Desulfurizing agent and application thereof
By using an aqueous solution containing transition metal ions, complexing agents, alkalis, stabilizers and accelerators as desulfurizers, the problems of low COS removal rate and catalyst deactivation in the prior art are solved, and efficient and environmentally friendly COS deactivation are achieved. Except for the effect, there is no additional sulfur-containing solid waste generated.
Patent Information
- Application Number
- CN202311054176.0
- Authority / Receiving Office
- CN · China
- Patent Type
- Applications(China)
- Current Assignee / Owner
- Filing Date
- 2023-08-21
- Publication Date
- 2025-02-21
AI Technical Summary
The prior art removes gases containing COS, and when used under aerobic conditions, the removal rate is low, and it is easy to cause catalyst deactivation, resulting in additional sulfur-containing solid waste, increasing production costs and causing pollution.
Provide an aqueous solution containing transition metal ions, complexing agents, alkalis, stabilizers and accelerators as desulfurization agents. Through the incorporation of accelerators, COS reacts rapidly in the aqueous phase to generate elemental sulfur, and desulfurization is recovered through oxidation regeneration. Avoid the production of additional sulfur-containing solid waste.
It achieves efficient removal of COS, with a desulfurization rate of ≥99%, no additional regenerative desulfurizer is required, the separation process is short, the resource utilization rate is high, and it is not affected by oxygen and carbon dioxide.
Smart Images
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Abstract
Description
Technical Field
[0001] The invention belongs to the technical field of gas purification and desulfurization, and particularly relates to a desulfurizer and application thereof. Background Art
[0002] Synthesis gas, calcium carbide tail gas, coke oven gas, and blast furnace gas are widely used in industrial production and daily life. These gases contain organic sulfides, primarily COS, which poses multiple hazards to industrial production and pollutes the environment. COS is chemically weak and difficult to remove using conventional desulfurization methods. Currently, the main removal technologies include hydrogenation reduction, hydrolysis conversion, organic amine absorption, solid-state adsorption, and liquid-phase absorption.
[0003] Hydrogenation conversion offers high removal accuracy, but hydrogenation catalysts are expensive and energy-intensive. Organic amine absorption and solid-state adsorption require frequent adsorbent regeneration, and COS in the desorbed product requires further treatment. Liquid-phase absorption utilizes wet desulfurization fluid to absorb COS, but its COS removal rate is low, ≤80%. Furthermore, due to its similar structure to CO2, COS competes with CO2 during dissolution, absorption, and adsorption. Consequently, COS removal rates in the presence of CO2 are only 20-50%. Therefore, organic amine absorption, solid-state adsorption, and liquid-phase absorption are only suitable for crude removal.
[0004] The hydrolysis conversion method uses a hydrolysis catalyst to make COS react with water to produce carbon dioxide and hydrogen sulfide. Compared with the above methods, the hydrolysis conversion method has become the mainstream method for COS removal due to its low reaction temperature, high conversion rate and low energy consumption. However, most of them are multiphase reactions. If a small amount of oxygen is present in this process, it is easy to cause sulfation on the surface of the hydrolysis catalyst, covering the active sites of the catalyst and causing the hydrolysis catalyst to deactivate. At the same time, the hydrogen sulfide produced by hydrolysis needs further treatment. For example, after hydrolysis, desulfurization agents such as iron oxide, zinc oxide or activated carbon are needed to further remove hydrogen sulfide, resulting in a long desulfurization process. In addition, the desulfurization agent becomes sulfur-containing solid waste after use, which not only increases the production cost of the enterprise but also causes new pollution. Therefore, it is necessary to develop a new desulfurization technology. Summary of the Invention
[0005] In response to the deficiencies of the prior art, the present invention provides a desulfurizer and its application. The desulfurizer has a high COS removal rate, COS directly generates elemental sulfur, which is easy to separate, and no additional sulfur-containing solid waste is generated, thus having wide practical value.
[0006] To achieve the above object, the present invention adopts the following technical solutions:
[0007] Provided is a desulfurizing agent, which is an aqueous solution containing transition metal ions, a complexing agent, an alkali, a stabilizer, and a accelerator; wherein:
[0008] By mass percentage, the transition metal ion is 0.01-5%, the base is 1-20%, the stabilizer is 1-20%, and the promoter is 0.001-0.2%;
[0009] The molar ratio of the complexing agent to the transition metal ion is 1.2 to 10:1;
[0010] The accelerator is a zinc or cobalt complex of an organic substance, and the organic substance is 1,4,7-triazacyclononane, 1,4,7,10-tetraazacyclododecane, porphyrin or phthalocyanine.
[0011] According to the above scheme, the transition metal ions are one or more of iron ions, manganese ions, and copper ions; preferably, the transition metal ions are iron ions, a combination of iron ions and manganese ions, a combination of iron ions and copper ions, or a combination of iron ions, manganese ions, and copper ions.
[0012] According to the above scheme, the complexing agent is one or more mixtures of EDTA, salicylic acid, polyaspartic acid, iminodisuccinic acid, diethylenetriaminepentacarboxylic acid, nitrilotriacetic acid, ethylenediaminetetraethylphosphonic acid, diethylenetriaminepentamethylphosphonic acid, and their salts. Complexing agents are used to stabilize metal ions in solution and prevent the formation of hydroxide precipitation from the reaction solution between the metal ions and the alkaline solution.
[0013] According to the above scheme, the base is one or more mixtures of sodium carbonate, potassium carbonate, sodium hydroxide, potassium hydroxide, ethylenediamine, ethanolamine, diethanolamine, triethanolamine, diglycolamine, piperazine, hydroxyethylpiperazine, aminoethylpiperazine, pyrazine, 2-aminopyrazine, pyridazine, 3-aminopyridazine, and isophoronediamine.
[0014] According to the above solution, the stabilizer is a water-soluble polyol, preferably a mixture of one or more of ethylene glycol, propylene glycol, butylene glycol, glycerol, polyethylene glycol, and glucose. The stabilizer mainly reduces the decomposition of the complexing agent during use.
[0015] According to the above scheme, the accelerator is prepared by adding 1,4,7-triazacyclononane, 1,4,7,10-tetraazacyclododecane, porphyrin or phthalocyanine to a zinc hydroxide or cobalt hydroxide suspension until the zinc hydroxide or cobalt hydroxide is completely dissolved.
[0016] According to the above solution, the desulfurizer also contains a sulfur dispersant and a corrosion inhibitor. The sulfur dispersant increases the size of the generated sulfur particles to facilitate filtration, and the corrosion inhibitor can slow down equipment corrosion.
[0017] Preferably, the sulfur dispersant is a polyethylene glycol surfactant; and the corrosion inhibitor is an imidazole compound.
[0018] Preferably, in the desulfurizer, the sulfur dispersant or corrosion inhibitor accounts for 0.001 to 0.5% by mass.
[0019] Provided is a use of the above-mentioned desulfurizing agent in catalytic removal of sulfur-containing gas, wherein the sulfur-containing gas contains carbonyl sulfide.
[0020] According to the above solution, the sulfur-containing gas also contains hydrogen sulfide.
[0021] According to the above scheme, the desulfurized gas is industrial raw gas such as natural gas, synthesis gas, calcium carbide tail gas, coke oven gas or blast furnace gas, wherein the blast furnace gas is blast furnace gas before residual pressure power generation (TRT) or blast furnace gas after TRT.
[0022] A desulfurization process is provided, comprising the following steps:
[0023] 1) placing the above-mentioned desulfurizing agent in a reactor, then introducing a sulfur-containing gas to fully contact and react with the desulfurizing agent at a reaction temperature of 40 to 90° C.; the sulfur-containing gas contains organic sulfur (COS);
[0024] 2) Sulfur is obtained by reaction, and after the reaction is completed, the sulfur is separated; the desulfurizer is oxidized and regenerated in an oxygen atmosphere, and the regenerated desulfurizer is returned to the desulfurization system, and step 1) is repeated.
[0025] According to the above solution, in step 1), the sulfur-containing gas also includes H2S.
[0026] According to the above scheme, the COS content in the sulfur-containing gas is ≤2000ppm, and the H2S content is ≤3000ppm.
[0027] According to the above scheme, in step 1), the sulfur-containing gas also includes carbon dioxide.
[0028] According to the above scheme, in step 1), the reactor is a packed tower, a plate tower, a spray tower, a bubble tower or a mixture thereof.
[0029] According to the above scheme, in step 1), the volume ratio of the sulfur-containing gas introduced per hour to the gas-liquid volume of the desulfurizer is 50 to 1500:1.
[0030] According to the above scheme, in step 2), the oxidative regeneration of the desulfurizer is as follows: if the sulfur-containing gas contains oxygen or air or oxygen-containing gas is added to the sulfur-containing gas, the oxygen content in the sulfur-containing gas is controlled to be between 0.01% and 2%, and the oxidative regeneration of the desulfurizer and the desulfurization reaction are carried out in the same reactor; if the sulfur-containing gas does not contain oxygen or the oxygen content is too low and additional air or oxygen-containing gas cannot be added, the oxidative regeneration process of the desulfurizer is carried out in a separate reactor, and the oxygen content in the sulfur-containing gas is controlled to be between 0.01% and 2% by introducing air or oxygen-containing gas to react with the desulfurizer to carry out oxidative regeneration of the desulfurizer.
[0031] Preferably, when a separate reactor is set up for the oxidation regeneration process of the desulfurizer, a tower reactor, a bubble reactor or a jet pump reactor is selected.
[0032] According to the above scheme, in step 2), sulfur is separated by sedimentation, filtration or centrifugation.
[0033] The beneficial effects of the present invention are:
[0034] 1. The desulfurizer of the present invention can make COS react quickly in the water phase by adding the accelerator, overcoming the problem that COS reacts slowly in the water phase, especially in the presence of carbon dioxide. Under the action of the accelerator, COS reacts quickly with water to form a hydrate and dissolves in water. The hydrate is hydrolyzed into HS under the action of alkali. - , HS - It is then rapidly oxidized into elemental sulfur by transition metal ions, the COS content in the aqueous phase becomes low, the COS solubility equilibrium is broken, and under the action of the promoter, COS in the gas phase continuously dissolves into the desulfurizer and generates elemental sulfur, solving the previous problem of slow conversion of COS in the aqueous phase. It can be used under aerobic conditions and is not affected by oxygen and carbon dioxide in sulfur-containing gases. When used to remove organic sulfur, the desulfurization rate is ≥99%, COS directly generates elemental sulfur, and pure elemental sulfur can be obtained for industrial application through simple separation. It has high resource utilization, short separation process, and no additional sulfur-containing solid waste is generated. It has wide practical value.
[0035] 2. The present invention provides a desulfurization process, in which a catalyst for removing organic sulfur is fully contacted and reacted with a sulfur-containing gas to directly obtain elemental sulfur. The elemental sulfur can be simply separated from the desulfurizer, and the desulfurizer can be reused after oxidation and regeneration. The desulfurizer does not require additional regeneration when used under aerobic conditions. The process has a high desulfurization rate, with a COS removal rate of over 99%. No additional sulfur-containing solid waste is generated. The obtained elemental sulfur can be directly used in industry. The desulfurizer oxidation and regeneration method is simple, and the entire desulfurization process is short, which has broad industrial application prospects. DETAILED DESCRIPTION
[0036] The present invention will be further explained below through specific examples.
[0037] Example 1
[0038] Take 2.8 grams of FeSO4.7H2O and dissolve it in 100 ml of water. Then add 4.4 grams of chelating agent EDTA to the FeSO4 solution, and then add 5 grams of base NaCO3. After stirring evenly, add 10 grams of stabilizer ethylene glycol to the solution to obtain solution 1.
[0039] 0.1 g of zinc hydroxide was added to 25 ml of water and stirred to form a suspension. Then 0.13 g of 1,4,7-triazacyclononane was added to the zinc hydroxide suspension and stirred for 30 minutes to completely dissolve the zinc hydroxide to obtain Solution 2.
[0040] The solution 2 is poured into the solution 1 and stirred evenly to obtain the desulfurizing agent of the present invention.
[0041] Example 2
[0042] Take 2.1 grams of FeSO4.7H2O and 0.423 grams of MnSO4.H2O and dissolve them in 100 ml of water. Then, add 7.4 grams of complexing agent iminodisuccinic acid to the FeSO4-MnSO4 mixed solution, and then add 6 grams of base NaOH. After stirring, add 3 grams of stabilizer propylene glycol to the solution to obtain solution 1.
[0043] 0.01 g of cobalt hydroxide was added to 10 ml of water and stirred to form a suspension. Then 0.02 g of 1,4,7,10-tetraazacyclododecane was added to the cobalt hydroxide suspension and stirred for 40 minutes to completely dissolve the cobalt hydroxide to obtain Solution 2.
[0044] The solution 2 is poured into the solution 1 and stirred evenly to obtain the desulfurizing agent of the present invention.
[0045] Example 3
[0046] Take 0.28 g of FeSO4.7H2O and dissolve it in 100 ml of water. Then add 0.5 g of nitrilotriacetic acid as a complexing agent to the FeSO4 solution, and then add 10 g of ethylenediamine as a base. After stirring evenly, add 5 g of glycerol as a stabilizer to the solution to obtain solution 1.
[0047] 0.1 g of zinc hydroxide was added to 50 ml of water and stirred to form a suspension. Then 0.065 g of 1,4,7-triazacyclononane and 0.09 g of 1,4,7,10-tetraazacyclododecane were added to the zinc hydroxide suspension and stirred for 30 min to completely dissolve the cobalt hydroxide to obtain Solution 2.
[0048] The solution 2 is poured into the solution 1 and stirred evenly to obtain the desulfurizing agent of the present invention.
[0049] Example 4
[0050] Take 0.56 g of FeSO4.7H2O and dissolve it in 100 ml of water. Then, add 2.5 g of diethylenetriamine pentacarboxylic acid as a complexing agent to the FeSO4 solution, and then add 18 g of diethanolamine as a base. After stirring evenly, add 6 g of glycerol as a stabilizer and 1 g of glucose to the solution to obtain solution 1.
[0051] Take 0.1 g of zinc hydroxide and 0.01 g of cobalt hydroxide, add them to 50 ml of water, and stir to form a suspension. Then take 0.20 g of 1,4,7,10-tetraazacyclododecane and add it to the zinc hydroxide suspension. Stir for 50 minutes to completely dissolve the cobalt hydroxide to obtain Solution 2.
[0052] The solution 2 is poured into the solution 1 and stirred evenly to obtain the desulfurizing agent of the present invention.
[0053] Example 5
[0054] Take 5.6 grams of FeSO4.7H2O and 0.2 grams of Cu(NO3)2.H2O and dissolve them in 100 ml of water. Then, add 10.5 grams of ethylenediaminetetraethylphosphonic acid (a complexing agent) to the FeSO4-Cu(NO3)2 mixed solution, then add 20 grams of diglycolamine (a base) and 3 grams of hydroxyethylpiperazine. After stirring evenly, add 2 grams of polyethylene glycol 500 (a stabilizer) to the solution to obtain Solution 1.
[0055] 0.01 g of zinc hydroxide was added to 10 ml of water and stirred to form a suspension. Then 0.02 g of 1,4,7,10-tetraazacyclododecane was added to the zinc hydroxide suspension and ultrasonicated for 10 minutes to completely dissolve the zinc hydroxide to obtain Solution 2.
[0056] The solution 2 is poured into the solution 1 and stirred evenly to obtain the desulfurizing agent of the present invention.
[0057] Example 6
[0058] Take 0.28 g of FeSO4.7H2O and dissolve it in 100 ml of water. Then, add 1.5 g of ethylenediaminetetraethylphosphonic acid (a complexing agent) to the FeSO4 solution, then add 10 g of isophoronediamine (a base) and 5 g of aminoethylpiperazine. After stirring, add 10 g of polyethylene glycol 300 (a stabilizer) and 2 g of glucose to the solution to obtain Solution 1.
[0059] 0.02 g of zinc hydroxide was added to 20 ml of water and stirred to form a suspension. Then 0.04 g of 1,4,7,10-tetraazacyclododecane was added to the zinc hydroxide suspension and stirred for 30 minutes to completely dissolve the zinc hydroxide to obtain Solution 2.
[0060] The solution 2 is poured into the solution 1 and stirred evenly to obtain the desulfurizing agent of the present invention.
[0061] Example 7
[0062] Take 0.162 g of FeCl3.6H2O and dissolve it in 100 ml of water. Then, add 0.8 g of diethylenetriamine penta (methylene phosphoric acid) as a complexing agent to the FeCl3 solution, then add 4.5 g of potassium hydroxide and 1 g of 3-aminopyridazine as alkali. After stirring, add 8 g of butanediol and 2 g of glucose as stabilizers to the solution to obtain solution 1.
[0063] 0.04 g of zinc hydroxide was added to 20 ml of water and stirred to form a suspension. Then 0.08 g of 1,4,7,10-tetraazacyclododecane was added to the zinc hydroxide suspension and stirred for 30 minutes to completely dissolve the zinc hydroxide to obtain Solution 2.
[0064] The solution 2 is poured into the solution 1 and stirred evenly to obtain the desulfurizing agent of the present invention.
[0065] Example 8
[0066] Take 0.160 g of Fe2O3 and pour it into a 250 ml beaker. Then add 1.8 g of complexing agent polyaspartic acid and 100 ml of water. After heating at 80°C to dissolve, add 2.5 g of ethanolamine and 2 g of 3-aminopyridazine. After stirring evenly, add 20 g of stabilizer glycerol to the solution to obtain Solution 1.
[0067] 0.04 g of zinc hydroxide was added to 20 ml of water and stirred to form a suspension. Then 0.08 g of 1,4,7,10-tetraazacyclododecane was added to the zinc hydroxide suspension and stirred for 30 minutes to completely dissolve the zinc hydroxide to obtain Solution 2.
[0068] The solution 2 is poured into the solution 1 and stirred evenly to obtain the desulfurizing agent of the present invention.
[0069] Example 9
[0070] Take 100 ml of the desulfurizer obtained in Example 4, add 0.2 g of sulfur dispersant PEG2000, 0.1 g of corrosion inhibitor ZH-2, and 0.2 g of sodium nitrate to obtain the desulfurizer of the present invention.
[0071] Comparative Example 1
[0072] Pour 0.50 g of Fe2O3 into a 250 ml beaker, then add 1.8 g of chelating agent EDTA and 100 ml of water. Heat at 80°C to dissolve, then add 5 g of base NaCO3. Stir the solution until evenly mixed, then add 10 g of stabilizer ethylene glycol to obtain Solution 1. Stir and mix thoroughly, then add water to adjust the solution volume to 125 ml to obtain Comparative Desulfurizer 1.
[0073] Comparative Example 2
[0074] Take 4.5 grams of EDTA salt and dissolve it in 100 ml of water. Then add 1.5 grams of diethanolamine, 1.0 grams of xylitol, 1.25 grams of 1000 mesh iron oxide, 0.45 grams of manganese oxide, 0.3 grams of zinc oxide, and 1.0 grams of sodium carbonate in sequence. Then heat to 85°C and maintain this temperature for 4 hours until the solid is completely dissolved or no longer dissolved. The desired desulfurizer solution is obtained by reaction. Then the pH value is adjusted to 9-10 with sodium carbonate solution to obtain comparative desulfurizer 2.
[0075] Example 10
[0076] 1) 100 ml of the desulfurizer obtained in Examples 1-8 and Comparative Examples 1-2 were respectively loaded into a bubbling bed reactor, and a sulfur-containing gas source without carbon dioxide and containing carbon dioxide was introduced, respectively. The sulfur-containing gas was passed into the bubbling bed reactor at 250 ml / min to react to obtain sulfur. After 6 hours of reaction, the import and export were analyzed by gas chromatography. The evaluation results are shown in Table 1.
[0077] 2) After the reaction is completed, the sulfur is separated, and the desulfurizer is simultaneously oxidized and regenerated during the catalytic reaction. The regenerated desulfurizer is returned to the desulfurization system and step 1) is repeated.
[0078] Table 1
[0079]
[0080] Example 11
[0081] 100 ml of the desulfurizer obtained in Example 9 was loaded into a bubbling bed reactor, and then a carbon dioxide-containing gas source 2 (315 mgs / Nm 3 COS+500mgs / Nm 3 +0.4% O2+25% CO2, residual nitrogen) evaluation, gas flow rate is shown in Table 2; sulfur is obtained by reaction, and the import and export are analyzed by gas chromatography, and the evaluation results are shown in Table 2;
[0082] 2) After the reaction is completed, the sulfur is separated, and the desulfurizer is simultaneously oxidized and regenerated during the catalytic reaction. The regenerated desulfurizer is returned to the desulfurization system and step 1) is repeated.
[0083] Table 2. Desulfurizer after adding dispersant and corrosion inhibitor
[0084]
[0085] As can be seen from Table 2, the performance of the desulfurizer remains basically unchanged after the addition of dispersant and corrosion inhibitor, which is beneficial to industrial application.
[0086] Example 12
[0087] Take 100ml of the desulfurizer obtained in Example 4 and put it into the bubbling bed reactor, and then introduce the carbon dioxide gas source 2 (315mgs / Nm 3 COS+500mgs / Nm 3 +0.4% O2+25% CO2) for 720h life test, the experimental results are shown in Table 3:
[0088] Table 3
[0089]
[0090] It can be seen from Table 3 that the desulfurization activity of the desulfurizer is stable during the 500h experimental period.
[0091] The present invention uses specific examples to illustrate the inventive concept in detail. The above embodiments are only intended to help understand the core concept of the present invention. It should be noted that any obvious modifications, equivalent substitutions, or other improvements made by a person skilled in the art without departing from the inventive concept should be included in the scope of protection of the present invention.
Claims
1. A desulfurizing agent, characterized in that: It is an aqueous solution containing transition metal ions, a complexing agent, a base, a stabilizer and a promoter; wherein: By mass percentage, the transition metal ion is 0.01-5%, the base is 1-20%, the stabilizer is 1-20%, and the promoter is 0.001-0.2%; The molar ratio of the complexing agent to the transition metal ion is 1.2 to 10:1; The accelerator is a zinc or cobalt complex of an organic substance, and the organic substance is 1,4,7-triazacyclononane, 1,4,7,10-tetraazacyclododecane, porphyrin or phthalocyanine.
2. The desulfurizing agent according to claim 1, characterized in that The transition metal ion is one or more of iron ion, manganese ion and copper ion; the complexing agent is one or more of EDTA, salicylic acid, polyaspartic acid, iminodisuccinic acid, diethylenetriaminepentacarboxylic acid, nitrilotriacetic acid, ethylenediaminetetraethylphosphonic acid, diethylenetriaminepentamethylphosphonic acid and a mixture of their salts.
3. The desulfurizing agent according to claim 1, characterized in that The base is one or more mixtures of sodium carbonate, potassium carbonate, sodium hydroxide, potassium hydroxide, ethylenediamine, ethanolamine, diethanolamine, triethanolamine, diglycolamine, piperazine, hydroxyethylpiperazine, aminoethylpiperazine, pyrazine, 2-aminopyrazine, pyridazine, 3-aminopyridazine, and isophoronediamine; and the stabilizer is a polyol soluble in water.
4. The desulfurizing agent according to claim 1, characterized in that The desulfurizing agent also contains a sulfur dispersant and a corrosion inhibitor.
5. Use of the desulfurizing agent according to any one of claims 1 to 4 in catalytic removal of sulfur-containing substances in sulfur-containing gas, wherein the sulfur-containing gas contains carbonyl sulfide.
6. The use according to claim 5, characterized in that: The desulfurized gas is natural gas, synthesis gas, calcium carbide tail gas, coke oven gas or blast furnace gas industrial raw material gas; the blast furnace gas is blast furnace gas before TRT or blast furnace gas after TRT; the sulfur-containing gas also contains hydrogen sulfide.
7. A desulfurization process, characterized in that: The following steps are involved: 1) placing the desulfurizing agent according to any one of claims 1 to 4 in a reactor, and then introducing sulfur-containing gas to fully contact and react with the desulfurizing agent at a reaction temperature of 40 to 90° C.; 2) Sulfur is obtained by reaction, and after the reaction is completed, the sulfur is separated; the desulfurizer is oxidized and regenerated in an oxygen atmosphere, and the regenerated desulfurizer is returned to the desulfurization system, and step 1) is repeated.
8. The process according to claim 7, characterized in that: In the step 1), the sulfur-containing gas also includes carbon dioxide.
9. The process according to claim 7, characterized in that: In the step 1), the volume ratio of the sulfur-containing gas introduced per hour to the gas-liquid volume of the desulfurizing agent is 50 to 1500:
1.
10. The process according to claim 7, characterized in that: In the step 2), the oxidative regeneration of the desulfurizer is as follows: if the sulfur-containing gas contains oxygen or air or oxygen-containing gas is added to the sulfur-containing gas, the oxygen content in the sulfur-containing gas is controlled to be between 0.01% and 2%, and the oxidative regeneration of the desulfurizer and the desulfurization reaction are carried out in the same reactor; if the sulfur-containing gas does not contain oxygen or the oxygen content is too low and additional air or oxygen-containing gas cannot be added, the oxidative regeneration process of the desulfurizer is carried out in a separate reactor, and the oxygen content in the sulfur-containing gas is controlled to be between 0.01% and 2% by introducing air or oxygen-containing gas to react with the desulfurizer to carry out oxidative regeneration of the desulfurizer.