CN102229827A - Method for producing synthetic natural gas - Google Patents
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Abstract
The invention discloses a method for producing synthetic natural gas, which belongs to the technical field of coal chemistry and new energy. The method for producing the synthetic natural gas comprises: dividing raw material gases from a general gas source into low-carbon synthetic gases with a hydrogen to carbon ratio, namely a (H2-CO2) to (H2+CO2) ratio, being 4.5 to 15.0 and high-carbon synthetic gases with a hydrogen to carbon ratio being 0 to 2.0; according to a reaction temperature requirement, mixing the low-carbon synthetic gases with steam at certain flow, allowing the mixed gases to enter a primary thermal-insulation reactor to undergo a methanation reaction, subjecting the gases from the primary thermal-insulation reactor to heat exchange, mixing the gases with the high-carbon synthetic gases at a certain flow, and allowing the newly mixed gases into a secondary thermal-insulation reactor to undergo a methanation reaction; repeating the previous process for several times; and finally, obtaining the synthetic natural gas by processes of heat exchange, cooling, drying, compression and the like. The method has the characteristics that: (1) circulating equipment is not used; (2) all reactions are performed in thermal-insulation reactors, multiple stages of reactors are connected in series, and the reaction space velocity is high; and (3) the hydrogen to carbon ratio of the whole reaction system can be regulated easily, and the methane content in the product gas may reach over 95 percent.
Description
Technical field
The present invention relates to a kind of method of production synthetic natural gas, belong to Coal Chemical Industry, technical field of new energies.
Background technology
Sweet natural gas is the clean energy of generally acknowledging, conveying, easy to use, and consumption is increasing, and natural gas source is fewer and feweri.With the coal is raw material, by explained hereafter synthetic natural gases (or instead of natural gas) such as gasification, conversion, methanations, is a kind of good arbitrary way to natural gas supply, is particularly suitable for the endowment of resources of China's " rich coal, oil starvation, weak breath ".
With the coal is the raw material production synthetic natural gas, is the comparatively complicated Technology that energy form transforms, and has only the U.S. one cover industrialized unit to be arranged in operation at present.This Technology comprises: processes such as gasification, conversion, acid gas removal, methanation, drying, compression, wherein methanation process much needs research, improvements in addition.Methanation reaction is as follows:
CO+3H
2＝CH
4+H
2O ΔH＝-206kJ/mol(1)
CO
2+4H
2＝CH
4+2H
2O ΔH＝-165kJ/mol(2)
Methanation is the chemical reaction that carbon monoxide, carbonic acid gas and H-H reaction generate methane, belong to strong exothermal reaction, methanation reaction heat is about 20% of synthetic gas total heating value, therefore for high efficiency this part heat energy that utilizes, generally all adopt the high-temperature heat insulation reactor, the high-grade superheated vapour of by-product.The temperature rise under adiabatic condition of methanation reaction process is very high, is guard catalyst, and temperature of reaction also needs strict control, generally adopts product gas flow round-robin method dilution fresh synthesis gas, reduces CO and CO in the unstripped gas
2Concentration, to reach the purpose of control reaction temperature.All adopt product gas flow round-robin method control reaction temperature as patent US4016189, US4205961, US4298694, CN200910085337.6, CN200910058611.0, CN201010173181.x etc.Reduce the wherein method of CO concentration of raw material by the circulation of product gas, comparatively effective to control reaction temperature, but increased operation energy consumption and facility investment greatly.
CN101775319A has proposed a kind of methanation process without recycle unit, adopts the water-cooled shell-and-tube reactor, preferably control reaction temperature.But this technology institute byproduct steam grade is lower, and utilization of Heat of Reaction efficient is not high; Owing to be subjected to the restriction of heat transfer rate, the air speed of reaction is less, conversion unit is comparatively huge in addition.
CN201010200095.5 has proposed a kind of synthetic natural gas technology without recycle unit, and the heat exchange type reactor is adopted in first step reaction, back series connection adiabatic reactor.
CN101880558A has proposed a kind of thermal insulation that circulates, can accurately control the scheme of hydrogen-carbon ratio, in preceding what adiabatic reactor, unstripped gas is a hydrogen-carbon ratio a little more than 3 synthetic gas, general hydrogen-carbon ratio is 3.0-3.3, in the reaction of back, add a certain amount of high concentration CO 2 gas, as the means of regulating hydrogen-carbon ratio.
Summary of the invention
The invention provides a kind of method of production synthetic natural gas, this method is without recycle unit, adopt fixed bed adiabatic formula reactor, can effectively solve methanation reaction temperature controlling problem, keep the advantage of adiabatic reaction technology by-product higher-grade steam and big air speed operation simultaneously.
The technical solution used in the present invention is: a kind of method of production synthetic natural gas may further comprise the steps:
(1) gasification by coal or other carbon raw material obtains unstripped gas, or the gas that is rich in carbon monoxide of other approach acquisition, through purifying treatment, removes behind catalyzer and the deleterious impurity of product gas, as total source of the gas;
(2) unstripped gas that total source of the gas is come is divided into two portions, and wherein a part obtains hydrogen-carbon ratio (H by hydrosphere transformation, carbonic acid gas acid gas removal, purification process and adjusting hydrogen-carbon ratio
2-CO
2)/(H
2+ CO
2The low-carbon (LC) synthetic gas of)=4.5-15.0, another part gas obtain the high-carbon synthetic gas that hydrogen-carbon ratio is 0-2.0;
(3) according to the requirement of catalyzer to temperature of reaction, after the vapor mixing of described low-carbon (LC) synthetic gas and certain flow, enter first step adiabatic reactor, carry out methanation reaction;
(4) gas that comes out from first step adiabatic reactor after heat exchange, adjusting temperature, mixes with the high-carbon synthetic gas of certain flow, enters second stage adiabatic reactor, carries out methanation reaction;
(5) process of step (4) repeats, and equals or near 3.0, through after the heat exchange, enters the next stage adiabatic reactor up to the hydrogen-carbon ratio of the gas that comes out from reactor, proceeds methanation reaction;
(6) gas that comes out from top reactor, through heat exchange, cooling, gas-liquid separation etc., remove the most of water in the air-flow, appropriate supplement adds low-carbon (LC) synthetic gas or the high-carbon synthetic gas in the above-mentioned step (2), accurately regulate the hydrogen-carbon ratio of air-flow, make hydrogen-carbon ratio reach 2.95-3.05, enter follow-up adiabatic reactor;
(7) from processes such as the heat exchange of last step adiabatic reactor effluent air process, cooling, drying and compressions, obtain the synthetic natural gas product.
It is the 2-8 level that described synthetic natural gas process adopts adiabatic reactor progression, and general adiabatic reactor progression changes with the composition of synthetic gas and the use temperature scope of catalyzer.
The invention has the beneficial effects as follows: it is the high-carbon synthetic gas of 0-2.0 that the unstripped gas that the method for this production synthetic natural gas is come total source of the gas is divided into low-carbon (LC) synthetic gas and the hydrogen-carbon ratio that hydrogen-carbon ratio is 4.5-15.0.According to temperature of reaction, after described low-carbon (LC) synthetic gas and the vapor mixing that need regulate, enter first step adiabatic reactor, carry out methanation reaction, the gas that comes out from first step adiabatic reactor, through after the heat exchange, mix with the high-carbon synthetic gas of certain flow, enter second stage adiabatic reactor, carry out methanation reaction, this process repeats repeatedly, passes through heat exchange, cooling, drying and compression process at last, obtains the synthetic natural gas product.The characteristics of this method are: (1) is without recycle unit; (2) all adopt adiabatic reactor, plural serial stage, reaction velocity is big; (3) be easy to regulate the hydrogen-carbon ratio of entire reaction system, methane content can reach more than 95% in the product gas.
Embodiment
Embodiment 1.
With brown coal is raw material, and coal gas consists of (V%) after the gas making:
H2:50.7; CO:34.1; 6O2:3.9; CH4:10.9; Rare gas element: 0.4
Hydrogen-carbon ratio is: (50.7-3.9)/(34.1+3.9)=1.23, and as the high-carbon synthetic gas.
With above-mentioned gas～69% carry out conversion, decarbonization process and handle after, synthetic gas (V%) composed as follows:
H
2: 75.0; CO:9.8; CO
2: 3.9; CH
4: 10.9; Rare gas element: 0.4
Hydrogen-carbon ratio is: (75.0-3.9)/and (9.8+3.9=5.18 is as the low-carbon (LC) synthetic gas.
As mentioned above, unstripped gas is divided into low-carbon (LC) synthetic gas and high-carbon synthetic gas two portions, and wherein the low-carbon (LC) synthetic gas accounts for 69% of total tolerance, and the high-carbon synthetic gas accounts for 31% of total tolerance, and total hydrogen-carbon ratio is about 2.994.Raw gas pressure is 2.0MPa.
The methanation reaction process is as follows:
(1) whole low-carbon (LC) synthetic gas are through (temperature 240-260 ℃) after the heat exchange, add the steam (temperature 240-260 ℃) that accounts for low-carbon (LC) synthetic gas flow about 15%, enter first step adiabatic reactor, carry out methanation reaction, the temperature of reactor outlet eluting gas is 690-710 ℃.
(2) behind first step adiabatic reactor effluent air process vapor superheater, waste heat boiler, interchanger, mix with the high-carbon synthetic gas of certain flow, mixed temperature is 240-260 ℃, enter second stage adiabatic reactor, proceed methanation reaction, the temperature of reactor outlet eluting gas is 690-710 ℃.
(3) behind second stage adiabatic reactor effluent air process vapor superheater, waste heat boiler, mix with the high-carbon synthetic gas of certain flow, mixed temperature is 240-260 ℃, enter third stage adiabatic reactor, proceed methanation reaction, the temperature of reactor outlet eluting gas is 690-710 ℃.
(4) behind third stage adiabatic reactor effluent air process vapor superheater, waste heat boiler, mix with the high-carbon synthetic gas of certain flow, mixing the back temperature is 240-260 ℃, enter fourth stage adiabatic reactor, proceed methanation reaction, the temperature of reactor outlet eluting gas is 680-700 ℃.
(5) behind fourth stage adiabatic reactor effluent air process vapor superheater, waste heat boiler, be cooled to 240-260 ℃, enter the level V adiabatic reactor, proceed methanation reaction, the temperature of reactor outlet eluting gas is 480-500 ℃.
(6) from level V adiabatic reactor effluent air through waste heat boiler, cooling after, be cooled to 45-60 ℃, gas-liquid separation, remove most of moisture.Add low-carbon (LC) synthetic gas or high-carbon synthetic gas, regulate hydrogen-carbon ratio, be warming up to 250-280 ℃ by heat exchange again to 2.95-3.05, enter the 6th grade of adiabatic reactor, proceed methanation reaction, the temperature of reactor outlet eluting gas is 350-400 ℃, consists of (V%):
H
2:≤0.5; CO :≤0.05; CO
2:≤0.5; CH
4: 〉=94%; Rare gas element: 1.6; Water: 1.5-3.
After removing moisture, methane content 〉=95%.
Above-mentioned methanation, top temperature are about 710 ℃, adopt high temperature resistant methanation catalyst.The high-temperature methanation catalyst of producing can meet the demands.
Embodiment 2.
To be rich in the CO unstripped gas is raw material, synthetic natural gas.As the CO of SiC production process by-product, a kind of classical group becomes: CO 96.6%, sulfide 3.4%.
84.7% of above-mentioned raw materials gas total amount is carried out sulfur-resisting transformation, decarburization, desulfurization, obtain the low-carbon (LC) synthetic gas (V%) of following composition: H
2: 89.0; CO:8.8; CO
2: 2.2
15.3% of above-mentioned raw materials gas total amount is carried out desulfurization, obtain the low-carbon (LC) synthetic gas (V%) of following composition: CO :～100.This is the high-carbon synthetic gas.
The methanation reaction process is as follows:
(1) whole low-carbon (LC) synthetic gas are through (temperature 240-260 ℃) after the heat exchange, add the steam (temperature 240-260 ℃) that accounts for low-carbon (LC) synthetic gas flow about 15%, enter first step adiabatic reactor, carry out methanation reaction, the temperature of reactor outlet eluting gas is 670-680 ℃.
(2) behind first step adiabatic reactor effluent air process vapor superheater, waste heat boiler, interchanger, mix with the high-carbon synthetic gas of certain flow, mixing the back temperature is 240-260 ℃, enter second stage adiabatic reactor, proceed methanation reaction, the temperature of reactor outlet eluting gas is 670-680 ℃.
(3) behind second stage adiabatic reactor effluent air process vapor superheater, waste heat boiler, mix with the high-carbon synthetic gas of certain flow, mixing the back temperature is 240-260 ℃, enter third stage adiabatic reactor, proceed methanation reaction, the temperature of reactor outlet eluting gas is 660-670 ℃.
(4) behind third stage adiabatic reactor effluent air process vapor superheater, waste heat boiler, be cooled to 240-260 ℃, enter fourth stage adiabatic reactor, proceed methanation reaction, the temperature of reactor outlet eluting gas is 480-500 ℃.
(6) from fourth stage adiabatic reactor effluent air through waste heat boiler, cooling after, be cooled to 45-60 ℃, gas-liquid separation, remove most of moisture; Add low-carbon (LC) synthetic gas or high-carbon synthetic gas, regulate hydrogen-carbon ratio, be warming up to 250-280 ℃ by heat exchange again to 2.95-3.05, enter the level V adiabatic reactor, proceed methanation reaction, the temperature of reactor outlet eluting gas is 350-400 ℃, consists of (V%):
H
2:≤0.5; CO :≤0.05; CO
2:≤0.5; CH
4: 〉=95%; Water: 1.5-3.
After removing moisture, methane content 〉=97%.
Claims (2)
1. method of producing synthetic natural gas, it is characterized in that: this method synthetic natural gas process may further comprise the steps:
(1) gasification by coal or other carbon raw material obtains unstripped gas, or the gas that is rich in carbon monoxide of other approach acquisition, through purifying treatment, removes behind catalyzer and the deleterious impurity of product gas, as total source of the gas;
(2) unstripped gas that total source of the gas is come is divided into two portions, and wherein a part obtains hydrogen-carbon ratio (H by hydrosphere transformation, carbonic acid gas acid gas removal, purification process and adjusting hydrogen-carbon ratio
2-CO
2)/(H
2+ CO
2The low-carbon (LC) synthetic gas of)=4.5-15.0, another part gas are that hydrogen-carbon ratio is the high-carbon synthetic gas of 0-2.0;
(3) according to the requirement of catalyzer to temperature of reaction, after the vapor mixing of described low-carbon (LC) synthetic gas and certain flow, enter first step adiabatic reactor, carry out methanation reaction;
(4) gas that comes out from first step adiabatic reactor after heat exchange, adjusting temperature, mixes with the high-carbon synthetic gas of certain flow, enters second stage adiabatic reactor, carries out methanation reaction;
(5) process of step (4) repeats, and equals or near 3.0, through after the heat exchange, enters the next stage adiabatic reactor up to the hydrogen-carbon ratio of the gas that comes out from reactor, proceeds methanation reaction;
(6) gas that comes out from top reactor, through heat exchange, cooling, gas-liquid separation etc., remove the most of water in the air-flow, appropriate supplement adds low-carbon (LC) synthetic gas or the high-carbon synthetic gas in the above-mentioned step (2), accurately regulate the hydrogen-carbon ratio of air-flow, make hydrogen-carbon ratio reach 2.95-3.05, enter follow-up adiabatic reactor;
(7) from processes such as the heat exchange of last step adiabatic reactor effluent air process, cooling, drying and compressions, obtain the synthetic natural gas product.
2. the method for a kind of production synthetic natural gas according to claim 1 is characterized in that: it is the 2-8 level that described synthetic natural gas process adopts adiabatic reactor progression.
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Cited By (13)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN102952597A (en) * | 2012-10-16 | 2013-03-06 | 大连瑞克科技有限公司 | Circulation-free process of synthesizing natural gas |
| CN103194286A (en) * | 2013-04-08 | 2013-07-10 | 西北化工研究院 | Methanation method for synthesizing substitute natural gas by using industrial hydrocarbon exhaust gas |
| CN103289769A (en) * | 2013-05-27 | 2013-09-11 | 中国寰球工程公司 | Method without circulation loop for producing synthetic natural gas by complete methanation of synthesis gas |
| CN103484182A (en) * | 2013-09-18 | 2014-01-01 | 大连瑞克科技有限公司 | Method for producing substitute natural gas through CO-rich industrial tail gas |
| CN103740424A (en) * | 2012-10-17 | 2014-04-23 | 中国石油化工股份有限公司 | Method of producing substitute natural gas from synthesis gas |
| CN103740423A (en) * | 2012-10-17 | 2014-04-23 | 中国石油化工股份有限公司 | Method of producing substitute natural gas from synthesis gas |
| CN103773526A (en) * | 2012-10-25 | 2014-05-07 | 中国石油化工股份有限公司 | Method for producing substitute natural gas |
| CN103773528A (en) * | 2012-10-25 | 2014-05-07 | 中国石油化工股份有限公司 | Preparation method of substitute natural gas |
| CN104031706A (en) * | 2014-05-27 | 2014-09-10 | 顾君尧 | Method for preparing natural gas by use of tail gas of calcium carbide furnace, and production device using same |
| CN104312651A (en) * | 2014-10-30 | 2015-01-28 | 北京华福工程有限公司 | Circulation-free methanation system |
| CN105087092A (en) * | 2014-05-19 | 2015-11-25 | 通用电气公司 | Natural gas production system and method thereof |
| CN108865307A (en) * | 2018-08-08 | 2018-11-23 | 中国五环工程有限公司 | Raw gas combined type full methanation technique and system without circulation loop |
| CN110243992A (en) * | 2018-03-09 | 2019-09-17 | 国家能源投资集团有限责任公司 | The preparation method and Catalyst evaluation test system of evaluating catalyst unstripped gas |
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Cited By (15)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN102952597A (en) * | 2012-10-16 | 2013-03-06 | 大连瑞克科技有限公司 | Circulation-free process of synthesizing natural gas |
| CN103740424A (en) * | 2012-10-17 | 2014-04-23 | 中国石油化工股份有限公司 | Method of producing substitute natural gas from synthesis gas |
| CN103740423A (en) * | 2012-10-17 | 2014-04-23 | 中国石油化工股份有限公司 | Method of producing substitute natural gas from synthesis gas |
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| CN103773528A (en) * | 2012-10-25 | 2014-05-07 | 中国石油化工股份有限公司 | Preparation method of substitute natural gas |
| CN103194286B (en) * | 2013-04-08 | 2014-07-09 | 西北化工研究院 | Methanation method for synthesizing substitute natural gas by using industrial hydrocarbon exhaust gas |
| CN103194286A (en) * | 2013-04-08 | 2013-07-10 | 西北化工研究院 | Methanation method for synthesizing substitute natural gas by using industrial hydrocarbon exhaust gas |
| CN103289769A (en) * | 2013-05-27 | 2013-09-11 | 中国寰球工程公司 | Method without circulation loop for producing synthetic natural gas by complete methanation of synthesis gas |
| CN103484182A (en) * | 2013-09-18 | 2014-01-01 | 大连瑞克科技有限公司 | Method for producing substitute natural gas through CO-rich industrial tail gas |
| CN105087092A (en) * | 2014-05-19 | 2015-11-25 | 通用电气公司 | Natural gas production system and method thereof |
| CN104031706A (en) * | 2014-05-27 | 2014-09-10 | 顾君尧 | Method for preparing natural gas by use of tail gas of calcium carbide furnace, and production device using same |
| CN104312651A (en) * | 2014-10-30 | 2015-01-28 | 北京华福工程有限公司 | Circulation-free methanation system |
| CN110243992A (en) * | 2018-03-09 | 2019-09-17 | 国家能源投资集团有限责任公司 | The preparation method and Catalyst evaluation test system of evaluating catalyst unstripped gas |
| CN108865307A (en) * | 2018-08-08 | 2018-11-23 | 中国五环工程有限公司 | Raw gas combined type full methanation technique and system without circulation loop |
| CN108865307B (en) * | 2018-08-08 | 2023-10-24 | 中国五环工程有限公司 | Combined complete methanation process and system for raw gas without circulation loop |
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Application publication date: 20111102 |