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Achieving high-efficient urea oxidation via regulating the rate-determining step over a V single atom incorporated Co hydroxide electrocatalyst

Baojie Zhang,Changti Pan,Hengjie Liu,Xingshun Wu,Hongliang Jiang,Li Yang,Zeming Qi,Guang Li,Lei Shan,Yunxiang Lin,Li Song,Yong Jiang

Urea oxidation reaction (UOR) has emerged as a competitive approach for many energy-related technologies due to the low overpotential and fast reaction dynamics. The main challenge lies in fabricating high-efficient catalysts with optimized electronic structure and understanding the intrinsic structure-related mechanisms. Here, we report a feasible strategy of regulating the rate-determining step (RDS) of UOR via an electrochemical reconstructed Co hydroxide catalyst incorporated with V single atoms. The optimal catalysts exhibit an enhanced UOR performance after V incorporation while remarkably suppressed the competitive oxygen evolution with the potential of 1.54 V (vs RHE) to achieve the current density of 30 mA cm −2 . Operando synchrotron-radiation Fourier transform infrared spectroscopy (SR-FTIR) combining density functional theory (DFT) calculations reveal that enabled by single atom V incorporation, the RDS of UOR has been changed from the first deprotonation step to the second one with a lower energy barrier of 2.05 eV (vs 2.6 eV), which is thermodynamically favorable for the overall reaction process.