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Title: Elucidating metal and ligand redox activities of a copper-benzoquinoid coordination polymer as the cathode for lithium-ion batteries

Abstract

A novel redox-active quinone-based organic building block 1,4-dicyano-2,3,5,6-tetrahydroxybenzene (LH4) has been synthesized and used as a bridging ligand to form a new 1D copper-benzoquinoid coordination polymer [CuL(DMF)2]n. The compound is able to deliver an initial capacity as high as 268 mA h g-1 at 30 mA g-1 (~C/2.5) when used as the cathode in Li batteries. Ex situ XPS and FT-IR reveal the involvement of both Cu and organic moieties in the multi-electron redox reaction. Cu K-edge XANES and EXAFS measurements confirm the change in the oxidation state and coordination environment of Cu during the discharge–charge process. In situ generated metallic nanoparticles have been observed by TEM. The obtained mechanistic understanding of the metal–organic electrode materials for Li-based batteries may pave the way for the design of next-generation energy-storage systems.

Authors:
 [1];  [2]; ORCiD logo [3]; ORCiD logo [2]; ORCiD logo [4];  [1];  [5]; ORCiD logo [2]
  1. Tamkang Univ., Taipei (Taiwan)
  2. National Cheng Kung Univ., Tainan City (Taiwan)
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  4. National Synchrotron Radiation Research Center, Hsinchu (Taiwan)
  5. National Taiwan Normal Univ., Taipei (Taiwan)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1777812
Alternate Identifier(s):
OSTI ID: 1557902
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Materials Chemistry. A
Additional Journal Information:
Journal Volume: 7; Journal Issue: 41; Journal ID: ISSN 2050-7488
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE

Citation Formats

Chang, Cheng-Han, Li, An-Che, Popovs, Ilja, Kaveevivitchai, Watchareeya, Chen, Jeng-Lung, Chou, Kai-Chun, Kuo, Ting-Shen, and Chen, Teng-Hao. Elucidating metal and ligand redox activities of a copper-benzoquinoid coordination polymer as the cathode for lithium-ion batteries. United States: N. p., 2019. Web. doi:10.1039/c9ta05244e.
Chang, Cheng-Han, Li, An-Che, Popovs, Ilja, Kaveevivitchai, Watchareeya, Chen, Jeng-Lung, Chou, Kai-Chun, Kuo, Ting-Shen, & Chen, Teng-Hao. Elucidating metal and ligand redox activities of a copper-benzoquinoid coordination polymer as the cathode for lithium-ion batteries. United States. https://doi.org/10.1039/c9ta05244e
Chang, Cheng-Han, Li, An-Che, Popovs, Ilja, Kaveevivitchai, Watchareeya, Chen, Jeng-Lung, Chou, Kai-Chun, Kuo, Ting-Shen, and Chen, Teng-Hao. Fri . "Elucidating metal and ligand redox activities of a copper-benzoquinoid coordination polymer as the cathode for lithium-ion batteries". United States. https://doi.org/10.1039/c9ta05244e. https://www.osti.gov/servlets/purl/1777812.
@article{osti_1777812,
title = {Elucidating metal and ligand redox activities of a copper-benzoquinoid coordination polymer as the cathode for lithium-ion batteries},
author = {Chang, Cheng-Han and Li, An-Che and Popovs, Ilja and Kaveevivitchai, Watchareeya and Chen, Jeng-Lung and Chou, Kai-Chun and Kuo, Ting-Shen and Chen, Teng-Hao},
abstractNote = {A novel redox-active quinone-based organic building block 1,4-dicyano-2,3,5,6-tetrahydroxybenzene (LH4) has been synthesized and used as a bridging ligand to form a new 1D copper-benzoquinoid coordination polymer [CuL(DMF)2]n. The compound is able to deliver an initial capacity as high as 268 mA h g-1 at 30 mA g-1 (~C/2.5) when used as the cathode in Li batteries. Ex situ XPS and FT-IR reveal the involvement of both Cu and organic moieties in the multi-electron redox reaction. Cu K-edge XANES and EXAFS measurements confirm the change in the oxidation state and coordination environment of Cu during the discharge–charge process. In situ generated metallic nanoparticles have been observed by TEM. The obtained mechanistic understanding of the metal–organic electrode materials for Li-based batteries may pave the way for the design of next-generation energy-storage systems.},
doi = {10.1039/c9ta05244e},
journal = {Journal of Materials Chemistry. A},
number = 41,
volume = 7,
place = {United States},
year = {Fri Aug 09 00:00:00 EDT 2019},
month = {Fri Aug 09 00:00:00 EDT 2019}
}

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