Palladium chalcogenide nanosheets with p-d orbital hybridization for enhanced alcohol electro-oxidation performance

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.