Pt single atom captured by oxygen vacancy-rich NiCo layered double hydroxides for coupling hydrogen evolution with selective oxidation of glycerol to formate

Abstract

By combining hydrogen evolution reaction (HER) with glycerol oxidation reaction (GOR), high-value chemicals can be obtained at the anode while saving energy to produce hydrogen. Herein, we synthesized PtSA-NiCo LDHs/NF by anchoring oxygen vacancies in NiCo LDHs with Pt to form Pt-O5 coordination. Density functional theory (DFT) revealed that PtSA reduced the d-band center and optimized ΔGH*. During HER, LDHs act as active sites to catalyze H-OH cleavage and promote the dissociation of H2O, while Pt single atoms act as the binding sites for H intermediates, and Pt-O bonds accelerate proton-electron coupling and promote the release of H2 molecules. In HER//GOR, a cell voltage of only 1.37 V is required to provide a current density of 100 mA cm−2 and to produce formate at the anode. This work enables energy-saving hydrogen production and high-value chemicals at the anode, a novel green electrocatalytic synthesis strategy with synergistic coupling and dual promotion.