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

Abstract

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.

Authors:
 [1];  [2];  [1];  [1];  [3];  [3];  [3];  [4];  [4];  [2]; ORCiD logo [1]
  1. Tianjin Univ., Tianjin (China). Dept. of Chemistry, Inst. of Molecular Plus, Tianjin Key Lab. of Molecular Optoelectronic Science
  2. 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
  3. Brookhaven National Lab. (BNL), Upton, NY (United States). Dept. of Chemistry
  4. School of Chemical Engineering and Technology, Tianjin University, Tianjin 300072 China
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V)
OSTI Identifier:
1597261
Report Number(s):
BNL-213603-2020-JAAM
Journal ID: ISSN 1433-7851; ANIE
Grant/Contract Number:  
SC0012704; 7JCJQJC44600; 16JCYBJC40900
Resource Type:
Accepted Manuscript
Journal Name:
Angewandte Chemie (International Edition)
Additional Journal Information:
Journal Name: Angewandte Chemie (International Edition); Journal Volume: 59; Journal ID: ISSN 1433-7851
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; 2D materials; cathodes; metal-organic framework; energy storage; lithium ion batteries

Citation Formats

Jiang, Qiang, Xiong, Peixun, Liu, Jingjuan, Xie, Zhen, Wang, Qinchao, Yang, Xiao-Qing, Hu, Enyuan, Cao, Yu, Sun, Jie, Xu, Yunhua, and Chen, Long. A Redox-Active 2D Metal-Organic Framework for Efficient Lithium Storage with Extraordinary High Capacity. United States: N. p., 2020. Web. doi:10.1002/anie.201914395.
Jiang, Qiang, Xiong, Peixun, Liu, Jingjuan, Xie, Zhen, Wang, Qinchao, Yang, Xiao-Qing, Hu, Enyuan, Cao, Yu, Sun, Jie, Xu, Yunhua, & Chen, Long. A Redox-Active 2D Metal-Organic Framework for Efficient Lithium Storage with Extraordinary High Capacity. United States. doi:10.1002/anie.201914395.
Jiang, Qiang, Xiong, Peixun, Liu, Jingjuan, Xie, Zhen, Wang, Qinchao, Yang, Xiao-Qing, Hu, Enyuan, Cao, Yu, Sun, Jie, Xu, Yunhua, and Chen, Long. Wed . "A Redox-Active 2D Metal-Organic Framework for Efficient Lithium Storage with Extraordinary High Capacity". United States. doi:10.1002/anie.201914395.
@article{osti_1597261,
title = {A Redox-Active 2D Metal-Organic Framework for Efficient Lithium Storage with Extraordinary High Capacity},
author = {Jiang, Qiang and Xiong, Peixun and Liu, Jingjuan and Xie, Zhen and Wang, Qinchao and Yang, Xiao-Qing and Hu, Enyuan and Cao, Yu and Sun, Jie and Xu, Yunhua and Chen, Long},
abstractNote = {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.},
doi = {10.1002/anie.201914395},
journal = {Angewandte Chemie (International Edition)},
number = ,
volume = 59,
place = {United States},
year = {2020},
month = {1}
}

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