Surface Reconstruction of Co4N Coupled with CeO2 toward Enhanced Alkaline Oxygen Evolution Reaction

Inorg Chem. 2022 Sep 5;61(35):14140-14147. doi: 10.1021/acs.inorgchem.2c02290. Epub 2022 Aug 19.

Abstract

Constructing the active interface in a heterojunction electrocatalyst is critical for the electron transfer and intermediate adsorption (O*, OH*, and HOO*) in alkaline oxygen evolution reaction (OER) but still remains challenging. Herein, a CeO2/Co4N heterostructure is rationally synthesized through the direct calcination of Ce[Co(CN)6], followed by thermal nitridation. The in situ electrochemically generated CoOOH on the surface of Co4N serves as the active site for the OER, and the coupled CeO2 with oxygen vacancy can optimize the energy barrier of intermediate reactions of the OER, which simultaneously boosts the OER performance. Besides, electrochemical measurement results demonstrate that oxygen vacancies in CeO2 and optimized absorption free energy originating from the electron transfer between CeO2 and CoOOH contribute to enhanced OER kinetics. This work provides new insight into regulating the interface heterostructure to rationally design efficient OER electrocatalysts under alkaline conditions.