CN105820850A - Method for production of synthetic natural gas by utilization of methanol - Google Patents
Method for production of synthetic natural gas by utilization of methanol Download PDFInfo
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- CN105820850A CN105820850A CN201510001223.4A CN201510001223A CN105820850A CN 105820850 A CN105820850 A CN 105820850A CN 201510001223 A CN201510001223 A CN 201510001223A CN 105820850 A CN105820850 A CN 105820850A
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Abstract
A method for production of synthetic natural gas by the utilization of methanol comprises the following steps: methanol and pure water are vaporized, or in a converter and by the use of a copper-based catalyst, methanol is cracked into hydrogen and carbon dioxide or a gas mixture I of hydrogen and carbon monoxide; the gas mixture I and purified and desulphurized hydrogen rich gas are blended to obtain a gas mixture II according to theoretical hydrogen consumption of CO and CO2 in the formula of 3H2+CO--CH4+H2O and 4H2+CO2--CH4+2H2O; the gas mixture II is sent into a thermal-insulation multistage fixed bed and undergoes a methanation reaction under the action of a nickel-based catalyst to synthesize methane; and methane is purified by the utilization of pressure swing adsorption or membrane separation. The invention has the following advantages: the technology is simple; product composition is single; for enterprises of releasing coke oven gas and methanol, comprehensive utilization of hydrogen-rich gas is realized; the method is environmentally friendly; low-priced unsalable methanol is converted into high-priced best-selling natural gas; cost is low; and the method has remarkable economic benefit and social benefit.
Description
Technical field
The invention belongs to natural gas preparation field, particularly to a kind of method utilizing methanol production synthetic natural gas.
Background technology
Natural Gas In China market is the poorest but also resource distribution is the most unbalanced, although coastal area establishes some imported L NG and receives harbour, unbalanced situation has been taken on a new look, but in Heilungkiang, Jilin, Hunan, Hubei, Jiangxi, Yunnan, Guizhou, the ground such as Sichuan, Gas Prices still remains high.And methanol industry production capacity is superfluous, price persistently drops, and many places have dropped to less than 2000 yuan per ton, and unsalable methanol at a low price is done raw material, and to make high price natural gas meaning salable the most great.
CN103483119A discloses " a kind of method of hydrogen rich gas producing firedamp by syngas ", the method is with hydrogen rich gas as primary raw material, methanol is adjuvant, by cracking and methanation synthetic natural gas, the method is with hydrogen rich gas as primary raw material, relatively costly, needs segmentation to react, complex process, the more difficult control of process conditions.
CN103820181A discloses " method and device thereof that a kind of methanol is converted into natural gas ", and the method is with methanol as raw material, and ethanol is additive, and Compound-acid makees catalyst, and conversion product has methane, ethane, ethylene etc..Its shortcoming is: with Compound-acid as catalyst, and to reaction, it requires height, and product is gaseous mixture, if needing single methane, in addition it is also necessary to subsequent separation process.
Summary of the invention
The technical problem to be solved in the present invention is to provide a kind of rational technology, with low cost, the method that what product component was single utilize methanol production synthetic natural gas.
The technical solution of the present invention is:
A kind of method utilizing methanol production synthetic natural gas, it specifically comprises the following steps that
S1, methanol and pure water are vaporized after or by methanol in converter with 0.5MPa～3MPa pressure, 200 DEG C～300 DEG C at a temperature of, utilize Cu-series catalyst, be hydrogen and carbon dioxide or hydrogen and carbon mono oxide mixture I by methanol decomposition；
S2, gaseous mixture I and the process obtained by S1 purify the hydrogen rich gas of sulphur removal according to 3H2+CO→CH4+H2O and 4H2+CO2→CH4+2H2CO, CO in O formula2The theoretical amounts of hydrogen that consumes carries out dispensing, obtains gaseous mixture II；
S3, gaseous mixture II good for S2 proportioning is sent into adiabatic multi-stage fixed-bed at a temperature of 200 DEG C～700 DEG C, at 0.9MPa～1.2MPa under, under the effect of nickel catalyst, carry out methanation reaction, synthesizing methane；
S4, pressure-variable adsorption or membrance separation is utilized to be purified by the methane that S3 synthesizes；
S5, methane pressure regulation after purification is made SNG, or compression forms CNG, or LNG product is made in liquefaction.
Described methanol is 1:1 with the mol ratio of water.
Described Cu-series catalyst is CuZnAl catalyst.
Described methanol is 3200:1 with the mass ratio of Cu-series catalyst.
Described gaseous mixture I and the cumulative volume of hydrogen rich gas through purification sulphur removal are 200:1 with the volume ratio of nickel catalyst.
The H contained in described hydrogen rich gas2Quality ＞ hydrogen rich gas in CO and CO that contain2The gross mass of hydrogen is consumed in methanation theory.
Described hydrogen rich gas is oven gas, oven gas tail gas or methanol purge gas.
In production process, the heat collection of release in methanation is got up, for methanol decomposition operation institute calorific requirement.
Beneficial effects of the present invention:
Rational technology, product component is single, and to having coke-stove gas and methanol purge gas enterprise, hydrogen-rich gas realizes comprehensive utilization；The amount of heat that methanation discharges can be reclaimed, heat for methanol decomposition, thus realize utilization of energy；Environmentally friendly, there is not a large amount of water consumption problems with coal gas and environmental issue；The most unsalable methanol is converted into high price natural gas salable, with low cost, there is significant economic benefit and social benefit.
Accompanying drawing explanation
Fig. 1 be methanol decomposition be H2With CO synthesizing methane process chart；
Fig. 2 be methanol decomposition be H2And CO2Synthesizing methane process chart (has hydrogen rich gas)；
Fig. 3 be methanol decomposition be H2And CO2Synthesizing methane process chart (without hydrogen rich gas).
Detailed description of the invention
Below in conjunction with the accompanying drawings the present invention is described further, is case study on implementation several of the present invention, it is impossible to limit the scope of the present invention with this, change that the most every scope under this invention is done and modification, all should belong in the range of letter lid of the present invention.
Embodiment 1
S1, as shown in Figure 1, after methanol and pure water are vaporized in converter with 0.5MPa pressure, at a temperature of 300 DEG C, described methanol is 1:1 with the mol ratio of water, utilize Cu-series catalyst, described Cu-series catalyst is CuZnAl catalyst, described methanol is 3200:1 with the mass ratio of Cu-series catalyst, is hydrogen and carbon dioxide mix gas I by methanol decomposition；
S2, gaseous mixture I and the process obtained by S1 purify the hydrogen rich gas of sulphur removal according to 3H2+CO→CH4+H2O and 4H2+CO2→CH4+2H2CO, CO in O formula2The theoretical amounts of hydrogen that consumes carries out dispensing, obtains gaseous mixture II；Described hydrogen rich gas is oven gas, the H contained in described hydrogen rich gas2Quality ＞ hydrogen rich gas in CO and CO that contain2The gross mass of hydrogen is consumed in methanation theory；
S3, being sent into by gaseous mixture II good for S2 proportioning adiabatic multi-stage fixed-bed at a temperature of 200 DEG C, under 1.2MPa, under the effect of nickel catalyst, the volume of described gaseous mixture II and the volume ratio of nickel catalyst are 200:1, carry out methanation reaction, synthesizing methane；
S4, membrance separation is utilized to be purified by the methane that S3 synthesizes；
S5, methane liquefaction after purification is made LNG product.
In production process, the heat collection of release in methanation is got up, for methanol decomposition operation institute calorific requirement.
Embodiment 2
S1, as shown in Figure 1, after methanol and pure water are vaporized in converter with 03MPa pressure, at a temperature of 200 DEG C, described methanol is 1:1 with the mol ratio of water, utilize Cu-series catalyst, described Cu-series catalyst is CuZnAl catalyst, described methanol is 3200:1 with the mass ratio of Cu-series catalyst, is hydrogen and carbon dioxide mix gas I by methanol decomposition；
S2, gaseous mixture I and the process obtained by S1 purify the hydrogen rich gas of sulphur removal according to 3H2+CO→CH4+H2O and 4H2+CO2→CH4+2H2CO, CO in O formula2The theoretical amounts of hydrogen that consumes carries out dispensing, obtains gaseous mixture II；Described hydrogen rich gas is oven gas tail gas, the H contained in described hydrogen rich gas2Quality ＞ hydrogen rich gas in CO and CO that contain2The gross mass of hydrogen is consumed in methanation theory；
S3, being sent into by gaseous mixture II good for S2 proportioning adiabatic multi-stage fixed-bed at a temperature of 700 DEG C, under 0.9MPa, under the effect of nickel catalyst, the volume of described gaseous mixture II and the volume ratio of nickel catalyst are 200:1, carry out methanation reaction, synthesizing methane；
S4, pressure-variable adsorption is utilized to be purified by the methane that S3 synthesizes；
S5, by after purification methane compress formed CNG.
In production process, the heat collection of release in methanation is got up, for methanol decomposition operation institute calorific requirement.
Embodiment 3
S1, as shown in Figure 1, after methanol and pure water are vaporized in converter with 2.5MPa pressure, at a temperature of 250 DEG C, described methanol is 1:1 with the mol ratio of water, utilize Cu-series catalyst, described Cu-series catalyst is CuZnAl catalyst, described methanol is 3200:1 with the mass ratio of Cu-series catalyst, is hydrogen and carbon dioxide mix gas I by methanol decomposition；
S2, gaseous mixture I and the process obtained by S1 purify the hydrogen rich gas of sulphur removal according to 3H2+CO→CH4+H2O and 4H2+CO2→CH4+2H2CO, CO in O formula2The theoretical amounts of hydrogen that consumes carries out dispensing, obtains gaseous mixture II；Described hydrogen rich gas is methanol purge gas, the H contained in described hydrogen rich gas2Quality ＞ hydrogen rich gas in CO and CO that contain2The gross mass of hydrogen is consumed in methanation theory；
S3, being sent into by gaseous mixture II good for S2 proportioning adiabatic multi-stage fixed-bed at a temperature of 500 DEG C, under 1.0MPa, under the effect of nickel catalyst, the volume of described gaseous mixture II and the volume ratio of nickel catalyst are 200:1, carry out methanation reaction, synthesizing methane；
S4, membrance separation is utilized to be purified by the methane that S3 synthesizes；
S5, SNG is made in methane pressure regulation after purification.
In production process, the heat collection of release in methanation is got up, for methanol decomposition operation institute calorific requirement.
Embodiment 4
S1, as shown in Figure 2, by methanol in converter with 0.5MPa pressure, at a temperature of 300 DEG C, described methanol is 1:1 with the mol ratio of water, utilize Cu-series catalyst, described Cu-series catalyst is CuZnAl catalyst, described methanol is 3200:1 with the mass ratio of Cu-series catalyst, is hydrogen and carbon mono oxide mixture I by methanol decomposition；
S2, gaseous mixture I and the process obtained by S1 purify the hydrogen rich gas of sulphur removal according to 3H2+CO→CH4+H2O and 4H2+CO2→CH4+2H2CO, CO in O formula2The theoretical amounts of hydrogen that consumes carries out dispensing, obtains gaseous mixture II；Described hydrogen rich gas is methanol purge gas, the H contained in described hydrogen rich gas2Quality ＞ hydrogen rich gas in CO and CO that contain2The gross mass of hydrogen is consumed in methanation theory；
S3, being sent into by gaseous mixture II good for S2 proportioning adiabatic multi-stage fixed-bed at a temperature of 200 DEG C, under 1.2MPa, under the effect of nickel catalyst, the volume of described gaseous mixture II and the volume ratio of nickel catalyst are 200:1, carry out methanation reaction, synthesizing methane；
S4, membrance separation is utilized to be purified by the methane that S3 synthesizes；
S5, by after purification compression formed CNG product.
In production process, the heat collection of release in methanation is got up, for methanol decomposition operation institute calorific requirement.
Embodiment 5
S1, as shown in Figure 2, by methanol in converter with 3MPa pressure, at a temperature of 200 DEG C, described methanol is 1:1 with the mol ratio of water, utilize Cu-series catalyst, described Cu-series catalyst is CuZnAl catalyst, described methanol is 3200:1 with the mass ratio of Cu-series catalyst, is hydrogen and carbon mono oxide mixture I by methanol decomposition；
S2, gaseous mixture I and the process obtained by S1 purify the hydrogen rich gas of sulphur removal according to 3H2+CO→CH4+H2O and 4H2+CO2→CH4+2H2CO, CO in O formula2The theoretical amounts of hydrogen that consumes carries out dispensing, obtains gaseous mixture II；Described hydrogen rich gas is oven gas tail gas, the H contained in described hydrogen rich gas2Quality ＞ hydrogen rich gas in CO and CO that contain2The gross mass of hydrogen is consumed in methanation theory；
S3, being sent into by gaseous mixture II good for S2 proportioning adiabatic multi-stage fixed-bed at a temperature of 700 DEG C, under 0.9MPa, under the effect of nickel catalyst, the volume of described gaseous mixture II and the volume ratio of nickel catalyst are 200:1, carry out methanation reaction, synthesizing methane；
S4, pressure-variable adsorption is utilized to be purified by the methane that S3 synthesizes；
S5, methane liquefaction after purification is made LNG product.
In production process, the heat collection of release in methanation is got up, for methanol decomposition operation institute calorific requirement.
Embodiment 6
S1, as shown in Figure 2, by methanol in converter with 2.5MPa pressure, at a temperature of 250 DEG C, described methanol is 1:1 with the mol ratio of water, utilize Cu-series catalyst, described Cu-series catalyst is CuZnAl catalyst, described methanol is 3200:1 with the mass ratio of Cu-series catalyst, is hydrogen and carbon mono oxide mixture I by methanol decomposition；
S2, gaseous mixture I and the process obtained by S1 purify the hydrogen rich gas of sulphur removal according to 3H2+CO→CH4+H2O and 4H2+CO2→CH4+2H2CO, CO in O formula2The theoretical amounts of hydrogen that consumes carries out dispensing, obtains gaseous mixture II；Described hydrogen rich gas is oven gas, the H contained in described hydrogen rich gas2Quality ＞ hydrogen rich gas in CO and CO that contain2The gross mass of hydrogen is consumed in methanation theory；
S3, being sent into by gaseous mixture II good for S2 proportioning adiabatic multi-stage fixed-bed at a temperature of 500 DEG C, under 1.0MPa, under the effect of nickel catalyst, the volume of described gaseous mixture II and the volume ratio of nickel catalyst are 200:1, carry out methanation reaction, synthesizing methane；
S4, pressure-variable adsorption is utilized to be purified by the methane that S3 synthesizes；
S5, SNG is made in methane pressure regulation after purification.
In production process, the heat collection of release in methanation is got up, for methanol decomposition operation institute calorific requirement.
In natural gas high price region, finding and have hydrogen rich gas enterprise and methanol resource, near hydrogen rich gas enterprise, factory is built in addressing, uses technical matters of the present invention to convert methanol into higher-priced natural gas.
Production scale is according to H unnecessary in hydrogen rich gas2Quantity, formulate methanol decomposition yield.
During with methanol and pure water for raw material, during if hydrogen rich gas source occurs abnormal, it is possible to take discharge (liquefaction storage) part CO2Form realize material balance, it is ensured that normal produce (as shown in Figure 3).
Producing carbon monoxide during cracking or the generation carbon dioxide that adds water the most does not changes its C/Hratio, nor affect on the yield of final products, technical scheme is the most feasible, and owing to CO is poisonous, boiling point is low is difficult to liquefaction storage, and CO2Nontoxic, boiling point is higher, storage of easily liquefying, and therefore, walks cracking and produce CO in actual production2Circuit more reasonable.
Without hydrogen-rich gas, when being not desired to again by-product carbon dioxide, it is also feasible for adding pure hydrogen in system, and the purest hydrogen often price is high, less economical.
Claims (8)
1. the method utilizing methanol production synthetic natural gas, is characterized in that: specifically comprise the following steps that
S1, methanol and pure water are vaporized after or by methanol in converter with 0.5MPa～3MPa pressure, 200 DEG C～300 DEG C at a temperature of, utilize Cu-series catalyst, be hydrogen and carbon dioxide or hydrogen and carbon mono oxide mixture I by methanol decomposition；
S2, gaseous mixture I and the process obtained by S1 purify the hydrogen rich gas of sulphur removal according to 3H2+CO→CH4+H2O and 4H2+CO2→CH4+2H2CO, CO in O formula2The theoretical amounts of hydrogen that consumes carries out dispensing, obtains gaseous mixture II；
S3, gaseous mixture II good for S2 proportioning is sent into adiabatic multi-stage fixed-bed at a temperature of 200 DEG C～700 DEG C, at 0.9MPa～1.2MPa under, under the effect of nickel catalyst, carry out methanation reaction, synthesizing methane；
S4, pressure-variable adsorption or membrance separation is utilized to be purified by the methane that S3 synthesizes；
S5, methane pressure regulation after purification is made SNG, or compression forms CNG, or LNG product is made in liquefaction.
The method utilizing methanol production synthetic natural gas the most according to claim 1, is characterized in that: described methanol is 1:1 with the mol ratio of water.
The method utilizing methanol production synthetic natural gas the most according to claim 1, is characterized in that: described Cu-series catalyst is CuZnAl catalyst.
The method utilizing methanol production synthetic natural gas the most according to claim 1, is characterized in that: described methanol is 3200:1 with the mass ratio of Cu-series catalyst.
The method utilizing methanol production synthetic natural gas the most according to claim 1, is characterized in that: the volume of described gaseous mixture II and the volume ratio of nickel catalyst are 200:1.
The method utilizing methanol production synthetic natural gas the most according to claim 1, is characterized in that: the H contained in described hydrogen rich gas2Quality ＞ hydrogen rich gas in CO and CO that contain2The gross mass of hydrogen is consumed in methanation theory.
The method utilizing methanol production synthetic natural gas the most according to claim 6, is characterized in that: described hydrogen rich gas is oven gas, oven gas tail gas or methanol purge gas.
The method utilizing methanol production synthetic natural gas the most according to claim 1, is characterized in that: in production process, and the heat collection of release in methanation is got up, for methanol decomposition operation institute calorific requirement.
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Cited By (6)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN106748646A (en) * | 2016-12-14 | 2017-05-31 | 李卫教 | A kind of power storage processing method and system |
| CN106833780A (en) * | 2017-03-07 | 2017-06-13 | 张群荣 | A kind of process units of novel biomass gasifying gas preparing natural gas |
| CN106883084A (en) * | 2017-03-07 | 2017-06-23 | 王亚壮 | A kind of method and system of new synthesizing methane |
| RU2631290C1 (en) * | 2016-07-25 | 2017-09-20 | Андрей Владиславович Курочкин | Low-temperature hydrogen plant |
| CN108102750A (en) * | 2016-11-25 | 2018-06-01 | 惠生工程（中国）有限公司 | A kind of technique of synthesis gas preparing natural gas |
| CN109266413A (en) * | 2018-10-30 | 2019-01-25 | 青岛联信催化材料有限公司 | A method of synthetic natural gas is produced using hydrogen retrieval impermeable gas |
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| GB1441277A (en) * | 1973-06-27 | 1976-06-30 | Davy Powergas Ltd | Catalytic production of methane from methanol |
| US4239499A (en) * | 1977-11-15 | 1980-12-16 | Engelhard Minerals And Chemicals Corporation | Production of a fuel gas and synthetic natural gas from methanol |
| CN1233584A (en) * | 1998-04-27 | 1999-11-03 | 中国科学院山西煤炭化学研究所 | Method for prodn. of hydrogen from methyl alcohol |
| CN103483119A (en) * | 2013-08-27 | 2014-01-01 | 新地能源工程技术有限公司 | Method for producing methanefrom hydrogen-rich synthetic gas |
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2015
- 2015-01-05 CN CN201510001223.4A patent/CN105820850A/en active Pending
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| GB1441277A (en) * | 1973-06-27 | 1976-06-30 | Davy Powergas Ltd | Catalytic production of methane from methanol |
| US4239499A (en) * | 1977-11-15 | 1980-12-16 | Engelhard Minerals And Chemicals Corporation | Production of a fuel gas and synthetic natural gas from methanol |
| CN1233584A (en) * | 1998-04-27 | 1999-11-03 | 中国科学院山西煤炭化学研究所 | Method for prodn. of hydrogen from methyl alcohol |
| CN103483119A (en) * | 2013-08-27 | 2014-01-01 | 新地能源工程技术有限公司 | Method for producing methanefrom hydrogen-rich synthetic gas |
Cited By (7)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| RU2631290C1 (en) * | 2016-07-25 | 2017-09-20 | Андрей Владиславович Курочкин | Low-temperature hydrogen plant |
| CN108102750A (en) * | 2016-11-25 | 2018-06-01 | 惠生工程（中国）有限公司 | A kind of technique of synthesis gas preparing natural gas |
| CN108102750B (en) * | 2016-11-25 | 2020-11-06 | 惠生工程（中国）有限公司 | Process for preparing natural gas from synthesis gas |
| CN106748646A (en) * | 2016-12-14 | 2017-05-31 | 李卫教 | A kind of power storage processing method and system |
| CN106833780A (en) * | 2017-03-07 | 2017-06-13 | 张群荣 | A kind of process units of novel biomass gasifying gas preparing natural gas |
| CN106883084A (en) * | 2017-03-07 | 2017-06-23 | 王亚壮 | A kind of method and system of new synthesizing methane |
| CN109266413A (en) * | 2018-10-30 | 2019-01-25 | 青岛联信催化材料有限公司 | A method of synthetic natural gas is produced using hydrogen retrieval impermeable gas |
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