A sulfur-carbon integrated removal system and method

By combining a proton-coupled electron transfer electrolysis system with an organic electrocoupling agent, the separation of SO2 oxidation reaction and CO2 electrochemical reduction is achieved, generating high-value products. This solves the problems of high energy consumption and high cost in the comprehensive utilization of sulfur and carbon in existing technologies, and realizes low carbon emissions and efficient integrated removal of sulfur and carbon.

CN119776868BActive Publication Date: 2026-03-24SICHUAN UNIV
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Patent Information

Authority / Receiving Office
CN · China
Patent Type
Patents(China)
Current Assignee / Owner
Filing Date
2024-12-31
Publication Date
2026-03-24

AI Technical Summary

Technical Problem

Existing CCUS equipment suffers from high capture costs and limited product utilization. Flue gas desulfurization technology also suffers from high energy consumption and high costs, making it difficult to achieve low carbon emissions and efficient comprehensive utilization of sulfur and carbon.

Method used

The proton-coupled electron transfer (PCET) electrolysis system utilizes solar photovoltaic units to provide electricity. Through an organic electrocoupling agent, SO2 oxidation and CO2 electrochemical reduction reactions are separated in the electrolysis system to generate high-value-added products such as H2SO4 and CH4.

Benefits of technology

It achieves low-energy-consumption and high-efficiency integrated sulfur and carbon removal, reduces the overall electrolysis energy consumption of the process, avoids the risk of catalyst poisoning, generates high-value chemical raw materials, and reduces the overall cost.

✦ Generated by Eureka AI based on patent content.

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Abstract

The application discloses a sulfur-carbon integrated removal system and method, and belongs to the field of electrochemistry, comprising the following steps: through the competition of organic matter electric coupling agent to replace the anode electrochemical SO2 oxidation reaction, combining the electrochemical carbon dioxide reduction to construct a proton cycle driven sulfur-carbon integrated removal system, which is used for deep recovery of low-grade SO2 oxidation reaction energy, realizes electrochemical reduction of CO2, and reduces electrolysis energy consumption of the whole process. The application realizes the separation of SO2 chemical oxidation reaction and CO2 electrochemical reduction reaction in time and space through spatial decoupling mode, avoids the problem that SO2 enters the electrochemical system to cause CO2 catalyst poisoning, does not need additional consumption of the electric coupling agent, is beneficial to realize lower cost and higher efficiency of sulfuric acid stable separation, and is helpful to occupy an advantage in the field of device design for clean utilization of fossil energy in the future.
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Description

Technical Field

[0001] This invention relates to the field of electrochemistry, and more specifically, to an integrated sulfur and carbon removal system and method. Background Technology

[0002] Global industrialization has led to the massive consumption of fossil fuels. my country’s energy structure, which is dominated by coal, will not change fundamentally in the short term. The problems of flue gas pollution (SO2) and carbon emissions (CO2) caused by coal combustion are becoming increasingly serious.

[0003] To meet future demands, coal-fired power plants need to utilize carbon capture, storage, and utilization (CCUS) technology to achieve low carbon emissions. Currently operating CCUS equipment in China generally suffers from high capture costs and limited product utilization. Furthermore, existing flue gas desulfurization technologies such as wet lime / limestone-gypsum methods, dual-alkali methods, and carbon-based catalytic methods also have drawbacks such as high energy consumption and high costs. Therefore, developing integrated sulfur and carbon removal technology is an effective way to solve the dilemma of low-carbon desulfurization emissions in coal-fired power plants. Summary of the Invention

[0004] The purpose of this invention is to overcome the shortcomings of the prior art and provide an integrated sulfur and carbon removal system and method that can autonomously obtain renewable energy using solar photovoltaic units and capture and convert flue gas generated from the combustion of fossil fuels into high-value-added chemical raw materials through electrochemical means. This will play a significant role in the future realization of low-carbon and desulfurization comprehensive utilization of traditional energy sources such as coal and fuel oil.

[0005] The objective of this invention is achieved through the following solution:

[0006] An integrated sulfur and carbon removal system includes: an electrolysis system, a renewable energy power generation device, a UPS rectifier, a power supply, a first valve, a cathode storage tank, a first pump, a second pump, a second valve, an anode reaction zone, a cathode reaction zone, a third pump, a third valve, a gas-liquid separator, a liquid product collection device, a gas dryer, a gas product collection device, an extraction device, an HSO collection device, a fourth valve, a fifth valve, an anode storage tank, a fourth pump, and a reduction tower;

[0007] The electrical energy of the power source can be provided by a renewable energy power generation device after being processed by a UPS rectifier;

[0008] The electrolysis system is connected to a power source via wires; one side of the electrolysis system has an anode reaction zone, and the other side has a cathode reaction zone; the anode reaction zone and the cathode reaction zone are separated by a proton exchange membrane; the cathode reaction zone of the electrolysis system is connected to the inlet of the cathode storage tank via a delivery pipe and a first valve; the bottom end of the cathode storage tank is connected to a first pump via a delivery pipe; the outlet of the first pump is connected to the cathode reaction zone of the electrolysis system via a delivery pipe.

[0009] The cathode storage tank is connected to a third pump via a delivery pipe, and the outlet of the third pump is connected to a gas-liquid separator via a delivery pipe. The side end of the gas-liquid separator is connected to the cathode storage tank via a delivery pipe and a third valve. The lower end of the gas-liquid separator is connected to a liquid product collection device via a delivery pipe. The top end of the gas-liquid separator is connected to a gas dryer via a gas delivery pipe, and the outlet of the gas dryer is connected to a gas product collection device via a gas delivery pipe.

[0010] The anode reaction zone of the electrolysis system is connected to the inlet of the anode storage tank via a delivery pipe and a second valve. The bottom end of the anode storage tank is connected to the second pump via a delivery pipe. The outlet of the second pump is connected to the anode reaction zone of the electrolysis system via a delivery pipe.

[0011] The anode storage tank is connected to the fourth pumping pump via a delivery pipe. The outlet of the fourth pumping pump is connected to the reduction tower via a delivery pipe. The lower end of the reduction tower is connected to the anode storage tank via a delivery pipe and a fourth valve.

[0012] The anode storage tank is connected to the extraction device via a fifth valve through a delivery pipe, and the side outlet of the extraction device is connected to the anode storage tank through a delivery pipe.

[0013] Furthermore, the liquid outlet at the bottom of the extraction device is connected to an HSO collection device via a liquid delivery pipe.

[0014] Furthermore, the interior of the cathode reaction zone is filled with NaHCO3 solution.

[0015] Furthermore, the interior of the anode reaction zone is provided with a solution containing an organic electrocoupling agent Q. The type of organic electrocoupling agent Q includes AQDS, ADS, BQDS, Fe(CN)63- / 4-, MDEA, Tiron, Tiron A and its derivatives, phenol and its derivatives, phenthiazide derivatives and ferrocene derivatives, or organic compounds with PCET electrochemical reaction activity.

[0016] Furthermore, the reduction tower is equipped with a catalyst capable of catalyzing the reaction between SO2 and organic matter electrocouplers, including platinum catalysts, palladium catalysts, V / Al2O3, graphite, activated carbon, gold catalysts, RuO2, WO3, and substances capable of catalyzing the oxidation of SO2.

[0017] Furthermore, the cathode reaction zone is provided with a catalyst capable of catalyzing the CO reduction reaction, including Ag, Fe, Cu-based catalysts, cobalt phthalocyanine, nickel phthalocyanine, and catalysts capable of catalyzing the CORR reaction.

[0018] A method for integrated sulfur and carbon removal includes the following steps:

[0019] S1, construct the integrated sulfur and carbon removal system as described above;

[0020] S2, the organic electrocoupling agent QH undergoes an oxidation reaction in the anodic reaction zone of the electrolysis system to Q, releasing protons H. + The solution enters the reduction tower through the second valve under the action of the fourth pump, where it reacts with SO to produce QH and sulfuric acid. QH returns to the anode reaction zone under the action of the second pump to complete the cycle. The solution in the anode storage tank is collected by the extraction device to the HSO collection device. The protons generated in the anode reaction pass through the proton exchange membrane to the cathode reaction zone and undergo a CO reduction reaction with CO under the action of a catalyst. The reacted solution enters the gas-liquid separator through the first valve under the action of the third pump. The gaseous product enters the gas product collection device through the gas drying pipe, and the liquid product enters the liquid product collection device. The self-reducing semi-decoupled integrated sulfur and carbon removal system constructed through the above steps can achieve integrated sulfur and carbon removal. The overall reaction formula of the entire system is:

[0021] .

[0022] The beneficial effects of this invention include:

[0023] This invention proposes a novel proton-cycle-driven integrated sulfur and carbon removal strategy and designs an integrated sulfur and carbon removal electrochemical system. The system is powered by renewable energy and uses an organic electrocoupling agent with PCET electrochemical reactivity as a medium. Based on the PCET reaction principle, it achieves temporal and spatial separation of the CO2 electrochemical reduction reaction and the SO2 oxidation reaction, thereby generating high-value products while simultaneously removing sulfur and carbon. Specifically, the novel integrated sulfur and carbon removal system of this invention achieves integrated sulfur and carbon removal through three main processes: solar photovoltaic power generation, electrochemical reduction of CO2, and chemical oxidation of SO2 to generate H2SO4. The organic electrocoupling agent circulates between the anode side of the electrolytic cell and a separate reaction vessel. In the electrolytic cell, the cathode undergoes the CO2 electrochemical reduction reaction (CO2RR), while the anode undergoes the electrochemical oxidation reaction of the organic electrocoupling medium. The oxidized medium is circulated to an external reduction reaction tower, where it reacts with SO2 under the action of a catalyst to achieve chemical reduction and regeneration, oxidizing SO2 to H2SO4. Excess sulfuric acid is then extracted. Taking the reduction to produce methane as an example, the overall reaction formula is: .

[0024] This invention proposes a novel integrated sulfur and carbon removal electrochemical system. By competitively replacing the anodic electrochemical SO2 oxidation reaction with an organic electrocoupler and combining it with electrochemical carbon dioxide reduction (CO2RR) technology, a proton cycle-driven integrated sulfur and carbon removal technology and system are constructed. This system deeply recovers the energy from the low-grade SO2 oxidation reaction, achieving CO2 electrochemical reduction and reducing the overall electrolysis energy consumption. Utilizing the redox principle, the organic electrocoupler replaces the SO2 electrochemical oxidation reaction with an organic electrocoupler. Simultaneously, the organic electrocoupler spontaneously undergoes chemical reduction under the action of a catalyst, separating the SO2 oxidation reaction and the CO2 reduction reaction on both temporal and spatial scales, eliminating the risk of catalyst poisoning caused by SO2 entering the electrochemical system. Attached Figure Description

[0025] To more clearly illustrate the technical solutions in the embodiments of the present invention or the prior art, the drawings used in the description of the embodiments or the prior art will be briefly introduced below. Obviously, the drawings described below are only some embodiments of the present invention. For those skilled in the art, other drawings can be obtained based on these drawings without creative effort.

[0026] Figure 1 This is a schematic diagram of the system structure according to an embodiment of the present invention;

[0027] In the diagram, 1-electrolysis system, 2-renewable energy power generation device, 3-UPS rectifier, 4-power supply, 5-first valve, 6-cathode storage tank, 7-first pump, 8-second pump, 9-second valve, 10-anode reaction zone, 11-cathode reaction zone, 12-third pump, 13-third valve, 14-gas-liquid separator, 15-liquid product collection device, 16-gas dryer, 17-gas product collection device, 18-extraction device, 19-H2SO4 collection device, 20-fourth valve, 21-fifth valve, 22-anode storage tank, 23-fourth pump, 24-reduction tower.

[0028] Figure 2 This is a schematic diagram illustrating the stability of the SOR on the anode side of the system according to an embodiment of the present invention under high current density.

[0029] Figure 3 This is a schematic diagram of the CO2 reduction stability on the cathode side of the system in an embodiment of the present invention. Detailed Implementation

[0030] All features disclosed in all embodiments of this specification, or steps in all methods or processes implied in the disclosure, may be combined and / or extended or replaced in any way, except for mutually exclusive features and / or steps.

[0031] In view of the problems in the background, the inventors of this invention believe that:

[0032] SO2, as a substance with significant reducing properties, contains abundant chemical energy and can be oxidized to sulfuric acid at a relatively low potential of 0.158V vs RHE. Furthermore, CO2 is a non-toxic, inexpensive, and abundant carbon source that can be reduced to high-value products such as methanol and methane. Utilizing the inherent advantages of SO2 and CO2 for targeted treatment, and introducing indirect SO2 oxidation and CO2 electroreduction into an electrolysis system, can achieve integrated sulfur and carbon removal while converting both into high-value-added products. This would be an effective strategy to solve the problems mentioned above.

[0033] Therefore, this invention aims to propose an electrolysis system that combines proton-coupled electron transfer (PCET). By introducing an organic electrocoupling agent as a medium, the SO2 oxidation reaction is separated from the electrochemical process. At the same time, the energy released by SO2 oxidation is used to promote the low-energy carbon dioxide electroreduction process CO2RR, thus constructing an electrochemical sulfur and carbon removal integrated system that can achieve low-energy, high-efficiency and stable sulfur and carbon removal.

[0034] Specifically, photovoltaic or wind power provides renewable electricity, which is then transmitted to the power source via a UPS rectifier. Driven by this renewable electricity, the cathode region of the electrolysis system undergoes an electrochemical reduction reaction of carbon dioxide (CO2RR). Under the action of a specific catalyst, carbon dioxide (CO2) is reduced to high-value-added products such as methane (CH4), carbon monoxide (CO), methanol (CH3OH), and formic acid (HCOOH). These products are then further processed through gas-liquid separation and gas drying to obtain gaseous and liquid products. Simultaneously, the anode region undergoes a PCET electrochemical oxidation reaction of an organic electrocoupler, releasing protons (H). + Protons are transferred to the cathode side through the proton exchange membrane for electrocatalytic CO2 reduction. The oxidized organic electrocoupler is circulated to an external buffer tank by a pump. The buffer tank solution is circulated to the reduction reaction tower by a pump. In the reduction reaction tower, it reacts with sulfur dioxide (SO2) and is chemically reduced to achieve regeneration. SO2 is oxidized to sulfuric acid (H2SO4). Then, it is further passed through an extraction tower to collect the sulfuric acid product.

[0035] Taking the reduction of CO2 to methane as an example, the reaction formula is as follows:

[0036] Cathode region: CO2 + 8H + +8e -→CH4+2H2O

[0037] Anode region: QH2-2e - →Q+2H +

[0038] Chemical reaction zone: Q + SO₂ + 2H₂O → QH₂ + SO₄ 2- +2H +

[0039] Overall reaction: CO2 + 4SO2 + 6H2O → CH4 + 4H2SO4

[0040] The sulfur and carbon integrated removal system of this invention can, in principle, separate the chemical oxidation reaction of SO2 and the electrochemical reduction reaction of CO2 in time and space through spatial decoupling, avoiding the problem of CO2 catalyst poisoning caused by SO2 entering the electrochemical system. It does not require additional consumption of mass-electro-coupled agents, which is conducive to achieving lower cost and more efficient stable separation of sulfuric acid, and helps to gain an advantage in the field of clean utilization of fossil energy in the future.

[0041] In a further implementation, combined with Figure 1 The details are as follows:

[0042] This invention provides an integrated sulfur and carbon removal system, comprising an electrolysis system 1 for electrolysis, a renewable energy power generation device 2, a UPS rectifier 3, a power supply 4, a first valve 5, a cathode storage tank 6, a first pump 7, a second pump 8, a second valve 9, an anode reaction zone 10, a cathode reaction zone 11, a third pump 12, a third valve 13, a gas-liquid separator 14, a liquid product collection device 15, a gas dryer 16, a gas product collection device 17, an extraction device 18, an H2SO4 collection device 19, a fourth valve 20, a fifth valve 21, an anode storage tank 22, a fourth pump 23, and a reduction tower 24.

[0043] The electrolysis system 1 is connected to the power supply 4 via a wire. The electrical energy of the power supply 4 is provided by the renewable energy generation device 2 after being processed by the UPS rectifier 3.

[0044] The electrolysis system 1 has an anode reaction zone 10 on one side and a cathode reaction zone 11 on the other side, with a proton exchange membrane separating the anode reaction zone 10 and the cathode reaction zone 11.

[0045] The cathode reaction zone 11 of the electrolysis system 1 is connected to the inlet of the cathode storage tank 6 via a liquid delivery pipe and a first valve 5. The bottom end of the cathode storage tank 6 is connected to the first pump 7 via a liquid delivery pipe. The outlet of the first pump 7 is connected to the cathode reaction zone 11 of the electrolysis system 1 via a liquid delivery pipe.

[0046] The cathode storage tank 6 is connected to the third pump 12 via a delivery pipe. The outlet of the third pump 12 is connected to the gas-liquid separator 14 via a delivery pipe. The side end of the gas-liquid separator 14 is connected to the cathode storage tank 6 via a delivery pipe and a third valve 13. The lower end of the gas-liquid separator 14 is connected to the liquid product collection device 15 via a delivery pipe. The top end of the gas-liquid separator 14 is connected to the gas dryer 16 via a gas delivery pipe. The outlet of the gas dryer 16 is connected to the gas product collection device 17 via a gas delivery pipe.

[0047] The anode reaction zone 10 of the electrolysis system 1 is connected to the inlet of the anode storage tank 22 via a delivery pipe and a second valve 9. The bottom end of the anode storage tank 22 is connected to the second pump 8 via a delivery pipe. The outlet of the second pump 8 is connected to the anode reaction zone 10 of the electrolysis system 1 via a delivery pipe.

[0048] The anode storage tank 22 is connected to the fourth pump 23 via a delivery pipe. The outlet of the fourth pump 23 is connected to the reduction tower 24 via a delivery pipe. The lower end of the reduction tower 24 is connected to the anode storage tank 22 via a delivery pipe and the fourth valve 20.

[0049] The anode storage tank 22 is connected to the extraction device 18 via the fifth valve 21 through the infusion pipe. The extraction device is connected to the anode storage tank 22 through the infusion pipe at the side outlet of the extraction device.

[0050] The liquid outlet at the bottom of the extraction device is connected to the H2SO4 collection device 19 via a liquid delivery pipe.

[0051] The interior of the cathode reaction zone 11 is filled with NaHCO3 solution.

[0052] The interior of the anode reaction zone 10 is provided with an acidic solution containing an organic electrocoupling agent.

[0053] The reduction tower 24 is equipped with substances that can catalyze the reaction between SO2 and organic matter electrocouplers, including platinum catalysts such as platinum on carbon, palladium catalysts such as palladium on carbon, V / Al2O3, graphite, activated carbon, gold catalysts, RuO2, WO3 and other substances that can catalyze the oxidation of SO2.

[0054] In a further embodiment, a corresponding integrated sulfur and carbon removal method is provided, comprising the following steps:

[0055] Mass-to-electrode coupling agents (MEAs) are required to be highly soluble redox couples capable of reversible redox reactions. They are characterized by excellent redox cycling ability, strong stability in dilute sulfuric acid, and a theoretical redox potential slightly higher than the theoretical potential for SO2 oxidation (0.158V vs. RHE), but still lower than the actual potential for SO2 generation on the electrode material. Organic MEAs Q include, but are not limited to, AQDS, ADS, BQDS, Fe(CN)63- / 4-, MDEA, Tiron, Tiron A and its derivatives, phenol and its derivatives, phenathiazide derivatives and ferrocene derivatives, or organic compounds with PCET electrochemical reactivity.

[0056] In this embodiment, AQDS / AQDSH2 is used as a mass-electric coupling agent in the system. This substance has good redox properties and is soluble in dilute sulfuric acid, which meets the basic requirements of a mass-electric coupling agent. The AQDS / AQDSH2 redox couple is used as a carrier circulating between the anode pool and the separate reactor to construct a self-reducing semi-decoupled sulfur and carbon integrated removal system to achieve integrated sulfur and carbon removal.

[0057] Mass-electric coupling agent AQDSH2 is dissolved in dilute sulfuric acid and undergoes an oxidation reaction in the anodic reaction zone 10 of the electrolytic cell to form AQDS. The solution then enters the anodic storage tank 22 through the second valve 9.

[0058]

[0059] The solution in the anode storage tank 22 is pumped into the reduction tower 24 via the fourth pump 23 and a delivery pipe. Under the action of a catalyst, AQDS undergoes a spontaneous redox reaction with SO2, producing AQDSH2 and H2SO4. The solution then returns to the anode storage tank 22 through the fourth valve 20.

[0060]

[0061] The solution in the anode storage tank 22 is returned to the anode reaction zone 10 via the second pump 8 and the delivery pipe, thereby completing the stable circulation of the mass-electric coupling agent.

[0062] In a further embodiment, a corresponding integrated sulfur and carbon removal method is provided, comprising the following steps:

[0063] In cathode reaction zone 11, an electrochemical reduction reaction of CO2 occurs under the catalysis of a specific catalyst. The catalyst design requirements are: high selectivity, good activity, and stability in the CO2RR electrochemical reduction reaction catalyzed by the catalyst. Cobalt phthalocyanine is selected as the catalyst for the cathode CO2 reduction reaction to meet the above requirements for the catalyst of the cathode reaction. The following reaction occurs in cathode reaction zone 11, and the solution enters the cathode storage tank 6 through the first valve 5:

[0064]

[0065] The solution in the cathode storage tank 6 enters the gas-liquid separator 14 through the third pump 12. The separated gas enters the gas product collection device 17 through the gas delivery pipe and the gas drying pipe 16. The separated liquid can return to the cathode storage tank 6 through the third valve 13, or it can be transported to the liquid product collection device 15 through the delivery pipe. The solution in the cathode storage tank 6 returns to the cathode reaction zone 11 through the first pump 7.

[0066] The overall reaction of the entire system is:

[0067] .

[0068] In summary, the present invention has the following advantages:

[0069] Figure 2 This is a schematic diagram illustrating the stability of the SOR on the anode side of the system according to an embodiment of the present invention under high current density. Figure 3 This is a schematic diagram of the CO2 reduction stability on the cathode side of the system in an embodiment of the present invention.

[0070] This invention innovatively combines a proton cycle-driven decoupling system with sulfur and carbon removal from fossil fuel flue gas, constructing an integrated electrochemical sulfur and carbon removal technology and system. By using an organic electrocoupling agent as a redox medium, the SO2 oxidation reaction and CO2 electrochemical reduction are coupled into one system to achieve integrated sulfur and carbon removal.

[0071] The sulfur and carbon removal process driven by proton cycle in this invention is as follows: the mass-electric coupling agent undergoes an oxidation reaction in the anode reaction zone of the electrolytic cell, and the oxidized mass-electric coupling agent is transferred to the reduction tower. Under the action of a catalyst, it undergoes a spontaneous redox reaction with SO2, realizing the reversible circulation of the mass-electric coupling agent and producing H2SO4. In the cathode reaction zone of the electrolytic cell, the CO2 reduction reaction occurs, and CH4 is produced under the action of a specific catalyst.

[0072] The system of this invention is conducive to achieving stable separation of products at a lower cost and with higher efficiency.

[0073] The entire system of this invention can be designed as a portable integrated device, or as an integrated sulfur and carbon removal system, to achieve low-cost and environmentally friendly treatment of sulfur- and carbon-containing waste gas.

[0074] This invention primarily targets the low-carbon utilization of fossil fuels, but it can also be applied to the field of air pollution control. Its essence is to fully recover the chemical energy released by SO2 oxidation to reduce the energy consumption of carbon dioxide electrochemical reduction. Related strategies can be extended to other small-molecule oxidation-coupled carbon reduction systems, generating a wide-ranging impact in energy-related research fields.

Claims

1. An integrated sulfur and carbon removal system, characterized in that, include: Electrolysis system (1), renewable energy power generation device (2), UPS rectifier (3), power supply (4), first valve (5), cathode storage tank (6), first pump (7), second pump (8), second valve (9), anode reaction zone (10), cathode reaction zone (11), third pump (12), third valve (13), gas-liquid separator (14), liquid product collection device (15), gas dryer (16), gas product collection device (17), extraction device (18), H2SO4 collection device (19), fourth valve (20), fifth valve (21), anode storage tank (22), fourth pump (23), and reduction tower (24); The electrical energy of the power source (4) can be supplied by the renewable energy power generation device (2) after being processed by the UPS rectifier (3); The electrolysis system (1) is connected to a power supply (4) via a wire; the electrolysis system (1) has an anode reaction zone (10) on one side and a cathode reaction zone (11) on the other side; the anode reaction zone (10) and the cathode reaction zone (11) are separated by a proton exchange membrane; the cathode reaction zone (11) of the electrolysis system (1) is connected to the inlet of the cathode storage tank (6) via a first valve (5) through a delivery pipe, the bottom end of the cathode storage tank (6) is connected to a first pump (7) via a delivery pipe, and the outlet of the first pump (7) is connected to the cathode reaction zone (11) of the electrolysis system (1) via a delivery pipe. The cathode storage tank (6) is connected to the third pump (12) via a delivery pipe. The outlet of the third pump (12) is connected to the gas-liquid separator (14) via a delivery pipe. The side end of the gas-liquid separator (14) is connected to the cathode storage tank (6) via a delivery pipe and a third valve (13). The lower end of the gas-liquid separator (14) is connected to the liquid product collection device (15) via a delivery pipe. The top end of the gas-liquid separator (14) is connected to the gas dryer (16) via a gas delivery pipe. The outlet of the gas dryer (16) is connected to the gas product collection device (17) via a gas delivery pipe. The anode reaction zone (10) of the electrolysis system (1) is connected to the inlet of the anode storage tank (22) through the second valve (9) via the inlet pipe. The bottom end of the anode storage tank (22) is connected to the second pump (8) through the inlet pipe. The outlet of the second pump (8) is connected to the anode reaction zone (10) of the electrolysis system (1) through the inlet pipe. The anode storage tank (22) is connected to the fourth pump (23) through a delivery pipe. The outlet of the fourth pump (23) is connected to the reduction tower (24) through a delivery pipe. The lower end of the reduction tower (24) is connected to the anode storage tank (22) through a delivery pipe and the fourth valve (20). The anode storage tank (22) is connected to the extraction device (18) via a fifth valve (21) through a delivery pipe, and the side outlet of the extraction device (18) is connected to the anode storage tank (22) through a delivery pipe. The anode reaction zone (10) contains a solution containing an organic electrocoupling agent Q. The type of organic electrocoupling agent Q is selected from AQDS, ADS, BQDS, and Fe(CN)6. 3- Fe(CN)6 4- MDEA, Tiron, Phenol, Phenythiazide, or Ferrocene; The reduction tower (24) is equipped with a catalyst that can catalyze the reaction of SO2 with an organic electrocoupler, selected from platinum, palladium, V / Al2O3, graphite, activated carbon, gold, RuO2 or WO3; The cathode reaction zone (11) is provided with a catalyst capable of catalyzing the CO2 reduction reaction, selected from Ag, Fe, Cu, cobalt phthalocyanine or nickel phthalocyanine.

2. The integrated sulfur and carbon removal system according to claim 1, characterized in that, The bottom outlet of the extraction device is connected to the H2SO4 collection device (19) via a delivery pipe.

3. The integrated sulfur and carbon removal system according to claim 1, characterized in that, The cathode reaction zone (11) is filled with NaHCO3 solution.

4. A method for integrated sulfur and carbon removal, characterized in that, Includes the following steps: S1, construct the integrated sulfur and carbon removal system as described in any one of claims 1 to 3; S2, the organic electrocoupling agent QH2 undergoes an oxidation reaction to Q in the anode reaction zone (10) of the electrolysis system (1) and releases protons H. + The solution enters the reduction tower (24) through the second valve (9) under the action of the fourth pump (23) and reacts with SO2 to generate QH2 and sulfuric acid. QH2 returns to the anode reaction zone (10) under the action of the second pump (8) to complete the cycle. The solution in the anode storage tank is collected in the H2SO4 collection device (19) through the extraction device (18). The protons generated by the anode reaction reach the cathode reaction zone (11) through the proton exchange membrane and react with CO2 under the action of the catalyst to undergo CO2 reduction reaction. The solution after the reaction enters the gas-liquid separator (14) through the first valve (5) under the action of the third pump (12). The gaseous product enters the gas product collection device (17) through the gas drying pipe (16), and the liquid product enters the liquid product collection device (15). The self-reducing semi-decoupled sulfur and carbon integrated removal system constructed through the above steps can realize the integrated removal of sulfur and carbon. The overall reaction formula of the whole system is: 。

Citation Information

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