CN112952123A - Electrode treated by persulfate and application thereof - Google Patents
Electrode treated by persulfate and application thereof Download PDFInfo
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- CN112952123A CN112952123A CN201911266846.9A CN201911266846A CN112952123A CN 112952123 A CN112952123 A CN 112952123A CN 201911266846 A CN201911266846 A CN 201911266846A CN 112952123 A CN112952123 A CN 112952123A
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- electrode
- zinc
- battery
- persulfate
- electrode material
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- JRKICGRDRMAZLK-UHFFFAOYSA-L peroxydisulfate Chemical compound [O-]S(=O)(=O)OOS([O-])(=O)=O JRKICGRDRMAZLK-UHFFFAOYSA-L 0.000 title claims abstract description 12
- 239000007772 electrode material Substances 0.000 claims abstract description 34
- KFZAUHNPPZCSCR-UHFFFAOYSA-N iron zinc Chemical compound [Fe].[Zn] KFZAUHNPPZCSCR-UHFFFAOYSA-N 0.000 claims abstract description 33
- 239000007864 aqueous solution Substances 0.000 claims abstract description 10
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims description 16
- 229910052799 carbon Inorganic materials 0.000 claims description 15
- 238000002791 soaking Methods 0.000 claims description 15
- USHAGKDGDHPEEY-UHFFFAOYSA-L potassium persulfate Chemical compound [K+].[K+].[O-]S(=O)(=O)OOS([O-])(=O)=O USHAGKDGDHPEEY-UHFFFAOYSA-L 0.000 claims description 6
- 238000000034 method Methods 0.000 claims description 5
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 5
- 239000000463 material Substances 0.000 claims description 4
- LCPVQAHEFVXVKT-UHFFFAOYSA-N 2-(2,4-difluorophenoxy)pyridin-3-amine Chemical compound NC1=CC=CN=C1OC1=CC=C(F)C=C1F LCPVQAHEFVXVKT-UHFFFAOYSA-N 0.000 claims description 3
- CHQMHPLRPQMAMX-UHFFFAOYSA-L sodium persulfate Substances [Na+].[Na+].[O-]S(=O)(=O)OOS([O-])(=O)=O CHQMHPLRPQMAMX-UHFFFAOYSA-L 0.000 claims description 3
- 239000004744 fabric Substances 0.000 claims description 2
- 230000007935 neutral effect Effects 0.000 claims description 2
- 238000005406 washing Methods 0.000 claims 1
- 230000000694 effects Effects 0.000 abstract description 8
- 238000004146 energy storage Methods 0.000 description 10
- QAOWNCQODCNURD-UHFFFAOYSA-N Sulfuric acid Chemical compound OS(O)(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-N 0.000 description 6
- 230000000052 comparative effect Effects 0.000 description 6
- HCHKCACWOHOZIP-UHFFFAOYSA-N Zinc Chemical compound [Zn] HCHKCACWOHOZIP-UHFFFAOYSA-N 0.000 description 5
- 238000006243 chemical reaction Methods 0.000 description 5
- 239000000243 solution Substances 0.000 description 5
- 239000011701 zinc Substances 0.000 description 5
- 229910052725 zinc Inorganic materials 0.000 description 5
- -1 hydroxide ions Chemical class 0.000 description 4
- 238000004140 cleaning Methods 0.000 description 3
- 239000003792 electrolyte Substances 0.000 description 3
- 239000007788 liquid Substances 0.000 description 3
- 230000010287 polarization Effects 0.000 description 3
- 238000012360 testing method Methods 0.000 description 3
- XFXPMWWXUTWYJX-UHFFFAOYSA-N Cyanide Chemical compound N#[C-] XFXPMWWXUTWYJX-UHFFFAOYSA-N 0.000 description 2
- CWYNVVGOOAEACU-UHFFFAOYSA-N Fe2+ Chemical compound [Fe+2] CWYNVVGOOAEACU-UHFFFAOYSA-N 0.000 description 2
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 2
- 238000005520 cutting process Methods 0.000 description 2
- 230000001351 cycling effect Effects 0.000 description 2
- 210000001787 dendrite Anatomy 0.000 description 2
- 230000008021 deposition Effects 0.000 description 2
- 238000005516 engineering process Methods 0.000 description 2
- 230000007613 environmental effect Effects 0.000 description 2
- 125000000524 functional group Chemical group 0.000 description 2
- 239000003014 ion exchange membrane Substances 0.000 description 2
- 229910052760 oxygen Inorganic materials 0.000 description 2
- 239000001301 oxygen Substances 0.000 description 2
- 238000002360 preparation method Methods 0.000 description 2
- 229920000557 Nafion® Polymers 0.000 description 1
- 230000004913 activation Effects 0.000 description 1
- 239000013543 active substance Substances 0.000 description 1
- 239000003513 alkali Substances 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 210000004027 cell Anatomy 0.000 description 1
- 238000013461 design Methods 0.000 description 1
- 238000011161 development Methods 0.000 description 1
- 238000012983 electrochemical energy storage Methods 0.000 description 1
- 238000003487 electrochemical reaction Methods 0.000 description 1
- 230000034964 establishment of cell polarity Effects 0.000 description 1
- 229910002804 graphite Inorganic materials 0.000 description 1
- 239000010439 graphite Substances 0.000 description 1
- XEEYBQQBJWHFJM-UHFFFAOYSA-N iron Substances [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 description 1
- 238000012423 maintenance Methods 0.000 description 1
- 238000004519 manufacturing process Methods 0.000 description 1
- 239000012528 membrane Substances 0.000 description 1
- 238000010248 power generation Methods 0.000 description 1
- 230000002035 prolonged effect Effects 0.000 description 1
- 238000003860 storage Methods 0.000 description 1
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Classifications
-
- 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
- H01M4/96—Carbon-based electrodes
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M8/00—Fuel cells; Manufacture thereof
- H01M8/18—Regenerative fuel cells, e.g. redox flow batteries or secondary fuel cells
- H01M8/184—Regeneration by electrochemical means
- H01M8/188—Regeneration by electrochemical means by recharging of redox couples containing fluids; Redox flow type 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
- 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
- Y02E60/30—Hydrogen technology
- Y02E60/50—Fuel cells
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- Chemical & Material Sciences (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Electrochemistry (AREA)
- General Chemical & Material Sciences (AREA)
- Life Sciences & Earth Sciences (AREA)
- Engineering & Computer Science (AREA)
- Manufacturing & Machinery (AREA)
- Sustainable Development (AREA)
- Sustainable Energy (AREA)
- Battery Electrode And Active Subsutance (AREA)
Abstract
The invention discloses an electrode treated by persulfate and application thereof in a zinc-iron flow battery, wherein an electrode material is soaked in an aqueous solution of persulfate for treatment, and compared with the original untreated electrode material, the electrode material has higher electrode activity, can effectively improve the conductivity of the battery, further improve the cycle performance and the efficiency of the battery, and simultaneously greatly improve the charge-discharge capacity and the energy density of the battery.
Description
Technical Field
The invention relates to a zinc-iron flow battery with a positive electrode treated by persulfate.
Background
The liquid flow energy storage battery is a new electrochemical energy storage technology, and compared with other energy storage technologies, the liquid flow energy storage battery has the advantages of high energy conversion efficiency, flexible system design, large storage capacity, free site selection, deep discharge, safety, environmental protection, low maintenance cost and the like, and can be widely applied to the aspects of power generation and energy storage of renewable energy sources such as wind energy, solar energy and the like, an emergency power supply system, a standby power station, an electric power system and the like, and peak clipping and valley filling and the like. The alkaline zinc-iron flow battery is considered to be a flow energy storage battery with high development potential due to the advantages of high safety, good stability, long service life (the service life is more than 15 years), low cost and the like.
Currently, the main limitation restricting the commercialization of the zinc-iron flow battery in the alkaline system is the cost problem. To reduce the cost, two main solutions are provided: one is to reduce the cost of each key material, such as the cost of ion exchange membrane, electrolyte and electrode bipolar plate; one is to increase the power density of the battery. Because the power density of the battery is improved, the same galvanic pile can be used for realizing larger power output, the occupied area and the space of the energy storage system can be reduced, the environmental adaptability and the mobility of the system are improved, and the application field of the liquid flow energy storage battery is expanded. To increase the power density of a battery, the operating current density is increased. However, an increase in operating current density results in a decrease in voltage efficiency and energy efficiency. In order to increase the operating current density of the cell without reducing energy efficiency, it is necessary to reduce the cell polarization, i.e., ohmic polarization, electrochemical polarization, and concentration polarization, as much as possible and to reduce the voltage loss.
The electrode is used as one of the key components of the zinc-iron flow battery in the alkaline system, and the performance of the electrode has great influence on the flow energy storage battery. The alkaline zinc-iron flow battery electrode material in the prior art has the problems of more working procedures, high production cost, poor electrocatalytic activity and the like. The electrocatalytic activity of the electrode directly determines the intrinsic reaction rate of the electrochemical reaction, and greatly influences the working current density and energy efficiency of the battery. Therefore, in order to achieve high operating current densities and energy efficiencies, suitable activation methods are also employed to maximize the electrocatalytic activity of the electrode material.
Disclosure of Invention
The invention aims to overcome the problems of the existing electrode material for the zinc-iron flow battery and provides an electrode for the zinc-iron flow battery. The method can greatly improve the reaction activity and the conductivity of the electrode, thereby obtaining the electrode material which has extremely low cost and excellent performance and is suitable for the zinc-iron flow battery of an alkaline system.
In order to achieve the purpose, the technical scheme adopted by the invention is as follows:
soaking the electrode material in aqueous solution of persulfate at the temperature of 60-80 ℃, taking out the electrode after soaking for 0.5-24 h, and repeatedly cleaning the electrode with water for later use;
in the soaking system, the final molar concentration of the aqueous solution of the persulfate is 0.01-2 mol/L;
wherein the soaking temperature is 60-80 ℃.
The electrode is made of carbon felt, carbon cloth or carbon paper material.
The persulfate is one or more of potassium persulfate and sodium persulfate.
The treated electrode is applied to a zinc-iron flow battery.
The zinc-iron flow battery is an alkaline zinc-iron flow battery or a neutral zinc-iron flow battery, preferably an alkaline zinc-iron flow battery; the negative electrode is a carbon felt electrode or a zinc electrode.
The beneficial results of the invention are as follows:
(1) the electrode material prepared by the invention has the advantages that the oxygen-containing functional groups on the surface are greatly increased, the electrode material improves the electrode activity, the conductivity is greatly improved, the internal resistance of the zinc-iron flow energy storage battery in an alkaline system is further reduced, and the battery operation efficiency is greatly improved.
(2) Meanwhile, when the zinc-iron flow battery system is used as a negative electrode, oxygen-containing functional groups generated on the surface can be used as reactive active sites for zinc deposition, the uniformity of zinc deposition is improved, zinc dendrites are inhibited, and the service life of the battery can be prolonged.
(3) The invention expands the variety and application range of the electrode material for the zinc-iron flow energy storage battery in the alkaline system.
The electrode material has the advantages of simple preparation method, environment-friendly process and high active substance concentration. Compared with the original electrode material, the alkaline zinc-iron flow battery assembled by the treated electrode material has higher comprehensive performance.
Drawings
FIG. 1 shows the electrode material prepared in example 1 and comparative example 1 in an alkaline zinc-iron flow battery at 80mA/cm2The charge and discharge performance at the current density of (c) was compared.
Detailed Description
The following examples are further illustrative of the present invention and are not intended to limit the scope of the present invention.
Example 1
Cutting a carbon felt with a proper size and a thickness of 6mm, soaking the carbon felt in 0.5mol/L aqueous solution of potassium persulfate at the temperature of 80 ℃, taking out the electrode after 12h, repeatedly cleaning the electrode with water, and airing the electrode for later use.
The prepared electrode material is used as a positive electrode and a negative electrode, the bipolar plate is a graphite plate, the ion exchange membrane is a Nafion membrane produced by DuPont, and the effective area is 48cm2Assembling the alkaline zinc-iron flow battery with the current density of 80mA/cm2. Wherein the positive electrolyte is a solution containing ferrous cyanide ions (Fe (CN))6 4-) Wherein the concentration of the ferrous cyanide ion is 1mol L-1The concentration of hydroxide ions is 3 mol/L; the electrolyte of the negative electrode is an alkali solution containing zincate ions, wherein the concentration of the zincate ions is 0.5mol L-1The concentration of hydroxide ions is 3 mol/L; the Coulombic Efficiency (CE) of the assembled alkaline zinc-iron flow battery is 98.8%, the Voltage Efficiency (VE) is 89.1%, and the Energy Efficiency (EE) is 88.0%. Battery life>And (5) 100 cycles.
Comparative example 1 (untreated cathode)
The electrode material was changed to untreated 6mm carbon felt compared to example 1, with the other conditions unchanged. The coulombic efficiency of the battery is 88.6%, the voltage efficiency is 83.3%, and the energy efficiency is 73.8%. Battery life <20 cycles.
Compared with untreated electrode materials, the coulombic efficiency, the energy efficiency and the cycling stability of the alkaline zinc-iron flow battery using the electrode material are obviously improved. The preparation of the electrode material by soaking in the potassium persulfate aqueous solution is proved to effectively improve the conductivity and the reaction activity of the electrode material, thereby improving the operation efficiency of the battery. Meanwhile, the treated electrode material can also inhibit the growth of zinc dendrites, and the stability of the battery is improved.
Comparative example 2 (electrode material treated with sulfuric acid)
Compared with the example 1, the untreated 6mm carbon felt is firstly soaked in 0.5mol/L sulfuric acid aqueous solution at the temperature of 80 ℃, the electrode is taken out after 12 hours and repeatedly cleaned by water, and is aired for standby, and other conditions are not changed. Through tests, the coulombic efficiency of the battery is 91.6%, the voltage efficiency is 83.7%, and the energy efficiency is 76.7%. Battery life <25 cycles.
Compared with comparative example 1, the alkaline zinc-iron flow battery using the electrode material treated by sulfuric acid has slightly improved coulombic efficiency, energy efficiency and cycle stability, but has a great gap from the zinc-iron flow battery assembled by the electrode material of the invention in example 1. The results show that the conductivity and the reaction activity of the electrode material can be more efficiently improved by preparing the electrode material by soaking the electrode material in the potassium persulfate aqueous solution, so that the battery efficiency and the cycle stability are greatly improved.
Example 2 (soaking time is not preferred)
Compared with the example 1, the soaking time is changed to 0.2h, and other conditions are not changed. Through tests, the coulombic efficiency of the battery is 94.7%, the voltage efficiency is 85.2%, and the energy efficiency is 80.7%. The battery life was 80 cycles.
Compared with comparative example 1, the alkaline zinc-iron flow battery with the electrode material soaked in the non-preferred time has certain improvements in coulombic efficiency, energy efficiency and cycle stability, but has a small difference compared with the preferred soaking time of the invention in example 1.
Example 3 (concentration of solution being a non-preferred condition)
Compared with example 1, the concentration of potassium persulfate was changed to 0.1mol/L, and other conditions were not changed. Through tests, the coulombic efficiency of the battery is 96.4%, the voltage efficiency is 87.0%, and the energy efficiency is 83.9%. The battery life was 80 cycles.
The coulombic efficiency, energy efficiency and cycling stability of the alkaline zinc-iron flow battery with the electrode material treated at the non-preferred solution concentration are improved to some extent compared with the comparative example 1, but there is still a small gap compared with the preferred soaking time of the invention in the example 1.
Example 4
Cutting a carbon felt with a proper size and a thickness of 6mm, firstly soaking the carbon felt in 0.6mol/L aqueous solution of sodium persulfate at the temperature of 60 ℃, taking out the electrode after 15h, repeatedly cleaning the electrode with water, and airing the electrode for later use. The other conditions were the same as in example 1.
Example 5
In the same manner as in example 1, the carbon felt of 6mm thickness was changed to 4 pieces of carbon paper material of 1mm thickness, and the other conditions were not changed.
Claims (4)
1. An electrode treated with persulfate, characterized in that:
the electrode material is one or more than two of carbon felt, carbon cloth or carbon paper material;
the treatment process comprises the steps of firstly soaking the electrode material in aqueous solution of persulfate at the temperature of 60-80 ℃, taking out the electrode material, and repeatedly washing the electrode material with water for later use after soaking for 0.1-24 h (preferably 0.5-12 h) to obtain an electrode;
the soaking system is characterized in that the final molar concentration of the aqueous solution of the persulfate is 0.01-2 mol/L (preferably 0.2-1 mol/L).
2. The zinc-iron flow battery of claim 1, wherein:
the persulfate is one or more of potassium persulfate and sodium persulfate.
3. Use of the electrode of claim 1 in a zinc-iron flow battery, wherein: the treated electrode is applied to a zinc-iron flow battery.
4. Use according to claim 1 or 3, characterized in that: the zinc-iron flow battery is an alkaline zinc-iron flow battery or a neutral zinc-iron flow battery, and is preferably an alkaline zinc-iron flow battery.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN201911266846.9A CN112952123A (en) | 2019-12-11 | 2019-12-11 | Electrode treated by persulfate and application thereof |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN201911266846.9A CN112952123A (en) | 2019-12-11 | 2019-12-11 | Electrode treated by persulfate and application thereof |
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| CN112952123A true CN112952123A (en) | 2021-06-11 |
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| CN201911266846.9A Pending CN112952123A (en) | 2019-12-11 | 2019-12-11 | Electrode treated by persulfate and application thereof |
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Citations (5)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN103887524A (en) * | 2014-04-11 | 2014-06-25 | 大连交通大学 | Modified treatment method of positive electrode graphite felt electrode of all-vanadium redox flow battery |
| CN104716335A (en) * | 2013-12-15 | 2015-06-17 | 中国科学院大连化学物理研究所 | Electrode for liquid flow batteries, preparation and application |
| US20180138520A1 (en) * | 2015-04-09 | 2018-05-17 | United Technologies Corporation | Method of treating carbon electrode |
| CN108352507A (en) * | 2015-11-13 | 2018-07-31 | 阿瓦隆电池（加拿大）公司 | Modified electrode for redox flow batteries |
| CN109546165A (en) * | 2018-12-13 | 2019-03-29 | 南开大学 | A kind of preparation method and application of zinc iodine solution galvanic battery carbon felt combination electrode material |
-
2019
- 2019-12-11 CN CN201911266846.9A patent/CN112952123A/en active Pending
Patent Citations (5)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN104716335A (en) * | 2013-12-15 | 2015-06-17 | 中国科学院大连化学物理研究所 | Electrode for liquid flow batteries, preparation and application |
| CN103887524A (en) * | 2014-04-11 | 2014-06-25 | 大连交通大学 | Modified treatment method of positive electrode graphite felt electrode of all-vanadium redox flow battery |
| US20180138520A1 (en) * | 2015-04-09 | 2018-05-17 | United Technologies Corporation | Method of treating carbon electrode |
| CN108352507A (en) * | 2015-11-13 | 2018-07-31 | 阿瓦隆电池（加拿大）公司 | Modified electrode for redox flow batteries |
| CN109546165A (en) * | 2018-12-13 | 2019-03-29 | 南开大学 | A kind of preparation method and application of zinc iodine solution galvanic battery carbon felt combination electrode material |
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