Molecular engineering of renewable cellulose biopolymers for solid-state battery electrolytes

Jinyang Li, Ziyang Hu, Sidong Zhang, Hongshen Zhang, Sijie Guo, Guiming Zhong, Yan Qiao (), Zhangquan Peng, Yutao Li (), Shuguang Chen, GuanHua Chen and An-Min Cao ()
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Jinyang Li: Chinese Academy of Sciences
Ziyang Hu: The University of Hong Kong
Sidong Zhang: Chinese Academy of Sciences
Hongshen Zhang: Chinese Academy of Sciences
Sijie Guo: Chinese Academy of Sciences
Guiming Zhong: Dalian Institute of Chemical Physics Chinese Academy of Sciences
Yan Qiao: University of Chinese Academy of Sciences
Zhangquan Peng: Dalian Institute of Chemical Physics Chinese Academy of Sciences
Yutao Li: University of Chinese Academy of Sciences
Shuguang Chen: The University of Hong Kong
GuanHua Chen: The University of Hong Kong
An-Min Cao: Chinese Academy of Sciences

Nature Sustainability, 2024, vol. 7, issue 11, 1481-1491

Abstract: Abstract As the most abundant and renewable biopolymer, cellulose has found applications in a range of fields such as healthcare, packaging, electronics and environmental remediation, contributing to the transition towards sustainability. Here we apply a green and scalable process transforming cellulose to a robust electrolyte exhibiting lithium (Li) ion conductivity of 1.09 × 10−3 S cm−1 with a transference number of 0.81 and mechanical strength of 12 MPa. Our process takes advantage of the rich hydroxyl groups in the cellulose which are replaced by phthalic anhydride through an esterification reaction to form cellulose phthalate (CP). Combined experimental and theoretical analyses reveal that the introduction of phthalate groups is essential to not only ensure effective multi-oxygen interaction with Li ions to create fast ion transportation channels, but also facilitates the intermolecular hydrogen bond responsible for the impressive mechanical properties. The CP biopolymer film is even compatible with most commercial cathode materials, and our solid-state Li/CP/LiFePO4 cells show better performance and notably good stability over 1,000 cycles than that of a baseline Li-ion cell with a flammable organic liquid electrolyte. Our study unlocks the enormous potential of cellulose utilization in batteries and opens an avenue for the development of abundant and sustainable solid-state electrolytes.

Date: 2024
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DOI: 10.1038/s41893-024-01414-7

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