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Citation: Wenwen Li, Ge Feng, Jia Liu, Xing Zhong, Zihao Yao, Shengwei Deng, Shibin Wang, Jianguo Wang. The Structural and Chemical Reactivity of Lattice Oxygens on β-PbO2 EOP Electrocatalysts[J]. Chinese Journal of Structural Chemistry, ;2022, 41(12): 221205. doi: 10.14102/j.cnki.0254-5861.2022-0153 shu

The Structural and Chemical Reactivity of Lattice Oxygens on β-PbO2 EOP Electrocatalysts

  • 1.

    Institute of Industrial Catalysis, State Key Laboratory Breeding Base of Green-Chemical Synthesis Technology, College of Chemical Engineering, Zhejiang University of Technology, Hangzhou 310032, P.R. China









  • Author Bio: Wenwen Li is currently a PhD candidate in the College of Chemical Engineering at Zhejiang University of Technology, China. Her research interests are the processes of electrochemical ozone production based on DFT calculations
    Ge Feng is currently a PhD candidate in the College of Chemical Engineering at Zhejiang University of Technology, China. Her research focuses on electrochemical water splitting reaction based on real electrocatalytic conditions
    Jia Liu is a PhD candidate in the School of Chemical Engineering, Zhejiang University of Technology, China. She is passionate about electrochemical ozone generation (EOP) research under neutral conditions, with a particular focus on the development of advanced electrocatalysts for EOP and the promotion of their industrial application
    Xing Zhong is a professor of College of Chemical Engineering at Zhejiang University of Technology, China. In recent years, he is mainly engaged in the research of green industrial micro-reaction engineering, and has accumulated rich experience in the development and industrialization of PEM electrolytic ozone generator
    Zihao Yao is an instructor of College of Chemical Engineering at Zhejiang University of Technology, China. His research involves the quantitative determination of C-C coupling mechanisms and detailed analyses on the activity and selectivity for Fischer-Tropsch synthesis using microkinetic modeling with coverage effects
    Shengwei Deng is an associate professor of College of Chemical Engineering at Zhejiang University of Technology, China. He is mainly engaged in polymer synthesis, multiscale simulation of structure and interface properties of supported catalysts based on multi-scale simulation method
    Shibin Wang is a lecture of College of Chemical Engineering at Zhejiang University of Technology, China. He completed his PhD in 2018 at University of Chinese Academy of Sciences and worked as the postdoc fellowship during 2018~2020 in Tsinghua University, China. He is currently engaged in the theoretical calculation of photocatalysis and electrocatalysis
    Jianguo Wang is a professor and the head of College of Chemical Engineering at Zhejiang University of Technology, China. He completed his PhD in Chemical Technology in 2004 at Tianjin University, China. Prior to that, he received his Master of Chemical Engineering from Nanjing Tech University, China. He leads a research group focusing on design, preparation and application of nano-micro catalysts based on theory and experiment. In addition to authoring 100+ publications, he collaborated with numerous companies and is committed to industrializing his research results
  • Corresponding author: Shibin Wang, wangshibin@zjut.edu.cn
  • Received Date: 13 June 2022
    Accepted Date: 23 August 2022
    Available Online: 6 September 2022

Figures(5)

  • The oxygen evolution reaction (OER) and electrochemical ozone production (EOP) attracted considerable attention due to their wide applications in electrocatalysis, but the detailed reaction mechanism of product formation as well as the voltage effect on O2/O3 formation still remains unclear. In this work, density functional theory calculations were used to systematically investigate the possible reaction mechanisms of OER and EOP on the PbO2 (110) surface, with the possible reaction network involving surface lattice oxygen atoms (LOM) proposed. The results show that the LOM-2 reaction pathway involving two surface lattice oxygen atoms (Olatt) and one oxygen atom from H2O was the most thermodynamically reactive. Different potential determining step (PDS) was obtained depending on the multiple reaction pathway, and the results show that the facile diffusion of Olatt would proceed the LOM pathway and promote the formation of surface oxygen vacancies (Ovac1/Ovac2). Furthermore, Ovac1/Ovac2 formation on the surface would trigger further reactions of H2O adsorption and splitting, which refilled the oxygen vacancy and ensured the considerable stability of the PbO2 (110) surface. Multiple H2O dissociation pathways were proposed on PbO2 (110) with oxygen vacancy sites: the acid-base interaction mechanism and the vacancy fulfilling mechanism.
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