Activation and Spillover of Hydrogen on Sub‐1 nm Palladium Nanoclusters Confined within Sodalite Zeolite for the Semi‐Hydrogenation of Alkynes

Autor:	Rentao Mu, Chengsheng Yang, Qiang Fu, Mingrun Li, Hao Tian, Xin Chang, Jinlong Gong, Jiubing Zhao, Zhi-Jian Zhao, Shuai Wang
Rok vydání:	2019
Předmět:	Hydrogen 010405 organic chemistry chemistry.chemical_element General Chemistry General Medicine 010402 general chemistry Photochemistry 01 natural sciences Catalysis 0104 chemical sciences Nanoclusters chemistry.chemical_compound Acetylene chemistry Sodalite Hydrogen spillover Zeolite Palladium
Zdroj:	Angewandte Chemie. 131:7750-7754
ISSN:	1521-3757 0044-8249
DOI:	10.1002/ange.201903827
Popis:	The search for efficient nontoxic catalysts able to perform industrial hydrogenations is a topic of interest, with relevance to many catalytic processes. Herein, we describe a mechanistic phenomenon for the activation and spillover of hydrogen for remarkable selectivity in the semi-hydrogenation of acetylene over sub-1 nm Pd nanoclusters confined within sodalite (SOD) zeolite (Pd@SOD). Specifically, hydrogen is dissociated on the Pd nanoclusters to form hydrogen species (i.e., hydrogen atoms and hydroxyl groups) that spill over the SOD surfaces. The design and utilization of the small-pore zeolite SOD (six-membered rings with 0.28×0.28 nm channels) is crucial as it only allows H2 diffusion into the channels to reach the encapsulated Pd nanoclusters and thus avoids over-hydrogenation to form ethane. Pd@SOD exhibits an ethylene selectivity of over 94.5 %, while that of conventional Pd/SOD is approximately 21.5 %.
Databáze:	OpenAIRE
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