CN115966783A - Aqueous zinc ion battery electrolyte and application thereof - Google Patents
Aqueous zinc ion battery electrolyte and application thereof Download PDFInfo
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- CN115966783A CN115966783A CN202310140907.7A CN202310140907A CN115966783A CN 115966783 A CN115966783 A CN 115966783A CN 202310140907 A CN202310140907 A CN 202310140907A CN 115966783 A CN115966783 A CN 115966783A
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- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
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Abstract
The application discloses water system zinc ion battery electrolyte and application thereof, the electrolyte comprises zinc salt, amphoteric molecule additive and pure water, the chemical general formula of the amphoteric molecule additive is M-R-N, wherein M contains a positively charged quaternary ammonium group, N is a negatively charged sulfonate group or carboxylate group, R is a saturated alkyl carbon chain, the saturated alkyl carbon chain is used for connecting the positively charged quaternary ammonium group and the negatively charged sulfonate group or carboxylate group, the amphoteric molecule additive is neutral charge, the electrolyte is applied to a zinc-based energy storage device, the zinc-based energy storage device comprises a zinc ion battery, a zinc ion mixed capacitor and a zinc air battery, corrosion of interface water molecules to a zinc cathode is reduced, dendritic crystal growth is inhibited, compact and uniform deposition is realized, and the utilization rate of the zinc metal cathode is improved.
Description
Technical Field
The invention belongs to the technical field of electrolyte, and particularly relates to a water-based zinc ion battery electrolyte and application thereof.
Background
In recent years, the problems of traditional energy shortage, environmental pollution and the like are becoming more severe, and the vigorous development of renewable energy sources is promoted. Meanwhile, the development of stable, reliable and safe energy storage technology is urgent. Although the conventional lithium ion battery occupies most of the energy storage market due to its excellent energy density and cycle stability, its inherent cost and safety problems severely limit its application in large-scale energy storage and wearable devicesApplication in a domain. The aqueous ion battery can fundamentally avoid the safety problem caused by thermal runaway of the inflammable organic electrolyte and greatly reduce the manufacturing cost. Wherein, the water system zinc ion battery has high theoretical capacity (the volume capacity is 5855mA h cm) -3 Mass specific capacity 820mA hr g -1 ) And the material and assembly cost is low, and the like, and the lithium ion battery becomes one of secondary batteries which are hopeful to replace the traditional lithium ion battery and realize large-scale industrialization.
The development of zinc ion batteries is greatly dependent on the breakthrough of the performance of metal zinc negative. The zinc metal cathode has the problems of dendritic crystal growth, electrolyte side reaction and the like, and the problems of low coulomb efficiency and limited cycle life are often caused especially under the conditions of large current/large capacity charge and discharge. In addition, the irreversible deposition/peeling of the negative electrode makes the zinc negative electrode have low utilization rate, and the energy density of the zinc ion battery is severely limited. In view of the above problems, researchers have conducted a great deal of research, which mainly includes: designing a three-dimensional current collector, constructing an artificial interface layer, developing an electrolyte additive and the like. Among them, improving the zinc negative electrode problem by introducing an electrolyte additive is one of the simplest and economical methods. The proper additive can be preferentially adsorbed on the interface, so that the ion concentration and the electric field distribution of the zinc cathode interface are effectively balanced, and the uniform deposition of zinc is realized; meanwhile, the solvation structure of zinc ions in the solution can be regulated and controlled, the content of interface active water molecules is obviously reduced, and the hydrogen evolution side reaction is effectively inhibited. Currently, researchers have reported many useful additives for aqueous zinc ion battery electrolytes, mainly including cationic additives, anionic additives, organic molecule additives, etc. However, the electrolytes developed so far still have the following problems. Firstly, the cationic additive can adjust the interface electric field and effectively shield the 'tip effect' in the zinc deposition process, but can not effectively adjust and control the solvation structure of zinc ions in the electrolyte. Secondly, for anionic additives and organic molecular additives, abundant nucleophilic sites can effectively adjust a zinc ion solvation structure and effectively inhibit hydrogen evolution reaction, but the additives are often poor in compatibility with zinc salt solutions, so that the additives are small in dissolubility range and cannot fully play a protection role. In addition, in the process of charging and discharging, the interface state is continuously and dynamically changed, and particularly in the process of heavy current and deep discharging, the protective effect of the additive on the cathode interface is greatly uncertain, so that the interface protective effect is possibly invalid, the utilization rate of the zinc cathode cannot be improved, and the energy density of the zinc ion battery is severely limited. Based on the above analysis, it is urgently needed to develop a novel electrolyte additive, inhibit dendritic crystal growth and hydrogen evolution side reaction, and improve the utilization rate of the zinc cathode.
Disclosure of Invention
The invention aims to solve the problems in the background art and provides a water-based zinc ion battery electrolyte and application thereof.
In order to achieve the purpose, the invention provides an aqueous zinc ion battery electrolyte, which comprises a zinc salt, an amphiphilic additive and pure water, wherein the chemical general formula of the amphiphilic additive is M-R-N, M contains a positively charged quaternary ammonium group, N is a negatively charged sulfonate group or carboxylate group, R is a saturated alkyl carbon chain, the saturated alkyl carbon chain is used for connecting the positively charged quaternary ammonium group and the negatively charged sulfonate group or carboxylate group, and the amphiphilic additive is neutral charge.
Preferably, the zinc salt comprises at least one of zinc sulfate, zinc chloride, zinc trifluoromethanesulfonate, zinc acetate and zinc nitrate.
Preferably, the concentration of the zinc salt in the electrolyte is 1 to 3M.
Preferably, the concentration of the amphoteric molecule additive in the electrolyte is 0.005 to 4M.
Preferably, M in the chemical formula of the amphiphilic molecular additive is (CH) 3 ) 3 N + -、C n H 2n+1 (CH 3 ) 2 N + -(n＝2～5)C 2 H 4 OH(CH 3 ) 2 N + -
One kind of (1).
Preferably, when N in the chemical formula of the amphiphilic additive is a negatively charged sulfonate group, the amphiphilic additive is a sulfonic amphiphilic molecule.
Preferably, the amphiphilic additive is a carboxylic acid-based amphiphilic molecule when N in the chemical formula of the amphiphilic additive is a negatively charged carboxylate group.
The invention also provides an application of the electrolyte in a zinc-based energy storage device, wherein the zinc-based energy storage device comprises at least one of a zinc ion battery, a zinc ion hybrid capacitor and a zinc-air battery.
The invention has the beneficial effects that:
1) The amphoteric molecule additive contained in the electrolyte provided by the invention is an amphoteric molecule containing positive charges and negative charges, the additive can be adsorbed on the surface of a zinc cathode in a self-adaptive manner in preference to water molecules, the corrosion of interfacial water molecules on the zinc cathode is effectively reduced, and meanwhile, the additive molecules adsorbed on a zinc electrode/electrolyte interface can be used for homogenizing an interfacial electric field and inhibiting the two-dimensional diffusion of zinc ions, so that the growth of dendritic crystals is effectively inhibited, and the compact and uniform deposition is realized.
2) According to the invention, the electrolyte is added with the amphiprotic molecular additive, and negative electricity groups of the amphiprotic molecular additive can participate in a solvation structure of zinc ions, so that water molecules of the solvation are reduced, and side reactions of interface hydrogen evolution are effectively inhibited.
3) Compared with the electrolyte without the additive, the electrolyte containing the amphiprotic molecular additive can greatly prolong the cycle life of the zinc/zinc symmetrical battery and obviously improve the utilization rate of a zinc metal cathode.
4) The amphoteric molecular additive in the electrolyte provided by the invention has solubility greater than 2M in zinc salt solution, has good compatibility with zinc ions, and has wide adjustable concentration range when being used with various zinc salts and other additives.
The features and advantages of the present invention will be described in detail by embodiments in conjunction with the accompanying drawings.
Drawings
FIG. 1 shows the zinc/zinc cell of example 1 and comparative example 1 of the present invention at 5mA cm -2 ，5mAh cm -2 Constant current charge and discharge curve diagram under the condition.
FIG. 2 shows zinc/zinc symmetrical cells at 5mA cm for example 2 and comparative example 2 of the present invention -2 ，5mAh cm -2 Constant current charge and discharge curve diagram under the condition.
Fig. 3 is an XRD pattern after 5 days of zinc sheet soaking in the electrolytes of example 3 and comparative example 3 of the present invention.
FIG. 4 is a graph showing the deposition profile of zinc on a copper foil in the electrolytes of example 3 and comparative example 3 of the present invention.
FIG. 5 shows zinc/zinc symmetrical cells at 10mA cm for example 3 and comparative example 3 of the present invention -2 ，10mAh cm -2 Constant current charge and discharge curve diagram under the condition.
FIG. 6 shows the zinc/zinc cell of example 4 and comparative example 4 of the present invention at 5mA cm -2 ，5mAh cm -2 Constant current charge and discharge curve diagram under the condition.
FIG. 7 shows zinc/zinc symmetric cells of example 4 and comparative example 4 of the present invention at 10mA cm -2 ，15mAh cm -2 Constant current charge and discharge curve diagram under the condition.
Detailed Description
In order to make the objects, technical solutions and advantages of the embodiments of the present application clearer, the technical solutions in the embodiments of the present application will be clearly and completely described below with reference to the drawings in the embodiments of the present application. It is to be understood that the embodiments described are only a few embodiments of the present application and not all embodiments.
Example 1
The embodiment provides an aqueous zinc ion battery electrolyte, which comprises a zinc salt, an amphiphilic molecular additive and pure water, wherein the chemical general formula of the amphiphilic molecular additive is M-R-N, wherein M is a quaternary ammonium group containing positive charges
N is a negatively charged sulfonate group>
R is a saturated alkyl carbon chain-C 3 H 6 The amphoteric molecular additive is abbreviated to PPS, saturated alkyl carbon chain-C 3 H 6 Quaternary ammonium groups for linking positively charged groups>
And negatively charged sulfonate groups>
The amphoteric molecule additive is sulfonic amphoteric molecule, the amphoteric molecule additive is neutral charge, zinc salt is zinc sulfate, the concentration of zinc sulfate in the electrolyte is 2M, and the concentration of the amphoteric molecule additive PPS in the electrolyte is 0.5M.
In the preparation of the electrolyte of this example, 0.05mol of PPS and 0.2mol of ZnSO were added 4 ·7H 2 O is completely dissolved in 100mL of deionized water to obtain a 2M zinc sulfate solution containing 0.5M PPS, and the solution is used as an electrolyte of a zinc ion battery.
Example 2
The embodiment provides an aqueous zinc ion battery electrolyte, which comprises a zinc salt, an amphiphilic additive and pure water, wherein the chemical general formula of the amphiphilic additive is M-R-N, wherein M is a compound containing a positively charged quaternary ammonium group (CH) 3 ) 3 N + -, N is a negatively charged sulfonate group
R is a saturated alkyl carbon chain-C 3 H 6 The amphoteric molecular additive is abbreviated as NDSB, saturated alkyl carbon chain-C 3 H 6 Quaternary ammonium groups (CH) for linking positively charged groups 3 ) 3 N + And also negatively charged sulfonate groups>
The amphoteric molecule additive is sulfonic amphoteric molecule, the amphoteric molecule additive is neutral charge, the zinc salt is zinc chloride, the concentration of the zinc chloride in the electrolyte is 2M, and the concentration of the amphoteric molecule additive NDSB in the electrolyte is highThe degree was 0.1M.
In preparing the electrolyte of this example, 0.01mol of NDSB and 0.2mol of ZnCl were added 2 Completely dissolved in 100mL of deionized water to obtain a 2M zinc chloride solution containing 0.1M NDSB, which was used as an electrolyte for a zinc ion battery.
Example 3
The embodiment provides an aqueous zinc ion battery electrolyte, which comprises a zinc salt, an amphiphilic additive and pure water, wherein the chemical general formula of the amphiphilic additive is M-R-N, wherein M is a compound containing a positively charged quaternary ammonium group (CH) 3 ) 3 N + -, N is a negatively charged carboxylate radical-COO - R is a saturated alkyl carbon chain-CH 2 -, the amphoteric molecular additive is abbreviated as BT, saturated alkyl carbon chain-CH 2 Quaternary ammonium groups (CH) for linking positively charged groups 3 ) 3 N + And a negatively charged carboxylate group-COO - The amphoteric molecule additive is carboxylic acid radical amphoteric molecule, the amphoteric molecule additive is neutral charge, the zinc salt is zinc sulfate, the concentration of the zinc sulfate in the electrolyte is 2M, and the concentration of the amphoteric molecule additive BT in the electrolyte is 0.5M.
In the preparation of the electrolyte of this example, 0.05mol of BT and 0.2mol of ZnSO were added 4 ·7H 2 And completely dissolving O in 100mL of deionized water to obtain a 2M zinc sulfate solution containing 0.5M BT, and taking the solution as the electrolyte of the zinc ion battery.
Example 4
The embodiment provides an aqueous zinc ion battery electrolyte, which comprises a zinc salt, an amphiphilic additive and pure water, wherein the chemical general formula of the amphiphilic additive is M-R-N, wherein M is a compound containing a positively charged quaternary ammonium group (CH) 3 ) 3 N + N is a negatively charged carboxylate radical-COO - R is a saturated alkyl carbon chain-CH with hydroxyl 2 CHOHCH 2 The amphoteric molecular additive is abbreviated as LCT, saturated alkyl carbon chain-CH 2 CHOHCH 2 Quaternary ammonium groups (CH) for linking positively charged groups 3 ) 3 N + And a negatively charged carboxylate group-COO - The amphiphilic additive is carboxylic acid group amphiproticThe amphoteric molecular additive is neutral charge, zinc salt is zinc sulfate, the concentration of zinc sulfate in the electrolyte is 2M, and the concentration of the amphoteric molecular additive LCT in the electrolyte is 0.5M.
In preparing the electrolyte of this example, 0.05mol of LCT and 0.2mol of ZnSO were added 4 ·7H 2 And completely dissolving O in 100mL of deionized water to obtain a 2M zinc sulfate solution containing 0.5M LCT, and taking the solution as the electrolyte of the zinc ion battery.
Comparative example 1
The electrolyte used in this comparative example was prepared in the same manner as in example 1 except that PPS was not added, and the electrolyte was a 2M zinc sulfate solution.
Comparative example 2
The electrolyte used in this comparative example was prepared in the same manner as in example 2 except that NDSB was not added, and the electrolyte was a 2M zinc chloride solution.
Comparative example 3
The electrolyte used in this comparative example was prepared as in example 3 except that no BT was added, and the electrolyte was a 2M zinc sulfate solution.
Comparative example 4
The electrolyte used in this comparative example was prepared as in example 4 except that LCT was not added and the electrolyte was a 2M zinc sulfate solution.
Test on the Effect of different electrolytes on the Life of Zinc ion batteries
The electrolyte of the embodiment 1, the comparison example 1, the embodiment 2 and the comparison example 2 is respectively taken to assemble the button type zinc/zinc symmetrical battery by taking a zinc sheet with the thickness of 0.1mm as an electrode and glass fiber as a diaphragm, and the electrolyte is arranged at 5mA cm -2 And 5mAh cm -2 The cycle performance of the batteries was tested under the conditions of (1), and the cycle lives of the batteries containing the electrolytes of example 1 and comparative example 1 are shown in fig. 1, and the cycle lives of the batteries containing the electrolytes of example 2 and comparative example 2 are shown in fig. 2.
As can be seen from FIG. 1, the current density was 5mA cm -2 And 5mAh cm -2 Under the conditions of high current and high deposition capacity, the cycle life of the battery with the electrolyte added with the PPS is as long as 290h, and the battery without the electrolyte of the PPSThe cycle life was only 58h.
As can be seen from FIG. 2, the current density was 5mA cm -2 And 5mAh cm -2 Under the conditions of high current and high deposition capacity, the battery cycle life of the electrolyte added with the NDSB is as long as 850h, and the battery cycle life of the electrolyte without the PPS is only 94h.
The electrolyte of the embodiment 3 and the electrolyte of the comparative example 3 are respectively taken to assemble the button zinc/zinc symmetrical battery by taking a zinc sheet with the thickness of 26 microns as an electrode and glass fiber as a diaphragm at the temperature of 10mA cm -2 ，10mAh cm -2 Deep discharge (zinc utilization of 65%) under the condition, and the zinc utilization and the cycle life of the battery are tested, and specific test results are shown in fig. 5.
As can be seen from fig. 5, the cycle life of the battery using the electrolyte of comparative example 3 containing no BT was less than 50h; the cycle life of the battery using the electrolyte containing BT of example 3 reached 300h.
The electrolyte of the embodiment 4 and the electrolyte of the comparative example 4 are respectively taken to assemble the button zinc/zinc symmetrical battery by taking a zinc sheet with the thickness of 30 microns as an electrode and glass fiber as a diaphragm at the concentration of 10mA cm -2 ，15mAh cm -2 The zinc utilization rate and the cycle life of the battery are tested by deep discharge under the condition (the zinc utilization rate is 85%), and the specific test result is shown in fig. 7.
As can be seen from fig. 7, the cycle life of the battery using the electrolyte of comparative example 4 containing no LCT was less than 1h; whereas the cycle life of the cell using the electrolyte containing LCT of example 4 reached 150h.
Test on the influence of different electrolytes on hydrogen evolution reaction of zinc sheets
The same amount of the electrolytes prepared in example 3 and comparative example 3 were taken, two zinc plates having the same volume and mass were immersed in the two electrolytes, respectively, and after standing for 5 days, crystal phase analysis was performed, and the specific test results are shown in fig. 3.
As can be seen from fig. 3, zinc sulfate by-products do not appear in the electrolyte containing BT in example 3, indicating that the zinc sheet has good stability in the electrolyte, and the electrolyte can effectively inhibit side reactions such as hydrogen evolution; in the electrolyte of the comparative example 3 without BT, the zinc sheet has a diffraction peak at 5-30 degrees, which is attributed to the basic zinc sulfate by-product, and the result shows that the zinc sheet is corroded by the electrolyte in the electrolyte and has serious hydrogen evolution reaction.
Test on influence of different electrolytes on deposition morphology of zinc sheet on copper foil
The electrolytes prepared in example 3 and comparative example 3 were used in equal amounts, and the deposition current density was 5mA cm -2 The deposition capacity was 1mAh cm -2 Under the conditions of (1), the deposition morphology of the two zinc sheets on the copper foil is respectively observed, and the specific test result is shown in fig. 4.
As can be seen from fig. 4, fig. 4a and 4b show the deposition morphology of the zinc sheet on the copper foil in the electrolyte without BT of comparative example 3, and it can be seen that the deposition morphology of the zinc sheet is relatively loose and has a large amount of dendrites; and FIG. 4c shows that the deposition morphology of the zinc sheet in the electrolyte containing BT in example 3 is uniform and dense, and no dendrite is generated.
Test on the Effect of different concentrations of amphoteric molecular additives on Battery Life
Respectively taking 0.005mol, 0.01mol, 0.05mol and 0.1mol of LCT and 0.2mol of ZnSO 4 ·7H 2 Dissolving O in 100mL deionized water completely to obtain 2M zinc sulfate solution containing LCT with different concentrations, using the solution as electrolyte of zinc ion battery, using 0.1mm thick zinc sheet as electrode, using glass fiber as diaphragm to assemble button zinc/zinc symmetrical battery, and measuring the total volume of electrolyte in 5mA cm -2 ，5mAh cm -2 The cycle performance of each symmetrical cell was tested under the conditions, and the specific test results are shown in fig. 6.
As can be seen from FIG. 6, the battery life was 620h for the LCT additive concentration of 0.05M, 950h for the LCT additive concentration of 0.1M, and 890h for the LCT additive concentration of 0.5M.
The above embodiments are illustrative of the present invention, and are not intended to limit the present invention, and any simple modifications of the present invention are within the scope of the present invention.
Claims (8)
1. An aqueous zinc ion battery electrolyte, characterized in that: the electrolyte comprises zinc salt, an amphoteric molecule additive and pure water, wherein the amphoteric molecule additive has a chemical general formula of M-R-N, wherein M contains a positively charged quaternary ammonium group, N is a negatively charged sulfonate group or carboxylate group, R is a saturated alkyl carbon chain which is used for connecting the positively charged quaternary ammonium group and the negatively charged sulfonate group or carboxylate group, and the amphoteric molecule additive is neutral charge.
2. The aqueous zinc ion battery electrolyte of claim 1, wherein: the zinc salt comprises at least one of zinc sulfate, zinc chloride, zinc trifluoromethanesulfonate, zinc acetate and zinc nitrate.
3. The aqueous zinc ion battery electrolyte of claim 1, wherein: the concentration of the zinc salt in the electrolyte is 1-3M.
4. The aqueous zinc ion battery electrolyte of claim 1, wherein: the concentration of the amphoteric molecule additive in the electrolyte is 0.005-4M.
5. The aqueous zinc ion battery electrolyte of claim 1, wherein: the chemical general formula of the amphoteric molecular additive is that M is (CH) 3 ) 3 N + -、C n H 2n|1 (CH 3 ) 2 N + -(n＝2～5)、C 2 H 4 OH(CH 3 ) 2 N + -、
One kind of (1).
6. The aqueous zinc ion battery electrolyte of claim 1, wherein: when N in the chemical general formula of the amphoteric molecular additive is a negatively charged sulfonate group, the amphoteric molecular additive is a sulfonic amphoteric molecule.
7. The aqueous zinc ion battery electrolyte of claim 1, wherein: when N in the chemical formula of the amphiprotic molecular additive is a negatively charged carboxylate group, the amphiprotic molecular additive is a carboxylic acid-based amphiprotic molecule.
8. Use of the electrolyte of any of claims 1 to 7 in a zinc-based energy storage device, characterized in that: the zinc-based energy storage device comprises at least one of a zinc ion battery, a zinc ion hybrid capacitor and a zinc-air battery.
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