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

被引:14
|
作者
Xu, Guangyue [1 ,2 ]
Zhang, Xiang [1 ]
Dong, Zhuoya [3 ]
Liang, Wanying [1 ]
Xiao, Tianci [4 ]
Chen, Huiyong [5 ]
Ma, Yanhang [3 ]
Pan, Yang [4 ]
Fu, Yao [1 ]
机构
[1] Univ Sci & Technol China, Hefei Natl Res Ctr Phys Sci Microscale, CAS Key Lab Urban Pollutant Convers, Anhui Prov Key Lab Biomass Clean Energy, Hefei 230026, Peoples R China
[2] Hefei Comprehens Natl Sci Ctr, Inst Energy, Hefei 230031, Peoples R China
[3] ShanghaiTech Univ, Sch Phys Sci & Technol, Shanghai 201210, Peoples R China
[4] Univ Sci & Technol China, Natl Synchrotron Radiat Lab, Hefei 230026, Anhui, Peoples R China
[5] Northwest Univ, Sch Chem Engn, Xian 710069, Shaanxi, Peoples R China
基金
中国国家自然科学基金; 国家重点研发计划;
关键词
Dehydrogenation; Ferric species; Propane; Single-Site Catalyst; Zeolite; ELECTRONIC POPULATION ANALYSIS; METAL-OXIDE CATALYSTS; OXIDATIVE DEHYDROGENATION; MOSSBAUER-SPECTROSCOPY; SELECTIVE CATALYSTS; ACTIVE-SITES; DESIGN; PERFORMANCE; MOLECULES; EXAFS;
D O I
10.1002/anie.202305915
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
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-1. This study provided guidance for the synthesis of structural heteroatomic zeolite and efficient propane non-oxidative dehydrogenation over early transition metals. A single-site catalyst comprised of ferric iron confined in an MFI-type zeolite framework was synthesized by a hydrothermal method involving rapid mixing at high temperature. The isolated Fe species in the framework formed distorted tetrahedra, which were beneficial for the selective dehydrogenation of propane. The catalyst had a silanol-free structure and was oxygen tolerant, hydrothermally stable, and resistant to coking.+image
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页数:7
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