Understanding Selectivity in CO2 Hydrogenation to Methanol for MoP Nanoparticle Catalysts Using In Situ Techniques

Autor:	Joseph A. Singh, Alessandro Gallo, Samuel K. Regli, Magnus Rønning, Joshua M. McEnaney, Eduardo Valle, Jonathan L. Snider, Stacey F. Bent, Thomas F. Jaramillo, Melis S. Duyar
Jazyk:	angličtina
Rok vydání:	2021
Předmět:	methanol synthesis MoP Diffuse reflectance infrared fourier transform Absorption spectroscopy Phosphide 010402 general chemistry Photochemistry lcsh:Chemical technology 01 natural sciences Catalysis lcsh:Chemistry chemistry.chemical_compound support effects Formate lcsh:TP1-1185 Physical and Theoretical Chemistry in situ characterization X-ray absorption spectroscopy 010405 organic chemistry 0104 chemical sciences chemistry lcsh:QD1-999 Methanol Selectivity CO2 hydrogenation
Zdroj:	Catalysts Volume 11 Issue 1 'Catalysts ', vol: 11, pages: 143-1-143-18 (2021) 143-? Catalysts, Vol 11, Iss 143, p 143 (2021)
ISSN:	2073-4344
DOI:	10.3390/catal11010143
Popis:	Molybdenum phosphide (MoP) catalyzes the hydrogenation of CO, CO2 , and their mixtures to methanol, and it is investigated as a high-activity catalyst that overcomes deactivation issues (e.g., formate poisoning) faced by conventional transition metal catalysts. MoP as a new catalyst for hydrogenating CO2 to methanol is particularly appealing for the use of CO2 as chemical feedstock. Herein, we use a colloidal synthesis technique that connects the presence of MoP to the formation of methanol from CO2 , regardless of the support being used. By conducting a systematic support study, we see that zirconia (ZrO2 ) has the striking ability to shift the selectivity towards methanol by increasing the rate of methanol conversion by two orders of magnitude compared to other supports, at a CO2 conversion of 1.4% and methanol selectivity of 55.4%. In situ X-ray Absorption Spectroscopy (XAS) and in situ X-ray Diffraction (XRD) indicate that under reaction conditions the catalyst is pure MoP in a partially crystalline phase. Results from Diffuse Reflectance Infrared Fourier Transform Spectroscopy coupled with Temperature Programmed Surface Reaction (DRIFTSTPSR) point towards a highly reactive monodentate formate intermediate stabilized by the strong interaction of MoP and ZrO2 . This study definitively shows that the presence of a MoP phase leads to methanol formation from CO2 , regardless of support and that the formate intermediate on MoP governs methanol formation rate. : © 2021 by the authors. Licensee MDPI, Basel, Switzerland. This article is an open access article distributed under the terms and conditions of the Creative Commons Attribution (CC BY) license (https:// creativecommons.org/licenses/by/ 4.0/).
Databáze:	OpenAIRE
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