Trace Amounts of Triple-Functional Additives Enable Reversible Aqueous Zinc-Ion Batteries from a Comprehensive Perspective

Ruwei Chen; Wei Zhang; Quanbo Huang; Chaohong Guan; Wei Zong; Yuhang Dai; Zijuan Du; Zhenyu Zhang; Jianwei Li; Fei Guo; Xuan Gao; Haobo Dong; Jiexin Zhu; Xiaohui Wang; Guanjie He

doi:10.1007/s40820-023-01050-4

Trace Amounts of Triple-Functional Additives Enable Reversible Aqueous Zinc-Ion Batteries from a Comprehensive Perspective

Nanomicro Lett. 2023 Mar 31;15(1):81. doi: 10.1007/s40820-023-01050-4.

Authors

Ruwei Chen^#^{1

2}, Wei Zhang^#¹, Quanbo Huang^#², Chaohong Guan³, Wei Zong¹, Yuhang Dai¹, Zijuan Du¹, Zhenyu Zhang¹, Jianwei Li¹, Fei Guo¹, Xuan Gao¹, Haobo Dong¹, Jiexin Zhu¹, Xiaohui Wang⁴, Guanjie He⁵

Affiliations

¹ Electrochemical Innovation Lab, Department of Chemical Engineering, University College London, London, WC1E 7JE, UK.
² State Key Laboratory of Pulp and Paper Engineering, South China University of Technology, Guangzhou, 510640, People's Republic of China.
³ University of Michigan-Shanghai Jiao Tong University Joint Institute, Shanghai Jiao Tong University, Shanghai, 200240, People's Republic of China.
⁴ State Key Laboratory of Pulp and Paper Engineering, South China University of Technology, Guangzhou, 510640, People's Republic of China. fewangxh@scut.edu.cn.
⁵ Electrochemical Innovation Lab, Department of Chemical Engineering, University College London, London, WC1E 7JE, UK. g.he@ucl.ac.uk.

^# Contributed equally.

Abstract

Although their cost-effectiveness and intrinsic safety, aqueous zinc-ion batteries suffer from notorious side reactions including hydrogen evolution reaction, Zn corrosion and passivation, and Zn dendrite formation on the anode. Despite numerous strategies to alleviate these side reactions have been demonstrated, they can only provide limited performance improvement from a single aspect. Herein, a triple-functional additive with trace amounts, ammonium hydroxide, was demonstrated to comprehensively protect zinc anodes. The results show that the shift of electrolyte pH from 4.1 to 5.2 lowers the HER potential and encourages the in situ formation of a uniform ZHS-based solid electrolyte interphase on Zn anodes. Moreover, cationic NH⁴⁺ can preferentially adsorb on the Zn anode surface to shield the "tip effect" and homogenize the electric field. Benefitting from this comprehensive protection, dendrite-free Zn deposition and highly reversible Zn plating/stripping behaviors were realized. Besides, improved electrochemical performances can also be achieved in Zn//MnO₂ full cells by taking the advantages of this triple-functional additive. This work provides a new strategy for stabilizing Zn anodes from a comprehensive perspective.

Keywords: Aqueous zinc-ion battery; Cationic shielding effect; Solid electrolyte interphase; Triple-functional additive; pH value.