CN1098700A - 高温蒸汽重整 - Google Patents
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- 239000003054 catalyst Substances 0.000 claims abstract description 48
- 229930195733 hydrocarbon Natural products 0.000 claims abstract description 18
- 150000002430 hydrocarbons Chemical class 0.000 claims abstract description 18
- 238000000034 method Methods 0.000 claims abstract description 14
- 239000004215 Carbon black (E152) Substances 0.000 claims abstract description 13
- 239000002245 particle Substances 0.000 claims abstract description 13
- 238000002407 reforming Methods 0.000 claims abstract description 10
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- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 description 2
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- 238000009835 boiling Methods 0.000 description 2
- 238000001193 catalytic steam reforming Methods 0.000 description 2
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- 239000004411 aluminium Substances 0.000 description 1
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- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 1
- 229910021529 ammonia Inorganic materials 0.000 description 1
- 230000015572 biosynthetic process Effects 0.000 description 1
- 239000011449 brick Substances 0.000 description 1
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- C01B2203/0844—Methods of heating the process for making hydrogen or synthesis gas by heat exchange with exothermic reactions, other than by combustion of fuel the non-combustive exothermic reaction being another reforming reaction as defined in groups C01B2203/02 - C01B2203/0294
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Abstract
本发明公开的是在重整反应器中，在以固定形式
的蒸汽重整催化剂的存在下，将高温蒸汽重整的方
法，其中催化剂床至少包括上下两层，在碳氢化合物
蒸汽重整中，上层的催化剂粒子是减活的。
Description
本发明的目的是制备富含氢气和一氧化碳的气体。具体地说，本发明涉及通过碳通过碳氢化合物原料的高温催化剂重整来制备这种气体的方法和反应器。
富含有氢气和一氧化碳的气体主要用作生产氨和甲醇的合成气体原料，还有用于炼钢以及作为燃料或家用煤气。
目前工业制备方法包括高温蒸汽重整过程如碳氢化物的自动热催化重整或初次和二次蒸重整。
高温蒸汽重整过程中，碳氢化合物原料和空气、氧气、或富氧空气在安装在反应器顶部的燃烧炉中一起燃烧。在此氧气的供应量应低于完全燃烧所需的量，流出气体中的氢气和一氧化碳主要通过燃烧反应生成：
无论何种碳氢化合物原料，这种反应都是强放热反应。这种方法最常用于较轻质原料的重整，其范围从天然气到沸点至200℃的粗汽油馏分。
在该过程中，只有部分碳氢化合物在上述燃烧反应（1，2）中被空气中所含的氧氧化。燃烧后气流中残留的碳氢化合物随后通过吸热反应进行催化蒸汽重整：
催化蒸汽重整过程在约900-1400℃的温度下完成。在进料中加入蒸汽是为了调节火焰温度和提高炉中流出气体中碳氢化合物的转化率。
在反应器的上部，混合了蒸汽的碳氢化合物进料与空气中所含的氧一起进行燃烧。然后在反应器的下部，在以固定床形式安置的催化剂的存在下，燃烧后气体中残存的碳氢化物被进行蒸汽重整。吸热的蒸汽重整反应所需的热能通过在反应器上部催化床上方的燃烧段所流出的热气体供给。当燃烧气体和催化剂接触后，通过在催化剂床上的蒸汽重整反应，气体温度降至900-1100℃。
为能承受入热燃烧反应（1，2）产生的高温。通过在反应器壳的内壁衬上耐温和耐火绝热材料来保护反应器外壳。
目前，上述类型的最常用的工业反应器的衬里材料含有90%以上的氧化铝。尽管这些材料是具有良好耐热和耐磨性的高强度铸件或砖，通过与含碳氧化物，蒸汽和氢气的高热燃烧气体接触，在反应器上部燃烧区周围常发生损坏。由于气体的还原性，耐火材料中的氧化铝被还原成铝的低氧化物，而这种低氧化物在反应器上部的高温环境下是易挥发的。
反应器衬里的挥发性降解产物与原料气中遇高温易挥发的杂质一起在温度低于降解产物和杂质的气化温度的反应器的部分区域和下游的反应设备中沉淀下来。
在置有高活性蒸汽重整催化剂床的反应器中，在床的上部其催化剂和表面的温度比燃烧气体低很多，因此固体的沉积主要在催化剂床的最顶层发生。
因此，固体沉降实际集中在催化剂床最顶部的藻层上，这样在该层，气体传送就受到限制，使得床的次层气流分布不均匀，最终在催化剂床上形成不利的直通通道。
现已发现在碳氢化物的蒸汽重整中，催化剂床的最顶层用减活的催化剂粒子，而在后续层中逐渐增加催化剂粒子的活性，这样就可避免高温催化蒸汽重整过程中出现的上述问题。由于吸热的蒸汽重整反应在更大面积的催化剂床范围的内进行，催化剂表面的温降得以平缓，从而在床的顶上部份只有很少的固体沉积现象发生。由此固体沉积被分散到大面积范围的催化剂床上，在催化剂床上的气体传送得到了大幅度改善。
根据该发现，本发明提供了在重整反应器中以固定床形式安置的蒸汽重整催化剂的存在下进行碳氢化合物高温蒸汽重整的改进方法，其中催化剂床最少由上下二层组成，在碳氢化合物的蒸汽重整中，上层的催化剂粒子均是减活了的粒子。
在用本发明方法操作本发明反应器时，预热至约400-700℃的碳氢化物原料被导入到位于具防火衬里反应器顶上的燃烧炉中。最好氧气的用量是使氧/碳摩尔数比达到0.5和0.7之间，蒸汽/碳摩尔数比最好在0.5和2.0之间。当本方法在自动热催化重整条件下进行操作时，适合本法的碳氢化物原料范围可从甲烷直至沸点为200℃的粗汽油馏分，包括天然气、液化石油气和初次重整后的气体。
从燃烧炉中流出的含未转换碳氢化合物的气体随后通过重整反应器中燃烧炉燃烧段下面的固定的蒸汽重整催化剂床。
在燃烧段的常规温度1000-1500℃的条件下，反应器衬里、燃烧炉的分解产物或工艺原料气体中的外来组分挥发出来并随流出气体带到催化剂床上。
由于流出气体中的残留碳氢化合物在催化剂上的吸热蒸汽重整，由具常规的蒸汽重整活性的催化剂如含镍和/或钼的催化剂组成的床上部的催化剂表面温度比周围气体的温度低约100-150℃。当常规蒸汽重整催化剂的活性降低到5%时，上部催化剂层的温差缩小到约25℃。结果，由一在催化剂床的上层催化剂表面的温度变化被减缓，催化剂表面固体化合物的沉积被分散到床中更大的区域。
从下面的表2可明显看出，在气体组成（表1）一定时，催化剂床的表面温度可在大温差范围内进行控制。所以所需的催化剂表面温度将取决于流出气体中固体的挥发性。
表1
| 气体组成（干计） | 进催化剂床 | 出催化剂床 |
| H2 mol% | 56.7 | 62.4 |
| N2 mol% | 7.0 | 6.1 |
| CO mol% | 21.4 | 21.5 |
| CO2 mol% | 8.3 | 8.3 |
| CH4 mol% | 5.7 | 0.94 |
| Ar mol% | 0.91 | 0.79 |
| H2O mol% | 33.9 | 28.2 |
表2
自动热重整
温度轮廓-催化剂床：
由丹麦Haldor Topsφe A/S提供的镍重整催化剂RKS-2
| 相对活性 | 100％ | 30％ | 10％ |
| 轴距（m） | 温度气体 催化剂 | 温度气体 催化剂 | 温度气体 催化剂 |
| 0.00 | 1150 1089 | 1150 1109 | 1150 1127 |
| 0.02 | 1106 1062 | 1119 1086 | 1132 1112 |
| 0.10 | 1020 1008 | 1045 1031 | 1078 1067 |
| 0.20 | 992 989 | 1007 1002 | 1040 1034 |
| 0.30 | 985 985 | 993 991 | 1018 1014 |
| 0.40 | 984 983 | 987 986 | 1005 1003 |
| 0.60 | 983 983 | 984 984 | 992 991 |
在工业用高温重整反应器中，将30至60厘米的催化剂床上层的常规重整催化剂的活性减低90%就通常足够使在催化剂床上部的固体沉积分散至不会限制气体传送的程度。
通过在反应气体的流动方式向下断增加催化剂的活性，将催化剂的各层再分成许许多多的亚层，这样固体沉呼物就可进一步分散到催化剂床较低的层中。
制备减低了重整活性的催化剂可通过将浸渍在适合载体上的活性材料量减少的方法或者将涂渍后的催化剂粒子浸滤去一部分活性物质。
减低催化活性还可以通过提高催化剂床上层催化剂粒子的粒径来实现。
Claims (4)
1、在重整反应器中，在以固定床形式的蒸汽重整催化剂的存在下，将碳氢化合物高温蒸汽重整的方法，其中催化剂床至少包括上下两层，在碳氢化合物蒸汽重整中，上层的催化剂粒子是减活的粒子。
2、权利要求1的方法，其中催化剂床上层的重整催化剂粒子的活性是下层催化剂粒子活性的1%至50%。
3、权利要求1的方法，其中催化剂床上层的厚度为0.30-0.60米。
4、权利要求1的方法，其中催化剂床下层包括许多亚层，其催化粒子的蒸汽重整活性是不断增加的。
Applications Claiming Priority (2)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| DK057693A DK170797B1 (da) | 1992-08-13 | 1993-05-17 | Fremgangsmåde til fremstilling af hydrogen- og carbonmonoxidrig gas |
| DK0576/93 | 1993-05-17 |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| CN1098700A true CN1098700A (zh) | 1995-02-15 |
| CN1037760C CN1037760C (zh) | 1998-03-18 |
Family
ID=8095121
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| CN94105617A Expired - Lifetime CN1037760C (zh) | 1993-05-17 | 1994-05-17 | 碳氢化合物的蒸汽重整方法 |
Country Status (7)
| Country | Link |
|---|---|
| US (1) | US5554351A (zh) |
| EP (1) | EP0625481B1 (zh) |
| CN (1) | CN1037760C (zh) |
| DE (1) | DE69412536T2 (zh) |
| ES (1) | ES2120538T3 (zh) |
| RU (1) | RU2119382C1 (zh) |
| ZA (1) | ZA943380B (zh) |
Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN105980040A (zh) * | 2013-11-15 | 2016-09-28 | 林德股份公司 | 用于烃的蒸汽重整和蒸汽裂解的方法和设备 |
Families Citing this family (18)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JP2835851B2 (ja) * | 1989-06-23 | 1998-12-14 | ヤマハ発動機株式会社 | 燃料電池用改質装置 |
| US5562818A (en) * | 1993-07-16 | 1996-10-08 | Uop | FCC feed injection with non-quiescent mixing |
| US6576203B2 (en) * | 1998-06-29 | 2003-06-10 | Ngk Insulators, Ltd. | Reformer |
| DE60010550T2 (de) * | 1999-03-05 | 2005-05-12 | Haldor Topsoe A/S | Verfahren zur autothermen katalytischen Dampf-Reformierung |
| US6641625B1 (en) | 1999-05-03 | 2003-11-04 | Nuvera Fuel Cells, Inc. | Integrated hydrocarbon reforming system and controls |
| CA2410927A1 (fr) * | 2002-11-05 | 2004-05-05 | Michel Petitclerc | Reacteur a chauffage electrique pour le reformage en phase gazeuse |
| US7102048B2 (en) * | 2002-12-17 | 2006-09-05 | Exxonmobil Chemical Patents Inc. | Methanol feed for producing olefin streams |
| US7255840B2 (en) * | 2003-06-26 | 2007-08-14 | Praxair Technology, Inc. | Autothermal reactor and method for production of synthesis gas |
| KR100637340B1 (ko) * | 2004-04-09 | 2006-10-23 | 김현영 | 고온 개질기 |
| GB0510514D0 (en) | 2005-05-24 | 2005-06-29 | Johnson Matthey Plc | Steam reforming |
| WO2007129109A2 (en) | 2006-05-08 | 2007-11-15 | Compactgtl Plc | Catalytic reactor comprising first and secondary flow channels arranged alternately |
| US20080260631A1 (en) | 2007-04-18 | 2008-10-23 | H2Gen Innovations, Inc. | Hydrogen production process |
| US8592492B2 (en) | 2010-03-08 | 2013-11-26 | Praxair Technology, Inc. | Using fossil fuels to increase biomass-based fuel benefits |
| US8916492B2 (en) | 2010-03-19 | 2014-12-23 | Haldor Topsoe A/S | Reforming catalyst |
| RU2452559C2 (ru) * | 2010-08-19 | 2012-06-10 | Общество с ограниченной ответственностью "СинТоп" | Реактор паровой и пароуглекислотной конверсии легких углеводородов для получения газа, содержащего водород и окись углерода |
| US9290422B2 (en) | 2012-11-27 | 2016-03-22 | Praxair Technology, Inc. | Hybrid plant for liquid fuel production |
| US9145525B2 (en) | 2013-06-26 | 2015-09-29 | Praxair Technology, Inc. | Acid gas management in liquid fuel production process |
| RU2571149C1 (ru) * | 2014-06-09 | 2015-12-20 | Федеральное государственное бюджетное учреждение "Национальный исследовательский центр "Курчатовский институт" | Реактор конверсии метана |
Family Cites Families (11)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| NL34213C (zh) * | 1931-01-17 | |||
| US2668101A (en) * | 1949-01-21 | 1954-02-02 | Nat Cylinder Gas Co | Method of preparing mixtures of hydrogen and carbon oxides |
| US2665979A (en) * | 1949-10-31 | 1954-01-12 | United Gas Improvement Co | Method of reforming gaseous hydrocarbons |
| FR1073309A (fr) * | 1951-05-04 | 1954-09-23 | Azote & Prod Chim | Perfectionnements aux procédés de fabrication d'hydrogène par réduction catalytique de la vapeur d'eau au moyen d'hydrocarbures |
| US2760917A (en) * | 1951-09-28 | 1956-08-28 | Gulf Research Development Co | Fluidized catalytic process for the destructive hydrogenation of hydrocarbons |
| GB725285A (en) * | 1952-01-15 | 1955-03-02 | Badische Anilin & Soda Fabrick | Catalytic conversion of carbon monoxide and steam into carbon dioxide and hydrogen |
| US4233179A (en) * | 1975-12-08 | 1980-11-11 | United Catalysts Inc. | Process for steam reforming of hydrocarbons |
| US4207211A (en) * | 1975-12-08 | 1980-06-10 | United Catalysts Inc. | Catalyst for steam reforming of hydrocarbons and process of preparing the catalyst |
| JPS6116133A (ja) * | 1984-06-29 | 1986-01-24 | Fuji Heavy Ind Ltd | ４輪駆動車 |
| JPS61161133A (ja) * | 1985-01-08 | 1986-07-21 | Mitsubishi Heavy Ind Ltd | 吸熱反応装置 |
| US4654458A (en) * | 1985-09-26 | 1987-03-31 | Amoco Corporation | Conversion of a lower alkane |
-
1994
- 1994-05-06 ES ES94107118T patent/ES2120538T3/es not_active Expired - Lifetime
- 1994-05-06 DE DE69412536T patent/DE69412536T2/de not_active Expired - Lifetime
- 1994-05-06 EP EP94107118A patent/EP0625481B1/en not_active Expired - Lifetime
- 1994-05-17 ZA ZA943380A patent/ZA943380B/xx unknown
- 1994-05-17 US US08/243,689 patent/US5554351A/en not_active Expired - Lifetime
- 1994-05-17 CN CN94105617A patent/CN1037760C/zh not_active Expired - Lifetime
- 1994-05-17 RU RU94016360A patent/RU2119382C1/ru active
Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN105980040A (zh) * | 2013-11-15 | 2016-09-28 | 林德股份公司 | 用于烃的蒸汽重整和蒸汽裂解的方法和设备 |
Also Published As
| Publication number | Publication date |
|---|---|
| CN1037760C (zh) | 1998-03-18 |
| ZA943380B (en) | 1995-04-04 |
| EP0625481B1 (en) | 1998-08-19 |
| EP0625481A1 (en) | 1994-11-23 |
| US5554351A (en) | 1996-09-10 |
| RU2119382C1 (ru) | 1998-09-27 |
| DE69412536T2 (de) | 1998-12-24 |
| RU94016360A (ru) | 1996-04-27 |
| ES2120538T3 (es) | 1998-11-01 |
| DE69412536D1 (de) | 1998-09-24 |
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