A Pt3 cluster anchored on a C2N monolayer as an efficient catalyst for electrochemical reduction of nitrobenzene to aniline: a computational study

Abstract

The electrochemical reduction of nitrobenzene to aniline (NBER) under ambient conditions is of great significance for sustainable industry and life. In this work, by means of density functional theory (DFT) computations, we have systematically investigated the potential of several (Pt_n, n = 1–6 and 13) nanoclusters anchored on a holey C₂N monolayer (Pt_n/C₂N) as NBER electrocatalysts. Our results revealed that Pt_n/C₂N materials exhibit high stability due to the strong interaction between the Pt-5d orbital and the N-2p orbital in C₂N. Interestingly, among these Pt_n/C₂N catalysts, Pt₃/C₂N is the most active catalyst for NBER because of its rather small limiting potential (−0.19 V), in which the hydrogenation of Ph–NO₂* to Ph–NOOH* is identified as the potential-determining step. Compared with other catalysts, the strongest binding strength of Ph–NOOH* on Pt₃/C₂N is responsible for its superior catalytic activity towards NBER. Our results provide a promising Pt cluster-based catalyst with high efficiency for NBER, which could open a new door for sustainable aniline production.