Aerobic oxidation desulfurization (AODS) represents a carbon-neutral way to desulfurize petroleum distillates, yet it currently suffers from low efficiency and high temperature for the activation of triplet oxygen. Here, we report a sub-nanometer-thick cobalt hydroxide nanosheet that hosts an atomic molybdenum (Mo/Co(OH)₂) catalyst for the efficient aerobic oxidation of thiophenic sulfides. The catalyst achieves a turnover frequency of two orders of magnitude over that of state-of-the-art multi-metallic oxide catalysts and activates the reaction at 60°C. Coupling detailed characterizations with theoretical calculations, we formulate a descriptor—the work function of hosting materials for this reaction, which well explains the host identity dependence of the corresponding catalytic performance. We achieve the complete AODS of real diesel at 80°C under ambient pressure with negligible decay in consecutive reuses, highlighting the appealing industrial potential of our catalyst. Our findings provide fundamental and technological insights into implementing high-efficiency catalysts for the carbon-neutral AODS process.

好氧氧化脱硫 (AODS) 是一种碳中和的石油馏分脱硫方法，但目前它的三线态氧活化效率低、温度高。在这里，我们报告了一种亚纳米厚的氢氧化钴纳米片，其中含有原子钼 (Mo/Co(OH) ₂) 用于噻吩硫化物高效好氧氧化的催化剂。该催化剂的周转频率比最先进的多金属氧化物催化剂高两个数量级，并在 60°C 下激活反应。将详细表征与理论计算相结合，我们制定了一个描述符——该反应的宿主材料的功函数，这很好地解释了相应催化性能的宿主身份依赖性。我们在环境压力下在 80°C 下实现了真正柴油的完整 AODS，在连续重复使用中衰减可忽略不计，突出了我们催化剂的吸引人的工业潜力。我们的研究结果为在碳中性 AODS 工艺中实施高效催化剂提供了基础和技术见解。