Fission products physical chemistry

Head : Florent LOUIS
Co-head : Laurent GASNOT

The research team results from collaborative research activities initiated in 2006 between the PC2A laboratory and the "Pôle de Sûreté Nucléaire" from the "Institut de Radioprotection et de Sûreté Nucléaire" IRSN on topics relative to the thermodynamics and chemical reactivity of fission products. The complimentary and the skills of both partners allowed to make long-lasting this collaboration during ten years within the framework of the common research laboratory IRSN/CNRS/Lille C3R "Chemical Kinetics, Combustion, and Reactivity" (2009 - 2019). The research activities concern problems covering a wide spectrum of the homogeneous and heterogeneous reactivity using different approaches (experimental, molecular simulations, modelling). The main objectives of the led researches are to validate the estimations of radio-contaminant releases if a severe nuclear power plant accident type Chernobyl and the more recent Fukushima disaster was to occur.

 

Several research activities are now under study :

Topic 1 : Iodine chemistry from the power plant to the atmosphere
Topic 2 : Interaction of gaseous iodine with sodium aerosols
Topic 3 : Revolatilisation of fission products deposits
Topic 4 : Gaseous iodine compounds metrology

Last publications of our team:

1) Unraveling the Tropospheric Microhydration Processes of Iodous Acid HOIO

2) Box modelling of gas-phase atmospheric iodine chemical reactivity in case of a nuclear accident

3) Microhydration of caesium metaborate: structural and thermochemical properties of CsBO2 + n H2O (n = 1–4) aggregates

4) A theoretical study of the microhydration processes of iodine nitrogen oxides

5) Reactivity of Hydrogen Peroxide with Br and I Atoms

Staff members

Researchers: Fèvre-Nollet V. (MCF HDR), Gasnot L. (PR), Lebègue P. (MCF), Louis F. (MCF, HDR), Pauwels J.F. (PREm), Ribaucour M. (MCF, HDR)
Administrative/Technical staff: Taamalli S. (IR, CDD)
Ph-D student: Infuso M. (PhLAM/PC2A, Oversee, 2019 - )

(* soutenance prévue)

PR : Professeur des Universités ; PREm : Professeur des Universités Emérite ; MCF : Maître de Conférences ; HDR : Habilité à Diriger des Recherches ; IR : Ingénieur de Recherche ; IE : Ingénieur d'Etude ; AI : Assistant-Ingénieur ; T : Technicien

Contracts and ongoing collaborations

  • PIA MiRE "Mitigation des Rejets à l’Environnement en cas d’accident nucléaire" (ANR-00-RSNR0013-01), 2014-2019
  • PIA Labex CaPPA "Chemical and Physical Properties of the Atmosphere" (ANR-11-LABX-0005-01), 2013-2022
  • Pr. Ivan Cernusak, Comenius University in Bratislava (Slovakia)
  • Pr. Alfonso Saiz-Lopez, CSIC (Espagne)
  • Pr. Gabriel da Silva, University of Melbourne (Australia)
  • Pr. Minh Tho Nguyen, KU Leuven (Belgium)
  • Dr. Duy Quang DAO, Da Nang University (Vietnam)

Ph-D in progress

Unravelling the atmospheric iodine chemistry using molecular simulations

The goal is to improve the understanding of the heterogeneous reactivity between gaseous iodinated species and aerosols present in the troposphere. To date, these heterogeneous interactions have not been considered in the atmospheric iodine dispersion models in case of a severe nuclear power plant accident. This is worrisome since such heterogeneous reactivity may play a major role in the iodine transport far from their emission sources. The importance of iodine in atmospheric chemistry has been highlighted by recent reviews. However, the atmospheric iodine heterogeneous reactivity studies have focused almost exclusively on determining the uptake coefficient of inorganic iodinated compounds (for example, I2, HI, and HOI) by water or ice. Those conditions are not fully relevant for our applications and have to be extended. Furthermore, photo-oxidation of gaseous CH3I and I2 in presence of O3 is known to produce IxOy aerosols, which are measured in the field campaigns. To the best of our knowledge, the influence of aerosols on the iodine photolysis processes in gas phase is not documented. Finally, the field measurements in Arctic and Antarctica pointed out the role of the low temperature in iodine chemistry in gas phase and in the formation of iodine-rich aerosols.

As a result, this thesis will provide a set of reliable kinetic and mechanistic data on iodine (photo)reactivity with atmospheric aerosols in order to improve the relevance and accuracy of iodine chemistry in dispersion models. The work will be based on molecular simulations; systems associating both the main iodinated gaseous species and representative atmospheric aerosols will be carefully selected.

Both molecular iodine (I2) and iodomethane (CH3I) are key iodine compounds of marine and biogenic origin that appears to be of central importance in understanding iodine chemistry in the troposphere. Further, in addition to their atmospheric interest, the reactivity of those compounds has gained much interest in the field of nuclear safety as they are the most probable gaseous iodine species to be released to the troposphere during a severe nuclear power plant accident of the type in Fukushima, Japan. As a result, this work will start on gaseous molecular iodine and iodomethane surface reactivity as a function of key inorganic and organic aerosols classes from the nanometric up to micrometric size. Model primary and secondary aerosols from marine origin will be considered, such as sodium chloride, sulphate, nitrate, and low to high oxidized organic aerosols.

 

Keywords : Iodine, aerosols, atmosphere, molecular simulations

Research program linked to the subject : PIA Labex CaPPA

Funding :  I-Site Oversee project

Ph-D student : Maxime INFUSO

Advisors : Denis DUFLOT / Florent LOUIS / Céline TOUBIN

Master in progress

Atmospheric chlorine chemistry modelling

The atmosphere is a complex chemical reactor in which a great number of reactions occurs. Most of these reactions are initiated by solar radiation and involves also chemical species either from natural or from anthropogenic sources. Although these compounds are present at very low level of concentration in the atmosphere (ppt to ppm), they could affect the environment and the climate. Human activities have noticeably changed the chemical composition of the atmosphere leading to the outcome of environmental problems such as global warming, or ozone depletion.

The reactions involving chlorine-containing species can modify the chemistry and the composition of the atmosphere. It stills however a lot of uncertainties in the understanding of the gas-phase atmospheric chemistry of these compounds.

The goal of this internship is to improve the understanding of the gas-phase reactivity of chlorine-containing species, to better address the lack of data in the field of atmospheric chemistry and to make a critical review of the literature to establish the chlorine chemical mechanism. 0D modelling studies will be conducted to evaluate the chlorine species speciation under various atmospheric conditions (temperature, photolysis, gas concentration, ...).

 

Keywords: Atmosphere, chlorine, chemical mechanism, numerical simulations

Research program linked to the subject : PIA Labex CaPPA

Student : Zainab SROUR

Advisors : Florent LOUIS / Valérie FEVRE-NOLLET

Alumni

 

Guest researchers: Prof. Ivan CERNUSAK (Comenius University, Bratislava, Slovakia), Prof. Ted S. DIBBLE (State University of New York College of Environmental Sciences and Forestry, Syracuse, USA), Dr. Duy Quang DAO (Da Nang University, Vietnam)

Post-doctoral fellows: Dr. Sonia TAAMALLI, Dr. Dorra KHIRI, Dr. Sarah KHANNICHE, Dr. Katarina SULKOVA, Dr. Michael BADAWI, Dr. Eddy THIRIOT, Dr. Arnaud VILLARD, Dr. Bertrand XERRI

Ph-D thesis: Dr. Camille FORTIN, Dr. Ankita JADON, Dr. Dorel OBADA, Dr. Jan SKOVIERA (co-tutelle avec la Slovaquie), Dr.  Faoulat MIRADJI, Dr. Adrien CARTONNET, Dr. Julien TRINCAL, Dr. Emmanuel MATHE, Dr. Romain VANDEPUTTE, Dr. Yathis DELICAT

Internships: Aurélie LOBBESTAEL (L3, Lille, 2020), Mélissa ACHAB (L3, Lille, 2020), Athmane HARCHAOUI (L3, Lille, 2020), Eliott DUBOIS (L3, ENSCM, 2019), Sandra BALLET (M1, Lille, 2019), Alexis DESCAMPS (L3, Lille, 2019), Laureine FERSING (L3, Lille, 2019), Morgane RIVOAL (L3, Lille, 2019), Guillaume LAMARQUE (L3, Lille, 2019), Anastasia ROTARI (L3, Lille, 2018), Geoffrey LEMOINE (L3, Lille, 2018), Cécile LAFONT (M1, ENSCM, 2018), Olivier ROUILLARD (Erasmus, Canada, 2018)