CN103159580B - 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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- CN103159580B CN103159580B CN201110425675.7A CN201110425675A CN103159580B CN 103159580 B CN103159580 B CN 103159580B CN 201110425675 A CN201110425675 A CN 201110425675A CN 103159580 B CN103159580 B CN 103159580B
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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
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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, relating to a kind of take sulfur-resistant catalytic deoxidization as the method for the purification methane of core, is specially a kind of method purifying methane in concentrate refuse embedded gas.With making a 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.Within 2005, China's domestic refuse amount of clearing reaches 1.56 hundred million t, with 1980 than increasing nearly 5 times.While refuse production increases considerably, its component and character also there occurs huge change compared with in the past, and wherein in domestic refuse, biodegradable organic content has risen to about 60%.The processing mode that organic domestic waste is suitable for has landfill and anaerobic digestion two kinds of methods, can produce a large amount of landfill gas in the process of process.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 the methane of 50% to 60%, and all the other are carbonic acid gas, nitrogen, oxygen and other minimum gas.Methane is a kind of strong greenhouse gases, and be also a kind of inflammable gas, as let alone unordered discharge, not only contaminate environment, causes serious Greenhouse effect, is also easy to catch fire and explosion hazard, is great potential safety hazard.Meanwhile, the calorific value Yue Keda 4500 ~ 5000kcal/Nm of landfill gas
3, being the half of Sweet natural gas, is a kind of very important resource.So the state of the unordered discharge of landfill gas must be changed, realize harmless treatment and recycling.
The landfill gas complicated that refuse landfill produces, purification difficulty.The recycling of refuse embedded gas is carried out in current more than 500 refuse landfill having more than 20 country in the world, but mainly refuse embedded gas dehydration is used for oil engine generating or fuel generation steam.The calorific value of undressed refuse embedded gas and transformation efficiency is lower and range of application is limited, in order to improve the use value of refuse embedded gas further, turn waste into wealth, utilize thickening-purification technology technology that refuse embedded gas is modified into the biomethane of high heating value both at home and abroad, and used the association area of natural gas applications.Utilize thickening-purification technology technology to make refuse embedded gas become the methane of high heating value, and for town gas and with Sweet natural gas be fuel facilities for transport and communication in, now become the new direction of external refuse embedded gas industry Application and Development.
At present, China refuse embedded gas utilizes and also concentrates on for heat and generating power, production facility small scale and not concentrating, but along with the transformation of idea, the maturation of technology, and the drive of gas utilization, will have wide market outlook from the refuse embedded gas clean fuel produced of purifying.In recent years, domestic 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 ' gas is waste ' phenomenon to a certain extent than the better landfill gas refined product of common natural gas quality.
Landfill gas contains the methane of 50% to 60%, 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 change of pressure and temperature.From refuse embedded gas (containing O
2) in not deoxidation directly adopt PSA be separated or cryogenic upgrading methane, certainly exist two processes, namely the methane concentration in refuse embedded gas is from 40%(volume content) concentrate to 95% is as gas product output, the methane in foreign gas (nitrogen, the oxygen) sepn process simultaneously in refuse embedded gas is from 40%(volume content) be down to 1% as exhaust gas emission.In the change procedure of this methane concentration, methane concentration has inevitably passed through limits of explosion (under oxygenous condition).Therefore, the core that effective deoxidation becomes Subsequent secure application is carried out to refuse embedded gas.
Summary of the invention
The present invention is according to above technical problem, the deoxidation difficult problem that can solve containing oxygen refuse embedded gas is provided, avoid in subsequent purification concentrate process, the operational condition that methane passes through limits of explosion occurs, refuse embedded gas containing various impurity is made the methane gas of high density, make a kind of method purifying methane in concentrate refuse embedded gas of its service requirements meeting civilian, vehicle fuel and national standard and the further requirement of chemical industry energy source use.
Technical scheme of the present invention is:
Purify a method for methane in concentrate refuse embedded gas, comprise the following steps:
(1), refuse embedded gas compression section: landfill gas is forced into 0.1 MPa through blower fan at ambient pressure, then is forced into 0.2 ~ 2.5MPa through compressor, then enter TSA operation;
(2), TSA operation: select aluminum oxide and silica gel or aluminum oxide and gac to be sorbent material, gas passes from two adsorption towers of parallel connection, the tower of Different periods is switched by valve, when unstripped gas is by one of them tower, sulphur in unstripped gas, phosphorus, arsenic, cyanogen impurity are removed by the sorbent material in this tower, aluminum oxide and silica gel or aluminum oxide and gac is selected to be sorbent material, another tower is then in regenerative process, by 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, enter when Heating temperature is 200 ~ 400 DEG C
Deoxidation reactor, at sulfur-tolerance deoxidation catalyst bed generation deoxygenation, the oxygen in gas is removed to 0.2%(V%) below, sulfur impurity, phosphorus, arsenic and cyanogen are converted into oxidation state species, gas space velocity 2000 ~ 15000 h simultaneously
-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
3when, this catalyzer normally can use and remove the oxygen in unstripped gas;
(4) depickling gas operation: be cooled to the gas of normal temperature to enter adsorption tower depickling gas, depickling gas selects any one method in pressure swing adsorption process, alkali wash, MDEA method or low-temp methanol washing method;
(5) concentrate operation: concentrate operation can select pressure-variable adsorption (PSA) method or low temperature processing.
Depickling gas operation can select pressure swing adsorption process (PSA), alkali wash, MDEA method or low-temp methanol to wash method, removes the CO in gas
2, SO
2and H
2s; Described concentrate operation is by methane concentration, separation of nitrogen component.
Alkali wash in step (4) selects Ca (OH)
2, NaOH or KOH be as alkali cleaning agent; Sulfur-resistant catalytic deoxidization operation in step (3) is made up of at least 1 deoxidation reactor and heating unit; TSA operation in step (2) adopts at least 2 adsorption towers, and the temperature operating ranges of TSA is 15 ~ 300 DEG C, adopts aluminum oxide and silica gel or aluminum oxide and gac to be sorbent material in TSA operation.
In the present invention, refuse embedded gas, through compressor supercharging, enters the TSA operation that more than two towers or two towers form, and the temperature operating ranges of TSA operation is 15 ~ 300 DEG C, can remove most impurity composition.
Refuse embedded gas compression section in step (1), enters TSA operation after preferably landfill gas being compressed to 0.7MPa at 40 DEG C.
Unstripped gas through TSA operation enters sulfur-resistant catalytic deoxidization operation, due in refuse embedded gas containing have an appointment 0.5 ~ 5% not wait O
2, and O
2existence have a strong impact on the processing safety of follow-up extracting and concentrating technology.Sulfur-resistant catalytic deoxidization selects the catalyzer of energy sulfur resistive, service temperature 200 ~ 400 DEG C, gas space velocity 2000 ~ 15000h
-1.In sulfur-resistant catalytic deoxidization process, the most of sulphur in landfill gas, phosphorus, arsenic, cyanogen are oxidized to oxide compound; Sulfur-tolerance deoxidation device is made up of at least 1 deoxidation reactor and heating unit, in sulfur-tolerance deoxidation operation, gas heating, at 200 ~ 400 DEG C, deoxygenation is occurred, the oxygen level in gas is removed to 0.2%(V%) below.Deoxidation principle is under catalyst action, the methane in stove and O
2there is catalyst combustion reaction and reach deoxygenation object.Hot gas after deoxidation and the cold air before entering deoxidation carry out heat exchange, 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 select pressure-variable adsorption (PSA) method, alkali wash, MDEA method or low-temp methanol to wash method.
Pressure-variable adsorption (PSA) method is made up of multiple stage adsorber and a series of time variable control valve.In PSA carbon rejection process, Adsorption Phase is for containing CO
2waste gas by inverse put with find time to discharge from desorb at the bottom of tower, methane is from absorption tower top output, and a part is replaced as the displacement gas system of returning, a part as gas product deliver to next operating unit for, carbonic acid gas is lower than 3%(v/v% herein).
Alkali wash selects Ca (OH)
2, NaOH or KOH as alkali cleaning agent, alkali cleaning is carried out at normal temperatures; After depickling, gas inorganic sulfur is lower than 0.1mg/Nm
3, carbonic acid gas is lower than 25 × 10
-6(v/v).
MDEA chemical name is N methyldiethanol amine, and be a kind of organic amine liquid, MDEA method refers to that gas enters from 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 rapidly absorbed into liquid phase, absorb saturated after MDEA solution 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 the CO that the good characteristic of (-50 ~-70 DEG C) methyl alcohol under utilizing low temperature removes in gas
2, H
2s, organosulfur and prussiate.After low-temperature rectisol, CO
2can 10 ~ 20 × 10 be removed to
-6(v/v), inorganic sulfur organosulfur is less than 0.1mg/Nm
3.
Concentrate operation selects PSA method or low temperature processing; PSA method concentrate methane: PSA is made up of multiple stage adsorber and a series of time variable control valve.In PSA concentrate methane process, will containing N
2absorption waste gas and displacement waste gas discharge from absorption tower top, Adsorption Phase methane is by inverse put and find time to obtain qualified methane gas from desorb at the bottom of tower, and a part is replaced as the displacement gas system of returning, a part as gas product deliver to out-of-bounds for.
Low temperature processing: the concentrate mode adopting low temperature fractionation, treated landfill gas enters cold box 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 re-heat can obtain gaseous methane product or obtains liquid product (LNG) through excessively cold.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, solve a difficult problem for refuse embedded gas sulfur-resistant catalytic deoxidization, the refuse embedded gas containing various impurity can be processed, there is methane yield high, plant running is stablized, the advantage that reliability is high, heat utilization ratio is high, reaches refuse embedded gas recycling, energy-saving and emission-reduction, the effect that turns waste into wealth;
(2), special design is all adopted in each operation of refuse embedded gas scavenging process, reach treatment process continuously and gas decontamination index up to standard, simultaneously by rational system design, the heat of each operation workshop section of the present invention can realize comprehensive use, without the need to extraneous supplemental heat source;
(3), increase sulfur-resistant catalytic deoxidization process, solve the potential safety hazard of passing through limits of explosion containing oxygen refuse embedded gas in extracting and concentrating technology process, the condition that refuse embedded gas impurity is complicated, operating mode is changeable can be met;
(4), in scavenging process without continuous pollutant emission, impurity curable is collected.
Accompanying drawing explanation
Fig. 1 is process flow sheet of the present invention.
Embodiment
Below in conjunction with embodiment, the present invention is described in further detail.
The present invention is not limited to embodiment below.The present invention expands to any new feature of disclosing in this manual or any combination newly, and the step of the arbitrary new method disclosed or process or any combination newly all belong to the scope that the present invention protects.
Embodiment 1:
Landfill gas forms
Foreign matter content is as following table:
H
2S:200ppm
Landfill gas input pressure: normal pressure
Landfill gas temperature :≤40 DEG C
Landfill gas flow: 3000 Nm
3/ h
Landfill gas is forced into 0.1MPa through blower fan at ambient pressure, at the temperature of 40 DEG C, is then pressurized to 0.7MPa through compressor, enters TSA operation, mainly removes the impurity such as the alkane in unstripped gas, aromatic hydrocarbons, sulfide, obtains the purified gas that impurity is less.Purified gas after TSA operation enters sulfur-resistant catalytic deoxidization operation.
Unstripped gas through TSA operation enters sulfur-resistant catalytic deoxidization operation, at about 400 DEG C, oxygen level in gas is removed to 0.2%(V/V%) below, then the first deoxidation aftercooler is entered, hot gas and the cold air entering deoxidation electric heater (preheater) front carry out heat exchange, recovery part heat, then depickling gas operation will be entered after gas cooling to normal temperature through the second water cooler.Unified gas after deoxidation step enters depickling gas operation, and depickling gas operation adopts PSA method, is sent to extracting and concentrating technology by 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 PSA method, methane concentrate is obtained the gas product of more than 95% (volume content).
Embodiment 2
Refuse embedded gas forms
Foreign matter content is as following table:
H
2S:200ppm
Landfill gas input pressure: normal pressure
Landfill gas temperature :≤40 DEG C
Landfill gas flow: 10000 Nm
3/ h
Landfill gas is forced into 0.1MPa through blower fan at ambient pressure, at 40 DEG C, is then pressurized to 1.5MPa through compressor, enters TSA operation.Mainly remove the impurity such as the alkane in unstripped gas, aromatic hydrocarbons, sulfide, obtain the purified gas that impurity is less.Purified gas after TSA enters sulfur-resistant catalytic deoxidization operation.
Unstripped gas through TSA operation enters sulfur-resistant catalytic deoxidization operation, at about 400 DEG C, oxygen level in gas is removed to 0.2%(V/V%) below, then the first deoxidation aftercooler is entered, hot gas and the cold air before entering deoxidation electric heater carry out heat exchange, recovery part heat, then depickling gas operation will be entered after gas cooling to normal temperature through the second water cooler.
Gas after deoxidation step enters depickling gas operation, and depickling gas operation adopts alkali wash, is sent to concentrate operation by after the acid gas removals such as the carbonic acid gas in gas, hydrogen sulfide, and 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, methane concentrate is obtained the gas product of more than 99% (volume content).
Claims (3)
1. purify a method for methane in concentrate refuse embedded gas, it 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 at ambient pressure, then is forced into 0.2 ~ 2.5MPa through compressor, then enter TSA operation;
(2), TSA operation: TSA operation adopts at least 2 adsorption towers, and the temperature operating ranges of TSA is 15 ~ 300 DEG C, selects aluminum oxide and silica gel or aluminum oxide and gac to be sorbent material; Gas passes from two adsorption towers of parallel connection, the tower of Different periods is switched by valve, when unstripped gas is by one of them tower, sulphur in unstripped gas, phosphorus, arsenic, cyanogen impurity are removed by the sorbent material in this tower, another tower is then in regenerative process, by 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 DEG C, at sulfur-tolerance deoxidation catalyst bed generation deoxygenation, oxygen in gas is removed to 0.2%(V%) below, sulfur impurity, phosphorus, arsenic and cyanogen are converted into oxidation state species, gas space velocity 2000 ~ 15000 h simultaneously
-1, after deoxidation, gas is again through being cooled to normal temperature, the sulfur-tolerant type dehydrogenation catalyst of employing, contains various sulfide and total sulfur content reaches 1000mg/m at unstripped gas
3when, this catalyzer normally can use and remove the oxygen in unstripped gas;
(4) depickling gas operation: be cooled to the gas of normal temperature to enter adsorption tower depickling gas, depickling gas selects any one method in pressure swing adsorption process, alkali wash, MDEA method or low-temp methanol washing method;
(5) concentrate operation: concentrate operation can select 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 select pressure-variable adsorption (PSA) method, alkali wash, MDEA method or low-temp methanol to wash method, removes the CO in gas
2, SO
2and H
2s; Described concentrate operation is by methane concentration, separation of nitrogen component.
3. the method for methane in purification concentrate refuse embedded gas according to claim 1, is characterized in that: the sulfur-resistant catalytic deoxidization operation in described step (3) is made up of at least 1 deoxidation reactor and heating unit.
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| CN201110425675.7A CN103159580B (en) | 2011-12-19 | 2011-12-19 | Method of purifying and extracting methane in waste landfill gas |
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| CN103306717B (en) * | 2013-07-03 | 2016-01-06 | 中煤科工集团重庆研究院有限公司 | Counter flow oxidation and residual-heat utilization method after ventilation air gas is concentrated |
| 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 |
| EP3463628B1 (en) * | 2016-05-24 | 2020-07-08 | 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 |
| 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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| CN1634813A (en) * | 2004-11-19 | 2005-07-06 | 四川天一科技股份有限公司 | Method for purification and recovery of methane from refuse landfill gas |
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| CN1634813A (en) * | 2004-11-19 | 2005-07-06 | 四川天一科技股份有限公司 | Method for purification and recovery of methane from refuse landfill gas |
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