SENSORS AND ACTUATORS B-CHEMICAL
·
2016
·
IF 4.758
Xilin Bai,Suying Xu,Gaofei Hu,Leyu Wang
The exploration of feasible, reliable sensors for the selective and sensitive detection of nitroaromatic explosives is a critical issue nowadays as mandated by homeland security concerns. Our endeavor is to develop an instant on-site visual and ultra-sensitive photothermal nanosensor for 2,4,6 -trinitrotoluene (TNT) detection, which could be applied on a broad scale with high selectivity and sensitivity. The fundamental principle of our work is that TNT could effectively induce the aggregation of the cysteamine-stabilized gold nanoparticles (Au NPs) by forming the Meisenheimer complex, which further enhanced the surface plasmon resonance (SPR) properties and the photothermal effects of Au NPs. Other coexisting nitroaromatics have negligible influences on the photothermal responses. By means of the temperature enhancement and photothermal imaging technique, the presence of TNT could be readily recognized and visualized, indicating wide potential applications in analytical sensing.
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ANALYTICAL CHEMISTRY
·
2017
·
IF 6.32
Weijun Kong,Xiaoning Zhao,Qiuju Zhu,Lingfeng Gao,Hua Cui
Until now, despite the great success acquired in scientific research and commercial applications, magnetic beads (MBs) have been used for nothing more than a carrier in most cases in bioassays. In this work, highly chemiluminescent magnetic beads containing N-(4-aminobutyl)-N-ethyl isoluminol (ABEI) and Co2+ (Co2+/ABEI/MBs) were first synthesized via a facile strategy. ABEI and Co2+ were grafted onto the surface of carboxylated MBs by virtue of a carboxyl group and electrostatic interaction. The as-prepared Co2+/ABEI/MBs exhibited good paramagnetic properties, satisfactory stability, and intense chemiluminescence (CL) emission when reacted with H2O2, which was more than 150 times that of ABEI functionalized MBs. Furthermore, it was found that 2,4,6-trinitrotoluene (TNT) aptamer could attach to the surface of Co2+/ABEI/MBs via electrostatic interaction and coordination interaction between TNT aptamer and Co2+, leading to a decrease in CL intensity due to the catalytic site Co2+ being blocked by the aptamer. In the presence of TNT, TNT would bind strongly with TNT aptamer and detach from the surface of Co2+/ABEI/MBs, resulting in partial restoration of the CL signal. Accordingly, label-free aptasensor was developed for the determination of TNT in the range of 0.05–25 ng/mL with a detection limit of 17 pg/mL. This work demonstrates that Co2+/ABEI/MBs are easily connected with recognition biomolecules, which are not only magnetic carriers but also direct sensing interfaces with excellent CL activity. It provides a novel CL interface with a magnetic property which easily separates analytes from the sample matrix to construct label-free bioassays.
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Journal of Physical Chemistry C
·
2016
·
IF 4.509
Bocheng Qiu,Yuanxin Deng,Qiaoying Li,Bin Shen,Mingyang Xing,Jinlong Zhang
The rational design and controllable synthesis of TiO2 and noble metal composite photocatalysts represent an unprecedented challenge for developing the solar-driven reduction of nitrobenzene (NB) to aminobenzene (AB), owing to the recombination over the interface between the noble metals and TiO2, which is harmful to the conversion efficiency of NB to AB. Here, we design a unique ternary structure (the high separation of TiO2 and Pt nanoparticles on the surface of reduced graphene oxide (RGO)) through the sol–gel and microwave-assisted strategies. The substrate of RGO can be used as an “electric wire” to effectively transfer the photogenerated electrons from the isolated TiO2 nanocrystals to the isolated Pt nanoparticles, which greatly decreases the interface recombination between TiO2 and Pt and further improves the conversion efficiency of NB to AB under the solar light irradiation. We anticipate our research provides a new way to overcome the interface recombination on the binary photocatalysts in the photocatalytic reaction.
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JOURNAL OF CHROMATOGRAPHY A
·
2016
·
IF 3.926
Yunzhong Zheng,Meiling Qi,Ruonong Fu
This work presents the first example of utilization of graphitic carbon nitride (g-C 3 N 4 ) as stationary phase for capillary gas chromatographic (GC) separations. The statically coated g-C 3 N 4 column showed the column efficiencies of 3760 plates/m and weak polarity. Its resolving capability and retention behaviours were investigated by using the Grob test mixture, and mixtures of diverse types of analytes, and structural and positional isomers. The results showed superior separation performance of the g-C 3 N 4 stationary phase for some critical analytes and preferential retention for aromatic analytes. Specifically, it exhibited high-resolution capability for aromatic and aliphatic isomers such as methylnaphthalenes and dimethylnaphthalenes , phenanthrene and anthracene and alkane isomers. In addition, g-C 3 N 4 column showed excellent thermal stability up to 280 °C and good repeatability with relative standard deviation (RSD) values less than 0.09% for intra-day, below 0.23% for inter-day and in the range of 1.9–8.4% for between-column, respectively. The advantageous separation performance shows the potential of g-C 3 N 4 and related materials as stationary phase in GC and other separation technologies.
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CHEMICAL ENGINEERING SCIENCE
·
2017
·
IF 2.895
Rong Chen,Hao Feng,Xun Zhu,Qiang Liao,Dingding Ye,Jian Liu,Ming Liu,Gang Chen,Kun Wang
Visualization study on the interaction of the Taylor flow behavior and the catalytic activity in a gas-liquid-solid microreactor for nitrobenzene hydrogenation was performed under the long-term operation. The results showed that the gas slug length was first declined rapidly due to hydrogen consumption and then almost unchanged along the flow direction. After operating with a few hours, the variation of the gas slug length became obscure at the upstream due to the nanocatalyst deactivation but obvious at the downstream. Finally, the gas slug length was nearly unchanged. Corresponding to the long-term operation, the nitrobenzene conversion was first kept stable and then gradually declined, which well responded to the flow behaviors. Besides, effects of the inlet nitrobenzene concentration and flow rates on the flow behaviors were also explored. This work reveals the inherent interaction between the Taylor flow behavior and catalytic reaction under the long-term operation.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2016
·
IF 4.758
Yu Zhu Fan,Ying Zhang,Na Li,Shi Gang Liu,Ting Liu,Nian Bing Li,Hong Qun Luo
In this work, novel water-soluble and blue fluorescent carbon dots (C-dots) were synthesized using one-pot hydrothermal method with malonic acid and urea, and were then used as a label-free fluorescent probe for selective, sensitive, and rapid determination of picric acid (PA). The sizes of the as-prepared C-dots were mainly distributed in the range of 1.5–3.0 nm with an average diameter of 2.5 nm. Moreover, the C-dots displayed blue fluorescence with an emission peak at 395 nm (320 nm excitation), which also showed good stability and anti-photobleaching ability. Interestingly, the fluorescence of C-dots could be selectively quenched by PA within 10 s. Based on this phenomenon, a label-free fluorescence assay was proposed for specific determination of PA. The fluorescence intensity of probe showed a linear response to PA in the concentration range of 0.1 to 26.5 μM with a low detection limit of 51 nM (S/N = 3). Finally, the resultant fluorescent probe was successfully applied to the detection of PA in real water samples.
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TALANTA
·
2016
·
IF 4.035
Meng Li Liu,Bin Bin Chen,Ze Xi Liu,Cheng Zhi Huang
Though many methods of detecting 2,4,6-trinitrophenol (TNP) mainly have been developed recent years, quantification of TNP in environmental matrixes still faces up to great challenges because all the nitroaromatic explosives reveal highly similar chemical structure. In the present work, we have developed a selective and sensitive method for detection of TNP by amorphous photoluminescent carbon nanodots (CNDs), which are prepared through a simple hydrothermal route using spermine and m-phenylenediamine (MPD) as precursors. The as-prepared CNDs are found to show blue–green photoluminescence, excitation-wavelength independence, and excellent chemical and optical stability. Owing to the strong characteristic absorption of TNP at 356 nm ( ε =1.048×10 4 cm −1 M −1 ), which has a good spectral overlap with the excitation band of CNDs, the fluorescence intensity of CNDs at 490 nm is linearly quenched with the adding concentration of TNP in the range of 0.1–100 μM. The developing assay based on inner filter effect (IFE) mechanism for the detection of TNP is selective and convenient, showing that the as-prepared CNDs have applicable prospect in the concept of simplicity and specificity in analytical chemistry .
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ACS Applied Materials & Interfaces
·
2017
·
IF 7.504
Cuiling Zhang,Shiming Zhang,Yinghan Yan,Fei Xia,Anni Huang,Yuezhong Xian
A new fluorescent polyimide covalent organic framework (PI-COF) has been successfully synthesized through solvothermal route using tetra(4-aminophenyl) porphyrin and perylenetracarboxylic dianhydride, which possesses porous crystalline and excellent thermal stability (>500 °C). Furthermore, few-layered PI covalent organic nanosheets (PI-CONs) can be easily obtained from the fluorescent PI-COF through a facile liquid phase exfoliation approach, which were confirmed by atomic force microscopy and transmission electron microscopy analysis. It is interesting that the fluorescent intensity of PI-CONs is obviously enhanced relative to that of PI-COF. The PI-CONs have been successfully utilized as an efficient fluorescent probe for the highly sensitive and selective detection of 2,4,6-trinitrophenol (TNP). The mechanism might be attributed to the combination of electron transfer and inner filter effect based on DFT calculations and spectral overlap data. The system exhibits a good linear response toward TNP over the range from 0.5 to 10 μM with a detection limit of 0.25 μM.
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CHEMICAL ENGINEERING JOURNAL
·
2016
·
IF 5.31
Xiaori Fu,Xiaogang Gu,Shuguang Lu,Virender K. Sharma,Mark L. Brusseau,Yunfei Xue,Muhammad Danish,George Y. Fu,Zhaofu Qiu,Qian Sui
Complete degradation of benzene by the Fe(III)-activated sodium percarbonate (SPC) system is demonstrated. Removal of benzene at 1.0 mM was seen within 160 min, depending on the molar ratios of SPC to Fe(III). A mechanism of benzene degradation was elaborated by free-radical probe-compound tests, free-radical scavengers tests, electron paramagnetic resonance (EPR) analysis, and determination of Fe(II) and H 2 O 2 concentrations. The degradation products were also identified using gas chromatography-mass spectrometry method. The hydroxyl radical (HO ) was the leading species in charge of benzene degradation. The formation of HO was strongly dependent on the generation of the organic compound radical (R ) and superoxide anion radical (O 2 − ). Benzene degradation products included hydroxylated derivatives of benzene (phenol, hydroquinone, benzoquinone, and catechol) and aliphatic acids (oxalic and fumaric acids). The proposed degradation pathways are consistent with radical formation and identified products. The investigation of selected matrix constituents showed that the Cl − and HCO 3 − had inhibitory effects on benzene degradation. Natural organic matter (NOM) had accelerating influence in degrading benzene. The developed system was tested with groundwater samples and it was found that the Fe(III)-activated SPC has a great potential in effective remediation of benzene-contaminated groundwater while more further studies should be done for its practical application in the future because of the complex subsurface environment.
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RSC Advances
·
2017
·Vol. 7
·期 6
·3443-3449
·
IF 3.108
Ying Duan,Min Zheng,Dongmi Li,Dongsheng Deng,Cuicui Wu,Yanliang Yang
The Pd/SBA-15 catalyst was synthesised through the reduction of PdCl2 by the surface-bonded vinyl group on vinyl-functionalized SBA-15, which was prepared via co-polymerization. XRD and XPS characterization confirmed the successful reduction of Pd(II) to Pd(0). Pd/SBA-15 showed a narrow palladium particle-size distribution of about 5–6 nm in the TEM image. The Pd/SBA-15 catalyst was effective for the hydrogenation of aromatic nitro compounds with zero-order kinetics, and the TOF for the hydrogenation of nitrobenzene was 1124 h−1 at 313 K and 1 atm H2. A steric effect was observed for the substituted nitroarenes.
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MICROCHIMICA ACTA
·
2016
·Vol. 184
·期 1
·73-80
·
IF 4.831
Shi Jian-Jun,Meng Lei-Xia,Yang Ping
The authors describe an electrochemiluminescence (ECL) assay for the determination of 2,4,6-trinitrotoluene (TNT) in soil. It is based on the finding that graphene quantum dots (GQDs) strongly enhance the ECL of CdSe quantum dots (CdSe QDs), and ECL is strongly quenched by TNT. In order to assemble the GQDs and CdSe QDs, the latter were functionalized with carboxy groups and then coupled to amino-functionalized GQDs (afGQDs). The resulting CdSe-GQDs conjugation was placed as a thin film on a glassy carbon electrode (GCE). The modified electrode displays an about 8-fold enhanced ECL intensity compared to an GCE with CdSe QDs only, and the onset potential of the ECL reaction is positively shifted by 140 mV. In the presence of TNT, the ECL is quenched due to the formation of the TNT-amine complex. The decrease in ECL intensity is related to the logarithm of the TNT concentration in the range from 0.01 to 100 ppb, with a detection limit as low as 3 ppt. The results of TNT assays in (spiked) soil samples showed recoveries between 99.2 and 105.0 % and relative standard deviations between 3.0 and 8.2 %. This strategy offers a new perspective for developing ECL assays based on the use of semiconductor nanoparticles and graphene-based nanomaterials.
A electrochemiluminescence (ECL) assay was developed for the detection of 2,4,6-trinitrotoluene (TNT). The method utilizes a combination of CdSe and graphene quantum dots (GQDs), and a glassy carbon electrode modified with poly(diallyldimethylammonium chloride)-protected graphene. The assay is simple and displays acceptable reproducibility.
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APPLIED SURFACE SCIENCE
·
2016
·
IF 3.15
Yijin Shu,Sina He,Lifang Xie,Hang Cheong Chan,Xiang Yu,Lichun Yang,Qingsheng Gao
The hydrogenation of nitroarenes to value-added aromatic amines requires active and selective catalysts. Due to the good efficiency, economic cost and high earth-abundance, Ni-based nanostructures emerge as the promising catalysts, which are however limited by the poor dispersion and unsatisfied durability. Herein, Mo 2 C nanowires was introduced as a versatile support towards the highly dispersive Ni owing to the strong metal-support interactions on carbide surface, accomplishing the high activity in the hydrogenation of 3-nitrobenzoic acid, 4-nitrobenzoic acid and nitrobenzene. However, the presence of water that promoted the selective hydrogenation unfortunately deactivated Ni species. An effective carbon coating was further introduced to remarkably enhance the stability, protecting active Ni from corrosive H + and H 2 O. This work elucidates a feasible way towards efficient and stable catalysts by the introduction of both carbide supports and carbon coating, shedding some light on the development of high-performance catalysts.
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