Clarifying the Origin of Oxygen Reduction Activity in Heteroatom-Modified Defective Carbon

Xuecheng Yan; Hongli Liu; Yi Jia; Longzhou Zhang; Wenjia Xu; Xin Wang; Jun Chen; Dongjiang Yang; Xiangdong Yao

Cell Reports Physical Science (Jul 2020)

Clarifying the Origin of Oxygen Reduction Activity in Heteroatom-Modified Defective Carbon

Xuecheng Yan,
Hongli Liu,
Yi Jia,
Longzhou Zhang,
Wenjia Xu,
Xin Wang,
Jun Chen,
Dongjiang Yang,
Xiangdong Yao

Affiliations

Xuecheng Yan: Queensland Micro- and Nanotechnology Centre, Griffith University, Nathan Campus, Nathan, QLD 4111, Australia
Hongli Liu: Collaborative Innovation Center for Marine Biomass Fibers, Materials, and Textiles of Shandong Province, Qingdao University, Qingdao 266071, P.R. China
Yi Jia: Queensland Micro- and Nanotechnology Centre, Griffith University, Nathan Campus, Nathan, QLD 4111, Australia
Longzhou Zhang: Queensland Micro- and Nanotechnology Centre, Griffith University, Nathan Campus, Nathan, QLD 4111, Australia; School of Materials Science and Engineering, Yunnan Key Laboratory for Micro/Nano Materials & Technology, Yunnan University, Kunming 650091, P.R. China
Wenjia Xu: Collaborative Innovation Center for Marine Biomass Fibers, Materials, and Textiles of Shandong Province, Qingdao University, Qingdao 266071, P.R. China
Xin Wang: Queensland Micro- and Nanotechnology Centre, Griffith University, Nathan Campus, Nathan, QLD 4111, Australia
Jun Chen: Intelligent Polymer Research Institute, ARC Centre of Excellence for Electromaterials Science, AIIM Facility, University of Wollongong, Innovation Campus, Wollongong, NSW 2522, Australia
Dongjiang Yang: Collaborative Innovation Center for Marine Biomass Fibers, Materials, and Textiles of Shandong Province, Qingdao University, Qingdao 266071, P.R. China
Xiangdong Yao: Queensland Micro- and Nanotechnology Centre, Griffith University, Nathan Campus, Nathan, QLD 4111, Australia; Corresponding author

Journal volume & issue: Vol. 1, no. 7
p. 100083

Abstract

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Summary: Metal-free oxygen reduction reaction (ORR) catalysts have been intensively studied during the past decade. For heteroatom-modified carbon materials, the influence of heteroatoms on the ORR remains unclear. Here, we use computational simulations to probe the role of heteroatoms in catalyzing the ORR; graphene with the pentagonal carbon (C5) defect is selected as a model catalyst in this study. Both theoretical and experimental results demonstrate that N and S co-doped graphenes without pentagons shows very poor ORR performance; however, in the presence of certain types of defects such as C5, the substitution of carbon atoms with N and S enhances the acidic ORR activity of the sample, implying the essential role of defects for the ORR. This work clarifies that heteroatoms themselves show limited contributions to the ORR, but they are powerful in tuning the electronic structures of defects for high ORR activity.

Published in Cell Reports Physical Science

ISSN: 2666-3864 (Online)
Publisher: Elsevier
Country of publisher: United States
LCC subjects: Science: Physics
Website: https://www.cell.com/cell-reports-physical-science

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