Spatial-five coordination promotes the high efficiency of CoN4 moiety in graphene-based bilayer for oxygen reduction electrocatalysis: A density functional theory study

doi:10.1016/j.cjche.2022.03.007

Abstract

Abstract: The searching of highly efficient catalysts for oxygen reduction reaction (ORR) has attracted particular attention. In this work, we construct the graphene-based bilayers BG/X that consists by the CoN₄ embedded graphene as the upper layer and the X modified graphene as the bottom layer (X = Si, P, S). The interfacial bonding between CoN₄ site and the X dopant is spontaneously formed due to the strong pd hybridization, which changes the Co ligand from the planar-four N₄ coordination into spatial-five N₄ + X one. The additive glue atom weakens too strong adsorptions of the ORR intermediates on CoN₄ site and thereby improves the ORR activities in comparison with the monolayer counterpart. From the free energy profiles, the overpotentials η are 0.47, 0.49 and 0.45 V for BG/Si_a, BG/P_a and BG/S_a, respectively, being comparable to that of state-of-the-art Pt material. Besides, the kinetic barriers for the bilayers are less than 0.75 eV, an indicative of the room temperature activity. Furthermore, the combination of thermodynamic and kinetic analysis ensures the preference of 4e^--OOH associative mechanism over 2e^--H₂O₂ mechanism, being beneficial for membrane stability against the H₂O₂ corrosion. Therefore, the graphene-based bilayers deliver the high efficiencies for oxygen reduction electrocatalysis. Therefore, the interfacial bonding in the graphene-based bilayers provides an interesting strategy to suppress the poisoning phenomenon for the material design from atom scale.

Key words: Catalysts, Oxygen reduction reaction (ORR), Graphene, Thermodynamic, Kinetic

摘要： The searching of highly efficient catalysts for oxygen reduction reaction (ORR) has attracted particular attention. In this work, we construct the graphene-based bilayers BG/X that consists by the CoN₄ embedded graphene as the upper layer and the X modified graphene as the bottom layer (X = Si, P, S). The interfacial bonding between CoN₄ site and the X dopant is spontaneously formed due to the strong pd hybridization, which changes the Co ligand from the planar-four N₄ coordination into spatial-five N₄ + X one. The additive glue atom weakens too strong adsorptions of the ORR intermediates on CoN₄ site and thereby improves the ORR activities in comparison with the monolayer counterpart. From the free energy profiles, the overpotentials η are 0.47, 0.49 and 0.45 V for BG/Si_a, BG/P_a and BG/S_a, respectively, being comparable to that of state-of-the-art Pt material. Besides, the kinetic barriers for the bilayers are less than 0.75 eV, an indicative of the room temperature activity. Furthermore, the combination of thermodynamic and kinetic analysis ensures the preference of 4e^--OOH associative mechanism over 2e^--H₂O₂ mechanism, being beneficial for membrane stability against the H₂O₂ corrosion. Therefore, the graphene-based bilayers deliver the high efficiencies for oxygen reduction electrocatalysis. Therefore, the interfacial bonding in the graphene-based bilayers provides an interesting strategy to suppress the poisoning phenomenon for the material design from atom scale.

关键词: Catalysts, Oxygen reduction reaction (ORR), Graphene, Thermodynamic, Kinetic

Libing Yu, Qiuyan Huang, Jing Wu, Erhong Song, Beibei Xiao. Spatial-five coordination promotes the high efficiency of CoN₄ moiety in graphene-based bilayer for oxygen reduction electrocatalysis: A density functional theory study[J]. Chinese Journal of Chemical Engineering, 2023, 54(2): 106-113.

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Spatial-five coordination promotes the high efficiency of CoN₄ moiety in graphene-based bilayer for oxygen reduction electrocatalysis: A density functional theory study

Spatial-five coordination promotes the high efficiency of CoN₄ moiety in graphene-based bilayer for oxygen reduction electrocatalysis: A density functional theory study

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