Activity Trends in the Propane Dehydrogenation Reaction Catalyzed by MIII Sites on an Amorphous SiO2 Model

One class of particularly active catalysts for the Propane Dehydrogenation (PDH) reaction are well-defined M(III) sites on amorphous SiO. In the present work, we focus on evaluating the catalytic trends of the PDH for four M(III) single-sites (Cr, Mo, Ga and In) on a realistic amorphous model of SiO...

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Bibliographic Details
Authors: Praveen, C. S., Comas-Vives, Aleix|||0000-0002-7002-1582
Format: article
Publication Date:2021
Country:España
Institution:Universitat Autònoma de Barcelona
Repository:Dipòsit Digital de Documents de la UAB
Language:English
OAI Identifier:oai:ddd.uab.cat:251396
Online Access:https://ddd.uab.cat/record/251396
https://dx.doi.org/urn:doi:10.1007/s11244-021-01535-9
Access Level:Open access
Keyword:MIII sites
Lewis acidic sites
Transition-metals
Silica
Propane dehydrogenation reaction
Amorphous model
Description
Summary:One class of particularly active catalysts for the Propane Dehydrogenation (PDH) reaction are well-defined M(III) sites on amorphous SiO. In the present work, we focus on evaluating the catalytic trends of the PDH for four M(III) single-sites (Cr, Mo, Ga and In) on a realistic amorphous model of SiO using density functional theory-based calculations and the energetic span model. We considered a catalytic pathway spanned by three reaction steps taking place on selected M-O pair of the SiO model: σ-bond metathesis of propane on a M-O bond to form M-propyl and O-H group, a β-H transfer step forming M-H and propene, and the H-H coupling step producing H and regenerating the initial M-O bond. With the application of the energetic span model, we found that the calculated catalytic activity for Ga and Cr is comparable to the ones reported at the experimental level, enabling us to benchmark the model and the methodology used. Furthermore, results suggest that both In(III) and Mo(III) on SiO are potential active catalysts for PDH, provided they can be synthesized and are stable under PDH reaction conditions.