DK173496B1 - Fremgangsmåde til fremstilling af syntesegas ved vanddampreformering under anvendelse af en katalyseret metaloverflade - Google Patents

Fremgangsmåde til fremstilling af syntesegas ved vanddampreformering under anvendelse af en katalyseret metaloverflade Download PDF

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DK173496B1
DK173496B1 DK199800948A DKPA199800948A DK173496B1 DK 173496 B1 DK173496 B1 DK 173496B1 DK 199800948 A DK199800948 A DK 199800948A DK PA199800948 A DKPA199800948 A DK PA199800948A DK 173496 B1 DK173496 B1 DK 173496B1
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reactor
reforming catalyst
catalyst
steam
reforming
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DK199800948A
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Peter Seier Christensen
Viggo Lucassen Hansen
R Rostrup-Nielsen J
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Topsoe Haldor As
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Priority to DK199800948A priority Critical patent/DK173496B1/da
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Priority to PCT/EP1999/004562 priority patent/WO2000003579A2/en
Priority to CA002340698A priority patent/CA2340698C/en
Priority to EP99932779A priority patent/EP1181240A2/en
Priority to CNB998094307A priority patent/CN1187259C/zh
Priority to JP2000559723A priority patent/JP3790426B2/ja
Priority to AU49045/99A priority patent/AU752810B2/en
Priority to RU2001101486/15A priority patent/RU2220901C2/ru
Priority to BR9912123-9A priority patent/BR9912123A/pt
Priority to US09/743,530 priority patent/US6746624B1/en
Publication of DK199800948A publication Critical patent/DK199800948A/da
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Priority to ZA2001/00293A priority patent/ZA200100293B/en

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Description

i DK 173496 B1
Denne opfindelse er rettet på fremgangsmåde til fremstilling af syntesegas ved vanddampreformering af et carbon-hydridfødemateriale i kontakt med katalyseret metaloverflade.
5 Betegnelsen benyttes om et katalysatorsystem, hvor et katalysatorlag er fæstnet på overfladen af et andet materiale, f.eks. metalliske overflader. Det andet materiale tjener som en understøttende struktur, der bebringer systemet styrke. Dette tillader udformning af katalysatorformer, 10 der ikke selv ville have en tilstrækkelig mekanisk styrke.
Syntesegas produceres ud fra carbonhydrider ved vanddampreformering ifølge reaktionerne (1)-(3):
CnHm + n H20 6 n CO + (n + y) H2 (-ΔΗ°298 < 0) (1) 15 CO + HzO W C02 + H2 (-ΔΗ°298 = 41 kJ/mol) (2) CH4 + HzO W CO + 3 H2 (-ΔΗ°298 = -206 kJ/mol) (3)
Kendt vanddampreformeringsteknik benytter reformeringskatalysatorer på form af pellets med diverse størrelser og 20 former. Disse katalysatorpellets anbringes i fast leje reaktorer (reformerrør). Reformeringsreaktionen er endotermisk.
I konventionelle reformere tilføres den nødvendige varme til reaktionen fra området uden for rørene normalt som en kombination af stråling og konvektion til den ydre side af et 25 reformerrør. Varmen overføres ved varmeledning gennem rørvæggen til den indre side af røret og overføres ved konvektion til gasfasen. Endelig overføres varme ved konvektion fra gasfasen til katalysatorpellets. Katalysatortemperaturen kan være mere end 100EC lavere end temperaturen af den indre 30 rørvæg ved samme aksiale position på reformerrøret.
En vanddampreformeringskatalysator, hvor det katalytisk aktive materiale er afsat på en metallisk nikkelbærer i form DK 173496 B1 2 af en snoet strimmel er omtalt i U.S. patent nr. 4.400.309.
Det anføres at en således udformet katalyseret overflade reducerer tryktabet over et reformerrør forsynet med denne form for katalysator og at kompressionsenergien reduceres i 5 forhold til de kendte partikkelformede vanddampreforming katalysatorer.
Det er blevet fundet, at trykfaldsreduktioner yderligere forbedres og varmetransporten bliver mere effektiv, når der benyttes katalyseret metaloverflade i vanddampreformerings-10 processen når den katalyserede overflade er i det væsentlige i samme for som væggen. Varmetransporten til katalysatoren forgår ved ledning fra den indre rørvæg. Dette ér en meget mere effektiv transportmekanisme end en transport ved konvektion gennem gasfasen. Resultatet er, at temperaturerne af 15 den indre rørvæg og af katalysatoren er næsten identiske (med en forskel under 5EC). Yderligere kan rørtykkelsen reduceres, se nedenfor, hvilket gør temperaturforskellen mindre mellem den ydre og indre side af reformerrøret. Det er således muligt både at have en højere katalysatortempera-20 tur og en lavere rørtemperatur under fastholdelse af alle andre betingelser, når konventionelle reformerrør erstattes med rør med katalyseret metaloverflade. En lav temperatur for den ydre rørvæg er efterstræbelsesværdig, da dette forlænger levetiden for røret. En høj kataltysatortemperatur er 25 fordelagtig, da reaktionshastigheden vokser med temperaturen, og da ligevægten i reaktion (3) forskydes mod højre, hviket medfører en bedre udnyttelse af fødematerialet.
Tryktabet over et katalysatorforsynet reformerrør er for samme rørdiameter meget lavere end i det konventienelle til-30 fælde. Dette tillader anvendelse af reaktorrør med en mindre diameter under stadig opretholdelse af et acceptabelt tryktab. En mindre rørdiameter medfører en forøget levetid for 3 DK 173496 B1 et rør, fører til tolerance for højere temperaturer og reducerer forbruget af rørmateriale.
Endelig reduceres katalysatormængden ved anvendelse af reformerrør med katalyseret metaloverflade i forhold til 5 konverntionelle reformere med et fast leje af reformeringskatalysatoren.
Fig. 1 viser den forreste del af et anlæg, der producerer syntesegas. Fødematerial 2 forudopvarmes, afsvovles i enhed 4, blandes med procesdamp 6 og opvarmes yderligere før 10 indgang til en adiabatisk præreformer 8. Effluentstrømmen fra præreformer 8 opvarmes yderligere i en i røggaskanalen 12 anbragt varmevekslerspiral og sendes til rørreformeren 14, hvor konversion af methan til hydrogen, carbonmonoxid og carbondioxid finder sted. Viderebearbejdningen af effluent-15 gassen fra rørreformeren afhænger af anvendelsen af produktet .
Katalyseret metaloverflade kan benyttes i to af de på Fig. 1 viste enheder: 1. I forudopvarmerspiral 10 til opvarmning af præreformer-20 effluentgassren før dennes indgang i rørreformer 14.
2. I rørreformer 14.
Katalytisk overtrækning af en metaloverflade (wash-coating) er en velkendt proces (en beskrivelse gives f. eks. i Cybulski, A. og Moulijn, J.A., Structured Catalysts and 25 Reactors, Marcel Dekker, Inc., New York, 1998, kapitel 3 og referencer heri). Et tyndt lag af en opslæmning indeholdende den keramiske precursor anbringes på overfladen, f.eks. ved hjælp af påsprøjtning, påmaling eller neddypning. Efter - påføringen af overtrækket tørres opslæmningen og kalcineres 30 ved en temperatur, der sædvanligvis er i området 350-1000EC. Endelig imprægneres det keramiske lag med det katalytisk 4 DK 173496 B1 aktive materiale. Alternativt påføres det katalytisk aktive materiale samtidigt med den keramiske precursor.
Der findes desværre en række ulemper ved reaktorer med katalyseret metaloverflade i forhold til fast leje 5 reaktorer:
Katalysatorlaget kan ikke erstattes, hvis det mister sin aktivitet, enten ved ældning eller ved forgiftning.
Katalysatorlaget kan kun anbringes på visse materialer. Reaktorrørene skal være fremstillet af en sådan type mate-10 riale, der kan være mere kostbar end et konventionelt rørmateriale. Vanddampreformeringsreaktionerne foregår under betingelser med tryk, og rørtykkelsen er stor, hvorfor materialeprisen i signifikant grad påvirker omkostningerne.
Ydermere kan produktionen af lange rør af katalysator-15 forsynet hardware være vanskelig. Reaktorrøret kan have en længde på 10 m eller mere. Det vil være svært at opnå en jævn tykkelse for reformeringskatalysatoren gennem hele sådan en længde, og midler til opnåelse af et jævnt lag, der kan benyttes i mindre skala, såsom centrifugering af røret 20 er vanskeligere at benytte for denne størrelse rør. Yderligere kan en passende varmebehandling af et rør af denne størrelse være vanskelig.
Disse ulemper kan overvindes ved som nævnt nedenfor at producere det katalysatorforsynede hardware adskilt fra 25 reaktoren.
En metalbærer skæres i passende størrelser. Arket wash-coates som beskrevet ovenfor. Efter denne washcoating formes arket til det relevante udseende. Alternativt formes arket til sit endelige udseende før en washcoating. Den 30 metalliske bærer formes, så den i det væsentlige har samme form som reaktorvæggen og er blevet anbragt i en direkte varmeledende forbindelse med reaktorvæggen.
5 DK 173496 B1
Det vil være muligt at udskifte katalysatorlaget, hvis det ikke mere har en stor nok katalytisk aktivitet. Det dyre stål, der benyttes til opnåelse af adhæsion af katalysatoren til metaloverfladen, vil kun omfatte en ringe del af total-5 metalforbruget. Det katalysatorforsynede hardware kan produceres i mindre sektioner, der vil være lettere at fremstille og håndtere.
I overenstemmelse hermed tilvejebringer denne opfindelse en fremgangsmåde til fremstilling af en hydrogen- og carbon-10 monoxidrig gas ved katalytisk vanddampreformering af et car-bonhydridfødemateriale, omfattende trinnene: (a) at føre en procesgas af carbonhydridfødemateriale gennem en første reaktor med en vanddampreformeringskatalysator op- 15 varmet af en varm gasstrøm; (b) at føre effluenten fra den første reaktor til en følgende rørreaktor indeholdende en vanddampreformeringskatalysator og opvarmet ved afbrænding af brændstof til opnåelse herved af en varm gasstrøm af vanddampreformeret produktgas 20 og en varm strøm af røggas, og som er ejendommelig ved, at en reformeringskatalysator er anbragt på en metallisk bærer med i det væsentlige samme form som væggen i reaktoren og anbragt i varmeledende forbindelse med reaktorvæggen.
I en specifik udførelsesform for opfindelsen tilveje-25 bringes reformeringskatalysatoren i reaktoren i trin b både med en metallisk bærer med i det væsentlige samme form som væggen i reaktoren og anbragt i varmeledende forbindelse med reaktorvæggen og som pellets af reformeringskatalysator.

Claims (4)

6 DK 173496 B1
1. Fremgangsmåde til fremstilling af en hydrogen- og carbonmonoxidrig gas ved katalytisk vanddampreformering af 5 et carbonhydridfødemateriale, omfattende trinnene: (a) at føre en procesgas af carbonhydridfødemateriale gennem en første reaktor med en vanddampreformeringskatalysator opvarmet af en varm gasstrøm; 10 (b) at føre effluenten fra den første reaktor til en følgende rørreaktor indeholdende en vanddampreformeringskatalysator og opvarmet ved afbrænding af brændstof til opnåelse herved af en varm gasstrøm af vanddampreformeret produktgas og en varm strøm af røggas, og kendetegnet ved, 15 at en reformeringskatalysator er anbragt på en metallisk bærer med i det væsentlige samme form som reaktorvæggen i varmeledende forbindelse med reaktorvæggen i det mindste i reaktoren i trin a.
2. Fremgangsmåde ifølge krav 1, kendetegnet ved, at 20 reformeringskatalysatoren i reaktoren i trin b både er forsynet med en metallisk bærer med i det væsentlige samme form som væggen i reaktoren og anbragt i varmeledende forbindelse med reaktorvæggen og foreligger som pellets af reformeringskatalysator.
3. Fremgangsmåde ifølge krav 1, kendetegnet ved, at reformeringskatalysatoren i trin b foreligger som pellets af reformeringskatalysator.
4. Fremgangsmåde ifølge krav 1, kendetegnet véd, at vanddampreformeringskatalysatoren omfatter nikkel og/eller 30 ædelmetaller. Produktion af syntesegas ved vanddampreformering under anvendelse af katalyseret metaloverflade.
DK199800948A 1998-07-16 1998-07-16 Fremgangsmåde til fremstilling af syntesegas ved vanddampreformering under anvendelse af en katalyseret metaloverflade DK173496B1 (da)

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Application Number Priority Date Filing Date Title
DK199800948A DK173496B1 (da) 1998-07-16 1998-07-16 Fremgangsmåde til fremstilling af syntesegas ved vanddampreformering under anvendelse af en katalyseret metaloverflade
CA002340698A CA2340698C (en) 1998-07-16 1999-07-01 Synthesis gas production by steam reforming using catalyzed hardware
EP99932779A EP1181240A2 (en) 1998-07-16 1999-07-01 Synthesis gas production by steam reforming using reactors the walls of which are catalytic
CNB998094307A CN1187259C (zh) 1998-07-16 1999-07-01 使用催化结构件的蒸汽转化法生产合成气
PCT/EP1999/004562 WO2000003579A2 (en) 1998-07-16 1999-07-01 Synthesis gas production by steam reforming using reactors the walls of which are catalytic
JP2000559723A JP3790426B2 (ja) 1998-07-16 1999-07-01 触媒化ハードウェアを使用した水蒸気改質による合成ガスの生成方法
AU49045/99A AU752810B2 (en) 1998-07-16 1999-07-01 Synthesis gas production by steam reforming using catalyzed hardware
RU2001101486/15A RU2220901C2 (ru) 1998-07-16 1999-07-01 Получение синтез-газа паровым реформингом с использованием катализированного оборудования
BR9912123-9A BR9912123A (pt) 1998-07-16 1999-07-01 Produção de gás de sìntese através de regeneração de vapor usando hardware catalisado
US09/743,530 US6746624B1 (en) 1998-07-16 1999-07-01 Synthesis gas production by steam reforming using catalyzed hardware
ZA2001/00293A ZA200100293B (en) 1998-07-16 2001-01-10 Synthesis gas production by steam reforming using catalyzed hardware

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DK199800948A DK173496B1 (da) 1998-07-16 1998-07-16 Fremgangsmåde til fremstilling af syntesegas ved vanddampreformering under anvendelse af en katalyseret metaloverflade
DK94898 1998-07-16

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ZA200100293B (en) 2002-06-26
WO2000003579A2 (en) 2000-01-27
AU752810B2 (en) 2002-10-03
DK199800948A (da) 2000-03-28
CN1342131A (zh) 2002-03-27
JP2002520247A (ja) 2002-07-09
BR9912123A (pt) 2001-04-10
JP3790426B2 (ja) 2006-06-28
EP1181240A2 (en) 2002-02-27
CA2340698A1 (en) 2000-01-27
AU4904599A (en) 2000-02-07
WO2000003579A3 (en) 2001-10-11
CN1187259C (zh) 2005-02-02
RU2220901C2 (ru) 2004-01-10
CA2340698C (en) 2004-11-30
US6746624B1 (en) 2004-06-08

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