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用于高效选择性加氢的亲水单原子催化剂的一般策略。

General Strategy toward Hydrophilic Single Atom Catalysts for Efficient Selective Hydrogenation.

机构信息

State Key Laboratory of Chemical Resource Engineering, Innovation Centre for Soft Matter Science and Engineering, College of Chemistry, Beijing University of Chemical Technology, Beijing, 100029, China.

CAS Key Laboratory of Nanosystem and Hierarchical Fabrication, CAS Center for Excellence in Nanoscience, National Center for Nanoscience and Technology, Beijing, 100190, China.

出版信息

Adv Sci (Weinh). 2022 Sep;9(25):e2202144. doi: 10.1002/advs.202202144. Epub 2022 Jul 7.

Abstract

Well dispersible and stable single atom catalysts (SACs) with hydrophilic features are highly desirable for selective hydrogenation reactions in hydrophilic solvents towards important chemicals and pharmaceutical intermediates. A general strategy is reported for the fabrication of hydrophilic SACs by cation-exchange approach. The cation-exchange between metal ions (M = Ni, Fe, Co, Cu) and Na ions introduced in the skeleton of metal oxide (TiO or ZrO ) nanoshells plays the key role in forming M /TiO and M /ZrO SACs, which efficiently prevents the aggregation of the exchanged metal ions. The as-obtained SACs are highly dispersible and stable in hydrophilic solvents including alcohol and water, which greatly facilitates the catalysis reaction in alcohol. The Ni /TiO SACs have been successfully utilized as catalysts for the selective C=C hydrogenation of cinnamaldehyde to produce phenylpropanal with 98% conversion, over 90% selectivity, good recyclability, and a turnover frequency (TOF) of 102 h , overwhelming most reported catalysts including noble metal catalysts.

摘要

具有亲水性的高分散性和稳定性的单原子催化剂(SACs)对于在亲水性溶剂中进行选择性氢化反应,从而合成重要化学品和药物中间体具有重要意义。本研究报道了一种通过离子交换法制备亲水性 SACs 的通用策略。金属氧化物(TiO 或 ZrO )纳米壳骨架中引入的金属离子(M=Ni、Fe、Co、Cu)与 Na 离子之间的离子交换在形成 M/TiO 和 M/ZrO SACs 中起着关键作用,这有效地阻止了交换金属离子的聚集。所获得的 SACs 在包括醇和水在内的亲水性溶剂中具有高分散性和稳定性,这极大地促进了醇中的催化反应。Ni/TiO SACs 已成功用作肉桂醛选择性 C=C 氢化反应的催化剂,以 98%的转化率、超过 90%的选择性、良好的可回收性和 102 h-1 的周转频率(TOF)生产苯丙醛,优于大多数报道的催化剂,包括贵金属催化剂。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/9e56/9443439/bd3facbec12a/ADVS-9-2202144-g002.jpg

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