Showing papers by "Bianhua Liu published in 2008"

Amine-capped ZnS-Mn2+ nanocrystals for fluorescence detection of trace TNT explosive.

Abstract: Mn2+-doped ZnS nanocrystals with an amine-capping layer have been synthesized and used for the fluorescence detection of ultratrace 2,4,6-trinitrotoluene (TNT) by quenching the strong orange Mn2+ photoluminescence. The organic amine-capped nanocrystals can bind TNT species from solution and atmosphere by the acid−base pairing interaction between electron-rich amino ligands and electron-deficient aromatic rings. The resultant TNT anions bound onto the amino monolayer can efficiently quench the Mn2+ photoluminescence through the electron transfer from the conductive band of ZnS to the lowest unoccupied molecular orbital (LUMO) of TNT anions. The amino ligands provide an amplified response to the binding events of nitroaromatic compounds by the 2- to ∼5-fold increase in quenching constants. Moreover, a large difference in quenching efficiency was observed for different types of nitroaromatic analytes, dependent on the affinity of nitro analytes to the amino monolayer and their electron-accepting abilities. T...

Resonance Energy Transfer-Amplifying Fluorescence Quenching at the Surface of Silica Nanoparticles toward Ultrasensitive Detection of TNT

Abstract: This paper reports a resonance energy transfer-amplifying fluorescence quenching at the surface of silica nanoparticles for the ultrasensitive detection of 2,4,6-trinitrotoluene (TNT) in solution and vapor environments. Fluorescence dye and organic amine were covalently modified onto the surface of silica nanoparticles to form a hybrid monolayer of dye fluorophores and amine ligands. The fluorescent silica particles can specifically bind TNT species by the charge-transfer complexing interaction between electron-rich amine ligands and electron-deficient aromatic rings. The resultant TNT−amine complexes bound at the silica surface can strongly suppress the fluorescence emission of the chosen dye by the fluorescence resonance energy transfer (FRET) from dye donor to the irradiative TNT−amine acceptor through intermolecular polar−polar interactions at spatial proximity. The quenching efficiency of the hybrid nanoparticles with TNT is greatly amplified by at least 10-fold that of the corresponding pure dye. Th...

Molecular imprinting at walls of silica nanotubes for TNT recognition.

Abstract: This paper reports the molecular imprinting at the walls of highly uniform silica nanotubes for the recognition of 2,4,6-trinitrotoluene (TNT). It has been demonstrated that TNT templates were efficiently imprinted into the matrix of silica through the strong acid−base pairing interaction between TNT and 3-aminopropyltriethoxysilane (APTS). TNT-imprinted silica nanotubes were synthesized by the gelation reaction between APTS and tetraethylorthosilicate (TEOS), selectively occurring at the porous walls of APTS-modified alumina membranes. The removal of the original TNT templates leaves the imprinted cavities with covalently anchored amine groups at the cavity walls. A high density of recognition sites with molecular selectivity to the TNT analyte was created at the wall of silica nanotubes. Furthermore, most of these recognition sites are situated at the inside and outside surfaces of tubular walls and in the proximity of the two surfaces due to the ultrathin wall thickness of only 15 nm, providing a bette...

Imprinting of Molecular Recognition Sites on Nanostructures and Its Applications in Chemosensors.

Abstract: Biological receptors including enzymes, antibodies and active proteins have been widely used as the detection platform in a variety of chemo/biosensors and bioassays. However, the use of artificial host materials in chemical/biological detections has become increasingly attractive, because the synthetic recognition systems such as molecularly imprinted polymers (MIPs) usually have lower costs, higher physical/chemical stability, easier preparation and better engineering possibility than biological receptors. Molecular imprinting is one of the most efficient strategies to offer a synthetic route to artificial recognition systems by a template polymerization technique, and has attracted considerable efforts due to its importance in separation, chemo/biosensors, catalysis and biomedicine. Despite the fact that MIPs have molecular recognition ability similar to that of biological receptors, traditional bulky MIP materials usually exhibit a low binding capacity and slow binding kinetics to the target species. Moreover, the MIP materials lack the signal-output response to analyte binding events when used as recognition elements in chemo/biosensors or bioassays. Recently, various explorations have demonstrated that molecular imprinting nanotechniques may provide a potential solution to these difficulties. Many successful examples of the development of MIP-based sensors have also been reported during the past several decades. This review will begin with a brief introduction to the principle of molecular imprinting nanotechnology, and then mainly summarize various synthesis methodologies and recognition properties of MIP nanomaterials and their applications in MIP-based chemosensors. Finally, the future perspectives and efforts in MIP nanomaterials and MIP-based sensors are given.

Oriented Vaterite CaCO3 Tablet-Like Arrays Mineralized at Air/Water Interface through Cooperative Regulation of Polypeptide and Double Hydrophilic Block Copolymer

Abstract: Highly oriented vaterite CaCO 3 tablet-like arrays were formed at the air/water interface through the cooperative mineralization regulated by polypeptide and double hydrophilic block copolymer under ambient conditions. The nearly parallel arrangement of CaCO 3 vaterite tablets at the air/water interface shows the remarkable resemblance to the morphology of nacreous layers. The poly(aspartic acid) (PASP) with high molecular weight (M w = 11 000) and low solubility in water promoted the formation of vaterite tablets at the air/water interface, and stabilized the vaterite tablets by aggregation at the air/water interface and adsorption at the surface of vaterite tablets. Meanwhile, the highly hydrophilic poly(ethylene glycol)-block-poly(methacrylic acid) (PEG-b-PMAA) played an important role in regulating the arrangement and orientation of vaterite CaCO 3 tablets, leading to the oriented tablet-like arrays at the air/water interface. Detailed experiments revealed that hydrophilic PEG-b-PMAA alone did not produce any form of CaCO 3 crystals at the air/water interface, but could induce the formation of calcite CaCO 3 particles in the water phase. However, high molecular weight PASP alone led to the formation of disk-like vaterite particles composed of helically aggregated nanoplates at the air/water interface, suggesting the regulating role of PEG-b-PMAA in the growth of vaterite tablet arrays. These results reported here provide a better understanding of the growth mechanism of nacreous layers and shells in nature.