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

Citation data:

ACS applied materials & interfaces, ISSN: 1944-8252, Vol: 10, Issue: 26, Page: 22110-22118

Publication Year:
2018
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Readers 8
Citations 1
Citation Indexes 1
Repository URL:
http://scholarworks.unist.ac.kr/handle/201301/24422
PMID:
29901390
DOI:
10.1021/acsami.8b04678
Author(s):
Lee, Hyun Ho; Lee, Jae Bin; Park, Yuwon; Park, Kern Ho; Okyay, Mahmut Sait; Shin, Dong-Seon; Kim, Sunghwan; Park, Jongnam; Park, Noejung; An, Byeong-Kwan; Jung, Yoon Seok; Lee, Hyun-Wook; Lee, Kyu Tae; Hong, Sung You Show More Hide
Publisher(s):
American Chemical Society (ACS); AMER CHEMICAL SOC
Tags:
Materials Science; conversion; high capacity; lithium-ion batteries; organic ligand; reaction mechanism
article description
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 C 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 after 100 cycles.