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Free keywords:
Alcohol oxidation reaction, C-C bond cleavage, C1 pathway selectivity, Chalcogenide, P-d orbital hybridization, Chalcogenides, Density functional theory, Electrocatalysts, Electrooxidation, Ethanol, Ethylene, Ethylene glycol, Palladium, Selenium compounds, Alcohol oxidation, Alcohol oxidation reaction, Bond cleavages, C-C bond cleavage, C-C bonds, C1 pathway selectivity, Chalcogenide, D orbitals, Orbital hybridization, Oxidation reactions, P-d orbital hybridization, Nanosheets
Abstract:
Ethanol oxidation reaction (EOR) is an important energy conversion process. Herein, we have proposed palladium chalcogenide nanosheets to improve C-C bond cleavage ability for EOR. The mass activity of the Te-Pd nanosheets (NSs)/C, which is higher than Se-Pd NSs/C and S-Pd NSs/C (6.9 A mg−1 and 5.3 A mg−1), has achieved 10.0 A mg−1, 12.5-fold higher than commercial Pd/C (0.8 A mg−1) and 8.3 times higher than Pd NSs/C (1.2 A mg−1). The Faradaic efficiency of C1 pathway for EOR on the Te-Pd NSs/C can improve to 56.6% compared with Pd NSs/C (25.7%) at 0.8 VRHE. Density functional theory calculations reveal that the orbital hybridization between Pd and Te weakens the adsorption energy of intermediates and reduces the energy barrier of the rate-determining steps in the C1 pathway. Besides, these palladium chalcogenide NSs can also serve as efficient electrocatalysts for ethylene glycol oxidation reaction and methanol oxidation reaction. © 2023 Elsevier B.V.
