CN115725346A - Preparation method of synthesis gas with high carbon monoxide concentration - Google Patents
Preparation method of synthesis gas with high carbon monoxide concentration Download PDFInfo
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- CN115725346A CN115725346A CN202111021657.2A CN202111021657A CN115725346A CN 115725346 A CN115725346 A CN 115725346A CN 202111021657 A CN202111021657 A CN 202111021657A CN 115725346 A CN115725346 A CN 115725346A
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J8/00—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes
- B01J8/02—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with stationary particles, e.g. in fixed beds
- B01J8/06—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with stationary particles, e.g. in fixed beds in tube reactors; the solid particles being arranged in tubes
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- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B32/00—Carbon; Compounds thereof
- C01B32/40—Carbon monoxide
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- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10K—PURIFYING OR MODIFYING THE CHEMICAL COMPOSITION OF COMBUSTIBLE GASES CONTAINING CARBON MONOXIDE
- C10K3/00—Modifying the chemical composition of combustible gases containing carbon monoxide to produce an improved fuel, e.g. one of different calorific value, which may be free from carbon monoxide
- C10K3/02—Modifying the chemical composition of combustible gases containing carbon monoxide to produce an improved fuel, e.g. one of different calorific value, which may be free from carbon monoxide by catalytic treatment
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P20/00—Technologies relating to chemical industry
- Y02P20/50—Improvements relating to the production of bulk chemicals
- Y02P20/52—Improvements relating to the production of bulk chemicals using catalysts, e.g. selective catalysts
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Abstract
The invention provides a preparation method of synthesis gas with high carbon monoxide concentration. The method comprises the following steps: filling a catalyst into a reactor; feeding raw material and water into reactor to contact with catalyst and convert them into CO and H 2 High CO concentration synthesis gas; wherein the catalyst is CO 2 And CH 4 A conversion catalyst; the raw material gas is CO 2 、CH 4 Mixed gas of, or CO 2 、CH 4 、H 2 The mixed gas of (1). The invention recovers CO 2 Reacting with methane or with a concentration of H 2 In CO 2 And CH 4 Under the action of the conversion catalyst, high-concentration CO synthesis gas is produced, and the CO gas is extracted by adsorbing PSA at constant temperature and variable pressure, so that the method has good economic benefit.
Description
Technical Field
The invention relates to a preparation method of synthesis gas with high carbon monoxide concentration, belonging to the technical field of synthesis gas preparation.
Background
As the climate becomes warm, the extreme climate frequently occurs, CO 2 The emission reduction is already known by adults, and CO is fully utilized 2 The method is a green low-carbon technology which is urgently needed. At present, CO is mostly utilized 2 And CH 4 The reaction is used for chemical production of chemical products such as butanol and octanol.
In the prior art, coal gasification synthesis gas or natural gas steam conversion synthesis gas is generally used as a raw material, coal is used as a raw material, the investment is large, and CO and H 2 The concentration of CO in the synthesis gas is low, and the cost for extracting CO is high.
Disclosure of Invention
In order to solve the above technical problems, the present invention provides a method for preparing a synthesis gas with a high CO concentration by using CO 2 And CH 4 Or by mixing with a certain concentration of H 2 By CO 2 And CH 4 And converting to obtain high-concentration CO synthetic gas.
In order to achieve the above object, the present invention provides a method for preparing a high CO concentration synthesis gas, comprising the steps of:
filling a catalyst into a reactor;
feeding raw material and water into reactor to contact with catalyst and convert them into CO and H 2 High CO concentration synthesis gas;
wherein the catalyst is CO 2 And CH 4 A conversion catalyst;
the raw material gas is CO 2 、CH 4 Mixed gas of, or CO 2 、CH 4 、H 2 The mixed gas of (2).
In the above method, preferably, the reactor is a variable temperature bed reactor, and the inlet temperature of the variable temperature bed reactor is 400-750 ℃, the outlet temperature is 700-950 ℃, the pressure is normal pressure-1.0 MPa, and the space velocity is 600-4000h -1 。
In the above method, preferably, the reactor is an isothermal bed reactor, and the temperature of the isothermal bed reactor is controlled to be 500-950 ℃, the pressure is normal pressure-1.0 MPa, and the space velocity is 600-4000h -1 。
In the above method, preferably, the active component of the catalyst is nickel, and the carrier is Al 2 O 3 MgO, caO or a reactant or mixture of two or more thereof, for example: caAl 2 O 4 。
In the above method, preferably, the content of nickel in the catalyst is 1 to 25%, and the balance is a carrier.
In the above method, preferably, the variable temperature bed reactor is powered by an induction coil wound around the outside of the reaction tube, and the number of turns of the induction coil wound around the reaction tube at different positions from the inlet to the outlet is different to control the temperature at the different positions.
In the above method, preferably, the isothermal bed reactor is energized using an induction coil which is uniformly wound around the outside of the reaction tube.
According to the specific embodiment of the invention, the isothermal bed reactor and the variable temperature bed reactor adopted by the invention can be both tubular, the catalyst is filled in the reaction tube, the induction coil is uniformly wound on the outer wall of the reaction tube, after the induction coil is electrified, electromagnetic induction is generated between the reaction tube and the induction coil, and the reaction tube generates heat, so that the heating of the raw materials in the reaction tube is realized. Wherein, the space between the reaction tube and the induction coil can be filled with heat insulation materials (such as cement, fireproof materials and the like).
According to the specific embodiment of the invention, when the isothermal bed reactor is powered by the induction coil, the induction coil is uniformly wound outside the reaction tube. Conventional CO 2 Methanation apparatus, CH 4 Steam reforming unit is through the burning of fuel, gas and provides the heat, burns the heat supply through the nozzle in the combustion chamber, then realizes the heating to the reaction tube through with the reaction tube heat transfer, and then the raw materials in the heating reaction tube, however because the temperature of different regions is inhomogeneous in the combustion chamber, leads to this kind of heat transfer often all inhomogeneous, and the heat can concentrate at local area, can't realize that the temperature homoenergetic of each part of catalyst is even control, and the transformation reaction is also inhomogeneous. The invention has the advantages of good passing feelingThe reaction tube is heated by the reaction coil, the heating efficiency is high, and the induction coils are uniformly distributed in the reaction tube, so that the reaction tube can uniformly generate electromagnetic induction, and isothermal reaction can be really realized.
According to the specific embodiment of the invention, when the induction coil is used for supplying energy to the temperature-variable bed reactor, the induction coil is wound outside the reaction tube, and the number of turns of the induction coil wound at different positions of the reaction tube from the inlet to the outlet is different so as to control the temperature at different positions, the temperature at the inlet is lower, the number of turns of the induction coil can be smaller, and the temperature gradually rises along with the gradual transition from the inlet to the outlet, and the number of turns of the induction coil also gradually increases. Although the conventional apparatus can make different positions of the reaction tube have different temperatures due to the problems of the conventional apparatus, the temperature control of the different positions of the reaction tube cannot be truly realized because the combustion is uncontrollable, and the temperature change degree of the variable temperature bed reactor cannot be controlled. The invention can control the electromagnetic induction heating degree by controlling the winding mode of the induction coil outside the reaction tube, thereby relatively and accurately controlling the temperature of the catalyst at different positions inside the reaction tube and realizing the control of the temperature change degree. Moreover, the technical scheme of the invention can adopt a plurality of reaction tubes simultaneously, and can realize different temperature control for different reaction tubes, thereby controlling the reaction processes and reaction results in different reaction tubes, which cannot be realized by the existing heating equipment.
In the above method, preferably, the frequency of the current input to the induction coil is a medium frequency or a high frequency, wherein the high frequency is 5-20KHz, preferably 8-16KHz, more preferably 10-15KHz, further preferably 12-14KHz, and specifically may be 8KHz, 8.5KHz, 9KHz, 9.5KHz, 10KHz, 10.5KHz, 11KHz, 11.5KHz, 12KHz, 12.5KHz, 13KHz, 13.5KHz, 14KHz, 14.5KHz, 15KHz, 15.5KHz, 16KHz, or may be a range in which the endpoints of the above range and the enumerated specific frequency values are combined with each other, such as 5-16KHz, 5-15KHz, 5-10KHz, 8-20KHz, 8-15KHz, 8-10KHz, 10-20KHz, 10-16KHz, 10-12KHz, 9-20KHz, 9-15KHz, 12-14KHz, 12-20KHz; the intermediate frequency is 300 to 3000Hz, preferably 400 to 2000Hz, more preferably 500 to 1000Hz, and specifically may be 300Hz, 400Hz, 500Hz, 600Hz, 700Hz, 800Hz, 900Hz, 1000Hz, 1100Hz, 1200Hz, 1300Hz, 1400Hz, 1500Hz, 1600Hz, 1700Hz, 1800Hz, 1900Hz, 2000Hz, 2100Hz, 2200Hz, 2300Hz, 2400Hz, 2500Hz, 2600Hz, 2700Hz, 2800Hz, 2900Hz, 3000Hz, or may be a range in which the endpoints of the above ranges and the specific frequency values listed are combined with each other, such as 300 to 3000Hz, 300 to 1500Hz, 600 to 3000Hz, 600 to 2000Hz, 1000 to 3000Hz, 1000 to 2000Hz, 1200 to 3000Hz, 1200 to 2000Hz, 1500 to 3000Hz, 1500 to 2000Hz, and the like.
In the above method, preferably, a frequency of the current input to the induction coil is adjusted by a power supply and a capacitance. The induction coil is connected with the power supply to form a loop, and the power supply is connected with the capacitor in parallel, as shown in fig. 1. The power supply used in the present invention may be a common industrial power supply, such as a medium frequency power supply and a high frequency power supply. The power of the power supply, which may be adjusted to a desired frequency, is preferably rated at 100-1000KW, more preferably 200-500KW. The specification of the capacitor can be selected according to the requirement, and the capacitor can be matched with a power supply to meet the frequency control requirement.
The induction coil used in the present invention may be one or a combination of two or more selected from ferrite coil, iron core coil, air core coil, copper core coil, and the like.
According to the specific embodiment of the present invention, the size of the reaction tube used in the present invention can be selected according to the need, wherein the inner diameter of the reaction tube can be 50-250mm, and the length can be selected according to the need of the reaction.
According to embodiments of the present invention, the material of the reaction tubes may be a metal or an alloy, respectively, including but not limited to the materials of reaction tubes generally used for steam reforming, reaction tubes for dry reforming. The metal or alloy is preferably one that can withstand a temperature of 1000 c, more preferably one that can withstand a temperature of 1200 c. The material of the reaction tube can be respectively selected from 316L stainless steel, 304S stainless steel, HK40 high-temperature furnace tube material, HP Micro Alloy steel or Manauritex (TM) steam cracking furnace material and the like.
In the above process, preferably, CO is used as the raw material gas 2 、CH 4 In the mixed gas of (2), CO 2 And CH 4 In a molar ratio of 1 to 4;
in the presence of CO as feed gas 2 、CH 4 、H 2 In the mixed gas of (2), CO 2 And CH 4 1-4 (preferably 2.5) 2 And (CO) 2 +CH 4 ) In a molar ratio of 0.1 to 2.
In the above process, preferably, the high CO concentration syngas has a CO concentration of above 30%, preferably above 40%.
The invention recovers CO 2 Reacting with methane or with a concentration of H 2 In CO 2 And CH 4 Under the action of the conversion catalyst, high-concentration CO synthesis gas is produced, and the CO gas is extracted by adsorbing PSA at constant temperature and variable pressure, so that the method has good economic benefit.
In order to reduce CO in industrial processes 2 The invention can utilize green electricity to supply energy, heat the catalyst bed layer through an intermediate frequency furnace and the like, perform isothermal bed control, and easily obtain high conversion rate and CO in the process 2 And (4) low emission. The natural gas can also be used for heating and energy supply, a box-type furnace is used for heating a furnace tube, the catalyst is filled in the furnace tube, the variable temperature bed reaction is realized, and the inlet temperature and the outlet temperature of the variable temperature bed reaction are low and high.
Drawings
FIG. 1 is a schematic circuit diagram of the power supply, the induction coil and the capacitor of the present invention.
FIG. 2 is a schematic diagram of the isothermal bed reactor employed in examples 1-5.
FIG. 3 is a schematic representation of a variable temperature bed reactor used in examples 6-7.
Detailed Description
The technical solutions of the present invention will be described in detail below in order to clearly understand the technical features, objects, and advantages of the present invention, but the present invention should not be construed as limiting the implementable scope of the present invention.
The catalysts used in the examples are shown in table 1, wherein the contents are in mass%.
TABLE 1
Examples 1 to 5
Examples 1-5 each provide a method for producing high CO synthesis gas using an isothermal bed reactor with heat supplied by means of a medium frequency furnace (as shown in fig. 2); the composition of the feed gas, process conditions, catalyst, conversion composition at 850 ℃ are shown in table 2.
TABLE 2
As can be seen from the data in table 2: by the method of the invention, CH can be generated 4 、CO 2 Conversion to CO and H 2 Thereby being CO 2 The methane-containing gas finds a new application, and the synthesis gas with high CO concentration (the CO content exceeds 30 percent and can reach more than 45 percent at most) is prepared, so that the synthesis gas can be used for a process for producing reduced iron by using a gas-based shaft furnace.
Examples 6 to 7
Examples 6-7 each provide a method for producing high CO synthesis gas using a variable temperature bed reactor with intermediate frequency furnace for heat supply (as shown in fig. 3); the composition of the feed gas, process conditions, catalyst, conversion composition at an inlet temperature of 500 ℃ and an outlet temperature of 900 ℃ are shown in table 3.
TABLE 3
As can be seen from the data in table 3: by the method of the invention, CH can be generated 4 、CO 2 Conversion to CO and H 2 Thereby being CO 2 The methane-containing gas finds a new application, and the synthesis gas with high CO concentration (the highest CO content can reach more than 45%) is prepared, so that the synthesis gas can be used for a process for producing reduced iron by using a gas-based shaft furnace.
Claims (10)
1. A process for the preparation of synthesis gas having a high carbon monoxide concentration comprising the steps of:
filling a catalyst in a reactor;
feeding raw material and water into reactor to contact with catalyst and convert them into CO and H 2 High CO concentration synthesis gas;
wherein the catalyst is CO 2 And CH 4 A conversion catalyst;
the raw material gas is CO 2 、CH 4 Mixed gas of (2), or CO 2 、CH 4 、H 2 The mixed gas of (2).
2. The method as claimed in claim 1, wherein the reactor is a variable temperature bed reactor, and the variable temperature bed reactor has an inlet temperature of 400-750 ℃, an outlet temperature of 700-950 ℃, a pressure of normal pressure-1.0 MPa, and a space velocity of 600-4000h -1 。
3. The method of claim 1, wherein the reactor is an isothermal bed reactor, and the isothermal bed reactor is controlled at a temperature of 500 ℃ to 950 ℃, a pressure of normal pressure to 1.0MPa, and a space velocity of 600 to 4000h -1 。
4. The method of claim 1, wherein the active component of the catalyst is nickel and the support is Al 2 O 3 MgO, caO or a mixture or two or more of them.
5. The process of claim 4, wherein the catalyst comprises nickel in an amount of 1 to 25% with the balance being a support.
6. The method of claim 2, wherein the variable temperature bed reactor is powered using an induction coil that is wound around the outside of the reaction tube and wherein the reaction tube is wound with different numbers of turns at different locations from the inlet to the outlet to control the temperature at the different locations.
7. The method of claim 3, wherein the isothermal bed reactor is energized using an induction coil that is uniformly wound around the outside of the reaction tube.
8. The method according to claim 6 or 7, wherein the frequency of the current input to the induction coil is a medium frequency or a high frequency, wherein the high frequency is 5-20KHz, preferably 8-16KHz, more preferably 10-15KHz; the intermediate frequency is 300-3000Hz, preferably 500-1000Hz;
preferably, the frequency of the current input to the induction coil is adjusted by a power supply and a capacitor;
preferably, the induction coil is connected with the power supply to form a loop, and the power supply is connected with the capacitor in parallel;
more preferably, the power of the power supply is 100-1000KW, more preferably 200-500KW;
preferably, the induction coil is selected from one or a combination of more than two of ferrite coil, iron core coil, air core coil and copper core coil.
9. A process as claimed in any one of claims 1 to 8, wherein the CO as feed gas is 2 、CH 4 In the mixed gas of (2), CO 2 And CH 4 In a molar ratio of 1 to 4;
in the presence of CO as feed gas 2 、CH 4 、H 2 In the mixed gas of (2), CO 2 And CH 4 In a molar ratio of 1 to 4 2 And (CO) 2 +CH 4 ) In a molar ratio of 0.1 to 2.
10. The process according to any of claims 1-9, wherein the high CO concentration syngas has a CO concentration above 30%, preferably above 40%.
Priority Applications (2)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN202111021657.2A CN115725346A (en) | 2021-09-01 | 2021-09-01 | Preparation method of synthesis gas with high carbon monoxide concentration |
| PCT/CN2022/116091 WO2023030367A1 (en) | 2021-09-01 | 2022-08-31 | Method for preparing synthesis gas with high carbon monoxide concentration |
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| Application Number | Priority Date | Filing Date | Title |
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| CN202111021657.2A CN115725346A (en) | 2021-09-01 | 2021-09-01 | Preparation method of synthesis gas with high carbon monoxide concentration |
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Family Cites Families (6)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPH05270803A (en) * | 1992-03-24 | 1993-10-19 | Toyo Eng Corp | Production of synthetic gas from methane and carbon dioxide as source material |
| MY128194A (en) * | 1997-04-11 | 2007-01-31 | Chiyoda Corp | Process for the production of synthesis gas |
| CN1126710C (en) * | 2000-08-01 | 2003-11-05 | 中国石化集团齐鲁石油化工公司 | Method of preparing gas contg. high concn. of carbon monooxide |
| CN101450790A (en) * | 2007-12-07 | 2009-06-10 | 上海焦化有限公司 | Method and apparatus for preparing synthesis gas by natural gas-carbon dioxide reforming |
| JP2015509905A (en) * | 2012-03-13 | 2015-04-02 | バイエル・インテレクチュアル・プロパティ・ゲゼルシャフト・ミット・ベシュレンクテル・ハフツングＢａｙｅｒ Ｉｎｔｅｌｌｅｃｔｕａｌ Ｐｒｏｐｅｒｔｙ ＧｍｂＨ | CO and / or H2 production method in alternate operation of two operation modes |
| CN112265962B (en) * | 2020-10-30 | 2022-03-04 | 庄焱法 | Electric cooperative heat supply reforming reaction system |
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2021
- 2021-09-01 CN CN202111021657.2A patent/CN115725346A/en active Pending
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- 2022-08-31 WO PCT/CN2022/116091 patent/WO2023030367A1/en unknown
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