Goo Bon Seung, Ham Kyungrok, Han Yeji, Lee Seunghoon, Jung Hayoon, Kwon Yongmin, Kim Youngmin, Hong Jong Wook, Han Sang Woo
Center for Nanotectonics, Department of Chemistry and KI for the NanoCentury, KAIST, Daejeon, 34141, Korea.
Department of Chemistry, University of Ulsan, Ulsan, 44610, Korea.
Angew Chem Int Ed Engl. 2022 Jun 7;61(23):e202202923. doi: 10.1002/anie.202202923. Epub 2022 Apr 5.
The existence of various surface active sites within a nanocrystal (NC) catalyst complicates understanding their respective catalytic properties and designing an optimal catalyst structure for a desired catalytic reaction. Here, we developed a novel approach that allows unequivocal investigation on the intrinsic catalytic reactivity of the edge and terrace atoms of NCs. Through the comparison of the catalytic behaviors of edge-covered Pd NCs, which were prepared by the selective deposition of catalytically inactive Au atoms onto the edge sites of rhombic dodecahedral (RD) Pd NCs, with those of the pristine RD Pd NCs toward alkyne hydrogenation and Suzuki-Miyaura coupling reactions, we could decouple the activity of the edge and {110}-plane atoms of the Pd NCs without uncertainties. We expect that this study will provide an opportunity to scrutinize the surface properties of various NC catalysts to a more precise level and devise ideal catalysts for intended catalytic reactions.
纳米晶体（NC）催化剂中存在各种表面活性位点，这使得理解它们各自的催化特性以及为特定催化反应设计最佳催化剂结构变得复杂。在此，我们开发了一种新方法，能够明确研究NC边缘和平台原子的本征催化活性。通过比较边缘覆盖的Pd NC的催化行为（通过将催化惰性的Au原子选择性沉积到菱形十二面体（RD）Pd NC的边缘位点上制备）与原始RD Pd NC对炔烃氢化和铃木-宫浦偶联反应的催化行为，我们可以明确区分Pd NC边缘和{110}面原子的活性，不存在不确定性。我们期望这项研究将提供一个机会，以更精确的水平审视各种NC催化剂的表面性质，并为预期的催化反应设计理想的催化剂。
