Zhao Hong, Li Boyang, Zhao Huacheng, Li Jianfeng, Kou Jinfang, Zhu Hanghang, Liu Bing, Li Zhenhua, Sun Xun, Dong Zhengping
State Key Laboratory of Applied Organic Chemistry, Laboratory of Special Function Materials and Structure Design of the Ministry of Education, College of Chemistry and Chemical Engineering, Lanzhou University, Lanzhou 730000, PR China.
Key Laboratory of Catalysis and Materials Sciences of the Ministry of Education, South-Central University for Nationalities, Wuhan 430074, PR China.
J Colloid Interface Sci. 2022 Jan 15;606(Pt 2):1524-1533. doi: 10.1016/j.jcis.2021.08.081. Epub 2021 Aug 16.
Heterogeneous noble metal-based catalysts with stable, precise structures and high catalytic performance are of great research interest for sustainable catalysis. Herein, we designed the novel sandwich-like metal-organic-framework composite nanocatalyst UiO-66-NH@Pt@mSiO using UiO-66-NH@Pt as the core, and mesoporous SiO as the shell. The obtained UiO-66-NH@Pt@mSiO catalyst shows a well-defined structure and interface, and the protection of the mSiO shell can efficiently prevent Pt NPs from aggregating and leaching in the reaction process. In the one-pot cascade reaction of nitroarenes and aromatic aldehydes to secondary amines, UiO-66-NH@Pt@mSiO shows excellent catalytic performance due to acid catalytic sites provided by UiO-66-NH and Pt hydrogenation catalytic sites. Furthermore, the porous structure of the UiO-66-NH@Pt@mSiO catalyst also enhances reactant diffusion and improves the reaction efficiency. This work provides a new avenue to meticulously design well-defined nanocatalysts with superior catalytic performance and stability for challenging reactions.
具有稳定、精确结构和高催化性能的多相贵金属基催化剂对于可持续催化具有极大的研究兴趣。在此,我们设计了一种新型的三明治状金属有机框架复合纳米催化剂UiO-66-NH@Pt@mSiO,以UiO-66-NH@Pt为核心,介孔SiO为壳层。所制备的UiO-66-NH@Pt@mSiO催化剂具有明确的结构和界面,mSiO壳层的保护能够有效防止Pt纳米颗粒在反应过程中聚集和浸出。在硝基芳烃与芳香醛一锅法级联反应生成仲胺的过程中,UiO-66-NH@Pt@mSiO由于UiO-66-NH提供的酸催化位点和Pt氢化催化位点而表现出优异的催化性能。此外,UiO-66-NH@Pt@mSiO催化剂的多孔结构还增强了反应物扩散并提高了反应效率。这项工作为精心设计具有卓越催化性能和稳定性的明确纳米催化剂以应对具有挑战性的反应提供了一条新途径。