High-Temperature Pretreatment Effect on Co/SiO2 Active Sites and Ethane Dehydrogenation

被引:15
作者
Yu, Kewei [3 ,4 ]
Srinivas, Sanjana [3 ,4 ]
Wang, Cong [3 ]
Chen, Weiqi [3 ]
Ma, Lu [1 ]
Ehrlich, Steven N. [1 ]
Marinkovic, Nebojsa [1 ]
Kumar, Pawan [2 ]
Stach, Eric A. [2 ]
Caratzoulas, Stavros [3 ]
Zheng, Weiqing [3 ]
Vlachos, Dionisios G. [3 ,4 ]
机构
[1] Brookhaven Natl Lab, Natl Synchrotron Light Source, Upton, NY 11973 USA
[2] Univ Penn, Dept Mat Sci & Engn, Philadelphia, PA 19104 USA
[3] Univ Delaware, RAPID Mfg Inst, Delaware Energy Inst, Catalysis Ctr Energy Innovat,Ctr Plast Innovat, Newark, DE 19716 USA
[4] Univ Delaware, Dept Chem & Biomol Engn, Newark, DE 19716 USA
来源
ACS CATALYSIS | 2022年 / 12卷 / 19期
基金
美国国家科学基金会;
关键词
ethylene; Lewis acid; earth-abundant catalysts; shale gas; dehydrogenation; SELECTIVE PROPANE DEHYDROGENATION; CATALYTIC DEHYDROGENATION; ELECTROSTATIC ADSORPTION; PROPYLENE HYDROGENATION; SURFACE SITES; COBALT OXIDE; CO(II) SITES; SILICA; SINGLE; SPECTROSCOPY;
D O I
10.1021/acscatal.2c03180
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
We report the synthesis, optimization, and characterization of Co/ SiO2 for ethane nonoxidative dehydrogenation. Co/SiO2 is synthesized via strong electrostatic adsorption using the widely available Co(NO3)2 as the precursor. We demonstrate that high-temperature pretreatment (900 degrees C) in an inert atmosphere can significantly enhance the initial activity of the Co/SiO2 catalyst. X-ray absorption near-edge spectroscopy (XANES), temperature-programmed reduction (TPR), and high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) suggest that highly dispersed Co(II) clusters are more active than Co0 or CoOx nanoparticles. Fourier transform infrared (FTIR) and isopropanol (IPA) temperature-programmed desorption and density func-tional theory (DFT) calculations suggest that high-temperature treatment significantly increases the density of active Lewis acid sites, possibly via surface dehydroxylation of the catalyst.
引用
收藏
页码:11749 / 11760
页数:12
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