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Lee, Hyun-Wook
Energy Storage and Electron Microscopy Laboratory
Research Interests
  • Energy storage, secondary batteries, transmission electron microscopy, real time analysis

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

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Title
Coordination Polymers for High-Capacity Li-Ion Batteries: Metal-Dependent Solid-State Reversibility
Author
Lee, Hyun HoLee, Jae BinPark, YuwonPark, Kern HoOkyay, Mahmut SaitShin, Dong-SeonKim, SunghwanPark, JongnamPark, NoejungAn, Byeong-KwanJung, Yoon SeokLee, Hyun-WookLee, Kyu TaeHong, Sung You
Keywords
conversion; high capacity; lithium-ion batteries; organic ligand; reaction mechanism
Issue Date
201807
Publisher
AMER CHEMICAL SOC
Citation
ACS APPLIED MATERIALS & INTERFACES, v.10, no.26, pp.22110 - 22118
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.
URI
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DOI
http://dx.doi.org/10.1021/acsami.8b04678
ISSN
1944-8244
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