Title :

Common intermediate species from reducing and activation of CoMo-based catalyst revealed via multivariate augmented system applied to time-resolved in situ XAS data

Author(s) :

Oliveira De Souza, Danilo [Auteur]
Unité de Catalyse et Chimie du Solide - UMR 8181 [UCCS]
Tougerti, Asma [Auteur]
Unité de Catalyse et Chimie du Solide (UCCS) - UMR 8181
Briois, Valérie [Auteur]
Synchrotron SOLEIL [SSOLEIL]
Lancelot, Christine [Auteur]
Unité de Catalyse et Chimie du Solide (UCCS) - UMR 8181
Cristol, Sylvain [Auteur]
Unité de Catalyse et Chimie du Solide (UCCS) - UMR 8181

Journal title :

Molecular Catalysis

Abbreviated title :

Mol. Catal.

Volume number :

530

Pages :

112619

Publisher :

Elsevier

Publication date :

2022-08-24

ISSN :

2468-8231

English keyword(s) :

Chemometric methods
Hydrodesulfurization
CoMo catalyst
Time -resolved XAS

HAL domain(s) :

Chimie/Catalyse

English abstract : [en]

Time-resolved spectroscopy has reached great importance in studies of chemical transformations, particularly in heterogeneous catalysis, where in situ or operando conditions are suitable to correlate precursor transformation ...
Show more >Time-resolved spectroscopy has reached great importance in studies of chemical transformations, particularly in heterogeneous catalysis, where in situ or operando conditions are suitable to correlate precursor transformation and/or genesis of active sites with catalytic efficiency. In this work we present advantages of using chemometric analysis to resolve multi-step chemical reactions in time-resolved XAS experiment. We followed complementary experiments (temperature programmed reduction and activation) of a Ti-supported CoMo HDS catalyst to unravel details in the evolution of the different species appearing during each process. A multivariate analysis uncovered that (i) at Mo K-edge, activation of oxidic precursor is a 3-step mechanism with one reduced-like and one oxysulfide species as intermediates and (ii) TPR is a 2-step process with in which the reduced intermediate is a common species between the two processes. This approach was fundamental to properly number the steps during the TPR and to correctly assign the first intermediate of the activation as a non-sulfide species. Further, when applied to low loading catalyst, remarkably structural differences on the kinetics was found, but a similar active phase was reach at the end. Thereby, using augmented analyses we demonstrated that a careful planning of the experiments is essential to resolve fine details in the kinetics of the reaction.Show less >

Language :

Anglais

Peer reviewed article :

Oui

Audience :

Internationale

Popular science :

Non

Administrative institution(s) :

Université de Lille
CNRS
Centrale Lille
ENSCL
Univ. Artois

Collections :

• Unité de Catalyse et Chimie du Solide (UCCS) - UMR 8181

Research team(s) :

Modélisation et spectroscopies (MODSPEC)
Catalyse pour l’énergie et la synthèse de molécules plateforme (CEMOP)

Submission date :

2024-01-20T00:41:54Z
2024-02-09T16:14:24Z
2024-02-20T09:43:08Z