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

Cheng Han Chang; An Che Li; Ilja Popovs; Watchareeya Kaveevivitchai; Jeng Lung Chen; Kai Chun Chou; Ting Shen Kuo; Teng Hao Chen

doi:10.1039/c9ta05244e

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

Cheng Han Chang, An Che Li, Ilja Popovs, Watchareeya Kaveevivitchai, Jeng Lung Chen, Kai Chun Chou, Ting Shen Kuo, Teng Hao Chen

Nanomaterials Chemistry Group

Research output: Contribution to journal › Article › peer-review

45 Scopus citations

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.

Original language	English
Pages (from-to)	23770-23774
Number of pages	5
Journal	Journal of Materials Chemistry A
Volume	7
Issue number	41
DOIs	https://doi.org/10.1039/c9ta05244e
State	Published - 2019

Funding

We acknowledge the nancial support from the Ministry of Science and Technology of Taiwan under grant MOST107-2113-M-032-007 (to T.-H. C.) and the Young Scholar Fellowship Program MOST108-2636-E-006-001 (to W. K.). The research of I. P. was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division.

Funders	Funder number
U.S. Department of Energy
Office of Science
Basic Energy Sciences
Ministry of Science and Technology, Taiwan	MOST107-2113-M-032-007

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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.",

author = "Chang, {Cheng Han} and Li, {An Che} and Ilja Popovs and Watchareeya Kaveevivitchai and Chen, {Jeng Lung} and Chou, {Kai Chun} and Kuo, {Ting Shen} and Chen, {Teng Hao}",

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year = "2019",

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AU - Chang, Cheng Han

AU - Li, An Che

AU - Popovs, Ilja

AU - Kaveevivitchai, Watchareeya

AU - Chen, Jeng Lung

AU - Chou, Kai Chun

AU - Kuo, Ting Shen

AU - Chen, Teng Hao

PY - 2019

Y1 - 2019

N2 - 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.

AB - 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.

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JF - Journal of Materials Chemistry A

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ER -

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

Abstract

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