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Title: Stabilization of Hexaaminobenzene in a 2D Conductive Metal–Organic Framework for High Power Sodium Storage

Abstract

Redox-active organic materials have gained growing attention as electrodes of rechargeable batteries. However, their key limitations are the low electronic conductivity and limited chemical and structural stability under redox conditions. Herein, we report a new cobalt-based ;2D conductive metal-organic framework (MOF), Co-HAB, having stable, accessible, dense active sites for high-power energy storage device through conjugative coordination between a redox-active linker, hexaaminobenzene (HAB), and a Co(II) center. Given the exceptional capability of Co-HAB for stabilizing reactive HAB, a reversible three-electron redox reaction per HAB was successfully demonstrated for the first time, thereby presenting a promising new electrode material for sodium-ion storage. Specifically, through synthetic tunability of Co-HAB, the bulk electrical conductivity of 1.57 S cm(-1) was achieved, enabling an extremely high rate capability, delivering 214 mAh g(-1) within 7 min or 152 mAh g(-1) in 45 s. Meanwhile, an almost linear increase of the areal capacity upon increasing active mass loading up to 9.6 mg cm(-2) was obtained, demonstrating 2.6 mAh cm(-2) with a trace amount of conducting agent.

Authors:
ORCiD logo; ; ;  [1]; ;  [2]; ORCiD logo [1]; ORCiD logo; ORCiD logo
  1. Berzelii Centre EXSELENT on Porous Materials, Department of Materials and Environmental Chemistry, Stockholm University, Stockholm SE-106 91, Sweden
  2. X-ray Science Division, Advanced Photon Source, Argonne National Laboratory, Argonne, Illinois 60439, United States
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1481204
DOE Contract Number:  
AC02-06CH11357
Resource Type:
Journal Article
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 140; Journal Issue: 32; Journal ID: ISSN 0002-7863
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
Electrochemistry; MOF; powder diffraction

Citation Formats

Park, Jihye, Lee, Minah, Feng, Dawei, Huang, Zhehao, Hinckley, Allison C., Yakovenko, Andrey, Zou, Xiaodong, Cui, Yi, and Bao, Zhenan. Stabilization of Hexaaminobenzene in a 2D Conductive Metal–Organic Framework for High Power Sodium Storage. United States: N. p., 2018. Web. doi:10.1021/jacs.8b06020.
Park, Jihye, Lee, Minah, Feng, Dawei, Huang, Zhehao, Hinckley, Allison C., Yakovenko, Andrey, Zou, Xiaodong, Cui, Yi, & Bao, Zhenan. Stabilization of Hexaaminobenzene in a 2D Conductive Metal–Organic Framework for High Power Sodium Storage. United States. doi:10.1021/jacs.8b06020.
Park, Jihye, Lee, Minah, Feng, Dawei, Huang, Zhehao, Hinckley, Allison C., Yakovenko, Andrey, Zou, Xiaodong, Cui, Yi, and Bao, Zhenan. Sat . "Stabilization of Hexaaminobenzene in a 2D Conductive Metal–Organic Framework for High Power Sodium Storage". United States. doi:10.1021/jacs.8b06020.
@article{osti_1481204,
title = {Stabilization of Hexaaminobenzene in a 2D Conductive Metal–Organic Framework for High Power Sodium Storage},
author = {Park, Jihye and Lee, Minah and Feng, Dawei and Huang, Zhehao and Hinckley, Allison C. and Yakovenko, Andrey and Zou, Xiaodong and Cui, Yi and Bao, Zhenan},
abstractNote = {Redox-active organic materials have gained growing attention as electrodes of rechargeable batteries. However, their key limitations are the low electronic conductivity and limited chemical and structural stability under redox conditions. Herein, we report a new cobalt-based ;2D conductive metal-organic framework (MOF), Co-HAB, having stable, accessible, dense active sites for high-power energy storage device through conjugative coordination between a redox-active linker, hexaaminobenzene (HAB), and a Co(II) center. Given the exceptional capability of Co-HAB for stabilizing reactive HAB, a reversible three-electron redox reaction per HAB was successfully demonstrated for the first time, thereby presenting a promising new electrode material for sodium-ion storage. Specifically, through synthetic tunability of Co-HAB, the bulk electrical conductivity of 1.57 S cm(-1) was achieved, enabling an extremely high rate capability, delivering 214 mAh g(-1) within 7 min or 152 mAh g(-1) in 45 s. Meanwhile, an almost linear increase of the areal capacity upon increasing active mass loading up to 9.6 mg cm(-2) was obtained, demonstrating 2.6 mAh cm(-2) with a trace amount of conducting agent.},
doi = {10.1021/jacs.8b06020},
journal = {Journal of the American Chemical Society},
issn = {0002-7863},
number = 32,
volume = 140,
place = {United States},
year = {2018},
month = {7}
}