Jin Yu, Wang Pengtang, Mao Xinnan, Liu Shangheng, Li Leigang, Wang Lu, Shao Qi, Xu Yong, Huang Xiaoqing
College of Chemistry, Chemical Engineering and Materials Science, Soochow University, 215123, Suzhou, Jiangsu, China.
State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005, China.
Angew Chem Int Ed Engl. 2021 Aug 2;60(32):17430-17434. doi: 10.1002/anie.202106459. Epub 2021 Jul 1.
Over the past decades, despite the substantial efforts that have been devoted to the modifications of Pt nanoparticles (NPs) to tailor their selectivities for hydrogenation reactions, there are still a lack of facile strategies for precisely regulation of the surface properties of NPs, especially for those with small sizes. In this work, we propose a top-down thermal annealing strategy for tuning the surface properties of Pt-based NPs (≈4 nm) without the occurrence of aggregation. Compared to conventional bottom-up methods, the present top-down strategy can precisely regulate the surface compositions of Pt-Cd NPs and other ternary Pt-Cd-M NPs (M=Fe, Ni, Co, Mn, and Sn). The optimized Pt-Cd NPs exhibit excellent selectivity toward phenylacetylene and 4-nitrostyrene hydrogenations with a styrene selectivity and 4-aminophenyl styrene selectivity of 95.2 % and 94.5 %, respectively. This work provides a general strategy for the surface reconstructions of Pt-based NPs, and promotes fundamental research on catalyst design for heterogeneous catalysis.
在过去几十年里，尽管人们为修饰铂纳米颗粒（NPs）以调整其氢化反应选择性付出了巨大努力，但仍缺乏精确调控纳米颗粒表面性质的简便策略，尤其是对于那些尺寸较小的纳米颗粒。在这项工作中，我们提出了一种自上而下的热退火策略，用于在不发生聚集的情况下调整铂基纳米颗粒（≈4 nm）的表面性质。与传统的自下而上方法相比，目前的自上而下策略可以精确调控Pt-Cd纳米颗粒以及其他三元Pt-Cd-M纳米颗粒（M = Fe、Ni、Co、Mn和Sn）的表面组成。优化后的Pt-Cd纳米颗粒对苯乙炔和4-硝基苯乙烯氢化反应表现出优异的选择性，苯乙烯选择性和4-氨基苯乙烯选择性分别为95.2%和94.5%。这项工作为铂基纳米颗粒的表面重构提供了一种通用策略，并推动了多相催化催化剂设计的基础研究。
