CN109888339A - Positive and negative anodes electrolyte and preparation method thereof and in A10It is applied in model flow battery - Google Patents
Positive and negative anodes electrolyte and preparation method thereof and in A10It is applied in model flow battery Download PDFInfo
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- CN109888339A CN109888339A CN201910240698.7A CN201910240698A CN109888339A CN 109888339 A CN109888339 A CN 109888339A CN 201910240698 A CN201910240698 A CN 201910240698A CN 109888339 A CN109888339 A CN 109888339A
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Abstract
The present invention relates to a kind of positive and negative anodes electrolyte and preparation method thereof and in A10It is applied in model flow battery, belongs to electrochemical field, can be widely applied to the extensive energy storage of new energy.A of the invention10The active material of electrolyte liquid described in model flow battery is K3Fe(CN)6, constant pH maintains with hexa-hydrochloric acid；Anode electrolyte active material is Fe (4,4 '-dmbpy)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 (4,4 '-dmbpy)3Cl2Redox realizes the electronic/electrical lotus in positive and negative anodes and solid energy storage material Fe4[Fe(CN)6]3Between transmit.Its energy density is up to the 2 times or more of existing all-vanadium flow battery, but the cost of active material only has its 1/10th.
Description
Technical field
The present invention relates to a kind of positive and negative anodes electrolyte and preparation method thereof and in A10It is applied in model flow battery, belongs to electricity
Chemical 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 positive and negative anodes electrolyte and preparation method thereof and in A10It is answered in model flow battery
With overcoming the shortcoming of existing flow battery, realize flow battery high-energy density and cost effective target.
A kind of positive and negative anodes electrolyte, including anode electrolyte and electrolyte liquid, 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 (4,4 '-dmbpy)3Cl2+0.0002-0.08M
C2H5NO2/HCl+0.02-1.6M NaCl；Wherein, 4,4 '-dmbpy are 4,4 '-dimethyl -2, and 2 '-bipyridyls, structural formula is such as
Under:
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 preparation method of the anode electrolyte, includes the following steps, following number indicates the amount of substance:
Step A weighs 1 part of FeCl2With 3 part 4,4 '-dimethyl -2,2 '-bipyridyls are soluble in water, are 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 (4,4 '-dmbpy)3Cl2+0.0002-
0.08M C2H5NO2/HCl+0.02-1.6M NaCl。
A of the invention10Model flow battery, 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 Prussian blue Fe4
[Fe(CN)6]3；Anode electrolyte active material is Fe (4,4 '-dmbpy)3Cl2, constant pH is with amion acetic acid-hydrochloric acid
It maintains, and corresponding positive solid-state energy storage material is Prussian blue Fe4[Fe(CN)6]3；Pass through intermediate K3Fe(CN)6With
Fe(4,4’-dmbpy)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.
A of the invention10Model flow battery is with K3Fe(CN)6As negative electrode active material, Fe (4,4 '-dmbpy)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 (4,4 '-dmbpy)3]3+/
[Fe(4,4’-dmbpy)3]2+Realize transmitting of the electronic/electrical lotus between electrode and solid-state energy storage material are Prussian blue, thus
Realize the storage and release of energy.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)6Prussia is given electron transmission
It is blue；Fe(4,4'-dmbpy)3Cl2It is oxidized to Fe (4,4 '-dmbpy)3Cl3, Fe (4,4 '-dmbpy)3Cl3Charge transfer to general
Shandong scholar is blue；When electric discharge, K4Fe(CN)6It is oxidized to K3Fe(CN)6, K3Fe(CN)6Fe is given charge transfer2[Fe(CN)6]；Fe(4,
4’-dmbpy)3Cl3It is reduced into Fe (4,4 '-dmbpy)3Cl2, Fe (4,4 '-dmbpy)3Cl2Fe [Fe is given electron transmission
(CN)6].The positive and negative electrode standard electric potential difference of battery cell is 0.65V.
A of the invention10Model flow battery is improved on the basis of existing flow battery, mainly by cathode, negative
Pole electrolyte, cathode solid energy storage material, anode, anode electrolyte, positive solid energy storage material and amberplex (diaphragm)
The pile that the multiple batteries monomer of composition is unified into, cathode solid energy storage material are placed in cathode pot, carry out electrolyte by pumping
The conveying of liquid, positive solid energy storage material are placed in positive tank, carry out the conveying of anode electrolyte by pumping.Cathode in pile
Room is linked to be circuit with cathode pot, electrolyte liquid delivery pump with electrolysis fluid catheter, and electrolyte liquid circulates in the circuit.
Cathode chamber in pile is linked to be circuit by electrolysis fluid catheter and positive tank, anode electrolyte delivery pump, and anode electrolyte is at this
It is circulated in circuit.
A of the invention10Model flow battery, due to selecting iron compound as electrolyte active material and solid-state energy storage material
Material, thus may be implemented cost effective.Meanwhile high energy is advantageously implemented come stored electrons and charge using solid iron compound
Metric density.A of the invention10Model flow battery energy density can reach the 2 times or more of existing all-vanadium flow battery energy density,
But the cost of active material only has its 1/10th.
Detailed description of the invention
Fig. 1 is A of the invention10The structural schematic diagram of model flow battery monomer.
Specific embodiment
(arrow is electrolyte flow direction in figure) as shown in Figure 1, A of the invention10Model flow battery is mainly by cathode, cathode
Electrolyte, cathode solid energy storage material, anode, anode electrolyte, positive solid energy storage material and amberplex (diaphragm) group
At the pile that is unified into of multiple batteries monomer, cathode solid energy storage material is placed in cathode pot, carries out electrolyte liquid by pumping
Conveying, positive solid energy storage material is placed in positive tank, carries out the conveying of anode electrolyte by pumping.Anode chamber in pile
It is linked to be circuit with cathode pot, electrolyte liquid delivery pump with electrolysis fluid catheter, electrolyte liquid circulates in the circuit.Electricity
Cathode chamber in heap is linked to be circuit by electrolysis fluid catheter and positive tank, anode electrolyte delivery pump, and anode electrolyte is in this time
It is circulated in road.The electrolyte liquid is 0.02-0.8M K3Fe(CN)6+0.02-1.6M C6H12N4/HCl+0.02-
The aqueous solution of 1.6M NaCl, anode electrolyte are 0.02-0.8M Fe (4,4 '-dmbpy)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 4,4 '-dimethyl -2 of presoma, in 2 '-bipyridyls,
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 invention10For model flow battery in charge and discharge process, positive and negative anodes electrolyte is defeated by positive and negative anodes electrolyte respectively
Pump is sent constantly to be pumped into battery cell, the flowing of electrolyte accelerates the substance transmittance process in electrode interface, advantageously reduces
Electrochemistry and concentration polarization in electrode reaction.The rated power of battery depends on the size of pile, and amount of capacity depends on electricity
Solve liquid and solid energy storage material.
A of the invention10When model flow battery charge and discharge, the negative, positive pole electrolyte in negative, positive pole tank is conveyed in electrolyte
Under the promotion of pump, is entered in negative, positive pole room by electrolysis fluid catheter and carry out electrode reaction, then flowed back to again in negative, positive pole tank,
Electronic/electrical lotus passes to negative, positive pole solid energy storage material.
The content of each substance is molar concentration in embodiment.
Embodiment 1: 100mL 0.02M 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: 100mL 0.4M 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: 100mL 0.8M 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 100mL 0.02M Fe (4,4 '-dmbpy)3Cl2+0.0002M C2H5NO2/HCl+0.02M
NaCl electrolyte
0.002mol FeCl is weighed first2It with 0.006mol 4,4 '-dmbpy, is placed in 250mL beaker, 50mL is added
Water is sufficiently stirred；Then 0.00002mol C is sequentially added2H5NO2, 0.00002molHCl, 0.002mol NaCl are sufficiently stirred
It mixes；Adding water to solution is 100mL, up to the electrolyte of required preparation.
Embodiment 5: it prepares 100mL 0.4M Fe (4,4 '-dmbpy)3Cl2+0.04M C2H5NO2/ HCl+0.8M NaCl electricity
Solve liquid
0.04mol FeCl is weighed first2It with 0.12mol 4,4 '-dmbpy, is placed in 250mL beaker, 50mL water is added,
It is sufficiently stirred；Then 0.004mol C is sequentially added2H5NO2, 0.004molHCl, 0.08mol NaCl are sufficiently stirred；It adds water to
Solution is 100mL, up to the electrolyte of required preparation.
Embodiment 6: it prepares 100mL 0.8M Fe (4,4 '-dmbpy)3Cl2+0.08M C2H5NO2/ HCl+1.6M NaCl electricity
Solve liquid
0.08mol FeCl is weighed first2It with 0.24mol 4,4 '-dmbpy, is placed in 250mL beaker, 50mL water is added,
It is sufficiently stirred；Then 0.008mol C is sequentially added2H5NO2, 0.008molHCl, 0.16mol NaCl are sufficiently stirred；It adds water to
Solution is 100mL, up to the electrolyte of required preparation.
Embodiment 7:
A of the invention10The anion-exchange membrane and cation-exchange membrane and battery case of model flow battery surround 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 10ml 0.02M 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 10ml 0.02M Fe (4,4 '-dmbpy)3Cl2+0.0002M C2H5NO2/
HCl+0.02M NaCl solution, Prussian blue in positive tank are 2.86 grams；Charging and discharging currents are 10mA, and electrolyte flow rate is
The energy density of 10mL/min, battery are 109Wh/L, are 2.18 times of all-vanadium flow battery energy density (50Wh/L).
Embodiment 8:
A of the invention10The anion-exchange membrane and cation-exchange membrane and battery case of model flow battery surround 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 10ml 0.4M K3Fe(CN)6+0.8M C6H12N4/ HCl+0.8M NaCl solution, in cathode pot
Prussian blue is 2.15 grams；Anode electrolyte is 10ml 0.4M Fe (4,4 '-dmbpy)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/
The energy density of min, battery are 116Wh/L, are 2.32 times of all-vanadium flow battery energy density (50Wh/L).
Embodiment 9:
A of the invention10The anion-exchange membrane and cation-exchange membrane and battery case of model flow battery surround 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 10ml 00.8M K3Fe(CN)6+1.6M C6H12N4/ HCl+1.6M NaCl solution, in cathode pot
It is Prussian blue be 2.15 grams；Anode electrolyte is 10ml 0.8M Fe (4,4 '-dmbpy)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/
The energy density of min, battery are 112Wh/L, are 2.24 times of all-vanadium flow battery energy density (50Wh/L).
Claims (9)
1. a kind of positive and negative anodes electrolyte, including anode electrolyte and electrolyte liquid, 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；
The composition of the anode electrolyte are as follows: 0.02-0.8M Fe (4,4 '-dmbpy)3Cl2+0.0002-0.08M C2H5NO2/
HCl+0.02-1.6M NaCl；Wherein, 4,4 '-dmbpy are 4,4 '-dimethyl -2, and 2 '-bipyridyls, structural formula is as follows:
2. the method for preparing electrolyte liquid described in claim 1, 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。
3. the method for preparing anode electrolyte described in claim 1, it is characterized in that: including the following steps, following number expression thing
The amount of matter:
Step A weighs 1 part of FeCl2With 3 part 4,4 '-dimethyl -2,2 '-bipyridyls are soluble in water, are 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 (4,4 '-dmbpy)3Cl2+0.0002-
0.08M C2H5NO2/HCl+0.02-1.6M NaCl。
4. the A that positive and negative anodes electrolyte is constituted described in claim 110Model flow battery, it is characterized in that: the electrolyte liquid
Active material be K3Fe(CN)6, constant pH is maintained with hexa-hydrochloric acid, and corresponding cathode solid-state
Energy storage material is Prussian blue Fe4[Fe(CN)6]3；Anode electrolyte active material is Fe (4,4 '-dmbpy)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；It is logical
Cross intermediate K3Fe(CN)6With Fe (4,4 '-dmbpy)3Cl2Redox realize the electronic/electrical lotus in positive and negative electrode and solid
Energy storage material Fe4[Fe(CN)6]3Between transmitting.
5. A according to claim 410Model flow battery, it is characterized in that: the pH of electrolyte liquid is 5.0-7.0；Just
The pH of pole electrolyte is 1.5-2.5.
6. A according to claim 410Model flow battery, it is characterized in that: the positive and negative electrode of battery cell selects carbon felt, stone
Black felt, graphite plate, graphite paper or carbon cloth inert material；Amberplex battery cell be divided into cathode chamber, anode chamber and in
Between sodium chloride electrolysis liquid chamber three parts, sodium chloride electrolyte concentration is 0.5-1.5M, and anode is in cathode chamber, and cathode is negative
In pole room；The amberplex selects cation-exchange membrane and anion-exchange membrane, and cation-exchange membrane is in cathode side, yin
Amberplex is in positive side.
7. A according to claim 410Model flow battery, it is characterized in that: the positive and negative electrode standard electric potential difference of battery cell
For 0.65V.
8. A according to claim 410Model flow battery, characterized in that 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 (4,4 '-dmbpy)3Cl2+0.0002-0.08M C2H5NO2/
HCl+0.02-1.6M NaCl；Wherein, 4,4 '-dmbpy are 4,4 '-dimethyl -2, and 2 '-bipyridyls, structural formula is as follows:
9. A according to claim 410Model flow battery, characterized in that electrode reaction is as follows:
Negative reaction:
Anode reaction:
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| CN201910240698.7A CN109888339A (en) | 2019-03-28 | 2019-03-28 | Positive and negative anodes electrolyte and preparation method thereof and in A10It is applied in model flow battery |
| 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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| CN201910240698.7A CN109888339A (en) | 2019-03-28 | 2019-03-28 | Positive and negative anodes electrolyte and preparation method thereof and in A10It is applied in model flow battery |
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Application publication date: 20190614 |