Jorge Gascon

Delft University of Technology, Delft, South Holland, Netherlands

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Publications (138)671.38 Total impact

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    ABSTRACT: Thin films of the well-known metal organic framework ZIF-8 were formed on zinc oxide nanorods through the reaction with 2-methyl imidazole solution. Deposition of a thin film of the linker solution allows the underlying zinc oxide nanorod morphology to be preserved, resulting in the facile and precise formation of a nanostructured hybrid materials in short reaction times and under conventional heating. The effect of various synthesis parameters on the morphology of the resulting thin film is reported.
    CrystEngComm 06/2015; DOI:10.1039/C5CE00590F · 3.86 Impact Factor
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    ABSTRACT: A preliminary study based on a conceptual process design methodology that includes a technical evaluation and an economic study has been carried out for the use of the metal-organic framework NH2-MIL-53(Al) as adsorbent for the separation of carbon dioxide from methane. Among the alternatives considered, a vacuum pressure swing adsorption was chosen in the detailed design phase. The combination of a design with columns in parallel and the possibility of recirculating some of the streams ensures a high degree of separation and a final product with high quality without compromising the operation costs. A comparison with the state-of-the-art technology, amine scrubbing, and with a process based on membranes demonstrates that the proposed process is competitive as a result of its low operation costs and the energy demand.
    Chemical Engineering & Technology 06/2015; DOI:10.1002/ceat.201400741 · 2.18 Impact Factor
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    ABSTRACT: CAU-10-H displays a highly suitable step-wise water adsorption behaviour for application in adsorption driven heat pumps and chillers. For actual application, manufacturing of coatings of this material on thermally conductive surfaces is highly desired. Direct, single-step, crystallization of CAU-10-H on either metallic or anodized aluminium yields a significant amount of by-product(s) and an inhomogeneous substrate coverage. Although adequate pretreatment of the substrates before crystallization improves the quality of obtained coatings, significant improvements are achieved only when crystal nucleation and growth are separated. More specifically, application of a reactive seeding approach with anodized aluminium leads to full coverage of the substrate surface, high MOF loading and high purity of the crystalline phase, homogeneous layer thickness, narrow crystal size distribution, and good stability in repeated water adsorption-desorption cycles.
    CrystEngComm 05/2015; DOI:10.1039/C5CE00789E · 3.86 Impact Factor
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    ABSTRACT: A single crystal to single crystal transmetallation process takes place in the three-dimensional (3D) metal-organic framework (MOF) of formula Mg(II) 2 {Mg(II) 4 [Cu(II) 2 (Me3 mpba)2 ]3 }⋅45 H2 O (1; Me3 mpba(4-) =N,N'-2,4,6-trimethyl-1,3-phenylenebis(oxamate)). After complete replacement of the Mg(II) ions within the coordination network and those hosted in the channels by either Co(II) or Ni(II) ions, 1 is transmetallated to yield two novel MOFs of formulae Co2 (II) {Co(II) 4 [Cu(II) 2 (Me3 mpba)2 ]3 }⋅56 H2 O (2) and Ni2 (II) {Ni(II) 4 [Cu(II) 2 (Me3 mpba)2 ]3 }⋅ 54 H2 O (3). This unique postsynthetic metal substitution affords materials with higher structural stability leading to enhanced gas sorption and magnetic properties. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
    Angewandte Chemie International Edition 04/2015; 127(22). DOI:10.1002/anie.201501691 · 11.34 Impact Factor
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    ABSTRACT: The promotion of a TiO2 photocatalyst by surface species consisting of cerium oxide and metal-promoted carbon nitride (g-C3N4) was analyzed to gain insight into the effect of Ca or Fe cationic species of the carbon nitride component in the overall performance of the photocatalytic system. The resulting materials were characterized with X-ray diffraction, time-resolved microwave conductivity (TRMC) and photoelectron, infrared, UV-visible and photoluminescence spectroscopies. The photoactivity of the materials in the gas phase elimination of toluene was evaluated under UV and sunlight-type illumination conditions and the corresponding true reaction quantum efficiency values calculated. The photoluminescence and TRMC analyses provide unequivocal evidence that the presence of Fe and Ca alter charge recombination to a different degree, leading to qualitatively different, promoting photochemical effects. This occurs exclusively in co-presence of ceria species at the titania surface and is thus characteristic of the ternary composite heterostructures.
    Applied Catalysis B Environmental 04/2015; 176-177. DOI:10.1016/j.apcatb.2015.04.051 · 6.01 Impact Factor
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    ABSTRACT: Depletion of crude oil resources and environmental concerns have driven a worldwide research on alternative processes for the production of commodity chemicals. Fischer-Tropsch synthesis is a process for flexible production of key chemicals from synthesis gas originating from non-petroleum-based sources. Although the use of iron-based catalysts would be preferred over the widely used cobalt, manufacturing methods that prevent their fast deactivation because of sintering, carbon deposition and phase changes have proven challenging. Here we present a strategy to produce highly dispersed iron carbides embedded in a matrix of porous carbon. Very high iron loadings (>40 wt %) are achieved while maintaining an optimal dispersion of the active iron carbide phase when a metal organic framework is used as catalyst precursor. The unique iron spatial confinement and the absence of large iron particles in the obtained solids minimize catalyst deactivation, resulting in high active and stable operation.
    Nature Communications 03/2015; 6:6451. DOI:10.1038/ncomms7451 · 10.74 Impact Factor
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    ABSTRACT: A combined experimental and simulation study for the separation of carbon dioxide and methane mixtures using NH2-MIL-53(Al) as adsorbent is presented. A fixed-bed model has been applied to simulate binary breakthrough experiments obtained in small lab-scale equipment (10 cm column, 1/4″ in diameter, 800 mg sample). A mixed Langmuir/Langmuir-Freundlich isotherm is used to capture the temperature dependence of the two-step isotherm and a linear driving force model to capture diffusion in the MOF crystals. The model is able to describe the experimental breakthrough data at 273 K over a pressure range of 1 to 20 bar. Displacement of methane by carbon dioxide, a large apparent roll-up effect, heats of adsorption and dispersion phenomena have been quantified taking into account post-column volumes often present in lab-scale equipment. The heat effects result in a maximum local temperature rise up to 20 K.
    Chemical Engineering Science 03/2015; 124:96-108. DOI:10.1016/j.ces.2014.10.028 · 2.61 Impact Factor
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    ABSTRACT: The field of metal-organic framework based mixed matrix membranes (M(4)s) is critically reviewed, with special emphasis on their application in CO2 capture during energy generation. After introducing the most relevant parameters affecting membrane performance, we define targets in terms of selectivity and productivity based on existing literature on process design for pre- and post-combustion CO2 capture. Subsequently, the state of the art in M(4)s is reviewed against these targets. Because final application of these membranes will only be possible if thin separation layers can be produced, the latest advances in the manufacture of M(4) hollow fibers are discussed. Finally, the recent efforts in understanding the separation performance of these complex composite materials and future research directions are outlined.
    Chemical Society Reviews 02/2015; 44(8). DOI:10.1039/c4cs00437j · 30.43 Impact Factor
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    ABSTRACT: A heterogeneous molecular catalyst based on Ir(III) Cp* (Cp*=pentamethylcyclopentadienyl) attached to a covalent triazine framework (CTF) is reported. It catalyses the production of hydrogen from formic acid with initial turnover frequencies (TOFs) up to 27 000 h(-1) and turnover numbers (TONs) of more than one million in continuous operation. The CTF support, with a Brunauer-Emmett-Teller (BET) surface area of 1800 m(2) g(-1) , was constructed from an optimal 2:1 ratio of biphenyl and pyridine carbonitrile building blocks. Biphenyl building blocks induce mesoporosity and, therefore, facilitate diffusion of reactants and products whereas free pyridinic sites activate formic acid towards β-hydride elimination at the metal, rendering unprecedented rates in hydrogen production. The catalyst is air stable, produces CO-free hydrogen, and is fully recyclable. Hydrogen production rates of more than 60 mol L(-1) h(-1) were obtained at high catalyst loadings of 16 wt % Ir, making it attractive towards process intensification. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
    ChemSusChem 02/2015; 8(5). DOI:10.1002/cssc.201403173 · 7.12 Impact Factor
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    ABSTRACT: Metal–organic frameworks (MOFs) are porous crystalline materials consisting of metal ions bound through coordination bonds to organic linkers. Much research over the last few decades have been devoted to the synthesis of these materials in view of their promising applications in, for example, catalysis, separation, gas storage, drug delivery and sensing. Among the variety of methods developed for the synthesis of MOFs are electrochemical techniques. These methods have several advantages such as mild synthesis conditions, shorter synthesis times and the possibility to control the reaction conditions directly during the synthesis process. However, the progress of electrosynthesis methods has lagged behind that of other methods such as solvothermal and microwave-assisted synthesis. In this Review, we summarise and critically assess research on the electrosynthesis of MOFs and provide a full picture of the developments within this field. The various ways in which electrochemistry has contributed to the synthesis of MOFs are explained, their strengths and shortcomings are discussed, and an outlook for future research is provided.
    02/2015; 2(4). DOI:10.1002/celc.201500101
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    ABSTRACT: The effect of synthesis pH and H2O/EtOH molar ratio on the textural properties of different aluminium trimesate metal organic frameworks (MOFs) prepared in the presence of the well-known cationic surfactant cetyltrimethylammonium bromide (CTAB) at 120 °C was studied with the purpose of obtaining a MOF with hierarchical pore structure. Depending on the pH and the solvent used, different topologies were obtained (namely, MIL-96, MIL-100 and MIL-110). On the one hand, MIL-110 was obtained at lower temperatures than those commonly reported in the literature and without additives to control the pH; on the other hand, MIL-100 with crystallite sizes as small as 30 ± 10 nm could be easily synthesized in a mixture of H2O and EtOH with a H2O/EtOH molar ratio of 3.4 at pH 2.6 in the presence of CTAB. The resulting material displays a hierarchical porosity that combines the microporosity from the MOF and the non-ordered mesopores defined in between the MOF nanoparticles. Interestingly, the maximum of the pore size distribution could be varied between 3 and 33 nm. Finally, at pH 2.5 and using water as a solvent, platelets of MIL-96, a morphology never observed before for this MOF, were synthesized with a (001) preferential crystal orientation, the (001) plane running parallel to the bipyramidal cages of the MIL-96 topology.
    CrystEngComm 02/2015; 17(7):1693-1700. DOI:10.1039/C4CE02324B · 3.86 Impact Factor
  • Chemical Communications 01/2015; 51(5):961-962. DOI:10.1039/c4cc90482f · 6.72 Impact Factor
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    ABSTRACT: We present a synthetic strategy for the efficient encapsulation of a derivative of a well-defined cobaloxime proton reduction catalyst within a photoresponsive metal-organic framework (NH2- MIL-125(Ti)). The resulting hybrid system Co@MOF is demonstrated to be a robust heterogeneous composite material. Furthermore, Co@MOF is an efficient and fully recyclable noble metal-free catalyst system for light-driven hydrogen evolution from water under visible light illumination.
    Energy & Environmental Science 12/2014; DOI:10.1039/C4EE02853H · 15.49 Impact Factor
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    ABSTRACT: Multiphase catalytic processes involve the combination of scale-dependent and scale-independent phenomena, often resulting in a compromised, sub-optimal performance. The classical approach of randomly packed catalyst beds using unstructured catalyst particles may be outperformed by the careful design of the catalyst at the nano-scale and by the judicious choice and design of reactor. Application of structured catalysts and reactor internals and the combination of advanced reactor and catalyst systems with in situ separation allow decoupling the various phenomena involved, opening the way to intensified processes on a large scale. The integral approach of Catalysis and Reaction Engineering discussed here will play a pivotal role in the development of novel, future-proof processes.
    12/2014; 5(2). DOI:10.1039/C4CY01406E
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    ABSTRACT: We report a series of powder X-ray diffraction experiments performed on the soft porous crystals MIL-53(Al) and NH2-MIL-53(Al) in a diamond anvil cell under different pressurization media. Systematic refinements of the obtained powder patterns demonstrate that these materials expand along a specific direction while undergoing total volume reduction under an increasing hydrostatic pressure. The results confirm for the first time the negative linear compressibility behaviour of this family of materials, recently predicted from quantum chemical calculations.
    CrystEngComm 12/2014; 17(2). DOI:10.1039/C4CE00436A · 3.86 Impact Factor
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    ABSTRACT: Abstracts: * Porous aromatic polymers as heterogeneous catalysts.pdf (182.8KB) - Uploading Abstracts
    14 AIChE Annual Meeting; 11/2014
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    ABSTRACT: Adsorptive characterization using nitrogen at 77 K is one of the most widely used techniques to assess textural properties of porous solids, such as pore volume, specific surface area and pore size distributions. Based on a thorough error analysis the influence of experimental uncertainties on the accuracy of volumetric nitrogen adsorption isotherms and derived properties using the most popular methods is analyzed in detail, comprising the pore volume and specific surface area determined using the method posed by Brunauer, Emmet and Teller (BET) and the pore size distribution according to the method developed by Barrett, Joyner and Halenda (BJH). Based on series of isotherms measurements with different sorbents (MOFs, zeolite, activated carbon and alumina) and on examples from literature (MIL-101), the extensive error analysis shows that these methods may yield highly inaccurate or even statistically irrelevant (BJH) results. To improve the meaningfulness of derived properties and to minimize statistical uncertainties, practical recommendations and guidelines are proposed for experimental operation variables and data analysis.
    Microporous and Mesoporous Materials 11/2014; 200:199–215. DOI:10.1016/j.micromeso.2014.08.048 · 3.21 Impact Factor
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    ABSTRACT: Composites incorporating two-dimensional nanostructures within polymeric matrices have potential as functional components for several technologies, including gas separation. Prospectively, employing metal-organic frameworks (MOFs) as versatile nanofillers would notably broaden the scope of functionalities. However, synthesizing MOFs in the form of freestanding nanosheets has proved challenging. We present a bottom-up synthesis strategy for dispersible copper 1,4-benzenedicarboxylate MOF lamellae of micrometre lateral dimensions and nanometre thickness. Incorporating MOF nanosheets into polymer matrices endows the resultant composites with outstanding CO2 separation performance from CO2/CH4 gas mixtures, together with an unusual and highly desired increase in the separation selectivity with pressure. As revealed by tomographic focused ion beam scanning electron microscopy, the unique separation behaviour stems from a superior occupation of the membrane cross-section by the MOF nanosheets as compared with isotropic crystals, which improves the efficiency of molecular discrimination and eliminates unselective permeation pathways. This approach opens the door to ultrathin MOF-polymer composites for various applications.
    Nature Material 11/2014; DOI:10.1038/nmat4113 · 36.43 Impact Factor
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    ABSTRACT: In this work we prepared alpha-alumina hollow-fiber supported SSZ-13 and ZSM-5 membranes by hydrothermal secondary growth. The effects of support surface roughness and porosity, zeolite topology and zeolite film thickness on the thermal behavior of composite membranes during detemplation were investigated. The quality of prepared membranes was characterized by SEM, single and mixture gas permeation tests and adsorption-branch permporometry. The surface roughness of alpha-alumina hollow fiber supports is shown to strongly influence the thermal stability of zeolite films. SSZ-13 and ZSM-5 membranes prepared on supports with rough surface could be safely detemplated without formation of cracks by calcination (450-500 degrees C), whereas membranes prepared on very smooth surface supports were cracked under similar conditions. In such case ozonication at lower temperature was found to be effective to detemplate the membranes without formation of cracks.
    Microporous and Mesoporous Materials 10/2014; 197:268–277. DOI:10.1016/j.micromeso.2014.06.022 · 3.21 Impact Factor
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    ABSTRACT: High-silica (gel Si/Al = 100) SSZ-13 membranes were prepared by hydrothermal secondary growth on the surface of [small alpha]-alumina hollow fiber supports. The membranes were evaluated for their performance in the separation of CO2 from equimolar mixtures with CH4 or N2. The maximum CO2-CH4 and CO2-N2 separation selectivities were found to be 42 and 12 respectively, with a high CO2 permeance of 3.0 [times] 10-7 mol m2 s-1 Pa-1 at 293 K and total feed pressure of 0.6 MPa. At the low aluminum content, the prepared membranes contain a very low number of defects, as follows from their H2/SF6 ideal selectivity of over 500 in the 293-473 K temperature range. Due to their hydrophobicity, water in the feed mixture has only a small influence on the permeance at temperatures above 353 K. Water improves the CO2-N2 and CO2-CH4 selectivity, which is attributed to preferential blocking of the hydrophilic, non-zeolitic defect pores. The hydrothermal stability of the high-silica SSZ-13 membrane was evaluated by a lon
    Journal of Materials Chemistry A 08/2014; 2(32-32):13083-13092. DOI:10.1039/C4TA02744B · 7.44 Impact Factor

Publication Stats

3k Citations
671.38 Total Impact Points

Institutions

  • 2008–2015
    • Delft University of Technology
      • • Department of Chemical Engineering
      • • Catalysis Engineering Group
      Delft, South Holland, Netherlands
  • 2012–2014
    • University of Valencia
      • • Inorganic Chemistry
      • • Instituto de Ciencia Molecular (ICMol)
      Valenza, Valencia, Spain
  • 2013
    • Cambridge Eco
      Cambridge, England, United Kingdom
  • 2004–2008
    • University of Zaragoza
      • Department of Chemical Engineering and Environmental Technology
      Caesaraugusta, Aragon, Spain