Synthesis of acrylates and Methacrylates from Coal-Derived Syngas

27 Pages·1997·0.57 MB·English

by  Makarand Gogate

DEVIRED- L MASOOERCTFALYRCA HSDTENETAMA LS YIFRSOCEAHTNYS
SAGNYS
7 79L99A91 C 1 /RIY/-1ONL10FHR3/CE/1ET30TR0AUQ
YE V SI.E PJM,SAEJT A DG.NORAGRA K:ASMROHTUA
HRP E EDL.SGR LROR A,EJE.HOBDCZLIORC
D LI.AONRHECG
LM.EASUTMAS
REPORT ISSUE DATE: 05/12/1997
56049CP49-22CA-ED
RESEARCH TRIANGLE INSTITUTE
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P. O. BOX 12194
RTP, NC 27709-2194
YNAPM OLCACIME HNCAMTSAE
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DISCLAIMER
se tdd yae eyc tr ftbneSonoi eh sant gtd nU nkaefosurr opaoo ans cwtpascre aaorswppiehrT
rie hfy tonr ao,nfoere hytcne gy anr aotnnemnrev osGeta tdSeti ne Uhrtehti e.NtnemnrevoG
ytilibisnopse rr oytilibai llage lyn asemuss ar o,deilpm ir osserpx e,ytnarra wyn aseka m,seeyolpme
sse c ,ortrocpud o,rsputara p,pnaoitamro fsyfnsnoieanlu f ,erssosuenetelp m,oyccaru cerchoatf
ontier eehcneref e.Rsthg idren wyoletavi repgnirf nt iodnlu oe wss uttia hsttneserp er,rodesolcsid
r,orerutcafun a,mkrameda r,tem aenda ryetbcivr er,sosseco r,ptcudo rlpaicremm occifice pysna
ycne gy anrtaonemnrev osGeta tdSeti ne Uhygtbnirov ar,fonoitadnemmoc e,rtnemesrod nseti
tcelf ererota tyslirassec et noonndier edhesserp xseroht ufsaonoini pd onsawe ie vh.Tfoereht
.foer eyhct n teyrngnoeaamnre vsoeGt adteS t eiefsnhooUtht
i
ABSTRACT
e ryalevitcell olcethc edB n,aynapm olCacime hnCamts a,E)IT Re(tutits neIlgnai rhTcraeseR
devired-la omco r)fAM Me(talyrcaht elmyht e fmsoisehtn yes hrt osfseco rlpev ogannipoleved
ygolonh cyegTr elnaEre d,eyFgr etfnnoEemtra p.e SD e.mhU ottrcfar tr neao dc,nsuagnys
h tniowitasned n so,tceitanoi psf oioarspeht nsfytossis nsoscec oprepts-ee rsh it.hrTetneC
ecudo r opltonaht ehmt i)wAA Md(i ccailyrcaht egmnitlus e frnooitacifiret sde n,aedyhedlamrof
k rsotwsyla ttoanMcatlu s ee.hrpT estisseht neytsanoip o edrnhepotsu c sonafahmt s.aAEMM
071 (snoitidno cereve ssse lhcu mt ayltneiciffe Estsylat a iclNanoitnevn oec hnta h)tm t 0ad3 nCa
(270 Eta hstwo hhsci hswisyla ntas oecvisnet x nedaemrofr esp alhethc e.B)m t0a 8d1 nCa
eehctud osoretpigolonh creet hht toeivwititep mpso eicstisseht neytsanoip osr'pnamtsaE
pets-eer hltethceB-namtsaE-I Te Rhdterapm oocs leav alhethc ed Bnnaamts a.Eedirdyhna
lonahtem etuor ot evif rehto ssecorp setuor ot .AMM ehT stluser wohs taht eht tcudorpAMM
eovtititep mts ositcoccud osr i pdh,nttan a AlrMpaMey / rb ,0olab5fMl2/ ¢dt2ea5cud onerabpc
. , n dpIon neTdiIeotRnthcsaatelsyn oebnr yastpc e posto,ersutAcp eoMx rcrMeleolhratpo
OiS/ b,Nstsylat aecdi xloat eymranr ePt-iS -eVlba tds neavit cdaepolev eedv anhamtsaE d,na
2
OiS/aT .edyhedlamr ohft idwi ccainoipo r rpeodirdyh ncainoipo r fpnooitasnedn orc osftsylat ac
2
noitasned n,osceitrep oerspab-d itcsayla t eaghcnt onmoaitaler rl oedc veaotnartsno m seIadThR
I Te Rhdte seuv alhethc ed Bnnaamts a.Eecnamrofr etpsylat amcret-gn od ln,adle inyoitcaer
OiS/ btNnecr e 0fpas2otlus elratnemirepxe A A,Msnoisrevn otcnatca efsromr en,titsylat ac
2
gnicnah n nesoesuc ohfcraes etrnerr u.Csisyla ncaimono creie hrt o,fdle iAy AdM n,aseitivitceles
dnnoaitaler ryotcrep oerspab-d i ecgfhanotidnatsre drneu t, tsaedbl enioyitc aneoritasned neohct
.emitefi ltsylata ceh tgnicnahne
ii
TABLE OF CONTENTS
Page
remialcsiD . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . I
tcartsbA . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . ii
selb adT nsaerug i fFtosiL . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . vi
smynorc Af otsiL . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . v
yrammu SevitucexE . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . iv
Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1
noissucs idD nsatluseR . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3
)leth c dennBaamts asEi(seht neytSanoip ok.rs1PaT . . . . . . . . . . . . . . . . . . . . . . . . 3
)I TsRi(syla tnaoCitasned nk.os2CaT . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 5
) n saI emT ditRrnds( oaua kttEysc Sraa.rTe3uRlS . . . . . . . . . . . . . . . . . . . . . . . . 10
)na m IntdTosnRiaa(tEau lkac vokEt ss .adE4TeMeDF . . . . . . . . . . . . . . . . . . . . 12
snoisulcnoC . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 17
1. Status . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 17
2. Forecast . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 18
secnerefeR . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 19
iii
LIST OF FIGURES
Number Page
1 seco rH pCe AhfctoitamehcS s . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1
2 C ’rutcafun aAm MrM osfeigolonhc entoitalynobrac- e . . . . . . . . . . . . . . . . . . . . . . . 2
2
3 dAeMsMab-HOeM/ rpPeOtHs-e elrehtthceB-namtsaE-ITR
de eefdyhedlamr olfanret xheti ws(secorp ) . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3
4 %nI0oO1sR(ira pe mutolccau vd,osrepsse cAoMrMp ) . . . . . . . . . . . . . . . . . . . . . 4
5 dAeMsMab-HOeM/ rpPeOtHs-e elrehtthceB-namtsaE-ITR
du tystivitisnes-ssecorp y . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 5
6 dyhedlamr odf ndai ccainoipo rrp omfsinahc eemvitatneserpeR e . . . . . . . . . . . . . . 6
7 d,niaS -%,a08T1.2:0 1P:- 1i kSnc -oeyVhtcivi tmcraet-gnoL
tsylat aicS- b%N01 s . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 7
8 dyhedlamr o ffeocru oes h stnailamr orf omfets yrsotca edreb-dexiF e . . . . . . . . . . . 9
9 OiS/ b% N0h1t itws eyttivit cmaret-gn ofslotluseR dlei yAAM-tsylata c s . . . . . . . 10
2
10 OiS/ b% N0h1t itws eyttivit cmaret-gn ofslotluseR AAM-tsylat ac
2
dn aOeCtar s . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 11
11 oitatnemurts nnioitc edseef—mets yrsotca eyrrru lnsamtsaE-ITR n . . . . . . . . . . . . 12
12 oitatnemurt snnoiit ctecsudorp—met sryostc ayerrr unlasmtsaE-ITR n . . . . . . . . . . 13
13 arga iwdolf—mets yrsotca eyrrru lnsamtsaE-ITR m . . . . . . . . . . . . . . . . . . . . . . . . 13
14 tcu d)oDrIpF /rCoGt(c entoeidtaz ienmoailf/yhpargotam osrahGc
981 0n1 urrotca eyrrru lmso rsfisylana 6 . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 14
15 setuo Rs(isehtn yA sMr Mosfyawht anpoitcaeR (cid:226) d na ª denote the
sisyla nfafoeda rrt osfyawht adpetceles ) . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 15
16 eet du–yohRedlam rloafnretxe/kcotsd erePfOH/kcotsd e H eeO:fse3aMC ª . . . . 16
17 noi tH aO –deeiMtx/uokocRo trsPdO eeeeMsf/ ak:Cc7o 1tEsMdDeef (cid:226) . . . . . . . 17
LIST OF TABLES
Number Page
1 noitca enRoitasnedn or Cosftsylat aiCS-bN s . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 6
2 tsylat aaCcil i nSmouibo i fNsonoitca enRoitasnednoC s . . . . . . . . . . . . . . . . . . . . . 8
3 eitivitcele Slacimeh Cdn asnoisrevnoC s . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 8
4 kcotsde eeFdyhedlamr ofnFoosirapmoC s . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 9
5 soMetMt ueolRbis stfosoPiL A . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 15
vi
LIST OF ACRONYMS
HCA nirdyhona yecnotecA
NEPSA gnireenig nseseco rrp omfets ydsecnavdA
KED enot elkyhteiD
EMD reht elyhtemiD
ACSE sisyla nlaacime hrc oyfpocsortce pnsortcelE
CG hpargot asmaoGrhc
DIF/CG rotcet endoitazin oeimalf/yhpargotamor hscaG
SM/CG yrtemortc espssam/yhpargotamo rshacG
OHCH edyhedlamroF
HTHP erusserp-h g,iehrutarepmet-hgiH
CGM lacimeh Csa GihsibustiM
AAM dic acilyrcahteM
AMM etalyrcahte mlyhteM
PM etanoipo rlpyhteM
MTBE reh tleytub-tr eltyhteM
USCN ytisrevi neUta taSnilor ahCtroN
AP di ccainoiporP
AAP edirdyh ncainoiporP
IOR tnemtsev nnnioruteR
SRI etu thict rsdanreIosfenRatS
SS lee tssselniatS
SEM epocsorc inmortce lgeninnacS
RTI etutits neIlgnai rhTcraeseR
STP derraudtnaarteSp mdentaerusserp
TCD rotce tyetdivitcud nloacmrehT
TEM epocsorc inmortce lneoitisnarT
DRX noitcarff iydar-X
FRX ecnecserou lyfar-X
v
EXECUTIVE SUMMARY
re v.Osevitavir eedtanoipo rfnpooitaren ee g hnktir olwatnemirep xs etdietelpm os canhamtsaE
e hr tolfed ocmimono ce ehgtnipolev eoedtm is ttdietov eydlirami rs panhamts a,Eretra utqs aelht
-ee reefhuh otlttacvud oedrheptrap msnoaachmt s,alEe dcoimmon o erc.hoestFsec olrlparevo
pets lonahtem etuor ot evif rehto ssecorp setuor ot ,AMM dna eht stluser wohs taht rof-ITR
evititepm ostcina lrpaey/b l0 rM 5aob2fl/¢ 2fe5oul aA vMtMcudo r,petu olrethceB-namtsaE
o ssnlaaahmt s.anEoitalynob reancyp otrppe c, sxAoeeMtt Musosrec or re h phefchthoatoteiw
elgnai rhTcraes e.Rhcraes elratnemirep xse t fitor asaspatrop enroitnev nyi elkarev edsepoleved
fnooitasnedn or cosftsylat aecvitcel ed snealba tpsolev eogdtniunitn os)ciIT Re(tutitsnI
OiS/ btNnecr e 0p.A2edyhedlamr ohft idwi ccainoipo r rpeodirdyh ncainoiporp s athsylat ac
2
00 3f osnoitidno cgnitarep olanimo nt adlei y)AAM (dic acilyrcahte mmumixa meh tnevig EC, 2
tsylat a)chs e5 o,6m 25tn1ge(gortin:edyhedlamrof:di ccainoipo rhp/lo m0m22:61: 2,7mta
,seitivitcel etscudo r,psnoisrevn otcnatca efsromr enttisylat asci hfetocnamrofr ee ph.Tegrahc
noitavitca emdret-gn oel h.Tnosirapm otcs olcethceB-namts a fEsois aeb hst adwle iAy MdMna
d08n1.a2:0 1P:-1i S e-eshVlatb assteas meiet rthst attste aiialdhetw othssyla tsa icyfhdotuts
O itSn/eacTrep etavitca esdtsylat aecer hlt l.Asnoitidn oncoitca elracitne dyillanim o tn,atsylat ac
2
d nIa T.Rnoitareneg eervitadi x yoeblbareneg eyrllaitr aep rda nnaoitisop eedk o ycybliramirp
ogtniunitn o scIi T.Rstsylat a bclNev oense h ntnooitacilp ptanet adapel iefv anhamtsaE
ts ael hrte v.Otsylat aeclba tgasnipolev e fdloa ohagt iswtsylat aecsab-di cear oemzisehtnys
se -nnrdoooii(fctAa t s ns er etddooscnifweaaltr rspdtesdb nadeet rx, aerIopeTsetRlrrapauq
nacire mhAtr oINI Ir Xorfeh te ohd tn7a9 9l1ir p,Aynamr e,Gcudl onIR iIsIisylat adCesaB
tpircsun agamnirape rypltnerr u scdi n)a79 9y1 a,M L,Iogaci h,Cyteic osSisylat aeC h ftgoniteeM
r ogfnireenig nrEotca elRacimeh Ce(cnerefn o ICgVnireenig nnEoitca elRacime heC hrtof
.)7 9,93 11e -n,8uaJda n,aaCtre b,lfAf n,asBtcud odsrnePassec oerlPbaniatsuS
iv
INTRODUCTION
)AA Md(i ccailyrcaht e fmsoisehtn yes hrt oyfgolonhc eltaicremm odcecitca rypled itws oemhT
H CeA h.T )e1rugi Fs(seco r)pHC An(irdyhona yecnote cea h st)iAM Me(talyrcaht elmyht edmna
edina yncegord yshuodraz adh ncaix oytlemert x fesoeititna ueqgr a flgonildn asheriuq esrsecorp
rdoedracs irdeht ie erhaci hswets aewtafl umsuinom mfsaotnuo msauoip oscetaren edgna
yllac-imono cde nyallatnemnoriv nyeltnerr u scyigolonhc eHt CeA h.Tts olcaitnatsb u tsdaemialcer
rgonisops irdeht i fetos oec h fteosuac eyblirami r,psnoisnap xwe eyn nra oeflbanetnu
.ets aewtaflus ie bhgtnitareneger
sisehtn yAs MrM osfseco rtpnemecalp erar oyfrtsud nliacime hec hntiht iewvi rgdnor t saseirehT
tnsiere trnailuci tes rriaa ep.h)T6 9,9 .1ytleeav i;paS5 9,9 .1ytleeav i;paS6 9,9 .1etlteaagoG(
desab-l adoeccud oyrlplacits e dmne oosrdaebh tt,audrbesab-muelo r tt tsaesoihpsntec oerhpt
ndCoes asbesseco re ph.Tsagnys evitca=rt tyallaicrem-m oec re2arug i nFniwo hnsoitalynobrac-
2
es ehfh cot.a)E9 8,9a1tte K;cbM5 9,9a15 9,9 .1ytleeavi peSr(utcafu n Aa rMmsoMefigolonhcet
oetdyhedlamr ohft idwesnedn oshcici h,wetaidemret neitanoip o hragpuor hste osgesseco rrpuof
] dIsnI ea I )ss ][e]esd rIrIse nfo[ uIscA a odt[eoAaA nxcrM MraioPAMemr (AhPeMt(ciuedorp
,lonah tnfeoomitad ilxaoit rdyaebpcud oesrdipyhedlam r]oIf IsIs[ec otnr aiPehtt o.N)(]VI[
noitadi xloaitr ae p hndtiecudo rrpet ae wh)T.A MoAM tAgMnitlus ee rhsteifiret soes lhacihw
)A Pd(i ccainoipo rmpr oo)ftAA Pe(dirdyh ncainoipo re phfntooit r soaepzylord ynhoitcaer
)s]iI IsIs[eco rsPs(ec onrapmtsaE-)I TeRt(utit senlIgna ihrcTrae s ee.hRdTelcy chsecirihw
:spe tgsniwoll oef h ftdoesirpmoc
Step 1: Propionate synthesis from ethylene (1) and ethylene plus propionic acid (2)
H HC=C +O C+H O (cid:247) HC HC HOOC (1)
2 2 2 3 2
HC HC H O +OOC C+H HC=C (cid:247) HC( HC O)OC . (2)
3 2 2 2 3 2 2
Step 2: Condensation of propionate with formaldehyde
HC( HC )OC O O+HCH (cid:247) HC HC(C= HOO C+)HC HC HOOC (3)
3 2 2 2 3 3 2
HC HC H O OO+HCCH (cid:247) HC HC(C= HOOC )+H O (4)
3 2 2 3 2
.
HC( HC )OC O + O2HCH (cid:247) 2HC HC(C= HOOC )+H O (5)
3 2 2 2 3 2
Figure 1. Schematic of the ACH process.
1
’’
Figure 2. C -carbonylation technologies for
2
MMA manufacture.
Step 3: Esterification with methanol
HC HC(C= HOO C+)HC HO (cid:247) HC HC(C= HCOOC) +H O. (6)
2 3 3 2 3 3 2
namts a yEdbecitca rypllaicremm o spc1ie t,Serutcafun aAm MrM osfseco rdpesopo rspi hntI
r oefgnell a shatcnese r,prevew o,ph2e t.St rnaw o psn3aei ktd Snyanapm olCacimehC
o wfdtoesopm ospcie tnsoitasnedn osci h.Tsseco re phfntooitartsnom eldaicremm olcufsseccus
nniwo hysrtemoihcio tlslare ve ohetv ihgci h)w] 4d [n]a3 [s(noitca enroitasnedn oectarapes
noitca e.R)5(
lufssec c ru aossfegnella hlcacinhc ey tee khttneserp esrpe to swttsr ie fh,treilr adeeta tssA
lethceB-namtsaE-I Te Rhfstouc oe fhnte eebv aehse h.Tsseco rspi hfntooitartsnom eldaicremmoc
.tro fhfcerae smearet
:s k dsoneawostt u ,cssoiifseht neytsanoip o,rp petts sreihfT
• d n,asisehtn yestanoipo rr potfsylat ascuoenego m ftoaonhempoleveD
• .sisylan acimonoc edn angise dyranimilerP
:sk s odanwetotsu co o s,fsleiatanoip o erhh ptteidwyhedlam rnfooofitasned n,opc edtnso ceehsT
• d n,anoitca enroitasnedn or cotfsylat aecsab-di cftaonempoleveD
• pets-e nr ootfsylat ancoitasnednoc-noitadi xloaitr alponaht edmenibm oftconempoleveD
.sisehtny sAMM
.snoitc egsniwoll oe f hndtiesserd dnae es bashla oegse hgtniveih cdaraw ostsergo rephT
2
RESULTS AND DISCUSSION
Task 1. Propionate Synthesis (Eastman and Bechtel)
os ld ansaseco rlplare ve ohr tolfed ocmimono cndeaepolev es danhamts a,Eretra utqs ae lhrtevO
oetmeh cnsoitasnedn oecvitadi xe ohfntooisnet xleaitnet oe phgtnipolev eoedtm is ttdietoved
.)lonaht efdmoaetsn ik(cotsde ee fhs)taEM Dr(eh tleyhtemid
-HOeM/ rpPeOtHs-e elrehtthceB-namts a lE re-ceodIihf oTmtpmRo onrn l oeaneocdIvtereod
d etrioa t pedm tnonuacaomrtsa Ee -ufetIlohcTatuRv ddeoehrntpi mnaaxme t,ssasEe cdoerspab
ta hetto N.(erutcafun aAm MrM osfeigolonhc e)tlaicremm oycllaitnet orp ol(aicremm orceh teovif
nniosirapm or codfe ssueigolonhc erteh teov iefse h)T.desab-sagn ysesitu onramtsaE-I TeRht
:er asisylan acimonoc esiht
• ,)s a ma&hHo Rs(seco rdpesab-H ClAanoitnevnoC
• ,sseco rdpesab-H C)ACG Ml(acime hsC aiGhsibust iwMeN
• I,)cilyrcaht enMap a,Jykcu Ls(seco rnpoitadi xeonelytub-
• td n,a)noy aiRhsibust i,Modoy Ks(seco rnpoitadi xloonatub-
• .)I C,Illeh Sn(oitalynobr aecnyporP
,sesseco rdpesab-H ClAanoitnevn oechT i d nnaoitadi xeonelytub- t e,rnaoitad ilxoonatub-
eh tn ilaicremmo ce blli wssecor placimeh Csa Gihsibusti Mwe neh tdn asessecor plaicremmoc
ev ashthg itrnet ae phd tnlale hydSbetnet asspiseco rnpoitalynobr aecnypo r.e pmhrT ertaen
nyiltnec edretrope rI ( CydIberiuq cnaeeb Chemical and Engineering News ,y7r9.a9p u1,rbeF
ytivitis nd,en)saeu ltacvud ortr ospn(oocitcud o,rt psloacti pr ea ondcsfoaismir a.p) m2eo1hcT
r odfe ssruiaey/b l0 M5fs2ois atbnetsis n .oAycticap aoectul atvcudo rd pntas olcatip afco
.Ademus s sayiticap arcaey/b l0M 0s1seco rnpoitalynobr aecnypo rep hrt o;fsetamit sceimonoce
.e3rug innFiwo hsA siMoeMttu olrethceB-namtsaE-I TfcRoitamehcs
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troper ,IRS( )3991 sa a gnitrats tniop rof leehtthceB- npaemttss-aeEe-rIhT-tRHOeM/rPOH
tnempiu qde n,aez irsotca e,recnal albairet asm'I RgSniyfid oymltneuqesb uds n,asseco rdpesab
tnec r n)e0aoyp2tivitcel ed snnaoisrevno ce(cnamrofr erpotca edreb-dex isf'I TtRcelf eonrtgised
0 0 f3sonoitidn ogcnitare ploanim o tntasylat aicS/bN Ecinoipo rfhpo/lo m0m22:61: 2, 7m ,t2Ca
namt s.a)Enoitc aer zfmims- 1-o. 7t1hr. so0t8o0es(t2my l, an5 tegagcortin:edyhedlamrof:dica
Figure 3. Eastman/RTI/Bechtel three-step HOPr/MeOH-based
MMA process (with external formaldehyde feed).
3