Research fields

Elaboration of new 3D porous materials, development of new/optimized synthesis processes, functionalization (post-synthesis or direct synthesis) and shaping (direct or ex situ)

M. Bonne, G. Chaplais, J. Daou, B. Lebeau, J.-L. Paillaud, J. Patarin, A. Ryzhikov, A. Simon-Masseron

Synthesis of microporous germanosilicates of topology -CLO and UTL. A new family of pyrrolidine derivatives was synthesized and tested in hydrothermal synthesis of microporous germanosilicates as organic structure directing agents (OSDA). One of them, N,N-dimethylperhydro-dicyclopenta[b, d]pyrrolium, made it possible to obtain a germanosilicate of topology -CLO with a very high purity and a Si/Ge ratio of 2, an absolute record for this topology initially known as gallophosphate. Similarly, (6R, 10S)-6,10-dimethyl-5-azoniaspiro [4,5]decane led to IM-12 of topology UTL, a microporous germanosilicate.

Brevet

M. Dodin, J. -L. Paillaud, P. Caullet, A. Defoin, Patent WO2013064786A1, 2013

Multiscale structural characterization of porous solids by coupling of powder X- rays diffraction and solid-state NMR

M. Bonne, G. Chaplais, J. Daou, L. Josien, B. Lebeau, C. Marichal, L. Michelin, J.-L. Paillaud, J. Patarin, A. Ryzhikov, S. Rigolet, A. Simon-Masseron

²⁹Si MAS NMR and ¹H-²⁹Si CP/MAS NMR were used to distinguish between two possible structures of zeolite IM-17 initially described in the Cmmm space group, one of which is interrupted. In addition, recent techniques of nano-electron diffraction have also confirmed the choice of the non-centrosymmetric space subgroup Amm2 (collaboration with Johannes Gutenberg, University Mainz).

Publication

Y. Lorgouilloux, M. Dodin, E. Mugnaioli, C. Marichal, P. Caullet, N. Bats, U. Kolb, U. J.-L. Paillaud  RSC Advances 2014, 4, 19440 DOI : 10.1039/c4ra01383b

Study of the formation mechanisms of porous solids

G. Chaplais, J. Daou, B. Lebeau, C. Marichal, J.-L. Paillaud, J. Patarin, S. Rigolet, A. Simon-Masseron

Thanks to the support of molecular modelling, various organic compounds capable of acting both as OSDAs and inhibitors in the crystal growth of materials (syntheses of nano-sponges or zeolite nanosheets) have been identified. This approach enables the preparation of ZSM-5 zeolite nanosheets by structural conversion of an in situ formed lamellar polysilicate magadiite in the presence of a mono-nitrogen bifunctional compound. This approach was then applied to the synthesis of zeolites EMC-1 (FAU) and EMC-2 (EMT) in the presence of a new bifunctional OSDA of di-aza-crown ether-type.

Publication

J. Dhainaut, T. J. Daou, Y. Bidal, N. Bats, B. Harbuzaru, G. Lapisardi, H. Chaumeil, A. Defoin, L. Rouleau, J. Patarin  CrystEngComm 2013, 15, 3009 DOI 10.1039/C3CE40118A

Optimization of materials and their properties through in-depth structural characterizations

M. Bonne, G. Chaplais, J. Daou, L. Josien, B. Lebeau, C. Marichal, L. Michelin, H. Nouali, J.-L. Paillaud, J. Patarin, A. Ryzhikov, S. Rigolet, A. Simon-Masseron

It has been shown for the first time that the endogenous radicals present in thermally carbonized porous silicas (TCPSi) can be used to improve the sensitivity of ¹H-¹³C CPMAS NMR using dynamic nuclear polarization (DNP). The originality of this work lies in the fact that a significant improvement in the ¹³C NMR signal of the TCPSi material was obtained without the addition of polarization agents. The presence of stable radicals in the TCPSi material has been demonstrated and their quantity determined by Electron Paramagnetic Resonance (EPR). The feasibility of the ¹H-¹³C CPMAS DNP NMR experiments has been proven and this technique has been used to obtain information on the chemical nature of the TCPSi.

Publication

J. Riikonen, S. Rigolet, C. Marichal, F. Aussenac, J. Lalevée, F. Morlet-Savary, P. Fioux, C. Dietlin, M. Bonne, B. Lebeau, V.-P. Lehto, Journal of Physical Chemistry C 2015, 119, 19272  DOI : 10.1021/acs.jpcc.5b05970

Evaluation of the adsorption capacity of pollutants in the gas phase and in the liquid phase by porous materials

G. Chaplais, J. Daou, B. Lebeau, H. Nouali, J. Patarin, A. Simon-Masseron

The syntheses of conventional zeolites result in powdered products, which are generally penalizing for numerous industrial applications. Therefore, the development of shaping methods for these materials with controllable morphologies and sizes is of great technological importance. In the case of the ADEME Méterdiox+ project, it is expected that the field device will be equipped with cartridges into which dioxins/furans adsorbent materials will be introduced. Consequently, the latter must be shaped to avoid the loss of load and the clogging of the cartridges observed when powders are used, as much as possible.

Publication

G. Rioland, L. Bullot, T. J. Daou, A. Simon-Masseron, G. Chaplais, D. Faye, E. Fiani, J. Patarin  RSC Advances 2016, 6, 2470 DOI :  10.1039/c5ra23258a

Development of efficient systems for the storage or the absorption of mechanical energy based on hydrophobic porous solids

G. Chaplais, J. Daou, B. Lebeau, C. Marichal, H. Nouali, J.-L. Paillaud, J. Patarin, A. Ryzhikov

The water intrusion-extrusion in hydrophobic pure silica zeolites (zeosils) leads to a molecular spring behaviour in the case of Silicalite-1 zeolite of topology MFI. During the extrusion, almost complete restitution of the stored energy is observed (energetic yield of 98 %). When concentrated solutions of electrolytes, such as LiCl, MgCl₂ or NaCl, are used instead of pure water, the energetic performances of the zeosils increase considerably. Thus, the stored energy is tripled in the case of the “Silicalite-1 – LiCl 20 M” system compared to one for the “Silicalite-1 – water” system.

Publication

I. Khay, T. J. Daou, H. Nouali, A. Ryzhikov, S. Rigolet, J. Patarin Journal of Physical Chemistry C 2014, 118, 3935 DOI : 10.1021/jp4105163