Anion doping promotes electrocatalyst reconfiguration for efficient C–C bond cleavage of 4-methylcyclohexanol†

Abstract

Electrochemical cleavage of the C–C bond is primarily employed to transform organic molecules derived from biomass into valuable short-chain chemicals. However, achieving high reaction activation for the cleavage of C–C bonds under mild conditions continues to present a significant challenge. We prepared NiX/GF (X represents doped anionic elements, S, Se, P) and obtained NiX-R/GF through reconfiguration by electrochemical activation using cyclic voltammetry. Among the prepared materials, Ni₂P-R/GF exhibited favorable electrochemical activity and achieved a high yield (88.1%) of 3-methyladipic acid through the oxidation of 4-methylcyclohexanol. Comprehensive ex/in situ electrochemical experiments demonstrate that incorporating P results in a reduced reconfiguration potential and a heterogeneous interface between NiOOH and Ni₂P. Density functional theory (DFT) calculations demonstrate that the enhanced performance exhibited by the reconfigured electrocatalyst is attributed to its unique geometric and electronic structural characteristics. The strategy of anion doping to enhance the electrochemical oxidation performance of anodes presents a sustainable approach for breaking C–C bonds.