Surface engineering in PbS via partial oxidation: towards an advanced electrocatalyst for reduction of levulinic acid to γ-valerolactone

Abstract

Development of mild and efficient strategies for biomass conversion is of great significance, and design of advanced catalysts is crucial for biomass valorization. Herein, we designed PbS-based electrocatalysts through a surface engineering strategy via partial oxidation, and the degree of surface oxidation of PbS to PbSO₄ could be easily tuned by calcination temperature. It was discovered that the prepared electrocatalysts could efficiently catalyze reduction of biomass-derived levulinic acid (LA) to γ-valerolactone (GVL) using water as the hydrogen source. Especially, the electrocatalyst calcined at 400 °C (PbS-400) showed outstanding performance with a current density of 13.5 mA cm⁻² and a GVL faradaic efficiency of 78.6%, which was far higher than the best results reported up to date. Moreover, GVL was the only product from LA reduction, indicating the excellent selectivity. Mechanism investigation showed that LA was converted through electrocatalytic hydrogenation of carbonyl groups of LA and subsequent intramolecular esterification.