Rational Design of an In-Situ Polymer-Inorganic Hybrid Solid Electrolyte Interphase for Realising Stable Zn Metal Anode under Harsh Conditions

Ruwei Chen; Wei Zhang; Chaohong Guan; Yundong Zhou; Ian Gilmore; Hao Tang; Zhenyu Zhang; Haobo Dong; Yuhang Dai; Zijuan Du; Xuan Gao; Wei Zong; Yewei Xu; Peie Jiang; Jiyang Liu; Fangjia Zhao; Jianwei Li; Xiaohui Wang; Guanjie He

doi:10.1002/anie.202401987

Rational Design of an In-Situ Polymer-Inorganic Hybrid Solid Electrolyte Interphase for Realising Stable Zn Metal Anode under Harsh Conditions

Angew Chem Int Ed Engl. 2024 Mar 25:e202401987. doi: 10.1002/anie.202401987. Online ahead of print.

Authors

Ruwei Chen^{1

2}, Wei Zhang¹, Chaohong Guan³, Yundong Zhou⁴, Ian Gilmore⁴, Hao Tang², Zhenyu Zhang⁵, Haobo Dong¹, Yuhang Dai¹, Zijuan Du¹, Xuan Gao¹, Wei Zong¹, Yewei Xu¹, Peie Jiang¹, Jiyang Liu¹, Fangjia Zhao¹, Jianwei Li¹, Xiaohui Wang², Guanjie He¹

Affiliations

¹ Department of Chemistry, University College London, London, WC1E 7JE, UK.
² State Key Laboratory of Pulp and Paper Engineering, South China University of Technology, Guangzhou, 510641, China.
³ University of Michigan-Shanghai Jiao Tong University Joint Institute, Shanghai Jiao Tong University, Shanghai, 200240, China.
⁴ National Physical Laboratory, Hampton Road, Teddington, TW11 0LW, UK.
⁵ Electrochemical Innovation Lab, Department of Chemical Engineering, University College London, London, WC1E 7JE, UK.

PMID: 38526053
DOI: 10.1002/anie.202401987

Abstract

The in-depth understanding of the composition-property-performance relationship of solid electrolyte interphase (SEI) is the basis of developing a reliable SEI to stablize the Zn anode-electrolyte interface, but it remains unclear in rechargeable aqueous zinc ion batteries. Herein, a well-designed electrolyte based on 2 M Zn(CF₃SO₃)₂-0.2 M acrylamide-0.2 M ZnSO₄ is proposed. A robust polymer (polyacrylamide)-inorganic (Zn₄SO₄(OH)₆.xH₂O) hybrid SEI is in situ constructed on Zn anodes through controllable polymerization of acrylamide and coprecipitation of SO₄ ^2- with Zn²⁺ and OH^-. For the first time, the underlying SEI composition-property-performance relationship is systematically investigated and correlated. The results showed that the polymer-inorganic hybrid SEI, which integrates the high modulus of the inorganic component with the high toughness of the polymer ingredient, can realize high reversibility and long-term interfacial stability, even under ultrahigh areal current density and capacity (30 mA cm^-2~30 mAh cm^-2). The resultant Zn||NH₄V₄O₁₀ cell also exhibits excellent cycling stability. This work will provide a guidance for the rational design of SEI layers in rechargeable aqueous zinc ion batteries.

Keywords: Aqueous Zinc-Ion batteries; Polymer-Inorganic SEI; Solid Electrolyte Interphase; Zinc Anode.

Abstract

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