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Title: Stone-Wales defect-rich carbon-supported dual-metal single atom sites for Zn-air batteries

Abstract

In this study, we aim to obtain a fundamental understanding of active sites near stone-wales (SW) defects rich nitrogen-doped graphene (DG) with specific coordination of carbon atom rings. It reveals that the SW rich defects (e.g., pentagon (5), pentagon—octagon—pentagon (i.e. 585), or pentagon-heptagon-heptagon-pentagon (5775) rings, appears correspondingly with carbon rings that brought active sites during catalytic reactions. Moreover, we anchored dual isolated metallic atoms (Ni/Fe) on DG support via linkers (O/N) called NiFe-DG. X-ray absorption spectroscopy indicates Ni/Fe metal single atoms are embedded via Fe-N4 and Ni-N4 coordination on DG surfaces. It exhibits high catalytic activity for oxygen reduction reaction (ORR) with an onset potential of 0.97 V, a half-wave potential of 0.86 V, and diffusion current density of 5.7 mA cm– 2, which is at par with commercial Pt/C. The catalyst shows superior stability, retained 82% of the initial current density even after 12 h under an applied potential of 0.86 V. Similarly, the oxygen evolution reaction (OER) overpotential of 358 mV was achieved at 10 mA cm– 2 with a lower Tafel slope value (76 mV/dec) than commercial Pt/C. It maintains 85% stability for 12 h at a constant potential of 1.588 V, shows better stability than commercialmore » Pt/C.« less

Authors:
 [1];  [2];  [3];  [4];  [5];  [5];  [6];  [6];  [7];  [3];  [5];  [3];  [8];  [2];  [1]
  1. Hong Kong University of Science and Technology (HKUST) (Hong Kong)
  2. Univ. of California, Irvine, CA (United States)
  3. Tsinghua Univ., Beijing (China)
  4. Washington Univ., St. Louis, MO (United States); Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
  5. Griffith University, Gold Coast, QLD (Australia)
  6. Argonne National Lab. (ANL), Argonne, IL (United States)
  7. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
  8. Argonne National Lab. (ANL), Argonne, IL (United States); Stanford Univ., CA (United States)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE); USDOE Office of Science (SC); Zhongshan City Bureau of Science and Technology; Guangdong-Hong Kong-Macao Intelligent Micro-Nano Optoelectronic Technology Joint Laboratory
OSTI Identifier:
1878233
Grant/Contract Number:  
AC02-06CH11357; 2019AG018; 2020B1212030010
Resource Type:
Accepted Manuscript
Journal Name:
Nano Energy
Additional Journal Information:
Journal Volume: 90; Journal ID: ISSN 2211-2855
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; stone-wales defects; nanocarbons; dual metal single atom sites; electrocatalyst

Citation Formats

Khan, Kishwar, Yan, Xingxu, Yu, Qiangmin, Bae, Sang-Hoon, White, Jessica Jein, Liu, Junxian, Liu, Tangchao, Sun, Chengjun, Kim, Jeehwan, Cheng, Hui-Ming, Wang, Yun, Liu, Bilu, Amine, Khalil, Pan, Xiaoqing, and Luo, Zhengtang. Stone-Wales defect-rich carbon-supported dual-metal single atom sites for Zn-air batteries. United States: N. p., 2021. Web. doi:10.1016/j.nanoen.2021.106488.
Khan, Kishwar, Yan, Xingxu, Yu, Qiangmin, Bae, Sang-Hoon, White, Jessica Jein, Liu, Junxian, Liu, Tangchao, Sun, Chengjun, Kim, Jeehwan, Cheng, Hui-Ming, Wang, Yun, Liu, Bilu, Amine, Khalil, Pan, Xiaoqing, & Luo, Zhengtang. Stone-Wales defect-rich carbon-supported dual-metal single atom sites for Zn-air batteries. United States. https://doi.org/10.1016/j.nanoen.2021.106488
Khan, Kishwar, Yan, Xingxu, Yu, Qiangmin, Bae, Sang-Hoon, White, Jessica Jein, Liu, Junxian, Liu, Tangchao, Sun, Chengjun, Kim, Jeehwan, Cheng, Hui-Ming, Wang, Yun, Liu, Bilu, Amine, Khalil, Pan, Xiaoqing, and Luo, Zhengtang. Mon . "Stone-Wales defect-rich carbon-supported dual-metal single atom sites for Zn-air batteries". United States. https://doi.org/10.1016/j.nanoen.2021.106488. https://www.osti.gov/servlets/purl/1878233.
@article{osti_1878233,
title = {Stone-Wales defect-rich carbon-supported dual-metal single atom sites for Zn-air batteries},
author = {Khan, Kishwar and Yan, Xingxu and Yu, Qiangmin and Bae, Sang-Hoon and White, Jessica Jein and Liu, Junxian and Liu, Tangchao and Sun, Chengjun and Kim, Jeehwan and Cheng, Hui-Ming and Wang, Yun and Liu, Bilu and Amine, Khalil and Pan, Xiaoqing and Luo, Zhengtang},
abstractNote = {In this study, we aim to obtain a fundamental understanding of active sites near stone-wales (SW) defects rich nitrogen-doped graphene (DG) with specific coordination of carbon atom rings. It reveals that the SW rich defects (e.g., pentagon (5), pentagon—octagon—pentagon (i.e. 585), or pentagon-heptagon-heptagon-pentagon (5775) rings, appears correspondingly with carbon rings that brought active sites during catalytic reactions. Moreover, we anchored dual isolated metallic atoms (Ni/Fe) on DG support via linkers (O/N) called NiFe-DG. X-ray absorption spectroscopy indicates Ni/Fe metal single atoms are embedded via Fe-N4 and Ni-N4 coordination on DG surfaces. It exhibits high catalytic activity for oxygen reduction reaction (ORR) with an onset potential of 0.97 V, a half-wave potential of 0.86 V, and diffusion current density of 5.7 mA cm– 2, which is at par with commercial Pt/C. The catalyst shows superior stability, retained 82% of the initial current density even after 12 h under an applied potential of 0.86 V. Similarly, the oxygen evolution reaction (OER) overpotential of 358 mV was achieved at 10 mA cm– 2 with a lower Tafel slope value (76 mV/dec) than commercial Pt/C. It maintains 85% stability for 12 h at a constant potential of 1.588 V, shows better stability than commercial Pt/C.},
doi = {10.1016/j.nanoen.2021.106488},
journal = {Nano Energy},
number = ,
volume = 90,
place = {United States},
year = {Mon Sep 20 00:00:00 EDT 2021},
month = {Mon Sep 20 00:00:00 EDT 2021}
}

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