Cooperative Formation of Inorganic-Organic Interfaces in the Synthesis of Silicate Mesostructures

Monnier, Alain; Schüth, Ferdi; Huo, Quan; Kumar, Dhananjay; Margolese, D.; Maxwell, Robert S.; Stucky, Galen D.; Krishnamurty, M.; Petroff, P. M.; Firouzi, Ali; Janicke, Michael T.; Chmelka, Bradley F.

doi:10.1126/science.261.5126.1299

Cited by 1,536 publications

(1,262 citation statements)

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“…Long-chain alkyl-quaternary ammonium molecules are universally used to synthesize mesoporous silica materials through the self-assembled liquid crystal templating route [20][21][22] . Recently, Ryoo and coworkers 8 succeeded in synthesizing polycrystalline mesostructured MFI (zeolite framework code by International Zeolite Association) zeolite using designed bifunctional surfactants 7,8,23 , in which the connection of the head groups of the multiple quaternary ammoniums to hydrophobic alkyl chains is the indispensable factor for the effective structure-directing agent to simultaneously form MFI zeolite and a mesoscale micellar structure.…”

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confidence: 99%

π–π interaction of aromatic groups in amphiphilic molecules directing for single-crystalline mesostructured zeolite nanosheets

et al. 2014

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One of the challenges in material science has been to prepare macro-or mesoporous zeolite. Although examples of their synthesis exist, there is a need for a facile yet versatile approach to such hierarchical structures. Here we report a concept for designing a single quaternary ammonium head amphiphilic template with strong ordered self-assembling ability through p-p stacking in hydrophobic side, which stabilizes the mesostructure to form singlecrystalline mesostructured zeolite nanosheets. The concept is demonstrated for the formation of a new type of MFI (zeolite framework code by International Zeolite Association) nanosheets joined with a 90°rotational boundary, which results in a mesoporous zeolite with highly specific surface area even after calcination. Low binding energies for this selfassembling system are supported by a theoretical analysis. A geometrical matching between the arrangement of aromatic groups and the zeolitic framework is speculated for the formation of single-crystalline MFI nanosheets.

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confidence: 99%

π–π interaction of aromatic groups in amphiphilic molecules directing for single-crystalline mesostructured zeolite nanosheets

et al. 2014

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“…With the volatilization of ethanol and the sluggish hydrolysis of the titanium isopropoxide precursor, the condensation of hydrolyzed TiO 2 precursor occurs accompanied by the decrease of the charge density of TiO 2 at the interface. This process is caused by the increase of the interfacial curvature of the surfactant matrix,37 leading to the formation of hybrid system surfactant‐TiO 2 nanoparticles (Figure 2b). The further condensation of aligned nanoparticles leads to a 3D superstructure of surfactant nanowires (Figure 2c).…”

Section: Resultsmentioning

confidence: 99%

Phases Hybriding and Hierarchical Structuring of Mesoporous TiO₂ Nanowire Bundles for High‐Rate and High‐Capacity Lithium Batteries

et al. 2015

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A hierarchical mesoporous TiO2 nanowire bundles (HM‐TiO2‐NB) superstructure with amorphous surface and straight nanochannels has been designed and synthesized through a templating method at a low temperature under acidic and wet conditions. The obtained HM‐TiO2‐NB superstructure demonstrates high reversible capacity, excellent cycling performance, and superior rate capability. Most importantly, a self‐improving phenomenon of Li+ insertion capability based on two simultaneous effects, the crystallization of amorphous TiO2 and the formation of Li2Ti2O4 crystalline dots on the surface of TiO2 nanowires, has been clearly revealed through ex situ transmission electron microcopy (TEM), high‐resolution transmission electron microscopy (HRTEM), X‐ray diffraction (XRD), Raman, and X‐ray photoelectron spectroscopy (XPS) techniques during the Li+ insertion process. When discharged for 100 cycles at 1 C, the HM‐TiO2‐NB exhibits a reversible capacity of 174 mA h g−1. Even when the current density is increased to 50 C, a very stable and extraordinarily high reversible capacity of 96 mA h g−1 can be delivered after 50 cycles. Compared to the previously reported results, both the lithium storage capacity and rate capability of our pure TiO2 material without any additives are among the highest values reported. The advanced electrochemical performance of these HM‐TiO2‐NB superstructures is the result of the synergistic effect of hybriding of amorphous and crystalline (anatase/rutile) phases and hierarchically structuring of TiO2 nanowire bundles. Our material could be a very promising anodic material for lithium‐ion batteries.

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“…[10][11][12][13]28 Moreover, strong acidities can induce intensive protonation of the PEO corona of triblock copolymer micelle, 13,37 which offers strong electrostatic and hydrogen bonding interactions with silica species, facilitating the assembly of silica precursors around the micelle template. [38][39][40][41][42][43] Under weak acidities actually only a very small amount of silica precipitated if hydrochloric acid or nitric acid was used as the acid source due to limited silica condensation reactions. However, it has been shown in this work that some largemolecule polyhydroxy carboxylic acids can also lead to highly ordered mesostructure even under moderately weak acidic conditions (pH 1.5-2.0).…”

Section: Effect Of Acidity and Acid Source On Mesostructurementioning

confidence: 99%

Promoted and Controllable Self-Assembly of Hydrolyzed Siloxane and Triblock Copolymer under Organic Polyhydroxy Acids

et al. 2009

Ind. Eng. Chem. Res.

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Large-molecule polyhydroxy organic acids such as tartaric acid and citric acid were found to significantly promote the cooperative formation of mesoporous silica SBA-15 with homogeneous well-defined hexagonal mesostructure under much weaker acidities without addition of volatile inorganic acids; therefore a novel environmental benign route for SBA-15 synthesis was developed. It is suggested that the polar groups of polyhydroxy acid molecules can greatly strengthen the assembly interactions between the silica species and the triblock copolymer by providing hydrogen bonding. More interestingly, by controlling the strength of hydrogen-bonding interaction that is dependent on the concentration of carboxylic acids, the particle size of the product can be tailored. The silica with small particle size synthesized with a small amount of polyhydroxy acids was favorable support of palladium catalyst for the complete oxidation of volatile organic compounds in atmosphere, probably due to the facilitated diffusion of reactant molecules.

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Cooperative Formation of Inorganic-Organic Interfaces in the Synthesis of Silicate Mesostructures

Abstract: I1I. SUPPLENIEN TARY NO &ES

Cited by 1,536 publications

References 9 publications

π–π interaction of aromatic groups in amphiphilic molecules directing for single-crystalline mesostructured zeolite nanosheets

π–π interaction of aromatic groups in amphiphilic molecules directing for single-crystalline mesostructured zeolite nanosheets

Phases Hybriding and Hierarchical Structuring of Mesoporous TiO₂ Nanowire Bundles for High‐Rate and High‐Capacity Lithium Batteries

Promoted and Controllable Self-Assembly of Hydrolyzed Siloxane and Triblock Copolymer under Organic Polyhydroxy Acids

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Cooperative Formation of Inorganic-Organic Interfaces in the Synthesis of Silicate Mesostructures

Abstract: I1I. SUPPLENIEN TARY NO &ES

Cited by 1,536 publications

References 9 publications

π–π interaction of aromatic groups in amphiphilic molecules directing for single-crystalline mesostructured zeolite nanosheets

π–π interaction of aromatic groups in amphiphilic molecules directing for single-crystalline mesostructured zeolite nanosheets

Phases Hybriding and Hierarchical Structuring of Mesoporous TiO2 Nanowire Bundles for High‐Rate and High‐Capacity Lithium Batteries

Promoted and Controllable Self-Assembly of Hydrolyzed Siloxane and Triblock Copolymer under Organic Polyhydroxy Acids

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Phases Hybriding and Hierarchical Structuring of Mesoporous TiO₂ Nanowire Bundles for High‐Rate and High‐Capacity Lithium Batteries