Method and device for preparing carbonyl sulfide from carbon dioxide and hydrogen sulfide mixed gas

文档序号:644106 发布日期:2021-05-14 浏览:28次 中文

阅读说明:本技术 一种二氧化碳和硫化氢混合气制取羰基硫的方法及装置 (Method and device for preparing carbonyl sulfide from carbon dioxide and hydrogen sulfide mixed gas ) 是由 赵璐 房克功 于 2020-12-31 设计创作,主要内容包括:本发明属于一种制取羰基硫的新方法,一种二氧化碳和硫化氢混合气合成羰基硫的方法,将碱土金属改性硅藻土置于双极板式反应器的反应腔内,通入氮气以除去反应器中的空气后,通入CO-2和H-2S混合气,接通连接高压电极和接地极的等离子体电源,调节电压至1-100千伏、频率1-30千赫兹,反应后得到羰基硫气体。本发明还涉及合成羰基硫的装置。(The invention belongs to a new method for preparing carbonyl sulfide, in particular to a method for synthesizing carbonyl sulfide by using carbon dioxide and hydrogen sulfide mixed gas 2 And H 2 And (3) switching on a plasma power supply for connecting the high-voltage electrode and the grounding electrode, regulating the voltage to 1-100 kilovolts and the frequency to 1-30 kilohertz, and reacting to obtain the carbonyl sulfide gas. The invention also relates to a device for synthesizing carbonyl sulfide.)

1. CO (carbon monoxide)2And H2The method for preparing carbonyl sulfide from S mixed gas is characterized by comprising the following steps: placing alkaline earth metal modified diatomite in the reaction cavity of a bipolar plate type reactor, introducing nitrogen to remove air in the reactor, and introducing CO2And H2S mixed gas, wherein CO is contained in the mixed gas250-99% by volume, H2The volume percentage of S is 1-50%, and the flow rate of the mixed gas is 50-9000 h-1The reaction pressure is 0.1-3 MPa, the reaction temperature is 120-,regulating voltage to 1-100 KV and frequency to 1-30 KHz to obtain carbonyl sulfide gas.

2. A CO as claimed in claim 12And H2The method for preparing carbonyl sulfide from S mixed gas is characterized by comprising the following steps: the diatomite in the alkaline earth metal modified diatomite is SiO2Diatomite and SiO with content higher than 75%250-75% of clay-containing diatomite and SiO2One or a mixture of two of clayey diatomite with content less than 50%.

3. A CO as claimed in claim 12And H2The method for preparing carbonyl sulfide from S mixed gas is characterized by comprising the following steps: the alkaline earth metal in the alkaline earth metal modified diatomite is one or a mixture of two of Be, Mg, Ca, Sr and Ba.

4. A CO as claimed in any one of claims 1 to 32And H2The bipolar plate type reactor used in the method for synthesizing carbonyl sulfide from S mixed gas is characterized in that: the bipolar plate type reactor is provided with an air inlet (1), a high-voltage electrode (2), a grounding electrode (3), a shell (4) and an air outlet (5), the external bipolar plate of the shell (4) is used as the high-voltage electrode (2), a built-in flat plate is installed on the axis of the shell (4) and used as the grounding electrode (3), a cuboid reaction cavity is formed in the shell (4), one end of the shell (4) is provided with the air inlet (1), the other end of the shell (4) is provided with the air outlet (5), the high-voltage electrode (2) is connected with high-voltage electricity through a wire, and the grounding electrode (.

5. An H according to claim 42S and CO2The bobbin type reactor used in the method for preparing carbonyl sulfide from mixed gas is characterized in that: the shell (4) is made of glass, quartz glass, ceramic or corundum.

Technical Field

The invention belongs to a new method for preparing carbonyl sulfide, and particularly relates to a method for preparing carbonyl sulfide from carbon dioxide and hydrogen sulfide mixed gas by combined action of plasma and alkaline earth metal modified diatomite.

Technical Field

Carbon dioxide (CO)2) As a greenhouse gas, the compound can cause global warming and ocean acidification, seriously damage the earth ecosystem and pose a great threat to human survival and development. And hydrogen sulfide (H)2S) is an acidic and corrosive toxic gas with the smell of rotten eggs, which often harms the personal safety and causes environmental pollution. In industry, H2S also poisons and deactivates the catalyst in the catalytic reaction.

In the exploitation and utilization of natural gas, petroleum and coal, a great deal of mixed CO is generated2And H2And S acid gas. At present, the mixed acid gas is treated by the Claus process in the industry, but the process only recovers the S element in the mixed acid gas to generate sulfur, andgeneration of H2O,CO2No reaction occurs in the whole process, namely hydrogen source recovery and carbon emission reduction cannot be realized. The applicant has realized CO in earlier research2And H2Please refer to patent ZL201710469388.3 in granted invention for preparing synthesis gas from S mixed acid gas. In further research, the applicant creatively adopts a new catalytic system to combine with the plasma to complete CO2And H2The S mixed acid gas is directly synthesized into carbonyl sulfide at low temperature by one step.

Carbonyl sulfide, formula: COS, one C atom is bonded to an O atom and an S atom, respectively, through two double bonds. Is a combustible toxic gas with colorless and smelly egg smell at normal temperature. However, carbonyl sulfide is an important organic synthesis intermediate, and is widely used in the pesticide industry for synthesizing insecticides, herbicides, and the like. In addition, the compound is also an important intermediate for synthesizing the carbamate herbicide and has important application in fine chemical varieties.

In the invention, industrial CO is directly reacted by adopting a one-step method2And H2S mixed waste gas is converted into carbonyl sulfide, thereby not only successfully producing important chemical intermediate carbonyl sulfide, but also completing CO2And H2S is a green and clean process for changing waste into valuable, and a new method for producing carbonyl sulfide is developed. The method has important value in the field of recycling waste resources in China and the field of carbonyl sulfide production.

The invention uses CO2And H2The S mixed acid gas is used as a reactant, alkaline earth metal modified diatomite is used as a catalyst, and the alkaline earth metal modified diatomite is connected with the plasma in parallel to realize CO2And H2The S mixed acid gas is directly converted into carbonyl sulfide at a lower temperature (120-150 ℃). Not only finish CO2And H2The harmless resource recycling process of S produces carbonyl sulfide, and the prior similar technology is not found through retrieval.

Disclosure of Invention

The invention aims to provide a novel method for preparing carbonyl sulfide and simultaneously completing the reaction of CO2And H2S mixed acidic waste gas resource and harmless treatment method.

Plasma is a fourth existing form of matter. Plasma processThe daughter is rich in excited species such as excited molecules, atoms, ions, energetic electrons and radicals, and other highly active species. The invention adopts the method of the synergy of the alkaline earth metal modified diatomite catalyst and the plasma to react CO2And H2The S mixed acid gas is excited to generate plasma high-activity reaction species, and the catalysis of the alkaline earth metal modified diatomite catalyst is combined to complete CO2And H2The S mixed acid gas is directly synthesized into carbonyl sulfide by a one-step method.

The process is described as follows: CO generation by discharge plasma2And H2The S mixed acid gas is excited to obtain excited active species, the discharge plasma area is filled with an alkaline earth metal modified diatomite catalyst, the excited species obtain a target product carbonyl sulfide under the catalytic action of the alkaline earth metal modified diatomite catalyst, and CO is realized2And H2The S mixed acid gas is directly synthesized into carbonyl sulfide by a one-step method. The plasma discharge can adopt a direct current power supply and also can adopt an alternating current power supply. The alkaline earth metal modified diatomite catalyst filled in the discharge plasma area is solid particles or solid powder.

CO (carbon monoxide)2And H2The S mixed gas carbonyl sulfide synthesizing process includes setting alkali earth modified diatomite inside the reaction cavity of double plate reactor, introducing nitrogen to eliminate air in the reactor, and introducing CO2And H2S mixed gas, wherein H in the mixed gas2S is 1-50% by volume, and CO2The volume percentage content is 50-99%, and the flow rate of the mixed gas is 50-9000 h-1The reaction temperature is 120-.

The diatomite in the alkaline earth metal modified diatomite is SiO2Diatomite and SiO with content higher than 75%250-75% of clay-containing diatomite and SiO2One or a mixture of two of clayey diatomite with content less than 50%.

The alkaline earth metal in the alkaline earth metal modified diatomite is one or a mixture of two of Be, Mg, Ca, Sr and Ba.

CO (carbon monoxide)2And H2A bipolar plate type reactor used in the method for synthesizing carbonyl sulfide from S mixed gas is provided with a gas inlet (1), a high-voltage electrode (2), a grounding electrode (3), a shell (4) and a gas outlet (5), an external bipolar plate of the shell (4) is used as the high-voltage electrode (2), a built-in flat plate is installed on the axis of the shell (4) and is used as the grounding electrode (3), a cuboid reaction cavity is arranged in the shell (4), the gas inlet (1) is arranged at one end of the shell (4), the gas outlet (5) is arranged at the other end of the shell (4), the high-voltage electrode (2) is connected with high-voltage electricity through a lead, and the grounding electrode (3).

The shell (4) is made of quartz glass, ceramic or corundum.

Compared with the prior art, the invention has the following advantages:

1. the invention discloses a new synthesis method of carbonyl sulfide;

2. realizes the preparation of the medical intermediate carbonyl sulfide and simultaneously leads CO2And H2S, recycling and harmlessness of the mixed acidic waste gas;

3. the introduction of the alkaline earth metal modified diatomite catalyst promotes CO2And H2Direct conversion of S and production of carbonyl sulfide;

4. the conversion rate of carbon dioxide can be higher than 80%, the conversion rate of hydrogen sulfide can reach 100%, and the selectivity of carbonyl sulfide can be higher than 99%.

Drawings

FIG. 1 is a schematic view of a bipolar plate type plasma discharge reactor according to the present invention;

FIG. 2 shows CO in the plasma of the present invention2And H25.7 wt% Sr-15.6 wt% Ba-doped 31 wt% clayey diatomaceous earth (30 wt% SiO) in example 17 at S conversion2) 47.7% by weight of clayed diatomaceous earth (60% by weight of SiO)2) A plot of carbonyl sulfide selectivity of the catalyst as a function of reaction time;

wherein, 1 is the air inlet, 2 is the high voltage electrode, 3 is the earth electrode, 4 is the casing, 5 is the gas outlet.

Detailed Description

The following describes the specific embodiment of the present invention in detail with reference to the technical scheme, and the content of carbonyl sulfide in the tail gas is analyzed on line by chromatography.

Example 1

The bipolar plate type reactor consists of an air inlet 1, a high-voltage electrode 2, a grounding electrode 3, a shell 4 and an air outlet 5, wherein an external bipolar plate of the shell 4 is used as the high-voltage electrode 2, a built-in flat plate is installed on the axis of the shell 4 and is used as the grounding electrode 3, a cuboid reaction cavity is arranged in the shell 4, one end of the shell 4 is provided with the air inlet 1, the other end of the shell 4 is provided with the air outlet 5, the high-voltage electrode 2 is connected with high-voltage electricity through a lead, and the grounding.

5 wt% Sr-doped clayey diatomaceous earth (31 wt% SiO)2) The catalyst is arranged in the reaction chamber, and the shell 4 is made of quartz glass. Nitrogen was introduced for 10 minutes to remove air from the reactor. Controlled by a mass flow meter to have a composition of 55 vol% H2S-35vol%CO2-10 vol% Ar gas mixture for 300h-1The flow of space velocity is through the bed. The reaction pressure is 1.8MPa, the reaction temperature is 120 ℃, a plasma power supply for connecting a high-voltage electrode and a grounding electrode is connected, the voltage is adjusted to 2 kilovolts, and the frequency is 9 kilohertz. The carbonyl sulfur content in the tail gas is analyzed on line by chromatography. The reaction results are shown in table 1:

TABLE 1H2S and CO2Conversion, carbonyl sulfide selectivity

H2S conversion rate,% CO2Conversion rate% Carbonyl sulfide selectivity,%)
43.2 51.7 31.9

Example 2

2 wt% Be-5 wt% Mg doped 32 wt% clayey diatomaceous earth (40 wt% SiO)2) -61% by weight of argillaceous diatomaceous earth (50% by weight of SiO)2) The catalyst is placed in the reaction chamber, the shell 4 is made of corundum, and nitrogen is introduced for 10 minutes to remove air in the reactor. Controlled by a mass flow meter to have a composition of 13 vol% H2S-87vol%CO2Mixed gas for 740h-1The flow of space velocity is through the bed. The reaction pressure is 1.7MPa, the reaction temperature is 140 ℃, a plasma power supply for connecting a high-voltage electrode and a grounding electrode is connected, the voltage is adjusted to 10 kilovolts, and the frequency is 7 kilohertz. The carbonyl sulfur content in the tail gas is analyzed on line by chromatography. The rest of the procedure is the same as in example 1, and the reaction results are shown in Table 2:

TABLE 2H2S and CO2Conversion, carbonyl sulfide selectivity

H2S conversion rate,% CO2Conversion rate% Carbonyl sulfide selectivity,%)
100 11.9 80.7

Example 3

9.5% Be-10% Ca doped 46% clayey diatomaceous earth (50% SiO by weight)2) 34.5% by weight of clayed diatomaceous earth (60% by weight of SiO)2) The catalyst is arranged in the reaction cavity, and the shellThe body 4 is made of ceramic, and nitrogen gas is introduced for 10 minutes to remove air in the reactor. Controlled by a mass flow meter to have a composition of 42 vol% H2S-51vol%CO2-7vol%N2The mixed gas is used for 7500h-1The flow of space velocity is through the bed. The reaction pressure is 0.1MPa, the reaction temperature is 149 ℃, a plasma power supply for connecting a high-voltage electrode and a grounding electrode is connected, the voltage is adjusted to 12 kilovolts, and the frequency is 10 kilohertz. The carbonyl sulfur content in the tail gas is analyzed on line by chromatography. The rest of the procedure is the same as in example 1, and the reaction results are shown in Table 3:

TABLE 3H2S and CO2Conversion, carbonyl sulfide selectivity

H2S conversion rate,% CO2Conversion rate% Carbonyl sulfide selectivity,%)
79.2 45.7 43.6

Example 4

28 wt% clayey diatomaceous earth (28 wt% SiO) doped with 0.9% Mg-2.3 wt% Ba2) 68.8% by weight of diatomaceous earth (80% by weight of SiO)2) The catalyst is placed in the reaction chamber, the shell 4 is made of glass, and nitrogen is introduced for 10 minutes to remove air in the reactor. Controlled by a mass flow meter to have a composition of 6 vol% H2S-94vol%CO29000h of mixed gas-1The flow of space velocity is through the bed. The reaction pressure is 0.4MPa, the reaction temperature is 111 ℃, a plasma power supply for connecting the high-voltage electrode and the grounding electrode is connected, and electricity is regulatedTo 80 kv and a frequency of 27 khz. The carbonyl sulfur content in the tail gas is analyzed on line by chromatography. The rest of the procedure is the same as in example 1, and the reaction results are shown in Table 4:

TABLE 4H2S and CO2Conversion, carbonyl sulfide selectivity

H2S conversion rate,% CO2Conversion rate% Carbonyl sulfide selectivity,%)
100 3.2 19.7

Example 5

76 wt% clayey diatomaceous earth (23 wt% SiO) doped with 15% Ca-5 wt% Sr2) 4% by weight of diatomaceous earth (92% by weight of SiO)2) The catalyst is placed in the reaction chamber, the shell 4 is made of corundum, and nitrogen is introduced for 10 minutes to remove air in the reactor. Controlled by a mass flow meter to have a composition of 31 vol% H2S-69vol%CO2The mixed gas is used for 700h-1The flow of space velocity is through the bed. The reaction pressure was 0.8MPa, the reaction temperature was 126 ℃, the plasma power supply connecting the high voltage electrode and the ground electrode was switched on, the voltage was adjusted to 14.5 kV, and the frequency was 26.5 kHz. The carbonyl sulfur content in the tail gas is analyzed on line by chromatography. The rest of the procedure is the same as in example 1, and the reaction results are shown in Table 5:

TABLE 5H2S and CO2Conversion, carbonyl sulfide selectivity

H2S conversion rate,% CO2Conversion rate% Carbonyl sulfide selectivity,%)
87.6 40.5 26.8

Example 6

73 wt% diatomaceous earth (83 wt% SiO) doped with 10% Ca-15 wt% Ba2) 2% by weight of clayed diatomaceous earth (65% by weight of SiO)2) The catalyst is placed in the reaction chamber, the shell 4 is made of corundum, and nitrogen is introduced for 10 minutes to remove air in the reactor. Controlled by a mass flow meter to have a composition of 36 vol% H2S-64vol%CO2The mixed gas is used for 3500h-1The flow of space velocity is through the bed. The reaction pressure is 1.8MPa, the reaction temperature is 150 ℃, a plasma power supply for connecting a high-voltage electrode and a grounding electrode is connected, the voltage is adjusted to 81.5 kilovolts, and the frequency is 12 kilohertz. The carbonyl sulfur content in the tail gas is analyzed on line by chromatography. The rest is the same as example 1, and the reaction results are shown in Table 6:

TABLE 6H2S and CO2Conversion, carbonyl sulfide selectivity

H2S conversion rate,% CO2Conversion rate% Carbonyl sulfide selectivity,%)
100 55.0 31.8

Example 7

19.8% Mg-4.2% Ca doped 45% clayey diatomaceous earth (34% SiO by weight)2) 31% by weight of clayed diatomaceous earth (71% by weight of SiO)2) The catalyst is placed in the reaction chamber, the shell 4 is made of ceramic, and nitrogen is introduced for 10 minutes to remove air in the reactor. Controlled by a mass flow meter to have a composition of 48 vol% H2S-52vol%CO2The mixed gas takes 7000h-1The flow of space velocity is through the bed. The reaction pressure is 3MPa, the reaction temperature is 136 ℃, a plasma power supply for connecting a high-voltage electrode and a grounding electrode is connected, the voltage is adjusted to 20 kilovolts, and the frequency is 3.5 kilohertz. The carbonyl sulfur content in the tail gas is analyzed on line by chromatography. The rest of the procedure was the same as in example 1, and the reaction results are shown in Table 7:

TABLE 7H2S and CO2Conversion, carbonyl sulfide selectivity

H2S conversion rate,% CO2Conversion rate% Carbonyl sulfide selectivity,%)
97.9 70.2 71.0

Example 8

13.5% Be-7.3 wt% Mg doped 76 wt% diatomaceous earth (92 wt% SiO)2) 3.2% by weight of clayed diatomaceous earth (74% by weight of SiO)2) The catalyst is placed in the reaction chamber, the shell 4 is made of quartz glass, and nitrogen is introduced for 10 minutes to remove air in the reactor. Controlled by a mass flow meter to have a composition of 19 vol% H2S-81vol%CO2The mixed gas takes 2000h-1The flow of space velocity is through the bed. The reaction pressure is 2MPa, the reaction temperature is 149 ℃, a plasma power supply for connecting a high-voltage electrode and a grounding electrode is connected, the voltage is adjusted to 70 kilovolts, and the frequency is 15 kilohertz. The carbonyl sulfur content in the tail gas is analyzed on line by chromatography. The rest is the same as example 1, and the reaction results are shown in Table 8:

TABLE 8H2S and CO2Conversion, carbonyl sulfide selectivity

H2S conversion rate,% CO2Conversion rate% Carbonyl sulfide selectivity,%)
100 17.7 60.2

Example 9

28 wt% clayey diatomaceous earth (42 wt% SiO) doped with 1% Sr-9.6 wt% Ba2) 61.4% by weight of diatomaceous earth (76% by weight of SiO)2) The catalyst is placed in the reaction chamber, the shell 4 is made of quartz glass, and nitrogen is introduced for 10 minutes to remove air in the reactor.Controlled by a mass flow meter to have a composition of 50 vol% H2S-50vol%CO2The mixed gas is used for 300h-1The flow of space velocity is through the bed. The reaction pressure is 0.6MPa, the reaction temperature is 121 ℃, a plasma power supply for connecting a high-voltage electrode and a grounding electrode is connected, the voltage is adjusted to 45 kilovolts, and the frequency is 20 kilohertz. The carbonyl sulfur content in the tail gas is analyzed on line by chromatography. The rest is the same as example 1, and the reaction results are shown in Table 9:

TABLE 9H2S and CO2Conversion, carbonyl sulfide selectivity

H2S conversion rate,% CO2Conversion rate% Carbonyl sulfide selectivity,%)
99.8 73.6 40.7

Example 10

90.5 wt% clayey diatomaceous earth (55 wt% SiO) doped with 9.5% Mg2) The catalyst is placed in the reaction chamber, the shell 4 is made of glass, and nitrogen is introduced for 10 minutes to remove air in the reactor. Controlled by a mass flow meter to have a composition of 2 vol% H2S-98vol%CO2The mixed gas is used for 50 hours-1The flow of space velocity is through the bed. The reaction pressure is 3MPa, the reaction temperature is 120 ℃, a plasma power supply for connecting a high-voltage electrode and a grounding electrode is connected, the voltage is adjusted to 15 kilovolts, and the frequency is 1 kilohertz. The rest of the procedure is the same as in example 1, and the reaction results are shown in Table 10:

TABLE 10H2S and CO2Conversion, carbonyl sulfide selectivity

H2S conversion rate,% CO2Conversion rate% Carbonyl sulfide selectivity,%)
100 1.5 98.8

Example 11

76 wt% diatomaceous earth (87 wt% SiO) doped with 0.8% Mg-1.5 wt% Sr2) 21.7% by weight of diatomaceous earth (80% by weight of SiO)2) The catalyst is placed in the reaction chamber, the shell 4 is made of corundum, and nitrogen is introduced for 10 minutes to remove air in the reactor. Controlled by a mass flow meter to have a composition of 5 vol% H2S-90ol%CO2-5vol%CH4The mixed gas is used for 1550h-1The flow of space velocity is through the bed. The reaction pressure is 2.6MPa, the reaction temperature is 135 ℃, a plasma power supply for connecting a high-voltage electrode and a grounding electrode is connected, the voltage is adjusted to 4.5 kilovolts, and the frequency is 27 kilohertz. The carbonyl sulfur content in the tail gas is analyzed on line by chromatography. The rest is the same as example 1, and the reaction results are shown in Table 11:

TABLE 11H2S and CO2Conversion, carbonyl sulfide selectivity

H2S conversion rate,% CO2Conversion rate% Carbonyl sulfide selectivity,%)
99.9 4.3 94.5

Example 12

Doped 57 wt% clayey diatomaceous earth doped with 3.6 wt% Ba (43 wt% SiO)2) 39.4% by weight of diatomaceous earth (78% by weight of SiO2) The catalyst is placed in the reaction chamber, the shell 4 is made of ceramic, and nitrogen is introduced for 10 minutes to remove air in the reactor. Controlled by a mass flow meter to have a composition of 45 vol% H2S-55vol%CO2The mixed gas is heated for 650h-1The flow of space velocity is through the bed. The reaction pressure is 1.9MPa, the reaction temperature is 146 ℃, a plasma power supply for connecting a high-voltage electrode and a grounding electrode is connected, the voltage is adjusted to 85.5 kilovolts, and the frequency is 24 kilohertz. The carbonyl sulfur content in the tail gas is analyzed on line by chromatography. The rest is the same as example 1, and the reaction results are shown in Table 12:

TABLE 12H2S and CO2Conversion, carbonyl sulfide selectivity

H2S conversion rate,% CO2Conversion rate% Carbonyl sulfide selectivity,%)
100 80.5 66.3

Example 13

5% Be-8.7% Ca doped 65% clay-containing diatomaceous earth (63% SiO by weight)2) 21.3% by weight of diatomaceous earth (89% by weight of SiO)2) The catalyst is placed in the reaction chamber, the shell 4 is made of ceramic, and nitrogen is introduced for 10 minutes to remove air in the reactor. Controlled by a mass flow meter to have a composition of 35 vol% H2S-55vol%CO2-10vol%H2The mixed gas is used for 320h-1The flow of space velocity is through the bed. The reaction pressure is 3MPa, the reaction temperature is 125 ℃, a plasma power supply for connecting the high-voltage electrode and the grounding electrode is connected, the voltage is adjusted to 3.5 kilovolts, and the frequency is 13 kilohertz. The carbonyl sulfur content in the tail gas is analyzed on line by chromatography. The rest is the same as example 1, and the reaction results are shown in Table 13:

TABLE 13H2S and CO2Conversion, carbonyl sulfide selectivity

H2S conversion rate,% CO2Conversion rate% Carbonyl sulfide selectivity,%)
99.2 67.1 54.3

Example 14

91.8 wt% clayey diatomaceous earth doped with 8.2 wt% Ca (8 wt%)SiO2) The catalyst is placed in the reaction chamber, the shell 4 is made of ceramic, and nitrogen is introduced for 10 minutes to remove air in the reactor. Controlled by a mass flow meter to have a composition of 35 vol% H2S-65vol%CO2The mixed gas is used for 5500h-1The flow of space velocity is through the bed. The reaction pressure is 1.6MPa, the reaction temperature is 130 ℃, a plasma power supply for connecting a high-voltage electrode and a grounding electrode is connected, the voltage is adjusted to 35 kilovolts, and the frequency is 30 kilohertz. The carbonyl sulfur content in the tail gas is analyzed on line by chromatography. The rest is the same as example 1, and the reaction results are shown in Table 14:

TABLE 14H2S and CO2Conversion, carbonyl sulfide selectivity

H2S conversion rate,% CO2Conversion rate% Carbonyl sulfide selectivity,%)
96.5 49.2 61.0

Example 15

17 wt% clayey diatomaceous earth doped with 1 wt% Mg-3.4 wt% Sr (10 wt% SiO)2) 78.6% by weight of diatomaceous earth (75% by weight of SiO)2) The reactor is placed in a reaction cavity, the shell 4 is made of ceramic, and nitrogen is introduced for 10 minutes to remove air in the reactor. Controlled by a mass flow meter to have a composition of 31 vol% H2S-69vol%CO2The mixed gas takes 900 hours-1The flow of space velocity is through the bed. The reaction pressure is 1.3MPa, the reaction temperature is 124 ℃, and the high-voltage electrode and the grounding electrode are connectedThe plasma power supply was adjusted to 44.5 kv at a frequency of 0.5 khz. The carbonyl sulfur content in the tail gas is analyzed on line by chromatography. The rest is the same as example 1, and the reaction results are shown in Table 15:

TABLE 15H2S and CO2Conversion, carbonyl sulfide selectivity

H2S conversion rate,% CO2Conversion rate% Carbonyl sulfide selectivity,%)
87.9 50.4 78.5

Example 16

28 wt% clayey diatomaceous earth (44 wt% SiO) doped with 2.5 wt% Sr-17.9 wt% Ba2) 51.6% by weight of clayed diatomaceous earth (66% by weight of SiO)2) The catalyst is placed in the reaction chamber, the shell 4 is made of corundum, and nitrogen is introduced for 10 minutes to remove air in the reactor. Controlled by a mass flow meter to have a composition of 49 vol% H2S-51vol%CO2The mixed gas takes 6000h-1The flow of space velocity is through the bed. The reaction pressure is 2.4MPa, the reaction temperature is 130 ℃, a plasma power supply for connecting a high-voltage electrode and a grounding electrode is connected, the voltage is adjusted to 90 kilovolts, and the frequency is 22 kilohertz. The carbonyl sulfur content in the tail gas is analyzed on line by chromatography. The rest of the procedure is the same as in example 1, and the reaction results are shown in Table 16:

TABLE 16H2S and CO2Conversion, carbonyl sulfide selectivity

H2S conversion rate,% CO2Conversion rate% Carbonyl sulfide selectivity,%)
88.7 80.6 71.3

Example 17

31 wt% clayey diatomaceous earth (30 wt% SiO) doped with 5.7 wt% Sr-15.6 wt% Ba2) 47.7% by weight of clayed diatomaceous earth (60% by weight of SiO)2) The catalyst is placed in the reaction chamber, the shell 4 is made of glass, and nitrogen is introduced for 10 minutes to remove air in the reactor. Controlled by a mass flow meter to have a composition of 1 vol% H2S-79vol%CO220 vol% CO gas mixture for 250h-1The flow of space velocity is through the bed. The reaction pressure was 1.6MPa, the reaction temperature was 129 ℃ and the plasma power supply connecting the high voltage electrode and the ground electrode was switched on, the voltage was adjusted to 41.5 kV and the frequency was 20.5 kHz. The carbonyl sulfur content in the tail gas is analyzed on line by chromatography. The rest is the same as example 1, and the reaction results are shown in Table 17:

TABLE 17H2S and CO2Conversion, carbonyl sulfide selectivity

H2S conversion rate,% CO2Conversion rate% Carbonyl sulfide selectivity,%)
100 0.3 99.9

Example 18

49 wt% Clay-containing diatomaceous earth (70 wt% SiO) doped with 2.4 wt% Mg-21.9 wt% Ba2) 26.7% by weight of clayed diatomaceous earth (51% by weight of SiO)2) The catalyst is placed in the reaction chamber, the shell 4 is made of quartz glass, and nitrogen is introduced for 10 minutes to remove air in the reactor. Controlled by a mass flow meter to have a composition of 21 vol% H2S-79vol%CO2The mixed gas takes 600 hours-1The flow of space velocity is through the bed. The reaction pressure is 1.7MPa, the reaction temperature is 121 ℃, a plasma power supply for connecting a high-voltage electrode and a grounding electrode is connected, the voltage is adjusted to 4 kilovolts, and the frequency is 12.5 kilohertz. The carbonyl sulfur content in the tail gas is analyzed on line by chromatography. The rest is the same as example 1, and the reaction results are shown in Table 18:

TABLE 18H2S and CO2Conversion, carbonyl sulfide selectivity

H2S conversion rate,% CO2Conversion rate% Carbonyl sulfide selectivity,%)
74.9 30.7 81.3

Example 19

16 wt% Ca-2.2 wt% Sr doped 53 wt% diatomaceous earth (72 wt% SiO)2) 28.8% by weight of clayed diatomaceous earth (56% by weight of SiO)2) The catalyst is placed in the reaction chamber, the shell 4 is made of ceramic, and nitrogen is introduced for 10 minutes to remove air in the reactor. Controlled by a mass flow meter to have a composition of 46 vol% H2S-54vol%CO2The mixed gas takes 6000h-1The flow of space velocity is through the bed. The reaction pressure is 2.3MPa, the reaction temperature is 127 ℃, a plasma power supply for connecting a high-voltage electrode and a grounding electrode is connected, the voltage is adjusted to 85 kilovolts, and the frequency is 7.5 kilohertz. The carbonyl sulfur content in the tail gas is analyzed on line by chromatography. The rest is the same as example 1, and the reaction results are shown in Table 19:

TABLE 19H2S and CO2Conversion, carbonyl sulfide selectivity

H2S conversion rate,% CO2Conversion rate% Carbonyl sulfide selectivity,%)
96.2 47.7 70.9

Example 20

20 wt% Be-3.9 wt% Ba-doped 75 wt% diatomaceous earth (90 wt% SiO)2) 1.1% by weight of diatomaceous earth (99% by weight of SiO)2) The catalyst is arranged in a reaction chamber, soThe shell 4 is made of corundum, and nitrogen is introduced for 10 minutes to remove air in the reactor. Controlled by a mass flow meter to have a composition of 29 vol% H2S-71vol%CO2The mixed gas is used for 7500h-1The flow of space velocity is through the bed. The reaction pressure is 1.5MPa, the reaction temperature is 132 ℃, a plasma power supply for connecting a high-voltage electrode and a grounding electrode is connected, the voltage is adjusted to 40 kilovolts, and the frequency is 3 kilohertz. The carbonyl sulfur content in the tail gas is analyzed on line by chromatography. The rest is the same as example 1, and the reaction results are shown in Table 20:

TABLE 20H2S and CO2Conversion, carbonyl sulfide selectivity

H2S conversion rate,% CO2Conversion rate% Carbonyl sulfide selectivity,%)
93.4 51.0 71.1

Example 21

44 wt% clayey diatomaceous earth (5 wt% SiO) doped with 19 wt% Mg-3 wt% Ba2) 34% by weight of diatomaceous earth (100% by weight of SiO)2) The catalyst is placed in the reaction chamber, the shell 4 is made of glass, and nitrogen is introduced for 10 minutes to remove air in the reactor. Controlled by a mass flow meter to have a composition of 4 vol% H2S-96vol%CO2The mixed gas takes 8500h-1The flow of space velocity is through the bed. The reaction pressure is 2.2MPa, the reaction temperature is 130 ℃, a plasma power supply for connecting the high-voltage electrode and the grounding electrode is connected, and the voltage is adjusted to 91.5 kilovoltAnd a frequency of 8 khz. The carbonyl sulfur content in the tail gas is analyzed on line by chromatography. The rest is the same as example 1, and the reaction results are shown in Table 21:

TABLE 21H2S and CO2Conversion, carbonyl sulfide selectivity

H2S conversion rate,% CO2Conversion rate% Carbonyl sulfide selectivity,%)
100 2.0 99.0

Example 22

3 wt% Be-6.7 wt% Ba-doped 83 wt% diatomaceous earth (90 wt% SiO)2) 7.3% by weight of diatomaceous earth (76% by weight of SiO)2) The catalyst is placed in the reaction chamber, the shell 4 is made of quartz glass, and nitrogen is introduced for 10 minutes to remove air in the reactor. Controlled by a mass flow meter to have a composition of 15 vol% H2S-85vol%CO2The mixed gas is used for 5000 hours-1The flow of space velocity is through the bed. The reaction pressure was 0.8MPa, the reaction temperature was 149 ℃ and the plasma power supply connecting the high voltage electrode and the ground electrode was switched on, the voltage was adjusted to 49.5 kV and the frequency was 30 kHz. The carbonyl sulfur content in the tail gas is analyzed on line by chromatography. The rest of the procedure is the same as in example 1, and the reaction results are shown in Table 22:

TABLE 22H2S and CO2Conversion, carbonyl sulfide selectivity

H2S conversion rate,% CO2Conversion rate% Carbonyl sulfide selectivity,%)
97.3 23.1 90.2

Example 23

91 wt% Clay-containing diatomaceous earth (62 wt% SiO) doped with 2 wt% Mg-5.5 wt% Ca2) 1.5% by weight of diatomaceous earth (88% by weight of SiO)2) The catalyst is placed in the reaction chamber, the shell 4 is made of corundum, and nitrogen is introduced for 10 minutes to remove air in the reactor. Controlled by a mass flow meter to have a composition of 12 vol% H2S-88vol%CO2The mixed gas is used for 1000h-1The flow of space velocity is through the bed. The reaction pressure is 2.1MPa, the reaction temperature is 130 ℃, a plasma power supply for connecting a high-voltage electrode and a grounding electrode is connected, the voltage is adjusted to 54.5 kilovolts, and the frequency is 5 kilohertz. The carbonyl sulfur content in the tail gas is analyzed on line by chromatography. The rest is the same as example 1, and the reaction results are shown in Table 23:

TABLE 23H2S and CO2Conversion, carbonyl sulfide selectivity

H2S conversion rate,% CO2Conversion rate% Carbonyl sulfide selectivity,%)
95.6 10.9 95.1

Example 24

69 wt% Clay-containing diatomaceous earth (66 wt% SiO) doped with 4 wt% Mg-1 wt% Sr2) 26% by weight of argillaceous kieselguhr (28% by weight of SiO)2) The catalyst is placed in the reaction chamber, the shell 4 is made of ceramic, and nitrogen is introduced for 10 minutes to remove air in the reactor. Controlled by a mass flow meter to have a composition of 7 vol% H2S-93vol%CO2The mixed gas is used for 150 hours-1The flow of space velocity is through the bed. The reaction pressure is 2.5MPa, the reaction temperature is 145 ℃, a plasma power supply for connecting the high-voltage electrode and the grounding electrode is connected, the voltage is adjusted to 5 kilovolts, and the frequency is 1 kilohertz. The carbonyl sulfur content in the tail gas is analyzed on line by chromatography. The rest is the same as example 1, and the reaction results are shown in Table 24:

TABLE 24H2S and CO2Conversion, carbonyl sulfide selectivity

H2S conversion rate,% CO2Conversion rate% Carbonyl sulfide selectivity,%)
39.9 11.3 96.2

Example 25

71 wt% Clay-containing diatomaceous earth (60 wt% SiO) doped with 18 wt% Ca-6.7 wt% Sr2) -4.3% by weight of argillaceous diatomaceous earth (49% by weight of SiO)2) The catalyst is placed in the reaction chamber, the shell 4 is made of ceramic, and nitrogen is introduced for 10 minutes to remove air in the reactor. Controlled by a mass flow meter to have a composition of 27 vol% H2S-73vol%CO2The mixed gas is used for 8000h-1The flow of space velocity is through the bed. The reaction pressure is 2.7MPa, the reaction temperature is 141 ℃, a plasma power supply for connecting a high-voltage electrode and a grounding electrode is connected, the voltage is adjusted to 55 kilovolts, and the frequency is 13 kilohertz. The carbonyl sulfur content in the tail gas is analyzed on line by chromatography. The rest is the same as example 1, and the reaction results are shown in Table 25:

TABLE 25H2S and CO2Conversion, carbonyl sulfide selectivity

H2S conversion rate,% CO2Conversion rate% Carbonyl sulfide selectivity,%)
95.6 37.2 80.8

Example 26

10 wt% Be-13.2 wt% Mg doped 54 wt% diatomaceous earth (99 wt% SiO)2) 22.8% by weight of argillaceous kieselguhr (28% by weight of SiO)2) The catalyst is placed in the reaction chamber, the shell 4 is made of glass, and nitrogen is introduced for 10 minutes to remove air in the reactor. Controlled by a mass flow meter to make up 41 vol% H2S-59vol%CO2The mixed gas takes 800h-1The flow of space velocity is through the bed. The reaction pressure is 0.2MPa, the reaction temperature is 135 ℃, a plasma power supply for connecting a high-voltage electrode and a grounding electrode is connected, the voltage is adjusted to 1 kilovolt, and the frequency is 6 kilohertz. The carbonyl sulfur content in the tail gas is analyzed on line by chromatography. The rest is the same as example 1, and the reaction results are shown in Table 26:

TABLE 26H2S and CO2Conversion, carbonyl sulfide selectivity

H2S conversion rate,% CO2Conversion rate% Carbonyl sulfide selectivity,%)
27.3 10.2 77.8

Example 27

9 wt% Mg-6.5 wt% Ca doped 33 wt% diatomaceous earth (78 wt% SiO2) 51.5% by weight of argillaceous kieselguhr (39% by weight of SiO)2) The catalyst is placed in the reaction chamber, the shell 4 is made of quartz glass, and nitrogen is introduced for 10 minutes to remove air in the reactor. Controlled by a mass flow meter to have a composition of 8 vol% H2S-92vol%CO29000h of mixed gas-1The flow of space velocity is through the bed. The reaction pressure is 1MPa, the reaction temperature is 125 ℃, a plasma power supply for connecting a high-voltage electrode and a grounding electrode is connected, the voltage is adjusted to 11.5 kilovolts, and the frequency is 22 kilohertz. The carbonyl sulfur content in the tail gas is analyzed on line by chromatography.The rest is the same as example 1, and the reaction results are shown in Table 27:

TABLE 27H2S and CO2Conversion, carbonyl sulfide selectivity

H2S conversion rate,% CO2Conversion rate% Carbonyl sulfide selectivity,%)
100 8.2 91.0

Example 28

12 wt% Be-19.5 wt% Sr doped 21 wt% clayey diatomaceous earth (13 wt% SiO)2) 47.5% by weight of clayed diatomaceous earth (62% by weight of SiO)2) The catalyst is placed in the reaction chamber, the shell 4 is made of glass, and nitrogen is introduced for 10 minutes to remove air in the reactor. Controlled by a mass flow meter to have a composition of 40 vol% H2S-60vol%CO2The mixed gas is used for 400 hours-1The flow of space velocity is through the bed. The reaction pressure was 0.2MPa, the reaction temperature was 149 ℃ and the plasma power supply connecting the high voltage electrode and the ground electrode was switched on, the voltage was adjusted to 34.5 kV and the frequency was 6.5 kHz. The carbonyl sulfur content in the tail gas is analyzed on line by chromatography.

The rest is the same as example 1, and the reaction results are shown in Table 28:

TABLE 28H2S and CO2Conversion, carbonyl sulfide selectivity

H2S conversion rate,% CO2Conversion rate% Carbonyl sulfide selectivity,%)
63.5 41.6 68.7

Example 29

23 wt% Mg doped 61 wt% diatomaceous earth (78 wt% SiO)2) 16% by weight of clayed diatomaceous earth (74% by weight of SiO)2) The catalyst is placed in the reaction chamber, the shell 4 is made of corundum, and nitrogen is introduced for 10 minutes to remove air in the reactor. Controlled by a mass flow meter to have a composition of 20 vol% H2S-80vol%CO2Mixed gas for 870h-1The flow of space velocity is through the bed. The reaction pressure is 0.5MPa, the reaction temperature is 139 ℃, a plasma power supply for connecting the high-voltage electrode and the grounding electrode is connected, the voltage is adjusted to 30 kilovolts, and the frequency is 5.5 kilohertz. The carbonyl sulfur content in the tail gas is analyzed on line by chromatography. The rest is the same as example 1, and the reaction results are shown in Table 29:

TABLE 29H2S and CO2Conversion, carbonyl sulfide selectivity

H2S conversion rate,% CO2Conversion rate% Carbonyl sulfide selectivity,%)
88.6 45.1 86.3

Example 30

9 wt% Be doped 80 wt% clayed diatomaceous earth (71 wt% SiO)2) 11% by weight of diatomaceous earth (88% by weight of SiO)2) The catalyst is placed in the reaction chamber, the shell 4 is made of quartz glass, and nitrogen is introduced for 10 minutes to remove air in the reactor. Controlled by a mass flow meter to have a composition of 5 vol% H2S-95vol%CO2The mixed gas is used for 500 hours-1The flow of space velocity is through the bed. The reaction pressure is 1.6MPa, the reaction temperature is 120 ℃, a plasma power supply for connecting a high-voltage electrode and a grounding electrode is connected, the voltage is adjusted to 60 kilovolts, and the frequency is 30 kilohertz. The carbonyl sulfur content in the tail gas is analyzed on line by chromatography. The rest of the procedure is the same as in example 1, and the reaction results are shown in Table 30:

TABLE 30H2S and CO2Conversion, carbonyl sulfide selectivity

H2S conversion rate,% CO2Conversion rate% Carbonyl sulfide selectivity,%)
100 2.3 98.7

Example 31

5 wt% Ca-27.1 wt% Ba-doped 16 wt% clayey diatomaceous earth (3 wt% SiO)2) 51.9% by weight of clayed diatomaceous earth (55% by weight of SiO)2) The catalyst is placed in the reaction chamber, the shell 4 is made of glass, and nitrogen is introduced for 10 minutes to remove air in the reactor. Controlled by a mass flow meter to have a composition of 38 vol% H2S-62vol%CO2The mixed gas is mixed for 4000 hours-1The flow of space velocity is through the bed. The reaction pressure is 2.4MPa, the reaction temperature is 130 ℃, a plasma power supply for connecting a high-voltage electrode and a grounding electrode is connected, the voltage is adjusted to 61.5 kilovolts, and the frequency is 25 kilohertz. The carbonyl sulfur content in the tail gas is analyzed on line by chromatography. The rest is the same as example 1, and the reaction results are shown in Table 31:

table 31H2S and CO2Conversion, carbonyl sulfide selectivity

H2S conversion rate,% CO2Conversion rate% Carbonyl sulfide selectivity,%)
80.2 43.2 43.9

Example 32

25 wt% Ca doped 42 wt% Clay-containing diatomaceous earth (54 wt% SiO)2) 33% by weight of argillaceous kieselguhr (25% by weight of SiO)2) The catalyst is placed in the reaction chamber, the shell 4 is made of ceramic, and nitrogen is introduced for 10 minutes to remove air in the reactor. Controlled by a mass flow meter, and the composition is 46 vol%H2S-54vol%CO2The mixed gas is used for 200 hours-1The flow of space velocity is through the bed. The reaction pressure is 2.0MPa, the reaction temperature is 150 ℃, a plasma power supply for connecting the high-voltage electrode and the grounding electrode is connected, the voltage is adjusted to 69.5 kilovolts, and the frequency is 0.5 kilohertz. The carbonyl sulfur content in the tail gas is analyzed on line by chromatography. The rest of the reaction was carried out in the same manner as in example 1, and the results are shown in Table 32:

TABLE 32H2S and CO2Conversion, carbonyl sulfide selectivity

H2S conversion rate,% CO2Conversion rate% Carbonyl sulfide selectivity,%)
93.2 70.1 69.3

Example 33

19 wt% Ca-11.8 wt% Ba-doped 16 wt% clayey diatomaceous earth (22 wt% SiO)2) -53.2% by weight of argillaceous diatomaceous earth (29% by weight of SiO)2) The catalyst is placed in the reaction chamber, the shell 4 is made of quartz glass, and nitrogen is introduced for 10 minutes to remove air in the reactor. Controlled by a mass flow meter to have a composition of 30 vol% H2S-70vol%CO2The mixed gas takes 460h-1The flow of space velocity is through the bed. The reaction pressure is 2.8MPa, the reaction temperature is 121 ℃, a plasma power supply for connecting a high-voltage electrode and a grounding electrode is connected, the voltage is adjusted to 100 kilovolts, and the frequency is 14.7 kilohertz. The carbonyl sulfur content in the tail gas is analyzed on line by chromatography. The rest of the procedure was the same as in example 1As shown in table 33:

TABLE 33H2S and CO2Conversion, carbonyl sulfide selectivity

H2S conversion rate,% CO2Conversion rate% Carbonyl sulfide selectivity,%)
83.6 50.1 67.9

Example 34

24 wt% Be-22 wt% Sr doped 8 wt% diatomaceous earth (84 wt% SiO)2) 46% by weight of argillaceous kieselguhr (25% by weight of SiO)2) The catalyst is placed in the reaction chamber, the shell 4 is made of glass, and nitrogen is introduced for 10 minutes to remove air in the reactor. Controlled by a mass flow meter to have a composition of 37 vol% H2S-63vol%CO2The mixed gas is used for 550 hours-1The flow of space velocity is through the bed. The reaction pressure was 0.7MPa, the reaction temperature was 136 deg.C, the plasma power supply connecting the high voltage electrode and the ground electrode was turned on, the voltage was adjusted to 29 kV, and the frequency was 18.5 kHz. The carbonyl sulfur content in the tail gas is analyzed on line by chromatography. The rest is the same as example 1, and the reaction results are shown in Table 34:

table 34H2S and CO2Conversion, carbonyl sulfide selectivity

H2S conversion rate,% CO2Conversion rate% Carbonyl sulfide selectivity,%)
83.2 45.9 58.7

Example 35

6 wt% Clay-containing diatomaceous earth (69 wt% SiO) doped with 4 wt% Be-31 wt% Ba2) 59% by weight of argillaceous kieselguhr (25% by weight of SiO)2) The catalyst is placed in the reaction chamber, the shell 4 is made of corundum, and nitrogen is introduced for 10 minutes to remove air in the reactor. Controlled by a mass flow meter to have a composition of 24 vol% H2S-76vol%CO2The mixed gas takes 8850h-1The flow of space velocity is through the bed. The reaction pressure is 1.4MPa, the reaction temperature is 129 ℃, a plasma power supply for connecting a high-voltage electrode and a grounding electrode is connected, the voltage is adjusted to 50 kilovolts, and the frequency is 8.5 kilohertz. The carbonyl sulfur content in the tail gas is analyzed on line by chromatography. The rest is the same as example 1, and the reaction results are shown in Table 35:

TABLE 35H2S and CO2Conversion, carbonyl sulfide selectivity

H2S conversion rate,% CO2Conversion rate% Carbonyl sulfide selectivity,%)
97.1 31.9 76.5

Example 36

A75 wt% clay-containing diatomaceous earth (58 wt% SiO) doped with 10 wt% Be-15 wt% Ca2) The catalyst is placed in the reaction chamber, the shell 4 is made of glass, and nitrogen is introduced for 10 minutes to remove air in the reactor. Controlled by a mass flow meter to have a composition of 16 vol% H2S-84vol%CO2The mixed gas takes 2000h-1The flow of space velocity is through the bed. The reaction pressure is 0.9MPa, the reaction temperature is 144 ℃, a plasma power supply for connecting a high-voltage electrode and a grounding electrode is connected, the voltage is adjusted to 21 kilovolts, and the frequency is 10.5 kilohertz. The carbonyl sulfur content in the tail gas is analyzed on line by chromatography. The rest is the same as example 1, and the reaction results are shown in Table 36:

TABLE 36H2S and CO2Conversion, carbonyl sulfide selectivity

H2S conversion rate,% CO2Conversion rate% Carbonyl sulfide selectivity,%)
89.1 10.0 71.2

Example 37

22 wt% Be-doped 78 wt% diatomaceous earth (98wt%SiO2) The catalyst is placed in the reaction chamber, the shell 4 is made of quartz glass, and nitrogen is introduced for 10 minutes to remove air in the reactor. Controlled by a mass flow meter to have a composition of 48 vol% H2S-52vol%CO2The mixed gas is used for 950 hours-1The flow of space velocity is through the bed. The reaction pressure is 1.8MPa, the reaction temperature is 130 ℃, a plasma power supply for connecting a high-voltage electrode and a grounding electrode is connected, the voltage is adjusted to 8 kilovolts, and the frequency is 9.5 kilohertz. The carbonyl sulfur content in the tail gas is analyzed on line by chromatography. The rest of the procedure was the same as in example 1, and the reaction results are shown in Table 37

TABLE 37H2S and CO2Conversion, carbonyl sulfide selectivity

H2S conversion rate,% CO2Conversion rate% Carbonyl sulfide selectivity,%)
56.7 27.6 59.0

Example 38

92 wt% clayey diatomaceous earth (48 wt% SiO) doped with 0.5 wt% Be-1.9 wt% Sr2) 5.6% by weight of diatomaceous earth (95% by weight of SiO)2) The catalyst is placed in the reaction chamber, the shell 4 is made of ceramic, and nitrogen is introduced for 10 minutes to remove air in the reactor. Controlled by a mass flow meter to have a composition of 22 vol% H2S-78vol%CO2The mixed gas is used for 4500h-1The flow of space velocity is through the bed. The reaction pressure is 2.1MPa, the reaction temperature is 125 ℃, and the high-voltage power supply is connected and connectedThe plasma power supply to the electrode and ground was adjusted to 9.5 kv and 18 khz. The carbonyl sulfur content in the tail gas is analyzed on line by chromatography. The rest of the procedure was the same as in example 1, and the reaction results are shown in Table 38

TABLE 38H2S and CO2Conversion, carbonyl sulfide selectivity

H2S conversion rate,% CO2Conversion rate% Carbonyl sulfide selectivity,%)
78.8 28.1 62.6

The experimental results show that the low-temperature plasma and the alkaline earth metal modified diatomite cooperate to break thermodynamic equilibrium limitation and realize high-selectivity conversion of the carbon dioxide and hydrogen sulfide mixed gas to prepare carbonyl sulfide, and the method is an effective method for efficiently preparing carbonyl sulfide.

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