Ionic nanoparticle networks: development and perspectives in the landscape of ionic liquid based materials

Néouze, Marie-Alexandra; Kronstein, Martin; Tielens, Frederik

doi:10.1039/c4cc02419b

Cited by 22 publications

(17 citation statements)

References 75 publications

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“…This phenomenon implies the formation of cationic networks from covalent POSS molecules, considering that the thermal stability for ionic covalent bonds is often inferior to that of covalent linkages. Similar results have been observed in such previous cationic materials as IL-like silica networks 33 and positively charged porous aromatic frameworks 30 . Figure 3b compares the FT-IR spectra of ClMePOSS and PCIF-1(M4).…”

Section: Resultssupporting

confidence: 89%

“…In contrast, the ionic sites within charged networks and the resultant strong electrostatic fields are more accommodable for ionic active species and guest molecules 24 . Therefore, porous ionic solid materials are becoming hot topics in areas of porous crystals 25 , MOFs 26 27 28 29 , polymers 30 31 32 , nanoparticle networks 33 , PMOs with ionic liquids framework 34 and mesoporous ionic liquid-polyoxometalate (IL-POM) hybrids 35 36 . Such rapid emergence of ionic solid materials is thanks to their fascinating ion-exchange properties and solid-state ionic nanospaces, enabling their applications in heterogeneous catalysis 27 28 34 35 36 , gas storage and separation 26 30 32 , and ionic pollutants adsorption 29 .…”

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confidence: 99%

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Construction of porous cationic frameworks by crosslinking polyhedral oligomeric silsesquioxane units with N-heterocyclic linkers

Chen

Zhou

Wang

et al. 2015

Sci Rep

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In fields of materials science and chemistry, ionic-type porous materials attract increasing attention due to significant ion-exchanging capacity for accessing diversified applications. Facing the fact that porous cationic materials with robust and stable frameworks are very rare, novel tactics that can create new type members are highly desired. Here we report the first family of polyhedral oligomeric silsesquioxane (POSS) based porous cationic frameworks (PCIF-n) with enriched poly(ionic liquid)-like cationic structures, tunable mesoporosities, high surface areas (up to 1,025 m2 g−1) and large pore volumes (up to 0.90 cm3 g−1). Our strategy is designing the new rigid POSS unit of octakis(chloromethyl)silsesquioxane and reacting it with the rigid N-heterocyclic cross-linkers (typically 4,4′-bipyridine) for preparing the desired porous cationic frameworks. The PCIF-n materials possess large surface area, hydrophobic and special anion-exchanging property, and thus are used as the supports for loading guest species PMo10V2O405−; the resultant hybrid behaves as an efficient heterogeneous catalyst for aerobic oxidation of benzene and H2O2-mediated oxidation of cyclohexane.

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Section: Resultssupporting

confidence: 89%

mentioning

confidence: 99%

Construction of porous cationic frameworks by crosslinking polyhedral oligomeric silsesquioxane units with N-heterocyclic linkers

Chen

Zhou

Wang

et al. 2015

Sci Rep

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“…In particular, models with 5.8, 5.8 with water inside the pores, 4.8, 3.6, 2.3 and 1.7 OH nm -2 have been developed. We have shown that our models represent very well the surface of real MCM-41 silica, as evidenced by the comparison with available experimental data, and are improved compared with earlier published models [70][71][72][73][74] . The simulated IR spectra additionally confirms that our models are realistic.…”

Section: Resultssupporting

confidence: 68%

Hydration in silica based mesoporous materials: a DFT model

Gierada

Petit

Handzlik

et al. 2016

Phys. Chem. Chem. Phys.

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The MCM-41 material is very commonly used as a support for catalysts. However, theoretical investigations are significantly limited due to the lack of appropriate models that well and accurately describe the real material and enable effective computation at the same time. In this work, our aim is to obtain calculable models at the DFT level of MCM-41 which are as close as possible to the real material. In particular the hydration degree has been investigated, and we present and characterize here for the first time a model for the MCM-41 unit cell filled with explicit solvent water molecules. This is particularly important, because the models developed here are aimed to be further applied in theoretical ab initio/DFT studies of adsorption or as a support for modelling active sites in catalysts.

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“…Moreover, these ILhybrid materials display solid-membrane like properties 19 and their properties have been investigated in detail. [20][21][22][23] The sputtering method is quite useful since the size of Pd-NPs can be easily controlled by the current discharge and metal concentration by the time of sputtering. [24][25][26] Moreover, in this method no by-products are generated and only Pd and the support are present in the catalytic material thus allowing a more accurate analysis of the interface Pd-support.…”

Section: Introductionmentioning

confidence: 99%

Catalytically Active Membranelike Devices: Ionic Liquid Hybrid Organosilicas Decorated with Palladium Nanoparticles

et al. 2016

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Ionic liquid (IL)-hybrid organosilicas based on 1-n-butyl-3-(3-trimethoxysilylpropyl)-imidazolium cations associated with hydrophilic and hydrophobic anions decorated with well dispersed and similar sized (1.8-2.1 nm) Pd nanoparticles (PdNPs) are amongst the most active and selective catalysts for the partial hydrogenation of conjugated dienes to monoenes. The location of the sputter-imprinted Pd-NPs on different supports, as determined by RBS and HS-LEIS analysis, is modulated by the strength of the contact ion pair formed between the imidazolium cation and the anion, rather than the IL-hybrid organosilica pore size and surface area. In contrast, the pore diameter and surface area of the hybrid supports display a direct correlation with the anion hydrophobicity. XPS analysis showed that the Pd(0) surface component decreases with increasing ionic bond strength between the imidazolium cation and the anions (contact ion pair). The finding is corroborated by changes in the coordination number associated with the Pd-Pd scattering in EXAFS measurements. Hence, the interaction of the IL with the metal surface is found to occur via IL contact pairs (or aggregates). The observed selectivities of ≥99% to monoenes at full diene conversion indicate that the selectivity is intrinsic to the electron deficient Pd-metallic surfaces in this "restricted" ionic environment. This suggests that ILhybrid organosilica/Pd-NPs under multiphase conditions ("dynamic asymmetric mixture") operate akin to catalytically active membranes, i.e. far from the thermodynamic equilibrium. Detailed kinetic investigations show that the reaction rate is zero-order with respect to hydrogen and dependent on the fraction of catalyst surfaces covered by either the substrate and/or the product. The reaction proceeds via rapid inclusion and sorption of the diene to the IL/Pd metal surface saturated with H species. This is followed by reversible hydride migration to generate a π-allyl intermediate. The reductive elimination of this intermediate, the formal ratedetermining step (RDS), generates the alkene that is rapidly expelled from the IL phase to the organic phase.

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Ionic nanoparticle networks: development and perspectives in the landscape of ionic liquid based materials

Cited by 22 publications

References 75 publications

Construction of porous cationic frameworks by crosslinking polyhedral oligomeric silsesquioxane units with N-heterocyclic linkers

Construction of porous cationic frameworks by crosslinking polyhedral oligomeric silsesquioxane units with N-heterocyclic linkers

Hydration in silica based mesoporous materials: a DFT model

Catalytically Active Membranelike Devices: Ionic Liquid Hybrid Organosilicas Decorated with Palladium Nanoparticles

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