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Université de Lille
Research Teams

Modelisation and spectroscopies for catalysis

[Translate to English:] Photo équipe de MODSPEC

Team leader : Prof. Sylvain Cristol

Assistant team leader : Dr Mélissandre Richard

Message from the Team Leaders

The activities of our team, “Modeling and Spectroscopies for Catalysis” (ModSpeC), focus on understanding, at the atomic scale, the complex mechanisms involved in heterogeneous or homogeneous catalysis, as well as the processes of catalyst synthesis and active phase/support interactions under various conditions.

To achieve this, we combine spectroscopic methods (IR, NAP-XPS, RAMAN, XAS, etc.) performed in situ or operando, with theoretical approaches, using experimental data from both model and real catalysts. This dual approach offers two main advantages: on the one hand, modeling refines the interpretation of spectroscopic data; on the other hand, spectroscopic characterizations validate the consistency of theoretical models.

Furthermore, studying catalytic reactions across different spatial and temporal scales deepens our understanding of active sites and elementary reaction steps.

This close interaction between modeling and experimentation is made possible by the integration of spectroscopists and theoretical chemists within the same team. This distinctive feature of UCCS fosters fruitful exchanges between both approaches, advancing our research.

 

Sylvain Cristol, Professor, University of Lille

Mélissandre Richard, Associate Professor, Centrale Lille

Keywords:

  • Molecular modeling (reaction mechanisms, DFT, DM, collective variables)

  • Spectroscopies (RAMAN, IR, XAS, NAP-XPS)

  • Reaction mechanisms

  • Supported, model, and disordered systems

  • Operando and time-resolved spectroscopies

  • Isotopic exchange (SSITKA) 

Research Topics

  • MODELING OF REACTION MECHANISMS: An alternative to the trial-and-error approach in the search for new catalysts is the modeling of reaction mechanisms to identify the rate-determining step and thus obtain insights into the parameters that can enhance the activity and selectivity of the catalyst. The study at the atomic scale is carried out using DFT (Density Functional Theory) computational methods. These are combined with the computational power of modern computers, enabling the design of active site models composed of a large number of atoms, and therefore representative of catalyst surfaces. The expertise of the ModSpeC team in this field lies in its ability to incorporate all available experimental data (reactivity and spectroscopic) to define the most relevant theoretical model, through continuous dialogue with experimentalists. One example of theoretical work, supported by the RSRN Mire initiative (PIA), aims to understand the chemical evolution of radioactive nuclei released into the atmosphere during a nuclear accident. In addition to classical quantum chemistry methods, we study the liquid/solid interface using quantum molecular dynamics to determine the solubilization mechanisms of hygroscopic salts. These developments can be applied to the study of solid/liquid or solid/solid interfaces in heterogeneous catalysis.

 

[Translate to English:] Diagramm State Diagramm

10.1016/j.jhazmat.2020.124519

 

PI : J-F Paul ; S. Pipolo

 

Associated Projects and Theses

  • PhD Thesis of Parul Goel - 2023-2026 (ongoing) “ Theoretical Study of High-Temperature Solid Oxide Fuel Cells Using Perovskites ” | Supervisor: J-F. Paul. Co-supervisor: S. Pipolo | Funding: KNOWSKITE-X 

  • PhD Thesis of Ashan Promie - 2024-2027 (ongoing) “Theoritical study of amonia synthesis on uranium nitride” | Supervisor: J-F. Paul | Funding: ULille

 

  • COLLECTIVE VARIABLES: Transformations in condensed matter—such as phase transitions, complex reactions, or precipitations—are collective processes during which many atoms or molecules change their relative positions. A detailed monitoring of such processes, for example via Molecular Dynamics (MD) simulations, requires accounting for a large number of degrees of freedom, which presents two main drawbacks: (i) a significant increase in the computational cost of performing biased MD simulations, and (ii) the loss of a clear visual representation of the transformation’s progress. Collective Variables (CVs) are functions of the system’s degrees of freedom that project the essential aspects of the process onto a small number—often one or two—of descriptors of the transformation. In addition to studying complex processes using MD and biased MD, we also contribute to the design and implementation (via the PLUMED code) of CVs capable of describing transformations involving a large number of degrees of freedom.

[Translate to English:] Schéma Variables collectives

 

10.1103/PhysRevLett.119.245701

 


PI : S. Pipolo ; J-F Paul

Recent Publications

J. Chem. Phys, 162, 9, (2025) DOI
Nature Meth. 16, 670 (2019) DOI
Phys. Rev. Lett. 119, 245701 (2017) DOI
Nature Comm. 8, 2257 (2017) DOI

 

  • TIME-RESOLVED SSITKA-IR COUPLING: Our approach to understanding reaction mechanisms in heterogeneous catalysis also involves the use of Steady-State Isotopic Transient Kinetic Analysis (SSITKA) coupled with Infrared (IR) spectroscopy, with a focus on small molecule activation processes at low temperatures.In parallel, the ModSpeC team has initiated the development of this technique toward increasingly fine time resolutions through the use of step-scan IR mode, allowing us to observe the fastest catalytic steps and reaction intermediates.
[Translate to English:] COUPLAGE SSITKA-IR

10.1016/j.catcom.2023.106684 et 10.1007/s11244-022-01722-2

 

PI : C. Dujardin ; M. Richard

Associated Projects and Theses

Coordination : M. Richard

  • STaRS AIMER Project: HdF Region; 2019-2021 ; 174 k€

Coordination : M. Richard

  • PhD Thesis of Amira Djaafri - 2022-2025 (ongoing) “Analysis of Isotopic Exchange in Time-Resolved Mode to Identify Fast Steps in Catalytic Mechanisms of Oxidation Reactions” | Supervisor: C. Dujardin. Co-supervisor:  M. Richard | Funding: ANR TRAIE 

  • PhD Thesis of Ibrahim Hatoum – Defended on 2023/12/15 “Understanding the Mechanisms of Small Molecule Activation and Development of New Low-Temperature Pollution Control Strategies in Heterogeneous Catalysis” | Supervisor: C. Dujardin. Co-supervisor: M. Richard | Funding: Centrale Lille

 

 

  • IN SITU & OPERANDO RAMAN AND IR SPECTROSCOPIES: The ModSpeC team has strong expertise in the characterization of catalysts under reaction conditions using RAMAN spectroscopy (including SERS) and IR spectroscopy. One of the team’s main research areas is understanding the structure of active phases in bulk and supported catalysts dedicated to energy production (fuel cells) and automotive depollution. A recent Horizon RIA project, involving nine European partners, was awarded to the team. This project focuses on developing mixed oxide electrode materials with perovskite structures, aiming to reduce the content of critical elements while maintaining optimal performance and ensuring fair economic viability

[Translate to English:] Spectroscopie Raman et IR

10.1039/C6CP02353C & 10.1002/cphc.202400432

 

 

PI : E. Berrier ; C. Dujardin ; M. Richard

 

Associated Projects and Theses

Coordination : E. Berrier

  • PhD Thesis of Valérie Theuns - 2023-2026 (ongoing) “ Study of the Structure and Operating Behavior of Mixed Oxide-Based Fuel Cell Electrodes Using In Situ Spectroscopies and Surface Analysis Techniques” | Supervisor: E. Berrier. Co-supervisor:  H. Tissot | Funding: KNOWSKITE-X 

  • PhD Thesis of Siavash Alizadeh - 2023-2026 (ongoing) “Preparation and Characterization of New Electrode Materials for Reversible SOFC/SOEC Systems” | Supervisors: E. Berrier & Y. Kolenko (INL) Co-supervisor: A. Rolle (UCCS) | Funding: INL - KNOWSKITE-X 

  • Thèse de Léonard Floarea - 2023-2026 (ongoing) “Influence of Fission Products on the Thermo-Physico-Chemical Properties of Molten Chloride Salts” | Supervisors: E. Berrier & M. Rivenet (UCCS) | Funding: CIFRE Orano 

 

  • TIME-RESOLVED IN SITU & OPERANDO XAS SPECTROSCOPY: Since the ANR SAXO project (2007–2011) and the team’s involvement in the EQUIPEX project that led to the creation of the beamline, the ModSpeC team has maintained numerous scientific collaborations with the Quick-XAS ROCK beamline at the SOLEIL synchrotron, primarily dedicated to catalysis and electrochemistry. The research topics developed by the team on the ROCK beamline include: (i) the ability to monitor spectral changes with sub-second time resolution; (ii) the possibility of recording spectra at two different absorption edges—either in a single acquisition when the energy ranges are close (e.g., K-edges of Fe and Ni, or Fe and Cu), or in alternating mode using the beamline’s dual monochromators; (iii) the study of catalysts under in situ or operando conditions over a wide range of temperatures (up to 700 °C) and pressures (up to 20 bar), thanks to the beamline’s wide array of reaction devices. In recent years, collaborative studies (with LCC, IPCMS, and UFRJ Brazil) have focused on bimetallic systems such as Ni-Fe/SiO₂ and Cu-Fe/SiO₂ under reduction or hydroconversion conditions, as well as bimetallic carbides such as Mo₂C-Ni or -Cu/SiO₂ under carburization and H₂ reactivation conditions. These studies have revealed the reactions governing the formation of active species and the types of chemical interactions between the metallic elements. New methodological developments are currently underway, particularly in hyperspectral imaging of the catalytic bed.

[Translate to English:] Spectroscopie XAS

10.1039/D2FD00095D                10.1016/j.apcatb.2023.122720

 

 

PI : E. Marceau ; A. Tougerti ; S. Cristol

 

Recent Publications

J. Synchrotron Rad., 31, 1084-1104 (2024). DOI

ChemCatChem, 16, e202300890 (2024). DOI

Appl. Catal. B, 331, 122720 (2023). DOI

Faraday Discuss., 242, 353-373 (2023). DOI

Chem. Catal., 2, 1686-1708 (2022). DOI

 

 

  • XAS AND IR IN ME-PSD MODE: The use of Modulation Excitation (ME) spectroscopy combined with Phase Sensitive Detection (PSD) data remains limited in the field of heterogeneous catalysis. The main challenge lies in the processing of the recorded signal, which requires the development of a mathematical framework and its implementation as software code in order to analyze large datasets. The goal of this project is to establish a solid foundation for ME-PSD data analysis to identify the electronic and geometric structures of active species, thanks to the close interaction between theory and experiment fostered by the ModSpeC team.

[Translate to English:] XAS ET IR EN MODE ME-PSD

PI : S. Cristol ; M. Richard ; A. Tougerti

 

Associated Projects and Theses

  • ANR MESCAT Project : ANR-21-CE50-0019 2021-2025 ; 482 k€ ; Coordination : S. Cristol 

  • PhD Thesis of Nabil Nassar - 2022-2025 (ongoing) “MES-IRTF to probe adsorption and reaction of small molecules on catalyst’s surface” | Supervisor: S. Cristol. Co-supervisor:  A. Tougerti | Funding: ANR MESCAT

  • PhD Thesis of Thèse de Lei Jiang –  Defended on 2024/09/25 “Phase Sensitive Detected XAS to study real industrial oxidation catalysts” | Supervisors: S. Cristol & V. Briois. Co-supervisor:  A. Tougerti | Funding: ULille/SOLEIL

 

 

  • RIXS & HERPFD-XAS: Core-Level X-ray Spectroscopies (XANES, EXAFS, RIXS, XES) are also central to the ModSpeC team’s research activities. The development of these various characterization techniques is carried out in close collaboration with the SOLEIL synchrotron as part of ANR and PIA projects. In addition, due to the vast amount of data generated by this type of spectroscopy, the team is actively involved in the development of chemometric methods for spectral analysis. Further developments are also underway in collaboration with the GALAXIES beamline for high-resolution X-ray absorption spectroscopy.

[Translate to English:] RIXS & HERPFD-XAS

    10.1002/anie.201300538                                                10.1021/acs.jpcc.0c03429

 

 

PI : S. Cristol ; A. Tougerti

  • NAP-XPS: Our research on NAP-XPS (Near-Ambient Pressure X-ray Photoelectron Spectroscopy) focuses both on exploring new types of samples—particularly model and real-world catalysts—and on developing advanced methodologies, such as time-resolved NAP-XPS. The ModSpeC team also investigates X-ray irradiation-induced effects, especially radiolysis phenomena and their consequences on the analyzed materials. These studies rely on the NAP-XPS spectrometer, installed since late 2022 on the surface analysis platform of the Chevreul Institute. This instrument enables the investigation of interfaces under near-atmospheric pressure conditions (up to 20 mbar), allowing access to systems previously incompatible with conventional XPS. It is the second device of its kind in France, following the one on the TEMPO beamline at the SOLEIL synchrotron, operational since 2013.

[Translate to English:] NAP-XPS

    10.1021/acs.jpcc.3c03676                                                 https://chevreul.univ-lille.fr/?page_id=2220

 

 

PI : J-F Paul ; S. Cristol ; H. Tissot

 

Associated Projects and Theses

  • PhD Thesis of Michele De Rocco – 2023-2026 (on going) “In-Operando Study of a Model Catalyst Based on Cu₂O Nanoparticles on Alumina” | Supervisor: S. Cristol. Co-supervisor:  H. Tissot & P. Simon | Funding: ULille

NANOPARTICLES AND THIN FILMS: The goal is to precisely describe, at the atomic scale, the mechanisms involved in a catalytic reaction on a catalyst. The complexity of catalytic systems, the low concentration of active species, and the heterogeneity of real catalysts make their characterization and understanding particularly challenging. To overcome these obstacles, an effective approach involves developing model catalysts that are simpler than their industrial counterparts and better suited to spectroscopic techniques. The model systems under study include nanoparticles with controlled size and shape (e.g., Cu₂O, high-entropy intermetallic nanoparticles—HEIs) and thin films prepared via spin coating (such as perovskites and delafossites). These model catalysts are investigated using operando techniques such as NAP-XPS and RAMAN spectroscopy.

[Translate to English:] Nanocube et Pérokvskite

PI : E. Berrier ; S. Cristol ; H. Tissot 

 

Associated Projects and Theses

  • PhD Thesis of Michele De Rocco – 2023-2026 (on going) “In-Operando Study of a Model Catalyst Based on Cu₂O Nanoparticles on Alumina” | Supervisor: S. Cristol. Co-supervisor:  H. Tissot & P. Simon | Funding: ULille

  • PhD Thesis of Valérie Theuns - 2023-2026 (ongoing) “ Study of the Structure and Operating Behavior of Mixed Oxide-Based Fuel Cell Electrodes Using In Situ Spectroscopies and Surface Analysis Techniques” | Supervisor: E. Berrier. Co-supervisor:  H. Tissot | Funding: KNOWSKITE-X 

  • WILL International Chair project HEI ! : University of Lille ; 2025-2029 ; 500 k€ ; Coordination: H. Tissot, in collaboration with Prof. S. Furukawa from Osaka University

  • IN SITU MANAGEMENT OF CATALYTIC SYNTHESES VIA RAMAN MONITORING AND AI: Instrumentation of a Raman spectrometer for real-time control and monitoring of in-situ reactions using artificial intelligence, in collaboration with INRIA and HORIBA France SAS. These developments are being carried out on the REALCATplatform.

 

PI : C. Dujardin 

Associated Projects and Theses

  • PhD Thesis of Clara Dubois – 2023-2026 (ongoing) “Raman Spectroscopy and Artificial Intelligence Serving Chemical Synthesis” | Supervisors: C. Dujardin & S. Dabo (INRIA) | Funding: CIFRE Horiba

  • ACCELERATION OF MODELING CALCULATIONS through the use of Machine Learning Force Fields (MLFF), we accelerate computational modeling. This includes interpreting NMR spectra of phosphorus and aluminum in complex glasses by computing NMR parameters and generating glassy structures via molecular dynamics combined with MLFF approaches.

 

PI : S. Cristol ; S. Pipolo

Associated Projects and Theses

  • PhD Thesis of Carla Dackane – 2024-2027 (ongoing) “LASER Glasses: Synthesis, Magnetic Resonance Characterization, and Structure Calculations Optimized by Machine Learning” | Supervisors:  S. Cristol & G. Tricot (LASIRE) | Funding: ULille

  • PhD Thesis of Marie Naylor – 2023-2026 (ongoing) “Study of Glass-Ceramic LATP Electrolyte Materials for the Development of Low-Carbon Energy Batteries” | Supervisors:  S. Cristol & G. Tricot (LASIRE) | Funding: ISite (UKent)

 

Team members

Name Function Employer
Elise Berrier CNRS Researcher CNRS
Sylvain Cristol Professor Univ. Lille
Christophe Dujardin Professor Centrale Lille
Eric Marceau Assistant Professor Univ. Lille
Jean-Francois Paul Professor Univ. Lille
Silvio Pipolo Assistant Professor Univ. Lille
Mélissandre Richard Assistant Professor Centrale Lille
Héloise Tissot CNRS Researcher CNRS
Asma Tougerti Assistant Professor Univ. Lille