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限域于沸石骨架中的铁单中心丙烷脱氢催化剂

Ferric Single-Site Catalyst Confined in a Zeolite Framework for Propane Dehydrogenation.

作者信息

Xu Guangyue, Zhang Xiang, Dong Zhuoya, Liang Wanying, Xiao Tianci, Chen Huiyong, Ma Yanhang, Pan Yang, Fu Yao

机构信息

Hefei National Research Center for Physical Sciences at the Microscale, iChEM, CAS Key Laboratory of Urban Pollutant Conversion, Anhui Province Key Laboratory of Biomass Clean Energy, University of Science and Technology of China, Hefei, 230026, China.

Institute of Energy, Hefei Comprehensive National Science Center, Hefei, 230031, China.

出版信息

Angew Chem Int Ed Engl. 2023 Oct 26;62(44):e202305915. doi: 10.1002/anie.202305915. Epub 2023 Sep 21.

DOI:10.1002/anie.202305915
PMID:37696765
Abstract

Non-oxidative dehydrogenation of propane is a highly efficient approach for industrial preparation of propene that is commonly catalyzed by noble Pt or toxic Cr catalysts and suffers from coking. In this work, ferric catalyst confined in a zeolite framework was synthesized by a hydrothermal procedure. The isolated Fe in the framework formed distorted tetrahedra, which were beneficial for the selective dehydrogenation of propane and reached over 95 % propene selectivity and over 99 % total olefins selectivity. This catalyst had a silanol-free structure and was oxygen tolerant, hydrothermally stable, and coke free, with a deactivation constant of 0.01 h . This study provided guidance for the synthesis of structural heteroatomic zeolite and efficient propane non-oxidative dehydrogenation over early transition metals.

摘要

丙烷的非氧化脱氢是一种用于工业制备丙烯的高效方法,通常由贵金属Pt或有毒的Cr催化剂催化,且存在积碳问题。在本工作中,通过水热法合成了限制在沸石骨架中的铁催化剂。骨架中孤立的Fe形成扭曲的四面体,这有利于丙烷的选择性脱氢,丙烯选择性超过95%,总烯烃选择性超过99%。该催化剂具有无硅醇结构,耐氧、水热稳定且无积碳,失活常数为0.01 h⁻¹。本研究为结构杂原子沸石的合成以及早期过渡金属上高效丙烷非氧化脱氢提供了指导。

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