Duan Linlin, Hung Chin-Te, Wang Jinxiu, Wang Changyao, Ma Bing, Zhang Wei, Ma Yuzhu, Zhao Zaiwang, Yang Chaochao, Zhao Tiancong, Peng Liang, Liu Di, Zhao Dongyuan, Li Wei
Laboratory of Advanced Materials, Department of Chemistry, Shanghai Key Lab of Molecular Catalysis and Innovative Materials, State Key Laboratory of Molecular Engineering of Polymers, iChEM, College of Chemistry and Materials Science, Fudan University, Shanghai, 200433, P. R. China.
Angew Chem Int Ed Engl. 2022 Oct 24;61(43):e202211307. doi: 10.1002/anie.202211307. Epub 2022 Sep 14.
A sulfhydryl monomicelles interfacial assembly strategy is presented for the synthesis of fully exposed single-atom-layer Pt clusters on 2D mesoporous TiO (SAL-Pt@mTiO ) nanosheets. This synthesis features the introduction of the sulfhydryl group in monomicelles to finely realize the controllable co-assembly process of Pt precursors within ordered mesostructures. The resultant SAL-Pt@mTiO shows uniform SAL Pt clusters (≈1.2 nm) anchored in ultrathin 2D nanosheets (≈7 nm) with a high surface area (139 m g ), a large pore size (≈25 nm) and a high dispersion (≈99 %). Moreover, this strategy is universal for the synthesis of other SAL metal clusters (Pd and Au) on 2D mTiO with high exposure and accessibility. When used as a catalyst for hydrogenation of 4-nitrostyrene, the SAL-Pt@mTiO shows a high catalytic activity (TOF up to 2424 h ), 100 % selectivity for 4-aminostyrene, good stability, and anti-resistance to thiourea poisoning under relatively mild conditions (25 °C, 10 bar).
提出了一种巯基单分子胶束界面组装策略，用于在二维介孔TiO（SAL-Pt@mTiO）纳米片上合成完全暴露的单原子层Pt簇。这种合成方法的特点是在单分子胶束中引入巯基，以精细地实现Pt前驱体在有序介观结构中的可控共组装过程。所得的SAL-Pt@mTiO显示出均匀的SAL Pt簇（≈1.2 nm）锚定在超薄二维纳米片（≈7 nm）中，具有高表面积（139 m² g）、大孔径（≈25 nm）和高分散性（≈99 %）。此外，该策略对于在二维mTiO上合成其他具有高暴露度和可及性的SAL金属簇（Pd和Au）具有通用性。当用作4-硝基苯乙烯加氢的催化剂时，SAL-Pt@mTiO在相对温和的条件（25 °C，10 bar）下显示出高催化活性（TOF高达2424 h⁻¹）、对4-氨基苯乙烯的100 %选择性、良好的稳定性以及抗硫脲中毒性能。
