Designing Solvated Double-Layer Polymer Electrolytes with Molecular Interactions Mediated Stable Interfaces for Sodium Ion Batteries

Jun Pan; Yuchen Zhang; Fu Sun; Markus Osenberg; André Hilger; Ingo Manke; Ruiguo Cao; Shi Xue Dou; Hong Jin Fan

doi:10.1002/anie.202219000

Designing Solvated Double-Layer Polymer Electrolytes with Molecular Interactions Mediated Stable Interfaces for Sodium Ion Batteries

Angew Chem Int Ed Engl. 2023 Apr 17;62(17):e202219000. doi: 10.1002/anie.202219000. Epub 2023 Mar 20.

Authors

Jun Pan¹, Yuchen Zhang², Fu Sun³, Markus Osenberg⁴, André Hilger⁴, Ingo Manke⁴, Ruiguo Cao², Shi Xue Dou⁵, Hong Jin Fan¹

Affiliations

¹ School of Physical and Mathematical Sciences, Nanyang Technological University, Singapore, 637371, Singapore.
² Hefei National Laboratory for Physical Science at the Microscale, CAS Key Laboratory of Materials for Energy Conversion, Department of Materials Science and Engineering, University of Science and Technology of China, Hefei, 230026, China.
³ Qingdao Institute of Bioenergy and Bioprocess Technology, Chinese Academy of Sciences, Qingdao, 266101, China.
⁴ Helmholtz-Zentrum Berlin für Materialien und Energie, Hahn-Meitner-Platz 1, 14109, Berlin, Germany.
⁵ Institute of Energy Materials Science, University of Shanghai for Science and Technology, Shanghai, 200093, China.

PMID: 36866855
DOI: 10.1002/anie.202219000

Abstract

Unstable cathode-electrolyte and/or anode-electrolyte interface in polymer-based sodium-ion batteries (SIBs) will deteriorate their cycle performance. Herein, a unique solvated double-layer quasi-solid polymer electrolyte (SDL-QSPE) with high Na⁺ ion conductivity is designed to simultaneously improve stability on both cathode and anode sides. Different functional fillers are solvated with plasticizers to improve Na⁺ conductivity and thermal stability. The SDL-QSPE is laminated by cathode- and anode-facing polymer electrolyte to meet the independent interfacial requirements of the two electrodes. The interfacial evolution is elucidated by theoretical calculations and 3D X-ray microtomography analysis. The Na_0.67 Mn_2/3 Ni_1/3 O₂ |SDL-QSPE|Na batteries exhibit 80.4 mAh g^-1 after 400 cycles at 1 C with the Coulombic efficiency close to 100 %, which significantly outperforms those batteries using the monolayer-structured QSPE.

Keywords: Double-Layer Polymer Electrolytes; Functional Filler; Molecular Intercalation; Quasi-Solid-State Sodium Ion Batteries; Stable Interfaces.

Abstract

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