CN112952214A - Aqueous zinc ion battery and preparation method thereof - Google Patents

Aqueous zinc ion battery and preparation method thereof Download PDF

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CN112952214A
CN112952214A CN201911256502.XA CN201911256502A CN112952214A CN 112952214 A CN112952214 A CN 112952214A CN 201911256502 A CN201911256502 A CN 201911256502A CN 112952214 A CN112952214 A CN 112952214A
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zinc
ion battery
electrode
aqueous
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付旭东
刘清亭
胡圣飞
张�荣
倪虎
张帅
温杰欣
舒文黎
王行雨
邵鑫宇
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Hubei University of Technology
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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
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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
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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
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    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/10—Energy storage using batteries
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Abstract

The invention discloses a water-based zinc ion battery and a preparation method thereof. The electrolyte comprises a positive electrode, a negative electrode, electrolyte and a diaphragm arranged between the positive electrode and the negative electrode, wherein the positive electrode is a conductive polymer nanowire array, and the negative electrode is a zinc nanosheet array. The preparation method comprises the following steps: (a) preparing a positive conductive polymer nanowire array; (b) preparing a negative electrode zinc nanosheet array; (c) and (3) preparing an aqueous zinc ion battery. The invention has the following advantages: the positive electrode and the negative electrode are in ordered structures, so that the transmission of zinc ions can be promoted, and the rate capability and the power density of the water system zinc ion battery can be improved; the active material in the electrode is directly connected with the current collector, so that the internal resistance of the battery is reduced; the electrode active material grows on the current collector in situ, and a binder is not needed, so that the weight and the cost are reduced, and the proportion of active substances is increased.

Description

Aqueous zinc ion battery and preparation method thereof
Technical Field
The invention relates to the technical field of zinc ion batteries, in particular to a water system zinc ion battery with ordered positive and negative electrodes and a preparation method thereof.
Background
With the development of wearable electronic products, mobile communication and electric vehicles, energy devices with high energy density and high power density are urgently needed. The lithium ion battery is a common energy device in the modern society, and lithium is more active and limited in lithium resources, so that the lithium ion battery is poor in safety and high in price. Compared with a lithium ion battery, the zinc ion battery can use an aqueous solution as an electrolyte, has better safety, and is rich in zinc storage in the earth crust and not limited by resources, so the water system zinc ion battery is a current research hotspot.
The radius of zinc ions is far larger than that of lithium ions, so that the electrode material of the zinc ion battery is more easily damaged in the charging and discharging processes; and secondly, the zinc ions move slowly, so that the cycling stability and the high-rate charge and discharge performance of the zinc ion battery are poor. Chinese patent (CN 108807910A) invented a water-based zinc ion battery, in which graphene-assisted zinc negative electrodes are applied to a water-based zinc ion battery system, and the stability and conductivity of the zinc negative electrodes are enhanced by graphene with excellent performance and stable structure, so that the ring stability of the water-based zinc ion battery is increased, but the large-rate charge-discharge performance of the water-based zinc ion battery is not obviously improved. In view of the above, the invention constructs the ordered positive and negative electrodes and assembles the water-based zinc ion battery, and the ordered electrodes can strengthen the transmission of zinc ions, thereby increasing the large-rate charge and discharge performance of the battery.
Disclosure of Invention
In view of the defects of the prior art, the invention aims to construct an ordered positive electrode and an ordered negative electrode and assemble an aqueous zinc ion battery, so as to strengthen zinc ion transmission and increase the high-rate charge and discharge performance of the battery.
In order to achieve the purpose, the invention adopts the following technical scheme:
in a first aspect, the present invention provides an aqueous zinc-ion battery, characterized in that: the cathode is a conductive polymer nanowire array, and the cathode is a zinc nanosheet array; the conductive polymer nanowire array and the zinc nanosheet array are loaded on a conductive substrate, the conductive substrate is carbon fiber cloth, carbon fiber paper or carbon felt, and the conductive substrate can serve as a current collector.
Preferably, the conductive polymer is one or more of polyaniline or polyaniline derivatives, polypyrrole or polypyrrole derivatives, polythiophene or polythiophene derivatives, and mixtures of two or more of the polyaniline or polyaniline derivatives, the polypyrrole or polypyrrole derivatives, and the polythiophene or polythiophene derivatives.
Further, the electrolyte is an aqueous solution of zinc salt.
Further, the separator is a non-woven fabric separator or a glass fiber separator.
Further, the separator is a non-woven fabric separator or a glass fiber separator.
Furthermore, the aqueous solution of the zinc salt is one or a mixture of two or more of zinc sulfate, zinc nitrate, zinc chloride, zinc acetate and zinc trifluoromethanesulfonate, and the concentration of zinc ions in the aqueous solution is 0.1mol/L to 10 mol/L.
In a second aspect, the present invention provides a method for producing the aqueous zinc-ion battery, comprising: the method comprises the following steps:
(a) preparing a positive conductive polymer nanowire array:
preparing a conducting polymer nanowire array by adopting an electrochemical method, wherein a conducting substrate is a working electrode, a graphite sheet is a counter electrode, and a saturated calomel electrode is a reference electrode; carrying out electrochemical polymerization reaction in a mixed solution of one or more than two of aniline or aniline derivatives, pyrrole or pyrrole derivatives, and thiophene or thiophene derivatives, and obtaining a conductive polymer nanowire array in situ on a conductive substrate as a positive electrode;
(b) preparing a negative electrode zinc nanosheet array:
preparing a zinc nanosheet array by adopting an electrochemical method, wherein the conductive substrate is a working electrode, the graphite sheet is a counter electrode, and the saturated calomel electrode is a reference electrode; electrodepositing in zinc sulfate aqueous solution, and electrodepositing a zinc nanosheet array in situ on a conductive substrate to serve as a negative electrode;
(c) preparation of an aqueous zinc ion battery:
and pressing the positive electrode and the negative electrode on two sides of the diaphragm, dripping electrolyte, and sealing to obtain the water-based zinc ion battery.
Preferably, the sum of the mixed concentration of one or more of aniline or aniline derivatives, pyrrole or pyrrole derivatives, thiophene or thiophene derivatives in the solution in the step (a) is 0.1mol/L to 2 mol/L; adding a doping agent into the solution obtained in the step (a), wherein the doping agent is any one of hydrochloric acid, sulfuric acid, perchloric acid, phosphoric acid, p-toluenesulfonic acid or naphthalenesulfonic acid; the concentration of the dopant in the solution is 0.1mol/L to 2 mol/L; the current density of the electropolymerization of step (a) is 0.05mA cm-2To 2mA cm-2Electropolymerization time is 18min to 720 min;
further, the concentration of zinc sulfate in the solution in the step (b) is 0.1mol/L to 2mol/L, sodium sulfate and boric acid are added into the solution, the concentration of sodium sulfate is 0.2mol/L to 4mol/L, and the concentration of boric acid is 0.1mol/L to 1 mol/L; the current density of the electrodeposition in the step (b) is-10 mA cm-2To-100 mA cm-2The electrodeposition time is 10min to 160 min.
Compared with the prior art, the invention has the following advantages and beneficial effects:
(1) the positive and negative electrodes of the water system zinc ion battery are in an ordered structure, so that the transmission of zinc ions can be promoted, and the rate capability and the power density of the zinc ion battery can be improved;
(2) the electrode active substance in the water system zinc ions is directly connected with the current collector, so that the internal resistance of the battery is reduced;
(3) the electrode active material in the water system zinc ions grows on the current collector in situ, and a binder is not needed, so that the weight and the cost are reduced, and the proportion of active substances is increased.
Drawings
FIG. 1 is an SEM image of a polyaniline nanowire array prepared in example 1;
FIG. 2 is an SEM image of a zinc nanosheet array prepared in example 1;
fig. 3 is the rate performance of the aqueous zinc-ion battery of example 1;
FIG. 4 is an SEM image of a polyaniline nanowire array prepared in example 2;
FIG. 5 is an SEM image of a polyaniline nanowire array prepared in example 3;
FIG. 6 is an SEM image of a zinc nanosheet array prepared in example 4;
FIG. 7 is an SEM image of the polypyrrole nanowire array prepared in example 5;
FIG. 8 is an SEM image of a polyaniline prepared in a comparative example;
fig. 9 is a graph showing rate performance of a comparative example aqueous zinc-ion battery.
Detailed Description
For a better understanding of the present invention, the present invention will be further explained in detail with reference to the accompanying drawings and specific examples, but the present invention is not limited to the following examples.
Example 1
(1) Preparing a positive conductive polymer nanowire array:
adding 4.65g aniline (0.05mol) into 100mL 1mol/L perchloric acid aqueous solution as electrolyte, immersing a conductive substrate into the electrolyte as a working electrode, using a graphite sheet as a counter electrode and a saturated calomel electrode as a reference electrode, and carrying out electrochemical polymerization through an electrochemical workstation, wherein the current density is 0.2mA cm-2Polymerizing for 180min to obtain polyaniline nanowire array as the anode material;
(2) preparing a negative electrode zinc nanosheet array:
adding 12.5g of zinc sulfate heptahydrate (0.043mol), 12.5g of sodium sulfate (0.088mol) and 2g of boric acid (0.032mol) into 100mL of deionized water to serve as an electrolyte, immersing a conductive substrate into the electrolyte to serve as a working electrode, using a graphite sheet as a counter electrode and a saturated calomel electrode as a reference electrode, and carrying out electrodeposition through an electrochemical workstation at a current density of-20 mA cm-2The electrodeposition time is 20min, and a zinc nanosheet array is obtained and used as a negative electrode material;
(3) preparation of an aqueous zinc ion battery:
and pressing the positive electrode and the negative electrode on two sides of the glass fiber diaphragm, dropwise adding 2mol/L zinc chloride electrolyte, sealing to obtain the water-system zinc ion battery, and performing performance test.
Example 2
(1) Preparing a positive conductive polymer nanowire array:
adding 4.65g aniline (0.05mol) into 100mL 1mol/L perchloric acid aqueous solution as electrolyte, immersing a conductive substrate into the electrolyte as a working electrode, using a graphite sheet as a counter electrode and using a saturated calomel electrode as a reference electrode, and carrying out electrochemical polymerization on an electrochemical workstation at a current density of 0.1mA cm-2Polymerizing for 360min to obtain polyaniline nanowire array as the anode material;
(2) preparing a negative electrode zinc nanosheet array:
adding 12.5g of zinc sulfate heptahydrate (0.043mol), 12.5g of sodium sulfate (0.088mol) and 2g of boric acid (0.032mol) into 100mL of deionized water to serve as an electrolyte, immersing a conductive substrate into the electrolyte to serve as a working electrode, immersing a graphite sheet as a counter electrode and a saturated calomel electrode as a reference electrode, and carrying out electrodeposition on an electrochemical workstation at a current density of-20 mA cm-2The electrodeposition time is 20min, and a zinc nanosheet array is obtained and used as a negative electrode material;
(3) preparation of an aqueous zinc ion battery:
and pressing the positive electrode and the negative electrode on two sides of the glass fiber diaphragm, dropwise adding 2mol/L zinc chloride electrolyte, sealing to obtain the water-system zinc ion battery, and performing performance test.
Example 3
(1) Preparing a positive conductive polymer nanowire array:
adding 4.65g aniline (0.05mol) into 100mL 1mol/L perchloric acid aqueous solution as electrolyte, immersing a conductive substrate into the electrolyte as a working electrode, using a graphite sheet as a counter electrode and using a saturated calomel electrode as a reference electrode, and carrying out electrochemical polymerization on an electrochemical workstation at a current density of 0.15mA cm-2The polymerization time is 240min, and the polyaniline nanowire array is obtained and used as the anode material;
(2) preparing a negative electrode zinc nanosheet array:
adding 12.5g of zinc sulfate heptahydrate (0.043mol), 12.5g of sodium sulfate (0.088mol) and 2g of boric acid (0.032mol) into 100mL of deionized water to serve as an electrolyte, immersing a conductive substrate into the electrolyte to serve as a working electrode, immersing a graphite sheet as a counter electrode and a saturated calomel electrode as a reference electrode, and carrying out electrodeposition on an electrochemical workstation at a current density of-20 mA cm-2The electrodeposition time is 20min, and a zinc nanosheet array is obtained and used as a negative electrode material;
(3) preparation of an aqueous zinc ion battery:
and pressing the positive electrode and the negative electrode on two sides of the glass fiber diaphragm, dropwise adding 2mol/L zinc chloride electrolyte, sealing to obtain the water-system zinc ion battery, and performing performance test.
Example 4
(1) Preparing a positive conductive polymer nanowire array:
adding 4.65g aniline (0.05mol) into 100mL 1mol/L perchloric acid aqueous solution as electrolyte, immersing a conductive substrate into the electrolyte as a working electrode, using a graphite sheet as a counter electrode and using a saturated calomel electrode as a reference electrode, and carrying out electrochemical polymerization on an electrochemical workstation at a current density of 0.2mA cm-2Polymerizing for 180min to obtain polyaniline nanowire array as the anode material;
(2) preparing a negative electrode zinc nanosheet array:
to 100mL of deionized water were added 12.5g of zinc sulfate heptahydrate (0.043mol), 12.5g of sodium sulfate (0.088mol) and 2g of boric acid (0.032mol) as an electrolyte solutionImmersing an electric substrate into electrolyte as a working electrode, taking a graphite sheet as a counter electrode and taking a saturated calomel electrode as a reference electrode, and carrying out electrodeposition on an electrochemical workstation at a current density of-20 mA cm-2The electrodeposition time is 40min, and the obtained zinc nanosheet array is used as a negative electrode material;
(3) preparation of an aqueous zinc ion battery:
and pressing the positive electrode and the negative electrode on two sides of the glass fiber diaphragm, dropwise adding 2mol/L zinc chloride electrolyte, sealing to obtain the water-system zinc ion battery, and performing performance test.
Example 5
(1) Preparing a positive conductive polymer nanowire array:
adding 3.35g pyrrole (0.05mol) into 100mL of 1mol/L perchloric acid aqueous solution as electrolyte, immersing a conductive substrate into the electrolyte as a working electrode, using a graphite sheet as a counter electrode and using a saturated calomel electrode as a reference electrode, and carrying out electrochemical polymerization on an electrochemical workstation at a current density of 1mA cm-2Polymerizing for 36min to obtain polypyrrole nanowire arrays as anode materials;
(2) preparing a negative electrode zinc nanosheet array:
adding 12.5g of zinc sulfate heptahydrate (0.043mol), 12.5g of sodium sulfate (0.088mol) and 2g of boric acid (0.032mol) into 100mL of deionized water to serve as an electrolyte, immersing a conductive substrate into the electrolyte to serve as a working electrode, immersing a graphite sheet as a counter electrode and a saturated calomel electrode as a reference electrode, and carrying out electrodeposition on an electrochemical workstation at a current density of-20 mA cm-2The electrodeposition time is 20min, and a zinc nanosheet array is obtained and used as a negative electrode material;
(3) preparation of an aqueous zinc ion battery:
and pressing the positive electrode and the negative electrode on two sides of the glass fiber diaphragm, dropwise adding 2mol/L zinc chloride electrolyte, sealing to obtain the water-system zinc ion battery, and performing performance test.
Comparative example
(1) Preparation of positive conductive polymer:
to 100mL of a 1mol/L perchloric acid aqueous solution was added 4.65g of aniline (0.05mol) as an electrolyte, and a conductive substrate was immersedElectrolyte is taken as a working electrode, a graphite sheet is taken as a counter electrode, a saturated calomel electrode is taken as a reference electrode, electrochemical polymerization is carried out on an electrochemical workstation, and the current density is 9mA cm-2Polymerizing for 4min to obtain polyaniline as the anode material;
(2) preparing negative electrode zinc:
directly taking a metal zinc sheet as a negative electrode, and cutting the zinc sheet into a battery with a proper size;
(3) preparation of an aqueous zinc ion battery:
and pressing the positive electrode and the negative electrode on two sides of the glass fiber diaphragm, dropwise adding 2mol/L zinc chloride electrolyte, sealing to obtain the water-system zinc ion battery, and performing performance test.

Claims (9)

1. An aqueous zinc-ion battery characterized in that: the cathode is a conductive polymer nanowire array, and the cathode is a zinc nanosheet array; the conductive polymer nanowire array and the zinc nanosheet array are loaded on a conductive substrate, the conductive substrate is carbon fiber cloth, carbon fiber paper or carbon felt, and the conductive substrate can serve as a current collector.
2. The aqueous zinc-ion battery according to claim 1, characterized in that: the conductive polymer is one or more of polyaniline or polyaniline derivatives, polypyrrole or polypyrrole derivatives, polythiophene or polythiophene derivatives.
3. The aqueous zinc-ion battery according to claim 1 or 2, characterized in that: the electrolyte is an aqueous solution of zinc salt.
4. The aqueous zinc-ion battery according to claim 1 or 2, characterized in that: the diaphragm is a non-woven fabric diaphragm or a glass fiber diaphragm.
5. The aqueous zinc-ion battery according to claim 3, characterized in that: the diaphragm is a non-woven fabric diaphragm or a glass fiber diaphragm.
6. The aqueous zinc-ion battery according to claim 5, characterized in that: the zinc salt aqueous solution is one or a mixture of two or more of zinc sulfate, zinc nitrate, zinc chloride, zinc acetate and zinc trifluoromethanesulfonate, and the concentration of zinc ions in the aqueous solution is 0.1mol/L to 10 mol/L.
7. A method of preparing an aqueous zinc-ion battery as claimed in claim 1 or 2 or 5 or 6, characterized in that: the method comprises the following steps:
(a) preparing a positive conductive polymer nanowire array:
preparing a conducting polymer nanowire array by adopting an electrochemical method, wherein a conducting substrate is a working electrode, a graphite sheet is a counter electrode, and a saturated calomel electrode is a reference electrode; carrying out electrochemical polymerization reaction in a mixed solution of one or more than two of aniline or aniline derivatives, pyrrole or pyrrole derivatives, and thiophene or thiophene derivatives, and obtaining a conductive polymer nanowire array in situ on a conductive substrate as a positive electrode;
(b) preparing a negative electrode zinc nanosheet array:
preparing a zinc nanosheet array by adopting an electrochemical method, wherein the conductive substrate is a working electrode, the graphite sheet is a counter electrode, and the saturated calomel electrode is a reference electrode; electrodepositing in zinc sulfate aqueous solution, and electrodepositing a zinc nanosheet array in situ on a conductive substrate to serve as a negative electrode;
(c) preparation of an aqueous zinc ion battery:
and pressing the positive electrode and the negative electrode on two sides of the diaphragm, dripping electrolyte, and sealing to obtain the water-based zinc ion battery.
8. The method for producing an aqueous zinc-ion battery according to claim 7, characterized in that:
one or more than two of aniline or aniline derivative, pyrrole or pyrrole derivative, thiophene or thiophene derivative in the solution in the step (a) are mixedThe sum of the concentrations of (A) is 0.1mol/L to 2 mol/L; adding a doping agent into the solution obtained in the step (a), wherein the doping agent is any one of hydrochloric acid, sulfuric acid, perchloric acid, phosphoric acid, p-toluenesulfonic acid or naphthalenesulfonic acid; the concentration of the dopant in the solution is 0.1mol/L to 2 mol/L; the current density of the electropolymerization of step (a) is 0.05mA cm-2To 2mA cm-2And the electropolymerization time is 18min to 720 min.
9. The method for producing an aqueous zinc-ion battery according to claim 8, characterized in that:
the concentration of zinc sulfate in the solution in the step (b) is 0.1-2 mol/L, sodium sulfate and boric acid are also added into the solution, the concentration of sodium sulfate is 0.2-4 mol/L, and the concentration of boric acid is 0.1-1 mol/L; the current density of the electrodeposition in the step (b) is-10 mA cm-2To-100 mA cm-2The electrodeposition time is 10min to 160 min.
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Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN113782702A (en) * 2021-08-25 2021-12-10 华中科技大学 Water-based zinc ion battery cathode, preparation method and battery
CN116365055A (en) * 2022-12-26 2023-06-30 起源智能科技(嘉兴)有限公司 Neutral silver-zinc secondary battery based on electrochemical in-situ growth electrode and preparation method thereof

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CN106229498A (en) * 2016-08-04 2016-12-14 武汉理工大学 A kind of negative material being applicable to Water based metal ion battery and preparation method thereof

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Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN113782702A (en) * 2021-08-25 2021-12-10 华中科技大学 Water-based zinc ion battery cathode, preparation method and battery
CN116365055A (en) * 2022-12-26 2023-06-30 起源智能科技(嘉兴)有限公司 Neutral silver-zinc secondary battery based on electrochemical in-situ growth electrode and preparation method thereof

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