Polymer hetero-electrolyte enabled solid-state 2.4-V Zn/Li hybrid batteries

Ze Chen; Tairan Wang; Zhuoxi Wu; Yue Hou; Ao Chen; Yanbo Wang; Zhaodong Huang; Oliver G Schmidt; Minshen Zhu; Jun Fan; Chunyi Zhi

doi:10.1038/s41467-024-47950-w

Polymer hetero-electrolyte enabled solid-state 2.4-V Zn/Li hybrid batteries

Nat Commun. 2024 May 3;15(1):3748. doi: 10.1038/s41467-024-47950-w.

Authors

Ze Chen^#¹, Tairan Wang^#¹, Zhuoxi Wu¹, Yue Hou¹, Ao Chen¹, Yanbo Wang¹, Zhaodong Huang¹, Oliver G Schmidt^{2

3}, Minshen Zhu^{4

5}, Jun Fan⁶, Chunyi Zhi^{7

8

9}

Affiliations

¹ Department of Materials Science and Engineering, City University of Hong Kong, 83 Tat Chee Avenue, Kowloon, Hong Kong, 999077, China.
² Research Center for Materials, Architectures, and Integration of Nanomembranes (MAIN), TU Chemnitz, 09126, Chemnitz, Germany.
³ Material Systems for Nanoelectronics, TU Chemnitz, 09107, Chemnitz, Germany, TU Chemnitz, 09126, Chemnitz, Germany.
⁴ Research Center for Materials, Architectures, and Integration of Nanomembranes (MAIN), TU Chemnitz, 09126, Chemnitz, Germany. minshen.zhu@main.tu-chemnitz.de.
⁵ Material Systems for Nanoelectronics, TU Chemnitz, 09107, Chemnitz, Germany, TU Chemnitz, 09126, Chemnitz, Germany. minshen.zhu@main.tu-chemnitz.de.
⁶ Department of Materials Science and Engineering, City University of Hong Kong, 83 Tat Chee Avenue, Kowloon, Hong Kong, 999077, China. junfan@cityu.edu.hk.
⁷ Department of Materials Science and Engineering, City University of Hong Kong, 83 Tat Chee Avenue, Kowloon, Hong Kong, 999077, China. cy.zhi@cityu.edu.hk.
⁸ Hong Kong Center for Cerebro-Cardiovascular Health Engineering (COCHE), Shatin, NT, HKSAR, China. cy.zhi@cityu.edu.hk.
⁹ Hong Kong Institute for Clean Energy, City University of Hong Kong, Kowloon, 999077, Hong Kong. cy.zhi@cityu.edu.hk.

^# Contributed equally.

Abstract

The high redox potential of Zn^0/2+ leads to low voltage of Zn batteries and therefore low energy density, plaguing deployment of Zn batteries in many energy-demanding applications. Though employing high-voltage cathode like spinel LiNi_0.5Mn_1.5O₄ can increase the voltages of Zn batteries, Zn²⁺ ions will be immobilized in LiNi_0.5Mn_1.5O₄ once intercalated, resulting in irreversibility. Here, we design a polymer hetero-electrolyte consisting of an anode layer with Zn²⁺ ions as charge carriers and a cathode layer that blocks the Zn²⁺ ion shuttle, which allows separated Zn and Li reversibility. As such, the Zn‖LNMO cell exhibits up to 2.4 V discharge voltage and 450 stable cycles with high reversible capacity, which are also attained in a scale-up pouch cell. The pouch cell shows a low self-discharge after resting for 28 days. The designed electrolyte paves the way to develop high-voltage Zn batteries based on reversible lithiated cathodes.