CN106711462B - Sodium-halide battery current collector and sodium-halide battery containing same - Google Patents

Sodium-halide battery current collector and sodium-halide battery containing same Download PDF

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CN106711462B
CN106711462B CN201510770536.6A CN201510770536A CN106711462B CN 106711462 B CN106711462 B CN 106711462B CN 201510770536 A CN201510770536 A CN 201510770536A CN 106711462 B CN106711462 B CN 106711462B
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current collector
sodium
corrosion
layer
cathode
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CN106711462A (en
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温兆银
胡英瑛
吴相伟
朱咏民
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Shanghai Energy Energy Technology Co., Ltd.
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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
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/64—Carriers or collectors
    • H01M4/66—Selection of materials
    • H01M4/665—Composites
    • H01M4/667—Composites in the form of layers, e.g. coatings
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/36—Accumulators not provided for in groups H01M10/05-H01M10/34
    • H01M10/38—Construction or manufacture
    • 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
    • Y02E60/10—Energy storage using batteries
    • 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
    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
    • Y02P70/50—Manufacturing or production processes characterised by the final manufactured product

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  • Engineering & Computer Science (AREA)
  • Manufacturing & Machinery (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Composite Materials (AREA)
  • Materials Engineering (AREA)
  • Secondary Cells (AREA)

Abstract

The invention relates to a sodium-halide battery current collector and a sodium-halide battery containing the same, wherein a cathode current collector of the sodium-halide battery comprises: the welding device comprises a conductive material, a corrosion-resistant layer coated on the surface of the conductive material, and a welding layer which is coated on a shell connecting part of the corrosion-resistant layer and has weldability. The cathode current collector comprises the corrosion-resistant layer and the welding layer, so that the cathode current collector has good corrosion resistance, can work in a medium-temperature acidic environment for a long time, has good welding performance, and can complete the full sealing of a battery. And the resistance of the cathode current collector is small, so that the internal resistance of the battery can not be increased almost, and the comprehensive performance of the battery can not be influenced.

Description

Sodium-halide battery current collector and sodium-halide battery containing same
Technical Field
The invention belongs to the field of energy materials, and relates to a sodium-halide battery, in particular to a multilayer current collector for a cathode of the sodium-halide battery, a sodium-halide battery comprising the multilayer current collector and a preparation method of the sodium-halide battery.
Background
Medium temperature sodium-halide batteries (also known as ZEBRA batteries) are due to their high theoretical specific energy (e.g. 790Wh kg for sodium-nickel chloride batteries)-1) Sodium-halide batteries generally employ β "-alumina ceramic as solid electrolyte and separator, sodium tetrachloroaluminate (NaAlCl)4) As a cathode molten salt electrolyte, the electrolyte was operated at a medium temperature of about 300 ℃. Due to the full sealing of the battery and NaAlCl4The selection of the cathodic current collector of the battery is faced with a series of problems of greater corrosivity, such as the corrosion resistance of the current collector and the weldability with the top cap affecting the cycle life and safety of the batteryImportant factor for full performance. Therefore, it is important and necessary to improve and optimize the cathode current collector of sodium-halide batteries.
As a cathode current collector for sodium-halide batteries, the following requirements need to be met: can resist the long-term corrosion of the molten sodium tetrachloroaluminate at the temperature of 1.300 ℃. 2. Good compatibility with cathode materials and no impurity elements. 3. And the top cover has weldability. The cathode current collector of sodium-halide battery disclosed in The prior art is hairpin nickel with built-in carbon felt (see "The sodium/nickel chloride battery", j.l. sudworth, j.power Sources,100(2001) 149-163). The current collector pair NaAlCl4The nickel and carbon have lower conductivity than common current collectors such as copper and aluminum, and the carbon felt occupies a large volume, thereby reducing the power density and the energy density of the battery. Korean patent application No. KR1020130070812 discloses the use of a carbon felt with an ultra-large porosity as a cathode current collector for a sodium secondary battery, and also such a current collector lowers the power density and energy density of the battery to some extent. Therefore, there is an urgent need for the development of a cathode current collector for sodium batteries having more excellent properties in various aspects.
Disclosure of Invention
In view of the problems of the prior art, the present invention is directed to a multilayer current collector for sodium-halide battery cathodes with good corrosion resistance, electrical conductivity, and weldability that does not substantially degrade the electrochemical performance of the battery upon meeting the basic requirements of the current collector.
In one aspect, the present invention provides a cathode current collector for a sodium-halide battery, the cathode current collector comprising: the welding device comprises a conductive material, a corrosion-resistant layer coated on the surface of the conductive material, and a welding layer which is coated on a shell connecting part of the corrosion-resistant layer and has weldability.
The cathode current collector comprises the corrosion-resistant layer and the welding layer, so that the cathode current collector has good corrosion resistance, can work in a medium-temperature acidic environment for a long time, has good welding performance, and can complete the full sealing of a battery. And the resistance of the cathode current collector is small, so that the internal resistance of the battery can not be increased almost, and the comprehensive performance of the battery can not be influenced.
Preferably, the conductive material is copper, aluminum, or stainless steel.
Preferably, the corrosion-resistant layer is densely coated on the whole surface of the conductive material, and the corrosion-resistant layer is preferably carbon material, nickel, silver, gold or platinum.
Preferably, the welding layer is nickel or nickel alloy.
Preferably, the thickness of the corrosion-resistant layer is 2 μm to 50 μm.
Preferably, the thickness of the welding layer is 200 μm to 2 mm.
In another aspect, the present invention provides a method of preparing the above cathode current collector, comprising:
firstly, modifying the surface of the conductive material by the corrosion-resistant layer in a chemical vapor deposition, coating, evaporation, electroplating, chemical plating or spraying manner;
and secondly, coating the welding layer on the shell connecting part of the corrosion-resistant layer in a chemical vapor deposition, evaporation, electroplating, chemical plating or spraying manner.
The preparation method is simple and easy to implement, low in cost and easy for large-scale production.
In yet another aspect, the present invention provides a sodium-halide battery comprising a metallic sodium anode, a conductive housing as an anode current collector, a solid electrolyte, a cathode, and the above-described cathode current collector disposed within the cathode and extending to a battery top cap and welded thereto by the weld layer.
The sodium-halide battery has the cathode current collector, so the sodium-halide battery has good corrosion resistance, can work in a medium-temperature acid environment for a long time, has good welding performance, and can complete the full sealing of the battery. And the resistance of the cathode current collector is small, so that the internal resistance of the battery can not be increased almost, and the comprehensive performance of the battery can not be influenced.
Preferably, the solid electrolyte is selected from the group consisting of sodium ion conductor ceramics, sodium ion conductor glass, and sodium ion conductor composites.
Preferably, the cathode comprises an active material and a molten salt electrolyte.
Preferably, the active material is comprised of an active metal, sodium halide, and other additives, such as β "-Al2O3、β-Al2O3、NASICON、Na5GdSi4O12Or ZrO2/β″-Al2O3Composite ceramics.
Preferably, the molten salt electrolyte is a sodium ion conductor molten salt and a mixture thereof or an ion and electron mixed conductor molten salt.
The invention has the following beneficial effects:
(1) the obtained cathode current collector has good corrosion resistance and can work in a medium-temperature acidic environment for a long time;
(2) the obtained cathode current collector has good welding performance and can complete the full sealing of the battery;
(3) the obtained cathode current collector has small resistance, the internal resistance of the battery is hardly increased, and the comprehensive performance of the battery is not influenced;
(4) the obtained cathode current collector has good compatibility with cathode materials, and no impurity element is introduced;
(5) the preparation method of the obtained cathode current collector is simple and easy to implement and low in cost;
(6) the raw material has strong selectivity and low price.
Drawings
Fig. 1 shows a schematic view of the internal structure of a cathode current collector in example 1;
fig. 2 shows a schematic view of the internal structure of a cathode current collector in example 2.
Detailed Description
The present invention will be further described with reference to the following embodiments with reference to the accompanying drawings. It is to be understood that the drawings and/or detailed description are only illustrative of the invention and are not restrictive thereof.
After extensive and intensive research, the inventors of the present invention have found that a multi-layered cathode current collector is obtained by a two-step process, which can simultaneously satisfy the basic requirements of the current collector without almost degrading the electrochemical performance of the battery, thereby obtaining a high-performance sodium-halide battery. Based on the above findings, the present invention has been completed.
The sodium-halide battery of the invention includes an anode, an anode current collector, a solid electrolyte, a cathode, and a cathode current collector. The battery comprises a battery anode (cathode), a battery cathode (anode), a battery current collector and a battery shell, wherein the battery anode (cathode) is metal sodium, the battery cathode (anode) is metal halide, and the battery current collector is the battery shell. For example, typical sodium-halide batteries include sodium-nickel halide batteries, sodium-iron halide batteries, and sodium-zinc halide batteries.
The cathode contains an active material and a molten salt electrolyte. The active substance consists of active metal, sodium halide and other additives. The active metals include, but are not limited to, nickel, iron, zinc, copper. Other additives include, but are not limited to, sodium fluoride, sodium iodide, metallic aluminum, sulfur, metallic sulfides. The molten salt electrolyte may be a sodium ion conductor molten salt and mixtures thereof or a mixed conductor molten salt of ions and electrons, such as sodium tetrachloroaluminate (NaAlCl)4) And the like.
The solid electrolyte is selected from the group consisting of sodium ion conductor ceramics, sodium ion conductor glasses, and sodium ion conductor composites, e.g., β "-Al2O3、β-Al2O3、NASICON、Na5GdSi4O12Or ZrO2/β″-Al2O3Composite ceramics.
Referring to fig. 1, the cathode current collector of the present invention is disposed within the metal halide cathode (preferably centrally disposed within the metal halide cathode) and extends to the cell top cap. The cathode current collector includes a double layer portion disposed within the cathode and a triple layer portion disposed between the cathode and the cell top cap. Preferably, the double-layer portion and the triple-layer portion are continuously distributed. Specifically, the cathode current collector includes a double-layer part disposed inside the metal halide cathode and including a conductive material and a corrosion-resistant layer coated on a surface of the conductive material, and a triple-layer part coated with a welding layer between the cathode and the battery top cap on the basis of the double-layer part. Thus, the sodium-halide cell of the invention comprises a cathode multilayer current collector with good corrosion resistance, electrical conductivity and weldability. Wherein the double layer portion of the multilayer current collector is disposed in the cathode material and the three layer portion is disposed in the weld between the cathode and the cap.
The conductive material is selected from common current collector materials such as copper, aluminum, stainless steel, and the like.
The corrosion-resistant layer can be selected from at least one of carbon materials and acid corrosion resistant materials such as nickel, silver, gold, platinum and the like. The carbon materials include, but are not limited to, graphite, graphene, and the like. The corrosion-resistant layer is densely coated on the surface of the conductive material. Preferably, the corrosion-resistant layer is densely coated on the whole surface of the conductive material. The thickness of the corrosion-resistant layer can be 2-50 μm. If the thickness of the corrosion-resistant layer is less than 2 μm, the corrosion-resistant strength is insufficient, and if the thickness of the corrosion-resistant layer is greater than 50 μm, the conductivity of the current collector is affected, and the polarization of the battery may be increased.
The welding layer may be composed of metallic nickel having weldability or a nickel alloy resistant to acid corrosion. The thickness of the welding layer can be 200 μm-2 mm. If the thickness of the welding layer is less than 200 μm, the welding difficulty is increased, and if the thickness of the welding layer is more than 2mm, the battery cost is increased, and the energy density of the battery is reduced. From the viewpoint of saving materials, the area of the welding layer may be as small as possible as long as the double-layered portion can be welded to the battery top cap.
The invention can prepare the cathode current collector by a two-step method, which comprises the following steps:
firstly, modifying the surface of the conductive material by the corrosion-resistant layer in a chemical vapor deposition, coating, evaporation, electroplating, chemical plating or spraying manner;
and secondly, coating the welding layer on the shell connecting part (such as the top part) of the double-layer current collecting part in a chemical vapor deposition, evaporation, electroplating, chemical plating or spraying mode.
In the cathode current collector of the present invention, the cathode current collector may be woven into any shape and structure suitable for the structure and current collecting effect of a battery.
The sodium-halide battery provided by the invention has the advantages that the contribution of the cathode current collector to the internal resistance of the battery is extremely small, and the resistivity is less than 1 x 10-7Omega m, in the long term of the batteryThe stability during cycling is good, for example, in the sodium-halide battery of the invention, after the battery is cycled for 200 times, the cathode is taken out, and the phenomenon that the current collector is obviously corroded is found.
The invention is further illustrated by the following examples to better illustrate the invention. It is also to be understood that the following examples are illustrative of the present invention and are not to be construed as limiting the scope of the invention, and that certain insubstantial modifications and adaptations of the invention by those skilled in the art may be made in light of the above teachings. The specific numerical values of the following examples are also merely one example of suitable ranges, that is, the range can be selected by those skilled in the art within the suitable ranges through the description herein, and are not limited to the specific numerical values of the following examples. Test methods in which specific conditions are not specified in the following examples are generally carried out under conventional conditions or under conditions recommended by the manufacturer. All percentages and parts are by weight unless otherwise indicated.
Example 1
Firstly, modifying a graphite layer (10 mu m) on the outer surface of a copper rod by using a coating method, then plating a layer of metal nickel (1.5mm) on the welding part at the top of the Cu @ graphite rod by using an electroplating method, and assembling a sodium-nickel halide battery with the designed capacity of 100mAh by using the prepared Cu @ graphite @ Ni current collector as a cathode current collector. Fig. 1 is a schematic structural diagram of a Cu @ graphite @ Ni current collector material. The resistivity of the Cu @ graphite @ Ni current collector is 6 x 10-8Omega m. The cathode was removed after the cell was cycled 200 times and no significant corrosion of the current collector was observed.
Example 2
Firstly, a metal nickel layer (20 mu m) is modified on the outer surface of a copper bar by an electroplating method, then a layer of metal nickel (1.5mm) is plated on the welding position at the top of a Cu @ Ni bar by the electroplating method, and the prepared Cu @ Ni @ Ni current collector is used as a cathode current collector to assemble a sodium-nickel halide battery with the designed capacity of 100 mAh. Fig. 2 is a schematic structural diagram of a Cu @ Ni current collector material. The resistivity of the Cu @ Ni @ Ni current collector is 8 x 10-8Omega m. The cathode was removed after the cell was cycled 100 times and no significant corrosion of the current collector was observed.
Example 3
Firstly, modifying a graphene layer (3 mu m) on the outer surface of a copper sheet by using a chemical vapor deposition method, then plating a layer of metal nickel (2mm) on the welding part at the top of the Cu @ graphene sheet by using an electroplating method, and assembling the prepared Cu @ graphene @ Ni current collector as a cathode current collector to design a sodium-nickel halide battery with the capacity of 100 mAh. The resistivity of the Cu @ graphene @ Ni current collector is 3 x 10-8Omega m. The cathode was removed after the cell was cycled 100 times and no significant corrosion of the current collector was observed.
Example 4
Firstly, modifying a graphene layer (2 mu m) on the outer surface of a copper sheet by using a chemical vapor deposition method, then plating a layer of metal nickel (1.5mm) on the welding part at the top of the Cu @ graphene sheet by using an evaporation method, and assembling the prepared Cu @ graphene @ Ni current collector as a cathode current collector to design a sodium-nickel halide battery with the capacity of 100 mAh. The resistivity of the Cu @ graphene @ Ni current collector is 3.5 x 10-8Omega m. The cathode was removed after the cell was cycled 100 times and no significant corrosion of the current collector was observed.
Example 5
Firstly, modifying a graphite layer (10 mu m) on the outer surface of an aluminum rod by using a coating method, then plating a layer of metal nickel (1.5mm) on the welding part at the top of the Al @ graphite rod by using an electroplating method, and assembling a sodium-nickel halide battery with the designed capacity of 100mAh by using the prepared Al @ graphite @ Ni current collector as a cathode current collector. The resistivity of the Al @ graphite @ Ni current collector is 7-10-8Omega m. The cathode was removed after the cell was cycled 100 times and no significant corrosion of the current collector was observed.
All documents referred to herein are incorporated by reference into this application as if each were individually incorporated by reference. Furthermore, it should be understood that various changes and modifications of the present invention can be made by those skilled in the art after reading the above teachings of the present invention, and these equivalents also fall within the scope of the present invention as defined by the appended claims.

Claims (8)

1. A cathode current collector for medium temperature sodium-halide batteries, characterized in that the cathode current collector comprisesComprises the following steps: the conductive material, the corrosion-resistant layer coated on the surface of the conductive material and the welding layer coated on the top of the corrosion-resistant layer and having weldability, wherein the corrosion-resistant layer is densely coated on the whole surface of the conductive material, the corrosion-resistant layer is a graphite layer or a graphene layer, the thickness of the corrosion-resistant layer is 2-50 mu m, the corrosion-resistant layer is modified on the surface of the conductive material in a chemical vapor deposition, coating, evaporation, electroplating, chemical plating or spraying manner, the welding layer is nickel or nickel alloy, the thickness of the welding layer is 200-2 mm, and the welding layer is coated on the top of the corrosion-resistant layer in a chemical vapor deposition, evaporation, electroplating, chemical plating or spraying manner; the cathode current collector is stable in a medium-temperature acidic environment; the resistivity of the cathode current collector is less than 1 x 10-7Ω· m。
2. The cathode current collector of claim 1, wherein the conductive material is copper, aluminum, or stainless steel.
3. A method of preparing the cathode current collector of claim 1 or 2, comprising:
firstly, modifying the surface of the conductive material by the corrosion-resistant layer in a chemical vapor deposition, coating, evaporation, electroplating, chemical plating or spraying manner;
and secondly, coating the welding layer on the top of the corrosion-resistant layer in a chemical vapor deposition, evaporation, electroplating, chemical plating or spraying manner.
4. An intermediate-temperature sodium-halide battery comprising a metallic sodium anode, an electrically conductive housing as an anode current collector, a solid electrolyte, a cathode, and the cathode current collector of claim 1 or 2, said cathode current collector being disposed inside said cathode and extending to a battery top cap and being welded thereto by said weld layer.
5. A medium-temperature sodium-halide battery according to claim 4, wherein the solid electrolyte is selected from the group consisting of sodium ion conductor ceramics, sodium ion conductor glasses and sodium ion conductor composites.
6. A medium-temperature sodium-halide battery according to claim 4 or 5, wherein the cathode comprises an active substance and a molten salt electrolyte.
7. A medium-temperature sodium-halide battery according to claim 6, wherein the active substance consists of active metals, sodium halide and other additives.
8. A medium-temperature sodium-halide battery according to claim 6, wherein the molten salt electrolyte is a sodium ion conductor molten salt and mixtures thereof or an ion and electron mixed conductor molten salt.
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CN109698389A (en) * 2017-10-23 2019-04-30 张建城 Na chloride single battery
CN108336357A (en) * 2017-12-14 2018-07-27 合肥国轩高科动力能源有限公司 A kind of ultralight affluxion body in lithium ion batteries and preparation method thereof
CN110660999A (en) 2018-09-30 2020-01-07 宁德时代新能源科技股份有限公司 Current collector, pole piece and electrochemical device
CN110943227B (en) * 2019-05-31 2021-03-09 宁德时代新能源科技股份有限公司 Composite current collector, electrode plate and electrochemical device
CN114520336B (en) * 2022-04-21 2022-08-02 宁德时代新能源科技股份有限公司 Current collector, manufacturing method and equipment thereof, and current collector prefabricated part

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