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Heteroatoms on Pentagon: Clarifying the Activity Origin of the Acidic Oxygen Reduction

30 Pages Posted: 10 Feb 2020 Sneak Peek Status: Review Complete

See all articles by Xuecheng Yan

Xuecheng Yan

Griffith University - Queensland Micro- and Nanotechnology Centre

Hongli Liu

Qingdao University - Collaborative Innovation Center for Marine Biomass Fibers, Materials and Textiles of Shandong Province

Yi Jia

Griffith University - Queensland Micro- and Nanotechnology Centre

Longzhou Zhang

Griffith University - Queensland Micro- and Nanotechnology Centre

Xin Wang

Griffith University - Queensland Micro- and Nanotechnology Centre

Jun Chen

University of Wollongong - Intelligent Polymer Research Institute

Dongjiang Yang

Qingdao University - Collaborative Innovation Center for Marine Biomass Fibers, Materials and Textiles of Shandong Province

Xiangdong Yao

Griffith University - Queensland Micro- and Nanotechnology Centre

More...

Abstract

Metal-free oxygen reduction reaction (ORR) catalysts have been intensively studied during the past decade. For heteroatoms modified carbon materials, the influence of heteroatoms on the ORR is still elusive. Herein, density functional theory (DFT) simulations were firstly used for better understanding the role of heteroatoms in catalyzing the ORR. As a model catalyst, graphene with pentagon (C5) defect was selected for studying the effect of heteroatoms in tuning the acidic ORR activity. Both theoretical and experimental results show that the N and S co-doped graphene without pentagons shows very poor ORR performance; however, in the presence of certain types of defects such as C5, the substitution of N and S to C atoms could greatly enhance the acidic ORR activity of the resulting sample, implying the essential role of defects for the ORR. This work clarifies that heteroatoms themselves show very limited contributions on the ORR, but they are powerful in tuning the electronic structures of defects for high ORR activity.

Keywords: Metal-free catalysis, oxygen reduction, heteroatom doping, Defect electrocatalysis, active sites

Suggested Citation

Yan, Xuecheng and Liu, Hongli and Jia, Yi and Zhang, Longzhou and Wang, Xin and Chen, Jun and Yang, Dongjiang and Yao, Xiangdong, Heteroatoms on Pentagon: Clarifying the Activity Origin of the Acidic Oxygen Reduction. Available at SSRN: https://ssrn.com/abstract=3532766 or http://dx.doi.org/10.2139/ssrn.3532766
This is a paper under consideration at Cell Press and has not been peer-reviewed.

Xuecheng Yan

Griffith University - Queensland Micro- and Nanotechnology Centre ( email )

Australia

Hongli Liu

Qingdao University - Collaborative Innovation Center for Marine Biomass Fibers, Materials and Textiles of Shandong Province

China

Yi Jia

Griffith University - Queensland Micro- and Nanotechnology Centre

Australia

Longzhou Zhang

Griffith University - Queensland Micro- and Nanotechnology Centre ( email )

Australia

Xin Wang

Griffith University - Queensland Micro- and Nanotechnology Centre

Australia

Jun Chen

University of Wollongong - Intelligent Polymer Research Institute

Australia

Dongjiang Yang

Qingdao University - Collaborative Innovation Center for Marine Biomass Fibers, Materials and Textiles of Shandong Province ( email )

China

Xiangdong Yao (Contact Author)

Griffith University - Queensland Micro- and Nanotechnology Centre ( email )

Australia

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