Semi‐Immobilized Ionic Liquid Regulator with Fast Kinetics toward Highly Stable Zinc Anode under −35 to 60 °C

Abstract

Aqueous zinc ion batteries (ZIBs) have been extensively investigated as a next‐generation energy storage system due to their high safety and low cost. However, the critical issues of irregular dendrite growth and intricate side reactions severely restrict the further industrialization of ZIBs. Here, a strategy to fabricate a semi‐immobilized ionic liquid interface layer is proposed to protect the Zn anode over a wide temperature range from −35 to 60 °C. The immobilized SiO2@cation can form high conjugate racks that can regulate the Zn2+ concentration gradient and self‐polarizing electric field to guarantee uniform nucleation and planar deposition; the free anions of the ILs can weaken the hydrogen bonds of the water to promote rapid Zn2+ desolvation and accelerate ion‐transport kinetics simultaneously. Because of these unique advantages, the cycling performance of the symmetric Zn batteries is greatly enhanced, evidenced by a cycling life of 1800 h at 20 mA cm−2, and a cycle lifespan of 2000 h under a wide temperature window from −35 to 60 °C. The efficiency of this semi‐immobilizing strategy is well demonstrated in various full cells including pouch cells, showing high performance at large current (20 A g−1) and wide temperatures with extra‐long cycles up to 80 000 cycles.

Construction of zwitterionic osmolyte-based hydrogel electrolytes towards stable zinc anode for durable aqueous zinc ion storage and integrated electronics

“…The activation energy ( E a ) was further obtained from the temperature-dependent EIS curves to elaborate the desolvation of Zn 2+ ions and transport behavior at the Zn anode/electrolyte interface according to the Arrhenius equation: 9,49 where R ct , A , R , E a , and T represent the interfacial resistance, pre-exponential factor, molar gas constant, activation energy, and Kelvin temperature, respectively. 18 Consequently, the activation energies in different hydrogel electrolytes were determined by fitting the linear relationship between the charge-transfer resistance and the tested temperature (ranging from 10 to 60 °C). The smaller activation energy of 34.0 kJ mol −1 for SPS–Zn (compared with the activation energy of 42.7 kJ mol −1 in the Zn(CF 3 SO 3 ) 2 liquid electrolyte (denoted as LE)) indicates that the SPS–Zn hydrogel electrolyte promotes the desolvation of hydrated Zn 2+ ion with decreased energy consumption, which facilitates the fast Zn deposition kinetics (Fig.…”

“…Several approaches have been proposed to regulate Zn deposition for stabilizing zinc anodes. 17,18 For instance, Cui et al engineered a polymeric protective coating to increase the nucleation barrier and conne the planar diffusion of Zn 2+ to prevent dendrite growth. 13 Lan et al engineered the articial interface by developing zincophilic metal-covalent organic frameworks to form a dense interface for homogenizing the ion ux and manipulating the Zn deposition behaviors.…”

Engineering a self-adaptive electric double layer on both electrodes for high-performance zinc metal batteries

“…Aqueous zinc metal batteries (ZMBs) are receiving intense attention in large-scale electric transportation due to their intrinsic safety and low cost. 1 Zinc (Zn) metal, the most appealing aqueous anode material, shows a large theoretical capacity (820 mA h g −1 or 5855 mA h cm −3 ), as well as superior safety ascribed to its high compatibility with aqueous electrolytes. 2 The electrolytes (for example, 2 M ZnSO 4 and 1 M Zn(CF 3 SO 3 ) 2 ) commonly used in aqueous Zn metal batteries have ultra-high ionic conductivity and enable fast charge and discharge.…”

Simultaneously Stabilizing Both Electrodes and Electrolytes by a Self‐Separating Organometallics Interface for High‐Performance Zinc‐Ion Batteries at Wide Temperatures

“…[ 11–14 ] On the other hand, Zn anode also exhibits poor thermodynamics and electrochemical stability in aqueous electrolytes because of inevitable chemical corrosion, metal dendrites, and other side reactions. [ 15–17 ]…”

“…[11][12][13][14] On the other hand, Zn anode also exhibits poor thermodynamics and electrochemical stability in aqueous electrolytes because of inevitable chemical corrosion, metal dendrites, and other side reactions. [15][16][17] Recently, significant efforts have been exerted to solve the aforementioned problems in aqueous ZIBs. [18] In terms of the cathode, many strategies, such as ion/molecules pre-intercalation, defect engineering, and structural modification, have been adopted to optimize structure stability and improve capacity and cycling performance.…”