CN113725445B - High-efficiency all-solid-state sodium-oxygen-water battery - Google Patents
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- CN113725445B CN113725445B CN202110941119.9A CN202110941119A CN113725445B CN 113725445 B CN113725445 B CN 113725445B CN 202110941119 A CN202110941119 A CN 202110941119A CN 113725445 B CN113725445 B CN 113725445B
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
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- H01M12/00—Hybrid cells; Manufacture thereof
- H01M12/08—Hybrid cells; Manufacture thereof composed of a half-cell of a fuel-cell type and a half-cell of the secondary-cell type
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- B—PERFORMING OPERATIONS; TRANSPORTING
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- H01M4/8647—Inert electrodes with catalytic activity, e.g. for fuel cells consisting of more than one material, e.g. consisting of composites
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- H01M2004/8678—Inert electrodes with catalytic activity, e.g. for fuel cells characterised by the polarity
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Abstract
The invention relates to a high-efficiency all-solid-state sodium-oxygen-water battery. The battery includes a nano-metal polymer electrode material; the electrode material is obtained by mixing and reacting metal nano particles, n-butyl acetate, 1-methoxy-2-propanol acetate and acrylic resin and standing. The invention synthesizes cathode materials by utilizing metal nano particles and polymers, assembles a chargeable high-performance all-solid-state sodium-oxygen-water battery, works in an environment with medium humidity, can be recycled for more than 100 times, and has low overpotential and high cycle efficiency.
Description
Technical Field
The invention belongs to the field of metal air batteries, and particularly relates to a high-efficiency all-solid-state sodium-oxygen-water battery.
Background
Rechargeable sodium-air batteries have received considerable attention over the past few years due to their higher theoretical energy density, abundant sodium resources, and lower cost. The normal structure of a sodium-air cell is a metallic sodium anode, a nonaqueous/aqueous sodium electrolyte, and a porous conductive cathode. During discharge, O 2 Is reduced and combined with Na at the cathode + Combines to form a discharge product (typically Na 2 O 2 、NaO 2 And some other sodium compounds). The porous electrode is not an active material, but rather a conductive stable framework carrying the reaction products, with lighter electrode materials providing higher specific energy. For the charging process, the previously formed discharge products must be thoroughly removed to prevent the channels of the electrode from being blocked by the discharge products and unnecessary side reaction products.
As a non-negligible component in air, moisture (H 2 O) is another important factor that sodium-air batteries are seriously considered. H in air 2 The concentration of O is generally expressed in terms of Relative Humidity (RH), which is calculated from the ratio of the actual water vapor pressure to the saturated water vapor pressure at the same temperature. It is widely believed that water reacts very readily with liquid electrolytes, so water is damaging to sodium-air batteries.
Currently, in the field of metal-oxygen batteries, high overpotential and low charge and discharge times of the battery are always difficulties to be overcome. The effect of water vapor on the liquid electrolyte during the transition from a metal-oxygen cell to a metal-air cell is again not negligible. Therefore, the development of high-performance and long-life metal-oxygen batteries is of great importance.
Disclosure of Invention
The invention aims to solve the technical problem of providing a high-efficiency all-solid-state sodium-oxygen-water battery, so as to overcome the defects of high overpotential, less charge and discharge times and the like of a metal-oxygen battery in the prior art.
The invention provides a nano metal polymer electrode material, which is obtained by mixing metal nano particles, n-butyl acetate, 1-methoxy-2-propanol acetate and acrylic resin for reaction and standing.
Preferably, in the above electrode material, the metal nanoparticles include one or two of nano silver particles and nano copper particles.
The invention also provides a preparation method of the nano metal polymer electrode material, which comprises the following steps:
mixing metal nano particles, n-butyl acetate, 1-methoxy-2-propanol acetate and acrylic resin for reaction, and standing to obtain the nano metal polymer electrode material, wherein the mass fraction of the metal nano particles is 35-65%, the mass fraction of the n-butyl acetate is 10-30%, the mass fraction of the 1-methoxy-2-propanol acetate is 10-30%, and the mass fraction of the acrylic resin is 5-10% based on the total mass of the metal nano particles, the n-butyl acetate, the 1-methoxy-2-propanol acetate and the acrylic resin.
Preferably, in the above preparation method, the mixing reaction time is 1.5 to 3 hours.
Preferably, in the above preparation method, the standing time is 11 to 13 hours.
The invention also provides an all-solid-state sodium-oxygen-water battery, which comprises the nano metal polymer electrode material.
Preferably, in the all-solid-state sodium-oxygen-water battery, the all-solid-state sodium-oxygen-water battery comprises an anode, a solid ion transport electrolyte and a nano metal polymer electrode material, wherein the nano metal polymer electrode material is a cathode.
More preferably, in the above all-solid sodium-oxygen-water battery, the anode is metallic sodium, and is sealed in a stainless steel container with a solid ceramic electrolyte and an epoxy glue (Locite).
More preferably, in the above all-solid sodium-oxygen-water battery, the solid ion-transport electrolyte is Na-beta "-Al 2 O 3 。
The invention adopts the metal nano polymer positive electrode material for the first time, successfully assembles the all-solid-state sodium-oxygen-water battery which can directly work under certain humidity, and systematically researches the influence of relative humidity on the electrochemical behavior and reaction mechanism of the all-solid-state sodium-oxygen-water battery. All solid state sodium oxygen cells were tested in a dry and wet environment. Electrochemical and chemical mechanisms of the reaction were systematically studied by electrochemical cycling in combination with various in-situ and ex-situ characterization techniques. A key role in performance for humidity effects is disclosed.
The invention carries out systematic research on the current circulation and the characterization of the corresponding discharge products, and clearly shows that NaOH is the main discharge product. Understanding the reaction mechanism and reaction path of sodium-oxygen-water battery under medium humidity condition is significant for the development of sodium-air battery with high performance and long service life from sodium-oxygen battery.
The invention uses solid electrolyte as the ion conductor, which well solves the problem that water has destructive effect on sodium-air battery.
Advantageous effects
The invention synthesizes cathode materials by utilizing metal nano particles and polymers, and assembles a chargeable high-performance all-solid-state sodium-oxygen-water battery. The battery can be recycled for more than 100 times under the environment of medium humidity, and the overpotential is low (the battery is too highThe potential is between 50mV and 75 mV), and the cycle efficiency is high. At O 2 Even if water is introduced in a trace amount, the over-potential of the charge can be even reduced by triggering a solution mechanism. At moderate relative humidity NaOH is the main product, and the system investigated the effect of water on sodium-oxygen-water cells and the complex reaction mechanism.
Drawings
Fig. 1 is a schematic structural diagram of an all-solid-state sodium-oxygen battery of the present invention.
FIG. 2 is a schematic illustration of the preparation of a metal nanoparticle polymer electrode material according to the present invention.
Fig. 3 is a schematic structural diagram of a solid sodium-oxygen-water battery in example 2 of the present invention.
FIG. 4 is a schematic diagram of a current cycling test apparatus according to the present invention.
Fig. 5 is a graph showing the cycle efficiency and cycle times of the nano-silver particle polymer electrode of the present invention compared to other sodium air/oxygen cells using different electrode materials.
Fig. 6 is a schematic diagram of electrochemical characteristics (including charge and discharge cycle number and charge and discharge plateau) of a battery assembled by the nano silver particle polymer electrode of the present invention.
Fig. 7 is an electrochemical graph of a battery assembled from a nano-silver particle polymer electrode (a) and a nano-copper particle polymer electrode (b) according to the present invention.
Detailed Description
The invention will be further illustrated with reference to specific examples. It is to be understood that these examples are illustrative of the present invention and are not intended to limit the scope of the present invention. Further, it is understood that various changes and modifications may be made by those skilled in the art after reading the teachings of the present invention, and such equivalents are intended to fall within the scope of the claims appended hereto.
The electrochemical performance of the battery was tested by using an EC-Lab electrochemical workstation, and the battery was charged and discharged at a current level of 20mA/g for 5 hours and for 5 hours, thus being recorded as a discharge period. The overpotential was calculated as the difference between the charge and discharge plateau. The cycle efficiency is calculated as the ratio of the discharge plateau to the charge plateau.
Example 1
Preparing a nano metal polymer electrode material:
the metal nanoparticle polymer cathode material consisted of metal nanoparticles (nano silver particles) (Alfa-Aesar, 20-40nm, 99.9%), n-butyl acetate (Alfa-Aesar, 99.5%), 1-methoxy-2-propanol acetate (Alfa-Aesar, 99%) and LR white acrylic resin (Sigma-Aldrich) (nano silver particles at 1mg, the latter two esters at 0.6mg, the last resin at 0.25 mg). The synthesis of the material was such that all ingredients were thoroughly mixed by means of magnetic stirring (2 hours). After the completion of the mixing, it was allowed to stand for 12 hours to discharge bubbles in the mixture. Coating the composite material on the solid electrolyte Al by spin coating (with the rotating speed of 6000 rpm) 2 O 3 (commercial Na-. Beta. -Al) 2 O 3 (Ionotec, diameter 10.5mm, thickness 0.7 mm)) to obtain a uniform metal nanoparticle polymer as a cathode material of a battery.
The nano silver particles are replaced by nano copper particles, and the rest are the same as the above, so as to prepare the metal nano particle polymer.
Example 2
Assembly of all-solid-state sodium-oxygen-water battery:
all-solid-state sodium-oxygen-water batteries consist of three main parts: an anode, a solid ion transport electrolyte, and a metal nanoparticle polymer cathode. Metallic sodium (Alfa-Aesar, 99.9%) was used as the anode, and sealed in a self-made stainless steel container with solid ceramic electrolyte and epoxy glue (Locite). Commercial Na-beta "-Al 2 O 3 (Ionotec, diameter 10.5mm, thickness 0.7 mm) was used as both separator and electrolyte in such sodium-oxygen-water cell systems. To avoid oxidation of the sodium electrode (or reaction with atmospheric moisture), the cell was assembled in a pure argon glove box. The specific assembly process comprises the following steps: in a glove box, 5g of a metal sodium block was taken, pressed on one side of the solid electrolyte, pressed, and then the solid electrolyte was covered on a stainless steel tank, and the metal sodium block was then pressed between the solid electrolyte and the stainless steel tank. Then in a solid electrolyte and stainless steel tankUniformly smearing epoxy resin glue between the two layers, and then standing for 12 hours until the epoxy resin glue is fixed. The battery was taken out of the glove box, 1mg of the metal nanoparticle polymer electrode of example 1 (the amount of electrode coated on the surface of the battery was 1 mg) was dropped on the surface of the solid electrolyte, and the electrode was uniformly coated on the surface of the electrolyte at 6000 rpm using a spin coater, and then the battery was put into the glove box and left to stand for 12 hours, thereby obtaining the battery.
Fig. 5 shows that: compared with the cycle efficiency and cycle times in other sodium air/oxygen batteries using different electrode materials, the invention has the advantage that the cycle efficiency and cycle times of the battery are greatly improved compared with those of the same type of battery (the SPC position in the figure).
Fig. 6 shows that: the electrochemical characteristic diagram (comprising the charge and discharge cycle times and the charge and discharge platform) of the invention has the cycle times of 100 circles, and the overpotential between the charge and discharge platforms is very small and is between 50mV and 75 mV.
Fig. 7 shows: compared with a battery assembled by taking nano silver particles as an electrode material, the battery assembled by taking nano copper particles as the electrode material has the advantages that the charging platform is obviously reduced, and the charging overpotential is obviously reduced.
Compared with the prior art, the invention is shown in the following table:
TABLE 1 summary of overpotential, cycle efficiency, and cycle performance of different air electrodes used in the non-aqueous sodium-oxygen and hybrid sodium-air batteries of the present invention
The references are as follows:
1.Hartmann,P.,et al.,A rechargeable room-temperature sodium superoxide(NaO2)battery.Nat Mater,2013.12(3):p.228-32.
2.Li,Y.,et al.,Superior catalytic activity of nitrogen-doped graphene cathodes for high energy capacity sodium-air batteries.Chem Commun(Camb),2013.49(100):p.11731-3.
3.Xu,S.,et al.,A rechargeable Na–CO2/O2battery enabled by stable nanoparticle hybrid electrolytes.J.Mater.Chem.A,2014.2(42):p.17723-17729.
4.Sun,Q.,et al.,Self-stacked nitrogen-doped carbon nanotubes as long-life air electrode for sodium-air batteries:Elucidating the evolution of discharge product morphology.Nano Energy,2015.12:p.698-708.
5.Zhang,S.,et al.,Graphene nanosheets loaded with Pt nanoparticles with enhanced electrochemical performance for sodium–oxygen batteries.Journal of Materials Chemistry A,2015.3(6):p.2568-2571.
6.Hu,Y.,et al.,Porous perovskite calcium–manganese oxide microspheres as an efficient catalyst for rechargeable sodium–oxygen batteries.Journal of Materials Chemistry A,2015.3(7):p.3320-3324.
7.Yin,W.W.,et al.,A long-life Na-air battery based on a soluble NaI catalyst.Chem Commun(Camb),2015.51(12):p.2324-7.
8.Kwak,W.-J.,et al.,Nanoconfinement of low-conductivity products in rechargeable sodium–air batteries.Nano Energy,2015.12:p.123-130.
9.Ma,J.-l.,et al.,Synthesis of porous and metallic CoB nanosheets towards a highly efficient electrocatalyst for rechargeable Na–O2 batteries.Energy&Environmental Science,2018.11(10):p.2833-2838.
10.Sahgong,S.H.,et al.,Rechargeable aqueous Na–air batteries:Highly improved voltage efficiency by use of catalysts.Electrochemistry Communications,2015.61:p.53-56.
11.Senthilkumar,B.,et al.,Exploration of cobalt phosphate as a potential catalyst for rechargeable aqueous sodium-air battery.Journal of Power Sources,2016.311:p.29-34.
12.Khan,Z.,et al.,Hierarchical urchin-shaped α-MnO2 on graphene-coated carbon microfibers:a binder-free electrode for rechargeable aqueous Na–air battery.NPG Asia Materials,2016.8(7):p.e294-e294.
13.Khan,Z.,et al.,Carambola-shaped VO2 nanostructures:a binder-free air electrode for an aqueous Na–air battery.Journal of Materials Chemistry A,2017.5(5):p.2037-2044.
14.Kang,Y.,et al.,Dual–phase Spinel MnCo2O4 Nanocrystals with Nitrogen-doped Reduced Graphene Oxide as Potential Catalyst for Hybrid Na–Air Batteries.Electrochimica Acta,2017.244:p.222-229.
15.Khan,Z.,et al.,Three-dimensional SnS2 nanopetals for hybrid sodium-air batteries.Electrochimica Acta,2017.257:p.328-334.
16.Kim,M.,H.Ju,and J.Kim,Single crystalline Bi2Ru2O7 pyrochlore oxide nanoparticles as efficient bifunctional oxygen electrocatalyst for hybrid Na-air batteries.Chemical Engineering Journal,2019.358:p.11-19.
17.Kim,M.,H.Ju,and J.Kim,Single crystalline thallium rhodium oxide pyrochlore for highly improved round trip efficiency of hybrid Na-air batteries.Dalton Trans,2018.47(42):p.15217-15225.
Claims (7)
1. the nano metal polymer all-solid-state sodium-oxygen-water electrolytic electrode material is characterized in that metal nano particles, n-butyl acetate, 1-methoxy-2-propanol acetate and acrylic resin are mixed and reacted, and the mixture is stood for obtaining, wherein the mass fraction of the metal nano particles is 35% -65%, the mass fraction of the n-butyl acetate is 10% -30%, the mass fraction of the 1-methoxy-2-propanol acetate is 10% -30%, and the mass fraction of the acrylic resin is 5% -10% based on the total mass of the metal nano particles, the n-butyl acetate, the 1-methoxy-2-propanol acetate and the acrylic resin; the metal nano particles comprise one or two of nano silver particles and nano copper particles; the mixing reaction time is 1.5-3 h.
2. A method of preparing a nano-metal polymer all-solid sodium-oxygen-water electrolysis electrode material according to claim 1, comprising:
mixing metal nano particles, n-butyl acetate, 1-methoxy-2-propanol acetate and acrylic resin for reaction, and standing to obtain the nano metal polymer electrode material, wherein the mass fraction of the metal nano particles is 35-65%, the mass fraction of the n-butyl acetate is 10-30%, the mass fraction of the 1-methoxy-2-propanol acetate is 10-30%, and the mass fraction of the acrylic resin is 5-10% based on the total mass of the metal nano particles, the n-butyl acetate, the 1-methoxy-2-propanol acetate and the acrylic resin.
3. The preparation method according to claim 2, wherein the standing time is 11-13 hours.
4. An all-solid sodium-oxygen-water battery comprising the nano-metal polymer all-solid sodium-oxygen-water battery electrode material of claim 1.
5. The all-solid sodium-oxygen-water battery of claim 4, wherein the all-solid sodium-oxygen-water battery comprises an anode, a solid ion-transport electrolyte, and a nano-metal polymer electrode material.
6. The all-solid-state sodium-oxygen-water battery of claim 5, wherein the anode is sodium metal, sealed in a stainless steel container with a solid ceramic electrolyte and an epoxy glue.
7. The all-solid-state sodium-oxygen-water battery of claim 5, wherein the solid-state ion transport electrolyte is Na- β "-Al 2 O 3 。
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| JP6203139B2 (en) * | 2014-07-02 | 2017-09-27 | 冨士色素株式会社 | Composition, electrode having porous layer containing the composition, and metal-air secondary battery having the electrode |
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