WO2025124239A1 - 一种零碳排放的海洋液化天然气生产系统装置及其方法 - Google Patents

一种零碳排放的海洋液化天然气生产系统装置及其方法 Download PDF

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WO2025124239A1
WO2025124239A1 PCT/CN2024/136588 CN2024136588W WO2025124239A1 WO 2025124239 A1 WO2025124239 A1 WO 2025124239A1 CN 2024136588 W CN2024136588 W CN 2024136588W WO 2025124239 A1 WO2025124239 A1 WO 2025124239A1
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natural gas
equipment
condenser
cryogenic distillation
marine
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French (fr)
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罗勇
王立华
陈建峰
初广文
邹海魁
孙宝昌
张亮亮
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Beijing University of Chemical Technology
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Beijing University of Chemical Technology
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    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10L—FUELS NOT OTHERWISE PROVIDED FOR; NATURAL GAS; SYNTHETIC NATURAL GAS OBTAINED BY PROCESSES NOT COVERED BY SUBCLASSES C10G OR C10K; LIQUIFIED PETROLEUM GAS; USE OF ADDITIVES TO FUELS OR FIRES; FIRE-LIGHTERS
    • C10L3/00—Gaseous fuels; Natural gas; Synthetic natural gas obtained by processes not covered by subclass C10G, C10K; Liquefied petroleum gas
    • C10L3/06—Natural gas; Synthetic natural gas obtained by processes not covered by C10G, C10K3/02 or C10K3/04
    • C10L3/08—Production of synthetic natural gas
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10L—FUELS NOT OTHERWISE PROVIDED FOR; NATURAL GAS; SYNTHETIC NATURAL GAS OBTAINED BY PROCESSES NOT COVERED BY SUBCLASSES C10G OR C10K; LIQUIFIED PETROLEUM GAS; USE OF ADDITIVES TO FUELS OR FIRES; FIRE-LIGHTERS
    • C10L3/00—Gaseous fuels; Natural gas; Synthetic natural gas obtained by processes not covered by subclass C10G, C10K; Liquefied petroleum gas
    • C10L3/06—Natural gas; Synthetic natural gas obtained by processes not covered by C10G, C10K3/02 or C10K3/04
    • C10L3/10—Working-up natural gas or synthetic natural gas
    • C10L3/101—Removal of contaminants
    • C10L3/102—Removal of contaminants of acid contaminants
    • C10L3/104—Carbon dioxide
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10L—FUELS NOT OTHERWISE PROVIDED FOR; NATURAL GAS; SYNTHETIC NATURAL GAS OBTAINED BY PROCESSES NOT COVERED BY SUBCLASSES C10G OR C10K; LIQUIFIED PETROLEUM GAS; USE OF ADDITIVES TO FUELS OR FIRES; FIRE-LIGHTERS
    • C10L3/00—Gaseous fuels; Natural gas; Synthetic natural gas obtained by processes not covered by subclass C10G, C10K; Liquefied petroleum gas
    • C10L3/06—Natural gas; Synthetic natural gas obtained by processes not covered by C10G, C10K3/02 or C10K3/04
    • C10L3/10—Working-up natural gas or synthetic natural gas
    • C10L3/101—Removal of contaminants
    • C10L3/105—Removal of contaminants of nitrogen

Definitions

  • the present invention relates to the technical field of marine natural gas production technology and application field, and more specifically, to a zero-carbon emission marine liquefied natural gas production system device and method thereof.
  • More than 10% of the world's natural gas resources are carbon-rich natural gas, mainly distributed in the South China Sea, the northwest shelf of Australia, Central America, southeast Brazil and other regions.
  • the South China Sea region has extremely rich natural gas resources, accounting for about 12% of the world's total oil and gas resources and 1/3 of the country's oil and gas resources.
  • Its CO2 content is generally between 15% and 80%, and 75% of the resources are distributed in deep sea areas, with high development costs and difficulties.
  • the challenges of developing carbon-rich natural gas come not only from technology, but also from environmental pressure. If such a large amount of CO2 is directly discharged into the atmosphere, it may aggravate the global greenhouse effect and climate change, bringing disaster to the entire human race.
  • the zero-carbon emission marine liquefied natural gas production process refers to the separation of CO2 from natural gas mined from offshore platforms, followed by a methanogenic reaction to produce liquefied natural gas. This can not only realize the resource utilization of CO2 in carbon-rich natural gas and reduce CO2 emissions, but also utilize the relatively complete marine liquefied natural gas infrastructure and integrate it with the original marine liquefied natural gas storage, transportation, distribution and consumption network. Therefore, this process is of great significance to solving the resource utilization of marine natural gas CO2 .
  • the traditional natural gas decarbonization process often uses a double-tower solvent absorption and desorption method to separate CO 2 from natural gas. If this method is applied to the decarbonization of natural gas on an offshore platform, on the one hand, it is necessary to introduce solvents such as ethanolamine to the offshore platform, which will bring a series of problems such as solvent transportation and processing. On the other hand, the double-tower operation scale is large and the operation is more complicated, which cannot meet the actual needs of small space on the offshore platform.
  • Chinese patent application CN 105444527A discloses a natural gas processing device and method, which includes a decarbonization system and a liquefaction system, the decarbonization system is connected to the liquefaction system, and also includes a refrigeration system, the decarbonization system and the liquefaction system are respectively connected to the refrigeration system, and the decarbonization system includes: a first heat exchanger and a packed distillation tower; the raw gas outlet of the first heat exchanger is connected to the raw gas inlet of the packed distillation tower.
  • the CO 2 methanation process uses a fixed bed reactor with high temperature, the reaction temperature is difficult to control, and carbon deposition is easy to occur, resulting in reduced catalyst activity, which is not conducive to the efficient conversion of CO 2. Therefore, the development of an efficient zero-carbon emission marine liquefied natural gas production process has important practical significance and industrial application value.
  • the first technical problem to be solved by the present invention is to provide a zero-carbon emission marine liquefied natural gas production system device.
  • the second technical problem to be solved by the present invention is to provide a method for producing marine liquefied natural gas with zero carbon emissions using the above-mentioned system device.
  • a zero-carbon emission marine liquefied natural gas production system device including a marine natural gas separation device, a water electrolysis hydrogen production device and a CO2 methanation device;
  • the marine natural gas separation device includes a marine natural gas storage tank, a first raw material delivery pump, a first condenser, a first cryogenic distillation device, a second raw material delivery pump, a second condenser, a second cryogenic distillation device, a natural gas condensation and drying device, and a natural gas pressurized liquefaction device;
  • the top of the first cryogenic distillation equipment is connected to the inlet of the second raw material delivery pump through a pipeline;
  • the outlet of the second raw material delivery pump is connected to the inlet of the second condenser through a pipeline, and the outlet of the second condenser is connected to the inlet of the second cryogenic distillation equipment through a pipeline; the outlet of the second cryogenic distillation equipment passes through the natural gas condensation and drying equipment and the natural gas pressure liquefaction equipment and then is transported to external users through the natural gas transmission pipeline network;
  • the bottom outlet of the first cryogenic rectification equipment is connected to a gas mixer via a pipeline;
  • the water electrolysis hydrogen production device comprises a water storage tank, a water delivery pump, clean energy power generation equipment, water electrolysis hydrogen production equipment and hydrogen delivery equipment;
  • the clean energy power generation equipment is electrically connected to the water electrolysis hydrogen production equipment to provide electrical energy therefor;
  • the water electrolysis hydrogen production equipment is connected to the gas mixer via the hydrogen delivery equipment;
  • the CO2 methanation device includes a gas mixer, a heat exchanger, a multi-stage heat transfer type ultra-gravity reactor and a third condenser;
  • the gas mixer, heat exchanger, multi-stage heat transfer ultra-gravity reactor and the third condenser are connected in sequence; the outlet of the third condenser is divided into two branches; the gas phase of the first branch leads to the natural gas condensation and drying equipment and the natural gas pressurized liquefaction equipment and then is transported to external users through the natural gas transmission pipeline network; the liquid phase of the second branch leads to the pipeline connecting the water storage tank and the water delivery pump through the pipeline.
  • the first cryogenic distillation equipment and the second cryogenic distillation equipment are rotary distillation separation equipment that can enhance gas-liquid mass transfer; the first cryogenic distillation equipment is used to separate carbon dioxide from raw marine natural gas; the second cryogenic distillation equipment is used to separate nitrogen from raw marine natural gas.
  • the operating temperature of the first cryogenic distillation equipment is -100 to 50°C, and the operating pressure is 0.1 to 10 MPa; the operating temperature of the second cryogenic distillation equipment is -180 to -50°C, and the operating pressure is 0.1 to 10 MPa.
  • the rotor of the multi-stage heat transfer type ultra-gravity reactor is loaded with a catalyst for catalyzing CO2 methanation, and the catalyst is loaded in a regular loading type or in bulk.
  • the reaction temperature in the rotor of the multi-stage heat transfer ultragravity reactor is 150-500°C, and the reaction pressure is 0.1-10 MPa. More preferably, the reaction temperature in the rotor is 250-400°C, and the reaction pressure is 0.1-2 MPa.
  • the internal rotor speed of the multi-stage heat transfer ultragravity reactor is 100 to 3000 r/min, and more preferably, the speed range is 500 to 1500 r/min.
  • the clean energy power generation equipment is one or more of solar photovoltaic power generation equipment, wind power generation equipment, and other surplus energy power generation equipment on an offshore natural gas platform.
  • the source of the raw water for the water electrolysis hydrogen production device is one or a combination of seawater, desalinated seawater, and water separated by the third condenser.
  • the water electrolysis hydrogen production equipment is one of an alkaline electrolyzer, a proton exchange membrane electrolyzer, a high-temperature solid oxide water electrolyzer or a solid polymer anion exchange membrane electrolyzer.
  • the present invention adopts the following technical solution :
  • a method for producing marine liquefied natural gas with zero carbon emissions using the above system device comprises the following steps:
  • the high-purity CO2 separated at the bottom of the first cryogenic distillation equipment and the H2 produced by the water electrolysis hydrogen production equipment are mixed in proportion in a gas mixer, and then preheated by a heat exchanger before entering a multi-stage heat transfer type ultra-gravity reactor; in the multi-stage heat transfer type ultra-gravity reactor, they alternately pass through the rotor reaction area and the stator heat exchange area to undergo CO2 methanation reaction and heat exchange respectively, and finally the product is condensed by the third condenser to obtain natural gas that meets the requirements, which is further condensed and dried by a natural gas condensation and drying equipment, pressurized and liquefied by a natural gas pressurized liquefaction equipment, and then transported to an external natural gas transportation pipeline network.
  • Any range described in the present invention includes the end value and any numerical value between the end values and any sub-range formed by the end value or any numerical value between the end values.
  • the present invention has the following beneficial effects :
  • the present invention provides a zero-carbon emission marine liquefied natural gas production system device and a production method thereof.
  • the method uses green hydrogen obtained by electrolyzing water with renewable energy and CO2 separated from marine natural gas for methanation reaction, thereby realizing the resource utilization of CO2 in marine natural gas, which is in line with the development trend of energy conservation and emission reduction.
  • the method can make use of the original liquefied natural gas transportation pipeline, reducing the investment in transportation and other equipment.
  • the present invention provides a means of natural gas decarbonization by low-temperature distillation, which avoids the transportation and treatment of solvents, reduces the number and scale of equipment, and better meets the actual needs of small space on the offshore platform.
  • CO2 methanation uses a multi-stage heat transfer high-gravity reactor, it can achieve rapid heat transfer and effectively regulate the contact time between the reactants and products and the catalyst, without causing excessive heat accumulation, and is easy to operate.
  • the process of the present invention unexpectedly found that the introduction of a multi-stage heat transfer high-gravity reactor for CO2 methanation reaction can reduce carbon deposition on the catalyst surface, improve the activity of the catalyst, and reduce investment in equipment and operating costs.
  • FIG1 shows a schematic diagram of a zero-carbon emission marine liquefied natural gas production system device of the present invention
  • FIG2 is a schematic diagram of a multi-stage heat transfer type high gravity reactor in a zero-carbon emission marine liquefied natural gas production system of the present invention
  • FIG3 shows a schematic diagram of a production system device in Comparative Example 5 in which three single-stage high-gravity reactors and two heat exchangers are used instead of a multi-stage heat transfer high-gravity reactor.
  • a zero-carbon emission marine liquefied natural gas production system device of the present invention includes a marine natural gas separation device 100 , a water electrolysis hydrogen production device 200 and a CO 2 methanation device 300 ;
  • the marine natural gas separation device 100 includes a marine natural gas storage tank 101, a first raw material delivery pump 102, a first condenser 103, a first cryogenic distillation device 104, a second raw material delivery pump 105, a second condenser 106, a second cryogenic distillation device 107, a natural gas condensation and drying device 108 and a natural gas pressurized liquefaction device 109;
  • the first cryogenic distillation equipment 104 is used to separate carbon dioxide from the raw marine natural gas; the second cryogenic distillation equipment 107 is used to separate nitrogen from the raw marine natural gas;
  • the marine natural gas storage tank 101, the first raw material delivery pump 102, the first condenser 103, and the first cryogenic distillation equipment 104 are connected in sequence through pipelines;
  • the water electrolysis hydrogen production device 200 includes a water storage tank 201, a water delivery pump 202, a clean energy power generation device 203, a water electrolysis hydrogen production device 204 and a hydrogen delivery device 205;
  • the water storage tank 201 is connected to the water electrolysis hydrogen production equipment 204 through a pipeline and a water delivery pump 202;
  • the clean energy power generation equipment 203 is electrically connected to the water electrolysis hydrogen production equipment 204 to provide electrical energy therefor;
  • the gas mixer 301, the heat exchanger 302, the multi-stage heat transfer ultra-gravity reactor 303 and the third condenser 304 are connected in sequence; the outlet of the third condenser 304 is divided into two branches; the gas phase of the first branch is led to the natural gas condensation and drying equipment 108 and the natural gas pressurized liquefaction equipment 109 and then transported to external users through the natural gas transmission pipeline network; the liquid phase of the second branch is led to the pipeline connecting the water storage tank 201 and the water delivery pump 202 through a pipeline.
  • the multi-stage heat transfer type ultra-gravity reactor 303 includes a motor 3031, a shell 3032, a rotor 3033, a heat exchange component 3034, a heat exchange medium inlet 3035, a reaction material inlet 3036, a dynamic seal 3037, a heat exchange medium outlet 3038, and a generated material outlet 3039.
  • the rotor 3033 and the catalyst therein are rotating components, and the heat exchange component 3034 is fixed to the shell.
  • a multi-stage heat transfer type supergravity reactor 303 is used as a reactor for CO2 methanation, and its purpose is not to simply enhance mass transfer and thereby improve reaction efficiency. Rather, it is because the fixed bed reactor is prone to carbon deposition, which leads to catalyst deactivation and reduced catalyst activity, which will be detrimental to the efficient conversion of CO2 ; the supergravity reactor effectively regulates the contact time between the reactants and products and the catalyst, does not cause excessive local accumulation of heat, and is easy to operate.
  • the supergravity reactor of the present invention is used for CO2 methanation reaction, which can reduce carbon deposition on the catalyst surface and improve catalyst activity.
  • the problem of the difficulty in heat transfer in the supergravity device used for CO2 methanation, a highly exothermic reaction process is effectively solved.
  • the source of raw water for the water electrolysis hydrogen production device 200 is one or a combination of seawater, desalinated seawater, and water separated by the third condenser.
  • a method for producing marine liquefied natural gas with zero carbon emissions using the above system device comprises the following steps:
  • the natural gas raw material mainly containing CH 4 , CO 2 , and N 2 after pretreatment is transported to the marine natural gas storage tank 101 through a pipeline, and then partially condensed by the first raw material delivery pump 102 and the first condenser 103 and transported to the first cryogenic distillation equipment 104.
  • the first cryogenic distillation equipment 104 separates CH 4 and N 2 at the top of the tower, and separates high-purity CO 2 at the bottom of the tower;
  • S2, CH4 and N2 extracted from the top of the first cryogenic distillation equipment 104 are condensed by the second raw material delivery pump 105 and the second condenser 106, and then transported to the second cryogenic distillation equipment 107.
  • the top of the second cryogenic distillation equipment 107 extracts N2 and empties it, and high-purity CH4 is separated from the bottom of the tower, and further condensed and dried by the natural gas condensation and drying equipment 108, pressurized and liquefied by the natural gas pressure liquefaction equipment 109, and then transported to the external natural gas transportation network;
  • the high-purity CO2 separated at the bottom of the first cryogenic distillation equipment 104 and the H2 produced by the water electrolysis hydrogen production equipment 204 are mixed in proportion in the gas mixer 301, and then preheated by the heat exchanger 302, and then enter the multi-stage heat transfer type ultra-gravity reactor 303.
  • the multi-stage heat transfer type ultra-gravity reactor 303 they alternately pass through the rotor reaction area and the stator heat exchange area to undergo CO2 methanation reaction and heat exchange respectively.
  • the product is condensed and dried by the third condenser 306 to obtain natural gas that meets the requirements. It is further condensed and dried by the natural gas condensation and drying equipment 108 and pressurized and liquefied by the natural gas pressure liquefaction equipment 109, and then transported to the external natural gas transportation pipeline network.
  • a method for producing marine liquefied natural gas with zero carbon emissions using the above system device as shown in FIG1 includes the following steps:
  • the natural gas raw material mainly containing about 40% CH 4 , 55% CO 2 , and 5% N 2 by volume is transported to the marine natural gas storage tank by pipeline, and then partially condensed by the first raw material delivery pump and the first condenser and transported to the first cryogenic distillation equipment.
  • the first cryogenic distillation equipment separates 88% CH 4 and 12% N 2 at the top of the tower, and separates high-purity 85% CO 2 at the bottom of the tower;
  • NiMn/ Al2O3 catalysts are respectively loaded into the rotor of the multi-stage heat transfer type ultra -gravity reactor, CO2 and H2 produced by the electrolysis water hydrogen production equipment are separated at the bottom of the first cryogenic distillation equipment, mixed in a gas mixer at a volume ratio of 1:4, and then preheated by a heat exchanger, and then enter the multi-stage heat transfer type ultra-gravity reactor to carry out CO2 methanation reaction under the conditions of 2MPa and 300°C.
  • the product is condensed and dried by the third condenser to obtain natural gas that meets the requirements, and is further condensed and dried by the natural gas condensation and drying equipment, pressurized and liquefied by the natural gas pressure liquefaction equipment, and then transported to the external natural gas transportation pipeline network.
  • Example 1 was repeated, except that a monoethanolamine double-tower absorption and desorption decarbonization process was used to replace the first cryogenic distillation equipment to remove CO 2 .
  • Example 1 was repeated, except that three fixed bed reactors were used instead of the multi-stage heat transfer supergravity reactor for the CO2 methanation reaction.

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Abstract

本发明公开了一种零碳排放的海洋液化天然气生产系统装置，包括海洋天然气分离装置、电解水制氢装置和CO2甲烷化装置；所述海洋天然气分离装置包括海洋天然气储罐、第一原料输送泵、第一冷凝器、第一低温精馏设备、第二原料输送泵、第二冷凝器、第二低温精馏设备、天然气冷凝干燥设备和天然气加压液化设备；所述电解水制氢装置包括水储罐、水输送泵、清洁能源发电设备、电解水制氢设备和氢气输送设备；所述CO2甲烷化装置包括气体混合器、换热器、多级移热式超重力反应器、第三冷凝器；本发明采用多级移热式超重力反应器，一方面可以解决该反应强放热过程超重力装置移热问题，另一方面有效减少了催化剂表面的积碳。

Description

一种零碳排放的海洋液化天然气生产系统装置及其方法 技术领域
本发明涉及海洋天然气生产工艺及应用领域技术领域。更具体地，涉及一种零碳排放的海洋液化天然气生产系统装置及其方法。
背景技术
全球超过10％的天然气资源是富碳天然气，主要分布在中国南海、澳大利亚西北大陆架、美洲中部、巴西东南等区域。中国南海地区拥有的天然气资源异常丰富，约占全球油气资源总量的12％，是全国油气资源的1/3，其CO2含量普遍在15％～80％之间，而且75％的资源分布在深海地区，开发成本高、难度大。富碳天然气的开发的挑战不仅来自于技术，还有环保的压力，如此大量的CO2如果直接排放到大气中，将可能会加剧全球温室效应和气候变化，给整个人类带来灾难。
零碳排放的海洋液化天然气生产工艺指的是将海上平台开采的天然气中CO2进行分离后，发生甲烷化反应生产液化天然气，既可以实现富碳天然气中CO2的资源化利用，减少CO2排放，又可以利用已经较为完善的海洋液化天然气基础设施，与原有海上液化天然气的储运、输配和消费网络融合。因此，该工艺对解决海洋天然气CO2资源化利用意义重大。
传统的天然气脱碳工艺往往采用双塔溶剂吸收解吸的方式，从天然气中分离得到CO2，该方法若应用于海洋平台天然气脱碳，一方面需要引入乙醇胺等溶剂至海洋平台，会带来溶剂输送、处理等一系列问题，另一方面，双塔操作规模大，操作更为复杂，不能满足海洋平台上空间容纳小的现实需要。例如：中国专利申请CN 105444527A公开了一种天然气处理装置及方法，该装置包括脱碳系统和液化系统，所述脱碳系统与所述液化系统连接，还包括制冷系统，所述脱碳系统与所述液化系统分别与所述制冷系统连接，所述脱碳系统包括：第一换热器和填料精馏塔；所述第一换热器的原料气出口与所述填料精馏塔的原料气入口连接。通过采用矩鞍环填料精馏塔脱碳代替传统的吸收、吸附等双塔脱碳流程，并通过制冷系统为脱碳过程提供冷量，减小了天然气脱碳装置的规模，简化了脱碳流程，并降低了处理装置的功耗。考虑到海洋平台空间限制，有必须要选用更紧凑型的精馏分离设备。
此外，CO2甲烷化过程采用固定床反应器温升高，反应温度不易控制，容易积碳，导致催化剂活性降低，这将不利于CO2的高效转化。因此，开发一种高效的零碳排放的海洋液化天然气生产工艺，具有重要的现实意义和工业应用价值。
发明内容
本发明要解决的第一个技术问题是提供一种零碳排放的海洋液化天然气生产系统装置。
本发明要解决的第二个技术问题是提供一种利用上述系统装置零碳排放生产海洋液化天然气的方法。
为解决上述第一个技术问题，发明采用的技术方案如下：
一种零碳排放的海洋液化天然气生产系统装置，包括海洋天然气分离装置、电解水制氢装置和CO2甲烷化装置；
所述海洋天然气分离装置包括海洋天然气储罐、第一原料输送泵、第一冷凝器、第一低温精馏设备、第二原料输送泵、第二冷凝器、第二低温精馏设备、天然气冷凝干燥设备和天然气加压液化设备；
所述海洋天然气储罐、第一原料输送泵、第一冷凝器、第一低温精馏设备依次通过管道连通；
所述第一低温精馏设备顶部通过管道与第二原料输送泵进口连通；
所述第二原料输送泵出口通过管道与第二冷凝器入口连通，所述第二冷凝器的出口通过管道与第二低温精馏设备入口连通；所述第二低温精馏设备的出口通过天然气冷凝干燥设备和天然气加压液化设备后通过天然气输送管网输送至外界用户；
所述第一低温精馏设备底部出口通过管道和气体混合器连通；
所述电解水制氢装置包括水储罐、水输送泵、清洁能源发电设备、电解水制氢设备和氢气输送设备；
所述水储罐通过管道和水输送泵与电解水制氢设备相连通；
所述清洁能源发电设备与电解水制氢设备电连接，为其提供电能；
所述电解水制氢设备通过氢气输送设备和气体混合器连通；
所述CO2甲烷化装置包括气体混合器、换热器、多级移热式超重力反应器和第三冷凝器；
所述气体混合器、换热器、多级移热式超重力反应器和第三冷凝器依次连通；所述第三冷凝器的出口分为两个分支；第一分支气相通向天然气冷凝干燥设备和天然气加压液化设备后通过天然气输送管网输送至外界用户；第二分支液相通过管道通向连接水储罐和水输送泵的管道上。
优选地，所述多级移热式超重力反应器包括电机、壳体、转子、换热部件、换热介质进口、反应物料进口、动密封、换热介质出口、生成物料出口。
优选地，所述第一低温精馏设备和第二低温精馏设备选用能强化气液传质的旋转式精馏分离设备；所述第一低温精馏设备用于分离原料海洋天然气中的二氧化碳；所述第二低温精馏设备用于分离原料海洋天然气中的氮气。
优选地，所述第一低温精馏设备的操作温度为-100～50℃、操作压力为0.1～10MPa；所述第二低温精馏设备的操作温度为-180～-50℃、操作压力为0.1～10MPa。
优选地，所述多级移热式超重力反应器转子内装载的是用于催化CO2甲烷化的催化剂，催化剂的装填类型是规整装填类型或散装类型。
优选地，多级移热式超重力反应器转子内反应温度为150～500℃、反应压力为0.1～10MPa，更优选地，转子内反应温度为250～400℃、反应压力为0.1～2MPa。
优选地，多级移热式超重力反应器内转子转速为100～3000r/min，更优选地，转速范围为500～1500r/min。
优选地，所述清洁能源发电设备为太阳能光伏发电设备、风能发电设备、海洋天然气平台上其他剩余能源发电设备中的一种或多种。
优选地，所述电解水制氢装置原料水的来源为海水、淡化海水、第三冷凝器分离出的水中的一种或几种组合。
优选地，所述电解水制氢设备为碱性电解槽、质子交换膜电解槽、高温固体氧化物水电解槽或固体聚合物阴离子交换膜电解槽中的一种。
为解决上述第二个技术问题，本发明采用如下的技术方案：
一种利用上述系统装置零碳排放生产海洋液化天然气的方法，包括以下步骤：
S1、经预处理后主要含CH4、CO2、N2的天然气原料由管道输送至海洋天然气储罐，再通过第一原料输送泵和第一冷凝器部分冷凝后输送至第一低温精馏设备中，第一低温精馏设备塔顶分离出CH4和N2、塔底分离得到高纯度的CO2；
S2、由第一低温精馏设备塔顶采出的CH4和N2，经过第二原料输送泵和第二冷凝器进行冷凝后，输送至第二低温精馏设备中，第二低温精馏设备塔顶采出N2排空，塔底分离出高纯度CH4，进一步经天然气冷凝干燥设备进行冷凝干燥、天然气加压液化设备进行加压液化后输送至外界天然气输运管网中；
S3、由清洁能源发电设备提供电能的电解水制氢设备制取出高纯度氢气；
S4、由所述第一低温精馏设备塔底分离得到高纯度CO2和电解水制氢设备制取的H2，在气体混合器内按比例进行混合，然后经过换热器预热后，进入到多级移热式超重力反应器中；在多级移热式超重力反应器中交替依次经过转子反应区域和定子换热区域，分别进行发生CO2甲烷化反应和热量交换，最后产物经过第三冷凝器进行冷凝得到符合要求的天然气，进一步经天然气冷凝干燥设备进行冷凝干燥、天然气加压液化设备进行加压液化后输送至外界天然气输运管网中。
本发明所记载的任何范围包括端值以及端值之间的任何数值以及端值或者端值之间的任意数值所构成的任意子范围。
如无特殊说明，本发明中的各原料均可通过市售购买获得，本发明中所用的设备可采用所属领域中的常规设备或参照所属领域的现有技术进行。
与现有技术相比较，本发明具有如下有益效果：
1.本发明提供了一种零碳排放的海洋液化天然气生产系统装置及其生产方法，该方法一方面采用可再生能源电解水获得的绿氢与海洋天然气分离得到的CO2进行甲烷化反应，实现了海洋天然气中CO2进行资源化利用，符合节能减排的发展趋势，另一方面可以借助原有的液化天然气输运管路，减少了运输等设备投资。
2.相比于传统的海洋平台上天然气脱碳工艺，本发明提供了一种低温精馏的天然气脱碳手段，避免了溶剂的输送和处理，减少了设备数量和规模，更好的满足海洋平台上空间容纳小的现实需要，此外，更惊奇的发现，选用更紧凑的旋转式精馏分离设备，将进一步减小设备体积，有利于减少CO2进行资源化利用过程的设备空间。
3.由于CO2甲烷化使用了多级移热式超重力反应器，可以实现快速移热并有效调控反应物和生成物与催化剂接触时间，不会造成热量过度堆积，易于操作，本发明工艺意外地发现引入多级移热式超重力反应器应用于CO2甲烷化反应，可减少了催化剂表面的积碳，提高催化剂的活性，同时减少设备及运行成本等投资。
附图说明
下面结合附图对本发明的具体实施方式作进一步详细的说明
图1示出本发明一种零碳排放的海洋液化天然气生产系统装置示意图；
图2示出本发明一种零碳排放的海洋液化天然气生产系统中多级移热式超重力反应器示意图；
图3示出了对比例5中采用三个单级超重力反应器和两个换热器代替多级移热式超重力反应器的生产系统装置示意图。
具体实施方式
为了更清楚地说明本发明，下面结合优选实施例对本发明做进一步的说明。本领域技术人员应当理解，下面所具体描述的内容是说明性的而非限制性的，不应以此限制本发明的保护范围。
参见图1所示，作为本发明的一个方面，本发明一种零碳排放的海洋液化天然气生产系统装置，包括海洋天然气分离装置100、电解水制氢装置200和CO2甲烷化装置300；
所述海洋天然气分离装置100包括海洋天然气储罐101、第一原料输送泵102、第一冷凝器103、第一低温精馏设备104、第二原料输送泵105、第二冷凝器106、第二低温精馏设备107、天然气冷凝干燥设备108和天然气加压液化设备109；
所述第一低温精馏设备104用于分离原料海洋天然气中的二氧化碳；所述第二低温精馏设备107用于分离原料海洋天然气中的氮气；
所述海洋天然气储罐101、第一原料输送泵102、第一冷凝器103、第一低温精馏设备104依次通过管道连通；
所述第一低温精馏设备104顶部通过管道与第二原料输送泵105进口连通；
所述第二原料输送泵105出口通过管道与第二冷凝器106入口连通，所述第二冷凝器106的出口通过管道与第二低温精馏设备107入口连通；所述第二低温精馏设备107的出口通过天然气冷凝干燥设备108和天然气加压液化设备109后通过天然气输送管网输送至外界用户；
所述第一低温精馏设备104底部出口通过管道和气体混合器301连通；
所述电解水制氢装置200包括水储罐201、水输送泵202、清洁能源发电设备203、电解水制氢设备204和氢气输送设备205；
所述水储罐201通过管道和水输送泵202与电解水制氢设备204相连通；
所述清洁能源发电设备203与电解水制氢设备204电连接，为其提供电能；
所述电解水制氢设备204通过氢气输送设备205和气体混合器301连通；
所述CO2甲烷化装置300包括气体混合器301、换热器302、多级移热式超重力反应器303和第三冷凝器304；
所述气体混合器301、换热器302、多级移热式超重力反应器303和第三冷凝器304依次连通；所述第三冷凝器304的出口分为两个分支；第一分支气相通向天然气冷凝干燥设备108和天然气加压液化设备109后通过天然气输送管网输送至外界用户；第二分支液相通过管道通向连接水储罐201和水输送泵202的管道上。
参见图2所示，所述多级移热式超重力反应器303包括电机3031、壳体3032、转子3033、换热部件3034、换热介质进口3035、反应物料进口3036、动密封3037、换热介质出口3038、生成物料出口3039。所述多级移热式超重力反应器303中，转子3033及其内的催化剂是旋转部件，换热部件3034是固定在壳体上的。
本发明中，使用了多级移热式超重力反应器303来作为CO2甲烷化的反应器，其目的不是简单的强化传质，进而提高反应效率。而是由于采用固定床反应器容易积碳，导致催化剂失活，催化剂活性降低，这将不利于CO2的高效转化；通过超重力反应器有效调控反应物和生成物与催化剂的接触时间，不会造成热量局部过度堆积，易于操作，本发明超重力反应器用于CO2甲烷化反应，能减少了催化剂表面的积碳，提高催化剂的活性，此外，通过在多级转子中间增加换热区域，有效解决了超重力装置用于CO2甲烷化这种强放热反应过程不易移热的问题。
在某些实施例中，所述第一低温精馏设备104和第二低温精馏设备107选自能强化气液传质的旋转式精馏分离设备；所述第一低温精馏设备104用于分离原料海洋天然气中的二氧化碳；所述第二低温精馏设备107用于分离原料海洋天然气中的氮气。本发明意外地发现，通过使用低温精馏设备来分离原料海洋天然气中的二氧化碳，和现有技术中通过吸附脱碳工艺相比，不仅避免了溶剂的输送和处理，减少了设备数量和规模，更好的满足海洋平台上空间容纳小的现实需要，而且生产效率上也大幅提高，可以至少提高20％左右的生产效率。
在某些实施例中，所述第一低温精馏设备104的操作温度为-100～50℃、操作压力为0.1～10MPa；所述第二低温精馏设备107的操作温度为-180～-50℃、操作压力为0.1-10MPa。当温度和压力低于或高于该范围一方面可能会导致相应的分离回收效率降低，另一方面可能会导致分离能耗增加。
在某些实施例中，所述多级移热式超重力反应器303的转子内装载的是用于催化CO2甲烷化的催化剂，催化剂的装填类型是规整装填类型或散装类型。
在某些实施例中，多级移热式超重力反应器303转子内的反应温度为150～500℃、反应压力为0.1～10MPa，更优选地，转子内的反应温度为250～400℃、反应压力为0.1～2MPa。在反应过程中，若反应温度高于500℃，催化剂可能会因烧结而失活，且CH4的选择性会受到热力学限制，但反应温度太低会导致反应速率变慢。升高压力有利于提高反应速率及平衡转化率，但压力过高会导致设备投资和能耗增加。
在某些实施例中，多级移热式超重力反应器303内转子转速为100～3000r/min，更优选地，转速范围为500～1500r/min。
在某些实施例中，所述清洁能源发电设备203为太阳能光伏发电设备、风能发电设备、海洋天然气平台上其他剩余能源发电设备中的一种或多种。
在某些实施例中，所述电解水制氢装置200原料水的来源为海水、淡化海水、第三冷凝器分离出的水中的一种或几种组合。
在某些实施例中，所述电解水制氢设备204为碱性电解槽、质子交换膜电解槽、高温固体氧化物水电解槽或固体聚合物阴离子交换膜电解槽中的一种。
作为本发明的第二个方面，本发明一种利用上述系统装置零碳排放生产海洋液化天然气的方法，包括以下步骤：
S1、经预处理后主要含CH4、CO2、N2的天然气原料由管道输送至海洋天然气储罐101，再通过第一原料输送泵102和第一冷凝器103部分冷凝后输送至第一低温精馏设备104中，第一低温精馏设备104塔顶分离出CH4和N2、塔底分离得到高纯度的CO2；
S2、由第一低温精馏设备104塔顶采出的CH4和N2，经过第二原料输送泵105和第二冷凝器106进行冷凝后，输送至第二低温精馏设备107中，第二低温精馏设备107塔顶采出N2排空，塔底分离出高纯度CH4，进一步经天然气冷凝干燥设备108进行冷凝干燥、天然气加压液化设备109进行加压液化后输送至外界天然气输运管网中；
S3、由清洁能源发电设备203提供电能的电解水制氢设备204制取出高纯度氢气；
S4、由所述第一低温精馏设备104塔底分离得到高纯度CO2和电解水制氢设备204制取的H2，在气体混合器301内按比例进行混合，然后经过换热器302预热后，进入到多级移热式超重力反应器303中，在多级移热式超重力反应器303中交替依次经过转子反应区域和定子换热区域，分别进行发生CO2甲烷化反应和热量交换，最后产物经过第三冷凝器306进行冷凝干燥得到符合要求的天然气，进一步经天然气冷凝干燥设备108进行冷凝干燥、天然气加压液化设备109进行加压液化后输送至外界天然气输运管网中。
实施例1
利用如图1所示的一种利用上述系统装置零碳排放生产海洋液化天然气的方法，包括以下步骤：
S1、经预处理后主要含体积分数约40％CH4、55％CO2、5％N2的天然气原料由管道输送至海洋天然气储罐，再通过第一原料输送泵和第一冷凝器部分冷凝后输送至第一低温精馏设备中，第一低温精馏设备塔顶分离出88％CH4和12％N2、塔底分离得到高纯度的85％CO2；
S2、由第一低温精馏设备塔顶采出的CH4和N2，经过第二原料输送泵和第二冷凝器进行冷凝后，输送至第二低温精馏设备中，第二低温精馏设备塔顶采出97％N2排空，塔底分离出高纯度97％的CH4，进一步经天然气冷凝干燥设备进行冷凝干燥、天然气加压液化设备进行加压液化后输送至外界天然气输运管网中；
S3、由太阳能发电设备提供电能的电解水制氢设备制取出高纯度99％氢气；
S4、在多级移热式超重力反应器转子内分别装填成型的NiMn/Al2O3催化剂，由所述第一低温精馏设备塔底分离得到CO2和电解水制氢设备制取的H2，在气体混合器内按体积比1:4比例进行混合，然后经过换热器预热后，进入到多级移热式超重力反应器中在2MPa，300℃条件下进行CO2甲烷化反应，最后产物经过第三冷凝器进行冷凝干燥得到符合要求的天然气，进一步经天然气冷凝干燥设备进行冷凝干燥、天然气加压液化设备进行加压液化后输送至外界天然气输运管网中。
对比例1
重复实施例1，其不同之处仅在于：采用单乙醇胺双塔吸收解吸脱碳工艺替代第一低温精馏设备来脱除CO2。
结果发现，脱碳设备投资成本将提高26％，年运行投资成本提高22％；脱碳效率将下降23％。
对比例2
重复实施例1，其不同之处仅在于：采用三个固定床反应器代替多级移热式超重力反应器用于CO2甲烷化反应。
结果发现：CO2转化率降低了16％；CH4选择性降低了7％。
对比例3
重复实施例1，其不同之处仅在于:采用三个固定床反应器代替多级移热式超重力反应器用于CO2甲烷化反应，发现达到相同甲烷产量的情况下，使用多级移热式超重力反应器的系统装置比使用固定床反应器的系统装置的运行时间缩短了28％；进一步对从反应器中卸出的催化剂进行XRD分析，发现固定床反应器催化剂比表面积相对于超重力反应器中催化剂比表面积缩小了约24％。
由此可见，在达到相同转化率的情况下，使用三个固定床反应器的系统装置，因为积碳的原因使得催化剂活性下降，使用寿命更短，转化率降低。
对比例4
重复实施例1，其不同之处仅在于：采用多段移热的固定床反应器代替多级移热式超重力反应器用于CO2甲烷化反应，发现达到相同甲烷产量的情况下，使用超重力反应器的系统装置比使用固定床反应器的系统装置的运行时间缩短了22％；此外，还发现甲烷化反应设备投资成本将提高29％，年运行投资成本提高12％。
主要是因为使用多段移热的固定床反应器，也会由于积碳的原因使得催化剂活性下降，使用寿命更短，转化率降低。
对比例5
参见图3所示，重复实施例1，其不同之处仅在于：采用三个单级超重力反应器和两个换热器代替多级移热式超重力反应器用于CO2甲烷化反应。
结果发现，保持达到相同CO2转化率的情况下，设备投资成本将提高13％，年运行投资成本提高8％。
显然，本发明的上述实施例仅仅是为清楚地说明本发明所作的举例，而并非是对本发明的实施方式的限定。对于所属领域的普通技术人员来说，在上述说明的基础上还可以做出其它不同形式的变化或变动。这里无法对所有的实施方式予以穷举。凡是属于本发明的技术方案所引伸出的显而易见的变化或变动仍处于本发明的保护范围之列。

Claims (10)

  1. 一种零碳排放的海洋液化天然气生产系统装置，其特征在于：包括海洋天然气分离装置、电解水制氢装置和CO2甲烷化装置；
    所述海洋天然气分离装置包括海洋天然气储罐、第一原料输送泵、第一冷凝器、第一低温精馏设备、第二原料输送泵、第二冷凝器、第二低温精馏设备、天然气冷凝干燥设备和天然气加压液化设备；
    所述海洋天然气储罐、第一原料输送泵、第一冷凝器、第一低温精馏设备依次通过管道连通；
    所述第一低温精馏设备顶部通过管道与第二原料输送泵进口连通；
    所述第二原料输送泵出口通过管道与第二冷凝器入口连通，所述第二冷凝器的出口通过管道与第二低温精馏设备入口连通；所述第二低温精馏设备的出口通过天然气冷凝干燥设备和天然气加压液化设备后通过天然气输送管网输送至外界用户；
    所述第一低温精馏设备底部出口通过管道和气体混合器连通；
    所述电解水制氢装置包括水储罐、水输送泵、清洁能源发电设备、电解水制氢设备和氢气输送设备；
    所述水储罐通过管道和水输送泵与电解水制氢设备相连通；
    所述清洁能源发电设备与电解水制氢设备电连接，为其提供电能；
    所述电解水制氢设备通过氢气输送设备和气体混合器连通；
    所述CO2甲烷化装置包括气体混合器、换热器、多级移热式超重力反应器和第三冷凝器；
    所述气体混合器、换热器、多级移热式超重力反应器和第三冷凝器依次连通；所述第三冷凝器的出口分为两个分支；第一分支气相通向天然气冷凝干燥设备和天然气加压液化设备后通过天然气输送管网输送至外界用户；第二分支液相通过管道通向连接水储罐和水输送泵的管道上。
  2. 根据权利要求1所述零碳排放的海洋液化天然气生产系统装置，其特征在于：所述多级移热式超重力反应器包括电机、壳体、转子、换热部件、换热介质进口、反应物料进口、动密封、换热介质出口、生成物料出口；优选地，所述第一低温精馏设备和第二低温精馏设备选自能强化气液传质的旋转式精馏分离设备。
  3. 根据权利要求1所述零碳排放的海洋液化天然气生产系统装置，其特征在于：所述第一低温精馏设备的操作温度为-100～50℃、操作压力为0.1～10MPa；所述第二低温精馏设备107的操作温度为-180～-50℃、操作压力为0.1～10MPa。
  4. 根据权利要求1所述零碳排放的海洋液化天然气生产系统装置，其特征在于：所述多级移热式超重力反应器内部从下至上依次是转动的反应模块和固定的移热模块，反应模块和换热模块的层数为1-10层，优选地，反应模块和换热模块的层数为2-6层；转子内装载的是用于催化CO2甲烷化的催化剂，催化剂的装填类型是规整装填类型或散装类型。
  5. 根据权利要求1所述零碳排放的海洋液化天然气生产系统装置，其特征在于：多级移热式超重力反应器的反应转子区域内的温度为150～500℃、反应压力为0.1～10MPa，优选地，转子区域内的温度为250～400℃、反应压力为0.1～2MPa。
  6. 根据权利要求1所述零碳排放的海洋液化天然气生产系统装置，其特征在于：多级移热式超重力反应器内转子转速为100～3000r/min，优选地，转速范围为500～1500r/min。
  7. 根据权利要求1所述零碳排放的海洋液化天然气生产系统装置，其特征在于：所述清洁能源发电设备为太阳能光伏发电设备、风能发电设备、海洋天然气平台上其他剩余能源发电设备中的一种或多种。
  8. 根据权利要求1所述零碳排放的海洋液化天然气生产系统装置，其特征在于：所述电解水制氢装置原料水的来源为海水、淡化海水、第三冷凝器分离出的水中的一种或几种组合。
  9. 根据权利要求1所述零碳排放的海洋液化天然气生产系统装置，其特征在于：所述电解水制氢设备为碱性电解槽、质子交换膜电解槽、高温固体氧化物水电解槽或固体聚合物阴离子交换膜电解槽中的一种。
  10. 一种利用上述权利要求1～9中任一所述系统装置生产海洋液化天然气的方法，其特征在于，包括以下步骤：
    S1、经预处理后主要含CH4、CO2、N2的天然气原料由管道输送至海洋天然气储罐，再通过第一原料输送泵和第一冷凝器部分冷凝后输送至第一低温精馏设备中，第一低温精馏设备塔顶分离出CH4和N2、塔底分离得到高纯度的CO2；
    S2、由第一低温精馏设备塔顶采出的CH4和N2，经过第二原料输送泵和第二冷凝器进行冷凝后，输送至第二低温精馏设备中，第二低温精馏设备塔顶采出N2排空，塔底分离出高纯度CH4，进一步经天然气冷凝干燥设备进行冷凝干燥、天然气加压液化设备进行加压液化后输送至外界天然气输运管网中；
    S3、由清洁能源发电设备提供电能的电解水制氢设备制取出高纯度氢气；
    S4、由所述第一低温精馏设备塔底分离得到高纯度CO2和电解水制氢设备制取的H2，在气体混合器内按比例进行混合，然后经过换热器预热后，进入到多级移热式超重力反应器中；在多级移热式超重力反应器中交替依次经过转动的反应模块和固定的移热模块，分别进行CO2甲烷化反应和热量交换，最后产物经过第三冷凝器进行冷凝得到符合要求的天然气，进一步经天然气冷凝干燥设备进行冷凝干燥、天然气加压液化设备进行加压液化后输送至外界天然气输运管网中。
PCT/CN2024/136588 2023-12-15 2024-12-04 一种零碳排放的海洋液化天然气生产系统装置及其方法 Pending WO2025124239A1 (zh)

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