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Correlation of the spin state and catalytic property of M-N4 single-atom catalysts in oxygen reduction reactions.
Zhang, Wei; Pan, Jin-Kong; Yu, Yi-Fan; Zhang, Xian-Jie; Wang, Jia-Hao; Chen, Wen-Xian; Zhuang, Gui-Lin.
Afiliação
  • Zhang W; 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. glzhuang@zjut.edu.cn.
  • Pan JK; 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. glzhuang@zjut.edu.cn.
  • Yu YF; Wanbangde Pharmaceutical Group Co., Ltd., China.
  • Zhang XJ; 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. glzhuang@zjut.edu.cn.
  • Wang JH; 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. glzhuang@zjut.edu.cn.
  • Chen WX; 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. glzhuang@zjut.edu.cn.
  • Zhuang GL; 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. glzhuang@zjut.edu.cn.
Phys Chem Chem Phys ; 25(16): 11673-11683, 2023 Apr 26.
Article em En | MEDLINE | ID: mdl-37051874
ABSTRACT
The rational design of high-performance catalysts for oxygen reduction reactions (ORRs) is of great importance for large-scale applications in the field of proton-exchange membrane fuel cells and the green synthesis of H2O2. The effect of spin states of paramagnetic metal ions on the selectivity of ORRs is significant for single-atom catalysts (SACs). In this work, via spin-polarization density functional theory (DFT) calculations, we systematically investigated the popular paramagnetic metal-nitrogen graphene (M-N4-C, M = Mn, Fe, and Co) SACs to mainly focus on the correlation of spin states and catalytic performance (e.g. activity and selectivity). Both thermodynamically and kinetically, it was found that Co-N4-C (S = 1/2) has excellent 2e- oxygen reduction performance (hydrogen peroxide production) with an ultralow overpotential of 0.03 V, and the hydrogenation of OOH* is the rate-determining step (RDS) with an energy barrier of 1.20 eV. The 4e- ORR tends to occur along the OOH dissociation pathway (O* + OH*) on Co-N4-C (S = 3/2), in which OOH* decomposition is the RDS with an energy barrier of 1.01 eV. It is proved that the spin magnetic moment is the key factor to regulate the ORR property via multi-angle electronic analysis. The spin states of catalysts play a crucial role in the activity and selectivity of ORRs mainly by manipulating the bond strength between OOH and catalysts. This will provide new insights for the rational design of ORR catalysts with magnetic metals.

Texto completo: 1 Base de dados: MEDLINE Idioma: En Ano de publicação: 2023 Tipo de documento: Article

Texto completo: 1 Base de dados: MEDLINE Idioma: En Ano de publicação: 2023 Tipo de documento: Article