CN110877899A - Method for treating low-concentration sulfur-containing acidic gas - Google Patents
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- C01B17/00—Sulfur; Compounds thereof
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- C01B17/04—Preparation of sulfur; Purification from gaseous sulfur compounds including gaseous sulfides
- C01B17/0404—Preparation of sulfur; Purification from gaseous sulfur compounds including gaseous sulfides by processes comprising a dry catalytic conversion of hydrogen sulfide-containing gases, e.g. the Claus process
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Abstract
The invention relates to a method for treating low-concentration sulfur-containing acidic gas, belonging to the technical field of gas purification. The invention relates to a method for treating low-concentration sulfur-containing acidic gas, which is characterized in that the low-concentration sulfur-containing acidic gas is sequentially treated by an incineration unit, a denitration unit and an absorption regeneration unit, wherein an absorbent adopted by the absorption regeneration unit comprises the following raw materials in percentage by weight: 10-30% of diisopropanolamine, 10-25% of compound component and the balance of water; the complex component is one or more of 2-amino-2-methyl-1-propanol, diethylethanolamine or methylethanolamine. The invention converts the acid gas with complex components into sulfur dioxide and ensures NOX、SO2The emission meets the latest national emission requirements, and SO in the tail gas2At 30mg/m3Hereinafter, NOXThe discharge is less than 50mg/m3Has obvious economic and environmental protection benefits.
Description
Technical Field
The invention relates to a method for treating low-concentration sulfur-containing acidic gas, belonging to the technical field of gas purification.
Background
According to the requirements of national emission Standard of pollutants for Petroleum refining industry (GB31570-2015), sulfur dioxide with the limit value of the emission concentration of atmospheric pollutants of the sulfur device is less than 400mg/Nm from 7 to 1 in 20173Especially less than 100mg/Nm3。
The treatment of low-concentration acid gas has been difficult, and the low-concentration acid gas has complex components and often contains thioether, mercaptan, methanol and CO2、NH3And HCN and other impurities cause a large amount of side reactions. At present, the treatment of low-concentration acid gas is basically carried out by mixing with other high-concentration acid gas and then feeding into a sulfur production furnace of a sulfur recovery device for treatment or adopting processes such as selective oxidation and the like, but the treatment of the acid gas by adopting the method is easy to generate a large amount of NOX or organic sulfur to cause flue gas SO2And the NOx emission seriously exceeds the standard.
CN104528659A discloses a sulfur recovery process for treating low-concentration acid gas by liquid sulfur circulation, which is characterized by comprising the following steps: atomizing liquid sulfur and H generated in coal chemical industry process2Mixing acid gases, carrying out Claus combustion by oxygen enrichment or air combustion supporting, carrying out two-stage Claus reaction on process gas generated by combustion, sequentially carrying out hydrogenation-direct oxidation and wet washing on tail gas generated by the two-stage Claus reaction, and recovering sulfur generated in the Claus combustion, the two-stage Claus reaction and the hydrogenation-direct oxidation processes. The invention adopts wet washing, only simply transfers the sulfur in the gas phase to the liquid sulfur, causes secondary pollution, and does not actually improve the recovery rate of the sulfur.
CN201510795018.X discloses a process for recovering low-sulfur emission sulfur from low-concentration acid gas, H2The low-concentration acid gas with the S content less than 5 percent is treated by a selective oxidation reactor and two adsorption desulfurization towers which can be connected in parallel and in series, so as to achieve the aim of desulfurization; selective oxidation reactorMiddle filling H2S is acid gas containing ammonia, HCN and the like. A selective oxidation catalyst, wherein the adsorption desulfurization tower is filled with a catalytic oxidation adsorption desulfurizer capable of being thermally regenerated; the total sulfur of the process exhaust gas is converted into SO by properly selecting the catalyst and the desulfurizer and accurately controlling the process conditions of each step2≤10mg/m3. The process still adopts a selective oxidation technology, is only suitable for cleaning acid gas and cannot treat the acid gas containing ammonia, HCN and other gases.
Disclosure of Invention
It is an object of the present invention to provide a process for treating a sulfur-containing acid gas at a low concentration, which converts an acid gas of a complicated composition into sulfur dioxide while ensuring NOX、SO2The emission meets the latest national emission requirements, and SO in the tail gas2At 30mg/m3Hereinafter, NOXThe discharge is less than 50mg/m3Has obvious economic and environmental protection benefits.
The invention relates to a method for treating low-concentration sulfur-containing acidic gas, which is characterized in that the low-concentration sulfur-containing acidic gas is sequentially treated by an incineration unit, a denitration unit and an absorption regeneration unit, wherein an absorbent adopted by the absorption regeneration unit comprises the following raw materials in percentage by weight: 10-30% of diisopropanolamine, 10-25% of compound component and the balance of water;
the complex component is one or more of 2-amino-2-methyl-1-propanol, diethyl glycol amine or methyl ethanolamine.
Preferably, the absorbent comprises the following raw materials in percentage by weight: 25% of diisopropanolamine, 10% of diethyldialkanolamine, 5% of methylethanolamine and 60% of water.
The main function of the diisopropanolamine in the invention is to absorb SO2The main functions of the compound components are to improve the selectivity of the absorbent and reduce the regeneration energy consumption. The sulfur tail gas not only contains SO2And also contains CO2Gas, diisopropanolamine not only absorbs SO2While also absorbing CO2The steric effect of the compound components is utilized to reduce CO2The co-absorption of the absorbent improves the sulfur capacity of the absorbent and reduces the regeneration energy consumption of the absorbent at the same time.
The incineration unit is to incinerate sulfur containing ether, mercaptan, hydrogen sulfide and NH3Acid gas of impurities such as HCN adopts a thermal incineration mode, the temperature of an incineration unit furnace is controlled to be 950-1350 ℃, so that components in the acid gas are completely combusted; the process gas after thermal incineration enters a denitration unit for treatment, the catalyst adopted by the denitration unit is an SCR catalyst and mainly used for removing NOX(ii) a After denitration, the tail gas enters an absorption and regeneration unit through quenching, and an absorbent adopted by the absorption and regeneration unit is a compound organic amine solvent and is used for absorbing SO in the tail gas2The absorbed rich solution enters a regeneration unit, and the regenerated SO2Returning to Claus sulfur recovery device, and absorbing the purified tail gas SO2Less than 30mg/m3And can be directly discharged.
The incineration unit can convert all the acid gas into SO2、N2、NOX、CO2In order to ensure the equivalent combustion of oxygen, the furnace temperature can be increased by adopting the forms of natural gas, hydrogen gas co-combustion and the like, and the rear part of the incinerator is connected with a waste heat boiler to generate medium-pressure steam for recovering heat.
The incinerator temperature is controlled to 950 ℃ and 1350 ℃ to ensure that the components in the acid gas are completely combusted.
In the low-concentration sour gas, H2S is 0-40% by volume, NH3The volume percentage of the five gases is 0-5%, the volume percentage of HCN is 0-50%, the volume percentage of thioether is 0-4%, the volume percentage of mercaptan is 0-8%, and the volume percentages of the five gases are not 0% at the same time.
The acid gas can be low-temperature methanol-washed acid gas, coal gasification flash steam, sulfur-tolerant shift waste gas, shift stripping tail gas, S-zorb flue gas, sewage stripping acid gas and the like.
The incinerator can be newly built, and the incinerator with the Claus tail gas treatment unit can also be used after being modified.
The SCR denitration catalyst adopted by the invention can be a noble metal catalyst, a metal oxide catalyst, an unsupported metal oxide catalyst or a molecular sieve catalyst, and has the main function ofConversion of NOX to N2。
The process flow in the absorption regeneration unit is as follows: introducing the denitrated gas into an absorption tower filled with the absorbent, and introducing SO2Absorbed by the absorbent; absorption of SO2The purified tail gas is discharged; containing SO2The rich solution enters a regeneration tower for regeneration, and regenerated SO2And the sulfur enters a sulfur recovery device for reutilization.
The temperature of the absorption tower is controlled to be 25-45 ℃; the temperature of the regeneration tower is controlled to be 110-125 ℃.
Absorption of SO2SO in the tail gas2The content is less than 30mg/m3。
After treatment of low concentration sour gas containing sulfur, NOXReduced to 50mg/m3The following.
Regenerated SO according to the invention2The treatment in the Claus sulfur recovery device refers to any part of the sulfur production furnace entering the sulfur recovery device before the hydrogenation reactor, and can be an air line and an acid gas line of the sulfur production furnace, a primary converter, a secondary converter and the like.
The specific process flow is as follows: the acid gas and air are mixed and then the combustible substance is completely combusted in the incinerator to generate SO2、NOX、CO2The process gas enters a denitration reactor to remove NOXConversion to N2Denitrated SO-containing2Cooling the process gas to 25-45 deg.c in a quenching tower, introducing into an amine liquid absorbing tower with compounded efficient organic amine solvent, and SO2Is absorbed by amine liquid to absorb SO2SO in the purified tail gas2The content is less than 30mg/m3Containing SO2The rich solution enters a regeneration tower for regeneration, and regenerated SO2And (4) entering a Claus sulfur recovery device for treatment. See in particular fig. 1.
The invention has the following beneficial effects:
(1) the compound organic amine desulfurizer of the invention has low cost and SO2The absorption rate is high;
(2) the invention uses SCR denitration catalyst and compound organic amine solution to convert acid gas with complex components into dioxideSulfur, NOXConversion to N2While ensuring NOXThe discharge is less than 50mg/m3，SO2The discharge is less than 30mg/m3The latest national emission requirement is met;
(3) the invention introduces the regenerated tail gas into the Claus sulfur recovery unit for treatment, avoids the influence of complex acid gas on the Claus sulfur recovery process, and meets the latest environmental protection standard;
(4) the invention is widely applied to low-concentration acid gas generated in industries such as petroleum refining, coal chemical industry and the like, and is particularly suitable for treating the low-concentration and complex-component acid gas generated by devices such as S-Zorb, low-temperature methanol washing, coal gasification and the like.
Drawings
FIG. 1 is a process flow diagram of the present invention;
in the figure: 1. air; 2. an acid gas; 3. an incinerator; 4. a waste heat boiler; 5. a denitration reactor; 6. a quench tower; 7. a water circulating pump; 8. a cooler; 9. sewage; 10. an absorption tower; 11. a rich solvent pump; 12. a lean-rich liquid heat exchanger; 13. barren liquor; 14. and (4) a regeneration tower.
Detailed Description
The present invention is further illustrated by the following examples, which are not intended to limit the practice of the invention.
Example 1
As shown in figure 1, the low-temperature methanol-washed acid gas is treated by adopting the process of the invention, natural gas is adopted for co-combustion, the combustible components are completely combusted, the temperature of the incinerator is controlled at 1300 ℃, the gas in the combustion process enters a denitration reactor, an unsupported metal oxide catalyst is filled in the denitration reactor, the reaction temperature is controlled at 150 ℃, tail gas after denitration is quenched and enters an absorption unit after being cooled to 40 ℃, absorption liquid used by the absorption unit is a compound solution of diisopropanolamine and 2-amino-2-methyl-1-propanol, wherein the diisopropanolamine is 30 percent (wt), the 2-amino-2-methyl-1-propanol is 15 percent (wt), the absorption temperature is 42 ℃, the absorbed rich liquid enters a regeneration tower for regeneration, and the regenerated SO is regenerated2And feeding the sulfur into an air line of a sulfur making furnace of a Claus sulfur device. At this time, the sulfur dioxide emission of the device is 15mg/m3，NOXDischarge 20mg/m3Sulfur dioxide emissions were reduced by 200mg/m compared to direct access to the Claus plant air line3，NOXEmission reduction 120mg/m3。
Example 2
As shown in figure 1, the process of the invention is adopted to treat the sewage stripping gas, hydrogen is adopted for co-combustion, the combustible components are completely combusted, the temperature of an incinerator is controlled to be 1280 ℃, the combustion process gas enters a denitration reactor, a molecular sieve catalyst is filled in the denitration reactor, the reaction temperature is controlled to be 230 ℃, tail gas after denitration enters rapid cooling, the tail gas after denitration enters an absorption unit after cooling at the temperature of 35 ℃, absorption liquid used by the absorption unit is a compound solution of diisopropanolamine and diethyldialkanolamine, wherein the diisopropanolamine accounts for 25 percent (wt), the diethyldialkanolamine accounts for 25 percent (wt), the absorption temperature is 38 ℃, the absorbed rich liquid enters a regeneration tower for regeneration, and regenerated SO is obtained2Is sent to the inlet of a first-stage converter of a Claus sulfur device sulfur production furnace. At this time, the sulfur dioxide emission of the device is 20mg/m3，NOXDischarge 30mg/m3Sulfur dioxide emissions are reduced by 160mg/m compared to direct access to the Claus plant acid gas line3，NOXEmission reduction 130mg/m3。
Example 3
As shown in figure 1, the coal gasification flash steam is treated by adopting the process of the invention, hydrogen is adopted for co-combustion, all combustible components are combusted, the temperature of an incinerator is controlled to 1350 ℃, the gas in the combustion process enters a denitration reactor, a metal oxide catalyst is filled in the denitration reactor, the reaction temperature is controlled to 280 ℃, tail gas after denitration enters rapid cooling, the tail gas after denitration enters an absorption unit after cooling, the temperature of the absorption unit is 38 ℃, absorption liquid used by the absorption unit is a compound solution of diisopropanolamine, diethyldialkanolamine and methylethanolamine, wherein the diisopropanolamine accounts for 25 percent (wt), the diethyldialkanolamine accounts for 10 percent (wt), the methylethanolamine accounts for 5 percent (wt), the absorption temperature is 39 ℃, the absorbed rich liquid enters a regeneration tower for regeneration, and the regenerated SO2Feeding into the inlet of a secondary converter of a Claus sulfur device sulfur production furnace. At this time, the sulfur dioxide emission of the device is 10mg/m3，NOXDischarge 27mg/m3Sulfur dioxide emissions are reduced as compared to treating the acid gas using selective oxidation techniquesLess than 300mg/m3，NOXEmission reduction 160mg/m3。
Example 4
As shown in figure 1, the process of the invention is adopted to treat S-Zorb tail gas, hydrogen is adopted for co-combustion, the combustible components are completely combusted, the temperature of the incinerator is controlled at 1100 ℃, the combustion process gas enters a denitration reactor, a non-supported metal oxide catalyst is filled in the denitration reactor, the reaction temperature is controlled at 100 ℃, the tail gas after denitration is quenched, the tail gas after denitration is cooled to 30 ℃ and enters an absorption unit, absorption liquid used by the absorption unit is a compound solution of diisopropanolamine and methylethanolamine, wherein the diisopropanolamine accounts for 25 percent (wt), the methylethanolamine accounts for 15 percent (wt), the absorption temperature is 35 ℃, the absorbed rich liquid enters a regeneration tower for regeneration, and the regenerated SO2Feeding into the inlet of a first-stage condenser of a Claus sulfur device sulfur production furnace. At this time, the sulfur dioxide emission of the device is 15mg/m3，NOXDischarge 28mg/m3The sulfur dioxide emission is reduced by 30mg/m compared with the direct entry into the Claus unit hydrogenation reactor3，NOXEmission reduction 20mg/m3。
Example 5
As shown in figure 1, the coal gasification flash steam and sulfur-tolerant shift waste gas are treated by the process of the invention, natural gas is adopted for co-combustion, the combustible components are completely combusted, the temperature of an incinerator is controlled at 1320 ℃, the combustion process gas enters a denitration reactor, a metal oxide catalyst is filled in the denitration reactor, the reaction temperature is controlled at 230 ℃, tail gas after denitration is quenched and cooled to 40 ℃, the cooled tail gas enters an absorption unit, absorption liquid used by the absorption unit is a compound solution of diisopropanolamine and diethyldialkanolamine, wherein the diisopropanolamine is 18 percent (wt), the diethyldialkanolamine is 24 percent (wt), the absorption temperature is 33 ℃, the absorbed rich liquid enters a regeneration tower for regeneration, and the regenerated SO2Feeding into the inlet of a first-stage condenser of a Claus sulfur device sulfur production furnace. At this time, the sulfur dioxide emission of the device is 23mg/m3，NOXDischarge 40mg/m3Sulfur dioxide emissions are reduced by 250mg/m compared to treating the acid gas using selective oxidation techniques3，NOXEmission reduction 310mg/m3。
Example 6
As shown in figure 1, the process of the invention is adopted to treat the sewage stripping gas, the low-temperature methanol washing acid gas and the sulfur-tolerant shift waste gas, natural gas is adopted for co-combustion, the combustible components are completely combusted, the temperature of an incinerator is controlled to be 1340 ℃, the combustion process gas enters a denitration reactor, a molecular sieve catalyst is filled in the denitration reactor, the reaction temperature is controlled to be 200 ℃, tail gas after denitration enters a quenching mode, the tail gas after denitration enters an absorption unit after cooling, the temperature is 30 ℃, absorption liquid used by the absorption unit is a compound solution of diisopropanolamine and 2-amino-2-methyl-1-propanol, wherein the diisopropanolamine accounts for 30 percent (wt), the 2-amino-2-methyl-1-propanol accounts for 10 percent (wt), the absorption temperature is 33 ℃, the absorbed rich liquid enters a regeneration tower for regeneration, and the regenerated SO is regenerated2Feeding into the inlet of a secondary converter of a Claus sulfur device sulfur production furnace. At this time, the sulfur dioxide emission of the device is 20mg/m3，NOXDischarge 30mg/m3Sulfur dioxide emissions are reduced by 240mg/m compared to direct access to the Claus unit acid gas line3，NOXEmission reduction 320mg/m3。
Example 7
As shown in figure 1, the process of the invention is adopted to treat low-temperature methanol-washed acid gas, natural gas is adopted for co-combustion, the combustible components are completely combusted, the temperature of an incinerator is controlled at 950 ℃, the combustion process gas enters a denitration reactor, the denitration reactor is filled with an unsupported metal oxide catalyst, the reaction temperature is controlled at 150 ℃, tail gas after denitration is quenched and cooled to 35 ℃, and then enters an absorption unit, absorption liquid used by the absorption unit is a compound solution of diisopropanolamine, 2-amino-2-methyl-1-propanol and methylethanolamine, wherein the diisopropanolamine accounts for 25 percent (wt), the 2-amino-2-methyl-1-propanol accounts for 15 percent (wt), the methylethanolamine accounts for 10 percent (wt), the absorption temperature is 37 ℃, the absorbed rich solution enters a regeneration tower for regeneration, and the regenerated SO is obtained.2And feeding the sulfur into an air line of a sulfur making furnace of a Claus sulfur device. At this time, the sulfur dioxide emission of the device is 18mg/m3，NOXDischarge 25mg/m3Sulfur dioxide emissions are reduced by 215mg/m compared to direct access to the Claus plant wind line3，NOXEmission reduction 110mg/m3。
Claims (10)
1. A method for treating low-concentration sulfur-containing acid gas is characterized by comprising the following steps: the low-concentration sulfur-containing acidic gas is treated by the incineration unit, the denitration unit and the absorption and regeneration unit in sequence, and the absorbent adopted by the absorption and regeneration unit comprises the following raw materials in percentage by weight: 10-30% of diisopropanolamine, 10-25% of compound component and the balance of water;
the complex component is one or more of 2-amino-2-methyl-1-propanol, diethylethanolamine or methylethanolamine.
2. The method of treating a low-concentration sour gas of claim 1, wherein: the absorbent comprises the following raw materials in percentage by weight: 25% of diisopropanolamine, 10% of diethylethanolamine, 5% of methylethanolamine and 60% of water.
3. The method of treating a low-concentration sour gas of claim 1, wherein: the furnace temperature of the incineration unit is controlled to be 950 ℃ and 1350 ℃.
4. The method of treating a low-concentration sour gas of claim 1, wherein: the catalyst adopted by the denitration unit is an SCR catalyst.
5. The method of treating a low-concentration sour gas of claim 1, wherein: in the low concentration of sour gas containing sulfur, H2S is 0-40% by volume, NH3The volume percentage of the five gases is 0-5%, the volume percentage of HCN is 0-50%, the volume percentage of thioether is 0-4%, the volume percentage of mercaptan is 0-8%, and the volume percentages of the five gases are not 0% at the same time.
6. The method of treating a low-concentration sour gas of claim 1, wherein: the process flow in the absorption regeneration unit is as follows: introducing the denitrated gas into the deviceAbsorption column with said absorbent, SO2Absorbed by the absorbent; absorption of SO2The purified tail gas is discharged; containing SO2The rich solution enters a regeneration tower for regeneration, and regenerated SO2And the obtained product enters a Claus sulfur recovery device for reutilization.
7. The method of treating a low-concentration sour gas of claim 6, wherein: the temperature of the absorption tower is controlled to be 25-45 ℃.
8. The method of treating a low-concentration sour gas of claim 6, wherein: the temperature of the regeneration tower is controlled to be 110-125 ℃.
9. The method of treating a low-concentration sour gas of claim 6, wherein: absorption of SO2SO in the tail gas2The content is less than 30mg/m3。
10. The method of treating a low-concentration sour gas of claim 1, wherein: after treatment of low concentration sour gas containing sulfur, NOXReduced to 50mg/m3The following.
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Application publication date: 20200313 |
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