Unraveling Two Pathways for Electrocatalytic Acetonitrile Reduction

Electrocatalytic hydrogenation (ECH) of organics offers a promising route for producing value-added chemicals. However, a deeper understanding of the reaction mechanism limits the efficient design of the catalysts. Herein, the two mechanisms are essentially identified on the Ni-based catalysts for acetonitrile hydrogenation, with a deeper understanding of their characteristics in view of their different performances. On this basis, an insight into the shift of the mechanism is proposed. Meanwhile, the optimization strategy of ECH is discovered, and the construction of Tafel sites (Ni/NiO interfaces) can greatly accelerate the kinetics, in addition to increasing the reactant coverage on the catalysts by modulating the electronic structures. Understanding the underlying mechanisms helps in manipulating the design of more efficient ECH catalysts.