Building highly active hybrid double–atom sites in C2N for enhanced electrocatalytic hydrogen peroxide synthesis

Yongyong Cao; JinYan Zhao; Xing Zhong; Guilin Zhuang; Shengwei Deng; Zhongzhe Wei; Zihao Yao; Jianguo Wang

Green Energy & Environment (Dec 2021)

Building highly active hybrid double–atom sites in C2N for enhanced electrocatalytic hydrogen peroxide synthesis

Yongyong Cao,
JinYan Zhao,
Xing Zhong,
Guilin Zhuang,
Shengwei Deng,
Zhongzhe Wei,
Zihao Yao,
Jianguo Wang

Affiliations

Yongyong Cao: College of Biological Chemical Science and Engineering, Jiaxing University, Jiaxing, 314001, China; Institute of Industrial Catalysis, College of Chemical Engineering, State Key Laboratory Breeding Base of Green–Chemical Synthesis Technology, Zhejiang University of Technology, Hangzhou, 310032, China
JinYan Zhao: Institute of Industrial Catalysis, College of Chemical Engineering, State Key Laboratory Breeding Base of Green–Chemical Synthesis Technology, Zhejiang University of Technology, Hangzhou, 310032, China
Xing Zhong: Institute of Industrial Catalysis, College of Chemical Engineering, State Key Laboratory Breeding Base of Green–Chemical Synthesis Technology, Zhejiang University of Technology, Hangzhou, 310032, China
Guilin Zhuang: Institute of Industrial Catalysis, College of Chemical Engineering, State Key Laboratory Breeding Base of Green–Chemical Synthesis Technology, Zhejiang University of Technology, Hangzhou, 310032, China
Shengwei Deng: Institute of Industrial Catalysis, College of Chemical Engineering, State Key Laboratory Breeding Base of Green–Chemical Synthesis Technology, Zhejiang University of Technology, Hangzhou, 310032, China
Zhongzhe Wei: Institute of Industrial Catalysis, College of Chemical Engineering, State Key Laboratory Breeding Base of Green–Chemical Synthesis Technology, Zhejiang University of Technology, Hangzhou, 310032, China
Zihao Yao: Institute of Industrial Catalysis, College of Chemical Engineering, State Key Laboratory Breeding Base of Green–Chemical Synthesis Technology, Zhejiang University of Technology, Hangzhou, 310032, China
Jianguo Wang: Institute of Industrial Catalysis, College of Chemical Engineering, State Key Laboratory Breeding Base of Green–Chemical Synthesis Technology, Zhejiang University of Technology, Hangzhou, 310032, China; Corresponding author.

Journal volume & issue: Vol. 6, no. 6
pp. 846 – 857

Abstract

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Two–electron (2e-) oxygen reduction reaction (ORR) shows great promise for on–site electrochemical synthesis of hydrogen peroxide (H2O2). However, it is still a great challenge to design efficient electrocatalysts for H2O2 synthesis. To address this issue, the logical design of the active site by controlling the geometric and electronic structures is urgently desired. Therefore, using density functional theory (DFT) computations, two kinds of hybrid double–atom supported on C2N nanosheet (RuCu@C2N and PdCu@C2N) are screened out and their H2O2 performances are predicted. PdCu@C2N exhibits higher activity for H2O2 synthesis with a lower overpotential of 0.12 V than RuCu@C2N (0.59 V), Ru3Cu(110) facet (0.60 V), and PdCu(110) facet (0.54 V). In aqueous phase, the adsorbed O2 is further stabilized with bulk H2O and the thermodynamic rate–determining step of 2e- ORR change. The activation barrier on PdCu@C2N is 0.43 eV lower than the one on RuCu@C2N with 0.68 eV. PdCu@C2N is near the top of 2e- ORR volcano plot, and exhibits high selectivity of H2O2. This work provides guidelines for designing highly effective hybrid double–atom electrocatalysts (HDACs) for H2O2 synthesis.

Published in Green Energy & Environment

ISSN: 2468-0257 (Online)
Publisher: KeAi Communications Co., Ltd.
Country of publisher: China
LCC subjects: Technology: Mechanical engineering and machinery: Renewable energy sources; Science: Biology (General): Ecology
Website: https://www.keaipublishing.com/en/journals/green-energy-and-environment/

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