CN109860673A - A16Model high energy density cells and its positive and negative anodes electrolyte and preparation method - Google Patents

A16Model high energy density cells and its positive and negative anodes electrolyte and preparation method Download PDF

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CN109860673A
CN109860673A CN201910240674.1A CN201910240674A CN109860673A CN 109860673 A CN109860673 A CN 109860673A CN 201910240674 A CN201910240674 A CN 201910240674A CN 109860673 A CN109860673 A CN 109860673A
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electrolyte
positive
energy density
hbpy
hcl
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谢志鹏
杨斌
刘柏雄
傅俊祥
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Jiangxi University of Science and Technology
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    • 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
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    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
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Abstract

The present invention relates to a kind of A16Model high energy density cells and its positive and negative anodes electrolyte and preparation method, belong to electrochemical field, can be widely applied to the extensive energy storage of new energy.A of the invention16The active material of electrolyte liquid described in model high energy density cells is K3Fe(CN)6, constant pH maintains with hexa-hydrochloric acid；Anode electrolyte active material is Fe (3m6 ' hbpy)3Cl2, constant pH maintains with amion acetic acid-hydrochloric acid；Positive and negative anodes solid-state energy storage material is Prussian blue Fe4[Fe(CN)6]3；Pass through intermediate K3Fe(CN)6With Fe (3m6 ' hbpy)3Cl2Redox realize the electronic/electrical lotus in positive and negative electrode and solid energy storage material Fe4[Fe(CN)6]3Between transmitting.Its energy density is up to the 2 times or more of existing all-vanadium flow battery, but active material cost only has its 1/10th.

Description

A16Model high energy density cells and its positive and negative anodes electrolyte and preparation method
Technical field
The present invention relates to a kind of A16Model high energy density cells and its positive and negative anodes electrolyte and preparation method, belong to electrification Field can be widely applied to the extensive energy storage of new energy.
Background technique
Widely replacing fossil energy using renewable energy such as solar energy, wind energies is after avoiding greenhouse effects catastrophic One of optimal strategy of fruit.However the intermittence of solar energy and wind energy brings huge challenge to the safety management of power grid.Intelligence A kind of reliable energy storage device of the development need of power grid carrys out the input and output of regulation power, to reach highest energy utilization effect Rate.In various extensive energy storage programs, draw water energy storage and compressed-air energy storage have a best cost-effectiveness, but two Person needs special geography and geologic requirements.In addition to this two, flow battery with its fast response time, can be quickly charged and discharged and The advantages that security performance is high becomes one of most potential large-scale energy storage device.The active material of flow battery is dissolved in In electrolyte；Under the promotion of pump, electrolyte is circulated between fluid reservoir and electrode chamber.This design feature keeps liquid stream electric The power in pond and capacity are mutually indepedent, can improve the flexibility of system design significantly, be conducive to meet the different need of client It asks.But the low energy densities of flow battery and inexpensive benefit are at the two big factors for hindering the application of its widespread commercialization.
Summary of the invention
The object of the present invention is to provide a kind of A16Model high energy density cells and its positive and negative anodes electrolyte and preparation method, Overcome the shortcoming of existing flow battery, realizes flow battery high-energy density and cost effective target.
A of the invention16Model high energy density cells are improved on the basis of existing flow battery, mainly by bearing Pole, electrolyte liquid, cathode solid energy storage material, anode, anode electrolyte, positive solid energy storage material and amberplex The pile that the multiple batteries monomer of (diaphragm) composition is unified into, cathode solid energy storage material are placed in cathode pot, are born by pumping The conveying of pole electrolyte, positive solid energy storage material are placed in positive tank, carry out the conveying of anode electrolyte by pumping.In pile Anode chamber with cathode pot, electrolyte liquid delivery pump be linked to be circuit with electrolysis fluid catheter, electrolyte liquid follows in the circuit Circulation is dynamic.Cathode chamber in pile is linked to be circuit, anolyte by electrolysis fluid catheter and positive tank, anode electrolyte delivery pump Liquid circulates in the circuit.
A of the invention16Model high energy density cells, key are that the active material of the electrolyte liquid is K3Fe (CN)6, constant pH is maintained with hexa-hydrochloric acid, and corresponding cathode solid-state energy storage material is general Shandong Scholar's indigo plant Fe4[Fe(CN)6]3；Anode electrolyte active material is Fe (3m6 ' hbpy)3Cl2, constant pH is with amion acetic acid-salt Acid maintains, and corresponding positive solid-state energy storage material is Prussian blue Fe4[Fe(CN)6]3；Pass through intermediate K3Fe (CN)6With Fe (3m6 ' hbpy)3Cl2Redox realize the electronic/electrical lotus in positive and negative electrode and solid energy storage material Fe4[Fe (CN)6]3Between transmitting.
The pH of electrolyte liquid is 5.0-7.0；The pH of anode electrolyte is 1.5-2.5.
The composition of the electrolyte liquid are as follows: 0.02-0.8M K3Fe(CN)6+0.02-1.6M C6H12N4/HCl+0.02- 1.6M NaCl。
The preparation method of the electrolyte liquid, includes the following steps, following number indicates the amount of substance:
Step A weighs 1 part of K3Fe(CN)6, it is soluble in water, it is sufficiently stirred；
Step B, weighs 1-2 parts of hexas and 1-2 parts of HCl are added in step A solution, is sufficiently stirred；
Step C weighs 1-2 parts of NaCl and is added in step B solution, is sufficiently stirred；
It is eventually adding water, by each substance constant volume to concentration range: 0.02-0.8M K3Fe(CN)6+0.02-1.6M C6H12N4/HCl+0.02-1.6M NaCl。
The composition of the anode electrolyte are as follows: 0.02-0.8M Fe (3m6 ' hbpy)3Cl2+0.0002-0.08M C2H5NO2/ HCl+0.02-1.6M NaCl；Wherein, 3m6 ' hbpy is 2,2 '-bipyridyl of 3- methyl -6 '-hydroxyl -, and structural formula is as follows:
The preparation method of the anode electrolyte, includes the following steps, following number indicates the amount of substance:
Step A weighs 1 part of FeCl2It is soluble in water with 3 parts of 2,2 '-bipyridyls of 3- methyl -6 '-hydroxyl -, it is sufficiently stirred；
Step B weighs 0.01-0.1 parts of C2H5NO2/ HCl is added in step A solution, is sufficiently stirred；
Step C weighs 1-2 parts of NaCl and is added in step B solution, is sufficiently stirred；
It is eventually adding water, by each substance constant volume to concentration range: 0.02-0.8M Fe (3m6 ' hbpy)3Cl2+0.0002- 0.08M C2H5NO2/HCl+0.02-1.6M NaCl。
A of the invention16Model high energy density cells are with K3Fe(CN)6As negative electrode active material, Fe (3m6 ' hbpy)3Cl2For positive active material, Prussian blue to be used as positive and negative anodes solid-state ergastic substances, electrode reaction is as follows,
Negative reaction:
Anode reaction:
Its working principle is that using intermediate electricity to [Fe (CN)6]3-/[Fe(CN)6]4-[Fe (3m6 ' hbpy)3]3+/[Fe (3m6’hbpy)3]2+Transmitting of the electronic/electrical lotus between electrode and solid-state energy storage material are Prussian blue is realized, to realize energy The storage and release of amount.When charge and discharge, positive and negative electrode electrolyte circulates in respective circuit, but solid energy storage material is not With electrolyte flow.When charging, K3Fe(CN)6It is reduced into K4Fe(CN)6, K4Fe(CN)6Electron transmission to Prussian blue；Fe (3m6’hbpy)3Cl2It is oxidized to Fe (3m6 ' hbpy)3Cl3, Fe (3m6 ' hbpy)3Cl3Charge transfer to Prussian blue；Electric discharge When, K4Fe(CN)6It is oxidized to K3Fe(CN)6, K3Fe(CN)6Fe is given charge transfer2[Fe(CN)6]；Fe(3m6'hbpy)3Cl3Also Original is at Fe (3m6 ' hbpy)3Cl2, Fe (3m6 ' hbpy)3Cl2Fe [Fe (CN) is given electron transmission6].The positive and negative electrode of battery cell Standard electric potential difference is 0.65V.
A of the invention16Model high energy density cells, due to selecting iron compound as electrolyte active material and solid-state Energy storage material, thus may be implemented cost effective.Meanwhile being conducive to reality using solid iron compound come stored electrons and charge Existing high-energy density.A of the invention16The energy density of model high energy density cells can reach existing all-vanadium flow battery energy The 2 times or more of density, but the cost of active material only has its 1/10th.
Detailed description of the invention
Fig. 1 is A of the invention16The structural schematic diagram of model high energy density cells monomer.
Specific embodiment
(arrow is electrolyte flow direction in figure) as shown in Figure 1, A of the invention16Model high energy density cells are mainly by bearing Pole, electrolyte liquid, cathode solid energy storage material, anode, anode electrolyte, positive solid energy storage material and amberplex The pile that the multiple batteries monomer of (diaphragm) composition is unified into, cathode solid energy storage material are placed in cathode pot, are born by pumping The conveying of pole electrolyte, positive solid energy storage material are placed in positive tank, carry out the conveying of anode electrolyte by pumping.In pile Anode chamber with cathode pot, electrolyte liquid delivery pump be linked to be circuit with electrolysis fluid catheter, electrolyte liquid follows in the circuit Circulation is dynamic.Cathode chamber in pile is linked to be circuit, anolyte by electrolysis fluid catheter and positive tank, anode electrolyte delivery pump Liquid circulates in the circuit.The electrolyte liquid is 0.02-0.8M K3Fe(CN)6+0.02-1.6M C6H12N4/HCl+ The aqueous solution of 0.02-1.6M NaCl, anode electrolyte are 0.02-0.8M Fe (3m6 ' hbpy)3Cl2+0.0002-0.08M C2H5NO2The aqueous solution of/HCl+0.02-1.6M NaCl.The cathode solid energy storage material and positive solid energy storage material are It is Prussian blue.
The electrolyte liquid selects K3Fe(CN)6It is dissolved into water, and C is added6H12N4/ HCl and NaCl are obtained.
The anode electrolyte selects presoma FeCl2It is dissolved in presoma 3- methyl -6 '-hydroxyl -2,2 '-bipyridyl In, and C is added2H5NO2/ HCl and NaCl are obtained.
The pH of electrolyte liquid is 5.0-7.0；The pH of anode electrolyte is 1.5-2.5.
The inert materials such as carbon felt, graphite felt, graphite plate, graphite paper or carbon cloth can be selected in the positive and negative electrode of battery cell.Ion Battery cell is divided into cathode chamber, anode chamber and the sodium chloride electrolysis of centre liquid chamber three parts, sodium chloride electrolyte by exchange membrane Concentration is 0.5-1.5M, and anode is in cathode chamber, and cathode is in anode chamber.The amberplex selects cation-exchange membrane And anion-exchange membrane.Cation-exchange membrane is in cathode side, and anion-exchange membrane is in positive side.
A of the invention16Model high energy density cells are in charge and discharge process, and positive and negative anodes electrolyte is respectively by positive and negative anodes electricity Solution liquid delivery pump is constantly pumped into battery cell, and the flowing of electrolyte accelerates the substance transmittance process in electrode interface, favorably Electrochemistry and concentration polarization in reduction electrode reaction.The rated power of battery depends on the size of pile, and amount of capacity takes Certainly in electrolyte and solid energy storage material.
A of the invention16When model high energy density cells charge and discharge, the negative, positive pole electrolyte in negative, positive pole tank is being electrolysed Under the promotion of liquid delivery pump, is entered in negative, positive pole room by electrolysis fluid catheter and carry out electrode reaction, then flow back to negative, positive pole again In tank, electronic/electrical lotus is passed to negative, positive pole solid energy storage material.
The content of each substance is molar concentration in embodiment.
Embodiment 1: 100mL0.02M K is prepared3Fe(CN)6+0.02M C6H12N4/ HCl+0.02M NaCl electrolyte
0.002mol K is weighed first3Fe(CN)6, it is placed in 250mL beaker, 50mL water is added, is sufficiently stirred；Then according to Secondary addition 0.002mol C6H12N4, 0.002mol/HCl is sufficiently stirred；0.002molNaCl is sequentially added, solution is added water to For 100mL, the electrolyte to get required preparation is sufficiently stirred.
Embodiment 2: 100mL0.4M K is prepared3Fe(CN)6+0.8M C6H12N4/ HCl+0.8M NaCl electrolyte
0.04mol K is weighed first3Fe(CN)6, it is placed in 250mL beaker, 50mL water is added, is sufficiently stirred；Then successively 0.08mol C is added6H12N4, 0.08mol/HCl is sufficiently stirred；0.08molNaCl is sequentially added, adding water to solution is The electrolyte to get required preparation is sufficiently stirred in 100mL.
Embodiment 3: 100mL0.8M K is prepared3Fe(CN)6+1.6M C6H12N4/ HCl+1.6M NaCl electrolyte
0.08mol K is weighed first3Fe(CN)6, it is placed in 250mL beaker, 50mL water is added, is sufficiently stirred；Then successively 0.16mol C is added6H12N4, 0.16mol/HCl is sufficiently stirred；0.16molNaCl is sequentially added, adding water to solution is The electrolyte to get required preparation is sufficiently stirred in 100mL.
Embodiment 4: it prepares 100mL0.02M Fe (3m6 ' hbpy)3Cl2+0.0002M C2H5NO2/HCl+0.02M NaCl Electrolyte
0.002mol FeCl is weighed first2And 0.006mol3m6 ' hbpy, it is placed in 250mL beaker, 50mL water is added, It is sufficiently stirred；Then 0.00002mol C is sequentially added2H5NO2, 0.00002molHCl, 0.002mol NaCl are sufficiently stirred； Adding water to solution is 100mL, up to the electrolyte of required preparation.
Embodiment 5: it prepares 100mL0.4M Fe (3m6 ' hbpy)3Cl2+0.04M C2H5NO2/ HCl+0.8M NaCl electrolysis Liquid
0.04mol FeCl is weighed first2And 0.12mol3m6 ' hbpy, it is placed in 250mL beaker, 50mL water is added, fills Divide stirring；Then 0.004mol C is sequentially added2H5NO2, 0.004molHCl, 0.08mol NaCl are sufficiently stirred；It adds water to molten Liquid is 100mL, up to the electrolyte of required preparation.
Embodiment 6: it prepares 100mL0.8M Fe (3m6 ' hbpy)3Cl2+0.08M C2H5NO2/ HCl+1.6M NaCl electrolysis Liquid
0.08mol FeCl is weighed first2And 0.24mol3m6 ' hbpy, it is placed in 250mL beaker, 50mL water is added, fills Divide stirring；Then 0.008mol C is sequentially added2H5NO2, 0.008molHCl, 0.16mol NaCl are sufficiently stirred；It adds water to molten Liquid is 100mL, up to the electrolyte of required preparation.
Embodiment 7:
A of the invention16Anion-exchange membrane and cation-exchange membrane and the battery case of model high energy density cells enclose It is separated at a sodium chloride electrolysis liquid chamber, and by the positive and negative pole room of battery；Positive and negative electrode is done with carbon felt, the apparent area of the two is equal For 10cm2.Electrolyte liquid is 10ml0.02M K3Fe(CN)6+0.02M C6H12N4/ HCl+0.02M NaCl solution, cathode pot In it is Prussian blue be 2.15 grams；Anode electrolyte is 10ml0.02M Fe (3m6 ' hbpy)3Cl2+0.0002M C2H5NO2/HCl + 0.02M NaCl solution, Prussian blue in positive tank are 2.86 grams；Charging and discharging currents are 10mA, electrolyte flow rate 10mL/ The energy density of min, battery are 105.5Wh/L, are 2.11 times of all-vanadium flow battery energy density (50Wh/L).
Embodiment 8:
A of the invention16Anion-exchange membrane and cation-exchange membrane and the battery case of model high energy density cells enclose It is separated at a sodium chloride electrolysis liquid chamber, and by the positive and negative pole room of battery；Positive and negative electrode is done with carbon felt, the apparent area of the two is equal For 10cm2.Electrolyte liquid is 10ml0.4M K3Fe(CN)6+0.8M C6H12N4/ HCl+0.8M NaCl solution, in cathode pot It is Prussian blue be 2.15 grams；Anode electrolyte is 10ml0.4M Fe (3m6 ' hbpy)3Cl2+0.04M C2H5NO2/HCl+0.8M NaCl solution, Prussian blue in positive tank are 2.86 grams；Charging and discharging currents are 10mA, electrolyte flow rate 10mL/min, electricity The energy density in pond is 112.5Wh/L, is 2.25 times of all-vanadium flow battery energy density (50Wh/L).
Embodiment 9:
A of the invention16Model high energy density cells anion-exchange membrane and cation-exchange membrane are surrounded with battery case One sodium chloride electrolysis liquid chamber, and the positive and negative pole room of battery is separated；Positive and negative electrode is done with carbon felt, the apparent area of the two is 10cm2.Electrolyte liquid is 10ml00.8M K3Fe(CN)6+1.6M C6H12N4/ HCl+1.6M NaCl solution, in cathode pot Prussian blue is 2.15 grams；Anode electrolyte is 10ml0.8M Fe (3m6 ' hbpy)3Cl2+0.08M C2H5NO2/HCl+1.6M NaCl solution, Prussian blue in positive tank are 2.86 grams；Charging and discharging currents are 10mA, electrolyte flow rate 10mL/min, electricity The energy density in pond is 108.5Wh/L, is 2.17 times of all-vanadium flow battery energy density (50Wh/L).

Claims (10)

1. a kind of A16Model high energy density cells, including amberplex, positive and negative anodes, positive and negative anodes electrolyte, it is characterized in that: institute The active material for stating electrolyte liquid is K3Fe(CN)6, constant pH with hexa-hydrochloric acid to maintain, and it is right therewith The cathode solid-state energy storage material answered is Prussian blue Fe4[Fe(CN)6]3；Anode electrolyte active material is Fe (3m6 ' hbpy)3Cl2, constant pH is maintained with amion acetic acid-hydrochloric acid, and corresponding positive solid-state energy storage material is Prussian blue Fe4 [Fe(CN)6]3；Pass through intermediate K3Fe(CN)6With Fe (3m6 ' hbpy)3Cl2Redox realize the electronic/electrical lotus positive and negative Electrode and solid energy storage material Fe4[Fe(CN)6]3Between transmitting.
2. a kind of A according to claim 116Model high energy density cells, characterized in that the pH of electrolyte liquid is 5.0—7.0；The pH of anode electrolyte is 1.5-2.5.
3. a kind of A according to claim 116Model high energy density cells, characterized in that the group of the electrolyte liquid Become: 0.02-0.8M K3Fe(CN)6+0.02-1.6M C6H12N4/HCl+0.02-1.6M NaCl。
4. a kind of A according to claim 116Model high energy density cells, characterized in that the group of the anode electrolyte Become: 0.02-0.8M Fe (3m6 ' hbpy)3Cl2+0.0002-0.08M C2H5NO2/HCl+0.02-1.6M NaCl；Wherein, 3m6 ' hbpy is 2,2 '-bipyridyl of 3- methyl -6 '-hydroxyl -, and structural formula is as follows:
5. a kind of A according to claim 116Model high energy density cells, it is characterized in that: the positive and negative electrode of battery cell Select carbon felt, graphite felt, graphite plate, graphite paper or carbon cloth inert material；Amberplex battery cell be divided into cathode chamber, Anode chamber and intermediate sodium chloride electrolysis liquid chamber three parts, sodium chloride electrolyte concentration are 0.5-1.5M, and anode is in cathode chamber In, cathode is in anode chamber；The amberplex selects cation-exchange membrane and anion-exchange membrane, cation-exchange membrane to exist Cathode side, anion-exchange membrane is in positive side.
6. a kind of A according to claim 116Model high energy density cells, it is characterized in that: the positive and negative electrode of battery cell Standard electric potential difference is 0.65V.
7. a kind of A according to claim 116Model high energy density cells, it is characterized in that: electrode reaction is as follows,
Negative reaction:
Anode reaction:
8. a kind of A16Model high energy density cells positive and negative anodes electrolyte, including anode electrolyte and electrolyte liquid, feature It is the composition of the electrolyte liquid are as follows: 0.02-0.8M K3Fe(CN)6+0.02-1.6M C6H12N4/HCl+0.02-1.6M NaCl；
The composition of the anode electrolyte are as follows: 0.02-0.8M Fe (3m6 ' hbpy)3Cl2+0.0002-0.08M C2H5NO2/HCl+ 0.02-1.6M NaCl；Wherein, 3m6 ' hbpy is 2,2 '-bipyridyl of 3- methyl -6 '-hydroxyl -, and structural formula is as follows:
9. the method for preparing electrolyte liquid described in claim 8, it is characterized in that: including the following steps, following number expression thing The amount of matter:
Step A weighs 1 part of K3Fe(CN)6, it is soluble in water, it is sufficiently stirred；
Step B, weighs 1-2 parts of hexas and 1-2 parts of HCl are added in step A solution, is sufficiently stirred；
Step C weighs 1-2 parts of NaCl and is added in step B solution, is sufficiently stirred；
It is eventually adding water, by each substance constant volume to concentration range: 0.02-0.8M K3Fe(CN)6+0.02-1.6M C6H12N4/HCl +0.02-1.6M NaCl。
10. the method for preparing anode electrolyte described in claim 8, it is characterized in that: including the following steps, following number expression thing The amount of matter:
Step A weighs 1 part of FeCl2It is soluble in water with 3 parts of 2,2 '-bipyridyls of 3- methyl -6 '-hydroxyl -, it is sufficiently stirred；
Step B weighs 0.01-0.1 parts of C2H5NO2/ HCl is added in step A solution, is sufficiently stirred；
Step C weighs 1-2 parts of NaCl and is added in step B solution, is sufficiently stirred；
It is eventually adding water, by each substance constant volume to concentration range: 0.02-0.8M Fe (3m6 ' hbpy)3Cl2+0.0002-0.08M C2H5NO2/HCl+0.02-1.6M NaCl。
CN201910240674.1A 2019-03-28 2019-03-28 A16Model high energy density cells and its positive and negative anodes electrolyte and preparation method Pending CN109860673A (en)

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CN201910709829.1A CN110416586B (en) 2019-03-28 2019-08-02 Iron-based flow battery, positive and negative electrolyte thereof and preparation method

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Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN117117273A (en) * 2023-10-18 2023-11-24 北京普能世纪科技有限公司 All-vanadium redox flow battery system

Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN117117273A (en) * 2023-10-18 2023-11-24 北京普能世纪科技有限公司 All-vanadium redox flow battery system
CN117117273B (en) * 2023-10-18 2024-03-08 北京普能世纪科技有限公司 All-vanadium redox flow battery system

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Application publication date: 20190607