Surface Charge and Electrostatic Spin Crossover Effects in CoN 4 Electrocatalysts

Duan, Zhiyao; Henkelman, Graeme

doi:10.1021/acscatal.0c02458

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Surface Charge and Electrostatic Spin Crossover Effects in CoN 4 Electrocatalysts

Duan, Zhiyao·Henkelman, Graeme

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Abstract

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 CoN 4 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. Here, this effect originates from a different potential of zero charge and capacitance of each spin state.

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY Co- and N-doped carbon binding energy constant-potential condition density functional theory electrical properties oxygen evolution reaction oxygen reduction reaction pH-dependent activity quantum mechanics radiology redox reactions spin crossover effect

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Duan, Zhiyao, Henkelman, Graeme. 2020-09-25. Surface Charge and Electrostatic Spin Crossover Effects in CoN 4 Electrocatalysts. https://doi.org/10.1021/acscatal.0c02458

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