A Redox-Active 2D Metal-Organic Framework for Efficient Lithium Storage with Extraordinary High Capacity

Jiang, Qiang; Xiong, Peixun; Liu, Jingjuan; Xie, Zhen; Wang, Qinchao; Yang, Xiao-Qing; Hu, Enyuan; Cao, Yu; Sun, Jie; Xu, Yunhua; Chen, Long

doi:10.1002/anie.201914395

A Redox-Active 2D Metal-Organic Framework for Efficient Lithium Storage with Extraordinary High Capacity

Journal Article · Wed Jan 01 00:00:00 EST 2020 · Angewandte Chemie (International Edition)

DOI:https://doi.org/10.1002/anie.201914395· OSTI ID:1597261

Jiang, Qiang ^[1]; Xiong, Peixun ^[2]; Liu, Jingjuan ^[1]; Xie, Zhen ^[1]; Wang, Qinchao ^[3]; Yang, Xiao-Qing ^[3]; Hu, Enyuan ^[3]; Cao, Yu ^[4]; Sun, Jie ^[4]; Xu, Yunhua ^[2]; ^[1]

Tianjin Univ., Tianjin (China). Dept. of Chemistry, Inst. of Molecular Plus, Tianjin Key Lab. of Molecular Optoelectronic Science
Tianjin Univ., Tianjin (China). School of Materials Science and Engineering, Key Lab. of Advanced Ceramics and Machining Technology Tianjin Key Lab. of Composite and Functional Materials
Brookhaven National Lab. (BNL), Upton, NY (United States). Dept. of Chemistry
School of Chemical Engineering and Technology, Tianjin University, Tianjin 300072 China

Metal–organic framework cathodes usually exhibit low capacity and poor electrochemical performance for Li-ion storage owing to intrinsic low conductivity and inferior redox activity. Now a redox-active 2D copper–benzoquinoid (Cu-THQ) MOF has been synthesized by a simple solvothermal method. The abundant porosity and intrinsic redox character endow the 2D Cu-THQ MOF with promising electrochemical activity. Superior performance is achieved as a Li-ion battery cathode with a high reversible capacity (387 mA h g^-1), large specific energy density (775 Wh kg^-1), and good cycling stability. The reaction mechanism is unveiled by comprehensive spectroscopic techniques: a three-electron redox reaction per coordination unit and one-electron redox reaction per copper ion mechanism is demonstrated. This elucidatory understanding sheds new light on future rational design of high-performance MOF-based cathode materials for efficient energy storage and conversion.

View Accepted Manuscript (DOE)

Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V)

Grant/Contract Number:: SC0012704

OSTI ID:: 1597261

Alternate ID(s):: OSTI ID: 1689989

Report Number(s):: BNL--213603-2020-JAAM

Journal Information:: Angewandte Chemie (International Edition), Journal Name: Angewandte Chemie (International Edition) Vol. 59; ISSN 1433-7851

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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2D materials
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A Redox-Active 2D Metal-Organic Framework for Efficient Lithium Storage with Extraordinary High Capacity

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