CN103159580A - Method of purifying and extracting methane in waste landfill gas - Google Patents
Method of purifying and extracting methane in waste landfill gas Download PDFInfo
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- CN103159580A CN103159580A CN2011104256757A CN201110425675A CN103159580A CN 103159580 A CN103159580 A CN 103159580A CN 2011104256757 A CN2011104256757 A CN 2011104256757A CN 201110425675 A CN201110425675 A CN 201110425675A CN 103159580 A CN103159580 A CN 103159580A
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E50/00—Technologies for the production of fuel of non-fossil origin
- Y02E50/30—Fuel from waste, e.g. synthetic alcohol or diesel
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P20/00—Technologies relating to chemical industry
- Y02P20/50—Improvements relating to the production of bulk chemicals
- Y02P20/584—Recycling of catalysts
Abstract
The invention belongs to the waste landfill gas purification field and relates to a method utilizing sulfur resistance catalytic deoxidization as core to purify methane, in particular to a method of purifying and extracting methane in waste landfill gas. The method comprises the following steps: a waste landfill gas compression process, a TSA process, a sulfur resistance catalytic deoxidization process, an acid gas removing process, and a concentration extracting process. In the acid gas removing process, pressure swing adsorption (PSA), alkali wash, methyldiethanolamine (MDEA) or low-temperature carbinol washing can be selected to remove carbon dioxide, sulfur dioxide and most hydrogen sulfide in gas. The concentration extracting process refers to concentrating the methane and separating nitrogen. The method achieves sulfur resistance catalytic deoxidization of the waste landfill gas, can process the waste landfill gas containing various impurities, and has the advantages of being high in methane recovery rate, stable in device operation, and high in reliability and heat utilization rate, and achieves the effects of recycling industrial effluent gas, conserving energy, reducing emission and turning waste into wealth.
Description
Technical field
The invention belongs to the purification concentrate field of refuse embedded gas, relate to a kind of method of the purification methane take sulfur-resistant catalytic deoxidization as core, be specially a kind of method that purifies methane in the concentrate refuse embedded gas.With the summary suggestion for revision.
Background technology
Along with the quickening of socioeconomic development and urbanization process, the generation of China's municipal solid waste increases sharply.China's domestic refuse amount of clearing reached 1.56 hundred million t in 2005, increased nearly 5 times with ratio in 1980.When refuse production increased considerably, huge variation had also occured with comparing in the past in its component and character, and wherein in domestic refuse, biodegradable organic content has risen to 60% left and right.The suitable processing mode of organic domestic waste has landfill and two kinds of methods of anaerobic digestion, can produce a large amount of landfill gas in the process of processing.2010, China's domestic refuse Methane production reached 11,000,000,000 Nm
3, close to 12% of China's natural gas ultimate production then.Landfill gas contains 50% to 60% methane, and all the other are carbonic acid gas, nitrogen, oxygen and other minimum gas.Methane is a kind of strong greenhouse gases, is also a kind of inflammable gas, as lets alone unordered discharging, and not only contaminate environment, cause serious Greenhouse effect, also is easy to catch fire and explosion hazard, is great potential safety hazard.Simultaneously, the calorific value Yue Keda 4500～5000kcal/Nm of landfill gas
3, be half of Sweet natural gas, be a kind of very important resource.So must change the state of the unordered discharging of landfill gas, realize harmless treatment and recycling.
The landfill gas complicated that refuse landfill produces purifies difficulty.The recycling of refuse embedded gas is carried out in more than 500 refuse landfill that has in the world at present more than 20 country, but is mainly that the refuse embedded gas dehydration is produced steam for oil engine generating or fuel.The calorific value of undressed refuse embedded gas and transformation efficiency are lower and range of application is limited, in order further to improve the use value of refuse embedded gas, turn waste into wealth, utilize the thickening-purification technology technology refuse embedded gas to be modified into the biomethane of high heating value both at home and abroad, and it is used the association area of natural gas applications.Utilize the thickening-purification technology technology to make refuse embedded gas become the methane of high heating value, and be used for town gas and the facilities for transport and communication take Sweet natural gas as fuel, now become the new direction of external refuse embedded gas industry Application and Development.
At present, China's refuse embedded gas utilization also concentrates on heat supply and generating, production facility small scale and unconcentrated, but the transformation along with idea, the maturation of technology, and the drive of gas utilization, the clean fuel of producing from the refuse embedded gas purification will have wide market outlook.In recent years, domestic Sweet natural gas consumption constantly increases, and natural air-air source is not enough, and the production capacity of Sweet natural gas increases relatively slow, will alleviate to a certain extent ' gas is waste ' phenomenon than the better landfill gas refined product of common natural gas quality.
Landfill gas contains 50% to 60% methane, and all the other are carbonic acid gas, nitrogen, oxygen and other minimum gas.Due at normal temperatures and pressures, the explosion ratio scope of methane and air Mixture is 5%～15%.This scope can change with the variation of pressure and temperature.(contain O from refuse embedded gas
2) in not deoxidation directly adopt PSA to separate or cryogenic upgrading methane, certainly exist two processes, being that methane concentration in refuse embedded gas is from the 40%(volume content) concentrate to 95% is as the gas product output, the methane in foreign gas (nitrogen, the oxygen) sepn process in refuse embedded gas is from the 40%(volume content simultaneously) be down to 1% as exhaust gas emission.In the change procedure of this methane concentration, methane concentration unavoidably can pass through limits of explosion (under oxygenous condition).Therefore, refuse embedded gas is carried out the core that effective deoxidation becomes follow-up safety applications.
Summary of the invention
The present invention is according to above technical problem, provide and to solve a deoxidation difficult problem that contains the oxygen refuse embedded gas, avoid in follow-up purification concentrate process, the operational condition that methane passes through limits of explosion occurs, the refuse embedded gas that will contain various impurity is made the methane gas of high density, makes its service requirements of satisfying civilian, vehicle fuel and national standard and further a kind of method that purifies methane in the concentrate refuse embedded gas of the requirement of chemical industry energy source use.
Technical scheme of the present invention is:
A kind of method that purifies methane in the concentrate refuse embedded gas comprises the following steps:
(1), refuse embedded gas compression section: landfill gas is forced into 0.1 MPa through blower fan under normal pressure, more compressed machine is forced into 0.2～2.5MPa, then enters the TSA operation;
(2), TSA operation: selecting aluminum oxide and silica gel or aluminum oxide and gac is sorbent material, gas passes from two adsorption towers of parallel connection, switch the tower of different periods by valve, when unstripped gas passes through one of them tower, sulphur in unstripped gas, phosphorus, arsenic, cyanogen impurity are removed by the sorbent material in this tower, selecting aluminum oxide and silica gel or aluminum oxide and gac is sorbent material, another tower is in regenerative process, be about to the impurity desorb that sorbent material adsorbs, so repeatedly realize the purification requirement of the operation of TSA;
(3), sulfur-resistant catalytic deoxidization operation: heat through preheater from TSA operation gas out, Heating temperature enters when being 200～400 ℃
Deoxidation reactor, at sulfur-tolerance deoxidation catalyst bed generation deoxygenation, the oxygen in gas is removed to 0.2%(V%) below, simultaneously sulfur impurity, phosphorus, arsenic and cyanogen are converted into the oxidation state material, gas space velocity 2000～15000 h
-1, after deoxidation, gas is again through being cooled to normal temperature, and the sulfur-tolerant type dehydrogenation catalyst of employing contains various sulfide and total sulfur content reaches 1000mg/m at unstripped gas
3Situation under, this catalyzer can normally use and remove the oxygen in unstripped gas;
(4) depickling gas operation: the gas that is cooled to normal temperature enters adsorption tower depickling gas, and depickling gas is selected any one method in pressure swing adsorption process, alkali wash, MDEA method or low-temp methanol washing method;
(5) concentrate operation: the concentrate operation can be selected pressure-variable adsorption (PSA) method or low temperature processing.
Depickling gas operation can be selected pressure swing adsorption process (PSA), alkali wash, MDEA method or low-temp methanol washing method, removes the CO in gas
2, SO
2And H
2S； Described concentrate operation is with methane concentration, separation of nitrogen component.
Alkali wash in step (4) is selected Ca (OH)
2, NaOH or KOH be as the alkali cleaning agent; Sulfur-resistant catalytic deoxidization operation in step (3) is comprised of at least 1 deoxidation reactor and heating unit; TSA operation in step (2) adopts at least 2 adsorption towers, and the temperature operation scope of TSA is 15～300 ℃, and adopting aluminum oxide and silica gel or aluminum oxide and gac in the TSA operation is sorbent material.
In the present invention, the compressed machine supercharging of refuse embedded gas enters the above TSA operation that forms of two towers or two towers, and the temperature operation scope of TSA operation is 15～300 ℃, can remove most impurity composition.
Refuse embedded gas compression section in step (1) preferably enters the TSA operation 40 ℃ of lower compression with landfill gas to 0.7MPa.
Unstripped gas through the TSA operation enters the sulfur-resistant catalytic deoxidization operation, owing to containing 0.5～5% O that does not wait that has an appointment in refuse embedded gas
2, and O
2Existence have a strong impact on the processing safety of follow-up extracting and concentrating technology.Sulfur-resistant catalytic deoxidization is selected the catalyzer of the anti-sulphur of energy, 200～400 ℃ of service temperatures, gas space velocity 2000～15000h
-1In the sulfur-resistant catalytic deoxidization process, the most of sulphur in landfill gas, phosphorus, arsenic, cyanogen are oxidized to oxide compound; The sulfur-tolerance deoxidation device is comprised of at least 1 deoxidation reactor and heating unit, in the sulfur-tolerance deoxidation operation, with under gas heating to 200～400 ℃, deoxygenation occurs, and the oxygen level in gas is removed to 0.2%(V%) below.The deoxidation principle is under catalyst action, the methane in stove and O
2Catalyst combustion reaction occurs reach the deoxygenation purpose.Hot gas after the deoxidation cold air front with entering deoxidation carried out heat exchange, the recovery part heat, and after deoxidation, gas is again through being cooled to normal temperature.
Gas after deoxidation carries out depickling gas, and depickling gas operation can be selected pressure-variable adsorption (PSA) method, alkali wash, MDEA method or low-temp methanol washing method.
Pressure-variable adsorption (PSA) method is comprised of many adsorbers and a series of time variable control valve.In the PSA carbon rejection process, Adsorption Phase is for containing CO
2Waste gas discharge by inverse put and the desorb of finding time at the bottom of the tower, methane is from absorption tower top output, a part is gone back to system as displacement gas and is replaced, a part as gas product deliver to next operating unit for, carbonic acid gas is lower than 3%(v/v% herein).
Alkali wash is selected Ca (OH)
2, NaOH or KOH be as the alkali cleaning agent, alkali cleaning is carried out at normal temperatures; After depickling, the gas inorganic sulfur is lower than 0.1mg/Nm
3, carbonic acid gas is lower than 25 * 10
-6(v/v).
The MDEA chemical name N methyldiethanol amine, is a kind of organic amine liquid, and the MDEA method refers to that gas enters from the bottom, absorption tower, and MDEA solution (lean solution) enters from top, absorption tower, both counter current contact, the CO in gas
2And most of H
2S is absorbed and enters liquid phase, and the MDEA solution that absorbs after saturated is reusable through regenerating; After depickling, gas vulcanization hydrogen is lower than 4mg/Nm3, and carbonic acid gas is lower than 50 * 10
-6(v/v).
Low-temp methanol washing method is to utilize the good characteristic of (50～-70 ℃) methyl alcohol under low temperature to remove CO in gas
2, H
2S, organosulfur and prussiate.After low-temperature rectisol, CO
2Can be removed to 10～20 * 10
-6(v/v), the inorganic sulfur organosulfur is less than 0.1mg/Nm
3
The concentrate operation is selected PSA method or low temperature processing; PSA method concentrate methane: PSA is comprised of many adsorbers and a series of time variable control valve.In PSA concentrate methane process, will contain N
2Absorption waste gas and displacement waste gas discharge from the absorption tower top, Adsorption Phase methane is by inverse put and find time that desorb obtains qualified methane gas at the bottom of the tower, a part is gone back to system as displacement gas and is replaced, a part as gas product deliver to out-of-bounds for.
Low temperature processing: adopt the concentrate mode of low temperature fractionation, treated landfill gas enters the ice chest system, enters low-temperature fractionating tower separation of methane and nitrogen through overcooling, and tower top obtains useless nitrogen, obtains pure methane at the bottom of tower.According to product demand, the methane at the bottom of tower can re-heat obtains the gaseous methane product or through the excessively cold liquid product (LNG) that obtains.Ice chest refrigeration system selectively-expandable refrigeration or hybrid refrigeration form.
Compared with prior art, beneficial effect of the present invention is:
(1) the present invention proposes the refuse embedded gas purification concentrating method of energy industrial scale first, solved the difficult problem of refuse embedded gas sulfur-resistant catalytic deoxidization, can process the refuse embedded gas that contains various impurity, has the methane yield high, install stable, the advantage that reliability is high, heat utilization ratio is high, the effect that reach refuse embedded gas recycling, energy-saving and emission-reduction, turns waste into wealth;
(2), each operation at the refuse embedded gas scavenging process all adopts special design, reach treatment process continuously and gas decontamination index up to standard, by rational system design, the heat that each operates workshop section of the present invention can be realized Integrated using, need not extraneous supplemental heat source simultaneously;
(3), increase sulfur-resistant catalytic deoxidization process, solved and contain the oxygen refuse embedded gas pass through the potential safety hazard of limits of explosion in the extracting and concentrating technology process, can satisfy the condition that refuse embedded gas impurity is complicated, operating mode is changeable;
(4), in scavenging process without pollutant emission continuously, the curable collection of impurity.
Description of drawings
Fig. 1 is process flow sheet of the present invention.
Embodiment
The present invention is described in further detail below in conjunction with embodiment.
The present invention is not limited to following embodiment.The present invention expands to any new feature or any new combination that discloses in this manual, and the arbitrary new method that discloses or step or any new combination of process all belong to the scope that the present invention protects.
Embodiment 1:
Landfill gas forms
Foreign matter content such as following table:
H
2S:200ppm
Landfill gas input pressure: normal pressure
Landfill gas temperature :≤40 ℃
Landfill gas flow: 3000 Nm
3/ h
Landfill gas is forced into 0.1MPa through blower fan under normal pressure, at the temperature of 40 ℃, then compressed machine is pressurized to 0.7MPa, enters the TSA operation, mainly removes the impurity such as alkane in unstripped gas, aromatic hydrocarbons, sulfide, obtains the less purified gas of impurity.Purified gas after the TSA operation enters the sulfur-resistant catalytic deoxidization operation.
Unstripped gas through the TSA operation enters the sulfur-resistant catalytic deoxidization operation, approximately under 400 ℃ with gas in oxygen level be removed to 0.2%(V/V%) below, then enter the first deoxidation aftercooler, hot gas and enter the front cold air of deoxidation electric heater (preheater) and carry out heat exchange, the recovery part heat, then through the second water cooler, gas cooling is entered depickling gas operation after normal temperature.Gas after unified process deoxidation step enters depickling gas operation, and depickling gas operation adopts the PSA method, will be sent to extracting and concentrating technology after the acid gas removals such as the carbonic acid gas in gas, hydrogen sulfide.Hydrogen sulfide is lower than 4mg/Nm
3, carbonic acid gas is lower than 50 * 10
-6(v/v).
Extracting and concentrating technology adopts the PSA method, the methane concentrate is obtained the gas product of (volume content) more than 95%.
Embodiment 2
Refuse embedded gas forms
Foreign matter content such as following table:
H
2S:200ppm
Landfill gas input pressure: normal pressure
Landfill gas temperature :≤40 ℃
Landfill gas flow: 10000 Nm
3/ h
Landfill gas is forced into 0.1MPa through blower fan under normal pressure, under 40 ℃, then compressed machine is pressurized to 1.5MPa, enters the TSA operation.Mainly remove the impurity such as alkane in unstripped gas, aromatic hydrocarbons, sulfide, obtain the less purified gas of impurity.Purified gas after TSA enters the sulfur-resistant catalytic deoxidization operation.
Unstripped gas through the TSA operation enters the sulfur-resistant catalytic deoxidization operation, approximately under 400 ℃ with gas in oxygen level be removed to 0.2%(V/V%) below, then enter the first deoxidation aftercooler, the hot gas cold air front with entering the deoxidation electric heater carried out heat exchange, the recovery part heat, then through the second water cooler, gas cooling is entered depickling gas operation after normal temperature.
Enter depickling gas operation through the gas after deoxidation step, depickling gas operation adopts alkali wash, will be sent to the concentrate operation after the acid gas removals such as the carbonic acid gas in gas, hydrogen sulfide, and the concentrate operation adopts low temperature processing, and hydrogen sulfide is lower than 4mg/Nm
3, carbonic acid gas is lower than 50 * 10
-6(v/v).
Extracting and concentrating technology adopts low temperature separation process, the methane concentrate is obtained the gas product of (volume content) more than 99%.
Claims (4)
1. method that purifies methane in the concentrate refuse embedded gas is characterized in that comprising the following steps:
(1), refuse embedded gas compression section: landfill gas is forced into 0.1 MPa through blower fan under normal pressure, more compressed machine is forced into 0.2～2.5MPa, then enters the TSA operation;
(2), TSA operation: selecting aluminum oxide and silica gel or aluminum oxide and gac is sorbent material; Gas passes from two adsorption towers of parallel connection, switch the tower of different periods by valve, when unstripped gas passes through one of them tower, sulphur in unstripped gas, phosphorus, arsenic, cyanogen impurity are removed by the sorbent material in this tower, another tower is in regenerative process, be about to the impurity desorb that sorbent material adsorbs, so repeatedly realize the purification requirement of TSA operation;
(3), sulfur-resistant catalytic deoxidization operation: enter deoxidation reactor from TSA operation gas out when preheater is heated to 200～400 ℃, at sulfur-tolerance deoxidation catalyst bed generation deoxygenation, oxygen in gas is removed to 0.2%(V%) below, simultaneously sulfur impurity, phosphorus, arsenic and cyanogen are converted into the oxidation state material, gas space velocity 2000～15000 h
-1, after deoxidation, gas is again through being cooled to normal temperature, and the sulfur-tolerant type dehydrogenation catalyst of employing contains various sulfide and total sulfur content reaches 1000mg/m at unstripped gas
3Situation under, this catalyzer can normally use and remove the oxygen in unstripped gas;
(4) depickling gas operation: the gas that is cooled to normal temperature enters adsorption tower depickling gas, and depickling gas is selected any one method in pressure swing adsorption process, alkali wash, MDEA method or low-temp methanol washing method;
(5) concentrate operation: the concentrate operation can be selected pressure-variable adsorption (PSA) method or low temperature processing.
2. the method for methane in purification concentrate refuse embedded gas according to claim 1 is characterized in that: described depickling gas operation can be selected pressure-variable adsorption (PSA) method, alkali wash, MDEA method or low-temp methanol washing method, removes the CO in gas
2, SO
2And H
2S； Described concentrate operation is with methane concentration, separation of nitrogen component.
3. the method for methane in purification concentrate refuse embedded gas according to claim 1, it is characterized in that: the sulfur-resistant catalytic deoxidization operation in described step (3) is comprised of at least 1 deoxidation reactor and heating unit.
4. the method for methane in purification concentrate refuse embedded gas according to claim 1, it is characterized in that: the TSA operation in described step (2) adopts at least 2 adsorption towers, the temperature operation scope of TSA is 15～300 ℃, and selecting aluminum oxide and silica gel or aluminum oxide and gac is sorbent material.
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| CN103353207A (en) * | 2013-07-18 | 2013-10-16 | 杭州凯德空分设备有限公司 | Device for purifying methane liquid from purified landfill gas |
| US20190126201A1 (en) * | 2016-05-24 | 2019-05-02 | Haldor Topsøe A/S | Method for the removal of oxygen from an industrial gas |
| US20190126199A1 (en) * | 2016-05-24 | 2019-05-02 | Haldor Topsøe A/S | A process for the purifying of a raw gas stream containing mainly c1-c5 hydrocarbons and carbon dioxide, and impurities of organic and inorganic sulfur compounds, halogenated and non-halogenated volatile organic compounds and oxygen |
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Cited By (8)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN103306717A (en) * | 2013-07-03 | 2013-09-18 | 中煤科工集团重庆研究院 | Method for utilizing superfluous heat of ventilation air gas concentrated and subjected to counterflow oxidation |
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| CN103353207B (en) * | 2013-07-18 | 2015-02-25 | 杭州凯德空分设备有限公司 | Device for purifying methane liquid from purified landfill gas |
| US20190126201A1 (en) * | 2016-05-24 | 2019-05-02 | Haldor Topsøe A/S | Method for the removal of oxygen from an industrial gas |
| US20190126199A1 (en) * | 2016-05-24 | 2019-05-02 | Haldor Topsøe A/S | A process for the purifying of a raw gas stream containing mainly c1-c5 hydrocarbons and carbon dioxide, and impurities of organic and inorganic sulfur compounds, halogenated and non-halogenated volatile organic compounds and oxygen |
| US10661224B2 (en) * | 2016-05-24 | 2020-05-26 | Haldor Topsoe A/S | Process for the purifying of a raw gas stream containing mainly C1-C5 hydrocarbons and carbon dioxide, and impurities of organic and inorganic sulfur compounds, halogenated and non-halogenated volatile organic compounds and oxygen |
| US10675585B2 (en) * | 2016-05-24 | 2020-06-09 | Haldor Topsoe A/S | Method for the removal of oxygen from an industrial gas |
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Address after: No. 5 high tech Zone Gaopeng road in Chengdu city of Sichuan Province in 610225 Applicant after: Southwest Chemical Research & Design Institute Co., Ltd. Address before: No. 5 high tech Zone Gaopeng road in Chengdu city of Sichuan Province in 610225 Applicant before: Xinan Chemical Research & Design Inst. |
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