Self-assembled hydrated copper coordination compounds as ionic conductors for room temperature solid-state batteries

Xiao Zhan, Miao Li, Xiaolin Zhao, Yaning Wang, Sha Li, Weiwei Wang, Jiande Lin, Zi-Ang Nan, Jiawei Yan, Zhefei Sun, Haodong Liu, Fei Wang, Jiayu Wan, Jianjun Liu (), Qiaobao Zhang () and Li Zhang ()
Additional contact information
Xiao Zhan: Xiamen University, Xiamen
Miao Li: Xiamen University, Xiamen
Xiaolin Zhao: Chinese Academy of Sciences
Yaning Wang: Chinese Academy of Sciences
Sha Li: Xiamen University, Xiamen
Weiwei Wang: Xiamen University, Xiamen
Jiande Lin: Xiamen University, Xiamen
Zi-Ang Nan: Xiamen University, Xiamen
Jiawei Yan: Xiamen University, Xiamen
Zhefei Sun: Xiamen University, Xiamen
Haodong Liu: UC San Diego
Fei Wang: Fudan University
Jiayu Wan: Shanghai Jiaotong University
Jianjun Liu: Chinese Academy of Sciences
Qiaobao Zhang: Xiamen University, Xiamen
Li Zhang: Xiamen University, Xiamen

Nature Communications, 2024, vol. 15, issue 1, 1-14

Abstract: Abstract As the core component of solid-state batteries, neither current inorganic solid-state electrolytes nor solid polymer electrolytes can simultaneously possess satisfactory ionic conductivity, electrode compatibility and processability. By incorporating efficient Li+ diffusion channels found in inorganic solid-state electrolytes and polar functional groups present in solid polymer electrolytes, it is conceivable to design inorganic-organic hybrid solid-state electrolytes to achieve true fusion and synergy in performance. Herein, we demonstrate that traditional metal coordination compounds can serve as exceptional Li+ ion conductors at room temperature through rational structural design. Specifically, we synthesize copper maleate hydrate nanoflakes via bottom-up self-assembly featuring highly-ordered 1D channels that are interconnected by Cu2+/Cu+ nodes and maleic acid ligands, alongside rich COO− groups and structural water within the channels. Benefiting from the combination of ion-hopping and coupling-dissociation mechanisms, Li+ ions can preferably transport through these channels rapidly. Thus, the Li+-implanted copper maleate hydrate solid-state electrolytes shows remarkable ionic conductivity (1.17 × 10−4 S cm−1 at room temperature), high Li+ transference number (0.77), and a 4.7 V-wide operating window. More impressively, Li+-implanted copper maleate hydrate solid-state electrolytes are demonstrated to have exceptional compatibility with both cathode and Li anode, enabling long-term stability of more than 800 cycles. This work brings new insight on exploring superior room-temperature ionic conductors based on metal coordination compounds.

Date: 2024
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DOI: 10.1038/s41467-024-45372-2

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