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Original Research ARTICLE Provisionally accepted The full-text will be published soon. Notify me

Front. Mater. | doi: 10.3389/fmats.2019.00294

Detrimental effects and prevention of acidic electrolytes on oxygen reduction reaction catalytic performance of heteroatom-doped graphene catalysts

 Jun Ma1,  Lele Gong1, Yang Shen1, Defeng Sun1, Bowen Liu1, Jing Zhang2,  Dong Liu1*, Lipeng Zhang1* and  Zhenhai Xia1, 3*
  • 1College of Chemical Engineering, Beijing University of Chemical Technology, China
  • 2College of Materials Science and Engineering, Northwestern Polytechnical University, China
  • 3Department of Materials Science and Engineering, University of North Texas, United States

Heteroatom-doped carbon based catalysts have been demonstrated as one type of the most promising electrocatalysts to replace traditional noble metal catalyst, such as Pt for oxygen reduction reaction (ORR) in proton-exchange membrane fuel cells (PEMFCs). However, experimental results have shown that the carbon based catalysts exhibit inferior catalytic activities in acidic than that in alkaline mediums. As the catalytic mechanisms is unclear, there is no effective strategy to design and synthesize highly efficient carbon based catalysts working in acidic medium. In this work, the density functional theory (DFT) methods was applied to understand the inferior performance of doped graphene in acid. Our results show that the excellent performance of doped graphene is downgraded by protonation of dopants and the adsorption of acidic anions. The ORR overpotentials were calculated to be higher due to the protonation and the aggregation extent of acid anion on the graphene surface. To enhance the catalytic activities, the adverse effects of protonation and acid anion should be minimized as much as possible. These insights provide a direction to boost the catalytic efficiency and stability of metal-free carbon based catalysts for clean energy conversions and storages.

Keywords: doping graphene nanoribbons, Oxygen Reduction Reaction, catalytic activity, Acidic medium, DFT simulation

Received: 02 Aug 2019; Accepted: 01 Nov 2019.

Copyright: © 2019 Ma, Gong, Shen, Sun, Liu, Zhang, Liu, Zhang and Xia. This is an open-access article distributed under the terms of the Creative Commons Attribution License (CC BY). The use, distribution or reproduction in other forums is permitted, provided the original author(s) and the copyright owner(s) are credited and that the original publication in this journal is cited, in accordance with accepted academic practice. No use, distribution or reproduction is permitted which does not comply with these terms.

* Correspondence:
Prof. Dong Liu, Beijing University of Chemical Technology, College of Chemical Engineering, Beijing, 100029, Beijing Municipality, China, liudong@mail.buct.edu.cn
Prof. Lipeng Zhang, Beijing University of Chemical Technology, College of Chemical Engineering, Beijing, 100029, Beijing Municipality, China, zhanglp@mail.buct.edu.cn
Prof. Zhenhai Xia, Beijing University of Chemical Technology, College of Chemical Engineering, Beijing, 100029, Beijing Municipality, China, Zhenhai.Xia@unt.edu