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

Yu, Kewei; Srinivas, Sanjana; Wang, Cong; Chen, Weiqi; Ma, Lu; Ehrlich, Steven N.; Marinkovic, Nebojsa; Kumar, Pawan; Stach, Eric A.; Caratzoulas, Stavros; Zheng, Weiqing; Vlachos, Dionisios G.

doi:10.1021/acscatal.2c03180

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

Journal Article · 12 September 2022 · ACS Catalysis

DOI: https://doi.org/10.1021/acscatal.2c03180 · OSTI ID:1973500

^[1]; Srinivas, Sanjana ^[1];

^[1]; Chen, Weiqi ^[1]; Ma, Lu ^[2]; Ehrlich, Steven N. ^[2]; Marinkovic, Nebojsa ^[2];

^[3];

^[1];

^[1]

Univ. of Delaware, Newark, DE (United States)
Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source
Univ. of Pennsylvania, Philadelphia, PA (United States)

Here, 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 °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 CoO_x nanoparticles. Fourier transform infrared (FTIR) and isopropanol (IPA) temperature-programmed desorption and density functional theory (DFT) calculations suggest that high-temperature treatment significantly increases the density of active Lewis acid sites, possibly via surface dehydroxylation of the catalyst.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: National Science Foundation (NSF); USDOE Office of Energy Efficiency and Renewable Energy (EERE); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0012704

OSTI ID:: 1973500

Report Number(s):: BNL-224374-2023-JAAM

Journal Information:: ACS Catalysis, Journal Name: ACS Catalysis Journal Issue: 19 Vol. 12; ISSN 2155-5435

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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

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