WO2022135515A1 - Hydrogen liquefaction system having ortho-parahydrogen conversion function - Google Patents
Hydrogen liquefaction system having ortho-parahydrogen conversion function Download PDFInfo
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- 239000001257 hydrogen Substances 0.000 title claims abstract description 172
- 229910052739 hydrogen Inorganic materials 0.000 title claims abstract description 172
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 title claims abstract description 147
- 238000006243 chemical reaction Methods 0.000 title claims abstract description 45
- 150000002431 hydrogen Chemical class 0.000 claims abstract description 40
- 239000003054 catalyst Substances 0.000 claims abstract description 37
- 239000007788 liquid Substances 0.000 claims abstract description 21
- 239000003507 refrigerant Substances 0.000 claims abstract description 15
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 claims abstract description 8
- ATUOYWHBWRKTHZ-UHFFFAOYSA-N Propane Chemical compound CCC ATUOYWHBWRKTHZ-UHFFFAOYSA-N 0.000 claims abstract description 8
- 229910052757 nitrogen Inorganic materials 0.000 claims abstract description 4
- 239000001294 propane Substances 0.000 claims abstract description 4
- XEEYBQQBJWHFJM-UHFFFAOYSA-N iron Substances [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 claims description 26
- 230000005540 biological transmission Effects 0.000 claims description 20
- 229910052742 iron Inorganic materials 0.000 claims description 10
- 239000010410 layer Substances 0.000 claims description 6
- 238000001914 filtration Methods 0.000 claims description 4
- 125000004435 hydrogen atom Chemical group [H]* 0.000 claims description 4
- 239000002245 particle Substances 0.000 claims description 4
- 239000011229 interlayer Substances 0.000 claims description 3
- 239000004576 sand Substances 0.000 claims description 3
- 238000007599 discharging Methods 0.000 abstract 2
- 238000010586 diagram Methods 0.000 description 4
- 239000012535 impurity Substances 0.000 description 4
- JEIPFZHSYJVQDO-UHFFFAOYSA-N iron(III) oxide Inorganic materials O=[Fe]O[Fe]=O JEIPFZHSYJVQDO-UHFFFAOYSA-N 0.000 description 4
- 238000000034 method Methods 0.000 description 4
- 238000009413 insulation Methods 0.000 description 3
- 230000009286 beneficial effect Effects 0.000 description 2
- 238000004140 cleaning Methods 0.000 description 2
- 238000006555 catalytic reaction Methods 0.000 description 1
- 238000004891 communication Methods 0.000 description 1
- 238000001816 cooling Methods 0.000 description 1
- 230000007423 decrease Effects 0.000 description 1
- 230000001419 dependent effect Effects 0.000 description 1
- 230000001066 destructive effect Effects 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 238000005265 energy consumption Methods 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 238000001704 evaporation Methods 0.000 description 1
- 230000008020 evaporation Effects 0.000 description 1
- 230000005283 ground state Effects 0.000 description 1
- 239000000203 mixture Substances 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 238000007789 sealing Methods 0.000 description 1
- 230000002269 spontaneous effect Effects 0.000 description 1
- 238000009834 vaporization Methods 0.000 description 1
- 230000008016 vaporization Effects 0.000 description 1
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- F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
- F25—REFRIGERATION OR COOLING; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS; MANUFACTURE OR STORAGE OF ICE; LIQUEFACTION SOLIDIFICATION OF GASES
- F25J—LIQUEFACTION, SOLIDIFICATION OR SEPARATION OF GASES OR GASEOUS OR LIQUEFIED GASEOUS MIXTURES BY PRESSURE AND COLD TREATMENT OR BY BRINGING THEM INTO THE SUPERCRITICAL STATE
- F25J1/00—Processes or apparatus for liquefying or solidifying gases or gaseous mixtures
- F25J1/02—Processes or apparatus for liquefying or solidifying gases or gaseous mixtures requiring the use of refrigeration, e.g. of helium or hydrogen ; Details and kind of the refrigeration system used; Integration with other units or processes; Controlling aspects of the process
- F25J1/0228—Coupling of the liquefaction unit to other units or processes, so-called integrated processes
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- F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
- F25—REFRIGERATION OR COOLING; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS; MANUFACTURE OR STORAGE OF ICE; LIQUEFACTION SOLIDIFICATION OF GASES
- F25J—LIQUEFACTION, SOLIDIFICATION OR SEPARATION OF GASES OR GASEOUS OR LIQUEFIED GASEOUS MIXTURES BY PRESSURE AND COLD TREATMENT OR BY BRINGING THEM INTO THE SUPERCRITICAL STATE
- F25J1/00—Processes or apparatus for liquefying or solidifying gases or gaseous mixtures
- F25J1/0002—Processes or apparatus for liquefying or solidifying gases or gaseous mixtures characterised by the fluid to be liquefied
- F25J1/0005—Light or noble gases
- F25J1/001—Hydrogen
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- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B3/00—Hydrogen; Gaseous mixtures containing hydrogen; Separation of hydrogen from mixtures containing it; Purification of hydrogen
- C01B3/0089—Ortho-para conversion
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- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B4/00—Hydrogen isotopes; Inorganic compounds thereof prepared by isotope exchange, e.g. NH3 + D2 → NH2D + HD
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- F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
- F16—ENGINEERING ELEMENTS AND UNITS; GENERAL MEASURES FOR PRODUCING AND MAINTAINING EFFECTIVE FUNCTIONING OF MACHINES OR INSTALLATIONS; THERMAL INSULATION IN GENERAL
- F16L—PIPES; JOINTS OR FITTINGS FOR PIPES; SUPPORTS FOR PIPES, CABLES OR PROTECTIVE TUBING; MEANS FOR THERMAL INSULATION IN GENERAL
- F16L55/00—Devices or appurtenances for use in, or in connection with, pipes or pipe systems
- F16L55/24—Preventing accumulation of dirt or other matter in the pipes, e.g. by traps, by strainers
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- F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
- F25—REFRIGERATION OR COOLING; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS; MANUFACTURE OR STORAGE OF ICE; LIQUEFACTION SOLIDIFICATION OF GASES
- F25J—LIQUEFACTION, SOLIDIFICATION OR SEPARATION OF GASES OR GASEOUS OR LIQUEFIED GASEOUS MIXTURES BY PRESSURE AND COLD TREATMENT OR BY BRINGING THEM INTO THE SUPERCRITICAL STATE
- F25J1/00—Processes or apparatus for liquefying or solidifying gases or gaseous mixtures
- F25J1/006—Processes or apparatus for liquefying or solidifying gases or gaseous mixtures characterised by the refrigerant fluid used
- F25J1/007—Primary atmospheric gases, mixtures thereof
- F25J1/0072—Nitrogen
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- F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
- F25—REFRIGERATION OR COOLING; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS; MANUFACTURE OR STORAGE OF ICE; LIQUEFACTION SOLIDIFICATION OF GASES
- F25J—LIQUEFACTION, SOLIDIFICATION OR SEPARATION OF GASES OR GASEOUS OR LIQUEFIED GASEOUS MIXTURES BY PRESSURE AND COLD TREATMENT OR BY BRINGING THEM INTO THE SUPERCRITICAL STATE
- F25J1/00—Processes or apparatus for liquefying or solidifying gases or gaseous mixtures
- F25J1/006—Processes or apparatus for liquefying or solidifying gases or gaseous mixtures characterised by the refrigerant fluid used
- F25J1/008—Hydrocarbons
- F25J1/0087—Propane; Propylene
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- F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
- F25—REFRIGERATION OR COOLING; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS; MANUFACTURE OR STORAGE OF ICE; LIQUEFACTION SOLIDIFICATION OF GASES
- F25J—LIQUEFACTION, SOLIDIFICATION OR SEPARATION OF GASES OR GASEOUS OR LIQUEFIED GASEOUS MIXTURES BY PRESSURE AND COLD TREATMENT OR BY BRINGING THEM INTO THE SUPERCRITICAL STATE
- F25J1/00—Processes or apparatus for liquefying or solidifying gases or gaseous mixtures
- F25J1/02—Processes or apparatus for liquefying or solidifying gases or gaseous mixtures requiring the use of refrigeration, e.g. of helium or hydrogen ; Details and kind of the refrigeration system used; Integration with other units or processes; Controlling aspects of the process
- F25J1/0221—Processes or apparatus for liquefying or solidifying gases or gaseous mixtures requiring the use of refrigeration, e.g. of helium or hydrogen ; Details and kind of the refrigeration system used; Integration with other units or processes; Controlling aspects of the process using the cold stored in an external cryogenic component in an open refrigeration loop
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- F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
- F25—REFRIGERATION OR COOLING; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS; MANUFACTURE OR STORAGE OF ICE; LIQUEFACTION SOLIDIFICATION OF GASES
- F25J—LIQUEFACTION, SOLIDIFICATION OR SEPARATION OF GASES OR GASEOUS OR LIQUEFIED GASEOUS MIXTURES BY PRESSURE AND COLD TREATMENT OR BY BRINGING THEM INTO THE SUPERCRITICAL STATE
- F25J1/00—Processes or apparatus for liquefying or solidifying gases or gaseous mixtures
- F25J1/02—Processes or apparatus for liquefying or solidifying gases or gaseous mixtures requiring the use of refrigeration, e.g. of helium or hydrogen ; Details and kind of the refrigeration system used; Integration with other units or processes; Controlling aspects of the process
- F25J1/0243—Start-up or control of the process; Details of the apparatus used; Details of the refrigerant compression system used
- F25J1/0257—Construction and layout of liquefaction equipments, e.g. valves, machines
- F25J1/0262—Details of the cold heat exchange system
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- F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
- F25—REFRIGERATION OR COOLING; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS; MANUFACTURE OR STORAGE OF ICE; LIQUEFACTION SOLIDIFICATION OF GASES
- F25J—LIQUEFACTION, SOLIDIFICATION OR SEPARATION OF GASES OR GASEOUS OR LIQUEFIED GASEOUS MIXTURES BY PRESSURE AND COLD TREATMENT OR BY BRINGING THEM INTO THE SUPERCRITICAL STATE
- F25J2205/00—Processes or apparatus using other separation and/or other processing means
- F25J2205/84—Processes or apparatus using other separation and/or other processing means using filter
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- F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
- F25—REFRIGERATION OR COOLING; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS; MANUFACTURE OR STORAGE OF ICE; LIQUEFACTION SOLIDIFICATION OF GASES
- F25J—LIQUEFACTION, SOLIDIFICATION OR SEPARATION OF GASES OR GASEOUS OR LIQUEFIED GASEOUS MIXTURES BY PRESSURE AND COLD TREATMENT OR BY BRINGING THEM INTO THE SUPERCRITICAL STATE
- F25J2210/00—Processes characterised by the type or other details of the feed stream
- F25J2210/42—Nitrogen
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- F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
- F25—REFRIGERATION OR COOLING; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS; MANUFACTURE OR STORAGE OF ICE; LIQUEFACTION SOLIDIFICATION OF GASES
- F25J—LIQUEFACTION, SOLIDIFICATION OR SEPARATION OF GASES OR GASEOUS OR LIQUEFIED GASEOUS MIXTURES BY PRESSURE AND COLD TREATMENT OR BY BRINGING THEM INTO THE SUPERCRITICAL STATE
- F25J2220/00—Processes or apparatus involving steps for the removal of impurities
- F25J2220/02—Separating impurities in general from the feed stream
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- General Engineering & Computer Science (AREA)
- Mechanical Engineering (AREA)
- Thermal Sciences (AREA)
- Physics & Mathematics (AREA)
- Chemical & Material Sciences (AREA)
- Organic Chemistry (AREA)
- Inorganic Chemistry (AREA)
- Combustion & Propulsion (AREA)
- Health & Medical Sciences (AREA)
- General Health & Medical Sciences (AREA)
- Separation By Low-Temperature Treatments (AREA)
- Hydrogen, Water And Hydrids (AREA)
Abstract
The present invention discloses a hydrogen liquefaction system having an ortho-parahydrogen conversion function, composed of seven hydrogen liquefaction cold boxes which are arranged in series. The structure of each hydrogen liquefaction cold box comprises a housing composed of an inner housing and an outer housing; the housing is internally provided with a spiral heat exchange pipe used for conveying a hydrogen liquefaction refrigerant, a first hydrogen conveying pipeline and a second hydrogen conveying pipeline that are used for conveying hydrogen/liquid hydrogen, and a catalyst feeding pipe and a catalyst discharging pipe that are used for filling or discharging an ortho-parahydrogen conversion catalyst into or out of the inner housing; pipeline filter nozzles are respectively provided in the first hydrogen conveying pipeline and the second hydrogen conveying pipeline; and the hydrogen liquefaction refrigerant arranged in the first hydrogen liquefaction cold box is liquefied propane, and the hydrogen liquefaction refrigerants arranged in the second hydrogen liquefaction cold box to the seventh hydrogen liquefaction cold box are all liquid nitrogen. The system can complete ortho-state and para-state conversion of hydrogen/liquid hydrogen while performing hydrogen liquefaction, and ensures that parahydrogen accounts for more than 95% while performing hydrogen liquefaction.
Description
本发明涉及氢液化技术，尤其涉及一种带正–仲氢转化的氢液化系统。The present invention relates to hydrogen liquefaction technology, in particular to a hydrogen liquefaction system with normal-parahydrogen conversion.
通常情况下氢是正氢和仲氢的混合物，正仲氢之间的平衡百分比与温度有关。室温下，氢气大约是由75％正氢和25％仲氢组成，随着温度的降低，具有高能量基态的正氢自发地向低能态的仲氢转化，从而使仲氢浓度不断升高：在77K时正氢含量为51％，仲氢含量为49％，20K时仲氢含量高达99.8％。Typically hydrogen is a mixture of ortho and para hydrogen, and the equilibrium percentage between ortho and para hydrogen is temperature dependent. At room temperature, hydrogen consists of approximately 75% orthohydrogen and 25% parahydrogen. As the temperature decreases, orthohydrogen with a high-energy ground state spontaneously converts to a low-energy state parahydrogen, thereby increasing the parahydrogen concentration: At 77K, the ortho-hydrogen content is 51%, the para-hydrogen content is 49%, and the para-hydrogen content is as high as 99.8% at 20K.
当直接将室温下的氢气液化时，得到的液氢处于非平衡状态，正氢会自发地向仲氢转化，而这个过程是一个放热过程；由于正仲氢转化放出的热量大于液态氢的汽化潜热，因此不论液氢储罐绝热性能多好，都会存在液氢蒸发，有研究表明液氢储存的第一天就蒸发了总储量的18％以上，导致液氢储罐的内压力增加，使得液氢储运存在重大挑战。为了减少氢液化时的损失以及再液化的能耗，尽可能延长液氢无损储存的时间，必须在氢液化的同时完成氢气/液氢正-仲态的转化、并确保氢液化的同时仲氢占比超过95％。因而急需研发一种在氢液化的同时完成氢气/液氢正-仲态的转化、并确保氢液化的同时仲氢占比超过95％的设备。When the hydrogen at room temperature is directly liquefied, the obtained liquid hydrogen is in a non-equilibrium state, and ortho-hydrogen will spontaneously convert to para-hydrogen, and this process is an exothermic process; since the heat released by the conversion of normal-para-hydrogen is greater than that of liquid hydrogen Because of the latent heat of vaporization, no matter how good the thermal insulation performance of the liquid hydrogen storage tank is, there will be liquid hydrogen evaporation. Some studies have shown that more than 18% of the total reserves of liquid hydrogen are evaporated on the first day of storage, resulting in an increase in the internal pressure of the liquid hydrogen storage tank. This makes liquid hydrogen storage and transportation a major challenge. In order to reduce the loss of hydrogen liquefaction and the energy consumption of reliquefaction, and to extend the time of non-destructive storage of liquid hydrogen as much as possible, it is necessary to complete the conversion of hydrogen/liquid hydrogen normal-parallel state at the same time as hydrogen liquefaction, and ensure that parahydrogen is liquefied at the same time. accounted for more than 95%. Therefore, there is an urgent need to develop a device that can complete the conversion of hydrogen/liquid hydrogen to the normal-parallel state at the same time as hydrogen liquefaction, and ensure that the parahydrogen accounts for more than 95% during hydrogen liquefaction.
发明内容SUMMARY OF THE INVENTION
本发明所需解决的技术问题是：提供一种在氢液化的同时完成氢气/液氢正-仲态的转化、并确保氢液化的同时仲氢占比超过95％的带正–仲氢转化的氢液化系统。The technical problem to be solved by the present invention is: to provide a normal-parahydrogen conversion with a normal-parahydrogen conversion in which the hydrogen/liquid hydrogen normal-parahydrogen is completed while the hydrogen is liquefied, and the parahydrogen accounts for more than 95% while the hydrogen is liquefied. hydrogen liquefaction system.
为解决上述问题，本发明采用的技术方案是：所述的一种带正–仲氢转化的氢液化系统，包括：七个顺序排列串联的氢液化冷箱；每个氢液化冷箱的结构包括：前后横卧放置的壳体，所述的壳体为由内壳体和外壳体构成的双层绝热回转壳体；在内壳体中设置有沿壳体轴线由前向后呈螺旋状盘旋的换热管，换热管的进口端密封穿过壳体前部的第一通孔后伸出外壳体外，换热管的出口端密封穿过壳体后部的第二通孔后伸出外壳体外，氢液化制冷剂从 换热管的进口端进入换热管中，然后从换热管的出口端排出；第一输氢管道的出口端密封穿过壳体前部的第三通孔后伸入内壳体中，第二输氢管道的进口端密封穿过壳体后部的第四通孔后伸入内壳体中，在第一输氢管道和第二输氢管道中分别设置有管道过滤嘴；催化剂进料管的出口端密封穿过壳体顶部的第五通孔后伸入内壳体中，催化剂出料管的进口端密封穿过壳体底部的第六通孔后伸入内壳体中，正仲氢转化催化剂通过催化剂进料管进入并充满于内壳体中；排列于后位的氢液化冷箱的第一输氢管道的进口端与排列于该氢液化冷箱相邻前位的氢液化冷箱的第二输氢管道的出口端密封连通；排列于第一位的氢液化冷箱中的氢液化制冷剂为液化丙烷，排列于第二位至第七位的氢液化冷箱中的氢液化制冷剂均为液氮。In order to solve the above problems, the technical solution adopted in the present invention is: the described hydrogen liquefaction system with normal-parahydrogen conversion, comprising: seven hydrogen liquefaction cold boxes arranged in series in sequence; the structure of each hydrogen liquefaction cold box It includes: a shell placed horizontally before and after, the shell is a double-layer heat-insulating rotary shell composed of an inner shell and an outer shell; the inner shell is provided with a spiral shape from front to back along the axis of the shell. The coiled heat exchange tube, the inlet end of the heat exchange tube is sealed through the first through hole at the front of the shell and then extends out of the outer shell, and the outlet end of the heat exchange tube is sealed through the second through hole at the rear of the shell and extends back Out of the outer shell, the hydrogen liquefied refrigerant enters the heat exchange tube from the inlet end of the heat exchange tube, and then is discharged from the outlet end of the heat exchange tube; the outlet end of the first hydrogen transmission pipeline is sealed through the third passage at the front of the shell. The hole extends into the inner shell, and the inlet end of the second hydrogen pipeline is sealed through the fourth through hole at the rear of the shell and then protrudes into the inner shell. In the first hydrogen pipeline and the second hydrogen pipeline Pipe filters are respectively provided; the outlet end of the catalyst feed pipe is sealed through the fifth through hole at the top of the casing and then protrudes into the inner casing, and the inlet end of the catalyst discharge pipe is sealed through the sixth through hole at the bottom of the casing It extends into the inner shell, and the normal and parahydrogen conversion catalyst enters and fills the inner shell through the catalyst feed pipe; The outlet ends of the second hydrogen pipelines of the hydrogen liquefaction cold box adjacent to the front position of the liquefaction cold box are sealed and connected; the hydrogen liquefaction refrigerant in the hydrogen liquefaction cold box arranged in the first position is liquefied propane, which is arranged in the second position The hydrogen liquefied refrigerant in the seventh hydrogen liquefied cold box is all liquid nitrogen.
进一步地，前述的一种带正–仲氢转化的氢液化系统，其中，所述的正仲氢转化催化剂为Fe
2O
3铁基催化剂，Fe
2O
3铁基催化剂的颗粒度为15～17微米；管道过滤嘴上的过滤滤芯的过滤精度不超过15微米。
Further, in the aforementioned hydrogen liquefaction system with normal-parahydrogen conversion, the normal-parahydrogen conversion catalyst is an Fe 2 O 3 iron-based catalyst, and the particle size of the Fe 2 O 3 iron-based catalyst is 15~ 17 microns; the filter element on the pipe filter has a filtration accuracy of no more than 15 microns.
进一步地，前述的一种带正–仲氢转化的氢液化系统，其中，管道过滤嘴上的过滤滤芯为SS316L五层烧结网。Further, in the aforementioned hydrogen liquefaction system with normal-parahydrogen conversion, the filter element on the pipe filter is SS316L five-layer sintered mesh.
进一步地，前述的一种带正–仲氢转化的氢液化系统，其中，管道过滤嘴由圆筒状底座和设置于圆筒状底座上的过滤滤芯构成，在圆筒状底座的外圆周面上设置有外螺纹段，在第一输氢管道和第二输氢管道中分别设置与外螺纹段匹配的内螺纹段，二个管道过滤嘴通过外螺纹段分别密封旋于对应第一输氢管道和第二输氢管道中。Further, the aforementioned hydrogen liquefaction system with normal-parahydrogen conversion, wherein, the pipeline filter is composed of a cylindrical base and a filter element arranged on the cylindrical base, on the outer circumferential surface of the cylindrical base. An external thread segment is provided, and an internal thread segment matching the external thread segment is respectively set in the first hydrogen transmission pipeline and the second hydrogen transmission pipeline, and the two pipeline filters are respectively sealed and screwed to the corresponding first hydrogen transmission pipeline and in the second hydrogen pipeline.
进一步地，前述的一种带正–仲氢转化的氢液化系统，其中，在内壳体与外壳体之间的中空夹层中填充满珠光砂。Further, in the aforementioned hydrogen liquefaction system with normal-parahydrogen conversion, the hollow interlayer between the inner shell and the outer shell is filled with pearlescent sand.
进一步地，前述的一种带正–仲氢转化的氢液化系统，其中，第一输氢管道和第二输氢管道的介质工作压力为0～3.5MPa，工作温度为20K～440K。Further, in the aforementioned hydrogen liquefaction system with normal-para-hydrogen conversion, the medium working pressure of the first hydrogen transport pipeline and the second hydrogen transport pipeline is 0-3.5MPa, and the working temperature is 20K-440K.
本发明的有益效果是：①该带正–仲氢转化的氢液化系统能在氢液化的同时完成氢气/液氢正-仲态的转化、并确保氢液化的同时仲氢占比超过95％；②各氢液化冷箱的结构简单、 紧凑，操作方便，可重复拆卸清理后使用；③管道过滤嘴的具体设计既能阻挡正仲氢转化催化剂、避免正仲氢转化催化剂的流失，又能过滤氢气中的杂质，避免氢气中的杂质堵塞管道。The beneficial effects of the present invention are: (1) The hydrogen liquefaction system with normal-parahydrogen conversion can complete the conversion of hydrogen/liquid hydrogen normal-parahydrogen state at the same time of hydrogen liquefaction, and ensure that the proportion of parahydrogen exceeds 95% while the hydrogen is liquefied ; ② The structure of each hydrogen liquefaction cold box is simple, compact, easy to operate, and can be used after repeated disassembly and cleaning; ③ The specific design of the pipe filter can not only block the normal-parahydrogen conversion catalyst, avoid the loss of the normal-parahydrogen conversion catalyst, but also filter Impurities in hydrogen to avoid impurities in hydrogen from clogging the pipeline.
图1是本发明所述的一种带正–仲氢转化的氢液化系统的结构示意图。FIG. 1 is a schematic structural diagram of a hydrogen liquefaction system with normal-parahydrogen conversion according to the present invention.
图2是图1中单个氢液化冷箱的结构示意图。FIG. 2 is a schematic structural diagram of a single hydrogen liquefaction cold box in FIG. 1 .
图3是图2中管道过滤嘴的结构示意图。FIG. 3 is a schematic structural diagram of the pipe filter in FIG. 2 .
图4是氢液化冷箱的另一种结构示意图。Fig. 4 is another structural schematic diagram of a hydrogen liquefaction cold box.
下面结合附图及优选实施例对本发明所述的技术方案作进一步详细的说明。The technical solutions of the present invention will be described in further detail below with reference to the accompanying drawings and preferred embodiments.
如图1、图2和图4所示，本实施例中所述的一种带正–仲氢转化的氢液化系统，包括：七个顺序排列串联的氢液化冷箱100。每个氢液化冷箱100的结构包括：前后横卧放置的壳体，所述的壳体为由内壳体2和外壳体1构成的双层绝热回转壳体。在内壳体2与外壳体1之间的中空夹层9中填充满珠光砂，用于绝热，以减少冷量损失。在内壳体2中设置有沿壳体轴线由前向后呈螺旋状盘旋的换热管3，换热管的进口端31密封穿过壳体前部的第一通孔后伸出外壳体1外，换热管的出口端32密封穿过壳体后部的第二通孔后伸出外壳体1外。在正常使用过程中，氢液化制冷剂从换热管的进口端31进入换热管3中，然后从换热管的出口端32排出。As shown in FIG. 1 , FIG. 2 and FIG. 4 , a hydrogen liquefaction system with normal-para hydrogen conversion described in this embodiment includes: seven hydrogen liquefaction cold boxes 100 arranged in series in sequence. The structure of each hydrogen liquefaction cold box 100 includes: front and rear casings lying horizontally, and the casing is a double-layer thermal insulation rotary casing composed of an inner casing 2 and an outer casing 1 . The hollow interlayer 9 between the inner shell 2 and the outer shell 1 is filled with pearlescent sand for heat insulation to reduce cooling loss. The inner shell 2 is provided with a heat exchange tube 3 spirally spiraling from front to back along the axis of the shell. 1, the outlet end 32 of the heat exchange tube is sealed through the second through hole at the rear of the casing and then protrudes out of the outer casing 1. During normal use, the hydrogen liquefied refrigerant enters the heat exchange tube 3 from the inlet end 31 of the heat exchange tube, and is then discharged from the outlet end 32 of the heat exchange tube.
如图2和图4所示，第一输氢管道4的出口端密封穿过壳体前部的第三通孔后伸入内壳体2中，第二输氢管道5的进口端密封穿过壳体后部的第四通孔后伸入内壳体2中，在第一输氢管道4和第二输氢管道5中分别设置有管道过滤嘴8。在正常使用过程中，氢气从第一输氢管道4的进口端进入第一输氢管道4中，进而进入内壳体2中，然后通过第二输氢管道5的进口端进入第二输氢管道5中，进而从第二输氢管道5的出口端输出。As shown in Figures 2 and 4, the outlet end of the first hydrogen transmission pipeline 4 is sealed through the third through hole at the front of the casing and then protrudes into the inner casing 2, and the inlet end of the second hydrogen transmission pipeline 5 is sealed through the inner casing 2. After passing through the fourth through hole at the rear of the casing, it extends into the inner casing 2 , and pipeline filters 8 are respectively arranged in the first hydrogen transport pipeline 4 and the second hydrogen transport pipeline 5 . During normal use, hydrogen enters the first hydrogen transmission pipeline 4 from the inlet end of the first hydrogen transmission pipeline 4 , then enters the inner shell 2 , and then enters the second hydrogen transmission pipeline through the inlet end of the second hydrogen transmission pipeline 5 . Pipeline 5, and then output from the outlet end of the second hydrogen pipeline 5.
七个顺序排列串联的氢液化冷箱100的串联方式为：排列于后位的氢液化冷箱的第一输氢管道的进口端与排列于该氢液化冷箱相邻前位的氢液化冷箱的第二输氢管道的出口端密 封连通。The series connection mode of seven hydrogen liquefaction cold boxes 100 arranged in series is: the inlet end of the first hydrogen transport pipeline of the hydrogen liquefaction cold box arranged in the rear position and the hydrogen liquefaction cold box arranged in the adjacent front position of the hydrogen liquefaction cold box. The outlet end of the second hydrogen transport pipeline of the tank is in sealed communication.
第一输氢管道4和第二输氢管道5的介质工作压力为0～3.5MPa，工作温度为20K～440K。The medium working pressure of the first hydrogen transport pipeline 4 and the second hydrogen transport pipeline 5 is 0-3.5MPa, and the working temperature is 20K-440K.
正仲氢自发转化是一个极其慢的过程，因此需采用催化剂加快正氢向仲氢的转化速率。本实施例中，如图2和图4所示，催化剂进料管6的出口端密封穿过壳体顶部的第五通孔后伸入内壳体2中，催化剂出料管7的进口端密封穿过壳体底部的第六通孔后伸入内壳体2中，正仲氢转化催化剂10通过催化剂进料管6进入并充满于内壳体2中。在正常使用过程中，催化剂进料管6的进口端、催化剂出料管7的出口端均处于常闭状态，在需要补充或更换正仲氢转化催化剂10时，通过催化剂进料管6、催化剂出料管7进行相应操作。The spontaneous conversion of ortho-parahydrogen is an extremely slow process, so a catalyst is required to accelerate the conversion rate of ortho- to para-hydrogen. In this embodiment, as shown in FIGS. 2 and 4 , the outlet end of the catalyst feed pipe 6 is sealed through the fifth through hole at the top of the casing and then protrudes into the inner casing 2 , and the inlet end of the catalyst discharge pipe 7 After sealing through the sixth through hole at the bottom of the shell, it extends into the inner shell 2 , and the normal parahydrogen conversion catalyst 10 enters and fills the inner shell 2 through the catalyst feed pipe 6 . During normal use, the inlet end of the catalyst feed pipe 6 and the outlet end of the catalyst discharge pipe 7 are in a normally closed state. The discharge pipe 7 is operated accordingly.
本实施例中，所述的正仲氢转化催化剂10采用Fe
2O
3铁基催化剂，Fe
2O
3铁基催化剂具有催化反应速率快、成本低、安全性能好、可重复使用等优点。Fe2O3铁基催化剂颗粒越小，氢原子与催化剂的接触面积越大，转化效果越好，本实施例中Fe
2O
3铁基催化剂的颗粒度为15～17微米。管道过滤嘴8上的过滤滤芯83的过滤精度不超过15微米。
In this embodiment, the normal and parahydrogen conversion catalyst 10 adopts Fe 2 O 3 iron-based catalyst, and the Fe 2 O 3 iron-based catalyst has the advantages of fast catalytic reaction rate, low cost, good safety performance, and reusability. The smaller the Fe2O3 iron-based catalyst particles, the larger the contact area between hydrogen atoms and the catalyst, and the better the conversion effect. In this embodiment, the particle size of the Fe2O3 iron-based catalyst is 15-17 microns. The filtering precision of the filter element 83 on the pipe filter 8 is not more than 15 microns.
如图3所示，本实施例中，管道过滤嘴8由圆筒状底座81和设置于圆筒状底座81上的过滤滤芯83构成，过滤滤芯83采用SS316L五层烧结网。在圆筒状底座81的外圆周面上设置有外螺纹段82，在第一输氢管道4和第二输氢管道5中分别设置与外螺纹段82匹配的内螺纹段，二个管道过滤嘴8通过外螺纹段82分别密封旋于对应第一输氢管道4和第二输氢管道5中。氢气从第一输氢管道4的进口端进入第一输氢管道4中，经第一输氢管道4中的管道过滤嘴8过滤后进入内壳体2中，然后通过第二输氢管道5的进口端进入第二输氢管道5中，经第二输氢管道5中的管道过滤嘴8过滤后从第二输氢管道5的出口端输出。As shown in FIG. 3 , in this embodiment, the pipe filter 8 is composed of a cylindrical base 81 and a filter element 83 arranged on the cylindrical base 81 , and the filter element 83 adopts SS316L five-layer sintered mesh. An external thread segment 82 is provided on the outer circumferential surface of the cylindrical base 81, an internal thread segment matching the external thread segment 82 is respectively provided in the first hydrogen transmission pipeline 4 and the second hydrogen transmission pipeline 5, and two pipeline filters 8 are respectively sealed and screwed into the corresponding first hydrogen transmission pipeline 4 and the second hydrogen transmission pipeline 5 through the external thread section 82 . The hydrogen enters the first hydrogen transmission pipeline 4 from the inlet end of the first hydrogen transmission pipeline 4, is filtered by the pipeline filter 8 in the first hydrogen transmission pipeline 4 and enters the inner shell 2, and then passes through the second hydrogen transmission pipeline 5. The inlet end enters the second hydrogen transportation pipeline 5 , and is filtered by the pipeline filter 8 in the second hydrogen transportation pipeline 5 , and then output from the outlet end of the second hydrogen transportation pipeline 5 .
单个氢液化冷箱100的工作原理为：氢液化制冷剂从换热管的进口端31进入换热管3中，与正仲氢转化催化剂10或氢气进行间接热交换，吸收正–仲氢转化的放热量、同时将氢气液化后从换热管的出口端32排出。氢气从第一输氢管道4的进口端进入内壳体2中，氢原 子与内壳体2中充满的Fe
2O
3铁基催化剂接触，Fe2O3铁基催化剂的非均匀磁场使得原本自旋方向一致的正氢分子旋向改变，变成自旋方向相反的仲氢分子，然后从从第二输氢管道5的出口端输出。
The working principle of a single hydrogen liquefaction cold box 100 is as follows: the hydrogen liquefied refrigerant enters the heat exchange tube 3 from the inlet end 31 of the heat exchange tube, conducts indirect heat exchange with the normal-parahydrogen conversion catalyst 10 or hydrogen, and absorbs the normal-parahydrogen conversion At the same time, the hydrogen is liquefied and discharged from the outlet end 32 of the heat exchange tube. The hydrogen enters the inner shell 2 from the inlet end of the first hydrogen pipeline 4, and the hydrogen atoms are in contact with the Fe2O3 iron-based catalyst filled in the inner shell 2. The non-uniform magnetic field of the Fe2O3 iron-based catalyst makes the original spin direction Consistent ortho-hydrogen molecules change their rotational directions to become para-hydrogen molecules with opposite spin directions, and then output from the outlet end of the second hydrogen transport pipeline 5 .
其中排于第一位的带正-仲氢转化的氢液化冷箱中的氢液化制冷剂采用液化丙烷，排列于第二位至第七位的带正-仲氢转化的氢液化冷箱中的氢液化制冷剂均采用液氮。利用7个串联的带正-仲氢转化的氢液化冷箱能够将氢气冷却至20K液氢，同时液氢中仲氢含量≥95％。Among them, the hydrogen liquefaction refrigerant in the hydrogen liquefaction cold box with n-para hydrogen conversion in the first place adopts liquefied propane, and the hydrogen liquefaction refrigerant in the hydrogen liquefaction cold box with n-para hydrogen conversion in the second to seventh places is arranged. All hydrogen liquefied refrigerants use liquid nitrogen. The hydrogen can be cooled to 20K liquid hydrogen by using 7 series-connected hydrogen liquefaction cold boxes with normal-parahydrogen conversion, and the parahydrogen content in the liquid hydrogen is greater than or equal to 95%.
以上所述仅是本发明的较佳实施例，并非是对本发明作任何其他形式的限制，而依据本发明的技术实质所作的任何修改或等同变化，仍属于本发明要求保护的范围。The above are only preferred embodiments of the present invention, and are not intended to limit the present invention in any other form, and any modifications or equivalent changes made according to the technical essence of the present invention still fall within the scope of protection of the present invention.
本发明的有益效果是：①该带正–仲氢转化的氢液化系统能在氢液化的同时完成氢气/液氢正-仲态的转化、并确保氢液化的同时仲氢占比超过95％；②各氢液化冷箱100的结构简单、紧凑，操作方便，可重复拆卸清理后使用；③管道过滤嘴8的具体设计既能阻挡正仲氢转化催化剂、避免正仲氢转化催化剂的流失，又能过滤氢气中的杂质，避免氢气中的杂质堵塞管道。The beneficial effects of the present invention are: (1) The hydrogen liquefaction system with normal-parahydrogen conversion can complete the conversion of hydrogen/liquid hydrogen normal-parahydrogen state at the same time of hydrogen liquefaction, and ensure that the proportion of parahydrogen exceeds 95% while the hydrogen is liquefied 2. The structure of each hydrogen liquefaction cold box 100 is simple, compact, easy to operate, and can be used after repeated disassembly and cleaning; 3. The specific design of the pipe filter 8 can not only block the normal-parahydrogen conversion catalyst, avoid the loss of the normal-parahydrogen conversion catalyst, but also It can filter the impurities in the hydrogen and avoid the impurities in the hydrogen to block the pipeline.
Claims (6)
- 一种带正–仲氢转化的氢液化系统，其特征在于：包括：七个顺序排列串联的氢液化冷箱；每个氢液化冷箱的结构包括：前后横卧放置的壳体，所述的壳体为由内壳体和外壳体构成的双层绝热回转壳体；在内壳体中设置有沿壳体轴线由前向后呈螺旋状盘旋的换热管，换热管的进口端密封穿过壳体前部的第一通孔后伸出外壳体外，换热管的出口端密封穿过壳体后部的第二通孔后伸出外壳体外，氢液化制冷剂从换热管的进口端进入换热管中，然后从换热管的出口端排出；第一输氢管道的出口端密封穿过壳体前部的第三通孔后伸入内壳体中，第二输氢管道的进口端密封穿过壳体后部的第四通孔后伸入内壳体中，在第一输氢管道和第二输氢管道中分别设置有管道过滤嘴；催化剂进料管的出口端密封穿过壳体顶部的第五通孔后伸入内壳体中，催化剂出料管的进口端密封穿过壳体底部的第六通孔后伸入内壳体中，正仲氢转化催化剂通过催化剂进料管进入并充满于内壳体中；排列于后位的氢液化冷箱的第一输氢管道的进口端与排列于该氢液化冷箱相邻前位的氢液化冷箱的第二输氢管道的出口端密封连通；排列于第一位的氢液化冷箱中的氢液化制冷剂为液化丙烷，排列于第二位至第七位的氢液化冷箱中的氢液化制冷剂均为液氮。A hydrogen liquefaction system with normal-para-hydrogen conversion is characterized in that: it comprises: seven hydrogen liquefaction cold boxes arranged in series in sequence; the structure of each hydrogen liquefaction cold box comprises: a shell placed horizontally in front and back; The shell is a double-layer adiabatic rotary shell composed of an inner shell and an outer shell; the inner shell is provided with a heat exchange tube spirally spiraling from front to back along the axis of the shell, and the inlet end of the heat exchange tube is arranged. The outlet end of the heat exchange tube is sealed and passes through the second through hole at the rear of the shell and then extends out of the outer shell, and the hydrogen liquefied refrigerant flows out of the heat exchange tube. The inlet end of the first hydrogen transfer pipe enters the heat exchange tube, and then is discharged from the outlet end of the heat exchange tube; the outlet end of the first hydrogen transfer pipe is sealed and protrudes into the inner shell after passing through the third through hole in the front of the shell, and the second transport pipe The inlet end of the hydrogen pipeline is sealed through the fourth through hole at the rear of the shell and then protrudes into the inner shell. Pipeline filters are respectively arranged in the first hydrogen transport pipeline and the second hydrogen transport pipeline; the outlet of the catalyst feed pipe The end seal passes through the fifth through hole at the top of the casing and then extends into the inner casing. The inlet end of the catalyst discharge pipe is sealed through the sixth through hole at the bottom of the casing and then extends into the inner casing. The catalyst enters and fills the inner shell through the catalyst feed pipe; the inlet end of the first hydrogen pipeline of the hydrogen liquefaction cold box arranged in the rear position and the hydrogen liquefaction cold box arranged in the adjacent front position of the hydrogen liquefaction cold box The outlet end of the second hydrogen pipeline is sealed and connected; the hydrogen liquefaction refrigerant in the hydrogen liquefaction cold box arranged in the first place is liquefied propane, and the hydrogen liquefaction refrigerant in the hydrogen liquefaction cold box arranged in the second to seventh places is liquefied The refrigerant is liquid nitrogen.
- 根据权利要求1所述的一种带正–仲氢转化的氢液化系统，其特征在于：所述的正仲氢转化催化剂为Fe 2O 3铁基催化剂，Fe 2O 3铁基催化剂的颗粒度为15～17微米；管道过滤嘴上的过滤滤芯的过滤精度不超过15微米。 The hydrogen liquefaction system with normal-parahydrogen conversion according to claim 1, wherein the normal-parahydrogen conversion catalyst is Fe 2 O 3 iron-based catalyst, particles of Fe 2 O 3 iron-based catalyst The degree of filtration is 15 to 17 microns; the filtration accuracy of the filter element on the pipe filter does not exceed 15 microns.
- 根据权利要求1或2所述的一种带正–仲氢转化的氢液化系统，其特征在于：管道过滤嘴上的过滤滤芯为SS316L五层烧结网。A hydrogen liquefaction system with normal-parahydrogen conversion according to claim 1 or 2, characterized in that: the filter element on the pipe filter is SS316L five-layer sintered mesh.
- 根据权利要求1或2所述的一种带正–仲氢转化的氢液化系统，其特征在于：管道过滤嘴由圆筒状底座和设置于圆筒状底座上的过滤滤芯构成，在圆筒状底座的外圆周面上设置有外螺纹段，在第一输氢管道和第二输氢管道中分别设置与外螺纹段匹配的内螺纹段，二个管道过滤嘴通过外螺纹段分别密封旋于对应第一输氢管道和第二输氢管道中。A hydrogen liquefaction system with normal-para-hydrogen conversion according to claim 1 or 2, characterized in that: the pipeline filter is composed of a cylindrical base and a filter element arranged on the cylindrical base, and the filter is in the cylindrical base. An external thread section is arranged on the outer circumferential surface of the base, and an internal thread segment matching the external thread segment is respectively set in the first hydrogen transmission pipeline and the second hydrogen transmission pipeline, and the two pipeline filters are respectively sealed and screwed to the corresponding thread through the external thread segment. in the first hydrogen pipeline and the second hydrogen pipeline.
- 根据权利要求1或2所述的一种带正–仲氢转化的氢液化系统，其特征在于：在内壳体与 外壳体之间的中空夹层中填充满珠光砂。A hydrogen liquefaction system with normal-parahydrogen conversion according to claim 1 or 2, characterized in that: the hollow interlayer between the inner shell and the outer shell is filled with pearlescent sand.
- 根据权利要求1所述的一种带正–仲氢转化的氢液化系统，其特征在于：第一输氢管道和第二输氢管道的介质工作压力为0～3.5MPa，工作温度为20K～440K。The hydrogen liquefaction system with normal-parahydrogen conversion according to claim 1, wherein the medium working pressure of the first hydrogen transport pipeline and the second hydrogen transport pipeline is 0～3.5MPa, and the working temperature is 20K～ 440K.
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