N-methyl Formamide Electrolyte Additive Enabling Highly Reversible Zn Anodes

Peter Joseph Chimtali; Xiya Yang; Quan Zhou; Shiqiang Wei; Zeinab Mohamed; Hassan Akhtar; Aad Al-Mahgari; Yuzhu Zhou; Hanchen Xu; Zijun Zhang; Dengfeng Cao; Shuangming Chen; Kefu Zhu; Xin Guo; Hongwei Shou; Xiaojun Wu; Changda Wang; Li Song

doi:10.1002/smll.202400673

N-methyl Formamide Electrolyte Additive Enabling Highly Reversible Zn Anodes

Small. 2024 May 3:e2400673. doi: 10.1002/smll.202400673. Online ahead of print.

Authors

Peter Joseph Chimtali¹, Xiya Yang¹, Quan Zhou¹, Shiqiang Wei¹, Zeinab Mohamed¹, Hassan Akhtar¹, Aad Al-Mahgari¹, Yuzhu Zhou¹, Hanchen Xu¹, Zijun Zhang¹, Dengfeng Cao¹, Shuangming Chen¹, Kefu Zhu¹, Xin Guo¹, Hongwei Shou^{1

2}, Xiaojun Wu^{1

2}, Changda Wang¹, Li Song^{1

3}

Affiliations

¹ National Synchrotron Radiation Laboratory, Key Laboratory of Precision and Intelligent Chemistry, School of Nuclear Science and Technology, University of Science and Technology of China, Hefei, Anhui, 230029, P. R. China.
² School of Chemistry and Material Sciences, University of Science and Technology of China, Hefei, Anhui, 230029, P. R. China.
³ Zhejiang Institute of Photonelectronics, Jinhua, Zhejiang, 321004, P. R. China.

PMID: 38700057
DOI: 10.1002/smll.202400673

Abstract

Parasitic side reactions and dendrites formation hinder the application of aqueous zinc ion batteries due to inferior cycling life and low reversibility. Against this background, N-methyl formamide (NMF), a multi-function electrolyte additive is applied to enhance the electrochemical performance. Studied via advanced synchrotron radiation spectroscopy and DFT calculations, the NMF additive simultaneously modifies the Zn²⁺ solvation structure and ensures uniform zinc deposition, thus suppressing both parasitic side reactions and dendrite formation. More importantly, an ultralong cycling life of 3115 h in the Zn||Zn symmetric cell at a current density of 0.5 mA cm^-2 is achieved with the NMF additive. Practically, the Zn||PANI full cell utilizing NMF electrolyte shows better rate and cycling performance compared to the pristine ZnSO₄ aqueous electrolyte. This work provides useful insights for the development of high-performance aqueous metal batteries.

Keywords: DFT calculations; N‐methyl formamide; advanced synchrotron radiation spectroscopy; electrolyte; solvation structure; zinc ion battery.

Abstract

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