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CN110957467B - Bromine ion battery - Google Patents

Bromine ion battery Download PDF

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CN110957467B
CN110957467B CN201911297405.5A CN201911297405A CN110957467B CN 110957467 B CN110957467 B CN 110957467B CN 201911297405 A CN201911297405 A CN 201911297405A CN 110957467 B CN110957467 B CN 110957467B
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ion battery
bromine
battery
electrolyte
bromine ion
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CN110957467A (en
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李明强
李航
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Dalian Xingyuan Liquid Flow Battery Co ltd
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Dalian 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
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
    • H01M4/133—Electrodes based on carbonaceous material, e.g. graphite-intercalation compounds or CFx
    • 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
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • 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
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
    • H01M10/0564—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of organic materials only
    • H01M10/0566—Liquid materials
    • H01M10/0568—Liquid materials characterised by the solutes
    • 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
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
    • H01M10/0564—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of organic materials only
    • H01M10/0566—Liquid materials
    • H01M10/0569—Liquid materials characterised by the solvents
    • 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
    • H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
    • H01M4/134—Electrodes based on metals, Si 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
    • H01M4/02—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
    • 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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    • 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
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/36—Selection of substances as active materials, active masses, active liquids
    • H01M4/58—Selection of substances as active materials, active masses, active liquids of inorganic compounds other than oxides or hydroxides, e.g. sulfides, selenides, tellurides, halogenides or LiCoFy; of polyanionic structures, e.g. phosphates, silicates or borates
    • H01M4/583—Carbonaceous material, e.g. graphite-intercalation compounds or CFx
    • H01M4/587—Carbonaceous material, e.g. graphite-intercalation compounds or CFx for inserting or intercalating light metals
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    • H01M2004/026—Electrodes composed of, or comprising, active material characterised by the polarity
    • H01M2004/027—Negative electrodes
    • H—ELECTRICITY
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    • H01M2004/026—Electrodes composed of, or comprising, active material characterised by the polarity
    • H01M2004/028—Positive electrodes
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Abstract

The invention provides a bromine ion battery, and belongs to the field of batteries. The battery adopts carbon black as an intercalation material of bromide ions, adopts ammonium bromide with the concentration of 1-2mol/L in a glycol non-aqueous system as electrolyte, and adopts three coordination metals of zinc, copper or nickel as a negative electrode material of the bromide ion battery to assemble the soft package battery. The invention provides a bromine ion battery based on the intercalation principle of bromine ions in a carbon material, and the bromine ions avoid the defects of toxicity, volatility and the like of elemental bromine and improve the safety of the battery. Meanwhile, the carbon black is low in price, the cost of the bromine ion battery is reduced, and the large-scale popularization is facilitated. The ethylene glycol ammonium bromide electrolyte of the non-aqueous system avoids the hydrogen evolution and oxygen evolution reaction, thereby ensuring the bromine ion battery to be stable in circulation and fully exerting the characteristic of high theoretical specific capacity of bromine ions. Three metals of zinc, copper and nickel are used as cathode materials of the bromine ion battery, so that the battery cost is reduced, and a theoretical basis is provided for the research of the cathode of the non-metal ion battery.

Description

Bromine ion battery
Technical Field
The invention relates to the field of batteries, and provides a novel bromine ion battery.
Background
In recent years, due to the demand for large-scale energy storage and the electrolyte safety and cost problems of commercial lithium batteries, the search for new ion batteries is becoming more urgent. Bromine due to its higher theoretical specific capacity (335 mAh/g)Br2) The method is widely applied to batteries, such as lithium bromine, magnesium bromine batteries and zinc bromine flow batteries [ Yao, X.H., Luo, J.R., Dong, Q ].&Wang,D.W.A rechargeable non-aqueous Mg-Br-2battery.Nano Energy 28,440-446,doi:10.1016/j.nanoen.2016.09.003(2016).；Chang,Z.et al.Rechargeable Li//Br battery:a promising platform for post lithium ion batteries.J Mater Chem A 2,19444-19450,doi:10.1039/c4ta04419c(2014).；Lai,Q.Z.,Zhang,H.M.,Li,X.F.,Zhang,L.Q.&Cheng,Y.H.A novel single flow zinc-bromine battery with improved energy density.J Power Sources 235,1-4,doi:10.1016/j.jpowsour.2013.01.193(2013).]However, bromine is toxic and volatile, which limits further development.
Bromine ions can perfectly solve the defect, meanwhile, most of bromine is applied to the battery to improve the performance of the battery based on the oxidation-reduction reaction of bromine, and the battery based on single bromine ion intercalation is not reported. In addition, the development of the non-metal ion battery is relatively slow, the feasibility of the halogen ion battery is proved by the appearance of the room-temperature fluorine ion battery, and three major problems need to be solved to solve the obstacle of the non-metal ion battery: 1) and selecting a positive active material. 2) And (4) selecting electrolyte. 3) And selecting the negative electrode coordination metal.
Disclosure of Invention
In order to solve the above problems, the present invention provides a bromine ion battery. The invention adopts carbon black as an intercalation material of bromide ions, adopts ammonium bromide in a glycol non-aqueous system as an electrolyte, and finds out three coordination metals of zinc, copper and nickel as a cathode of the bromide ion battery through a large number of experiments to form the complete bromide ion battery based on the glycol organic system electrolyte.
In order to achieve the purpose, the invention adopts the technical scheme that:
a bromine ion battery is assembled by adopting carbon black as an intercalation material of bromine ions, adopting ammonium bromide in a glycol non-water system as an electrolyte and adopting three coordination metals of zinc, copper and nickel as a cathode of the bromine ion battery.
Firstly, putting carbon black and a binder PVDF into an agate grinding pot according to the mass ratio of 80:20, grinding and pulping by using N-methylpyrrolidone NMP as a solvent, coating the pulp on a stainless steel foil with the thickness of 50 microns, putting the stainless steel foil in a vacuum drying oven, and drying for 12 hours at the temperature of 80 ℃ to prepare a working electrode plate serving as an intercalation material.
Secondly, adopting ammonium bromide as electrolyte and ethylene glycol as solvent to prepare electrolyte with the concentration of 1-2 mol/L.
And finally, respectively using three metals of zinc foil, copper foil or nickel foil as cathode materials of the bromine ion battery.
The invention has the beneficial effects that: the invention provides a bromine ion battery based on the intercalation principle of bromine ions in a carbon material, and the bromine ions avoid the defects of toxicity, volatility and the like of elemental bromine and improve the safety of the battery. Meanwhile, the carbon black is low in price, the cost of the bromine ion battery is reduced, and the large-scale popularization is facilitated. The ethylene glycol ammonium bromide electrolyte of the non-aqueous system avoids the hydrogen evolution and oxygen evolution reaction, thereby ensuring the bromine ion battery to be stable in circulation and fully exerting the characteristic of high theoretical specific capacity of bromine ions. Three metals of zinc, copper and nickel are used as cathode materials of the bromine ion battery, so that the battery cost is reduced, and a theoretical basis is provided for the research of the cathode of the non-metal ion battery.
Drawings
FIG. 1(a) is a schematic diagram of a bromine ion battery
FIG. 1(b) is a schematic diagram of coordination of ammonium ions and negative metal during charge and discharge.
FIG. 2 is an X-ray photoelectron spectroscopy (XPS) plot of a bromide intercalated positive carbon black material when fully charged; (a) is XPS main graph, (b) is bromine peak diagram, (c) is carbon peak diagram, and (d) is oxygen peak diagram.
Fig. 3 is a graph showing the cycle performance of a bromide ion battery in which zinc foil, copper foil and nickel foil are used as negative electrodes, respectively.
Detailed Description
The present invention is further explained below.
The invention adopts carbon black as an intercalation material of bromide ions, adopts ammonium bromide in a glycol non-aqueous system as an electrolyte, and finds out three coordination metals of zinc, copper and nickel as a cathode of the bromide ion battery through a large number of experiments to form the complete bromide ion battery based on the glycol organic system electrolyte. Ammonium bromide takes place hydrolysis reaction easily in aqueous, can lead to electrolyte inefficacy to influence battery life, so it is infeasible to adopt water system electrolyte, fortunately, ammonium bromide has stability also fabulous when higher solubility in ethylene glycol, so solved bromide ion battery cycle life's problem. In addition, when three metals of zinc, copper and nickel are respectively used as negative electrode materials for charging and discharging, the schematic diagram of the battery and the reaction schematic diagram of the negative electrode are shown in the attached drawing 1, ammonium ions are gathered around the negative electrode metal during charging, electrons on the outer layer of the metal are attracted to deviate, a shared electron pair structure is formed, and when discharging is carried out, the ammonium ions are far away from the negative electrode, the structure disappears, and the electrons on the outer layer of the metal are reset. Meanwhile, XPS characterization is performed after the zinc foil is used as the cathode of the bromine ion battery and is fully charged, and as shown in figure 2, bromine ions can be seen to enter the carbon black of the anode in an intercalation mode in the charging process. And finally, cheap carbon black is adopted as an intercalation material, so that the battery has low cost and is favorable for further popularization and application.
Example 1
Putting carbon black and a binder (PVDF) into an agate grinding pot according to the mass ratio of 80:20, grinding and pulping by using N-methylpyrrolidone (NMP) as a solvent, then coating the pulp on a plurality of stainless steel foils with the thickness of 50 micrometers and the area of 2.5cm x 2.5cm, finally putting the coated sheets into a vacuum drying box, and drying for 12 hours at 80 ℃ to obtain the working electrode sheet. 1.96g of ammonium bromide was dissolved in 10ml of ethylene glycol to prepare 2mol/L of an electrolyte. A zinc foil with the thickness of 50 microns is used as a cathode material of the bromine ion battery to be assembled into a soft package battery for performance test, as shown in figure 3, under the condition that the charge-discharge current density is 2A/g, the capacity of the bromine ion battery still reaches 141mAh/g after 3000 cycles.
Example 2
Putting carbon black and a binder (PVDF) into an agate grinding pot according to the mass ratio of 80:20, grinding and pulping by using N-methylpyrrolidone (NMP) as a solvent, then coating the pulp on a plurality of stainless steel foils with the thickness of 50 micrometers and the area of 2.5cm x 2.5cm, finally putting the coated sheets into a vacuum drying box, and drying for 12 hours at 80 ℃ to obtain the working electrode sheet. 1.96g of ammonium bromide was dissolved in 10ml of ethylene glycol to prepare 2mol/L of an electrolyte. A copper foil with the thickness of 50 microns is used as a cathode material of the bromine ion battery, the bromine ion battery is assembled into a soft package battery for performance test, as shown in figure 3, and the capacity of the bromine ion battery after 500 cycles is 85mAh/g under the condition of the charge-discharge current density of 2A/g.
Example 3
Putting carbon black and a binder (PVDF) into an agate grinding pot according to the mass ratio of 80:20, grinding and pulping by using N-methylpyrrolidone (NMP) as a solvent, then coating the pulp on a plurality of stainless steel foils with the thickness of 50 micrometers and the area of 2.5cm x 2.5cm, finally putting the coated sheets into a vacuum drying box, and drying for 12 hours at 80 ℃ to obtain the working electrode sheet. 1.96g of ammonium bromide was dissolved in 10ml of ethylene glycol to prepare 2mol/L of an electrolyte. A nickel foil with the thickness of 50 microns is used as a cathode material of the bromine ion battery to assemble a soft package battery for performance test, as shown in figure 3, under the condition that the charge-discharge current density is 2A/g, the capacity of the bromine ion battery after 500 cycles is 85 mAh/g.
Comparative example 1
Putting carbon black and a binder (PVDF) into an agate grinding pot according to the mass ratio of 80:20, grinding and pulping by using N-methylpyrrolidone (NMP) as a solvent, then coating the pulp on a plurality of stainless steel foils with the thickness of 50 micrometers and the area of 2.5cm x 2.5cm, finally putting the coated sheets into a vacuum drying box, and drying for 12 hours at 80 ℃ to obtain the working electrode sheet. 1.96g of ammonium bromide was dissolved in 10ml of water to prepare 2mol/L of an electrolyte. A zinc foil, a copper foil and a nickel foil with the thickness of 50 micrometers are respectively used as cathode materials of the bromine ion battery and assembled into a soft package battery for performance test, and a discharge platform of the battery is found not to appear, so that the aqueous electrolyte is not suitable for the bromine ion battery.
Comparative example 2
Putting carbon black and a binder (PVDF) into an agate grinding pot according to the mass ratio of 80:20, grinding and pulping by using N-methylpyrrolidone (NMP) as a solvent, then coating the pulp on a plurality of stainless steel foils with the thickness of 50 micrometers and the area of 2.5cm x 2.5cm, finally putting the coated sheets into a vacuum drying box, and drying for 12 hours at 80 ℃ to obtain the working electrode sheet. 1.96g of ammonium bromide was dissolved in 10ml of ethylene glycol to prepare 2mol/L of an electrolyte. The lithium ion battery is characterized in that aluminum foil, titanium foil, magnesium foil, iron foil and other metal materials with the thickness of 50 microns are used as cathode materials of the bromine ion battery, and the bromine ion battery is assembled into a soft package battery for performance test, and has no performance, so that the ethylene glycol ammonium bromide electrolyte is not suitable for all metal materials, is only suitable for three metal materials of zinc foil, copper foil and nickel foil at present, and has no defect.
The above-mentioned embodiments only express the embodiments of the present invention, but not should be understood as the limitation of the scope of the invention patent, it should be noted that, for those skilled in the art, many variations and modifications can be made without departing from the concept of the present invention, and these all fall into the protection scope of the present invention.

Claims (1)

1. A bromine ion battery is characterized in that carbon black is used as an intercalation material of bromine ions, ammonium bromide in a glycol non-aqueous system is used as an electrolyte, and three coordination metals of zinc, copper or nickel are used as a negative electrode material of the bromine ion battery to assemble a soft package battery;
the intercalation material is as follows: putting carbon black and a binder PVDF into an agate grinding pot according to the mass ratio of 80:20, grinding and pulping by using N-methylpyrrolidone NMP as a solvent, coating the pulp on a stainless steel foil, and drying in a vacuum drying oven to obtain the composite material;
in the electrolyte: ammonium bromide is used as electrolyte, ethylene glycol is used as solvent, and the concentration is 1-2 mol/L.
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* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN112803095B (en) * 2021-01-29 2022-10-28 中国科学技术大学 Aqueous halogen-hydrogen secondary battery
CN113140809B (en) * 2021-04-22 2022-05-10 大连理工大学 High-performance rechargeable bromine ion battery based on two-dimensional material MoS2 and preparation method thereof

Citations (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN1870335A (en) * 2006-04-13 2006-11-29 复旦大学 Energy storage battery based on bromide ion conduction
CN107305951A (en) * 2016-04-18 2017-10-31 张维雷 A kind of zinc-bromine flow battery

Patent Citations (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN1870335A (en) * 2006-04-13 2006-11-29 复旦大学 Energy storage battery based on bromide ion conduction
CN107305951A (en) * 2016-04-18 2017-10-31 张维雷 A kind of zinc-bromine flow battery

Non-Patent Citations (1)

* Cited by examiner, † Cited by third party
Title
Development of carbon coated membrane for zinc/bromine flow battery with high power density;Liqun Zhang;《Journal of Power Sources》;20130401;全文 *

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