CN109411739A - A kind of self power generation, the Zn-CoNC zinc and air cell of long-life and its application - Google Patents

A kind of self power generation, the Zn-CoNC zinc and air cell of long-life and its application Download PDF

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CN109411739A
CN109411739A CN201811015261.5A CN201811015261A CN109411739A CN 109411739 A CN109411739 A CN 109411739A CN 201811015261 A CN201811015261 A CN 201811015261A CN 109411739 A CN109411739 A CN 109411739A
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conc
zif
zinc
air cell
nano material
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CN109411739B (en
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卢锡洪
朱琳
于明浩
曾银香
童叶翔
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Sun Yat Sen University
National Sun Yat Sen University
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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
    • H01M4/86—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
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B82—NANOTECHNOLOGY
    • B82Y—SPECIFIC USES OR APPLICATIONS OF NANOSTRUCTURES; MEASUREMENT OR ANALYSIS OF NANOSTRUCTURES; MANUFACTURE OR TREATMENT OF NANOSTRUCTURES
    • B82Y30/00—Nanotechnology for materials or surface science, e.g. nanocomposites
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • 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
    • 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
    • H01M4/36—Selection of substances as active materials, active masses, active liquids
    • H01M4/38—Selection of substances as active materials, active masses, active liquids of elements or alloys
    • H01M4/42—Alloys based on zinc
    • 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
    • H01M4/8663—Selection of inactive substances as ingredients for catalytic active masses, e.g. binders, fillers
    • H01M4/8673—Electrically conductive fillers
    • 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
    • H01M4/88—Processes of manufacture
    • H01M4/8825—Methods for deposition of the catalytic active composition
    • 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
    • H01M4/90—Selection of catalytic material
    • H01M4/9041—Metals or alloys
    • 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
    • H01M4/90—Selection of catalytic material
    • H01M4/9075—Catalytic material supported on carriers, e.g. powder carriers
    • H01M4/9083—Catalytic material supported on carriers, e.g. powder carriers on carbon or graphite
    • 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

Abstract

The present invention provides a kind of self power generation, the Zn-CoNC zinc and air cell of long-life, the just extremely CoNC Al of the Zn-CoNC battery2O3Nano material, cathode are business Zn piece；The CoNC@Al2O3Nano material is that Zn/Co-ZIF first is prepared using hydro-thermal method in substrate, and then by ALD technique for atomic layer deposition, Zn/Co-ZIF@Al is made in deposition of aluminium oxide in Zn/Co-ZIF nano material2O3, last Zn/Co-ZIF@Al2O3In N2With 500 DEG C ~ 900 DEG C high annealings under atmosphere, CoNC@Al is obtained2O3Nano material.The present invention passes through the conductive Al that ALD technique for atomic layer deposition wraps up one layer of high stability on Zn/Co-ZIF first2O3, while so that it is had superior ORR and OER performance, further promoted Zn-CoNC battery cyclical stability, finally obtain with high-energy density, long-life, can self power generation Zn-CoNC zinc and air cell flexible, have great application prospect in terms of energy storage.

Description

A kind of self power generation, the Zn-CoNC zinc and air cell of long-life and its application
Technical field
The invention belongs to electrochemical energy storage cell technical fields, more particularly, to a kind of self power generation, the Zn- of long-life CoNC zinc and air cell and its application.
Background technique
With the sharp increase of world population and the continuous development of human society, people increasingly increase the various demands of the energy Long, traditional fossil energy cannot obviously meet future society to the various demands of the energy for a long time.In addition, with electronic technology Rapid development, various portable electronic products it is a large amount of universal, demand of the people to electrochmical power source is continuously increased, to its performance It is required that being also continuously improved.However, a series of new green energy such as wind energy, solar energy, geothermal energy, ocean energy is often deposited The problem of landing pit is unevenly distributed weighing apparatus, it usually needs be translated into electric energy and be just easy to use.Therefore, the depth of new energy is realized Degree exploitation and efficiently utilize, develop high-energy-density, cleaning, safety electrochmical power source system become social development important need.
In this context, people expand a series of research to zinc and air cell.Zinc and air cell is the chemistry of first use The energy, be with the oxygen in air as a positive electrode active material, using metallic zinc as the battery of negative electrode active material.Air electrode benefit Energy is exported with the reduction of oxygen in air, and itself is not consumed during the reaction, therefore the capacity of zinc and air cell is only dependent upon The dosage of metallic zinc.Just since zinc and air cell system has specific energy height, discharging voltage balance, cheap and to environmental compatible Etc. special advantages, thus become energy field actively develops in recent years one of hot spot system, be with a wide range of applications.Though The advantage that right zinc and air cell has other batteries incomparable, however since it is open system, cause using when there are many Problem, thus limit its commercialization process.The major obstacle of alkaline zinc and air cell development be battery in active state vulnerable to The influence of environment and electrolyte " dry " or the moisture absorption and carbonating occurs.This is mainly due to zinc and air cell cathode active materials (oxygen) must be entered in battery by the external world, and battery could work normally.Battery need to not only absorb oxygen from external environment in this way, but also There is also with the exchanging of other substances (such as moisture content exchange and absorbing carbon dioxide).Just due to the influence of water and carbon dioxide, and Lead to fan-out capability decline and the capacity attenuation of battery.In addition, the opening of zinc and air cell, also brings centainly to cell sealing Difficulty, this be all zinc and air cell commercialization must solve the problems, such as.Further, since its open structure make battery design and Electrode process has the difficulty of particularity, causes zinc and air cell so far still without widely commercialization and application.
Therefore, it explores and is suitble to industrialized air electrode new preparation technology, it is current for how improving its continuous use time Significant challenge.
Summary of the invention
The purpose of the present invention is to provide a kind of self power generation, the long-life, stable circulation Zn-CoNC zinc and air cell.
Another object of the present invention is to provide above-mentioned self power generation, the long-life, stable circulation Zn-CoNC zinc and air cell Using.
The present invention is effectively utilized atomic deposition technique, and one layer of Al is coated on CoNC material2O3Protective film makes composition Zn-CoNC stability test is significantly promoted, and substantially increases it and the time is used continuously.
Above-mentioned technical purpose of the invention is achieved through the following technical solutions:
In technical solution of the present invention, by the temperature and time of adjusting hydrothermal, to grow one layer in flexible carbon cloth substrate Granular size and the Zn/Co-ZIF nano particle being evenly distributed；By setting suitable ALD atomic layer deposition temperature and aluminium oxide Thickness degree coats the highly conductive aluminium oxide that a layer thickness is suitable, performance is stable on the surface Zn/Co-ZIF, to make CoNC@Al2O3 The stability of positive electrode gets a promotion；By being made annealing treatment under suitable atmosphere with certain temperature, it is finally obtained A kind of high crystalline, the CoNC@Al haveing excellent performance2O3Electrode material.
Technical solution of the present invention is specifically:
A kind of self power generation, the Zn-CoNC zinc and air cell of long-life, the just extremely CoNC Al of the Zn-CoNC battery2O3Nanometer Material, cathode are business Zn piece；
The CoNC@Al2O3Nano material is that Zn/Co-ZIF first is prepared using hydro-thermal method in carbon cloth substrate, is then led to ALD technique for atomic layer deposition is crossed, Zn/Co-ZIF@Al is made in deposition of aluminium oxide in Zn/Co-ZIF nano material2O3, finally Zn/Co-ZIF@Al2O3In N2Under atmosphere with 500 DEG C~900 DEG C high annealing 1~10 hour, obtain CoNC@Al2O3Nanometer material Material；
The condition of hydro-thermal reaction is hydro-thermal reaction 2~4 hours at a temperature of 120 DEG C, up to Zn/Co-ZIF nanometers after drying after hydro-thermal Material；
0.5~1.5mmol zinc nitrate and 1~5mmol cobalt nitrate are added in 80mL methanol solution, separately by the first of 3.0~4.0g Base imidazoles is added in 80mL methanol solution, and the two mixing is used as hydrothermal solution, the hydro-thermal 2 under the conditions of in carbon cloth substrate with 120 DEG C ~4 hours, up to Zn/Co-ZIF nano material after the carbon cloth drying that hydro-thermal is obtained.
Preferably, by ALD technique for atomic layer deposition, on the carbon cloth of growth Zn/Co-ZIF deposition of aluminium oxide to get Zn/Co-ZIF@Al2O3, actual conditions are as follows: forerunner source is trimethyl aluminium and water, and temperature is 50 DEG C~180 DEG C, and coating film thickness is 20~200cycles.
Preferably, the business Zn piece with a thickness of 0.15-0.25mm.
Preferably, Zn/Co-ZIF@Al2O3In N2Under atmosphere with 700 DEG C high annealing 1~2 hour.
Preferably, by ALD technique for atomic layer deposition, forerunner source is trimethyl aluminium and water, and temperature is 180 DEG C, plates film thickness Degree is 50cycles.
Compared with the existing technology, the present invention has the advantage that and effect:
Nano-electrode material CoNC@Al has directly been synthesized in the present invention on flexible carrier2O3Anode not only increases electrode material The specific surface area of material, and it is effectively increased the performance of Zn-CoNC battery, and cathode uses commercial zinc metal sheet, so as to answer For flexible Zn-CoNC battery assembly.Meanwhile the conductive Al of one layer of suitable thickness is coated in CoNC electrode surface2O3Nanometer material Material, so that Zn/Co-ZIF particle is able to maintain original crystal form in calcination process.In addition, additionally using solid gel Electrolyte, it is both above-mentioned to combine, the performance of the ORR/OER of zinc and air cell on the one hand can be improved, it on the other hand can be into one Step promotes the cyclical stability of Zn-CoNC battery, so as to improve the cycle life of Zn-CoNC battery.
Detailed description of the invention
Fig. 1: being (a) scanning electron microscope (SEM) picture of CoNC electrode in embodiment 1, is (b) CoNC@in embodiment 1 Al2O3Scanning electron microscope (SEM) picture of electrode.
Fig. 2 is CoNC@Al in embodiment 12O3The X-ray powder diffraction figure of electrode.
Fig. 3: being (a) CoNC@Al in embodiment 12O3The ORR curve of battery is (b) CoNC@Al in embodiment 12O3Electricity The OER curve in pond is (c) the cycle life test curve of battery in embodiment 1.
Specific embodiment
Further illustrate the present invention below in conjunction with specific embodiments and the drawings, but embodiment the present invention is not done it is any The restriction of form.Unless stated otherwise, the present invention uses reagent, method and apparatus is the art conventional reagents, method And equipment.
Unless stated otherwise, agents useful for same and material of the present invention are commercially available.
Embodiment 1
Zn/Co-ZIF positive electrode is synthesized by what hydrothermal method was realized on flexible carbon cloth.To surpass in dehydrated alcohol The commercial carbon cloth (2cm × 3cm) of sonication after ten minutes is used as flexible substrates, and 1mmol zinc nitrate and 4mmol cobalt nitrate are added Enter in 80mL methanol solution, separately 3.7g methylimidazole is added in 80mL methanol solution, the two mixing is used as hydrothermal solution, water Hot temperature is 120 DEG C, and the time is 2 hours.Al2O3Layer is obtained by ALD atomic layer deposition, and forerunner source is trimethyl aluminium (TMA) with water (H2O), temperature is 60 DEG C, coating film thickness: 20cycles.
Finally by Zn/Co-ZIF@Al2O3In N2Under atmosphere with 700 DEG C high annealing 1~2 hour, obtain CoNC@Al2O3 Nano material；
Zn negative electrode material is first polished smooth, it is ensured that contact is abundant using the business zinc metal sheet of thinner thickness using preceding.
Performance test: to CoNC the and CoNC@Al of preparation2O3Electrode has carried out the test of Flied emission scanning electron microscopy Electronic Speculum, As a result as shown in Figure 1, scanning electron microscope diagram is shown grown one layer of uniform granular size on flexible carbon cloth fiber Moderate Zn/Co-ZIF nano particle is deposited with one layer of Al2O3Particle be still able to maintain its original crystal form after the annealing process.Figure 2, which use X-ray powder diffraction, tests, and test result shows to test resulting CoNC@Al2O3Positive crystallization degree is higher.Figure 3a, b use the line style sweep test test in electrochemical method to study ORR the and OER performance of Zn-CoNC battery, pass through Curve, which can be seen that this Zn-CoNC battery, good ORR and OER performance, and has Al2O3The material property of layer is more It is excellent.In addition, still having good stable circulation after the continuous charge and discharge for a long time of this Zn-CoNC battery it can be seen from Fig. 3 c Property.In conclusion this Zn-CoNC battery has long-life, self power generation, high circulation stability, have in terms of energy storage Very big application prospect.
Embodiment 2-10
The operating process of embodiment 2-13 is same as Example 1, and difference is time and the ALD of hydrothermal synthesis Zn/Co-ZIF The temperature of deposition of aluminium oxide and its coating film thickness.
Specific hydrothermal synthesis time, synthesis temperature, the temperature of ALD deposition aluminium oxide and its coating film thickness and each embodiment The results are shown in Table 1.
The time-controllable of 1. hydrothermal synthesis of table
In conclusion the obtained material property of embodiment 13 its to analyse oxygen to play spike potential be 1.647V, measured spike potential plays peak Current potential is smaller (close to zero), illustrates that its performance is better, which is optimum condition.

Claims (6)

1. the Zn-CoNC zinc and air cell of a kind of self power generation, long-life, which is characterized in that the Zn-CoNC battery just extremely CoNC@Al2O3Nano material, cathode are business Zn piece；
The CoNC@Al2O3Nano material is that Zn/Co-ZIF first is prepared using hydro-thermal method in carbon cloth substrate, is then passed through ALD technique for atomic layer deposition, Zn/Co-ZIF@Al is made in deposition of aluminium oxide in Zn/Co-ZIF nano material2O3, last Zn/ Co-ZIF@Al2O3In N2Under atmosphere with 500 DEG C ~ 900 DEG C high annealing 1 ~ 10 hour, obtain CoNC@Al2O3Nano material；
The condition of hydro-thermal reaction is hydro-thermal reaction 2 ~ 4 hours at a temperature of 120 DEG C, up to Zn/Co-ZIF nanometers after drying after hydro-thermal Material；
0.5 ~ 1.5mmol zinc nitrate and 1 ~ 5mmol cobalt nitrate are added in 80mL methanol solution, separately by the methyl of 3.0 ~ 4.0 g Imidazoles is added in 80mL methanol solution, and the two mixing is used as hydrothermal solution, the hydro-thermal 2 ~ 4 under the conditions of in carbon cloth substrate with 120 DEG C Hour, up to Zn/Co-ZIF nano material after the carbon cloth drying that hydro-thermal is obtained.
2. Zn-CoNC zinc and air cell according to claim 1, which is characterized in that by ALD technique for atomic layer deposition, Deposition of aluminium oxide is on the carbon cloth of growth Zn/Co-ZIF to get Zn/Co-ZIF@Al2O3, actual conditions are as follows: forerunner source is trimethyl Aluminium and water, temperature are 50 DEG C ~ 180 DEG C, and coating film thickness is 20 ~ 200cycles.
3. Zn-CoNC zinc and air cell according to claim 1, which is characterized in that the business Zn piece with a thickness of 0.15- 0.25mm。
4. Zn-CoNC zinc and air cell according to claim 1, which is characterized in that Zn/Co-ZIF@Al2O3In N2Under atmosphere With 700 DEG C high annealing 1 ~ 2 hour.
5. Zn-CoNC zinc and air cell according to claim 2, which is characterized in that preceding by ALD technique for atomic layer deposition Drive source is trimethyl aluminium and water, and temperature is 180 DEG C, coating film thickness 50cycles.
6. any Zn-CoNC zinc and air cell of claim 1 to 5 is preparing the application in energy storage material.
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Publication number Priority date Publication date Assignee Title
CN110429284A (en) * 2019-07-01 2019-11-08 中山大学 A kind of high capacity, powerful flexible Zinc ion battery and its application
CN112072087A (en) * 2020-08-25 2020-12-11 浙江工业大学 Preparation method and application of zinc ion battery negative electrode composite material
CN112072087B (en) * 2020-08-25 2022-02-18 浙江工业大学 Preparation method and application of zinc ion battery negative electrode composite material
CN112090441A (en) * 2020-09-28 2020-12-18 浙江师范大学 Preparation method, product and application of cobalt-based carbon nano material
CN112090441B (en) * 2020-09-28 2023-04-25 浙江师范大学 Preparation method, product and application of cobalt-based carbon nanomaterial
CN114807975A (en) * 2022-06-22 2022-07-29 国家电投集团氢能科技发展有限公司 Non-noble metal oxygen evolution catalyst and preparation method and application thereof
CN114807975B (en) * 2022-06-22 2022-09-09 国家电投集团氢能科技发展有限公司 Non-noble metal oxygen evolution catalyst and preparation method and application thereof

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