11/11/2011

AII1LSn A8nISnLk
2009ch10770
1L8M
AL8
Kinetics anu Nechanism :catalytic
steam iefoiming of Bio oil

AbsLracL
1 Tstiact
2 LroducLlo
aL 8orml LlLraLur
4 klLlc SLud
3 uaLa aalsls
6 AssssmL o modl compoud
7 Mchalsm o 8lo oll corslo
8 Cocluslo
9 ulscusslo ad susLlo

Kinetics anu Nechanism :catalytic steam
iefoiming of Bio oil
Abstract
1h sLam rorml o Lh modl compouds was lsLlaLd l Lh LmpraLur ra 630930 C
or L d ad 8h supporLd o alumla ad a crlazlrcola sampl 1h modl compouds usd wr
acLlc acld phol acLo ad Lhaol 1h aLur o Lh supporL appard Lo pla a slllcaL rol l
Lh acLllL o Lhs caLalsLs 1h us o crlazlrcola a rdo mld old lad Lo hlhr P
2
llds as
compard Lo Lh cas o Lh alumlasupporLd caLalsLs A blooll obLald rom Lh asL prolsls o
bch wood was rormd ad a slmllar llds o hdro ad C

as Lh modl compouds or
Lh crlazlrcola supporLd caLalsLs 1h us o auLoLhrmal codlLlos (l addlLlo o molcular
o Lo Lh d) rducd Lh LL o carbo ormaLlo buL also ld Lo a lmporLaL loss l Lrms
o hdro lld 1h caLalsL also appard Lo dacLlaL asLr l Lh prsc o
2
nrLhlss lL
ls cocludd LhaL Lh coLluous rorml o prolsls blooll ls aslbl or Lhs caLalsLs 1h oal ls
Lo ldLl lclL caLalsLs buL also Lo lucldaL racLlo mchalsms ad klLlcs
ZtroductioZ
CurrLl Lhr ls raL lLrsL l Lh us o hdro as ul spclall l hlhlclc ssLms such
as ul clls ad lLs appllcaLlo l Lh LrasporLaLlo scLor 1h mal procsss or hdro
producLlo ar caLalLlc sLam rorml o aLural as ad oll drld aphLha ad parLlal oldaLlo o
ha olls 8lomass has b proposd as a alLraLl bcaus Lhls rwabl rsourc dos oL
coLrlbuL Lo a L lcras l aLmosphrlc C2







1h blooll ca ha a r dslL L Llms larr Lha blomass ad ls Lhror sulLabl or
LrasporL varlous Lcholols such as blomass caLalLlc prolsls blomass sLam asllcaLlo (lcludl
asllcaLlo udr suprcrlLlcal codlLlos) ad sLam rorml o llqulds drld rom blomass such
as blooll Labl olls or bloLhaol ar currLl bl lsLlaLd Lo produc hdro CaLalLlc
sLam rorml o prolsls olls has b plord rcLl 1hls procss bls wlLh a asL prolsls o
blomass Lo produc blooll whlch (lLhr as a whol or usl spcllc racLlos) ca b corLd Lo
hdro la caLalLlc sLam rorml ollowd l cssar b a shlL corslo sLp
1h blooll coLals umrous oaLd oralc compouds aclds alcohols aldhds kLos
uras subsLlLuLd phollcs ad compl oaLs drld rom blomass carbohdraLs ad lll
SLam rorml o Lh slmpl moomrlc maLrlals ls Lhrmodamlcall ad chmlcall aslbl
SLam rorml o Lh Llr blooll ls also Lhrmodamlcall aslbl 8looll ls a mlLur o
oaLs ordr Lo prold a kowld bas or Lh dsl o acLl ad sLabl caLalsLs or sLam
rorml o blooll sLudls ha b llLlaLd wlLh modl oaLs AcLlc acld (PAc) has b
chos as a modl compoud l Lhls sLud bcaus lL ls a ma[or compoL o blooll (up Lo 2 wL) L
ls kow LhaL sLam rorml ad waLr as shlL racLlo (C + P2 _ C2 + P2) occur slmulLaousl
ad Lh orall sLolchlomLr ls rprsLd
CPCP + 2P2 2C2 + 4P2
Compard wlLh dlrcL blomass sLam asllcaLlosom adaLas o caLalLlc sLam rorml o
prolsls olls ha b rporLd such adaLa ls Lh poLLlal producLlo ad rcor o
aluabl coproducLs rom blooll LhaL could lmpro Lh coom o Lh Llr procss lor lsLac
Lh llldrld ollomrrlch racLlo ca b usd as a rplacmL or phol l phol
ormaldhd rsls or corLd lLo aromaLlc hdrocarbos ad Lhrs or us as hlhocLa
asollbldl compoLs whras Lh aquous racLlo ls sLam rormd or hdro
producLlo AoLhr adaLa ls Lh us o a lmplmLaLlo sLraL basd o small Lo mdlum
slzd rloal asL prolsls ulLs producl blooll LhaL ca b LrasporLd Lo a cLral rorml ulL
1hls sLraL would achl hdro producLlo aL a compLlLl cosL
Cxygenate keform|ng L|terature
LlLraLur o Lh sLam rorml o oaLs alls wlLhl Lwo caLorls rorml slmpl alcohols
such as mLhaol ad Lhaol ad rorml oaLd aromaLlcs l crsols A lar bod o
lormaLlo has Lhus b accumulaLd o Lh caLalLlc rorml o mLhaol 1h comparlso wlLh
mLha ls Lhus approprlaL MLha rqulrs hlh LmpraLurs (300C) Lo b cLll sLam
rormd 1h ollowl mchalsm has b proposd (8oss) (1) mLha or a oLhr hdrocarbo
ls dlssoclaLll adsorbd o Lh mLal slLs (2) P2 ls also dlssoclaLll adsorbd o Lh Al slLs
hdrolaLl Lh suracs () mLalcaLalzd dhdroaLlo Laks plac craLl adsorbd
hdrocarbodrld ramLs (4) Lh P surac roups mlraL Lo Lh mLal slLs acLlaLd b Lh
LmpraLur ad Lh Luall orm lLrmdlaLs ladl Lo carbo olds
MLhaol ca b sLam rormd aL much lowr LmpraLurs (00 C) Lha mLha A
arlL o caLalsLs ar capabl o carrl ouL Lh corslo lcludl rducd nlbasd
prparaLlos rducd Cu/Z shlL prparaLlosCu/Sl2 ad d/Sl2 Cu/Zr2 ad d/Z
1wo mal mchalsms ha b proposd (!la)
(1) Lh dcomposlLlo shlL mchalsm whr Lh chmlsorbd mLhaol ls LoLall
dhdroaLd o Lh mLal surac prlor Lo orml C (Lh shlL racLlo Lh procds
wlLh Lh adsorbd waLrdrld spcls)
(2) Lh ormaL mchalsm basd o Lh ormaLlo o mLhl ormaL sLr o Lh caLalsL
surac bLw Lwo adsorbd spcls PC ad PC 1h sLr ls hdrolzd Lo mLhaol
ad ormlc acld 1h laLLr dcomposs dlrcLl Lo C2 ad P2 wlLh 100 slcLllL l o C
ls ormd
CaLalasL ampl Cu alo shows r hlh slcLllL Loward acLaldhd (88 aL 230 C)
whras Lh prsc o a supporL (Al2 Sl2 Zr2 or Z) markdl acLs Lhls slcLllL
ad producs sral oLhr lLrmdlaLs aL slllcaL cocLraLlos Carcla ad Labord
(1991) coducLd a Lhrmodamlc sLud o Lh rorml o Lhaol Lo P2 1h cocludd
LhaL P2 producLlo rqulrs LmpraLurs hlhr Lha Lhos dd or Lh rorml o
mLhaol ad LhaL sLamLoLhaol raLlos hlhr Lha 10 (qulalL sLamLocarbo raLlos
hlhr Lha 3) wr rqulrd Lo prL carbo ormaLlo SLam rorml o oaLd
aromaLlcs has b dlrcLd Loward Lh dalklaLlo o crsol 1h racLlo procds aL
LmpraLurs o 400300 C ad sLamLocarbo raLlos o 6 usl d 8h or nl o alumla
slllcaor chromlaalumla uurl sLam rorml o oaLd aromaLlcs dhdrolaLlo
procds aL a slllcaL raL Lo produc aromaLlc spcls o Lh caLalsL surac LhaL ar
subsquLl sLam rormd 1h blooll composlLlos mak lL clar LhaL challs l
caLalLlc sLam rorml wlll b llkd Lo Lh ablllL Lo hadl Lh prolLlc lll# racLlo
ad Lh carbohdraLdrld racLlo acLlc acld aldhds alcohols (suars ad
ahdrosuars)ad ollomrs L ls llkl LhaL Lh ollomrlc ramLs lLhr lll or
carbohdraLdrld oc codsd as blooll caoL b rolaLlllzd wlLhouL slllcaL
char ormaLlo
1hus Lhs opLlos ar posslbl Cl Lh hLrolL o Lh aquous racLlo nl basd
caLalsLs opraLl l Lh 700800 C ra accordl Lo Lh llLraLur rlwd abo souhL
Lo b abl Lo carr ouL Lh sLam rorml corslo
ComplL sLam rorml ls dscrlbd b Lh ollowl racLlo

C

+ (2 -)P
2
C
2
+ 2 + /2 - P
2

noL LhaL Lh lld ls also llucd b Lh waLr as shlL racLlo dpdl o Lh codlLlos o Lh
racLlos

C + P
2
C
2
+ P
2
uu Lo Lh hlh LmpraLur o Lh racLlo lL ls llkl LhaL parLlal Lhrmal dcomposlLlo ad Lh
8oudouard racLlo ca occur slmulLaousl

C

+ ass (P
2
P
2
C C
2
CP
4
) + cok
(4)
2C C
2
+ C
kesu|ts of Cata|yt|c Steam keform|ng

A8AML1L8 8u10 8un 11 8un 12 8un 1
CaLalsL nAlLa(12) nlAlLa(12) nlAlLa(8) nlAlLa(8)
1mp(C) 630 630 630 630
S/C 338 338 338 338
CaLalsL wlhL() 129 078 129 080
W/ma 12 19 02 189
Llquld dl
raL(/ml)
180 176 186 183
1lm 36 336 64 331
?lld1oLal
as/AcLlc acld
09614 10911 11670 1179
Cas(/ acLlc
acld) P2
0077 0060 0090 0078
Co 0296 01 029 016
Co2 0484 0347 0631 0617
CP4 0097 013 0126 0131
1h addlLlo o laLhaum l Lh caLalsL composlLlo dlmllshs Lh P2 lld obLald wlLh Lh nlAl
caLalsL
iZWtic Study:
cata|yst preparat|on: 1h L d 8h supporLd o alumla ad crla/zlrcola caLalsLs wr
prpard b Lh lclplL wLss mLhod usl LunuA dunuA ad 8hlLraL as Lh mLal
prcursors rspcLll 1h alumla was prcalcld aL 830 C or 13 h prlor Lo lmpraLlo a
Lplcal lmpraLlo procdur Lh mLal prcursor was dlssold l a mllmum amouL o waLr (l
[usL ouh Lo wL all Lh supporL) ad addd Lo Lh supporL 1h Lhlck slurr obLald was kpL or 1 h
aL room LmpraLur bor drl orlhL aL 100 C 1h caLalsLs wr lall calcld aL 830 C or
2 h


A mlLur mad up o Lh oaL compoud ad waLr l Lh approprlaL molar raLlo was
lLroducd Lo Lh prhaLr ssLm usl srls o arlous slzs ad a srl pump 1h blooll usd
radll polmrlsd abo 80 C ad so car had Lo b Lak so LhaL lL rmald as cool as posslbl uLll
coLacLd wlLh Lh hoL sLam rorml caLalsL 1h racLaLs wr lLroducd lLo Lh racLor b Lwo
sparaL srl pump assmblls usl a 10 cm

srl or Lh blooll ad a 23 cm

srl or waLr
1h dlamLr o Lh dl usd was such LhaL blooll ad waLr droplLs wr ormd ad droppd
oLo Lh caLalsL bd b ralL r ca 3 s 1h Llp o Lh waLr srl was locaLd dlrcLl abo
LhaL o Lh dl o Lh blooll srl
ata acqu|s|t|on1h racLor luL was passd Lhrouh a lc Lrap Lo rmo codsabl producL
ad racLaL apours 1h composlLlo o Lh ass aLr Lh Lrap was dLrmld b a oll as
chromaLoraph (CC rklLlmr AuLossLm xL) qulppd wlLh a Lhrmal coducLllL dLcLor (1Cu)
Lo dLrml Lh cocLraLlos o P
2
C
2

2
n
2
CP
4
ad C Pdro was dLcLd usl lLro
as a rrc as whras hllum was usd as a rrc or all oLhr ass
ata aZalysis
1h 1Cu slals o asphas producLs wr corLd Lo molar proporLlos usl callbraLlo curs
1h umbr o mols o producLs ormd pr ulL o Llm was drld rom Lh molar proporLlos wlLh
rspcL Lo LhaL o Lh lLral sLadard n
2
ad Lh kow n
2
low raL 1h acLllL o dlrL caLalsLs
or Lh rorml racLlo was compard l Lrms o P
2
C C
2
ad CP
4
llds lor Lh asous
producLs oLhr Lha hdro Lh lld was dld as Lh umbr o mols o as ormd pr mol o
carbo d 1h dlrc bLw 100 ad Lh sum o Lh C C
2
ad CP
4
llds rlaLd Lo Lh
carbo l Lh producLs LhaL wr oL aalsd b Lh CC ( Lha ad hlhr hdrocarbos)
carboacous maLrlals dposlLd l Lh racLor ad Lh ucorLd racLaL lLsl 1hror our
acLual carbo balac corrspodd Lo 100 - (C + C
2
+ CP
4
) lld
1h hdro lld dld as Lh raLlo o Lh cocLraLlo o P
2
l Lh acLual luL as Lo Lh
LhorLlcal amouL o hdro LhaL ca b obLald wh complL rorml Lo C
2
ad P
2
occurs

addlLlo Lwo oLhr paramLrs wr usd Lo ldlcaL Lh llLlal proporLlo o waLr ad o Lh
sLam Lo carbo raLlo (S/C) ad Lh o Lo carbo raLlo (/C)
)

noL LhaL Lh sLam Lo carbo raLlo (S/C) rporLd hr dld Lak lLo accouL Lh prsc o waLr l
Lh blooll whlch was abouL 29 wL 1h o Lo carbo raLlo o Lh blooll was 034 wh o
molcular o was addd (Lh o prsL l Lh addd waLr ls oL Lak l accouL Lo calculaL
/C)
lor Lh modl compoud Lh as hourl spac loclL (CPSv) ls dld

Lh cas o Lh blooll Lh composlLlo o whlch ls r compl a as qulalL hourl spac
loclL (CPSv) dld as Lh olumLrlc as low LhaL would b obsrd l all Lh carbos l Lh
d wr l Lh orm o mLha pr ulL olum o caLalsL
noL all olums wr calculaLd aL 1 aLm ad 23 C
Table 1. Activity of various catalysts for steam reforming of model compounds in terms of COx yield
CataIyst CO + CO
2
yieId (%)

Acetic acid Acetone EthanoI PhenoI
1% Pt-Al
2
O
3
+ + ~ ++
1% Rh-Al
2
O
3
++ ++ ++ ++
1% Pd-Al
2
O
3
+ ++ ++ +
1% Pt-CeZrO
2
+ ++ + ++
CataIyst CO + CO
2
yieId (%)

Acetic acid Acetone EthanoI PhenoI
1% Rh-CeZrO
2
+ ++ ++ ++
1% Pd-CeZrO
2
0 ++ 0 ++
(~) 2040% ; (0) 4060%; (+) 6080%; (++) >80%.
Table 2. Activity of various catalysts for steam reforming of model compounds in terms of hydrogen yield
CataIyst Hydrogen yieId (%)

Acetic acid Acetone EthanoI PhenoI
1% Pt-Al
2
O
3
~ ~ -- ++
1% Rh-Al
2
O
3
0 + + ++
1% Pd-Al
2
O
3
~ ~ 0 0
1% Pt-CeZrO
2
+ + 0 ++
1% Rh-CeZrO
2
+ + + ++
1% Pd-CeZrO
2
0 0 ~ ++
(- -) <20% ; (~) 2040%; (0) 4060%; (+) 6080%; (++) >80%.
AssWssmWZt of modWl compouZds
1h acLllL o Lh caLalsLs or Lh rorml o Lh arlous modl compouds usd l Lh prsL sLud
ls smbollcall summarlsd l Lh 1abl1 ad 1abl2 1h alm o Lh prsL work o Lh sLam
rorml o modl compouds was Lo ldLl Lh mosL rsaLll sLam rorml caLalsL amo a
llmlLd sL o sampls LhaL wr aallabl ad oL Lo dLrml Lh hlhsL lLrlslc racLlo raL or
ach mLal Lh laLLr cas a carul aalsls o Lh mLal dlsprslo bor ad spclall aLr
racLlo would b rqulrd 1h P
2
lld obsrd l Lh absc o Lh obl mLalbasd maLrlal was
alwas lowr Lha 10 sLrssl Lh ssLlal rol o Lhs caLalsLs or a lclL producLlo o
hdro 1h sLam rorml o Lh modl compouds rald LhaL Lh 8h ad L caLalsLs wr l
ral Lh mosL acLl ad Lh d caLalsLs wr Lh lasL acLl or Lh producLlo o hdro l Lh
prsL cas L ad 8hbasd caLalsLs ha oL b rporLd Lo dlspla a hlhr lLrlslc caLalLlc
acLllL Lha d or nl couLrparLs or a umbr o sLam rorml racLlos 1h lowr acLllL o Lh
dbasd maLrlals obsrd l Lh prsL cas could ha also b rlaLd Lo a lowr mLal
dlsprslo whLhr llLlall or udr racLlo codlLlos (oL masurd) 1h acLllL ad slcLllL
wr also llucd b Lh aLur o Lh supporL mplod l Lh crlazlrcola maLrlals dlsplal
a hlhr acLllL Lha Lh alumla sampls SupporLs such as zlrcola ha b proposd Lo aour Lh
acLlaLlo o sLam 1h Lplcal ordr o acLllL wlLh rspcL Lo P
2
producLlo was1 8hCZr
2
1
LCZr
2
1 8hAl
2

1 dCZr
2
1 LAl
2

1 dAl
2

Steam reforming of the bio-oil
L ls llkl LhaL Lh llLlal molculs orml Lh blooll wr ull corLd ( b polmrlsl
crackl cokl alo wlLh Lh sLam rorml) Lo som producL abo a LmpraLur LhaL was lowr
Lha LhaL mplod l Lh currL work Powr Lh polL o Lh prsL work was Lo sLud C

+

P
2
llds ad oL Lh corslo o Lh blooll as such 1h calculaLlos o Lh llds l Lhls cas wr
mad usl Lh ara composlLlo o Lh blooll as show l Lh ollowl quaLlo
CP
12

034
+ 146P
2
2C
2
+ 212P
2
Cosldrl LhaL carbo dposlLlo ls llkl Lo occur durl Lh sLam rorml o Lh blooll Lh
prlmLs wr carrld ouL usl a sLam Lo carbo raLlo hlhr Lha sLolchlomLr l S/C 108
lsLad o 146 Slc Lh dllr o Lh blooll was oL sLrlcLl coLluous (l droplLs wr d Lo Lh
racLor r 3 s o ara) Lh racLor luL showd som prlodlc arlaLlos wlLh Llm 1h
LmpraLur masurd aL Lh boLLom o Lh caLalsL bd Lplcall arld b 0 C du Lo Lh sLro
doLhrmlc aLur o Lh rorml racLlo 1hs cLs ca plal Lh lucLuaLlo o Lh C

ad
P
2
llds obsrd or Llm
WcbaZism of bio-oil coZbWrsioZ:

lrom Lh daLa lL L ad 8h sm Lo b Lh mosL acLl mLals whll crlazlrcola mld olds ld Lo
bLLrprorml caLalsLs Lha alumla 1h prcls dLalls o Lh corslo paLhwa o Lh blooll Lo
C

ad hdro ls mosL llkl compl l parLlcular du Lo Lh arlL o Lh chmlcal compouds

prsL l Lh blooll L ls also llkl LhaL dlrL mchalsms would opraL dpdl o Lh aLur
o Lh mLal ad LhaL o Lh supporL
lw mchalsms ha b proposd or Lh S8 o oaLs ad o o Lhm ls a blucLloal
mchalsm L has b proposd or Lh S8 o acLlc buL slmllar mchalsms mlhL occur or oLhr
oaLs 1h mal lda ls LhaL Lh sLam ad acLlc acld dlssoclaLll adsorp o Lh supporL ad
mLal rspcLll C spcls ca dsorp whll CP spcls ca racL wlLh Pspcls aL Lh mLal
supporL lLrac orml P2 ad C or combl orml cok 1h lcrasd acLllL obsrd or Lh
crlazlrcola could posslbl b assoclaLd wlLh Lh rdo proprLls o Lhls sampl whlch would op
a addlLloal racLlo paLhwa as compard Lo Lh sL o racLlos occurrl o Lh alumlabasd




maLrlals L has b proposd LhaL Lh rdo old could b lold l Lh acLlaLlo o sLam L is
possible that the metal would be involved in the activation of the hydrocarbon and oxygenated molecules, the
fragments of which would then react with lattice oxygen at the interface of the metal and the redox support.
nfIuence of the temperature

Shows LhaL Lh C

lld lcrass wlLh hlhr LmpraLurs 1h LmpraLur also llucs Lh raLlo

o Lh ass ormd parLlcular Lh C
2
/C raLlo dcrasd wh Lh LmpraLur lcrasd
probabl l rlaLlo Lo Lh waLr as shlL (WCS) racLlo
nfIuence of the inIet oxygen partiaI pressure


Lh cas o Lh sLam rorml o Lhaol Lh addlLlo o
2
had alrad prod blclal or Lh
corslo Lo C

ad o slllcaL rducLlo o Lh hdro lld was rporLd A dLrlmLal cL

o o was acLuall obsrd as Lh hdro lld was srl dcrasd wlLh lcrasl
cocLraLlo o
2
l Lh d dsplL Lh lmpromL l Lrms o llmlLl cok dposlLlo.


nfIuence of the cataIyst


LprlmLs rald LhaL Lh alumlasupporLd caLalsLs wr lss acLl Lha Lhos
supporLd o crlazlrcola boLh l Lrm o C

lld ad hdro producLlo

oZclusioZs
CaLalLlc sLam rorml o blooll ls a promlsl procss or hdro producLlo rom blomass1h
sLam rorml o a srls o modl compouds slmllar Lo Lhos oud l blooll wr sLudld or a
sL o obl mLalbasd caLalsLs AcLlc acld acLo Lhaol ad phol could b lclLl
rormd Lo hdro or a obl caLalsL 8asd o Lh hdro lld Lh Lplcal ordr o acLllL
was 1 8hCZr
2
1 LCZr
2
1 8hAl
2

1 dCZr
2
1 LAl
2

1 dAl
2

1h
crlazlrcola supporLs wr loball much mor lclL Lha Lh alumla A blooll obLald rom Lh
asL prolsls o bch wood was rormd ad a slmllar llds o hdro ad C

as Lh modl
compouds or Lh crlazlrcola supporLd caLalsLs 1h us o auLoLhrmal codlLlos (l addlLlo
o molcular o Lo Lh d) rducd Lh LL o carbo ormaLlo buL also ld Lo a lmporLaL
loss l Lrms o hdro lld 1h caLalsL also appard Lo dacLlaL asLr l Lh prsc o
2

nrLhlss lL ls cocludd LhaL Lh coLluous rorml o prolsls blooll ls aslbl or Lhs
caLalsLs
iscussioZ aZd suggWstioZ:
1 CL/ar blomass aallabl or r ad uls producLlo rprsLs poLLlal or 100 ML/ar
hdro LhaL could suppl 00 mllllo ul cll hlcls roducl hdro rom domsLlc rsourcs
such as blomass ca rduc dpdc o pLrolum ad lld lrLuall zro rhous as
mlsslos P2 producLlo rom blomass would compL wlLh wlLh blo ul ad CP producLlo
ral as baslc dsLock aallablllL ls llmlLd producLlo rom blomass wlll oL blL rom
coomls o sal CosLs ar pcLd Lo b hlh wlLh compard Lo coal asllcaLlo or as rorml as
o commrclal plaL A radual buL slow dacLlaLlo was obsrd corrspodl Lo a dcras o ca
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. Ramrez-Salgado and A. Estrada-Martnez. J. Power Sources, 129 (2004)
M.A. Pea, .L.G. Gmez and .L.G. Fierro. 55. Cata. : Gen., 144 (1996)
M. Marquevich, G.W. Sonneman, F. Castells and D. Montan. Green Chem., 4 (2002)
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L ChorL ad S Czrlk Notote 418 (2002) p 928
v llrro v klouz Akdlm ad C MlrodaLos otol 1oJo 7S (2002) p 141
An laLslkosLas u kodarlds ad xL vrklos otol 1oJo 7S (2002) p 143
S Caallaro etq loels 14 (2000) p 1193