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

被引：22

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

页码：11749 / 11760

页数：12

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