Amine Coordinated Electron-Rich Palladium Nanoparticles for Electrochemical Hydrogenation of Benzaldehyde

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Yang, Qin
Ge, Bingqing
Yuan, Pei
Luo, Shuting
Zhang, Hongwei
Zhao, Zhengyu
Zhang, Jiujun
Wang, Shidong
Bao, Xiaojun
Yao, Xiangdong
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2023
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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 (NH2-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 NH2-R groups, which strengthens both the adsorption of benzaldehyde and the adsorbed hydrogen (Hads) on Pd, preventing the combination of Hads to form H2, 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.

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Advanced Functional Materials
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33
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25
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Chemical sciences
Engineering
Physical sciences
Science & Technology
Physical Sciences
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Chemistry, Multidisciplinary
Chemistry, Physical
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Yang, Q; Ge, B; Yuan, P; Luo, S; Zhang, H; Zhao, Z; Zhang, J; Wang, S; Bao, X; Yao, X, Amine Coordinated Electron-Rich Palladium Nanoparticles for Electrochemical Hydrogenation of Benzaldehyde, Advanced Functional Materials, 2023, 33 (25), pp. 2214588