Coordination Polymers for High-Capacity Li-Ion Batteries: Metal-Dependent Solid-State Reversibility

Hyun Ho Lee, Jae Bin Lee, Yuwon Park, Kern Ho Park, Mahmut Sait Okyay, Dong Seon Shin, Sunghwan Kim, Jongnam Park, Noejung Park, Byeong Kwan An, Yoon Seok Jung, Hyun Wook Lee, Kyu Tae Lee, Sung You Hong

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13 Citations (Scopus)

Abstract

Electrode materials exploiting multielectron-transfer processes are essential components for large-scale energy storage systems. Organic-based electrode materials undergoing distinct molecular redox transformations can intrinsically circumvent the structural instability issue of conventional inorganic-based host materials associated with lattice volume expansion and pulverization. Yet, the fundamental mechanistic understanding of metal-organic coordination polymers toward the reversible electrochemical processes is still lacking. Herein, we demonstrate that metal-dependent spatial proximity and binding affinity play a critical role in the reversible redox processes, as verified by combined 13C solid-state NMR, X-ray absorption spectroscopy, and transmission electron microscopy. During the electrochemical lithiation, in situ generated metallic nanoparticles dispersed in the organic matrix generate electrically conductive paths, synergistically aiding subsequent multielectron transfer to π-conjugated ligands. Comprehensive screening on 3d-metal-organic coordination polymers leads to a high-capacity electrode material, cobalt-2,5-thiophenedicarboxylate, which delivers a stable specific capacity of ∼1100 mA h g-1 after 100 cycles.

Original languageEnglish
Pages (from-to)22110-22118
Number of pages9
JournalACS Applied Materials and Interfaces
Volume10
Issue number26
DOIs
Publication statusPublished - 2018 Jul 5

All Science Journal Classification (ASJC) codes

  • Materials Science(all)

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    Lee, H. H., Lee, J. B., Park, Y., Park, K. H., Okyay, M. S., Shin, D. S., Kim, S., Park, J., Park, N., An, B. K., Jung, Y. S., Lee, H. W., Lee, K. T., & Hong, S. Y. (2018). Coordination Polymers for High-Capacity Li-Ion Batteries: Metal-Dependent Solid-State Reversibility. ACS Applied Materials and Interfaces, 10(26), 22110-22118. https://doi.org/10.1021/acsami.8b04678