Surface Charge and Electrostatic Spin Crossover Effects in CoN4 Electrocatalysts
Surface Charge and Electrostatic Spin Crossover Effects in CoN4 Electrocatalysts
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DOI：
10.1021/acscatal.0c02458
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发表时间：
2020-10-16
期刊：
影响因子：
12.9
通讯作者：
Henkelman, Graeme
中科院分区：
文献类型：
--
作者：
Duan, Zhiyao;Henkelman, Graeme
Carbon materials doped with nitrogen and 3d transition metals have attracted a great deal of interest for catalyzing electrochemical reactions such as water splitting, oxygen reduction, and carbon dioxide reduction. Here, we employed density functional theory to study Co-N-doped carbon as electrocatalysts for the oxygen reduction and oxygen evolution reactions. Specifically, we investigated the interplay among adsorption energies, the spin state of the CoN4 active center, and the applied potential. We found that adsorption energies strongly depend on both the applied potential and the spin state of the Co center. Furthermore, spin state transitions induced by the applied potential also play an important role in determining the adsorption energies. This effect originates from a different potential of zero charge and capacitance of each spin state.
