A Synergistic Strategy of Organic Molecules Introduced a High Zn²⁺Flux Solid Electrolyte Interphase for Stable Aqueous Zinc-Ion Batteries

Abstract

Aqueous rechargeable zinc-ion batteries (ARZIBs) are considered as attractive candidates for the next generation of high-safety and low-cost energy storage in large-scale power grids. However, challenges such as the dendrites and the corrosion on the zinc (Zn) surface result in short battery life and low reversibility of Zn plating/stripping. In this work, a method of preconditioning of a zinc anode in hybrid electrolytes (based on poly­(ethylene glycol)-200 and H2O) to form a solid electrolyte interphase (SEI) that prevents anode corrosion and dendrites is proposed. Though surface composition analysis and density functional theory calculation, this SEI has dense organic and inorganic components due to the induction of organic molecules and anions and has rapid kinetic and high-throughput properties for the transport of zinc ions. As a result, the SEI-modified Zn anode can maintain a low-voltage hysteresis stable cycle for more than 1600 h in aqueous electrolyte. The anode also exhibits impressive reversibility with a high Coulomobic efficiency of 99.23% over 1300 cycles. Furthermore, the ARZIB encapsulated by this anode and Mn-doped V6O13 cathode enables an outstanding electrochemical stability (181.8 mAh g–1 after 800 cycles at room temperature, 102.2 mAh g–1 after 1000 cycles at −15 °C). This work provides an intriguing idea for the stability maintenance of the anode for ARZIBs or other metal-ion batteries.

. Insights into the design of mildly acidic aqueous electrolytes for improved stability of Zn anode performance in zinc-ion batteries

“…On the contrary, the molecules containing polar groups have a great affinity to water and exhibit hydrophilicity. Some polar organics, like alcohols [27,[40][41][42][43][44][45] , sulfones [39,46] , and nitriles [47][48][49] , are widely utilized as additives/cosolvents in Zn batteries. Their introduction can not only maintain the homogeneity of electrolytes but also restrict water activity by breaking the H-bond network of water.…”

“…In addition, the wettability of Zn metal in electrolytes can be assessed by DFT calculation. The strong binding energy between the adsorbate [1, 3,25,42,43,60] . (B) Characterization approaches for studying Zn/electrolyte interfacial structures and compositions, including Raman, FTIR, NMR, XPS, and XRD.…”

“…However, excessive voltage polarization is a common issue with such electrolytes. The increase in salt concentrations results in decreased ionic conductivity and increased [3,17,18,23,25,27,31,33,36,37,[39][40][41][42][43][44][45][46][47][48][49][50][59][60][61][69][70][71][72][73][74][75][83][84][85][86][87][88][89][90][91][94][95][96][97][98][99][100][101][102][103]…”

“…In light of this, combining the merits of aqueous electrolytes and organic electrolytes, researchers have developed organic/aqueous hybrid electrolytes, where the organic solvents are regarded as cosolvents in aqueous electrolytes. Alcohols [27,[40][41][42][43][44][45] , ethers [25,69,120,121] , esters [50,31,[122][123][124] , sulfones [39,46] , nitriles [47][48][49] , and amides [125,126] are the currently known organic cosolvents. Abundant carboxyl groups in alcohols can be seen as H-bond acceptors; these carboxyl groups interact with water and break water H-bond networks, thereby reducing the activity of water.…”

Dual Pre-Insertion Strategy to Achieve High-Performance Vanadium Oxide toward Advanced Cylindrical Zinc Ion Batteries

“…Among these, lithium-ion batteries (LIBs) dominate the energy market due to their high energy density, long cycle life, and high operating voltage. However, low safety, scarcity of lithium resources, and high costs are serious obstacles to the further application of LIBs. − Among the alternatives, metal ion batteries and zinc ion batteries (ZIBs) are favored by researchers because of their environmental friendliness, low cost, and high safety. − Particulary, the high theoretical capacity (820 mAh g –1 ) and low redox potential (−0.76 V vs. standard hydrogen electrode (SHE)) of Zn metal − are attractive for commercial applications. However, the practical application of zinc ion batteries still suffers from some side reactions, dendrites, and dissolution of cathode materials.…”