Amine Coordinated Electron‐Rich Palladium Nanoparticles for Electrochemical Hydrogenation of Benzaldehyde
Qin Yang, Bingqing Ge, Pei Yuan, Shuting Luo, Hongwei Zhang, Zhengyu Zhao, Jiujun Zhang, Shidong Wang, Xiaojun Bao, Xiangdong Yao
Abstract
Abstract Electrocatalytic hydrogenation (ECH) is a burgeoning strategy for the sustainable utilization of hydrogen. However, how to effectively suppress the competitive hydrogen evolution reaction (HER) is a big challenge to ECH catalysis. In this study, amine (NH 2 R)‐coordinated Pd nanoparticles loaded on carbon felt (Pd@CF) as a catalyst is successfully synthesized by a one‐step solvothermal reduction method using oleylamine as the reducing agent. An exceptional ECH reactivity on benzaldehyde is achieved on the optimal Pd@CF catalyst in terms of a high conversion (89.7%) and selectivity toward benzyl alcohol (89.8%) at −0.4 V in 60 min. Notably, the Faradaic efficiency for producing benzyl alcohol is up to 90.2%, much higher than that catalyzed by Pd@CF‐without N‐group (41.1%) and thecommercial Pd/C (20.9%). The excellent ECH performance of Pd@CF can be attributed to the enriched electrons on Pd surface resulted from the introduction of NH 2 R groups, which strengthens both the adsorption of benzaldehyde and the adsorbed hydrogen (H ads ) on Pd, preventing the combination of H ads to form H 2 , that is, inhibiting the HER. This study gives a new insight into design principles of highly efficient electrocatalysts for the hydrogenation of unsaturated aldehydes molecules.