WO2019122660A1 - Procédé cryogénique de déazotation d'un gaz de décharge - Google Patents
Procédé cryogénique de déazotation d'un gaz de décharge Download PDFInfo
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- WO2019122660A1 WO2019122660A1 PCT/FR2018/053338 FR2018053338W WO2019122660A1 WO 2019122660 A1 WO2019122660 A1 WO 2019122660A1 FR 2018053338 W FR2018053338 W FR 2018053338W WO 2019122660 A1 WO2019122660 A1 WO 2019122660A1
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- B01D53/22—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols by diffusion
- B01D53/225—Multiple stage diffusion
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- B01D53/04—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols by adsorption, e.g. preparative gas chromatography with stationary adsorbents
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- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
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- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
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Definitions
- the invention relates to a process for producing bio methane by biogas purification, for example biogas from non-hazardous waste storage facilities (ISDND). It also relates to an installation for implementing the method.
- ISDND non-hazardous waste storage facilities
- the present invention relates to a method of treatment by coupling a membrane permeation and a cryogenic distillation of a gaseous stream containing at least methane, carbon dioxide, air gases (nitrogen and oxygen) and pollutants (H 2 S and volatile organic compounds (VOCs)).
- the objective is to produce a gaseous stream rich in methane whose methane content is in line with the needs of its use and to limit as much as possible the impact of CH 4 discharges into the atmosphere (high greenhouse gas) ).
- the invention relates in particular to the purification of biogas from non-hazardous waste storage facilities, hereinafter ISDND (Non-Hazardous Waste Storage Facility), with the aim of producing biomethane in accordance with the injection into a natural gas system or in local use as a vehicle fuel.
- ISDND Non-Hazardous Waste Storage Facility
- ISDNDs The anaerobic digestion of organic wastes in ISDNDs produces a significant amount of biogas throughout ISDND's lifetime and even several years after shutdown and closure of ISDND.
- methane and carbon dioxide - biogas is a powerful greenhouse gas; At the same time, it constitutes a significant source of renewable energy in the context of the scarcity of fossil fuels.
- Biogas contains several polluting compounds and must be purified to allow commercial development. There are several processes for recovering and purifying biogas.
- Biogas mainly contains methane (CH 4 ) and carbon dioxide (CO 2 ) in varying proportions depending on the method of production.
- the gas also contains a proportion of air gases (nitrogen and oxygen) and, to a lesser extent, water, hydrogen sulphide, and volatile organic compounds (VOCs).
- air gases nitrogen and oxygen
- VOCs volatile organic compounds
- the proportions of the biogas components differ.
- the biogas comprises, on dry gas, 30 to 60% of methane, 15 to 50% of CO2, 0 to 30% of nitrogen, 0 to 6% of oxygen, 0 to 1% of hosts and a few tens to thousands of milligrams per normal cubic meters of VOCs and a number of other trace impurities.
- Biogas is valued in different ways. It may, after partial treatment, be recovered near the production site to provide heat, electricity or both (cogeneration). The high content of carbon dioxide and nitrogen reduces its calorific value, increases the compression and transport costs and limits the economic interest of its valuation to this use of proximity.
- Biomethane thus completes the natural gas resources with a renewable part produced in the heart of the territories. It is usable for exactly the same uses as natural gas of fossil origin. It can feed a natural gas network, a filling station for vehicles.
- the modes of valorization of the biomethane are determined according to the local contexts: local energy needs, possibilities of valorization as biomethane fuel, existence close to networks of distribution or transport of natural gas in particular. Creating synergies between the different actors working on a territory (farmers, industrialists, public authorities), the production of biomethane helps the territories to acquire a greater energy autonomy.
- the document US Pat. No. 8,221,524 B2 describes a process for enriching a gas with CH 4 by up to 88% by different recycling steps.
- the process consists of compressing the gas stream and then passing it over an adsorbent to remove VOCs.
- the gas stream is then subjected to a membrane separation step and then to a pressure swing adsorption step (PSA).
- PSA pressure swing adsorption step
- the adsorbent used in the PSA is of the CMS (carbon molecular sieve) type and makes it possible to eliminate the nitrogen and a small part of the oxygen.
- EP1979446 discloses a biogas purification process of removing hhS, compressing the gas, filtering it to remove particles. The gas is then subjected to a membrane separation step to remove CO2 and GO2, from drying by passing through a PSA then in different filters and finally again in a PSA to eliminate nitrogen. The gas is finally liquefied.
- US2004 / 0103782 discloses a biogas purification process of eliminating gas compression, filtering it to remove particles, subjecting it to a pressure swing adsorption (PSA) step to remove VOCs, and then membrane separation to remove most of the CO2 as well as a fraction of the oxygen.
- PSA pressure swing adsorption
- US5964923 and US5669958 disclose a method of treating a gaseous effluent comprising dehydrating the gas, condensing it through an exchanger, subjecting the gas to membrane separation, and then cryogenic separation.
- US2010 / 077796 discloses a purification process of subjecting the gaseous stream to a membrane separation, treating the permeate in a distillation column, and then mixing the methane gas from the column, after vaporization, with the retentate obtained at room temperature. the outcome of membrane separation.
- EP0772665 describes the use of a cryogenic distillation column for the separation of mine gas composed mainly of CFI 4 , CO2 and nitrogen.
- One of the problems that the invention proposes to solve is that of providing a biogas purification process complying with the above constraints, that is to say a process that is safe, with optimal yield, producing a biomethane high quality substitutable for natural gas and which meets environmental standards including the destruction of polluting compounds such as VOCs and compounds with strong greenhouse effect such as CFI 4 .
- the gas thus produced can be recovered in gaseous form either by injection into a gas network or for mobility applications.
- the CO2 is mainly removed on the membrane step. This imperfect separation leaves in the purified gas a CO2 content frequently between 0.5 mol% and 1.5 mol%. It is possible to reduce the content of CO2 in the purified gas by sizing the unit of separation (involving consumption more important of the compressor). In all cases the CO2 content in the purified gas can never be much lower (same order of magnitude of concentration).
- This purified gas containing, among others, the remainder of CO2, methane, a little oxygen and nitrogen (between 1% and 20% mol) is then treated in a cryogenic unit.
- the temperatures reached in this unit are of the order of -100 ° C. or lower, which at low pressure (between Patm and about thirty bar) results in a solidification of the CO2 contained in the gas to be treated.
- a frequently used solution is to use a purification step based on adsorption technology (TSA, Temperature Swing Adsorption).
- TSA Temperature Swing Adsorption
- This technology makes it possible to reach very low levels of CO2 (for example 50ppmv in the case of a liquefied natural gas). At these levels, the CO2 does not solidify at the temperatures considered even at low pressure because it is still soluble in methane.
- this purification unit is relatively expensive and requires the use of a so-called regeneration gas to be able to evacuate the stopped CO2.
- the gas frequently used is either the nitrogen that has been separated in the cryogenic stage or the methane product at the outlet of NRU. If nitrogen is used, it may be necessary to degrade the efficiency of the unit or add nitrogen to achieve the required flow rate. If production methane is used, CO2 concentration peaks associated with desorption may appear to make the gas out of specification.
- the inventors of the present invention have then developed a solution to solve the problems raised above.
- the subject of the present invention is a method for producing biomethane by purifying a biogas feed stream, comprising the following steps:
- the solution that is the object of the present invention is therefore not to further reduce the CO2 content at the outlet of the membrane step while ensuring a sufficient solubility of the CO2 in the gas to be treated (mainly methane) in order to avoid a crystallization and that at any point of the process.
- the TSA stage for slaughtering the majority of CO2 is therefore removed.
- the gas that supplies the cryogenic section therefore contains between 0.3 mol% and 2 mol% of CO2.
- the subject of the invention is also:
- step a) further comprises a step of purifying the compressed gaseous gas stream at pressure P1.
- step a) the separation of CO2 and oxygen from the feed gas stream is carried out by a unit comprising at least two stages of separating membranes.
- step b) the gaseous stream depleted in CO2 from step a) undergoes expansion to a pressure P3 between 15 bar abs and 40 bar abs before entering said distillation column.
- P3 is greater than 25 bar absolute.
- a process as defined above characterized in that prior to expansion, the gaseous stream depleted of CO2 from step a) is at least partially condensed in a heat exchanger.
- a process as defined above characterized in that the gaseous stream depleted of CO2 from step a) is at least partially condensed in a heat exchanger countercurrent CH 4 enriched stream from step c) and at least a portion of the nitrogen stream separated in step b).
- the subject of the invention is also:
- a pretreatment unit for removing all or part of the VOCs, the water, the sulfur compounds of the gas stream to be treated
- a compressor capable of compressing said gaseous flow at a pressure of between 50 and 100 bar;
- TSA for removing CO2 at levels less than 0.3 mol%.
- the heat exchanger may be any heat exchanger, unit or other arrangement adapted to allow the passage of a number of flows, and thus allow a direct or indirect heat exchange between one or more lines of refrigerant, and a or multiple feed streams.
- the reference refers to a liquid flow and the pipe that carries it, the pressures considered are absolute pressures and the percentages considered are molar percentages.
- the plant comprises a source of biogas to be treated (1), a pre-treatment unit (5) comprising a compression unit (2) and a unit for purifying CO2 and Ü2 (23), a VOC and water purification unit (3), a cryodistillation unit (4), and finally a methane gas recovery unit (6). All devices are interconnected by pipes.
- the CO2 purification unit (23) combines, for example, two membrane separation stages.
- the membranes are chosen to allow the separation of at least 90% of the CO2 and about 50% of GO2.
- the retentate from the first separation is then directed to the second membrane separation.
- the permeate from the second membrane separation is recycled through a pipe connected to the main circuit upstream of the compressor. This step makes it possible to produce a gas (7) with less than 3% CO2 and with a CH 4 yield greater than 90%.
- the temperature of this stream is typically ambient, if necessary air or water cooling steps can be incorporated.
- the compression unit (2) is for example in the form of a piston compressor.
- This compressor compresses the gas stream (7) at a pressure of, for example, between 50 and 80 bar.
- the outgoing flow is designated in the figure by the reference (8).
- the VOC and water purification unit (3) comprises two bottles (9, 10). They are loaded with adsorbents chosen specifically to allow the adsorption of water and VOCs, and their subsequent desorption during regeneration.
- the bottles work alternately in production mode and regeneration mode.
- the bottles (9, 10) are supplied with gaseous flow at their lower part.
- the pipe in which the gas flow (8) flows is split into two pipes (1 1, 12), each equipped with a valve (13, 14) and feeding the lower part respectively of the first bottle (9) and the second bottle (10).
- the valves (13, 14) will be alternately closed depending on the saturation level of the bottles.
- the valve (13) is closed and the valve (14) is opened to begin charging the second bottle (10).
- From the upper part of each of the bottles opens a pipe respectively (15 and 16).
- Each of them splits into two pipes respectively (17, 18) and (19, 20).
- the purified flow of water and VOC from the first bottle flows through the pipe (18) while the purified flow of water and VOC from the second PSA flows through the pipe (20).
- the two pipes are joined to form a single pipe (21) supplying the cryogenic unit (4).
- the cryodistillation unit (4) is fed by the pipe (21) in which circulates the gas stream (22) to be purified. It contains three elements respectively a heat exchanger (24), a reboiler (25), a distillation column (26).
- the exchanger (24) is preferably a brazed plate heat exchanger made of aluminum or stainless steel. It cools the gas stream (22) flowing in the pipe (21) by heat exchange with the flow of liquid methane (27) withdrawn from the distillation column (26). The gas stream (22) is cooled (28) to a temperature of about -100 ° C. The two-phase flow (28) resulting therefrom may alternatively ensure the reboiling of the bottom reboiler (25) of the column (26) and the heat generated (29) is transferred to the bottom of the column (26).
- the cooled fluid (28) is expanded by means of a valve (30) at a pressure for example between 20 bar absolute and 45 bar absolute bar absolute.
- the fluid then in the diphasic state or in the liquid state (31) is introduced into the column (26) at a stage E1 located in the upper part of said column (26) at a temperature, for example between -1 10 ° C and -100 ° C.
- the liquid (31) then separates in the column (26) to form a gas (32) through the condenser (33).
- the cooling of the condenser (33) may, for example be provided by a refrigerating cycle using nitrogen and or methane.
- a portion (36) of the liquid (37) exiting the distillation column vessel (26) at a temperature between -120 ° C and -90 ° C is sent to the reboiler (25) where it partially vaporizes. .
- the formed gas (29) is returned to the column vessel (26).
- the other portion (38) of the remaining liquid (37) is pumped by means of a pump (39) to form the liquid methane stream (27) which vaporizes in the exchanger (24) to form a methane product pure gas (40).
- This pumping step is carried out at a high pressure, typically above 25 bar absolute, preferably above 50 bar absolute or the critical pressure of the fluid. This level of pressure makes it possible to avoid the accumulation of CO2 in the last drop of vaporization of the exchange line.
- the gas is very poor in heavy hydrocarbons, the dew point of the gas below the critical pressure is very low (typically below -90 ° C).
Abstract
Description
Claims
Priority Applications (5)
Application Number | Priority Date | Filing Date | Title |
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KR1020207017512A KR20200096541A (ko) | 2017-12-21 | 2018-12-17 | 배출 가스로부터 질소를 제거하는 극저온 방법 |
US16/954,753 US20210172677A1 (en) | 2017-12-21 | 2018-12-17 | Cryogenic process for removing nitrogen from a discharge gas |
CA3085235A CA3085235A1 (fr) | 2017-12-21 | 2018-12-17 | Procede cryogenique de deazotation d'un gaz de decharge |
EP18839833.3A EP3727649A1 (fr) | 2017-12-21 | 2018-12-17 | Procédé cryogénique de déazotation d'un gaz de décharge |
CN201880079693.4A CN111565821A (zh) | 2017-12-21 | 2018-12-17 | 从排出气体中除去氮气的低温方法 |
Applications Claiming Priority (2)
Application Number | Priority Date | Filing Date | Title |
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FR1762858A FR3075659B1 (fr) | 2017-12-21 | 2017-12-21 | Procede de production d'un courant de gaz naturel a partir d'un courant de biogaz. |
FR1762858 | 2017-12-21 |
Publications (1)
Publication Number | Publication Date |
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WO2019122660A1 true WO2019122660A1 (fr) | 2019-06-27 |
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PCT/FR2018/053338 WO2019122660A1 (fr) | 2017-12-21 | 2018-12-17 | Procédé cryogénique de déazotation d'un gaz de décharge |
Country Status (7)
Country | Link |
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US (1) | US20210172677A1 (fr) |
EP (1) | EP3727649A1 (fr) |
KR (1) | KR20200096541A (fr) |
CN (1) | CN111565821A (fr) |
CA (1) | CA3085235A1 (fr) |
FR (1) | FR3075659B1 (fr) |
WO (1) | WO2019122660A1 (fr) |
Cited By (4)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
TWI697451B (zh) * | 2019-07-18 | 2020-07-01 | 聯捷運輸股份有限公司 | 灌充設備及其熱交換裝置與氣體回收方法及灌充方法 |
EP4101917A1 (fr) * | 2021-06-09 | 2022-12-14 | L'air Liquide, Societe Anonyme Pour L'etude Et L'exploitation Des Procedes Georges Claude | Méthode de séparation et de liquéfactions de méthane et de dioxyde de carbone avec élimination des impuretés de l'air présente dans le méthane |
US11946691B2 (en) | 2021-06-09 | 2024-04-02 | L'Air Liquide, Société Anonyme pour l'Etude et l'Exploitation de Procédés Georges Claude | Cryogenic purification of biogas with pre-separation and external solidification of carbon dioxide |
US11976879B2 (en) | 2022-06-09 | 2024-05-07 | L'air Liquide, Societe Anonyme Pour L'etude Et L'exploitation Des Procedes | Process for the separation and liquefaction of methane and carbon dioxide with pre-separation upstream of the distillation column |
Families Citing this family (3)
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EP3820970A4 (fr) | 2018-07-10 | 2022-06-01 | Iogen Corporation | Procédé et système de production de combustible à partir du biogaz |
US11946006B2 (en) | 2019-07-09 | 2024-04-02 | lOGEN Corporation | Method and system for producing a fuel from biogas |
KR102324814B1 (ko) * | 2020-08-18 | 2021-11-11 | 정두섭 | 휘발성 유기화합물 회수 시스템 |
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- 2018-12-17 EP EP18839833.3A patent/EP3727649A1/fr not_active Withdrawn
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TWI697451B (zh) * | 2019-07-18 | 2020-07-01 | 聯捷運輸股份有限公司 | 灌充設備及其熱交換裝置與氣體回收方法及灌充方法 |
EP4101917A1 (fr) * | 2021-06-09 | 2022-12-14 | L'air Liquide, Societe Anonyme Pour L'etude Et L'exploitation Des Procedes Georges Claude | Méthode de séparation et de liquéfactions de méthane et de dioxyde de carbone avec élimination des impuretés de l'air présente dans le méthane |
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US11946691B2 (en) | 2021-06-09 | 2024-04-02 | L'Air Liquide, Société Anonyme pour l'Etude et l'Exploitation de Procédés Georges Claude | Cryogenic purification of biogas with pre-separation and external solidification of carbon dioxide |
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Also Published As
Publication number | Publication date |
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KR20200096541A (ko) | 2020-08-12 |
EP3727649A1 (fr) | 2020-10-28 |
FR3075659B1 (fr) | 2019-11-15 |
CN111565821A (zh) | 2020-08-21 |
CA3085235A1 (fr) | 2019-06-27 |
US20210172677A1 (en) | 2021-06-10 |
FR3075659A1 (fr) | 2019-06-28 |
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