Description

The catalytic conversion of CO2 into energy-relevant molecules is a promising route to address current energy and environmental challenges; however, it is still hindered by an incomplete understanding of the elementary mechanisms governing CO2 activation and reduction. This PhD project aims to elucidate these mechanisms in heterogeneous catalysis, with particular emphasis on photo-assisted conditions, by combining steady-state isotopic transient kinetic analysis (SSITKA) with time-resolved operando infrared spectroscopy. This original approach, recently developed at UCCS, will enable the correlation of quantitative kinetic information (residence times, surface populations, and formation rates of reaction intermediates) with the spectroscopic identification of reactive surface species. The research will focus on metallic and photoactive catalysts supported on yttria-stabilized zirconia (YSZ), whose oxygen vacancies and basic sites promote CO2 adsorption and polarization. Infrared spectroscopy will be used to monitor carbonate, carboxylate, and formate species, as well as adsorbed CO, and to follow their evolution under irradiation. The objective is to identify the respective roles of the YSZ support, oxygen vacancies, and metal–support interfaces in CO2 activation and reduction, in order to establish relationships between surface structure, reaction intermediates, and selectivity, and ultimately to provide a rational basis for the design of more efficient and selective catalysts for CO2 reduction.

Skills required

Applicants holding an engineering degree or a Master’s degree (MSc) with a research orientation and having a background in heterogeneous catalysis are invited to apply by submitting a CV, a cover letter, and their academic transcripts.

Bibliography

Remarkable Enhancement of O2Activation on Yttrium-Stabilized Zirconia Surface in a Dual Catalyst Bed
Mélissandre Richard; Fabien Can; Daniel Duprez; Sonia Gil; Anne Giroir-Fendler; Nicolas Bion
Angewandte Chemie International Edition 2014-08
DOI: 10.1002/anie.201403921

Insight into the true role of hydrogen-carbonate species in CO oxidation over Pd/Al2O3 catalyst using SSITKA-transmission IR technique
Ibrahim Hatoum, Mélissandre Richard, Christophe Dujardin
Catalysis Communications 179 (2023) 106684-106690
https://doi.org/10.1016/j.catcom.2023.106684

Catalytic methane combustion at low temperatures over YSZ-supported metal oxides: Evidence for lattice oxygen participation via the use of C18O2
Catalysis Communications 2023
DOI: 10.1016/j.catcom.2023.106704

Investigation of Methane Oxidation Reactions Over a Dual-Bed Catalyst System using18O Labelled DRIFTS coupling
Melissandre Richard; Daniel Duprez; Nicolas Bion; Fabien Can
ChemSusChem, 2016
DOI: 10.1002/cssc.201601165

Keywords

heterogeneous catalysis, spectroscopy, photocatalysis, CO2 activation