Topological defects induced by N incorporation-evaporation strategy promote the metal-support interaction over Pd/NC for catalytic formic acid dehydrogenation

Abstract

Hydrogen (H2) production from formic acid (FA) decomposition is considered to be the application pattern of clean energy with board prospects. However, in precious metal-based catalysts, the weak metal-support interaction always leads to the reduction of exposure and utilization of active centers. Herein, N incorporation-evaporation strategy was employed to generate more topological carbon defects to deposit Pd nanoparticles (Pd NPs). The results demonstrate that topological defects are able to promote the electron transfer at the Pd-carbon interface, resulting in enhanced metal-support interaction. The Pd/NC800 catalyst with numerous topological defects exhibits significant activity (turnover frequency of 1251 h−1) and stability under mild conditions because of highly dispersed Pd centers with a modulated electronic state. The mechanism of enhancing metal-support interaction through topological defects was discussed through theoretical calculations, and it was found that the optimal topological configuration is the 5–8-5 defect induced by pyrrolic N. This work casts a new light on understanding the interaction between carbon configurations and active metals.