:. Patent 2,036,642) whl~h, in order to i.ncrease the ~trength, ~re manu~actured by mean~3 of a special binder mixtu~e whiah also contaLns caloiu~ hyl1roz:lde ~s a binder in ~
quantlty o~ a~o~ 2~ by weight. ~n thi~s ca!;e the in$~ial. mixt:ure i~ heat-trealted at a~ou~ 250-C in ~he unmo:lded ~tate and is molded i~to the ~inal ~uel briquettes nf~er ~ooling.
In pr2,ctice, ~uel bri~uettes col1talning ~ine-grain hi.gh-a.sh ~on~ont c:oal a~ caxbon carr~er hav,~3 ~e-~n disclosed experimental-ly wlth addition~ of ~ine-graln calcium carbona~e a~ desul~urlz-ation agent, due conside~ation be$ng g:Lven to sto$chiometrlcaspects. TherQ 3~e no pxoblem~ as~cciated with th~ ¢om~ustion temperat~res oacUrring with such fuel briqllettes, ~u~h temperat~res be~ng aete~tnined by the coal ash ~ontent. The regulred de5ulfurization ~5 unsat~ ac1:ory ~nd ~orreYponding ~0 2uel bri~uettes hav~ ound little use :in practice.
5~JE.~'S OF ~H~ YX~TIO~
An o~eot of tha invention ~8 to provide ~uel bri~uetteq ¢ontainlng petroleum co~e or mainly petroleum coXe whlch wlll burn in z. co~txo1led fashion involving no pro~le~s for the combus~ion appllance.
~ nother ob~e~t o~ the inven~ion is 1;o pr.ov~de an improved metho~ of` maXlng fuel ~riguettes.
~ 2 J
17~44 S~MMA~ OF TH~ INVE~IO~~
To this end, the invention relates to i.uel bric~ettes com3-,ri~-ing a ~ine-gxaill c~lrbon aar~ie~ ca,nsistLn5~ of petroleum coke o~
~ mixtur~3 o~ ma~nly petroleu~ c:oke and coal (preferably non-c~ak-5 lng coal~ wi~h ~ ~i.nder and wlt;h a ~ine-gxain COmbUStiOll inhlbitor m~xed therein in the fo~ of calc~um carbonate an~for dolomite~ whi~h has~ beer~ ~dded to the init:ial fuel briquette mix~ure in a quan~i.ty in ex~e~ of 2~ ~y weight, volati:Le ~on&tl~u-~nts ~elnq elimi.nated Pro~ the fruel briquette.
Th~ term volatile ~ons~t~ents denote~ ~ate~ vApor, ~snd ~l~o hydroc~rbon~. Test~ hâve Bhowrl that vol3t:ile con~tituento are libe~ated at ev~n ~ery 3.ow temperatures. ~he volatlle const;Ltu-e~t~ ori~3inate ~om the inltial mi~ture, ~.g., from the binder.
The heat treatment i5 eP~ected neverthele~;s even i~ there are no volat~le constituents present.
A 6at:l6faatory heat treatmerlt is obtained even at te~npera~
tures of littlo ovor 100-C. The temperatures o~ t,he ~eat tr~at-ment 6hould not ~xc~eed 500'~.
In th~æ ~uel bric~ettes aa¢ordlng t~ the t nvention, the ~alaium aar~onat:e 2Ind~0r the dolo~ite ~ulI111 a new fun~tio~, i.e. thal; o~ a ao~ ustic~n inhi~itGr. The addition of calciu~
carbonatl3 and~or dolomi~e has ~een mixed lnto the initial mixture Ln a quan~ity suffi~ient ~or this puxpose and w:ith ~
flneness sufflc:ient; ~or this purpose. ~uring the heat-~rea~ment the fue~ briquett~si unde~go hardening. They do not dis~ntegrate on handl lng .
In ad~ition, ~hey ret:ain th~ir shape ~ufflcient:ly du~ing combus~$on, even when bllrning ~way.
[ 3 ~
20058~3 Conse~uently, durlng combust:ioni of the fuel bri.quettes aocording to th~ inventi>on a calcium-contcl~n~ng a~;h laye~ o~
adequa~e th~eknessi continually forms around the lr,,dividual brlquett~es and enclo~es tho un~urn.ed cor~ like a closed she:ll as it were, ~o~m~ ~ dlffuGi.on bar~ler to the oxygen requir~3d ~or combustion o~ the car~on ca~ri~r and allows oxygen to pZ16S only ln a quanti~y 6uch that the~e are no distur~ingly high tempexatt~xes. The ~uantity of co~bustion ~nhibitor ~ixed into the product is adjusted in thiC way.
3ur~nc3 bu~ning, ao ths d~amet~r of th~ unburned core decrea~es the ash layer .become~ thicker an~ mor~ ota~l~ as ~l ~hell, BO that no ~sturbingly high te~per,~tures occur duxirlcJ
the entire combu~t1on of the fuel ~risuet~.~s accordin~ to the invention~ On the othe~ hand, the tem~er~tures are adequate for desul~uri.zatlon, calc1um ~ulfite o:r c~lcium ~ulfate, or magnesium ~ulf~te or m~g~eslum ~ul~ate ~or~ing and going int:o the ash. A~ording~ to the ~nvention, ther~efore, it ~8 ~lso possible to use petroleu~ cok- having a hil~h 6ulfur content.
Thei degree of desul~uri~tlon tS a's much a.s 80~ and moxe.
There are nu~erous possibil~ties of development withln the inventlon. A prefe~rred embodi~ent of the invention whic:h i~;
particularly lmport;ant econom$~ally, s~nce ~arge quantit:ies of petroleuT~ coke and pitch, are forme~ in pet;roleum di~tillation, is chara~terized in that. the carbon carrier consists of petroleur~ aoXe and the combustton inhibito~ has been added to the initial mixkure~ ln a quantity in exce~ of 3% by welght.
Fuel briquett;es aocord~ng to the invention have prov~d ~atis~actory ~n wh~.ch the bi~der i~ a bitLlminous bri~ue~.tin~
XC~OS83;~
~lhder, e.g. pitch, W~iCh has ~een added to the ini.tial l~ixture in a quantlty of 5 l:o 10~ by weight;, pre~era~ly ln a guantity o~
abou~ 8% by ~eight.
Also satisfa~ory are ~uel brl~uettes in wh$ch t.he binder :Ls ~u~ltQ w.~ste li~uor, which ha~ beeln ad~ed to the lnitla:l mlxture in a quantity o~ ~ to 10~ by weight., prefera~ly in a quant~ty of a~out 6~ by we~ght. Ot~er bind~r~ c~n b~3 used according to 1;he inventlon. The c:o~ustion inhibitor i~ preferably solely ca~cium carbonate. The grai.n ~iz:e of th~
carbon carrler in the fuel ~riq~lettes according to ~h~ invent;lon 3hould not be exc~sC~ive but ~s usually belc~w 3 mm. Some larg~3r q~n-slze component:s do not ha~e an adver~:e ef~ect. Th~. graln ~iz~ of th~ oombusti.on inh$b~to~ should ~e 60 ad~u~ted aR to give the ef~ects desc~ d. A graln ~ize o~ le~s than 1 mm i~
there~ore advantage,ously used.
~ he fuel bri~let~es aooxding to the invent~on can be manu~actured in vari,ous ways us~.ng convQntional br~quettlng technology ald~. More particul~rly, brlqu~tting presse~ can ~)e used. ~h13 subject o~ the~ ~nvent,ion i8 alsc~ a process for productlon of ~uel briguettes of' the compo~;ltion indicated, wherein the ~ne~grzlin c~,r~oh cz,rrier, the binder and the ine-grain CombUE;t~ on ~nhib~tor a~e mixed and pre~orms a~e mo].ded ~rom the mixture an~l wherein by a heat trez\tment of a tempere~ure below the ~eaction t:emper2ture o~ the combustion 25 inh~ bitor the pr~3for~s are hardened and any volatile con~tltuents present are ~uff~Lciently comp~et.ely eliminated. Hydrocarbons ~re also liberated even ~t 300'C. W~ter vapor is el~minated too at tempe~a~ul-es a~ove l.Q0-C i~ thQ pre~orm~ co~tain water.
~ 5 ]
2~0S83~
In a preferred embodiment of the im ent.~.on the heat treatment i~ carried out in a rotary tubul~r furn~lc~ c~ntaining an immex~ion bed 20r t~e preform~, ~uch bed consisting O:e ~ine-grain pe~roleum coke (G~man Paten'c l~ocument 37 2~ 4,64) . Tl~o hardening S desc~ri~ed 16 obta.ined witll a ~ery non-in~ur:Lous e~fect in the ~mmer6~0n bed.
The ~u21 br1quet:1:e~ o~' the inven,tion thus adva~nt;ageou~y c~mprise a~ body heat-~treat:ed to clrive off volat~les and predomlnan~ly con~lt:uted of a fi.ne-gr~$n c~rbon carrier ~;elec:t:ed Srom ~he group wh~ch con~ t~ Or pQt~o~um c:o~e, coal and ~ixt,ure~
thereoS, a blnder ret:ainirJg th~ body in a co:herent form, and zl ~ne-grain combu~iorl ~nhibitor pre~nt in a.n amount in exces~; of 2% ~y we~ght oS a oompos~tion oo~tai:n~ng thel carrier, bincler substanc~ alnd combus~ion ~nhi~tor~ f:rom which the b~dy 1~
~ormed, the combu~tion inhi~itor be~ng sale~ted from ~he yroup wh1ch cons1st~ of ~alcium car~bonate, dolomite and mixture~
thereo2.
The me~hod compr1ses the steps oe:
(a) so2~ng A ~omposltion consist~ng e~sent~ally o2 a flne-grain cnrbon carri-r ~lected from the l3roup wh~c~ c~nsist~
of petroleum co~e, coal an~ mixtures thereof~ a binder capa~le oi' retalnlng ~l body o~ ~he carbon car~or ln a cohe~en~ i~orm, and fine-graln com~ust,lon.~nhi~itor selected from ~he group wh~ch cons~sts oP caloium carbonate, dolo~:ite ~nd m~xtures thexeo~
present ln an amo~nt ~n ex~es~ of 2% by weigh~ of the compo~ition;
(~ molding preforms having conf:Lguratlons o~ ~riquettes from the compos~,t~on; and ~ 6 ]
2(~C)5833 ~ c~ heating the p~eforms to ~ temperatule ~ufficient t:o na~den th~ preform~ ~nto fuel briqu~sttes and to drive Of~
vol~tllo aono~ucn~ ro~ thc ~ s~ tne temperac~re ~ei.ng below a ~e~ction te~perat.u~ o~ the car~bon ,~arrler with t:he combustion inh~bitor.
~U~7 DEs~xIprIoN ~ EY~9'I~
Th~ above and other ob~ects, featurel~ and advantages of my i~vention ~111 be~o~e more readily app~rent from ~h~e ~ollowing description, reference be~ng made to the acaompanying h~ghly diagrammatic drawln(~ 1n whlch th~e ~c~le l?IGUI~E of wnich i~
b~ocX diagram illu~trating the me~hc)d o~ tho invent.ion.
~e~ EI~8~1P~
As can be seen ~rom the drawin~, petroleLIm coke or a m~xture o~ petroleum coke and non-ca~lng coal f~,om E~ource 10, a binder ~5 which can be pitch o:r wa~te ~ul~ite liquor ~'~om a ~ou~ce 11 and the combustion inhibitor in the ~or~l of c~ ium carbonate, dolomite or ~ixturol~ th~r~!of Pro~ a ~our~e 12 are blonded in mixture 13 and the mixtur~ i~ mo:Ldec~ to ~on~l briquettes o ~
~iz~ and s:hape corr~3ponding to the charcoa:L briquet:tes utilized ~or domestic pu~pose~i. The preform~, are then ~ub~ected to hea~
trea~ent at 15 in a rotary tube ~o~mation with a p~troleum cok:e in a immer~ion ~ed t;he~eo~ in t~e rotary tube formation to ~rive of~ volat~Les as represented at 16. The prc~duo~ ic the fuel br~uettes shown ~t 17.
t 7 ) 1744~
~ IFIC ~XA~5~LE~, A compo~1tion con~1st:lng essenti.a11y o~ 8% ~y WC!lght ~itch, 5 by weight o~ calcium carbonate o~ a grcund l:o a part:icle l3~ze rango o~ 0.1 to 0.5 ~m ancl the ba1arl~e ~Qt~o1eum co~e with a paxtlcle BiZe rang~ of 0,S to 2.5 mm ~ b1ende~ ~n ~ con~çntiona1 mixer and ~he resu1ting mixture i~ then molded to ~orm br:lq~ett.es.
The resultlng pre~orms are then heat treated in a rotary ~ube ~ormat1On by 1mmersion in ~ petro1eum coXe bed at a ~empe~ature o~
300'C to driv~ of~ vo~ati1e8 and harden the preform~ into t~e briquettes.
Th- br1quette~ ar~ ~ound to burn ~n a h1qh1y uni~orm ~anner wlthout the formation o~ hot ~pots with little emi~sion o~ ~ul~ur compounds. The a~h is ~ound to cont~in su1f'ur compounds wh~ch drive from the su1fur content of the petro1eum coke.
Similar result~ are o~tained when 6% wa~te 8u1fite 1iguor i~
subst~tute~ ~or the pitch binder.
~ 8
In a preferred embodiment of the im ent.~.on the heat treatment i~ carried out in a rotary tubul~r furn~lc~ c~ntaining an immex~ion bed 20r t~e preform~, ~uch bed consisting O:e ~ine-grain pe~roleum coke (G~man Paten'c l~ocument 37 2~ 4,64) . Tl~o hardening S desc~ri~ed 16 obta.ined witll a ~ery non-in~ur:Lous e~fect in the ~mmer6~0n bed.
The ~u21 br1quet:1:e~ o~' the inven,tion thus adva~nt;ageou~y c~mprise a~ body heat-~treat:ed to clrive off volat~les and predomlnan~ly con~lt:uted of a fi.ne-gr~$n c~rbon carrier ~;elec:t:ed Srom ~he group wh~ch con~ t~ Or pQt~o~um c:o~e, coal and ~ixt,ure~
thereoS, a blnder ret:ainirJg th~ body in a co:herent form, and zl ~ne-grain combu~iorl ~nhibitor pre~nt in a.n amount in exces~; of 2% ~y we~ght oS a oompos~tion oo~tai:n~ng thel carrier, bincler substanc~ alnd combus~ion ~nhi~tor~ f:rom which the b~dy 1~
~ormed, the combu~tion inhi~itor be~ng sale~ted from ~he yroup wh1ch cons1st~ of ~alcium car~bonate, dolomite and mixture~
thereo2.
The me~hod compr1ses the steps oe:
(a) so2~ng A ~omposltion consist~ng e~sent~ally o2 a flne-grain cnrbon carri-r ~lected from the l3roup wh~c~ c~nsist~
of petroleum co~e, coal an~ mixtures thereof~ a binder capa~le oi' retalnlng ~l body o~ ~he carbon car~or ln a cohe~en~ i~orm, and fine-graln com~ust,lon.~nhi~itor selected from ~he group wh~ch cons~sts oP caloium carbonate, dolo~:ite ~nd m~xtures thexeo~
present ln an amo~nt ~n ex~es~ of 2% by weigh~ of the compo~ition;
(~ molding preforms having conf:Lguratlons o~ ~riquettes from the compos~,t~on; and ~ 6 ]
2(~C)5833 ~ c~ heating the p~eforms to ~ temperatule ~ufficient t:o na~den th~ preform~ ~nto fuel briqu~sttes and to drive Of~
vol~tllo aono~ucn~ ro~ thc ~ s~ tne temperac~re ~ei.ng below a ~e~ction te~perat.u~ o~ the car~bon ,~arrler with t:he combustion inh~bitor.
~U~7 DEs~xIprIoN ~ EY~9'I~
Th~ above and other ob~ects, featurel~ and advantages of my i~vention ~111 be~o~e more readily app~rent from ~h~e ~ollowing description, reference be~ng made to the acaompanying h~ghly diagrammatic drawln(~ 1n whlch th~e ~c~le l?IGUI~E of wnich i~
b~ocX diagram illu~trating the me~hc)d o~ tho invent.ion.
~e~ EI~8~1P~
As can be seen ~rom the drawin~, petroleLIm coke or a m~xture o~ petroleum coke and non-ca~lng coal f~,om E~ource 10, a binder ~5 which can be pitch o:r wa~te ~ul~ite liquor ~'~om a ~ou~ce 11 and the combustion inhibitor in the ~or~l of c~ ium carbonate, dolomite or ~ixturol~ th~r~!of Pro~ a ~our~e 12 are blonded in mixture 13 and the mixtur~ i~ mo:Ldec~ to ~on~l briquettes o ~
~iz~ and s:hape corr~3ponding to the charcoa:L briquet:tes utilized ~or domestic pu~pose~i. The preform~, are then ~ub~ected to hea~
trea~ent at 15 in a rotary tube ~o~mation with a p~troleum cok:e in a immer~ion ~ed t;he~eo~ in t~e rotary tube formation to ~rive of~ volat~Les as represented at 16. The prc~duo~ ic the fuel br~uettes shown ~t 17.
t 7 ) 1744~
~ IFIC ~XA~5~LE~, A compo~1tion con~1st:lng essenti.a11y o~ 8% ~y WC!lght ~itch, 5 by weight o~ calcium carbonate o~ a grcund l:o a part:icle l3~ze rango o~ 0.1 to 0.5 ~m ancl the ba1arl~e ~Qt~o1eum co~e with a paxtlcle BiZe rang~ of 0,S to 2.5 mm ~ b1ende~ ~n ~ con~çntiona1 mixer and ~he resu1ting mixture i~ then molded to ~orm br:lq~ett.es.
The resultlng pre~orms are then heat treated in a rotary ~ube ~ormat1On by 1mmersion in ~ petro1eum coXe bed at a ~empe~ature o~
300'C to driv~ of~ vo~ati1e8 and harden the preform~ into t~e briquettes.
Th- br1quette~ ar~ ~ound to burn ~n a h1qh1y uni~orm ~anner wlthout the formation o~ hot ~pots with little emi~sion o~ ~ul~ur compounds. The a~h is ~ound to cont~in su1f'ur compounds wh~ch drive from the su1fur content of the petro1eum coke.
Similar result~ are o~tained when 6% wa~te 8u1fite 1iguor i~
subst~tute~ ~or the pitch binder.
~ 8
Claims (19)
1. A fuel briquette for combustion to produce heat, comprising a body heat-treated to drive off volatiles and predominantly constituted of a fine-grain carbon carrier selected from the group which consists of petroleum coke, coal and mixtures thereof, a binder retaining said body in a coherent form, and a fine-grain combustion inhibitor present in an amount in excess of 2% by weight of, a composition. containing said carrier, binder substance and combustion inhibitor from which said body is formed, said combustion inhibitor being selected from the group which consists of calcium carbonate, dolomite and mixtures thereof.
2. The fuel briquette defined in claim 1 wherein said coal is a noncaking coal.
3. The fuel briquette defined in claim 1 wherein said carbon carrier consists of petroleum coke and said combustion inhibitor is present in an amount corresponding to in excess of 3% by weight of said composition.
4. The fuel briquette defined in claim 1 wherein said binder is a bituminous briquetting binder present in an amount corresponding to 5 to 10% by weight of said composition.
5. The fuel briquette defined in claim 4 wherein said binder is pitch and is present in an amount corresponding to about 8%
by weight of said composition.
[ 9 ]
by weight of said composition.
[ 9 ]
6. The fuel briquette defined in claim 1 wherein said binder is a sulfite waste liquor present in an amount corresponding to 5 to 10% by weight of said composition.
7. The fuel briquette defined in claim 6 wherein said binder is present in an amount corresponding to about 6% by weight of said composition.
8. The fuel briquette defined in claim 1 wherein said combustion inhibitor is solely calcium carbonate.
9. The fuel briquette defined in claim 1 wherein said combustion inhibitor has a grain size of less than 1 mm.
10. The fuel briquette defined in claim 1 wherein said carbon carrier has a grain size of less than 3 mm.
11. A method of making fuel briquettes for combustion to produce heat, comprising the steps of:
(a) forming a composition consisting essentially of a fine-grain carbon carrier selected from the group which consists of petroleum coke, coal and mixtures thereof, a binder capable of retaining a body of said carbon carrier in a coherent form, and a fine-grain combustion inhibitor selected from the group which consists of calcium carbonate, dolomite and mixtures thereof present in an amount in excess of 2% by weight of said composition;
(b) molding preforms having configurations of briguettes [ 10 ]
from said composition; and (c) heating said preforms to a temperature sufficient to harden said performs into fuel briquettes and to drive off volatile constituents from said briquettes, said temperature being below a reaction temperature of said carbon carrier with said combustion inhibitor.
(a) forming a composition consisting essentially of a fine-grain carbon carrier selected from the group which consists of petroleum coke, coal and mixtures thereof, a binder capable of retaining a body of said carbon carrier in a coherent form, and a fine-grain combustion inhibitor selected from the group which consists of calcium carbonate, dolomite and mixtures thereof present in an amount in excess of 2% by weight of said composition;
(b) molding preforms having configurations of briguettes [ 10 ]
from said composition; and (c) heating said preforms to a temperature sufficient to harden said performs into fuel briquettes and to drive off volatile constituents from said briquettes, said temperature being below a reaction temperature of said carbon carrier with said combustion inhibitor.
12. The method defined in claim 11 wherein said healing in step (c) is carried out at a temperature of less than 500°C.
13. The method defined in claim 12 wherein the heating in step (c) is carried out in a rotary tubular furnace containing an immersion bed for said preforms, said bed consisting of fine-grain petroleum coke.
14. The method defined in claimed 13 wherein said coal is a noncaking coal.
15. The method defined in claimed 13 wherein said carbon carrier consists of petroleum coke and said combustion inhibitor is present in an amount corresponding to in excess of 3% by weight of said composition.
16. The method defined in claim 15 wherein said binder is a bituminous briquetting binder present in an amount of 5 to 10%
by weight of said composition.
[ 11 ]
by weight of said composition.
[ 11 ]
17. The method defined in claim 15 wherein said binder is a sulfite waste liquor present in an amount of 5 to 10% by weight of said composition.
18. The method defined in claim 15 wherein said combustion inhibitor is solely calcium carbonate.
19. The method defined in claim 15 wherein said combustion inhibitor has a grain size of less than 1 mm and said carbon carrier has a grain size of less than 3 mm.
[ 12 ]
[ 12 ]
Applications Claiming Priority (2)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
DEP3843449.0-24 | 1988-12-23 | ||
DE3843449A DE3843449A1 (en) | 1988-12-23 | 1988-12-23 | FUEL BRIQUETTES AND PRODUCTION METHOD |
Publications (1)
Publication Number | Publication Date |
---|---|
CA2005833A1 true CA2005833A1 (en) | 1990-06-23 |
Family
ID=6369982
Family Applications (1)
Application Number | Title | Priority Date | Filing Date |
---|---|---|---|
CA002005833A Abandoned CA2005833A1 (en) | 1988-12-23 | 1989-12-18 | Fuel briquettes with combustion inhibitor and method of making same |
Country Status (11)
Country | Link |
---|---|
EP (1) | EP0374402B1 (en) |
JP (1) | JPH0668110B2 (en) |
AT (1) | ATE85641T1 (en) |
CA (1) | CA2005833A1 (en) |
DE (2) | DE3843449A1 (en) |
DK (1) | DK658689A (en) |
ES (1) | ES2039056T3 (en) |
GR (1) | GR3007517T3 (en) |
IE (1) | IE63118B1 (en) |
PT (1) | PT92629B (en) |
TR (1) | TR25967A (en) |
Cited By (1)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
CN104973880A (en) * | 2015-06-25 | 2015-10-14 | 云南永昌硅业股份有限公司 | Carbonaceous pellet and preparation method thereof |
Families Citing this family (4)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
DE4214434C1 (en) * | 1992-05-06 | 1993-07-15 | Applied Industrial Materials Corp., Deerfield, Ill., Us | |
CN101948708B (en) * | 2010-10-12 | 2013-01-16 | 张家港华汇特种玻璃有限公司 | Solid fuel composition and application thereof in glass melting |
CN108956663B (en) * | 2018-08-23 | 2020-12-29 | 索通发展股份有限公司 | Method for measuring carbon roasting temperature by using petroleum coke Lc value |
CN112879918A (en) * | 2021-02-05 | 2021-06-01 | 云南大地丰源环保有限公司 | Method for inhibiting coking of hazardous waste rotary kiln |
Family Cites Families (8)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
GB219772A (en) * | 1923-06-06 | 1924-08-07 | Wilhelm Habets | Method of improving coke as fuel for stoves and the like |
DE476319C (en) * | 1926-07-25 | 1929-05-15 | Koks Und Halbkoks Brikettierun | Process for the production of briquettes, in particular from fuels and from fine ores, blast furnace dust and the like. Like. Using a mixture of sulphite waste liquor and inorganic substances as a binder |
US2036642A (en) * | 1933-05-08 | 1936-04-07 | Pukli Frank Martin | Solid fuel briquette and method of making the same |
GB1547419A (en) * | 1975-10-30 | 1979-06-20 | Mcdowell Wellman Eng Co | Method of producing pelletized fixed sulphur fuel and product |
IT1066137B (en) * | 1976-08-04 | 1985-03-04 | Centro Speriment Metallurg | SEMICOKE BRIQUETTES HARDENING PROCESS |
JPS57137388A (en) * | 1981-02-17 | 1982-08-24 | Matsushita Electric Ind Co Ltd | Solid fuel |
US4515601A (en) * | 1982-05-03 | 1985-05-07 | Charters John E | Carbonaceous briquette |
DE3727464A1 (en) * | 1987-08-18 | 1989-03-02 | Applied Ind Materials | Process and system for the production of fuel briquettes |
-
1988
- 1988-12-23 DE DE3843449A patent/DE3843449A1/en active Granted
-
1989
- 1989-10-13 EP EP89119047A patent/EP0374402B1/en not_active Expired - Lifetime
- 1989-10-13 AT AT89119047T patent/ATE85641T1/en not_active IP Right Cessation
- 1989-10-13 ES ES198989119047T patent/ES2039056T3/en not_active Expired - Lifetime
- 1989-10-13 DE DE8989119047T patent/DE58903530D1/en not_active Expired - Fee Related
- 1989-11-07 IE IE358189A patent/IE63118B1/en not_active IP Right Cessation
- 1989-12-14 JP JP1322789A patent/JPH0668110B2/en not_active Expired - Lifetime
- 1989-12-18 CA CA002005833A patent/CA2005833A1/en not_active Abandoned
- 1989-12-19 TR TR90/0005A patent/TR25967A/en unknown
- 1989-12-20 PT PT92629A patent/PT92629B/en not_active IP Right Cessation
- 1989-12-22 DK DK658689A patent/DK658689A/en not_active Application Discontinuation
-
1993
- 1993-03-31 GR GR930400699T patent/GR3007517T3/el unknown
Cited By (1)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
CN104973880A (en) * | 2015-06-25 | 2015-10-14 | 云南永昌硅业股份有限公司 | Carbonaceous pellet and preparation method thereof |
Also Published As
Publication number | Publication date |
---|---|
JPH03121194A (en) | 1991-05-23 |
EP0374402A3 (en) | 1990-08-22 |
JPH0668110B2 (en) | 1994-08-31 |
DE3843449A1 (en) | 1990-06-28 |
PT92629B (en) | 1995-09-12 |
GR3007517T3 (en) | 1993-08-31 |
DK658689A (en) | 1990-06-24 |
PT92629A (en) | 1990-06-29 |
EP0374402A2 (en) | 1990-06-27 |
IE63118B1 (en) | 1995-03-22 |
ATE85641T1 (en) | 1993-02-15 |
DE58903530D1 (en) | 1993-03-25 |
IE893581L (en) | 1990-06-23 |
TR25967A (en) | 1993-11-01 |
DK658689D0 (en) | 1989-12-22 |
ES2039056T3 (en) | 1993-08-16 |
EP0374402B1 (en) | 1993-02-10 |
DE3843449C2 (en) | 1991-05-23 |
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