CN1880414A - Method for optimization of synthetic gas components by reversed water-gas shift reaction technology and flow therefor - Google Patents
Method for optimization of synthetic gas components by reversed water-gas shift reaction technology and flow therefor Download PDFInfo
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- CN1880414A CN1880414A CN 200610020836 CN200610020836A CN1880414A CN 1880414 A CN1880414 A CN 1880414A CN 200610020836 CN200610020836 CN 200610020836 CN 200610020836 A CN200610020836 A CN 200610020836A CN 1880414 A CN1880414 A CN 1880414A
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- gas
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- reverse water
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- 238000006243 chemical reaction Methods 0.000 title claims abstract description 25
- 238000000034 method Methods 0.000 title claims abstract description 24
- 238000005457 optimization Methods 0.000 title claims abstract description 4
- 238000005516 engineering process Methods 0.000 title description 5
- OKKJLVBELUTLKV-UHFFFAOYSA-N Methanol Chemical compound OC OKKJLVBELUTLKV-UHFFFAOYSA-N 0.000 claims abstract description 99
- 239000007789 gas Substances 0.000 claims abstract description 72
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 claims abstract description 20
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims abstract description 17
- 229910002092 carbon dioxide Inorganic materials 0.000 claims abstract description 16
- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 claims abstract description 15
- LCGLNKUTAGEVQW-UHFFFAOYSA-N Dimethyl ether Chemical compound COC LCGLNKUTAGEVQW-UHFFFAOYSA-N 0.000 claims abstract description 12
- 150000002430 hydrocarbons Chemical class 0.000 claims abstract description 10
- 239000003345 natural gas Substances 0.000 claims abstract description 10
- 239000001569 carbon dioxide Substances 0.000 claims abstract description 7
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 claims abstract description 6
- 229910002091 carbon monoxide Inorganic materials 0.000 claims abstract description 6
- 229930195733 hydrocarbon Natural products 0.000 claims abstract description 6
- 239000007788 liquid Substances 0.000 claims abstract description 6
- 238000005810 carbonylation reaction Methods 0.000 claims abstract description 3
- 238000003786 synthesis reaction Methods 0.000 claims description 48
- 230000015572 biosynthetic process Effects 0.000 claims description 38
- 230000001965 increasing effect Effects 0.000 claims description 9
- 239000002994 raw material Substances 0.000 claims description 8
- 239000001257 hydrogen Substances 0.000 claims description 6
- 229910052739 hydrogen Inorganic materials 0.000 claims description 6
- 239000004215 Carbon black (E152) Substances 0.000 claims description 5
- XLOMVQKBTHCTTD-UHFFFAOYSA-N Zinc monoxide Chemical compound [Zn]=O XLOMVQKBTHCTTD-UHFFFAOYSA-N 0.000 claims description 4
- AMWRITDGCCNYAT-UHFFFAOYSA-L hydroxy(oxo)manganese;manganese Chemical compound [Mn].O[Mn]=O.O[Mn]=O AMWRITDGCCNYAT-UHFFFAOYSA-L 0.000 claims description 4
- 239000000203 mixture Substances 0.000 claims description 4
- 239000003054 catalyst Substances 0.000 claims description 3
- 238000006555 catalytic reaction Methods 0.000 claims description 3
- QPLDLSVMHZLSFG-UHFFFAOYSA-N Copper oxide Chemical compound [Cu]=O QPLDLSVMHZLSFG-UHFFFAOYSA-N 0.000 claims description 2
- 239000005751 Copper oxide Substances 0.000 claims description 2
- 229910017773 Cu-Zn-Al Inorganic materials 0.000 claims description 2
- 229910000431 copper oxide Inorganic materials 0.000 claims description 2
- 230000000694 effects Effects 0.000 claims description 2
- TWNQGVIAIRXVLR-UHFFFAOYSA-N oxo(oxoalumanyloxy)alumane Chemical compound O=[Al]O[Al]=O TWNQGVIAIRXVLR-UHFFFAOYSA-N 0.000 claims description 2
- 239000011787 zinc oxide Substances 0.000 claims description 2
- 239000007795 chemical reaction product Substances 0.000 claims 1
- 230000003750 conditioning effect Effects 0.000 claims 1
- 125000004435 hydrogen atom Chemical class [H]* 0.000 claims 1
- 230000002194 synthesizing effect Effects 0.000 abstract description 4
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 abstract description 3
- 230000009466 transformation Effects 0.000 abstract 2
- 230000006315 carbonylation Effects 0.000 abstract 1
- 239000000463 material Substances 0.000 description 6
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 3
- 150000002431 hydrogen Chemical class 0.000 description 3
- 239000001301 oxygen Substances 0.000 description 3
- 229910052760 oxygen Inorganic materials 0.000 description 3
- 239000000047 product Substances 0.000 description 3
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 description 2
- 239000003034 coal gas Substances 0.000 description 2
- 150000001875 compounds Chemical class 0.000 description 2
- 238000005265 energy consumption Methods 0.000 description 2
- 238000010438 heat treatment Methods 0.000 description 2
- 238000004519 manufacturing process Methods 0.000 description 2
- 238000010926 purge Methods 0.000 description 2
- 238000000629 steam reforming Methods 0.000 description 2
- 230000009286 beneficial effect Effects 0.000 description 1
- 239000006227 byproduct Substances 0.000 description 1
- 229910052799 carbon Inorganic materials 0.000 description 1
- 239000003245 coal Substances 0.000 description 1
- 238000001816 cooling Methods 0.000 description 1
- 239000003607 modifier Substances 0.000 description 1
- 150000002894 organic compounds Chemical class 0.000 description 1
- 239000003209 petroleum derivative Substances 0.000 description 1
- 230000001105 regulatory effect Effects 0.000 description 1
- 238000000926 separation method Methods 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
- 230000000153 supplemental effect Effects 0.000 description 1
- 238000005038 synthesis gas manufacturing Methods 0.000 description 1
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Abstract
This invention relates to a method for improving methanol yield, comprising: do one or multi counter-water gas transformation reactions to synthetic gas(comprising hydrogen gas, carbon monoxide,carbon dioxide) to optimize the modulation of each component, especially to improve the CO concentration, so as to improve the space-time yield of the following methanol synthesizing. This method is specially useful in the component ratio modulation of synthetic gas produced by natural gas and steam transformation, and can be used in optimization of synthesizing reactions of methanol, dimethyl ether, liquid hydrocarbons and carbonylation raw gas.
Description
The technical field is as follows:
the technical field of the invention is the chemical field of coal, petroleum and natural gas
Technical background:
at present, the raw materials for producing oxygen-containing compounds such as methanol and the like worldwide mainly comprise two types, namely coal and natural gas. The natural gas is taken as a raw material, and the synthesis gas (hydrogen, carbon dioxide, carbon monoxide and the like) is mainly prepared by adopting the steam reforming reaction of the natural gas; the synthesis of oxygen-containing compounds such as methanol and the like by using coal as a raw material mainly adopts the technologies of water gas making and the like to prepare synthesis gas. The synthesis gas produced by the two methods is used for synthesizing oxygen-containing organic compounds such as methanol and the like. However, due to the conventional synthesis gas production technology and process, the ratio of the three components of hydrogen, carbon dioxide and carbon monoxide in the produced synthesis gas is not optimized for the subsequent synthesis reaction of methanol and the like. It is manifested by a high content of hydrogen and carbon dioxide, and an insufficient content of carbon monoxide. The gas composition ratio is unfavorable for the subsequent methanol synthesis reaction, and is mainly characterized by low reaction rate and low conversion per pass, so that the methanol synthesis reaction has large circulation volume and high energy consumption, and the excessive hydrogen and carbon dioxide need to be discharged, so that the discharged gas has large quantity, and the synthesis gas making process is not economical.
The invention content is as follows:
the invention relates to a method for optimally adjusting each component of synthesis gas (mixed gas consisting of hydrogen, carbon monoxide, carbon dioxide and the like) by performing one-section or multi-section reverse water-gas shift reaction on the synthesis gas, in particular to a method for improving the concentration of CO, thereby increasing the space-time yield of the subsequent synthesis reaction of methanol and the like and achieving the yield-increasing effect of methanol and the like. The method is particularly suitable for adjusting the component proportion of the synthesis gas prepared by the conversion of the steam of the natural gas, and can be suitable for the synthesis reaction of methanol, dimethyl ether, liquid hydrocarbon (GTL) and the like and the optimization of the raw material gas of the carbonylation reaction.
The catalyst adoptedby the invention is a modified Mn-Cu-Zn-Al catalyst, wherein the content of copper oxide is 20-50% (wt), the content of zinc oxide is 22-48% (wt), the content of aluminum oxide is 25-48% (wt), the content of manganese oxide is 5-20% (wt), and the content of a modifier is 3-10% (wt).
The reaction pressure adopted by the invention is normal pressure to 10MPa, and the specific selection of the reaction pressure depends on the manufacturing pressure of the synthesis gas and the synthesis pressure of the methanol and the like, and can be close to one of the two or between the two.
The reaction temperature is 300-800 ℃, and the specific temperature depends on the composition condition of the raw material synthesis gas, the regulation requirement of the synthesis gas and the like. The typical flow proposed by the invention is shown in the figure.
Description of the drawings:
rich in H2And CO2With make-up H and synthesis gas recycle gas (feed line 28)2And/or CO2Mixing gas (material line 12), then performing heat exchange and temperature rise through a tower gas heat exchanger 2(B20), then entering a heating furnace (B21) for heating to 300-800 ℃, then entering a reverse water gas shift reactor (B2) for reverse water gas shift reaction, cooling the reacted gas through a tower gas heat exchanger heat exchange 2(B20), further performing heat exchange and temperature reduction through a heat exchanger (B22), entering an alcohol-containing water separator (B23), separating out dry gas (material line 22) containing alcohol water, compressing the dry gas (material line 22) through compressors B24 and B10, mixing the dry gas with a fresh synthesizer (material line 24), entering a tower gas heat exchanger 1(B11) for heat exchange and temperature rise, and then enteringmethanolAnd a synthesis reactor (B1) for methanol synthesis reaction. After the reaction, the gas is gradually cooled by B11 and B12 and enters a crude methanol separator (B13) to separate crude methanol. After separation of the crude methanolThe dry gas (feed line 27), a portion of which is let down, and the remaining portion (feed line 28) is recycled to the reverse water gas shift reaction unit.
The specific implementation mode is as follows:
when the natural gas is used as raw material to produce methanol, dimethyl ether, liquid hydrocarbon (GTL) and other products, the natural gas is first converted into H-containing gas through steam conversion reaction2、CO、CO2The synthesis gas with equal components is utilized to further synthesize products such as methanol, dimethyl ether, liquid hydrocarbon (GTL) and the like.
Due to the limitations of synthesis gas manufacturing technology and process, the components of the prepared synthesis gas often do not meet the ideal requirements of the subsequent synthesis process on the raw material gas. For example, for methanol synthesis, the hydrogen-carbon proportionality coefficient R value [ R ═ (H)2-CO2)/(CO+CO2)]Is required to be in the range of 2.05-2.15, and meets the requirement of CO2The content of CO is required to be as high as possible under the condition that the concentration is not lower than 5 percent (vol), the R value of the synthetic gas prepared by the steam reforming reaction of natural gas is often larger than 3, and the component proportion of the synthetic gas is unreasonable.
On the other hand, in some cases with supplemental CO2In the process of producing synthesis gas, CO in the synthesis gas2Higher levels, althoughR values may be desirable, due to CO2The concentration is high, so that the synthesis speed of the product is low, the capacity of the device can not be fully exerted, the circulation gas quantity is increased, the purge gas quantity is large, and the unit material consumption is increased. At the same time, from CO2And H2By-product H in methanol synthesis2O, which causes the methanol concentration in the crude methanol to be reduced and increases the rectification load.
Based on CO in synthesis gas2、H2The invention utilizes the undesirable proportion condition of high content and low content of CO, and utilizes the inverse water gas shift catalytic reaction:
through reaction, CO is generated, the content of CO is increased, and the content of CO is reduced2And H2And (4) content. The gas after the reaction is used for synthesizing methanol, dimethyl ether, liquid hydrocarbon (GTL) and the like after water is separated. The optimized and regulated synthesis gas components show the following advantages for the whole process:
(1) the space-time yield of subsequent reactions such as methanol synthesis and the like is improved, so that the yield increasing effect is achieved;
(2) the circulating gas quantity is reduced, and the power consumption of the circulating compressor is reduced;
(3) the size of a subsequent synthesis device is reduced;
(4) the concentration of the crude methanol is improved, and the rectification load and the energy consumption are reduced;
(5) is beneficial to reducing the purge gas amount and reducing the material unit consumption.
Claims (5)
1. The invention relates to a method for optimally adjusting each component of synthesis gas (mixed gas consisting of hydrogen, carbon monoxide, carbon dioxide and the like) by performing one-section or multi-section reverse water-gas shift reaction on the synthesis gas, in particular to a method for improving the concentration of CO, thereby increasing the space-time yield of the subsequent synthesis reaction of methanol and the like and achieving the yield-increasing effect of methanol and the like. The method is particularly suitable for adjusting the component proportion of the synthesis gas prepared by the conversion of the steam of the natural gas, and can be suitable for the synthesis reaction of methanol, dimethyl ether, liquid hydrocarbon and the like and the optimization of the raw material gas of the carbonylation reaction.
2. The method of adjusting syngas composition of claim 1 wherein the CO in the syngas is produced by one or two stage reverse water gas shift reaction2The conversion rate of the reverse water gas conversion reaches 20-80%. By reverse water gas shift reaction, CO concentration (anhydrous dry basis concentration) in reaction product gas is increased, and CO is reduced2And H2Concentration (dry basis concentration on a dry basis).
3. The method of claim 1, wherein the catalyst is Mn-Cu-Zn-Al, the copper oxide content is 20-50% (wt), the zinc oxide content is 22-48% (wt), the aluminum oxide content is 25-48% (wt), and the manganese oxide content is 5-20% (wt).
4. The reverse water gas shift process of claim 1 for conditioning the synthesis gas components in combination with methanol synthesis. The method is characterized in that a reverse water gas shift catalytic reaction and a methanol synthesis reaction process are combined, the concentration of CO in the synthesis gas entering the methanol synthesis tower is increased through the reverse water gas shift reaction, the methanol synthesis rate is increased through the change, and the productivity of methanol synthesis equipment is improved. Typical examples of which are shown in the drawings of the specification, but are not limited to the flows in the drawings of the specification.
5. The method of adjusting the composition of synthesis gas according to claim 1, characterized in that the one or more stages of reverse water gas shift catalytic reaction are carried out in an adiabatic reactor or a fire tube reactor.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN 200610020836 CN1880414A (en) | 2006-05-17 | 2006-05-17 | Method for optimization of synthetic gas components by reversed water-gas shift reaction technology and flow therefor |
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| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN 200610020836 CN1880414A (en) | 2006-05-17 | 2006-05-17 | Method for optimization of synthetic gas components by reversed water-gas shift reaction technology and flow therefor |
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| CN1880414A true CN1880414A (en) | 2006-12-20 |
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| CN103242134A (en) * | 2013-04-25 | 2013-08-14 | 深圳市炬能生物质气化科技有限公司 | Pyrolysis gasification and purification method of household garbage |
| CN103418392A (en) * | 2012-05-14 | 2013-12-04 | 浙江海洋学院 | Reverse water gas shift catalyst and preparation method thereof |
| CN103687665A (en) * | 2011-05-11 | 2014-03-26 | 奇努克终极回收有限公司 | Synthesis gas processing and system using copper catalyst in two step reactions at475-525 DEG C and 250-290 DEG C |
| CN104471037A (en) * | 2012-06-29 | 2015-03-25 | 沙特基础工业公司 | Method of forming a syngas mixture |
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| CN107285995A (en) * | 2016-04-12 | 2017-10-24 | 中国石油化工股份有限公司 | The method that methanol is prepared using carbon dioxide and hydrogen |
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| CN109096050A (en) * | 2017-06-21 | 2018-12-28 | 中国石油化工股份有限公司 | Utilize the method for carbon dioxide and hydrogen gas production methanol |
| CN111348622A (en) * | 2020-03-04 | 2020-06-30 | 中国海洋石油集团有限公司 | Preparation system and preparation method for preparing synthesis gas from carbon-rich natural gas |
| CN113824153A (en) * | 2021-10-29 | 2021-12-21 | 西安交通大学 | Electric power energy system under underground space supports |
| CN114015472A (en) * | 2020-07-15 | 2022-02-08 | 中国石油大学(华东) | Reverse water-gas shift reaction and coal-to-methanol process coupling water electrolysis hydrogen production |
| CN116283489A (en) * | 2021-12-10 | 2023-06-23 | 国家能源投资集团有限责任公司 | Method and system for producing methanol |
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| CN103687665B (en) * | 2011-05-11 | 2015-08-12 | 奇努克终极回收有限公司 | The synthesis gas process of the use copper catalyst of two-step reaction and system at 475-525 DEG C and 250-290 DEG C |
| CN103418392A (en) * | 2012-05-14 | 2013-12-04 | 浙江海洋学院 | Reverse water gas shift catalyst and preparation method thereof |
| CN103418392B (en) * | 2012-05-14 | 2015-10-28 | 浙江海洋学院 | A kind of Reversed Water-gas Shift Catalysts and its preparation method |
| CN104471037A (en) * | 2012-06-29 | 2015-03-25 | 沙特基础工业公司 | Method of forming a syngas mixture |
| CN103242134A (en) * | 2013-04-25 | 2013-08-14 | 深圳市炬能生物质气化科技有限公司 | Pyrolysis gasification and purification method of household garbage |
| CN105518111A (en) * | 2013-07-31 | 2016-04-20 | 沙特基础工业公司 | A process for the production of olefins through fischer-tropsch based synthesis |
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