CN102516029B - Method for synthesising methanol by complete cycle of carbon monoxide, carbon dioxide and hydrogen - Google Patents
Method for synthesising methanol by complete cycle of carbon monoxide, carbon dioxide and hydrogen Download PDFInfo
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- CN102516029B CN102516029B CN201110426194.8A CN201110426194A CN102516029B CN 102516029 B CN102516029 B CN 102516029B CN 201110426194 A CN201110426194 A CN 201110426194A CN 102516029 B CN102516029 B CN 102516029B
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- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E50/00—Technologies for the production of fuel of non-fossil origin
- Y02E50/10—Biofuels, e.g. bio-diesel
Abstract
The invention discloses a method for synthesising methanol by the complete cycle of carbon monoxide, carbon dioxide and hydrogen, comprising the following steps of: adjusting the content of carbon dioxide in raw material gases for synthesising methanol to control the intensity of heat release in a reaction for synthesising methanol, so as to achieve the matching of heat released from the synthesis reaction and the heat transfer of a methanol synthesis tower, wherein the concentration in mole percentage of carbon dioxide in the synthesising gases is 10.0-20.5%; performing gas-liquid separation and boosting on the unreacted carbon monoxide, carbon dioxide and hydrogen after catalytic reaction on the raw material gases consisting of carbon monoxide, carbon dioxide and hydrogen, and then returning all the unreacted gases to the inlet of the synthesis tower; and adjusting the ratio of the carbon monoxide to the carbon dioxide to the hydrogen in a fresh gas, and enabling the synthesising gases entering in the synthesis tower to satisfy a hydrogen-carbon ratio of 2.00-2.80. The method disclosed by the invention realizes the complete cycle of carbon monoxide, carbon dioxide and hydrogen, reduces energy and the losses of non-renewable resources, optimizes the process technology for synthesising methanol, and decreases production cost.
Description
Technical field
The present invention relates to the processing method of synthetic gas synthesizing methanol in chemical field, relate in particular to the synthetic gas methanol synthetizing technology of mesolow (not containing inert nitrogen gas) high carbon dioxide content.
Background technology
Along with economic fast development and petroleum resources are petered out, substitute energy has become one of center of gravity of China's science technology and industry development.In the face of resources supplIes and the national conditions of China's " oil starvation, weak breath, coal resources are relatively abundant ", alcohol-ether fuel has become a kind of substitute energy that has development prospect.
Mesolow synthesizing methanol technology is one of important Technology of coal chemical technology.In recent years, China's mesolow synthesizing methanol industrial development is rapid, and capacity and demand amount all increases simultaneously and rapidly.Synthesizing methanol full scale plant scale effect is obvious, and methyl alcohol maximizes and produces is the inexorable trend of following domestic development of carbinol industry.The maximization of methyl alcohol is produced the higher requirement of catalst for synthesis of methanol proposition, also requires further to improve synthesizing methanol reaction process, to ensure normally carrying out of methanol industry production simultaneously.
Existing methyl alcohol maximization production equipment mainly adopts the synthetic gas synthesizing methanol of the carbon monoxide that contains nitrogen, carbonic acid gas, hydrogen.The reaction of co hydrogenation synthesizing methanol is strong exothermal reaction, response intensity is larger, liberated heat is just more, thereby the amplitude that causes catalst for synthesis of methanol bed temperature to raise is larger, cause to a certain extent catalst for synthesis of methanol overheated and occur sintering, thereby cause catalyzer to lose activity fast.For ensureing the life-span of catalyzer, in synthetic gas, add a large amount of nitrogen, reduce the intensity of reaction, to ensure that reaction heat is moved out of.
CO+2H
2→CH
3OH +90.64KJ/mol
CO
2+3H
2→CH
3OH+H
2O +48.02KJ/mol
In traditional synthesizing methanol full scale plant due to the existence of inert nitrogen gas in synthetic gas, and synthetic gas recycle ratio is relatively large, a nitrogen content in circulation synthetic gas raises along with the increase of cycle index, therefore, need in process of production regularly to give off the venting of speeding and meet the requirement of building-up reactions hydrogen-carbon ratio to ensure the composition of raw material inlet tower gas.In full scale plant, the synthetic gas that contains nitrogen that gives off system generally arrives the more than 10% of circulating flow rate.Not only cause the pollution of environment, and wasted resource.
Summary of the invention
The main purpose of patent of the present invention is to overcome the problem of above existence, a kind of method of carbon monoxide, carbonic acid gas and hydrogen synthesising methanol by complete cycle is provided, to realize the recycle to extinction of unstripped gas carbon monoxide, carbonic acid gas, hydrogen, reduce the loss of energy and Nonrenewable resources, optimize methanol synthetizing technology technology, and reduce production costs.
In order to reach above object, the present invention adopts following technical scheme:
A kind of method of carbon monoxide, carbonic acid gas and hydrogen synthesising methanol by complete cycle, the content that is adjusted in carbonic acid gas in the unstripped gas of synthesizing methanol is controlled the intensity of synthesizing methanol exothermic heat of reaction, reaches the mating of transfer of heat of building-up reactions liberated heat and methyl alcohol synthetic reactor; Wherein, the mole percent concentration ratio of carbonic acid gas in synthetic gas is 10.0～20.5%;
Unstripped gas carbon monoxide, carbonic acid gas and hydrogen unreacted carbon monoxide, carbonic acid gas and hydrogen after catalyzed reaction all return to the entrance of synthetic tower through gas-liquid separation, after boosting;
It is 2.00～2.80 that the synthetic gas that regulates the ratio of carbon monoxide in virgin gas, carbonic acid gas and hydrogen to make to enter synthetic tower meets hydrogen-carbon ratio.
Preferably, to meet hydrogen-carbon ratio be 2.67 to synthetic gas.
Preferably, the mole percent concentration ratio of carbonic acid gas in synthetic gas is 20.0%.
The mole percent concentration ratio of carbon monoxide in synthetic gas is 6.0～18.0%.
Preferably, the mole percent concentration ratio of carbon monoxide in synthetic gas is 10.0%.
The applicable temperature of building-up reactions is 200～280 DEG C; Applicable pressure is 4.5～8.5MPa; Gas phase air speed is 5000～12000h
-1.
Preferably, the applicable temperature of building-up reactions is 250 DEG C; Applicable pressure is 8.0MPa; Gas phase air speed is 10000h
- 1.
The applicable catalyzer main ingredient of building-up reactions is CuO/ZnO/Al
2o
3.
Can find out from the chemical reaction of carbon monoxide, synthesizing methanol by hydrogenating carbon dioxide, carbon dioxide-synthesized methanol exothermic heat of reaction amount is relatively little, and, because the chemical reaction inertia of carbonic acid gas is stronger, therefore in synthesizing methanol reaction, the heat that the change in concentration of carbonic acid gas can regulate synthesizing methanol reaction to generate, in addition, carbonic acid gas can well shift the reaction Heat of Formation of carbon monoxide synthesizing methanol, reduce the temperature rise amplitude of beds, thus the catalytic activity and the work-ing life that have well kept catalyzer.
The mating of transfer of heat that reaches building-up reactions liberated heat and methyl alcohol synthetic reactor,, can effectively migrate out the reaction Heat of Formation of beds, reduces beds temperature rise amplitude, thereby well keep activity and the stability of catalyzer; Unreacted carbon monoxide, carbonic acid gas and hydrogen all return to the entrance of synthetic tower through gas-liquid separation, after boosting, due to nonnitrogenous gas in reaction cycle gas, therefore, reduced the loss of carbon monoxide, carbonic acid gas in the unstripped gas that the bleed air exhaust of speeding in traditional methanol synthetizing technology causes;
Synthetic gas meets the requirement of hydrogen-carbon ratio, can keep the intensity of synthesizing methanol reaction and methanol output stable.
Described in the application, the beneficial effect of technology is:
The method of the invention has realized the recycle to extinction of unstripped gas carbon monoxide, carbonic acid gas, hydrogen, has reduced the loss of energy and Nonrenewable resources, has optimized methanol synthetizing technology technology, and has reduced production cost.
Embodiment
Below in conjunction with embodiment, foregoing invention content of the present invention is described in further detail.
But this should be interpreted as to the scope of the above-mentioned theme of the present invention only limits to following embodiment.Without departing from the idea case in the present invention described above, according to ordinary skill knowledge and customary means, make various replacements and change, all should comprise within the scope of the invention.
Embodiment 1
Synthesizing methanol reaction Raw inlet tower gas body consists of: CO8.0%, CO
215.13%, H
276.87%, raw material inlet tower gas hydrogen-carbon ratio is 2.67, and temperature of reaction is 250 DEG C, and reaction pressure is 8.0MPa, and reaction velocity is 10000h
-1, adopt 200mlCuO/ZnO/Al
2o
3industry catalst for synthesis of methanol is fixed a catalyzed reaction.After gas-liquid separation, exhaust gas consists of: CO, 3.00%; CO
2, 17.92%; H
2, 79.08%, exhaust gas amount is 1.60Nm
3/ h.Under existing industrial catalst for synthesis of methanol effect, the per pass conversion of carbon monoxide is 70.00%, and the per pass conversion of carbonic acid gas is 5.19%, and it is 676.84kj/h that heat is emitted in reaction.In reaction process, average temperature rising is 5 DEG C, and unreacted raw material and gaseous products methyl alcohol, water etc. are taken away heat and is about 13.25kj/h, and the ratio of shared reaction Heat of Formation is about 1.96%.The amount of supplementing virgin gas is 0.40Nm
3/ h, the consisting of of virgin gas: CO, 28.08%; CO
2, 3.94%; H
2, 67.98%, the hydrogen-carbon ratio of the inlet tower gas after adjustment is 2.67.Reaction exhaust gas and virgin gas reenter synthetic tower after mixing and recycle after boosting.
Embodiment 2
Synthesizing methanol reaction Raw inlet tower gas body consists of: CO, 6.0%; CO
2, 20.5%; H
2, 73.50%.Raw material inlet tower gas hydrogen-carbon ratio is 2.0, and temperature of reaction is 240 DEG C, and reaction pressure is 8.5MPa, and reaction velocity is 10000h
-1, adopt 200mlCuO/ZnO/Al
2o
3industry catalst for synthesis of methanol is fixed a catalyzed reaction.After gas-liquid separation, exhaust gas consists of: CO, 2.51%; CO
2, 23.11%; H
2, 74.37%, exhaust gas amount is 1.67Nm
3/ h.Under existing industrial catalst for synthesis of methanol effect, the per pass conversion of carbon monoxide is 65.00%, and the per pass conversion of carbonic acid gas is 5.8%, and it is 422.38kj/h that heat is emitted in reaction.In reaction process, average temperature rising is 2 DEG C, and unreacted raw material and gaseous products methyl alcohol, water etc. are taken away heat and is about 8.30kj/h, and the ratio of shared reaction Heat of Formation is about 2.02%.The amount of supplementing virgin gas is 0.33Nm
3/ h, the consisting of of virgin gas: CO, 23.70%; CO
2, 7.22%; H
2, 69.07%, the hydrogen-carbon ratio of the inlet tower gas after adjustment is 2.0.Reaction exhaust gas and virgin gas mixing reenter synthetic tower and recycle after boosting.
Embodiment 3
Synthesizing methanol reaction Raw inlet tower gas body consists of: CO, 10.0%; CO
2, 12.90%; H
2, 77.10%.Raw material inlet tower gas hydrogen-carbon ratio is 2.8, and temperature of reaction is 200 DEG C, and reaction pressure is 8.0MPa, and reaction velocity is 5000h
-1, adopt 200mlCuO/ZnO/Al
2o
3industry catalst for synthesis of methanol is fixed a catalyzed reaction.After gas-liquid separation, exhaust gas consists of: CO, 6.06%; CO
2, 14.88%; H
2, 79.06%, exhaust gas amount is 0.82Nm
3/ h.Under existing industrial catalst for synthesis of methanol effect, the per pass conversion of carbon monoxide is 50.00%, and the per pass conversion of carbonic acid gas is 4.93%, and it is 170.24kj/h that heat is emitted in reaction.In reaction process, average temperature rising is 2.5 DEG C, and unreacted raw material and gaseous products methyl alcohol, water etc. are taken away heat and is about 3.28kj/h, and the ratio of shared reaction Heat of Formation is about 1.93%.The amount of supplementing virgin gas is 0.18Nm
3/ h, the consisting of of virgin gas: CO, 28.52%; CO
2, 3.61%; H
2, 67.87%, the hydrogen-carbon ratio of the inlet tower gas after adjustment is 2.8.Reaction exhaust gas and virgin gas mixing reenter synthetic tower and recycle after boosting.
Embodiment 4
Synthesizing methanol reaction Raw inlet tower gas body consists of: CO, 18.0%; CO
2, 11.50%; H
2, 70.50%.Raw material inlet tower gas hydrogen-carbon ratio is 2.0, and temperature of reaction is 250 DEG C, and reaction pressure is 8.0MPa, and reaction velocity is 12000h
-1, adopt 200mlCuO/ZnO/Al
2o
3industry catalst for synthesis of methanol is fixed a catalyzed reaction.After gas-liquid separation, exhaust gas consists of: CO, 13.45%; CO
2, 14.91%; H
2, 71.64%, exhaust gas amount is 1.77Nm
3/ h.Under existing industrial catalst for synthesis of methanol effect, the per pass conversion of carbon monoxide is 45.00%, and the per pass conversion of carbonic acid gas is 4.60%, and it is 1174.8kj/h that heat is emitted in reaction.In reaction process, average temperature rising is 8 DEG C, and unreacted raw material and gaseous products methyl alcohol, water etc. are taken away heat and is about 24.48kj/h, and the ratio of shared reaction Heat of Formation is about 2.08%.The amount of supplementing virgin gas is 0.63Nm
3/ h, the consisting of of virgin gas: CO, 30.66%; CO
2, 2.00%; H
2, 67.33%, the hydrogen-carbon ratio of the inlet tower gas after adjustment is 2.0.Reaction exhaust gas and virgin gas mixing reenter synthetic tower and recycle after boosting.
Embodiment 5
Synthesizing methanol reaction Raw inlet tower gas body consists of: CO, 15.0%; CO
2, 10.00%; H
2, 75.00%.Raw material inlet tower gas hydrogen-carbon ratio is 2.6, and temperature of reaction is 210 DEG C, and reaction pressure is 4.5MPa, and reaction velocity is 12000h
-1, adopt 200mlCuO/ZnO/Al
2o
3industry catalst for synthesis of methanol is fixed a catalyzed reaction.After gas-liquid separation, exhaust gas consists of: CO, 11.31%; CO
2, 11.81%; H
2, 76.88%, exhaust gas amount is 1.91Nm
3/ h.Under existing industrial catalst for synthesis of methanol effect, the per pass conversion of carbon monoxide is 40.00%, and the per pass conversion of carbonic acid gas is 6.00%, and it is 870.22kj/h that heat is emitted in reaction.In reaction process, average temperature rising is 6.0 DEG C, and unreacted raw material and gaseous products methyl alcohol, water etc. are taken away heat and is about 18.44kj/h, and the ratio of shared reaction Heat of Formation is about 2.12%.The amount of supplementing virgin gas is 0.49Nm
3/ h, the consisting of of virgin gas: CO, 29.41%; CO
2, 2.94%; H
2, 67.65%, the hydrogen-carbon ratio of the inlet tower gas after adjustment is 2.6.Reaction exhaust gas and virgin gas mixing reenter synthetic tower and recycle after boosting.
Embodiment 6
Synthesizing methanol reaction Raw inlet tower gas body consists of: CO, 11.0%; CO
2, 15.00%; H
2, 74.00%.Raw material inlet tower gas hydrogen-carbon ratio is 2.27, and temperature of reaction is 250 DEG C, and reaction pressure is 5.5MPa, and reaction velocity is 10000h
-1, adopt 200mlCuO/ZnO/Al
2o
3industry catalst for synthesis of methanol is fixed a catalyzed reaction.After gas-liquid separation, exhaust gas consists of: CO, 7.13%; CO
2, 17.47%; H
2, 75.40%, exhaust gas amount is 1.60Nm
3/ h.Under existing industrial catalst for synthesis of methanol effect, the per pass conversion of carbon monoxide is 48.00%, and the per pass conversion of carbonic acid gas is 6.50%, and it is 638.16kj/h that heat is emitted in reaction.In reaction process, average temperature rising is 5 DEG C, and unreacted raw material and gaseous products methyl alcohol, water etc. are taken away heat and is about 13.26kj/h, and the ratio of shared reaction Heat of Formation is about 2.08%.The amount of supplementing virgin gas is 0.39Nm
3/ h, the consisting of of virgin gas: CO, 26.75%; CO
2, 4.94%; H
2, 68.31%, the hydrogen-carbon ratio of the inlet tower gas after adjustment is 2.27.Reaction exhaust gas and virgin gas mixing reenter synthetic tower and recycle after boosting.
Embodiment 7
Synthesizing methanol reaction Raw inlet tower gas body consists of: CO, 8.0%; CO
2, 18.00%; H
2, 74.00%.Raw material inlet tower gas hydrogen-carbon ratio is 2.15, and temperature of reaction is 280 DEG C, and reaction pressure is 4.5MPa, and reaction velocity is 5000h
-1, adopt 200mlCuO/ZnO/Al
2o
3industry catalst for synthesis of methanol is fixed a catalyzed reaction.After gas-liquid separation, exhaust gas consists of: CO, 3.99%; CO
2, 20.76%; H
2, 75.25%, exhaust gas amount is 0.80Nm
3/ h.Under existing industrial catalst for synthesis of methanol effect, the per pass conversion of carbon monoxide is 60.00%, and the per pass conversion of carbonic acid gas is 7.40%, and it is 394.96kj/h that heat is emitted in reaction.In reaction process, average temperature rising is 6 DEG C, and unreacted raw material and gaseous products methyl alcohol, water etc. are taken away heat and is about 8.10kj/h, and the ratio of shared reaction Heat of Formation is about 2.05%.The amount of supplementing virgin gas is 0.20Nm
3/ h, the consisting of of virgin gas: CO, 24.33%; CO
2, 6.75%; H
2, 68.92%, the hydrogen-carbon ratio of the inlet tower gas after adjustment is 2.15.Reaction exhaust gas and virgin gas mixing reenter synthetic tower and recycle after boosting.
Comparative example
Synthesizing methanol reaction Raw inlet tower gas body consists of: CO, 16.23%; CO
2, 6.74%; N
2, 8.35%; H
2, 68.08%.Hydrogen-carbon ratio is 2.67, and temperature of reaction is 250 DEG C, and reaction pressure is 8.0MPa, and reaction velocity is 10000h
-1, adopt 200mlCuO/ZnO/Al
2o
3industry catalst for synthesis of methanol is fixed a catalyzed reaction.After gas-liquid separation, exhaust gas consists of: CO, 8.77%; CO
2, 9.50%; N
2, 12.55%; H
2, 69.18%, exhaust gas amount is 1.33Nm
3/ h.Under existing industrial catalst for synthesis of methanol effect, the per pass conversion of carbon monoxide is 64.06%, and the per pass conversion of carbonic acid gas is 6.19%, and it is 1256.59kj/h that heat is emitted in reaction.In reaction process, average temperature rising is 10 DEG C, and unreacted raw material and gaseous products methyl alcohol, water etc. are taken away heat and is about 121.82kj/h, and the ratio of shared reaction Heat of Formation is about 1.94%.The amount of supplementing virgin gas is 0.67Nm
3/ h, the consisting of of virgin gas: CO, 31.64%; CO
2, 1.27%; H
2, 67.09%, the hydrogen-carbon ratio of the inlet tower gas after adjustment is 2.67.Reaction exhaust gas and virgin gas mixing reenter synthetic tower and carry out after boosting.Consisting of after one hour gas-liquid separator separates of synthetic gas circulation: CO, 6.18%; CO
2, 10.79%; N
2, 23.39%; H
2, 59.64%;～2.5% methyl alcohol;～0.5% water.The bleed air exhaust of speeding amount is :～0.2Nm
3/ h, wherein loses methyl alcohol 7.24g/h, carbon monoxide 0.01236Nm
3/ h.
Claims (5)
1. a method for carbon monoxide, carbonic acid gas and hydrogen synthesising methanol by complete cycle, is characterized in that:
The content that is adjusted in carbonic acid gas in the unstripped gas of synthesizing methanol is controlled the intensity of synthesizing methanol exothermic heat of reaction, reaches the mating of transfer of heat of building-up reactions liberated heat and methyl alcohol synthetic reactor; Wherein, the mole percent concentration ratio of carbonic acid gas in synthetic gas is 10.0～20.5%, and the mole percent concentration ratio of carbon monoxide in synthetic gas is 6.0～18.0%;
Unstripped gas carbon monoxide, carbonic acid gas and hydrogen unreacted carbon monoxide, carbonic acid gas and hydrogen after catalyzed reaction all return to the entrance of synthetic tower through gas-liquid separation, after boosting;
Regulate the ratio of carbon monoxide in virgin gas, carbonic acid gas and hydrogen, it is 2.00～2.80 that the synthetic gas that makes to enter synthetic tower meets hydrogen-carbon ratio;
The applicable temperature of building-up reactions is 200～280 DEG C; Applicable pressure is 4.5～8.5MPa; Gas phase air speed is 5000～12000h
-1; The applicable catalyzer main ingredient of building-up reactions is CuO/ZnO/Al
2o
3.
2. the method for carbon monoxide according to claim 1, carbonic acid gas and hydrogen synthesising methanol by complete cycle, is characterized in that: it is 2.67 that synthetic gas meets hydrogen-carbon ratio.
3. the method for carbon monoxide according to claim 2, carbonic acid gas and hydrogen synthesising methanol by complete cycle, is characterized in that: the mole percent concentration ratio of carbonic acid gas in synthetic gas is 20.0%.
4. the method for carbon monoxide according to claim 1, carbonic acid gas and hydrogen synthesising methanol by complete cycle, is characterized in that: the mole percent concentration ratio of carbon monoxide in synthetic gas is 10.0%.
5. the method for carbon monoxide according to claim 1, carbonic acid gas and hydrogen synthesising methanol by complete cycle, is characterized in that: the applicable temperature of building-up reactions is 250 DEG C; Applicable pressure is 8.0MPa; Gas phase air speed is 10000h
-1.
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| CN104672056A (en) * | 2013-11-30 | 2015-06-03 | 崔胜民 | Automatic carbon supplementing product-increasing and consumption-reducing process of methanol production |
| EP3208258A1 (en) * | 2016-02-16 | 2017-08-23 | Fundació Privada Institut Català d'Investigació Química (ICIQ) | Methanol production process |
| CN112142558A (en) * | 2020-08-31 | 2020-12-29 | 南京聚拓化工科技有限公司 | Single-power double-circulation methanol production method |
| CN112194566A (en) * | 2020-09-29 | 2021-01-08 | 浙江工业大学 | Device and process for synthesizing methanol based on carbon dioxide hydrogenation |
| CN114907186A (en) * | 2022-04-24 | 2022-08-16 | 中国成达工程有限公司 | Method for directly preparing methanol from carbon dioxide and hydrogen |
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| CN101386564B (en) * | 2008-10-29 | 2011-12-28 | 西南化工研究设计院 | Technique for synthesizing methanol by hydrogen and carbon dioxide |
| CN101429098B (en) * | 2008-12-03 | 2011-10-26 | 西南化工研究设计院 | Method for synthesis of methanol with CO, CO2 and H#[-2] |
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