State Key Laboratory of Heavy Oil Processing, CNPC Key Laboratory of Catalysis, College of Chemistry and Chemical Engineering, China University of Petroleum (East China), Qingdao 266580, China.
School of Materials Science and Engineering, Institute of Advanced Materials, China University of Petroleum (East China), Qingdao 266580, China.
ACS Appl Mater Interfaces. 2023 Apr 19;15(15):19653-19664. doi: 10.1021/acsami.3c00810. Epub 2023 Apr 4.
Well-dispersed PdIn bimetallic alloy nanoparticles (1-4 nm) were immobilized on mesostructured silica by an in situ capture-alloying strategy, and PdIn-InO interfaces were rationally constructed by changing the InO loading and reduction temperature. The catalytic performance for benzyl alcohol partial oxidation was evaluated, and a catalytic synergy was observed. The Pd-rich PdIn-InO interface is prone to be formed on the catalyst with a low InO loading after being reduced at 300 °C. It was demonstrated that the Pd-rich PdIn-InO interface was more active for benzyl alcohol partial oxidation than In-rich PdIn species, which was likely to be formed at a high reduction temperature (400 °C). The high catalytic activity on the Pd-rich PdIn-InO interface was attributed to the exposure of more Pd-enriched active sites, and an optimized PdIn-InO/Pd assemble ratio enhanced the oxygen transfer during partial oxidation. The density functional theory (DFT) calculation confirmed that the Pd-rich PdIn(111)-InO interface facilitated the activation of oxygen molecules, resulting in high catalytic activity.
高度分散的 PdIn 双金属合金纳米粒子（1-4nm）通过原位捕捉合金化策略固定在介孔二氧化硅上，并通过改变 InO 负载量和还原温度合理构建了 PdIn-InO 界面。评价了其对苯甲醇部分氧化的催化性能，观察到了催化协同作用。在还原温度为 300°C 时，低 InO 负载量的催化剂上容易形成富 Pd 的 PdIn-InO 界面。结果表明，富 Pd 的 PdIn-InO 界面对苯甲醇部分氧化的活性高于在较高还原温度（400°C）下形成的富 In 的 PdIn 物种。在富 Pd 的 PdIn-InO 界面上具有高催化活性归因于暴露了更多富含 Pd 的活性位，并且优化的 PdIn-InO/Pd 组装比增强了部分氧化过程中的氧转移。密度泛函理论（DFT）计算证实，富 Pd 的 PdIn(111)-InO 界面有利于氧分子的活化，从而表现出高催化活性。
