Oxidative dehydrogenation and dry reforming of n-butane with CO2 over NiFe bimetallic catalysts

被引：43
作者：
Li, Xiaodan [1 ,2 ]
Yan, Binhang [1 ,3 ]
Yao, Siyu [3 ]
Kattel, Shyam [3 ]
Chen, Jingguang G. [2 ,3 ]
Wang, Tiefeng [1 ]
机构：
[1] Tsinghua Univ, Dept Chem Engn, Beijing Key Lab Green React Engn & Technol, Beijing 100084, Peoples R China
[2] Columbia Univ, Dept Chem Engn, New York, NY 10027 USA
[3] Brookhaven Natl Lab, Chem Dept, New York, NY 11973 USA
来源：
APPLIED CATALYSIS B-ENVIRONMENTAL | 2018年 / 231卷
基金：
中国国家自然科学基金;
关键词：
Oxidative dehydrogenadon; Dry reforming; n-Butane; 1,3-Butadiene; CO2; SYngas; NiFe bimetallic catalysts; AUGMENTED-WAVE METHOD; CARBON-DIOXIDE; SUPPORTED CATALYSTS; SOFT OXIDANT; TRANSITION-METALS; SYNGAS PRODUCTION; ELECTRON-GAS; BUTADIENE; ALKANES; OLEFINS;
D O I：
10.1016/j.apcatb.2018.02.063
中图分类号：
O64 [物理化学（理论化学）、化学物理学];
学科分类号：
070304 ; 081704 ;
摘要：
The oxidative dehydrogenation of n-butane to 1,3-butadiene using CO2 as a soft oxidant is investigated over oxide-supported NiFe bimetallic catalysts. Dry reforming of n-butane with CO2 to syngas is also studied under identical conditions for comparison. The Ni(1)ire(3)/CeO2 catalyst is identified as a promising catalyst for the oxidative dehydrogenation to 1,3-butadiene via the C-H bond cleavage, while the Ni3Fe1/CeO2 catalyst mainly promotes the dry reforming pathway via the C-C bond scission. The oxidation states of Ni and Fe are determined by X-ray absorption fine structure (XAFS) measurements under reaction conditions. Density functional theory (DFT) calculations are performed to further understand the different reaction pathways. Furthermore, the effect of oxide supports is studied for the Ni1Fe3 bimetallic catalysts, showing that highly reducible supports, CeO2 and CeO2-ZrO2, promote the production of 1,3-butadiene, whereas the ZrO2 support significantly suppresses the oxidative dehydrogenation.
引用
收藏
页码：213 / 223
页数：11
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