Phosphorylated Covalent Organic Framework Membranes Toward Ultrafast Single Lithium-Ion Transport

Xiao Pang; Benbing Shi; Yawei Liu; Yunliang Li; Yafang Zhang; Tiantian Wang; Shuting Xu; Xiaoyao Wang; Ziwen Liu; Na Xing; Xu Liang; Ziting Zhu; Chunyang Fan; Ying Liu; Hong Wu; Zhongyi Jiang

doi:10.1002/adma.202413022

Phosphorylated Covalent Organic Framework Membranes Toward Ultrafast Single Lithium-Ion Transport

Adv Mater. 2024 Nov 12:e2413022. doi: 10.1002/adma.202413022. Online ahead of print.

Authors

Xiao Pang^{1

2}, Benbing Shi^{1

2}, Yawei Liu³, Yunliang Li^{4

5}, Yafang Zhang⁶, Tiantian Wang^{4

7}, Shuting Xu³, Xiaoyao Wang^{1

2}, Ziwen Liu^{1

2}, Na Xing^{1

2}, Xu Liang^{1

2}, Ziting Zhu^{1

2}, Chunyang Fan^{1

2}, Ying Liu⁷, Hong Wu^{1

2}, Zhongyi Jiang^{1

2

8}

Affiliations

¹ Key Laboratory for Green Chemical Technology of Ministry of Education, School of Chemical Engineering and Technology, Tianjin University, Tianjin, 300072, China.
² Zhejiang Institute of Tianjin University, Ningbo, Zhejiang, 315201, China.
³ Beijing Key Laboratory of Ionic Liquids Clean Process, CAS Key Laboratory of Green Process and Engineering, Institute of Process Engineering, Chinese Academy of Sciences, Beijing, 100190, China.
⁴ Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, Beijing, 100190, China.
⁵ School of Physical Sciences, University of Chinese Academy of Sciences, Beijing, 100049, China.
⁶ School of Chemical Engineering, Zhengzhou University, Zhengzhou, 450001, China.
⁷ College of Chemistry, Beijing Normal University, Beijing, 100875, China.
⁸ Joint School of National University of Singapore and Tianjin University, International Campus of Tianjin University, Binhai New City, Fuzhou, 350207, China.

PMID: 39530691
DOI: 10.1002/adma.202413022

Abstract

Developing all-solid-state electrolytes, the chips for lithium-metal batteries, with superior electrochemical and mechanical properties awaits the disruptive materials. Herein, ionic covalent organic framework membranes are explored as solid-state electrolytes for single Li⁺ conduction. In the membrane, the anion groups act as Li⁺ transporter, determining Li⁺ binding capacity and releasing ability, whereas the oxygen-containing groups act as Li⁺ co-transporter, creating relay sites between adjacent Li⁺ transporters for rapid hopping. The membrane exhibits an unprecedented Li⁺ conductivity of 1.7 mS cm^-1 with a Li⁺-transference number close to unity at room temperature. Additionally, the membrane possesses high flexibility, low interfacial resistance, and excellent cycling performance at room temperature. This work paves an unprecedented path for the advancement of next-generation Li⁺ conductors in solid-state electrolytes.

Keywords: all‐solid‐state electrolyte; binding‐releasing‐hopping mechanism; covalent organic framework membrane; single Li+ conduction.

Abstract

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