Enhanced Electrochemical Hydrogenation of Benzaldehyde to Benzyl Alcohol on Pd@Ni-MOF by Modifying the Adsorption Configuration

• DOI: 10.1021/acsami.3c13920
• Publication Date: 2024-02-02T12:01:30Z
• Authors: Li Gong; Chao Yue Zhang; Junshan Li; Guillem Montaña-Mora; Marc Botifoll; Tiezhu Guo; Jordi Arbiol; Jin Yuan Zhou; Tanja Kallio; Paulina R. Martín...; Andreu Cabot
• Keywords: Benzaldehyde; Benzyl alcohol

Electrocatalytic hydrogenation (ECH) approaches under ambient temperature and pressure offer significant potential advantages over thermal processes but require highly active efficient electrocatalysts. The performance of such electrocatalysts strongly depends not only on the phase also architecture surface chemistry support material. Herein, Pd nanoparticles supported a nickel metal–organic framework (MOF), Ni-MOF-74, are prepared, their activity toward ECH benzaldehyde (BZH) in 3 M acetate (pH 5.2) aqueous electrolyte is explored. An outstanding rate up to 283 μmol cm–2 h–1 with Faradaic efficiency (FE) 76% reached. Besides, higher FEs 96% achieved using step-function voltage. Materials Studio density functional theory calculations show these performances be associated Ni-MOF that promotes H-bond formation, facilitates water desorption, induces favorable tilted BZH adsorption nanoparticles. In this configuration, bonded by carbonyl group rather than through aromatic ring, thus reducing energy barriers elemental reaction steps increasing overall efficiency.