David Farrusseng

Claude Bernard University Lyon 1, Villeurbanne, Rhône-Alpes, France

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Publications (132)562.09 Total impact

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    ABSTRACT: The first photosensitization of a rhodium-based catalytic system for CO2 reduction is reported, with formate as the sole carbon-containing product. Formate has wide industrial applications and is seen as valuable within fuel cell technologies as well as an interesting H2-storage compound. Heterogenization of molecular rhodium catalysts is accomplished via the synthesis, post-synthetic linker exchange, and characterization of a new metal–organic framework (MOF) Cp*Rh@UiO-67. While the catalytic activities of the homogeneous and heterogeneous systems are found to be comparable, the MOF-based system is more stable and selective. Furthermore it can be recycled without loss of activity. For formate production, an optimal catalyst loading of ∼10 % molar Rh incorporation is determined. Increased incorporation of rhodium catalyst favors thermal decomposition of formate into H2. There is no precedent for a MOF catalyzing the latter reaction so far.
    ChemSusChem 01/2015; 8(4). DOI:10.1002/cssc.201403345 · 7.48 Impact Factor
  • Jerome Canivet, David Farrusseng
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    ABSTRACT: Post-functionalisation of metal–organic frameworks is a very efficient and elegant method for designing tailor-made chiral solids for selective asymmetric catalysis. However, erroneous data and misinterpretation can easily occur. We report some best practices in amino acid grafting and use.
    RSC Advances 01/2015; 5(15). DOI:10.1039/C4RA12783H · 3.71 Impact Factor
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    ABSTRACT: Transition-metal nanoparticles (Co, Ni, and Cu) encapsulated in hollow zeolite single crystals were prepared by recrystallization of impregnated bulk MFI crystals in the presence of tetrapropylammonium (TPAOH) solutions. The size and number of particles in hollow MFI depended mainly on the aluminum content. The encapsulation of the nanoparticles prevented them from growing, thus enabling the control of particle size even after high temperature treatments. For low metal loadings (<3 wt %), the mean particle sizes for Co, Ni, and Cu in hollow silicalite-1 were 3.5 +/- 0.3, 3.1 +/- 0.5, and 1.5 +/- 0.2 nm, respectively. In the case of hollow ZSM-5, higher loadings (similar to 8 wt %) could be obtained with mean particle sizes of 17 +/- 2 nm, 13 +/- 2 nm, and 15 +/- 2 nm for Co, Ni, and Cu systems. The mechanism of transition metal nanoparticle formation was markedly different from that of noble metals. At high pH values, transition-metal cations first reacted with dissolved silica species yielding fibrous metal phyllosilicates that were located inside the crystal cavities. The metal phyllosilicates were then converted into nanoparticles upon reduction under H-2 at high temperature (500-750 degrees C). Silicalite-1 encapsulated Ni particles were used in the catalytic hydrogenation of substituted benzenes and showed an outstanding size-selectivity effect. Ni particles were accessible to toluene but not to mesitylene, confirming that the activity is directly related to the diffusion properties of molecules through the zeolite membrane.
    Chemistry of Materials 01/2015; 27(1):276-282. DOI:10.1021/cm503921f · 8.54 Impact Factor
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    ABSTRACT: A novel, powerful method based on a microkinetic approach is described for the estimation of the oxygen transport parameters of mixed electronic conducting materials (MIECs). This method is validated on the perovskite La0.6Sr0.4Co0.2Fe0.8O3-δ and has been applied on Ba0.5Sr0.5Co0.8Fe0.2O3-δ. This approach is original and relevant in that the surface kinetic rate constants are measured using a sample in powder form. In contrast to methods previously used, such as isotope exchange depth profiling (IEDP) and electrical conductivity relaxation (ECR), which determine the global exchange kinetic parameter, our microkinetic modelling approach allows the estimation of the forward and reverse kinetic rates accounting for the oxygen vacancy concentration. Also, the self-diffusion rate coefficient has been estimated at different oxygen partial pressures. This microkinetic approach, which combines SSITKA (steady-state isotopic transient kinetic analysis) and thermogravimetric measurements at controlled oxygen partial pressure, has the potential to significantly accelerate the characterization of oxygen transport in perovskites and related materials in the future. In this study, the kinetic parameters were measured in a temperature window between 873 K and 1173 K, and at two oxygen pressure conditions (21 kPa and 1 kPa) that are appropriate for simulating the semi-permeability of oxygen in a membrane in a process of oxygen separation from air.
    Physical Chemistry Chemical Physics 11/2014; DOI:10.1039/c4cp04243c · 4.20 Impact Factor
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    ABSTRACT: 2,5-dihydroxyterephthalic acid (H4dhtp) was synthetized in a 18g-scale by carboxylation of hydroquinone in molten potassium formate. The hydrated form of Ni2(dhtp) MOF (also known as CPO-27-Ni and MOF-74(Ni)),was obtained in 92% yield by refluxing for 1h a water suspension of the H4dhtp linker with an aqueous solution of nickel acetate. The ensuing characterization of the material (XRD, HRTEM, TGA, N2 adsorption at 77K - SBET = 1233 m²/g) confirmed the obtention of a metal-organic framework of at least equal quality than the ones obtained from the previously reported routes (CPO-27-Ni and MOF-74(Ni)), with a different morphology (namely, well-separated 1 µm platelets for the herein reported water-based route). The temperature dependence of the magnetic susceptibility was measured and satisfactorily simulated assuming a Heisenberg (H = -2JΣSiSi+1) ferromagnetic intrachain interaction (J = +8.1 cm-1) with antiferromagnetic interchain interaction (J’ = -1.15 cm-1). Overall, the reaction in water appears to follow easily distinguishable steps, the first being the deprotonation of H4dhtp by acetate counterion, leading to a soluble nickel adduct of the linker, en route to the MOF self-assembly.
    Journal of Materials Chemistry A: Materials for Energy and Sustainability 07/2014; 2(42):17757-17763. DOI:10.1039/C4TA03066D
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    ABSTRACT: A set of 15 metal–organic frameworks (MIL-53, MIL-68, MIL-125, UiO-66, ZIF) exhibiting different pore size, morphology, and surface chemistry is used to unravel the numerous behaviors of water adsorption at room temperature in this class of materials. Outstanding “S”-shaped (type V) adsorption isotherms are observed for MIL-68 type solids. We show that the underlying mechanism of water adsorption can be rationalized using a simple set of three parameters: the Henry constant (i.e. the slope of the adsorption pressure in the low pressure range), the pressure at which pore filling occurs, and the maximum water adsorption capacity. While the Henry constant and pore filling pressure mostly depend on the affinity of water for the surface chemistry and on pore size, respectively, these two parameters are correlated as they both reflect different aspects of the hydrophobicity–hydrophilicity of the material. For a given type of porous structure, the functionalization of the material by hydrophilic moieties such as hydrogen bonding groups (amine or aldehyde) systematically leads to an increase in the Henry constant concomitantly with a decrease in the pore filling pressure. As for the adsorption mechanism, we show that, for a given temperature, there is a critical diameter (Dc 20 Å for water at room temperature) above which pore filling occurs through irreversible capillary condensation accompanied by capillary hysteresis loops. Below this critical diameter, pore filling is continuous and reversible unless the material exhibits some adsorption-induced flexibility.
    New Journal of Chemistry 06/2014; 38(7). DOI:10.1039/C4NJ00076E · 3.16 Impact Factor
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    ABSTRACT: Two cobalt imidazolate metal–organic frameworks were evaluated as a bactericidal material against the growt h of the Gram-negative bacteria Pseudomonas putida and Escherichia coli. Under the most unfavourable conditions, within the exponential growth phase and in the culture media for both microorganisms, the growth inhibition reached over 50% for concentrations of biocidal material in the 5–10 mg L�-1 range. The release of metal gives excellent durability with the antibacterial effect persisting after 3 months. Both cobalt-based materials can be prepared with simple, cheap and easily accessible commercial ligands, leading to a more affordable possible future application as antimicrobial materials.
    Chemosphere 06/2014; 113:188-192. DOI:10.1016/j.chemosphere.2014.05.029 · 3.50 Impact Factor
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    ABSTRACT: This review article presents the fundamental and practical aspects of water adsorption in Metal-Organic Frameworks (MOFs). The state of the art of MOF stability in water, a crucial issue to many applications in which MOFs are promising candidates, is discussed here. Stability in both gaseous (such as humid gases) and aqueous media is considered. By considering a non-exhaustive yet representative set of MOFs, the different mechanisms of water adsorption in this class of materials are presented: reversible and continuous pore filling, irreversible and discontinuous pore filling through capillary condensation, and irreversibility arising from the flexibility and possible structural modifications of the host material. Water adsorption properties of more than 60 MOF samples are reported. The applications of MOFs as materials for heat-pumps and adsorbent-based chillers and proton conductors are also reviewed. Some directions for future work are suggested as concluding remarks.
    Chemical Society Reviews 05/2014; 43(16). DOI:10.1039/c4cs00078a · 30.43 Impact Factor
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    ABSTRACT: The hydrogen uptake in hybrid sorbents consisting of n-alkane solvents confined in mesoporous silica aerogel is measured at different temperatures from 273 to 313 K and pressures up to 40 bar. An apparent “oversolubility” effect is observed as the H2 uptake in the hybrid sorbents is much larger than that in bulk solvents. The H2 uptake in the hybrid sorbents is found to increase with increasing temperature, which suggests that the flexibility and conformation of n-alkane molecules confined in the aerogel play a crucial role; high-entropy (disordered) alkane configurations lead to the creation of numerous cavities which make it possible to solubilize a larger number of H2 molecules. This departs from adsorption-driven solubility effects for which the number of solubilized molecules decreases with increasing temperature. For a given temperature and pressure, it is found that the number of solubilized H2 molecules per unit volume increases with decreasing alkane chain length. Such an effect, which is observed for both the bulk alkanes and the alkanes confined in the silica aerogel, can be rationalized by considering the number density of CHx (x = 2 or 3) groups; for a given temperature, the latter number density decreases with decreasing alkane chain length so that the free volume available to solubilize H2 molecules increases.
    The Journal of Physical Chemistry C 05/2014; 118(20):10720–10727. DOI:10.1021/jp411526f · 4.84 Impact Factor
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    ABSTRACT: Recently, the use of mixtures of organic-building-block linkers has given chemists an additional degree of freedom for engineering metal-organic frameworks (MOFs) with specific properties; however, the poor characterization of the chemical complexity of such MixMOF structures by conventional techniques hinders the verification of rational design. Herein, we describe the application of a technique known as photothermal induced resonance to individual MixMOF microcrystals to elucidate their chemical composition with nanoscale resolution. Results show that MixMOFs isoreticular to In-MIL-68, obtained either directly from solution or by postsynthetic linker exchange, are homogeneous down to approximately 100 nm. Additionally, we report a novel in situ process that enables the engineering of anisotropic domains in MOF crystals with submicron linker-concentration gradients.
    Angewandte Chemie International Edition 03/2014; 53(11). DOI:10.1002/anie.201309295 · 11.34 Impact Factor
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    ABSTRACT: Highly controlled "ship-in-a-bottle" platinum nanoparticles in silicalite-1 hollow single crystals have been prepared. This catalyst is highly active for toluene hydrogenation but shows no activity for the hydrogenation of 1,3,5-trimethylbenzene.
    Chemical Communications 01/2014; 50(15). DOI:10.1039/c3cc48648f · 6.38 Impact Factor
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    ABSTRACT: Hierarchical zeolitic imidazolate framework-8 nanocrystals catalyze esterification of glycerol with oleic acid at low temperature and become hierarchical upon local transformation of the framework
    ChemCatChem 12/2013; DOI:10.1002/cctc.201300581 · 5.18 Impact Factor
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    ABSTRACT: a b s t r a c t The establishment of periodic trends is a powerful approach for rational design of heterogeneous cata-lysts. It deals with measuring or computing a physico-chemical descriptor of a solid which is correlated to the activity in a specific catalytic reaction. In this work, the metal–carbon bond energy (E MC), calcu-lated in the M 2 C carbide phases was calculated as a bulk descriptor to predict the catalytic activity of metal supported catalysts for the selective hydrogenation of styrene. A set of different metals (Cu, Pt, Pd, Ir, Co, Ni, Ru and Rh) supported on silica were prepared and characterized. Experimental TOFs were measured in a semi-batch reactor. The TOF follows the order Pd > Rh > Ru, Pt, Ir > Ni > Co > Cu which dif-fers from the well established hydrogenation of ethylene. We show that the metal–carbon bond energy (E MC) calculated by DFT from the corresponding M 2 C carbide bulk structure correlates the TOF of styrene hydrogenation over the 8 metal catalysts according to a double volcano curve. The predictive model indicates Pd is the most active monometallic phase and suggests quantitative guidelines for the rational design of very active catalyst compositions.
    Journal of Catalysis 11/2013; 307:352. DOI:10.1016/j.jcat.2013.08.009 · 6.07 Impact Factor
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    ABSTRACT: In this study, we report a novel approach for suppressing coke formation in direct-methane solid oxide fuel cells (SOFCs) with a conventional nickel cermet anode by simply adding ammonia to the fuel gas. Because ammonia preferentially occupies the acidic sites of the anode catalyst materials, a significant decrease in the coke formation rate is realized by introducing ammonia into the methane gas. In addition, hydrogen, a decomposition product of ammonia, also acts as an additional fuel for the SOFCs, resulting in high cell performance. At 700 °C, the coke formation rate over the Ni-YSZ anode is suppressed by 71% after the addition of 33.3% NH3 into CH4. Suppressed coke formation is also observed for other Ni catalysts such as Ni/Al2O3, a common catalyst for methane reforming that has been successfully used as the anode catalyst layer for SOFCs operating on methane, which suggests that introducing NH3 as an additive gas is a general method for suppressing the coke formation. The addition of ammonia can also effectively improve the power output and operational stability and offers a novel means for developing new coke-resistant SOFCs operating on widely available hydrocarbons for clean power generation to realize a sustainable future.
    Journal of Power Sources 10/2013; 240:232–240. DOI:10.1016/j.jpowsour.2013.04.014 · 5.21 Impact Factor
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    ABSTRACT: We report an original and scalable synthesis pathway to produce encapsulated gold nanoparticles. Precise control of the gold particles is achieved in the range of 1-10 nm through the impregnation of silicalite-1 with a controlled concentration of gold solution, followed by dissolution-recrystallization of the zeolite.
    Chemical Communications 08/2013; 49(76). DOI:10.1039/c3cc44843f · 6.38 Impact Factor
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    ABSTRACT: We report two new microporous mixed-metals triazolate based MOFs made from zinc and nickel salts combined with either 1,2,4-triazole or 3,5-diamino-1,2,4-triazole. Their structures, refined from X-ray powder diffraction, their CO2 adsorption and photoluminescent properties show a direct correlation with the structure of their parent organic ligand.
    CrystEngComm 07/2013; 15(45). DOI:10.1039/c3ce41260a · 3.86 Impact Factor
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    ABSTRACT: The number and strength of adsorption sites for Xe in silver-modified zeolites are estimated from isotherm measurements at various temperatures over a broad range of pressure (from 1 ppm to atmospheric pressure). Fully and partially exchanged silver zeolites were synthesized starting from Na-ZSM-5(25), Na-ZSM-5(40), Na-Beta, NaX, and NaY. We have discovered that silver-modified zeolites may present one or two distinct adsorption sites depending on the nature of the material and silver loadings. The strongest adsorption sites are characterized by isosteric heat of adsorption in the order of −40 to −50 kJ·mol–1. For Pentasil-type zeolites, we observe a linear 2:1 correlation between the total amount of silver and the number of strong sites. The highest concentration of strong sites is found for fully silver exchanged ZSM-5 (5.7 × 10–4 mol/g), which presents the largest silver content for Pentasil-type zeolite. The equilibrium constant of Ag-ZSM-5 at low pressure is about 50 times larger than that of AgX. Qualitative correlations were established between Xe adsorption isotherms and Xe NMR signals. We show that Xe NMR could be used as a quantitative method for the characterization of the strength and of the number of strong Xe adsorption sites on silver-exchanged zeolites. The numbers of strong adsorption sites responsible for the Xe adsorption at 10–1000 ppm can be determined by the length of the plateau observed at low Xe uptake. In practice, our findings give guidelines for the discovery and optimization of silver-loaded zeolites for the capture of Xe at ppm levels. It appears that the amount of silver is a key parameter. Silver-modified ZSM-5 shows adsorption capacities 2–3 orders of magnitude larger than currently applied adsorbents for atmospheric Xe capture.
    The Journal of Physical Chemistry C 07/2013; 117(29):15122–15129. DOI:10.1021/jp403934r · 4.84 Impact Factor
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    ABSTRACT: Three molecular mechanisms for gas uptake in a solvent confined in mesopores are identified. On the one hand, CO2 uptake is an adsorption-driven phenomenon that arises from the strong interaction between the gas molecules and the pore surface. On the other hand, H2 uptake is a confinement-induced enhanced solubility in which solubility is favored in the regions of low solvent density formed by the layering of the solvent. In partially filled pores, adsorption at the gas/liquid solvent interface is a third mechanism that leads to large gas uptakes. This study, which sheds light on previously reported yet unclear oversolubility in pores, provides a guide to design hybrid porous catalysts consisting of a solvent confined in a porous solid.
    Journal of Physical Chemistry Letters 06/2013; 4(14):2274–2278. DOI:10.1021/jz401143x · 6.69 Impact Factor
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    ABSTRACT: A novel concept that employs dual chamber SOFC technology with a porous electrolyte, which allows the controlled distribution of gaseous O2 at the anode side, was successfully designed using an all porous structure. The oxidative reforming of hydrocarbon streams can consequently operate in a similar fashion to single chamber SOFCs, but within a safer, better controlled process.
    Energy & Environmental Science 06/2013; 6(7):2119-2123. DOI:10.1039/C3EE40131F · 15.49 Impact Factor
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    L. Baumes, C. Mirodatos, D. Farrusseng

Publication Stats

2k Citations
562.09 Total Impact Points

Institutions

  • 2004–2014
    • Claude Bernard University Lyon 1
      • Institut de recherches sur la catalyse et l'environnement de Lyon (IRCELYON)
      Villeurbanne, Rhône-Alpes, France
  • 1999–2013
    • French National Centre for Scientific Research
      • Institut de recherches sur la catalyse et l`environment de Lyon (IRCELYON)
      Lutetia Parisorum, Île-de-France, France
  • 2011–2012
    • University of Lyon
      Lyons, Rhône-Alpes, France
  • 2007
    • Ghent University
      Gand, Flemish, Belgium
  • 2001–2007
    • Max Planck Institute for Coal Research
      Mülheim-on-Ruhr, North Rhine-Westphalia, Germany
    • Ecole Nationale Supérieure de Chimie de Montpellier
      Montpelhièr, Languedoc-Roussillon, France
  • 2005
    • Delft University of Technology
      Delft, South Holland, Netherlands