A new type of sol-gel organic-inorganic hybrid material was developed and used for the production of biosensors. This material is composed of silica sol and a grafting copolymer of poly(vinyl alcohol) with 4-vinylpyridine. It prevents the cracking of conventional sol-gel-derived glasses and eliminates the swelling of the hydrogel. The optimum composition of the hybrid material was first examined, and then glucose oxidase was immobilized in this matrix to demonstrate its application. The characteristics of the biosensor were studied by cyclic voltammetry and chronoamperometry. The biosensor exhibited a series of good properties: high sensitivity (600 nA mmol-1 L-1), short response time (11 s) and remarkable long-term stability in storage (at least 5 months). In addition, the characteristics of the second-generation biosensor with the use of tetrathiafulvalene as a mediator were discussed.
Nanostructured Ag nanoparticles (Ag-NPs)/nanoporous ZnO micrometer-rods (n-ZnO MRs) have been synthesized by a two-step method. The n-ZnO MRs was initially prepared by solvothermal-assisted heat treatment. The rods had the diameter ranged from 90 to 150 nm and length between 0.5 and 3 μm. They were found to be porous and were composited of ZnO nanopartiles with size of about 20 nm. In the second stage, Ag-NPs with a diameter of 20-50 nm were anchored onto the surface of the as-prepared n-ZnO MRs by a photoreduction method. The Ag-NPs/n-ZnO MRs were evaluated for their ability to degrade methylene blue (MB) solution under visible to ultraviolet (UV) light irradiation. The rate of degradation of the as-prepared Ag-NPs/n-ZnO MRs was more than twice and nearly 5.6 times faster than that of using bare n-ZnO MRs under the UV and solar light irradiation, respectively. The formation of Schottky barriers in the regions between the Ag-NPs and n-ZnO MRs had improved the charge separation and consequently enhanced the efficiency of the degradation process. Moreover, the as-prepared hybrid structure exhibited high photostability, and 98% of degradation efficiency could be maintained even after being used five times. This endurance was attributed to the retardation of photocorrosion of ZnO as a result of the low concentration of surface defects in the as-prepared n-ZnO MRs. It also minimized the surface defects of the as-prepared n-ZnO MRs and consequently further inhibited the photocorrosion of ZnO when the deposited Ag-NPs were much more inclined to combine with the chemisorbed oxygen.
High yield production of micro/nanostructured nanoparticulate TiO2 microspheres (NTMs) via a facile microwave-assisted hydrothermal approach was investigated. The rapid and uniform microwave heating could reduce the reaction time to 30 min, an order of magnitude shorter than that of conventional hydrothermal methods. The characterization data confirmed that the resultant NTMs were highly uniform in size, having an average diameter of ∼0.5 μm. The obtained NTMs were found to be constructed by well-crystallized anatase phase nanoparticles ranging from 5 to 10 nm that can be readily controlled by the microwave radiation temperature. Nitrogen sorption isotherm analysis revealed that the obtained NTMs possessed abundant mesoporous structures with a high specific surface area of 124 m(2) g(-1). An in situ self-aggregation formation process under controllable pH in presence of urea was proposed. The results obtained from the application of NTMs for simultaneous photocatalytic decontamination of Cr(VI) and methyl orange (MO) demonstrated a strong synergistic effect that dramatically enhanced both Cr(VI) reduction and MO oxidation removal efficiencies. This work not only enriched the synthesis methods of the micro/nanostructured TiO2, but also provided a new means to improve the photocatalytic efficiency via structural-induced synergistic effect, applicable to the other catalysis systems.
A versatile method was developed to synthesize nickel silicate, silica, and silica-nickel composite porous hollow spheres by using silica spheres as templates. In the preparation, silica spheres were treated with a mixture of NiSO(4)·6H(2)O and NH(3)·H(2)O. The nickel-based ingredient reacted with the silica to form a shell while the alkaline solution could remove the silica core, thus forming the nickel silicate hollow spheres. After these spheres were further treated with hydrogen in reduction or with HCl in etching, they became silica-nickel hollow spheres or silica hollow spheres, respectively. The sizes of these hollow spheres depended on the concentration of the precursor. Our investigation also found that their surface properties or magnetic properties could be tailored by adjusting the fabrication parameters.
A novel poly(vinyl alcohol) grafting 4-vinylpyridine self-gelatinizable copolymer was adapted to immobilize glucose oxidase. The reduction of hydrogen peroxide (H2O2) was detected at a Prussian Blue (PB) modified graphite electrode. A stable and sensitive glucose amperometric biosensor is described. The copolymer is a good biocompatible polymer in which the glucose oxidase retains high activity. Moreover, the copolymer can adhere firmly to the inorganic PB membrane. The sensor showed an apparent Michaelis-Menten constant of 18 +/- 0.2 mM and a maximum current density of 1.14 microA cm-2 mM-1. The linear range is from 5 microM to 4.5 mM glucose and the detection limit is 0.5 microM glucose. The catalytic efficiency of PB for the reduction of H2O2 is higher than that for the oxidation of H2O2. Glucose concentrations in serum samples from healthy persons and diabetic patients were determined using the sensor. The results compared well with those provided by the hospital using a spectroscopy method.
Reliable prediction
of the properties of nanosystems with radical
nature has been tremendously challenging for common computational
approaches. Aiming to overcome this, we employ thermally-assisted-occupation
density functional theory (TAO-DFT) to investigate various electronic
properties (e.g., singlet–triplet energy gaps, vertical ionization
potentials, vertical electron affinities, fundamental gaps, symmetrized
von Neumann entropy, active orbital occupation numbers, and visualization
of active orbitals) associated with a series of triangle-shaped graphene
nanoflakes with
n
fused benzene rings at each side
(denoted as
n
-triangulenes), which can be extended
from triangulene. According to our TAO-DFT results, the ground states
of
n
-triangulenes are singlets for all the values
of
n
studied (
n
= 3, 5, 7, 9, ...,
and 21). Moreover, the larger the values of
n
, the
more significant the polyradical nature of
n
-triangulenes.
There are approximately (
n
– 1) unpaired electrons
for the ground state of
n
-triangulene. The increasing
polyradical nature of the larger
n
-triangulenes should
be closely related to the fact that the active orbitals tend to be
mainly concentrated at the periphery of
n
-triangulenes,
apparently increasing with the molecular size.
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