Litcius/Paper detail

High-Temperature Pretreatment Effect on Co/SiO<sub>2</sub> Active Sites and Ethane Dehydrogenation

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

2022ACS Catalysis34 citationsDOIOpen Access PDF

Abstract

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 CoOx 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.

Topics & Concepts

DehydrogenationCatalysisXANESFourier transform infrared spectroscopyAdsorptionDensity functional theoryDesorptionThermal desorption spectroscopyChemistryScanning transmission electron microscopyInfrared spectroscopyInorganic chemistryPhotochemistryMaterials scienceAnalytical Chemistry (journal)Physical chemistrySpectroscopyTransmission electron microscopyChemical engineeringNanotechnologyOrganic chemistryComputational chemistryQuantum mechanicsPhysicsEngineeringCatalytic Processes in Materials ScienceCatalysis and Oxidation ReactionsCatalysts for Methane Reforming