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.

中文翻译：

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通过部分氧化在 PbS 中进行表面工程：将乙酰丙酸还原为 γ-戊内酯的先进电催化剂†

开发温和高效的生物质转化策略具有重要意义，而先进催化剂的设计对于生物质的增值至关重要。在此，我们通过部分氧化的表面工程策略设计了基于 PbS 的电催化剂，并且 PbS 表面氧化为 PbSO ₄的程度可以通过煅烧温度轻松调节。发现所制备的电催化剂可以以水为氢源有效地催化生物质衍生的乙酰丙酸（LA）还原为γ-戊内酯（GVL）。特别是在 400 ℃煅烧的电催化剂（PbS-400）表现出优异的性能，电流密度为 13.5 mA cm ^-2并且 GVL 法拉第效率为 78.6%，远高于迄今为止报告的最佳结果。此外，GVL 是 LA 还原的唯一产物，表明其具有优异的选择性。机理研究表明，LA 是通过 LA 的羰基的电催化氢化和随后的分子内酯化作用转化的。