Max Planck Cardiff Centre on the Fundamentals of Heterogeneous Catalysis, FUNCAT, Cardiff Catalysis Institute, School of Chemistry, Cardiff University, Main Building, Park Place, Cardiff CF103AT, United Kingdom.
Westfälische Wilhelms-Universität Münster, Organisch-Chemisches Institut, Corrensstraße 36, 48149 Münster, Germany.
J Am Chem Soc. 2022 Aug 31;144(34):15431-15436. doi: 10.1021/jacs.2c04828. Epub 2022 Aug 17.
Heterogeneous palladium catalysts modified by N-heterocyclic carbenes (NHCs) are shown to be highly effective toward the direct synthesis of hydrogen peroxide (HO), in the absence of the promoters which are typically required to enhance both activity and selectivity. Catalytic evaluation in a batch regime demonstrated that through careful selection of the N-substituent of the NHC it is possible to greatly enhance catalytic performance when compared to the unmodified analogue and reach concentrations of HO rivaling that obtained by state-of-the-art catalysts. The enhanced performance of the modified catalyst, which is retained upon reuse, is attributed to the ability of the NHC to electronically modify Pd speciation.
负载 N-杂环卡宾(NHCs)的多相钯催化剂在没有通常用于提高活性和选择性的促进剂的情况下,被证明对直接合成过氧化氢(HO)非常有效。在间歇反应条件下的催化评价表明,通过仔细选择 NHC 的 N-取代基,可以与未修饰的类似物相比,极大地提高催化性能,并达到与最先进的催化剂相当的 HO 浓度。改性催化剂的增强性能在重复使用时得以保留,这归因于 NHC 改变 Pd 形态的能力。