Büchele Simon, Chen Zupeng, Fako Edvin, Krumeich Frank, Hauert Roland, Safonova Olga V, López Núria, Mitchell Sharon, Pérez-Ramírez Javier
Institute for Chemical and Bioengineering, Department of Chemistry and Applied Biosciences, ETH Zürich, Vladimir-Prelog-Weg 1, 8093, Zürich, Switzerland.
Institute of Chemical Research of Catalonia and, The Barcelona Institute of Science and Technology, Av. Països Catalans 16, 43007, Tarragona, Spain.
Angew Chem Int Ed Engl. 2020 Oct 26;59(44):19639-19644. doi: 10.1002/anie.202005842. Epub 2020 Aug 13.
Chemical modifiers enhance the efficiency of metal catalysts in numerous applications, but their introduction often involves toxic or expensive precursors and complicates the synthesis. Here, we show that a porous boron nitride carrier can directly modify supported palladium nanoparticles, originating unparalleled performance in the continuous semi-hydrogenation of alkynes. Analysis of the impact of various structural parameters reveals that using a defective high surface area boron nitride and ensuring a palladium particle size of 4-5 nm is critical for maximizing the specific rate. The combined experimental and theoretical analyses point towards boron incorporation from defects in the support to the palladium subsurface, creating the desired isolated ensembles determining the selectivity. This practical approach highlights the unexplored potential of using tailored carriers for catalyst design.
化学修饰剂在众多应用中提高了金属催化剂的效率，但它们的引入通常涉及有毒或昂贵的前驱体，并且使合成过程复杂化。在这里，我们表明多孔氮化硼载体可以直接修饰负载的钯纳米颗粒，在炔烃的连续半加氢反应中产生无与伦比的性能。对各种结构参数影响的分析表明，使用有缺陷的高比表面积氮化硼并确保钯颗粒尺寸为4 - 5纳米对于最大化比速率至关重要。实验和理论分析相结合表明，硼从载体缺陷掺入钯的次表面，形成了决定选择性的所需孤立原子团。这种实用方法突出了使用定制载体进行催化剂设计的未被探索的潜力。
