Ceramic hydrogen pump and hydrogen purification device for hydrogen-oxygen fuel cell

Through the integrated molded ceramic hydrogen pump body module, the sealing failure problem caused by the complex structure of the high-power hydrogen pump module and the poor thermal expansion behavior is solved, which improves the service life and reliability of the hydrogen pump and simplifies the structure.

CN114622231BActive Publication Date: 2024-12-31CERAMIC CELLS CO LTD
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Patent Information

Application Number
CN202210336133.0
Authority / Receiving Office
CN · China
Patent Type
Patents(China)
Current Assignee / Owner
Filing Date
2022-03-31
Publication Date
2024-12-31
Estimated Expiration
2042-03-31

AI Technical Summary

Technical Problem

The complex structure and poor thermal expansion behavior of existing high-power hydrogen pump modules lead to seal failure, affecting service life and reliability.

Method used

The integrated ceramic hydrogen pump pump module is adopted, including a positive electrode assembly, an electrolyte membrane and an anode assembly, to form a sealing structure through sintering, reducing differences in thermal expansion behavior and improving sealing and reliability.

Benefits of technology

It effectively solves the problem of sealing failure, improves the service life and reliability of the hydrogen pump module, simplifies the structure, and reduces the impact of thermal expansion deformation on reliability.

✦ Generated by Eureka AI based on patent content.

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Abstract

The present invention discloses a ceramic hydrogen pump and a hydrogen purification device for a hydrogen-oxygen fuel cell. The ceramic hydrogen pump comprises a pump body module, which comprises a positive electrode assembly, an electrolyte diaphragm and a negative electrode assembly sequentially arranged along a first direction. The positive electrode assembly dissociates hydrogen in a mixed gas to generate hydrogen ions, and the electrolyte diaphragm allows the hydrogen ions to pass through and reach the negative electrode assembly, and the negative electrode assembly reduces the hydrogen ions to generate hydrogen. In this embodiment, the positive electrode assembly, the electrolyte diaphragm and the negative electrode assembly are integrally formed, which solves the problem in the prior art that the positive electrode assembly, the electrolyte diaphragm and the negative electrode assembly have sealing failure due to different thermal expansion behaviors, thereby affecting the service life and reliability of the high-power hydrogen pump module.
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Description

Technical Field

[0001] The present invention relates to the technical field of hydrogen-oxygen fuel cells, and in particular to a ceramic hydrogen pump and a hydrogen purification device for hydrogen-oxygen fuel cells. Background Art

[0002] The membrane electrode of hydrogen-oxygen fuel cells includes a catalytic layer, a diffusion layer, and a proton exchange membrane. During the reaction process, if there are impurities in hydrogen, such as sulfides, etc., the platinum-carbon catalyst will be poisoned, which will lead to reduced catalyst activity, reduced fuel cell power, shortened life, etc. There are many ways to purify hydrogen. In the prior art, a ceramic hydrogen pump can be used to purify hydrogen. The ceramic hydrogen pump is generally composed of an electrolyte, a negative electrode, and a positive electrode, wherein the electrolyte can conduct protons. Driven by electricity, hydrogen dissociates into protons at the positive electrode and is transmitted to the negative electrode through an electrolyte diaphragm. The protons combine with external circuit electrons at the negative electrode to generate hydrogen. In order to meet the high-throughput requirements of practical applications, hydrogen pump monomers, negative electrode current collectors, positive electrode current collectors, and connectors are often packaged in series at 800-1000°C through negative electrode seals and positive electrode seals to form a high-power hydrogen pump module with a relatively complex structure. In addition, the different thermal expansion behaviors between hydrogen pump monomers, seals, and connectors increase the risk of sealing failure, affecting the service life and reliability of high-power hydrogen pump modules. Summary of the invention

[0003] The main purpose of the present invention is to propose a ceramic hydrogen pump, which aims to solve the problems of complex structure and easy failure of sealing in the prior art when using a high-power hydrogen pump module for hydrogen purification, and further improve the service life and reliability of the hydrogen pump module.

[0004] To achieve the above object, the ceramic hydrogen pump proposed by the present invention comprises:

[0005] The invention comprises a pump body module, wherein the pump body module comprises a positive electrode assembly, an electrolyte membrane and a negative electrode assembly arranged in sequence along a first direction, wherein the positive electrode assembly is used to dissociate hydrogen in a mixed gas to generate hydrogen ions, the electrolyte membrane is used to allow the hydrogen ions to pass through, and the negative electrode assembly is used to reduce the hydrogen ions to generate hydrogen, wherein the positive electrode assembly, the electrolyte membrane and the negative electrode assembly are integrally formed.

[0006] Optionally, the positive electrode assembly comprises a positive electrode connector, a positive electrode current collector and a positive electrode arranged in sequence, and the positive electrode is arranged adjacent to the electrolyte separator;

[0007] The negative electrode assembly comprises a negative electrode connector, a negative electrode current collector and a negative electrode arranged in sequence, and the negative electrode is arranged adjacent to the electrolyte membrane;

[0008] The positive electrode connector, the positive electrode current collector, the positive electrode, the electrolyte film, the negative electrode, the negative electrode, the negative electrode current collector and the negative electrode connector are sintered into one body.

[0009] Optionally, the positive electrode and / or the negative electrode are made of a material including metal, alloy, electronic conductive oxide and oxygen ion / proton-electron mixed conductive oxide; and / or,

[0010] The thickness of the positive electrode and / or the negative electrode is H2, wherein 0.1 mm ≤ H2 ≤ 1 mm, and the porosity of the positive electrode and / or the negative electrode is 0.1%-70%; and / or,

[0011] The material of the positive electrode connector and / or the negative electrode connector includes a high temperature alloy, a conductive oxide or a conductive composite ceramic, and the thermal expansion coefficient of the material of the positive electrode connector and / or the negative electrode connector is T1, and the thermal expansion coefficient of the electrolyte membrane is T2, wherein -30% ≤ (T1-T2) / T2 ≤ 30%; and / or,

[0012] The thickness of the positive electrode connector and / or the negative electrode connector is H3, wherein 0.2 mm ≤ H3 ≤ 3 mm; and / or,

[0013] The positive electrode current collector and / or the negative electrode current collector are made of a material including metal, alloy, conductive oxide or conductive composite ceramic.

[0014] Optionally, the positive electrode and / or the negative electrode are made of materials including Ni, Fe, Co, FeNi3, Ce 1- x Sm x O 2–δ 、Ni-Ce 1-x Sm x O 2–δ 、Ni-Ce 1-x G x O 2–δ , (La 1-x Sr x )(Cr 1-y Fe y ) 3–δ , (La 1-x Sr x )(Cr 1-y Mn y ) 3–δ , (La 1-x Sr x )TiO 3–δ ,La 2-x Sr x Fe 2-y-zNi y Mo z O 6-δ at least one of them, where 0 < x < 1, 0 < y < 1, 0 < z < 1, 0 < δ < 1; and / or,

[0015] the material of the positive electrode connector and / or the negative electrode connector includes stainless steel 430L, stainless steel 446, stainless steel Crofer, (La 1-x Sr x )TiO 3–δ and La 2-x Sr x Fe 2-y-z Ni y Mo z O 6-δ at least one of them, where 0 < x < 1, 0 < y < 1, 0 < z < 1, 0 < δ < 1; and / or,

[0016] the material of the positive electrode current collector and / or the negative electrode current collector includes Ni, Fe, Co, FeNi3, 430L, 446, Crofer, Ni-Ce 1-x Sm x O 2–δ , Ni-Ce 1-x Gd x O 2–δ , (La 1-x Sr x )(Cr 1-y Fe y )O 3–δ , (La 1-x Sr x )(Cr 1-y Mn y )O 3–δ and (La 1-x Sr x )TiO 3–δ , La 2-x Sr x Fe 2-y-z Ni y Mo z O 6-δ at least one of them, where 0 < x < 1, 0 < y < 1, 0 < z < 1, 0 < δ < 1.

[0017] Optionally, the positive electrode assembly is formed with a first receiving groove with an opening facing the electrolyte diaphragm and a first air inlet channel communicating with the first receiving groove, and the first air inlet channel is used to allow the mixed gas to enter the first receiving groove;

[0018] The negative electrode assembly is formed with a second receiving groove facing the electrolyte diaphragm and a second gas outlet channel communicating with the second receiving groove, and the second gas outlet channel is used to discharge the hydrogen gas generated in the second receiving groove.

[0019] Optionally, the groove depth of the first receiving groove and / or the second receiving groove in the thickness direction of the electrolyte diaphragm is H, where 0.1 mm ≤ H ≤ 3 mm.

[0020] Optionally, a plurality of pump body modules are provided, and the plurality of pump body modules are arranged in sequence along the first direction. Among two adjacent pump body modules, the first receiving groove of one positive electrode assembly communicates with the first gas inlet channel of another positive electrode assembly, or the second receiving groove of one negative electrode assembly communicates with the second exhaust channel of another negative electrode assembly.

[0021] Optionally, a plurality of pump body modules are provided, and the plurality of pump body modules are arranged in sequence along the first direction. Among two adjacent pump body modules, the positive electrode assembly of one pump body module is electrically connected to the negative electrode assembly of another pump body module.

[0022] Optionally, the material of the electrolyte diaphragm includes CeO 2–δ , LaGaO 3–δ , BaCeO 3–δ , BaZrO 3–δ , BaZr 1-x-y Ce x Y y O 3–δ , Sr2Sc 1+x , Nb 1–x O 6–δ , La 5.5 , WO 11.25-δ and Ba3Ca 1+x , Nb 2–x O9, at least one of which, where 0 < x < 1, 0 < δ < 1; and / or,

[0023] The thickness of the electrolyte diaphragm is T1, where 1 μm ≤ H1 ≤ 100 μm.

[0024] To achieve the above object, a hydrogen purification device for a hydrogen-oxygen fuel cell proposed by the present invention, the hydrogen purification device for the hydrogen-oxygen fuel cell includes the ceramic hydrogen pump as described above, and the ceramic hydrogen pump includes:

[0025] The invention comprises a pump body module, wherein the pump body module comprises a positive electrode assembly, an electrolyte membrane and a negative electrode assembly arranged in sequence along a first direction, wherein the positive electrode assembly is used to dissociate hydrogen in a mixed gas to generate hydrogen ions, the electrolyte membrane is used to allow the hydrogen ions to pass through, and the negative electrode assembly is used to reduce the hydrogen ions to generate hydrogen, wherein the positive electrode assembly, the electrolyte membrane and the negative electrode assembly are integrally formed.

[0026] In the technical solution provided by the present invention, the pump body module includes a positive electrode assembly, an electrolyte membrane and a negative electrode assembly arranged in sequence along a first direction, the positive electrode assembly dissociates hydrogen in the mixed gas to generate hydrogen ions, the electrolyte membrane allows the hydrogen ions to pass through and reach the negative electrode assembly, and the negative electrode assembly reduces the hydrogen ions to generate hydrogen. In this embodiment, the positive electrode assembly, the electrolyte membrane and the negative electrode assembly are integrally formed, which solves the problem in the prior art that the positive electrode assembly, the electrolyte membrane and the negative electrode assembly fail to seal due to different thermal expansion behaviors, thereby affecting the service life and reliability of the high-power hydrogen pump module. BRIEF DESCRIPTION OF THE DRAWINGS

[0027] In order to more clearly illustrate the embodiments of the present invention or the technical solutions in the prior art, the drawings required for use in the embodiments or the description of the prior art will be briefly introduced below. Obviously, the drawings described below are only some embodiments of the present invention. For ordinary technicians in this field, other drawings can be obtained based on the structures shown in these drawings without paying creative work.

[0028] Figure 1 A schematic structural diagram of an embodiment of a ceramic hydrogen pump provided by the present invention;

[0029] Figure 2 for Figure 1 Exploded view of the ceramic hydrogen pump.

[0030] Description of Figure Numbers:

[0031] Label name Label name 100 Ceramic hydrogen pump 12 Electrolyte membrane 1 Pump body module 13 Negative electrode components 11 Positive electrode components 131 Negative connector 111 Positive electrode connector 132 Negative current collector 112 Positive current collector 133 Negative electrode 113 Positive electrode 134 Second container 114 First tank 135 Second outlet channel 115 The first intake passage 136 Second intake passage 116 The first outlet channel

[0032] The realization of the purpose, functional features and advantages of the present invention will be further explained in conjunction with embodiments and with reference to the accompanying drawings. DETAILED DESCRIPTION

[0033] The following will be combined with the drawings in the embodiments of the present invention to clearly and completely describe the technical solutions in the embodiments of the present invention. Obviously, the described embodiments are only part of the embodiments of the present invention, not all of the embodiments. Based on the embodiments of the present invention, all other embodiments obtained by ordinary technicians in this field without creative work are within the scope of protection of the present invention.

[0034] It should be noted that if the embodiments of the present invention involve directional indications (such as up, down, left, right, front, back, etc.), the directional indications are only used to explain the relative position relationship, movement status, etc. between the components under a certain specific posture (as shown in the accompanying drawings). If the specific posture changes, the directional indication will also change accordingly.

[0035] In addition, if there are descriptions involving "first", "second", etc. in the embodiments of the present invention, the descriptions of "first", "second", etc. are only used for descriptive purposes and cannot be understood as indicating or implying their relative importance or implicitly indicating the number of technical features indicated. Therefore, the features defined as "first" and "second" may explicitly or implicitly include at least one of the features. In addition, the meaning of "and / or" appearing in the full text includes three parallel schemes. Taking "A and / or B" as an example, it includes scheme A, or scheme B, or a scheme that satisfies both A and B. In addition, the technical solutions between the various embodiments can be combined with each other, but it must be based on the ability of ordinary technicians in the field to implement. When the combination of technical solutions is contradictory or cannot be implemented, it should be deemed that such a combination of technical solutions does not exist and is not within the scope of protection required by the present invention.

[0036] The membrane electrode of hydrogen-oxygen fuel cell includes a catalyst layer, a diffusion layer and a proton exchange membrane. During the reaction process, if there are impurities in hydrogen, such as sulfides, etc., the platinum-carbon catalyst will be poisoned, which will lead to reduced catalyst activity, reduced fuel cell power, shortened life, etc. There are many ways to purify hydrogen. In the prior art, a ceramic hydrogen pump can be used to purify hydrogen. The ceramic hydrogen pump is generally composed of an electrolyte, a negative electrode and a positive electrode, wherein the electrolyte can conduct protons. Driven by electricity, hydrogen dissociates into protons at the positive electrode and is transmitted to the negative electrode through the electrolyte diaphragm. The protons combine with external circuit electrons at the negative electrode to generate hydrogen. In order to meet the high-throughput requirements of practical applications, the hydrogen pump monomer, the negative electrode current collector, the positive electrode current collector and the connector are often packaged in series at 800-1000°C through the negative electrode seal and the positive electrode seal to form a high-power hydrogen pump module with a relatively complex structure. In addition, the different thermal expansion behaviors between the hydrogen pump monomer, the seal and the connector increase the risk of sealing failure, affecting the service life and reliability of the high-power hydrogen pump module.

[0037] The present invention provides a ceramic hydrogen pump, wherein: Figure 1 to Figure 2 A schematic structural diagram of an embodiment of a ceramic hydrogen pump provided by the present invention.

[0038] See also Figure 1 to Figure 2The ceramic hydrogen pump 100 includes a pump body module 1, which includes a positive electrode assembly 11, an electrolyte membrane 12 and a negative electrode assembly 13 arranged in sequence along a first direction, the positive electrode assembly 11 is used to dissociate hydrogen in the mixed gas to generate hydrogen ions, the electrolyte membrane 12 is used to allow the hydrogen ions to pass through, and the negative electrode assembly 13 is used to reduce the hydrogen ions to generate hydrogen, wherein the positive electrode assembly 11, the electrolyte membrane 12 and the negative electrode assembly 13 are integrally formed.

[0039] In the above implementation, the pump body module 1 includes a positive electrode assembly 11, an electrolyte membrane 12 and a negative electrode assembly 13 arranged in sequence along a first direction. The positive electrode assembly 11 dissociates the hydrogen in the mixed gas to generate hydrogen ions, and the electrolyte membrane 12 allows the hydrogen ions to pass through and reach the negative electrode assembly 13. The negative electrode assembly 13 is used to reduce the hydrogen ions to generate hydrogen. In this embodiment, the positive electrode assembly 11, the electrolyte membrane 12 and the negative electrode assembly 13 are integrally formed, which solves the problem in the prior art that the positive electrode assembly 11, the electrolyte membrane 12 and the negative electrode assembly 13 fail to seal due to different thermal expansion behaviors, thereby affecting the service life and reliability of the high-power hydrogen pump module.

[0040] Specifically, refer to Figure 2 The positive electrode assembly 11 includes a positive electrode connector 111, a positive electrode collector 112 and a positive electrode 113 arranged in sequence, and the positive electrode 113 is arranged adjacent to the electrolyte membrane 12. The negative electrode assembly 13 includes a negative electrode connector 131, a negative electrode collector 132 and a negative electrode 133 arranged in sequence, and the negative electrode 133 is arranged adjacent to the electrolyte membrane 12. By sintering the positive electrode connector 111, the positive electrode collector 112, the positive electrode 113, the electrolyte membrane 12, the negative electrode 133, the negative electrode collector 132 and the negative electrode connector 131 into one, no sealing member is required, thereby improving the sealing and reliability of the ceramic hydrogen pump 100.

[0041] Furthermore, when the ceramic hydrogen pump 100 is working, the positive electrode 113 needs to be electrically connected to the positive electrode of the external power supply, and the negative electrode 133 needs to be electrically connected to the negative electrode of the external power supply. To this end, the materials made of the positive electrode 113 and / or the negative electrode 133 include metals, alloys, electronic conductive oxides and oxygen ion / proton-electron mixed conductive oxides.

[0042] Specifically, the positive electrode 113 and / or the negative electrode 133 are made of materials including Ni, Fe, Co, FeNi3, Ce 1-x Sm x O 2–δ 、Ni-Ce1-x Sm x O 2–δ 、 Ni - Ce 1-x Gd x O 2–δ 、 (La 1-x Sr x )(Cr 1-y Fe y )O 3–δ 、 (La 1-x Sr x )(Cr 1-y Mn y )O 3–δ 、 (La 1-x Sr x )TiO 3–δ 、 La 2-x Sr x Fe 2-y-z Ni y Mo z O 6-δ At least one of the above - mentioned materials. In the above - mentioned materials, the value ranges of x, y, δ, and z are 0 < x < 0.5, 0 < y < 0.5, 0 < δ < 1, and 0 < z < 0.5. Of course, in other embodiments, the values of x, y, δ, and z can be selected as needed, and the present application does not make any limitations in this regard.

[0043] Specifically, the thickness of the positive electrode 113 and / or the negative electrode 133 is H2, where 0.1 mm ≤ H2 ≤ 1 mm. With such a setting, while satisfying the strength, the weight of the positive electrode 113 and / or the negative electrode 133 is reduced. The porosity of the positive electrode 113 and / or the negative electrode 133 is 0.1% - 70%. With such a setting, while satisfying the strength, the positive electrode 113 adsorbs as much hydrogen as possible, and then dissociates hydrogen ions under the action of a catalyst. The negative electrode 133 adsorbs as many electrons as possible and reacts with hydrogen ions, thus generating a large amount of hydrogen.

[0044] Specifically, the material of the positive electrode connector 111 and / or the negative electrode connector 131 includes superalloy, conductive oxide or conductive composite ceramic, and the thermal expansion coefficient of the material of the positive electrode connector 111 and / or the negative electrode connector 131 is T1, and the thermal expansion coefficient of the electrolyte diaphragm 12 is T2, where -30% ≤ (T1 - T2) / T2 ≤ 30%. With such a setting, the thermal expansion coefficient of the material of the positive electrode connector 111 and / or the negative electrode connector 131 is relatively close to the thermal expansion coefficient of the electrolyte diaphragm 12, avoiding, when the ceramic hydrogen pump 100 is operating, due to excessive temperature, the positive electrode connector 111 and / or the negative electrode connector 131 and the electrolyte diaphragm 12 undergoing expansion deformation, and reducing the reliability and service life of the ceramic hydrogen pump 100.

[0045] Further, the material of the positive electrode connector 111 and / or the negative electrode connector 131 includes at least one of 430L stainless steel, 446 stainless steel, Crofer stainless steel, (La 1-x Sr x )TiO 3–δ and La 2-x Sr x Fe 2-y-z Ni y Mo z O 6-δ In this way, the positive electrode connector 111 and / or the negative electrode connector 131 can conduct electricity and be directly electrically connected to an external power source, with a simple structure. In the above materials, the value ranges of x, y, δ, and z are 0 < x < 0.5, 0 < y < 0.5, 0 < δ < 1, and 0 < z < 0.5. Of course, in other embodiments, the values of x, y, δ, and z can be selected as needed, and the present application does not limit this.

[0046] Specifically, the thickness of the positive electrode connector 111 and / or the negative electrode connector 131 is H3, where 0.2 mm ≤ H3 ≤ 3 mm. Within this thickness range, the positive electrode connector 111 and / or the negative electrode connector 131 can meet its own strength requirements while reducing the weight of the positive electrode connector 111 and / or the negative electrode connector 131.

[0047] Specifically, the material of the positive electrode current collector 112 and / or the negative electrode current collector 132 includes metal, alloy, conductive oxide or conductive composite ceramic.

[0048] Further, the material of the positive electrode current collector 112 and / or the negative electrode current collector 132 includes at least one of Ni, Fe, Co, FeNi3, 430L, 446, Crofer, Ni-Ce 1-x Smx O 2–δ , Ni-Ce 1-x Gd x O 2–δ , (La 1-x Sr x )(Cr 1-y Fe y )O 3–δ , (La 1-x Sr x )(Cr 1-y Mn y )O 3–δ and (La 1-x Sr x )TiO 3–δ , La 2-x Sr x Fe 2-y-z Ni y Mo z O 6-δ at least one of them. In the above-mentioned made materials, the value ranges of x, y, δ, and z are 0 < x < 0.5, 0 < y < 0.5, 0 < δ < 1, and 0 < z < 0.5. Of course, in other embodiments, the values of x, y, δ, and z can be selected as needed, and this application does not make any limitations in this regard.

[0049] The positive electrode assembly 11 is formed with a first receiving groove 114 having an opening facing the electrolyte diaphragm 12 and a first air inlet passage 115 communicating with the first receiving groove 114. The negative electrode assembly 13 is formed with a second receiving groove 134 facing the electrolyte diaphragm 12 and a second air outlet passage 135 communicating with the second receiving groove 134. A mixed gas containing hydrogen is transported into the first receiving groove 114 through the first air inlet passage 115. The mixed gas enters the first receiving groove 114, and the positive electrode assembly 11 dissociates the hydrogen in the mixed gas to generate hydrogen ions. The generated hydrogen ions pass through the electrolyte diaphragm 12 and enter the second receiving groove 134. The hydrogen ions react with the electrons provided by the negative electrode assembly 13 in the second receiving groove 134 to generate hydrogen, and the regenerated hydrogen is discharged through the second air outlet passage 135, thereby realizing the purification of hydrogen.

[0050] In order to facilitate the discharge of the purified hydrogen, in one embodiment, the positive electrode assembly 11 is further formed with a first gas outlet channel 116, which is in communication with the first container 114. When the reaction of the mixed gas entering the first container 114 is completed, the reacted mixed gas is discharged from the first gas outlet channel 116. The negative electrode assembly 13 is further formed with a second gas inlet channel 136, which is in communication with the second container 134. Hydrogen is transported into the second container 134 through the first gas inlet channel 115, so that the gas pressure in the second container 134 increases, thereby discharging the hydrogen generated by the reaction.

[0051] In order to facilitate the discharge of the purified hydrogen, in another embodiment, the second gas outlet channel 135 is connected to a negative pressure device, and a pressure difference is generated between the first container 114 and the air inlet of the negative pressure device, thereby sucking out the hydrogen generated in the second container.

[0052] It should be noted that there can be many types of negative pressure devices. For example, the negative pressure device can be a negative pressure vacuum pump, an air pump, etc. Since the technologies of the negative pressure vacuum pump and the air pump are mature, this application does not further describe the specific structure and working principle of the negative pressure vacuum pump and the air pump.

[0053] Specifically, the groove depth of the first containing groove 114 and / or the second containing groove 134 along the thickness direction of the electrolyte membrane 12 is H, wherein 0.1 mm≤H≤3 mm. Such an arrangement improves the gas flow rate of the first containing groove 114 and / or the second containing groove while ensuring the performance of the positive electrode assembly 11 and / or the negative electrode assembly 13.

[0054] In order to improve the power of the ceramic hydrogen pump 100, refer to Figure 2, the pump body modules 1 are provided in plurality, and the plurality of pump body modules 1 are sequentially arranged along the first direction. In two adjacent pump body modules 1, the first container 114 of one positive electrode component 11 is connected to the first air inlet channel 115 of another positive electrode component 11, or the second container 134 of one negative electrode component 13 is connected to the second air outlet channel 135 of another negative electrode component 13. In this arrangement, when the first container 114 of the positive electrode component 11 is connected to the first air inlet channel 115 of another positive electrode component 11, the first containers 114 of the plurality of positive electrode components 11 are arranged in series, that is, when the mixed gas enters the first container 114 of the positive electrode component 11 from the first air inlet channel 115 of the positive electrode component 11 at the head end of the series connection, the mixed gas in the first container 114 will sequentially reach the plurality of positive electrode components along the series flow path. The first containers 114 of the plurality of positive electrode assemblies 11 are filled with hydrogen ions under the action of the corresponding positive electrode assembly 11, and then the hydrogen ions pass through the electrolyte membrane 12 to reach the corresponding second containers 134, and the hydrogen ions react with the electrons provided by the negative electrode assembly 13 in the second containers 134 to generate hydrogen. Since the second containers 134 of one negative electrode assembly 13 are connected to the second outlet channel 135 of another negative electrode assembly 13, the second containers 134 of the plurality of negative electrode assemblies 13 are arranged in series, and the hydrogen generated in the second containers 134 of the negative electrode assembly 13 at the head end can pass through the plurality of second containers 134 arranged in series in sequence along the series flow path, and finally be discharged from the second outlet channel 135 of the second containers 134 of the negative electrode assembly 13 at the tail end of the series. Since the plurality of second containers 134 are arranged in series, the pressure of the discharged hydrogen is increased.

[0055] It should be noted that, in the above, the head end is the pump body module 1 that first contacts the gas, and the tail end is the pump body module 1 that last contacts the gas. Of course, in other embodiments, the head end and the tail end can be set as needed, and this application does not limit this.

[0056] Specifically, refer to Figure 1 , a plurality of the pump body modules 1 are arranged, and the plurality of the pump body modules 1 are arranged in sequence along the first direction. In two adjacent pump body modules 1, the positive electrode component 11 of one pump body module 1 is electrically connected to the negative electrode component 13 of the other pump body module 1. In this way, the plurality of pump body modules 1 are arranged in series in sequence to form a composite pump body module 1. The composite body module has two oppositely arranged ends, one end of which is provided with a positive electrode component 11, and the other end is provided with a negative electrode component 13. When connected to an external power supply, it is only necessary to connect the positive electrode component 11 to the positive electrode of the power supply, and the negative electrode component 13 to the negative electrode of the power supply, and the circuit is simple.

[0057] It should be noted that in other embodiments, it is also possible to electrically connect the positive electrode assemblies 11 of one pump body module 1 to the positive electrode assemblies 11 of another pump body module 1 among the multiple pump body modules 1, and electrically connect the negative electrode assemblies 13 of one pump body module 1 to the negative electrode assemblies 13 of another pump body module 1, so as to achieve the parallel connection of the multiple pump body modules 1. Of course, among the multiple pump body modules 1, it is possible to have both series and parallel connections for the multiple pump body modules 1. Specifically, the present application does not make any limitation in this regard.

[0058] Specifically, the material of the electrolyte diaphragm 12 includes CeO 2–δ , LaGaO 3–δ , BaCeO 3–δ , BaZrO 3–δ , BaZr 1-x-y Ce x Y y O 3–δ , Sr2Sc 1+x Nb 1–x O 6–δ , La 5.5 WO 11.25-δ and Ba3Ca 1+x Nb 2–x O9, at least one of them. Among the above-mentioned materials, the value ranges of x, y, δ, and z are 0 < x < 0.5, 0 < y < 0.5, and 0 < δ < 1. Of course, in other embodiments, the values of x and δ can be selected as needed, and the present application does not make any limitation in this regard.

[0059] Furthermore, the thickness of the electrolyte diaphragm 12 is H1, where 1 μm ≤ H1 ≤ 100 μm. Within this thickness range, both the denseness of the electrolyte diaphragm 12 and the effect of proton transfer are ensured.

[0060] The present invention also provides a hydrogen purification device for a hydrogen-oxygen fuel cell. The hydrogen purification device for the hydrogen-oxygen fuel cell includes the above-mentioned ceramic hydrogen pump 100. The specific structure of the ceramic hydrogen pump 100 refers to the above embodiments. Since the hydrogen purification device for the hydrogen-oxygen fuel cell of the present invention adopts all the technical solutions of the above-mentioned embodiments, it has at least all the beneficial effects brought by all the technical solutions of the above-mentioned embodiments, and will not be elaborated one by one here.

[0061] The above are only the preferred embodiments of the present invention, and do not limit the patent scope of the present invention accordingly. Any equivalent structural transformation made under the concept of the present invention by using the content of the specification and drawings of the present invention, or directly / indirectly applied in other related technical fields, is included in the patent protection scope of the present invention.

Claims

1. A ceramic hydrogen pump, characterized in that: The pump body module comprises a positive electrode assembly, an electrolyte membrane and a negative electrode assembly arranged in sequence along a first direction, the positive electrode assembly is used to dissociate hydrogen in a mixed gas to generate hydrogen ions, the electrolyte membrane is used to allow the hydrogen ions to pass through, and the negative electrode assembly is used to reduce the hydrogen ions to generate hydrogen, wherein the positive electrode assembly, the electrolyte membrane and the negative electrode assembly are integrally formed; The positive electrode assembly is formed with a first container having an opening facing the electrolyte diaphragm and a first air inlet channel connected to the first container, wherein the first air inlet channel is used to allow the mixed gas to enter the first container; The negative electrode assembly is formed with a second container disposed toward the electrolyte diaphragm and a second gas outlet channel communicating with the second container, wherein the second gas outlet channel is used to discharge hydrogen generated in the second container; The depth of the first containing groove and / or the second containing groove along the thickness direction of the electrolyte diaphragm is H, wherein 0.1 mm≤H≤3 mm; The pump body modules are provided in plurality, and the plurality of pump body modules are sequentially arranged along the first direction, and in two adjacent pump body modules, the first containing groove of one positive electrode assembly is connected to the first air inlet channel of the other positive electrode assembly, and the second containing groove of one negative electrode assembly is connected to the second air exhaust channel of the other negative electrode assembly; The positive electrode assembly comprises a positive electrode connector, a positive electrode current collector and a positive electrode arranged in sequence, and the positive electrode is arranged adjacent to the electrolyte membrane; The negative electrode assembly comprises a negative electrode connector, a negative electrode current collector and a negative electrode arranged in sequence, and the negative electrode is arranged adjacent to the electrolyte membrane; The positive electrode connector, the positive electrode current collector, the positive electrode, the electrolyte film, the negative electrode, the negative electrode, the negative electrode current collector and the negative electrode connector are sintered into one body; The positive electrode and / or the negative electrode are made of materials including metals, alloys, electronic conductive oxides and oxygen ion / proton-electron mixed conductive oxides; and / or, The thickness of the positive electrode and / or the negative electrode is H2, wherein 0.1 mm ≤ H2 ≤ 1 mm, and the porosity of the positive electrode and / or the negative electrode is 0.1%-70%; and / or, The positive electrode connector and / or the negative electrode connector are made of a material including a high temperature alloy, a conductive oxide or a conductive composite ceramic, and the thermal expansion coefficient of the material of the positive electrode connector and the negative electrode connector is T1, and the thermal expansion coefficient of the electrolyte membrane is T2, wherein -30%≤(T1-T2) / T2≤30%; and / or, The thickness of the positive electrode connector and / or the negative electrode connector is H3, wherein 0.2 mm ≤ H3 ≤ 3 mm; and / or the material of the positive electrode collector and / or the negative electrode collector includes metal, alloy, conductive oxide or conductive composite ceramic.

2. The ceramic hydrogen pump according to claim 1, characterized in that: The material used to make the positive electrode and / or the negative electrode includes Ni, Fe, Co, FeNi3, Ce 1-x Sm x O 2-δ , Ni-Ce 1-x Sm x O 2-δ , Ni-Ce 1-x Gd x O 2-δ , (La 1-x Sr x )(Cr 1- y Fe y )O 3-δ , (La 1-x Sr x )(Cr 1-y Mn y )O 3-δ , (La 1-x Sr x )TiO 3-δ , La 2-x Sr x Fe 2-y-z Ni y Mo z O 6-δ at least one of them, where 0 < x < 1, 0 < y < 1, 0 < z < 1, 0 < δ < 1; and / or, The material used to make the positive electrode connector and / or the negative electrode connector includes stainless steel 430L, stainless steel 446, stainless steel Crofer, (La 1-x Sr x )TiO 3-δ and La 2-x Sr x Fe 2-y-z Ni y Mo z O 6-δ at least one of them, where 0 < x < 1, 0 < y < 1, 0 < z < 1, 0 < δ < 1; and / or, The positive electrode current collector and / or the negative electrode current collector are made of materials including Ni, Fe, Co, FeNi3, 430L, 446, Crofer, Ni-Ce 1-x Sm x O 2-δ 、Ni-Ce 1-x G x O 2-δ , (La 1-x Sr x )(Cr 1-y Fe y ) 3-δ , (La 1-x Sr x )(Cr 1-y Mn y ) 3-δ and (La 1-x Sr x )TiO 3-δ ,La 2-x Sr x Fe 2-y-z Ni y Mo z O 6-δ At least one of which 0 <x<1,0<y<1,0<z<1,0<δ<1。 3. The ceramic hydrogen pump according to claim 1, characterized in that: A plurality of the pump body modules are provided, and the plurality of the pump body modules are arranged in sequence along the first direction. Among two adjacent pump body modules, the positive electrode component of one pump body module is electrically connected to the negative electrode component of the other pump body module.

4. The ceramic hydrogen pump according to claim 1, characterized in that: The material used to make the electrolyte diaphragm includes CeO 2-δ , LaGaO 3-δ , BaCeO 3-δ , BaZrO 3-δ , BaZr 1-x-y Ce x Y y O 3-δ , Sr2Sc 1+x Nb 1-x O 6-δ , La 5.5 WO 11.25-δ , and Ba3Ca 1+ x Nb 2-x O9, at least one of which, where 0 < x < 1, 0 < δ < 1; and / or, The thickness of the electrolyte separator is H1, wherein 1 μm≤H1≤100 μm.

5. A hydrogen purification device for a hydrogen-oxygen fuel cell, characterized in that: It comprises the ceramic hydrogen pump as claimed in any one of claims 1 to 4.