WO2021203932A1 - Électrode composite pour cellule à flux, cellule à flux, et pile - Google Patents

Électrode composite pour cellule à flux, cellule à flux, et pile Download PDF

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Publication number
WO2021203932A1
WO2021203932A1 PCT/CN2021/081315 CN2021081315W WO2021203932A1 WO 2021203932 A1 WO2021203932 A1 WO 2021203932A1 CN 2021081315 W CN2021081315 W CN 2021081315W WO 2021203932 A1 WO2021203932 A1 WO 2021203932A1
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Prior art keywords
layer
distribution
flow battery
composite electrode
distribution layer
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PCT/CN2021/081315
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English (en)
Chinese (zh)
Inventor
范永生
刘庆华
缪平
Original Assignee
国家能源投资集团有限责任公司
北京低碳清洁能源研究院
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Publication of WO2021203932A1 publication Critical patent/WO2021203932A1/fr

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    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/02—Details
    • H01M8/0202—Collectors; Separators, e.g. bipolar separators; Interconnectors
    • H01M8/0258—Collectors; Separators, e.g. bipolar separators; Interconnectors characterised by the configuration of channels, e.g. by the flow field of the reactant or coolant
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
    • H01M4/8605—Porous electrodes
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
    • H01M4/8647—Inert electrodes with catalytic activity, e.g. for fuel cells consisting of more than one material, e.g. consisting of composites
    • H01M4/8657—Inert electrodes with catalytic activity, e.g. for fuel cells consisting of more than one material, e.g. consisting of composites layered
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/02—Details
    • H01M8/0202—Collectors; Separators, e.g. bipolar separators; Interconnectors
    • H01M8/023—Porous and characterised by the material
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/02—Details
    • H01M8/0202—Collectors; Separators, e.g. bipolar separators; Interconnectors
    • H01M8/023—Porous and characterised by the material
    • H01M8/0241—Composites
    • H01M8/0245—Composites in the form of layered or coated products
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/18—Regenerative fuel cells, e.g. redox flow batteries or secondary fuel cells
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/18—Regenerative fuel cells, e.g. redox flow batteries or secondary fuel cells
    • H01M8/184—Regeneration by electrochemical means
    • H01M8/188—Regeneration by electrochemical means by recharging of redox couples containing fluids; Redox flow type batteries
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/24—Grouping of fuel cells, e.g. stacking of fuel cells
    • H01M8/2455—Grouping of fuel cells, e.g. stacking of fuel cells with liquid, solid or electrolyte-charged reactants
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/30—Hydrogen technology
    • Y02E60/50—Fuel cells

Definitions

  • the present invention relates to the technical field of energy storage, in particular to a composite electrode, a flow battery and an electric stack for a flow battery.
  • energy storage can increase the utilization of renewable energy and improve the stability of the power grid. It is mainly used for grid-connected renewable energy, peak-shaving and valley-filling, peak-shaving and frequency-modulation. Among them, the flow battery has become one of the main technologies for large-scale energy storage due to its advantages of long life, safety and reliability, power and capacity can be individually designed.
  • the flow battery is generally composed of a power unit and a capacity unit.
  • the energy storage and release are realized by the change of the valence state of the active material.
  • the electrolyte flows through the inside of the stack as a power unit to convert electrical energy and chemical energy, thereby realizing power input and output. Therefore, under the premise of determining the electrolyte system, the performance of the stack determines the power and efficiency of the energy storage system.
  • the electrolyte flows through the inside of the stack and reacts on the surface of the electrodes to realize the conversion of chemical energy and electrical energy.
  • factors such as electrolyte fluid distribution and concentration difference polarization have a greater impact on the electrochemical reaction, which in turn affects the functionality and efficiency of the stack.
  • a graphite felt or a carbon felt-like porous material is usually used as the electrode.
  • the electrolyte flows through the porous electrode and participates in the reaction. It can be seen that while the electrode provides an electrochemical reaction site, it also plays a role in distributing the electrolyte. Therefore, in the traditional stack design, it is necessary to balance the thickness of the electrode, electrochemical activity, porosity and conductivity. This is not good for maximizing various functions at the same time, so the stack cannot be made at a high current density. Run down.
  • the purpose of the present invention is to provide a composite electrode, a flow battery and a stack for a flow battery, which can realize the effective separation of the electrochemical reaction field and the electrolyte distribution field of the electrode, thereby improving the battery output power and energy efficiency .
  • one aspect of the present invention provides a composite electrode for a flow battery, the composite electrode comprising: a distribution layer for distributing electrolyte; and a reaction layer for receiving the distribution layer Electrolyte, and provide a place for electrochemical reaction of the electrolyte.
  • the distribution layer is at least one of graphite felt and metal fiber woven material.
  • the porosity of the distribution layer is greater than 50%, the thickness is less than 4 mm, and the fiber diameter is greater than 10 ⁇ m.
  • the porosity of the distribution layer is greater than 70%, the thickness ranges from 1.5 to 3 mm, and the fiber diameter is greater than 15 ⁇ m.
  • the reaction layer is at least one of graphite felt, carbon felt, porous carbon fiber material, powdered carbon material, porous metal material, and metal fiber woven material.
  • the porosity of the reaction layer is greater than 60%, and the thickness is less than 3 mm.
  • the total thickness of the reaction layer and the distribution layer is less than 5 mm in a free state, and the compression ratio ranges from 10% to 30%.
  • the total thickness of the reaction layer and the distribution layer ranges from 2 to 4.5 mm in a free state, and the compression ratio ranges from 15% to 25%.
  • another aspect of the present invention also provides a flow battery comprising: a positive electrode and a negative electrode separator, wherein at least one of the positive electrode and the negative electrode is the one used for the flow battery Composite electrode.
  • another aspect of the present invention also provides an electric stack, which includes: a plurality of the flow batteries described above.
  • the present invention creatively separates the electrochemical reaction field and the electrolyte distribution field of the composite electrode by arranging the distribution layer and the reaction layer.
  • the distribution layer can greatly reduce the uneven distribution due to flow.
  • Figure 1 is a schematic diagram of a composite electrode for a flow battery provided by an embodiment of the present invention
  • Figure 2 is a schematic diagram of a flow battery provided by an embodiment of the present invention.
  • Fig. 3 is a schematic diagram of an electric stack provided by an embodiment of the present invention.
  • FIG. 1 is a schematic diagram of a composite electrode 10 for a flow battery provided by an embodiment of the present invention.
  • the composite electrode 10 may include: a distribution layer 1 for distributing electrolyte; and a reaction layer 2 for receiving the electrolyte of the distribution layer and providing a place for electrochemical reaction of the electrolyte.
  • the distribution layer 1 may be at least one of graphite felt and metal fiber woven material.
  • graphite felt and metal fiber woven materials have flexible characteristics, the contact area between the distribution layer 1 and the reaction layer 2 is relatively large, which is beneficial to reduce the contact resistance.
  • graphite felt and metal fiber woven materials use the rapid flow distribution of electrolyte, which can be uniformly distributed in a short time through a special design (described in the next paragraph), which can avoid the influence of factors such as concentration difference polarization on the electricity. The impact of chemical reactions.
  • the porosity, thickness and fiber diameter of the distribution layer 1 have been designed and studied.
  • the porosity of the distribution layer 1 is greater than 50%, the thickness is less than 4 mm, and the fiber diameter is greater than 10 ⁇ m, higher electrical conductivity and excellent fluid distribution characteristics of the distribution layer 1 can be ensured at the same time.
  • the porosity of the distribution layer 1 is greater than 70%, the thickness is in the range of 1.5 to 3 mm, and the fiber diameter is greater than 15 ⁇ m, the conductivity of the distribution layer 1 can be increased by 10%, and the electrolyte is The flow resistance in the distribution layer 1 can be reduced by 20%.
  • the reaction layer 2 may be at least one of a porous carbon fiber material, a powdered carbon material, and a porous metal material.
  • the porosity and thickness of the reaction layer 2 are designed and studied. When the porosity of the reaction layer 2 is greater than 60% and the thickness is less than 3 mm, higher electrochemical activity of the reaction layer 2 can be ensured. In contrast, when the porosity of the reaction layer 2 is 70% and the thickness is in the range of 0.5 to 2 mm, the reaction layer 2 has higher electrochemical activity and can significantly reduce the surface resistance by more than 20%. , Thus providing an extremely excellent place for electrode reaction.
  • the total thickness and compression ratio of the distribution layer 1 and the reaction layer 2 in a free state were designed and studied.
  • the compression ratio is in the range of 10% to 30%, it can ensure that the electrolyte is distributed uniformly while reducing the thickness of the reaction layer 2. Concentration polarization.
  • the total thickness of the reaction layer 2 and the distribution layer 1 is in the free state in the range of 2 to 4.5 mm, and the compression ratio is in the range of 15% to 25%, it is possible to ensure that the electrolyte is distributed
  • the distribution in the layer 1 can significantly reduce the concentration polarization in the reaction layer 2 at the same time.
  • the present invention creatively separates the electrochemical reaction field and the electrolyte distribution field of the composite electrode by arranging the distribution layer and the reaction layer.
  • the distribution layer can greatly reduce the uneven distribution due to flow.
  • FIG. 2 is a schematic diagram of a flow battery 100 provided by an embodiment of the present invention.
  • the flow battery 100 may include a positive electrode 20, a negative electrode 30, and a separator 50, wherein at least one of the positive electrode 20 and the negative electrode 30 is the composite electrode 10 for a flow battery.
  • the positive electrode 20 and the negative electrode 30 in the flow battery 100 are both composite electrodes 10, as shown in FIG. 3.
  • the positive electrode 20 and the negative electrode 30 may respectively provide a place for the positive electrode reaction and the negative electrode reaction for the flow battery 100.
  • the positive electrode reaction may include: the mutual conversion of pentavalent vanadium ions and tetravalent vanadium ions, the mutual conversion of trivalent iron ions and divalent iron ions, and other electric pair redox reactions.
  • the negative electrode reaction may include: the mutual conversion of trivalent vanadium ions and divalent vanadium ions, the mutual conversion of trivalent chromium ions and divalent chromium ions, and other electric pair redox reactions.
  • the separator 50 may be located at an intermediate position between the positive electrode 20 and the negative electrode 30 to allow the conductive ions reacted by the positive electrode and the negative electrode to pass through, and prevent other ions and solvents from passing through.
  • Conducting the above ions may include, but are not limited to H +, Na +, K + , Li +, Cl -, OH - plasma.
  • the material of the diaphragm 50 may be at least one of a sulfonic acid type diaphragm material, a polymer porous membrane material, an organic/inorganic composite material, and an inorganic diaphragm material. As shown in FIG. 3, taking the diaphragm 50 as a reference, the reaction layer 2 is on both sides of the diaphragm 50, and the distribution layer 1 is on the outside of the reaction layer 2.
  • the flow battery 100 may further include: a bipolar plate 110, an electrode frame 40, and a flow pipe (not shown).
  • a bipolar plate 110 both the positive electrode 20 and the negative electrode 30 are on the inner side of the bipolar plate 110
  • a current lead-out plate (not shown) for deriving the current of the positive electrode 20 and the negative electrode 30 .
  • the two ends of the bipolar plate 110 are designed with electrode frames 40, as shown in FIG. 2.
  • the flow pipeline is used to introduce the electrolyte into the electrode frame 40, so as to flow into the flow battery 100 through the electrode frame 40, and then perform the battery charging process.
  • the electrode frame 40 has a fluid channel through which the electrolyte can flow into the distribution layer 1 of the composite electrode 10.
  • the electrolyte is rapidly and uniformly distributed in the distribution layer 1, and then transferred from the distribution layer 1 to the reaction layer 2.
  • the electrochemical reaction is carried out, and then, the reacted product is transferred to the distribution layer 1 and leaves the battery 100 with the flow of the electrolyte.
  • the electrode frame 40 can be made of a polymer material, the polymer material can be polypropylene (PP), polyethylene (PE), polyvinyl chloride (PVC), polyvinylidene fluoride (PVDF) and other materials and At least one of its modified materials, or a material compounded with other polymer fibers.
  • the flow battery 100 may further include a sealing member 60 for sealing the electrolyte inside.
  • the material of the sealing member 60 may be at least one of EPDM, nitrile rubber, fluorine rubber and other materials.
  • the present invention creatively adopts composite electrodes as the positive electrode and/or negative electrode of the flow battery. Because the composite electrode can effectively separate the distribution layer and the reaction layer, the distribution layer can greatly reduce the factors. Dead zone and channeling caused by uneven distribution; at the same time, special designs can be made for the distribution layer and the reaction layer (for example, use a material with higher electrochemical activity as the reaction layer, and use the characteristics of enhanced fluid flow distribution and conductivity Excellent material as the distribution layer), thereby improving the output power and energy efficiency of the flow battery.
  • FIG. 3 is a schematic diagram of an electric stack 200 provided by an embodiment of the present invention.
  • the electric stack 200 may include a plurality of the flow batteries 100 described above.
  • the flow battery 100 includes a positive electrode, a negative electrode and a separator.
  • the stack 200 further includes a plurality of bipolar plates 110 for connecting the plurality of flow batteries in series, as shown in FIG. 3.
  • both ends of the bipolar plate 110 are designed with electrode frames 40, so that the electrode frames 40 connect each flow battery 100 in parallel in terms of electrolyte circulation.
  • the stack 200 may further include: an end plate 120 for fixing the plurality of flow batteries 100.
  • a current lead plate (not shown) is designed between the bipolar plate of the flow battery on the leftmost side and the rightmost side of the stack 200 and the end plate 120 to derive the current of all positive electrodes and all negative electrodes.
  • the stack 200 may further include: a flow pipe (not shown, only the interface 130 of the flow pipe is shown) for introducing the electrolyte into the electrode frame 40 in the flow battery 100, thereby It flows into the flow battery 100 through the electrode frame 40, and then the battery charging process is performed.
  • the electric stack 200 is formed by a plurality of flow batteries 100 connected in series through a bipolar plate 110, and superimposed and fastened into a whole.
  • the electrolyte enters the electrode frame 40 of each flow battery 100 through a flow pipe (not shown), and then enters the distribution layer 1 of the composite electrode 10 through the fluid channel of the electrode frame 40, and the electrolyte flows rapidly in the distribution layer 1
  • the electrolyte is basically uniformly distributed, and then the electrolyte is transferred from the distribution layer 1 to the reaction layer 2 for electrochemical reaction, and the reacted product is transferred to the distribution layer 1 and leaves the battery as the electrolyte flows.
  • the flow battery 100 can work in a charged state or a discharged state, and can switch between the two states.
  • the structure of the cell stack 200 composed of the flow battery 100 provided in the first embodiment is shown in FIG. 3. Specifically, 2 mm thick carbon felt is used as the reaction layer 2 of the positive electrode 20 and the negative electrode 30 of the flow battery 100, and 3 mm thick graphite felt is used as the distribution layer 1 of the positive electrode 20 and the negative electrode 30, and the electrode size is 200 mm x 200 mm.
  • a flat carbon-plastic composite bipolar plate is used as the bipolar plate 110, an electrode frame 40 with fluid distribution channels, and a seal 60 made of EPDM rubber are used.
  • the porosity of the carbon felt in Example 1 is 90%, the activated carbon felt has a fiber diameter of 10 ⁇ m; the porosity of the graphite felt is 86%, the fiber diameter is 15 ⁇ m, and the surface resistance is less than 0.15 ⁇ *cm 2 .
  • the difference between the stack 200 provided in the second embodiment and the first embodiment is that 1.5 mm thick carbon felt is used as the reaction layer 2 of the positive electrode 20 and the negative electrode 30 of the flow battery 100, and 3.5 mm thick graphite felt is used as the positive electrode 20. And the distribution layer 1 of the negative electrode 30.
  • the difference between the stack 200 provided in this embodiment 3 and the embodiment 1 is that a 1mm thick multilayer carbon paper is used as the reaction layer 2 of the positive electrode 20 and the negative electrode 30 of the flow battery 100, and a 4mm thick graphite felt is used as the positive electrode 20. And the distribution layer 1 of the negative electrode 30.
  • the porosity of the carbon paper in Example 3 is greater than 70%.
  • the difference between the stack provided in this embodiment and Embodiment 1 is that carbon felt with a thickness of 5 mm is used as the positive electrode and the negative electrode of the flow battery.
  • the porosity of the carbon felt in this embodiment is 90%, and the activated carbon felt has a fiber diameter of 10 ⁇ m.
  • the initial concentration of the positive electrode electrolyte in the above embodiments is 0.8mol L -1 V 4+ (tetravalent vanadium)+0.8mol L -1 V 5+ (5-valent vanadium)+3mol L -1 H 2 SO 4
  • the negative electrode The initial concentration of the electrolyte is 0.8 mol L -1 V 2+ (divalent vanadium) + 0.8 mol L -1 V 3+ (trivalent vanadium) + 3 mol L -1 H 2 SO 4 .
  • the output performance test of the stack in the foregoing embodiments is measured by a potentiostat.
  • the present invention creatively uses a plurality of flow batteries (the flow battery uses composite electrodes as the positive and/or negative electrodes of the flow battery) to form a stack, because the composite electrodes can achieve effective distribution and reaction layers.
  • the distribution layer can greatly reduce the dead zone and channel flow caused by uneven flow distribution; meanwhile, the distribution layer and the reaction layer can be specially designed (for example, the use of higher electrochemically active).
  • the material is used as the reaction layer, and the material with the characteristics of enhancing fluid flow distribution and excellent electrical conductivity is used as the distribution layer), so as to improve the output power and energy efficiency of the stack.

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  • Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Manufacturing & Machinery (AREA)
  • Sustainable Development (AREA)
  • Sustainable Energy (AREA)
  • Composite Materials (AREA)
  • Inert Electrodes (AREA)
  • Fuel Cell (AREA)

Abstract

La présente invention se rapporte au domaine technique du stockage d'énergie. L'invention concerne une électrode composite pour une cellule à flux, une cellule à flux et une pile. L'électrode composite comprend : une couche de distribution, utilisée pour la distribution d'un électrolyte ; et une couche de réaction, utilisée pour recevoir l'électrolyte de la couche de distribution et fournir un site de réaction électrochimique pour l'électrolyte. La présente invention, en fournissant une couche de distribution et une couche de réaction, permet de séparer efficacement un site de réaction électrochimique et un site de distribution d'électrolyte d'une électrode composite, la couche de distribution étant apte à réduire considérablement les zones mortes et la canalisation provoquée par une distribution irrégulière du flux. En même temps, la couche de distribution et la couche de réaction peuvent être conçues séparément et spécialement (par exemple un matériau ayant une activité électrochimique élevée étant utilisé en tant que couche de réaction, et un matériau ayant une propriété de renforcement de distribution d'écoulement de fluide et une excellente conductivité électrique étant utilisé en tant que couche de distribution), améliorant ainsi la puissance de sortie et l'efficacité énergétique d'une cellule ou d'une pile prenant l'électrode composite selon la présente invention en tant qu'anode et/ou cathode.
PCT/CN2021/081315 2020-04-10 2021-03-17 Électrode composite pour cellule à flux, cellule à flux, et pile WO2021203932A1 (fr)

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CN202010278572.1A CN113517451A (zh) 2020-04-10 2020-04-10 用于液流电池的复合电极、液流电池及电堆
CN202010278572.1 2020-04-10

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CN117374293B (zh) * 2023-12-07 2024-03-08 北京普能世纪科技有限公司 一体化电极和包含其的液流电池

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* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN116230999A (zh) * 2023-04-26 2023-06-06 北京星辰新能科技有限公司 一种标准40尺集装箱式液流电池系统
CN116230999B (zh) * 2023-04-26 2023-07-18 北京星辰新能科技有限公司 一种标准40尺集装箱式液流电池系统

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