Enhancing the dynamic structural evolution of NiOOH on nickel nitride surface for efficient 5-hydroxymethylfurfural oxidation

NiOOH generated in situ from pre-catalysts plays a key role in the 5-hydroxymethylfurfural electrooxidation reaction. However, the dynamic structural evolution of NiOOH remains relatively difficult and unclear. In this work, we focus on V-Ni 3 N as a case study. Density functional theory calculations, in-situ spectroscopy, and experimental results demonstrate that the V doping modulates the charge redistribution between the nickel and nitrogen in Ni 3 N and weakens the covalency of the Ni−N bonds, leading to easier formation of N vacancies and enhanced adsorption of OH* on Ni 3 N catalyst. This facilitates the transformation of the Ni−N bond into the Ni−O bond, thereby promoting the formation of active NiOOH for HMF oxidation. In addition, the doped V atoms enhance the interaction between NiOOH and HMF molecules and reduce the energy barrier of the rate-determining step. Thus, V-Ni 3 N/CC presents an excellent catalytic performance in terms of high 2,5-furandicarboxylic acid selectivity.