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

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 Delta GH*. 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.

Automated summary

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. PtSA-NiCo LDHs/NF were synthesized by anchoring oxygen vacancies in NiCo LDHs with Pt to form Pt-O5 coordination. The study showed that LDHs act as active sites for catalyzing H-OH cleavage and promoting H2O dissociation during HER, while Pt single atoms serve as binding sites for H intermediates and accelerate proton-electron coupling to promote H2 release. In HER//GOR, a current density of 100 mA cm-2 and formate production at the anode can be achieved with a cell voltage of only 1.37 V. The work presents a novel green electrocatalytic synthesis strategy with synergistic coupling and dual promotion, enabling energy-saving hydrogen production and high-value chemicals at the anode.