Monodisperse Metal Clusters 10 Angstroms in Diameter in a Polymeric Host: The "Monomer as Solvent' Approach

Golden, J. H.; Deng, Haibin; DiSalvoa, Francis J.; Fréchet, Jean M. J.; Thompson, Patrick M.

doi:10.1126/science.268.5216.1463

Cited by 143 publications

(69 citation statements)

References 14 publications

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“…Indeed, the UV absorption spectra reported for ETS-10 samples have not shown any correlation between the band-gap energy and the length of the crystals along the [110] direction (L [110] ; Figure SI-1 and Table SI-1 in the Supporting Information). [16,[19][20][21] We now report an unprecedented and highly reliable method of synthesizing ETS-10 crystals of uniform sizes with average L [110] values of 0.3, 2, 5, 10, and 20 mm (denoted as E-0.3, E-2, E-5, E-10, and E-20, respectively).The starting materials for our synthesis of ETS-10 were sodium silicate (Na 2 SiO 3 , 35 % SiO 2 , 18% Na 2 O), [Ti(iPrO) 4 ], H 2 SO 4 , NaOH, and KF. First, concentrated H 2 SO 4 (4.5 g) was added to [Ti(iPrO) 4 ] (5.7 g), and then distilled deionized water (35 g) was added.…”

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“…These materials are widely used as catalysts, catalyst supports, adsorbents, ion-exchangers, and molecular sieves. ETS-10 (Na 2 TiSi 5 O 13 ) is a unique titanosilicate zeolite that contains regularly spaced 1D TiO 3 2À molecular wires (-O-Ti(O-) 4 -O-) with a diameter (d) of 0.67 nm. ETS-10 has two polymorphs: polymorth A (space group P4 1 or P4 3 , not shown) and polymorph B (space group C2/c).…”

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Length‐Dependent Band‐Gap Shift of TiO₃²⁻ Molecular Wires Embedded in Zeolite ETS‐10

Jeong¹,

Lee²,

Yoon³

2007

Angew Chem Int Ed

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Efforts have been directed at the synthesis and characterization of 1D quantum-confined semiconductor materials, since they have great potential to be widely used as building blocks for nanoscale electronic devices and other novel applications. [1][2][3][4][5][6][7][8][9][10][11] Of the 1D quantum-confined semiconductor materials, molecular wires are the thinnest. [1][2][3][4][5] However, examples of molecular wires are still very rare, and there is no method of synthesizing them in uniform diameters and controlled lengths. Accordingly, the relationship between the wire length (l) and the band-gap energy (E g ) in the quantum confinement region has not yet been determined for molecular wires, despite the fact that this relationship is crucial for the elucidation of the properties of the wires.Zeolites are crystalline inorganic materials having nanometer-sized pores and channels with uniform shapes and sizes. These materials are widely used as catalysts, catalyst supports, adsorbents, ion-exchangers, and molecular sieves. ETS-10 (Na 2 TiSi 5 O 13 ) is a unique titanosilicate zeolite that contains regularly spaced 1D TiO [12-15] Each TiO 3 2À wire is surrounded by nanoporous silica with a pore size of 8 5 2 . In highly crystalline ETS-10, the lengths of the TiO 3 2À molecular wires are greater than 25 nm. [16,17] Hence, it would be difficult to determine the l-E g relationship in the quantum confinement region unless the Bohr radius of the exciton in the molecular wire were to exceed 25 nm, since the quantum confinement effect (E g increases with decreasing l) is observed only in the region in which l is smaller than the exciton Bohr radius.The diameter of the TiO 3 2À molecular wire in ETS-10 is comparable to that of a single-wall carbon nanotube (d = 0.7 nm).[2] However, from the point of view of titanates, an important class of inorganic materials widely used in industry, the TiO 3 2À molecular wire is ultimately the thinnest wire. Furthermore, no other molecular wires or nanorods have been produced in the form of a superlattice embedded in a chemically inert large-band-gap medium. ETS-10 can be produced in large quantities at low cost by hydrothermal synthesis.[12-15] Therefore, ETS-10 provides an unprecedented opportunity to systematically study the l-E g relationship of the titanate molecular wire and to explore the applications of molecular-wire superlattices as advanced materials.Zecchina and co-workers, however, assumed that the band gap of the TiO 3 2À wire in ETS-10 is independent of the length of the wire when the length is greater than 25 nm. [16,17] This assumption has been widely accepted by the community during the last decade. [18,19] The verification of its validity has not been possible owing to the inability to synthesize highquality ETS-10 crystals of different sizes.[20] The standard approach to vary the size of a zeolite crystal is to vary the reaction time and temperature. Unfortunately, this standard approach has not worked for ETS-10. For instance, Southon and Howe demonstrated that, for a...

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Length‐Dependent Band‐Gap Shift of TiO₃²⁻ Molecular Wires Embedded in Zeolite ETS‐10

Jeong¹,

Lee²,

Yoon³

2007

Angew Chem Int Ed

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“…Furthermore, it is highly important that the monomer should act as both the ligand and solvent for the inorganic nanoparticles. [10] It has been reported that polar organic solvent molecules, such as N,N-dimethylformamide (DMF) and dimethyl sulfoxide (DMSO), co-ordinate to the surface of ZnS or CdS nanocrystallites and can effectively stabilize them. [11] Thus, it is expected that a monomer with a similar structure to DMF can be selected as both the solvent and ligand for the nanoparticles.…”

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A Facile Route to ZnS–Polymer Nanocomposite Optical Materials with High Nanophase Content via γ‐Ray Irradiation Initiated Bulk Polymerization

et al. 2006

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Transparent ZnS/polymer bulk nanocomposites with high particle contents are prepared via γ‐ray irradiation initiated polymerization. This strategy involves the design and tailoring of the surface of the nanoparticles and choice of the monomer as well as the selection of the polymerization route. The figure shows a TEM image of a bulk nanocomposite containing mercaptoethanol‐capped ZnS with a particle content of 20 wt %.

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“…[1][2][3][4][5][6][7] In heterogeneous catalysis, particle aggregation leads to reduction of effective surface area and degradation of catalytic performance. [1,[8][9][10] On semiconductor surfaces, film agglomeration may give rise to electric short, electron migration, and device degradation.…”

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First‐Principles Simulations of Conditions of Enhanced Adhesion Between Copper and TaN(111) Surfaces Using a Variety of Metallic Glue Materials

Han

Zhou

et al. 2009

Angew Chem Int Ed

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Monodisperse Metal Clusters 10 Angstroms in Diameter in a Polymeric Host: The "Monomer as Solvent' Approach

Cited by 143 publications

References 14 publications

Length‐Dependent Band‐Gap Shift of TiO₃²⁻ Molecular Wires Embedded in Zeolite ETS‐10

Length‐Dependent Band‐Gap Shift of TiO₃²⁻ Molecular Wires Embedded in Zeolite ETS‐10

A Facile Route to ZnS–Polymer Nanocomposite Optical Materials with High Nanophase Content via γ‐Ray Irradiation Initiated Bulk Polymerization

First‐Principles Simulations of Conditions of Enhanced Adhesion Between Copper and TaN(111) Surfaces Using a Variety of Metallic Glue Materials

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Monodisperse Metal Clusters 10 Angstroms in Diameter in a Polymeric Host: The "Monomer as Solvent' Approach

Cited by 143 publications

References 14 publications

Length‐Dependent Band‐Gap Shift of TiO32− Molecular Wires Embedded in Zeolite ETS‐10

Length‐Dependent Band‐Gap Shift of TiO32− Molecular Wires Embedded in Zeolite ETS‐10

A Facile Route to ZnS–Polymer Nanocomposite Optical Materials with High Nanophase Content via γ‐Ray Irradiation Initiated Bulk Polymerization

First‐Principles Simulations of Conditions of Enhanced Adhesion Between Copper and TaN(111) Surfaces Using a Variety of Metallic Glue Materials

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Length‐Dependent Band‐Gap Shift of TiO₃²⁻ Molecular Wires Embedded in Zeolite ETS‐10

Length‐Dependent Band‐Gap Shift of TiO₃²⁻ Molecular Wires Embedded in Zeolite ETS‐10