Mechanistic Studies of Transition Metal-Terephthalate Coordination Complexes upon Electrochemical Lithiation and Delithiation
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- Mechanistic Studies of Transition Metal-Terephthalate Coordination Complexes upon Electrochemical Lithiation and Delithiation
- Lee, Hyun Ho; Park, Yuwon; Kim, Su Hwan; Yeon, Sun-Hwa; Kwak, Sang Kyu; Lee, Kyu Tae; Hong, Sung You
- Issue Date
- WILEY-V C H VERLAG GMBH
- ADVANCED FUNCTIONAL MATERIALS, v.25, no.30, pp.4859 - 4866
- Redox-active organic molecules are intriguing candidates as active electrode materials for next-generation rechargeable batteries due to their structural diversity, environmental friendliness, and solution-phase preparation processes. Recently, a transition metal-organic coordination approach is exploited to construct high capacity anodes for lithium-ion rechargeable batteries. Here, a family of transition metal-organic coordination complexes with terephthalate ligands is synthesized that exhibit reversible capacities above 1100 mA h g-1. The reaction mechanism to describe the multi-electron redox processes is investigated at the molecular-level via the synchrotron-sourced X-ray absorption spectroscopy and solid-state NMR analyses. The spectroscopic studies reveal that the electrochemical process involves oxidation state changes of the transition metals followed by additional lithium insertion/extraction in the conjugated aromatic ligands. The combined approaches assisted by synthetic organic chemistry and solid-state analysis provide mechanistic insights into excessive lithiation processes that have implications for the design of high-performance anode materials. The multi-electron redox mechanism of transition metal terephthalates upon electrochemical lithiation and delithiation is investigated via synchrotron-sourced X-ray absorption spectroscopy and solid state 13C NMR analysis. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
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