Nature Communications (Feb 2024)

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,
  • Li Zhang

DOI
https://doi.org/10.1038/s41467-024-45372-2
Journal volume & issue
Vol. 15, no. 1
pp. 1 – 14

Abstract

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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.