Статья

General Immobilization of Ultrafine Alloyed Nanoparticles within Metal–Organic Frameworks with High Loadings for Advanced Synergetic Catalysis

Fengfeng ChenState Key Laboratory of Pulp and Paper Engineering, School of Chemistry and Chemical Engineering and Analytical and Testing Centre, South China University of Technology, Guangzhou 510640, ChinaKui ShenState Key Laboratory of Pulp and Paper Engineering, School of Chemistry and Chemical Engineering and Analytical and Testing Centre, South China University of Technology, Guangzhou 510640, ChinaJunying ChenState Key Laboratory of Pulp and Paper Engineering, School of Chemistry and Chemical Engineering and Analytical and Testing Centre, South China University of Technology, Guangzhou 510640, ChinaXianfeng YangState Key Laboratory of Pulp and Paper Engineering, School of Chemistry and Chemical Engineering and Analytical and Testing Centre, South China University of Technology, Guangzhou 510640, ChinaJie CuiState Key Laboratory of Pulp and Paper Engineering, School of Chemistry and Chemical Engineering and Analytical and Testing Centre, South China University of Technology, Guangzhou 510640, ChinaYingwei LiState Key Laboratory of Pulp and Paper Engineering, School of Chemistry and Chemical Engineering and Analytical and Testing Centre, South China University of Technology, Guangzhou 510640, China

2019en

ABI

Аннотация

The development of a general synthesis approach for creating fine alloyed nanoparticles (NPs) in the pores of metal-organic frameworks (MOFs) shows great promise for advanced synergetic catalysis but has not been realized so far. Herein, for the first time we proposed a facile and general strategy to immobilize ultrafine alloyed NPs within the pores of an MOF by the galvanic replacement of transition-metal NPs (e.g., Cu, Co, and Ni) with noble-metal ions (e.g., Pd, Ru, and Pt) under high-intensity ultrasound irradiation. Nine types of bimetallic alloyed NPs of base and noble metals were successfully prepared and immobilized in the pores of MIL-101 as a model host, which showed highly dispersed and well-alloyed properties with average particle sizes ranging from 1.1 to 2.2 nm and high loadings of up to 10.4 wt %. Benefiting from the ultrafine particle size and high dispersity of Cu-Pd NPs and especially the positive synergy between Cu and Pd metals, the optimized Cu-Pd@MIL-101 exhibited an extremely high activity for the homocoupling reaction of phenylacetylene under unprecedented base- and additive-free conditions and room temperature, affording at least 19 times higher yield (98%) of 1,4-diphenylbuta-1,3-diyne than its monometallic counterparts. This general strategy for preparing various MOF-immobilized alloyed NPs potentially paves the way for the development of highly active metal catalysts for a variety of reactions.

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Идентификаторы

DOI: 10.1021/acscentsci.8b00805

Цитирования и источники

Цитирований: 2Использованных источников: 0

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