Bibliographic Details
| Title: |
Metal Doping Activation of Anion-Mediated Electron Transfer in Catalytic Reactions |
| Authors: |
Zhang, Chao Yue, Yu, Jing, Huang, Chen, Sun, Guowen, Balcells, Lluís, Li, Jiayue, Qi, Xuede, Yi, Cheng Zhu, Herrero-Martín, Javier, Simonelli, Laura, Fauth, Francois, He, Ren, Pan, Xiaobo, Li, Junshan, Arbiol, Jordi, Zhou, Jin Yuan, Cabot, Andreu |
| Source: |
Journal of the American Chemical Society; February 2025, Vol. 147 Issue: 8 p7070-7082, 13p |
| Abstract: |
Heteroatom-doping has emerged as a transformative approach to producing high-performance catalysts, yet the current trial-and-error approach to optimize these materials remains ineffective. To enable the rational design of more efficient catalysts, models grounded in a deeper understanding of catalytic mechanisms are essential. Existing models, such as d-band center theory, fall short in explaining the role of dopants, particularly when these dopants do not directly interact with reactants. In this study, we synthesize various heteroatom-doped catalysts to explore the correlation between the electronic effects of the dopants and catalyst activity. Using Co-MoS2as a model catalyst and the Li–S redox reaction within the cathode of Li–S batteries as a test system, we show the interaction between cobalt sites and adjacent lattice sulfur atoms disrupts the intrinsic structural and electronic symmetry of MoS2. This disruption enhances the transfer of spin-polarized electrons from metal centers to lattice sulfur and promotes the adsorption of reactant intermediates. Furthermore, by analyzing 20 different dopant elements, we establish a linear relationship between the electron density in the lattice sulfur and catalyst activity toward the reduction of sulfur species, a relationship that extends to other catalytic systems, such as the hydrogen evolution reaction. |
| Database: |
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