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1.
Sci Rep ; 5: 13126, 2015 Aug 18.
Article in English | MEDLINE | ID: mdl-26283473

ABSTRACT

It is extremely important to understand the properties of supported metal nanoparticles at the atomic scale. In particular, visualizing the interaction between nanoparticle and support, as well as the strain distribution within the particle is highly desirable. Lattice strain can affect catalytic activity, and therefore strain engineering via e.g. synthesis of core-shell nanoparticles or compositional segregation has been intensively studied. However, substrate-induced lattice strain has yet to be visualized directly. In this study, platinum nanoparticles decorated on graphitized carbon or tin oxide supports are investigated using spherical aberration-corrected scanning transmission electron microscopy (Cs-corrected STEM) coupled with geometric phase analysis (GPA). Local changes in lattice parameter are observed within the Pt nanoparticles and the strain distribution is mapped. This reveals that Pt nanoparticles on SnO2 are more highly strained than on carbon, especially in the region of atomic steps in the SnO2 lattice. These substrate-induced strain effects are also reproduced in density functional theory simulations, and related to catalytic oxygen reduction reaction activity. This study suggests that tailoring the catalytic activity of electrocatalyst nanoparticles via the strong metal-support interaction (SMSI) is possible. This technique also provides an experimental platform for improving our understanding of nanoparticles at the atomic scale.

2.
Sci Rep ; 5: 11807, 2015 Jul 02.
Article in English | MEDLINE | ID: mdl-26133654

ABSTRACT

Graphene oxide (GO) is hydrophilic and swells significantly when in contact with water. Here, we investigate the change in thickness of multilayer graphene oxide membranes due to intercalation of water, via humidity-controlled observation in an environmental scanning electron microscope (ESEM). The thickness increases reproducibly with increasing relative humidity. Electron energy loss spectroscopy (EELS) reveals the existence of water ice under cryogenic conditions, even in high vacuum environment. Additionally, we demonstrate that freezing then thawing water trapped in the multilayer graphene oxide membrane leads to the opening up of micron-scale inter-lamellar voids due to the expansion of ice crystals.

3.
Microscopy (Oxf) ; 64(5): 335-40, 2015 Oct.
Article in English | MEDLINE | ID: mdl-26115957

ABSTRACT

The dislocation shielding field at a crack tip was experimentally proven at the atomic scale by measuring the local strain in front of the crack tip using high-resolution transmission electron microscopy (HRTEM) and geometric phase analysis (GPA). Single crystalline (110) silicon wafers were employed. Cracks were introduced using a Vickers indenter at room temperature. The crack tip region was observed using HRTEM followed by strain measurements using GPA. The measured strain field at the crack tip was compressive owing to dislocation shielding, which is in good agreement with the strain field calculated from elastic theory.

4.
Angew Chem Int Ed Engl ; 53(48): 13078-82, 2014 Nov 24.
Article in English | MEDLINE | ID: mdl-25303774

ABSTRACT

To fully understand the fundamental properties of light-energy-converting materials, it is important to determine the local atomic configuration of photofunctional centers. In this study, direct imaging of one- and two-Tb-atom emission centers in a two-dimensional Tb-doped Ca2Ta3O10 nanocrystal was carried. The emission centers were located at the Ca sites in the perovskite structure, and no concentration-based quenching was observed even when the emission centers were in close proximity to each other. The relative photoluminescence efficiency for green emission of the nanosheet suspension was 38.1%. Furthermore, the Tb-doped Ca2Ta3O10 nanocrystal deposited co-catalyst showed high photocatalytic activity for hydrogen production from water (quantum efficiency: 71% at 270 nm). Tb(3+) dopants in the two-dimensional crystal might have the potential to stabilize the charge separation state.

5.
Chem Commun (Camb) ; 50(83): 12515-8, 2014 Oct 25.
Article in English | MEDLINE | ID: mdl-25189284

ABSTRACT

Water splitting activity of a GaN:ZnO photocatalyst was improved by meso-hexakis(pentafluorophenyl) [26]hexaphyrin (3). The hexaphyrin (3) assisted the water splitting reaction over the GaN:ZnO photocatalyst by using visible light energy around 600 nm.

6.
ACS Appl Mater Interfaces ; 5(21): 11080-6, 2013 Nov 13.
Article in English | MEDLINE | ID: mdl-24143949

ABSTRACT

Crystalline mesoporous Ta2O5 has been successfully synthesized by a one-pot route using P-123 as the structure directing agent (SDA). A series of crystalline mesoporous Ta2O5 samples has been prepared by changing the calcination temperature. The surface area decreased and the pore size increased with the increasing calcination temperature, which were the results of crystallite growth. At the same time, the pore volume was well maintained, which means limited shrinkage during the calcination of elevated temperature. The porous structure and crystal structure of as-synthesized mesoporous Ta2O5 were characterized by XRD, TG-DTA, SEM, TEM, and N2 sorption techniques. The photocatalytic activity of the as-synthesized mesoporous Ta2O5 with the cocatalyst NiOx for overall water splitting under ultraviolet (UV) light irradiation was systematically evaluated. The photocatalytic activity of crystalline mesoporous Ta2O5 showed about 3 times that of commercial Ta2O5 powder and 22 times that of amorphous mesoporous Ta2O5.

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