Environmental Science-Nano
·
2016
·Vol. 4
·期 2
·493-502
·
IF 5.896
Jialuo Yu,Xiaoyan Wang,Qi Kang,Jinhua Li,Dazhong Shen,Lingxin Chen
A novel molecular imprinting fluorescence nanosensor was constructed via a facile surface imprinting polymerization one-pot synthesis strategy for highly selective and sensitive recognition and detection of 4-nitrophenol (4-NP) based on an electron-transfer induced fluorescence quenching mechanism. 2-Aminoethyl methacrylate hydrochloride (AMA) was first used as a surfactant to interact with aqueous carboxyl-CdTe quantum dots (QDs) and the resultant AMA-modified QDs were used as a core support and a fluorescent signal source. Then, an ultrathin 4-NP imprinted shell (ca. 4 nm) was formed on the QD surface (i.e., QD@MIPs) by a simple facile free radical polymerization step. The one-pot synthesis simplified the imprinting process and shortened the experimental period. The imprinted sites bound the template of 4-NP efficiently through the hydrogen bonding interactions and showed excellent recognition selectivity for 4-NP over its analogues with a high imprinting factor of 9.1. The electron transfer process between QDs and 4-NP led to significant fluorescence quenching of the QD@MIPs nanosensor, by which 4-NP could be sensed, and high detection sensitivity up to 0.051 μM was attained. Furthermore, the sensor was successfully applied to determine 4-NP in seawater and lake water samples, presenting high recoveries in the range of 92.7–109.2% at three spiking levels with the relative standard deviation within 3.1–4.8%. The simple, rapid, reliable QD@MIPs-based method proved to be potentially applicable for the highly selective and sensitive fluorescence determination of trace 4-NP in complicated environmental water samples.
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JOURNAL OF CHROMATOGRAPHY A
·
2024
·
IF 3.8
Zenghui Xu,Abudurexiti Reheman,Zhihao Lu,Shuiqiang Yu,Zhiwei Sun,Jinmao You
The detection of aromatic aldehydes, considered potential genotoxic impurities, holds significant importance during drug development and production. Current analytical methods necessitate complex pre-treatment processes and exhibit insufficient specificity and sensitivity. This study presents the utilization of naphthalenediimide as a pre-column derivatisation reagent to detect aromatic aldehyde impurities in pharmaceuticals via high-performance liquid chromatography (HPLC). We screened a series of derivatisation reagents through density functional theory (DFT) and investigated the phenomenon of photoinduced electron transfer (PET) for both the derivatisation reagents and the resulting products. Optimal experimental conditions for derivatisation were achieved at 40 °C for 60 min. This approach has been successfully applied to detect residual aromatic aldehyde genotoxic impurities in various pharmaceutical preparations, including 4-Nitrobenzaldehyde, 2-Nitrobenzaldehyde, 1,4-Benzodioxane-6-aldehyde, and 5-Hydroxymethylfurfural. The pre-column derivatisation method significantly enhanced detection sensitivity and reduced the limit of detection (LOD), which ranged from 0.002 to 0.008 μg/ml for the analytes, with relative standard deviations < 3 %. The correlation coefficient (R 2 ) >0.998 demonstrated high quality. In chloramphenicol eye drops, the concentration of 4-Nitrobenzaldehyde was measured to be 8.6 µg/mL below the specified concentration, with recoveries ranging from 90.0 % to 119.2 %. In comparison to existing methods, our work simplifies the pretreatment process, enhances the sensitivity and specificity of the analysis, and offers comprehensive insights into impurity detection in pharmaceutical preparations.
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Materials Today Chemistry
·
2024
·
IF 6.7
Bo Shen,Zhengqiu Chen,Huaming Mao,Jungang Yin,Yu Ren,Wei Dai,Shuanglong Zhao,Xiaoyu Chong,Hongwei Yang
In this study, we report a cuprous oxide nano-framework catalyst with abundant oxygen vacancies and multiple exposed crystalline surfaces. The catalyst exhibits excellent catalytic performance in the hydro-reduction reaction of 4-nitrophenol (4-NP) to 4-aminophenol (4-AP) with good reusability. Experimental and theoretical simulations showed that the construction of oxygen vacancies induced a change in the corresponding atomic configuration and electronic properties of the catalyst, which contributed to the improvement of the adsorption of 4-NP and the capture and activation of H atoms, thus accelerating the transfer process of reactive hydrogen and electrons to 4-NP using the catalyst as a mediator. In addition, the rough surface of the nano-framework exposed a variety of crystalline facets, among which the (210) facets possessed more suitable H atom adsorption energy and more electron transfer compared to the (100) facet, which further improved the hydrogenation performance of the catalyst. This study provides a catalyst design strategy based on the synergy of oxygen vacancies and crystalline surfaces for the efficient degradation of organic pollutants.
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Arabian Journal of Chemistry
·
2017
·
IF 4.553
Waqar Uddin,Gang Hu,Xuanxuan Sun,Hui Zhang,Yegui Wang,Lin Hu
A novel method for identification of two aromatic isomers of mono hydroxy benzoic acid (HBA) was reported by using their different perturbation effects on the potential oscillations of a Belousov-Zhabotinsky (BZ) system. In such a system, a macrocyclic complex of Cu [CuL](ClO 4 ) 2 was used as catalyst in which ligand L is 5,7,7,12,14,14-hexamethyl-1,4,8,11-tetraazacyclotetradeca-4,11-diene. To the BZ system, 3-hydroxy benzoic acid (3-HBA) could temporarily quench and regenerate potential oscillations with damping characters after inhibition time (t in ) while 4-hydroxy benzoic acid (4-HBA) could only change the oscillation amplitude (ΔA) to give damping oscillations with no inhibition time. Thus, these two isomers of HBA were identified. Reaction mechanisms of BZ have been proposed by FKN model. An explanation of perturbation mechanism is that, although 3-HBA reacted with BrO 2 while 4-HBA reacted with BrO 3 − , they all produced 1,4-quinone.
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ELECTROCHIMICA ACTA
·
2017
·
IF 4.798
Yuan Chen,Xiao-Mi Liu,Xi Wu,Xue-Chen Liu,Wen-Hao Dong,Bing-Kai Han,Xin Du,Cong Zhang,Yan-Yan Zhang,Hong-Tao Wang,Qiang Chen
Novel approachs to functionalize carboxylated multi-walled carbon nanotubes (CMWCNTs) array with poly- l -histidine (PLH) on a self-assembled monolayer (SAM) of 4-aminothiophenol (4ATP) were developed for the first time. With help of π–π interaction and chelation of the side imidazole groups in poly- l -histidine, the array showed efficient electron transfer and mild biocompatibility. By immobilizing glucose oxidase (GOx) to AuNPs electrodeposited on the array, a high-powered glucose biosensor with excellent electrocatalytic performance was fabricated and applied for glucose determination in human serum samples. The prepared biosensor exhibited highly sensitive response to glucose under the operating voltage of 600 mV with sensitivity of 96.04 μA mM −1 cm −2 , linear range of 0.005–6.5 mM, lowest detection limit (LOD) of 0.7 μΜ (S/N = 3) and Michaelis constant ( K M ) of 3.92 mM. Compared with other glucose sensors previously reported, this work showed higher sensitivity, lower detection limit and wider linear range. Furthermore, the developed array may provide a promising platform for various biosensors fabrication.
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Energy & Environmental Science
·
2017
·Vol. 10
·期 11
·2401-2410
·
IF 29.518
Ya-Fang Qi,Dong-Xing Kou,Wen-Hui Zhou,Zheng-Ji Zhou,Qing-Wen Tian,Yue-Na Meng,Xin-Sheng Liu,Zu-Liang Du,Si-Xin Wu
Although the substitution of Cu by Ag to suppress CuZn defects offers several advantages in overcoming the large open-circuit voltage (Voc) deficit for Cu2ZnSn(S,Se)4 (CZTSSe) solar cells, an excellent performance has not been achieved to date primarily due to the Fermi level pinning at the CdS/absorber interface and large recombination at the absorber/Mo interface. Herein, we developed a composition grading strategy to achieve a V-shaped Ag-graded structure with a higher Ag content on both the back and front surfaces of the (Cu,Ag)2ZnSn(S,Se)4 (CAZTSSe) layer. The key advantages of this Ag-graded structure are as follows: the higher content towards the CdS/absorber interface can create weak n-type donor defects and retard Fermi level pinning, whereas the lower content at the interlayer maintains the conductivity and light absorption; moreover, the other higher content towards Mo back contact can effectively suppress the recombination and improve the utilization of long-wave incident light. By appropriately adjusting the Ag gradient, we demonstrated a significant increase in Voc, and an unexpected conversion efficiency of 11.2% was achieved. This is the highest efficiency achieved to date for Ag-substituted CZTSSe solar cells, and the result supports a new aspect that synthesis of a composition-graded CAZTSSe absorber has great potential for future research.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
·
IF 9.4
Binxuan Diao,Fuhao Jiang,Heqing Ye,Rui Wang,Hongjiang Li,Haoran Zhang,Sang Woo Joo,Chenhao Cong,Se Hyun Kim,Xinlin Li
Two-dimensional metal – organic frameworks (2D MOFs) hold great promise as electrochemically active materials. However, their application in MOF nanocomposite electrodes in solution engineering is limited by structural self-stacking and imperfect conductive pathways. In this study, we used meso -tetra(4-carboxyphenyl ) porphine (TCPP) with off-domain π-bonds to reconstitute Zn-TCPP (ZMOF) and poly(3,4-ethylenedioxythiophene) polystyrene sulfonate (PEDOT:PSS) through an interfacial modulation strategy involving electrostatic coupling and hydrogen bonding, creating a conductive composite with a nanosheet structure. The negatively charged PSS and ZMOF formed a three-dimensional interconnected conductive network with excellent interfaces. The positively charged PEDOT, fine tuned with the lamellar structure, established strong π-π stacking interactions between the porphyrin and thiophene rings. ZMOF also induced changes in the PEDOT chain structure, weakening PSS entanglement and enhancing charge-transport properties. The specific capacitance of the prepared supercapacitor was as high as 967.8 F g −1 . Flexible supercapacitors produced on a large scale using dispensing printing technology exhibited an energy density of 1.85 μWh cm −2 and a power density of 7.08 μW cm −2 . This interfacial modulation strategy also exhibited excellent wearable properties, with 96 % capacitance retention at a 180° bending angle and stable cycling performance. This study presented a significant advancement in the functionalization of 2D materials, highlighting their potential for device-grade capacitive architectures.
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Molecular Catalysis
·
2024
·
IF 3.9
Xuecai Wei,Xiaoyang Yue,Quan Yuan,Ying He,Li Ma,Liya Zhou,Guanhua Liu,Yunting Liu,Yanjun Jiang
Ethyl ( S )-4‑chloro-3-hydroxybutyrate [( S )-CHBE] is attractive as a necessary intermediate for the production of highly valued products in pharmaceutical industries. Nowadays, alcohol dehydrogenases play an increasingly essential role in the asymmetric synthesis of chiral alcohols. In this work, a nicotinamide adenine dinucleotide (NADH)-dependent alcohol dehydrogenase from Pseudomonas bacterium ( Pb ADH) was obtained by genome mining method and identified to exhibit an excellent tolerance against the high substrate and product concentrations. For the regeneration of NADH, Bacillus megaterium glucose dehydrogenase ( Bm GDH) was successfully co-expressed with Pb ADH in E. coli cells. So much as 3.5 M (574 g/L) ethyl 4-chloroacetoacetate (COBE) can be converted to ( S )-CHBE completely with a > 99 % ee value under the catalysis by recombinant cells, even in a monophasic aqueous media with a single batch charge of substrate. In addition, in order to verify the substrate scope of Pb ADH, six other α/β-ketone esters and aromatic ketones were also evaluated as substrates at high substrate concentrations (100–650 g/L), and the corresponding chiral alcohols with highly optical purity were also achieved by co-expressed E. coli cells.
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DALTON TRANSACTIONS
·
2018
·Vol. 47
·期 12
·4315-4324
·
IF 4.099
Li Sun,Yuechao Yin,Fa Wang,Wenxian Su,Lixin Zhang
Au–Ag alloy nanoparticles (NPs) less than 10 nm in size were synthesized using sucrose as a reductant and surfactant. Au–Ag alloy NPs with a homogeneous composition were continuously obtained by changing the synthesis time from 2 to 40 min in one pot. Based on the UV-Vis, ICP, TEM, HR-TEM, EDX and SAED analyses, the synthesis mechanism of Au–Ag alloy NPs was deduced. Under hydrolysis conditions, sucrose showed a stronger reducibility compared with glucose, fructose and their mixture. And the as-prepared Au–Ag alloy NPs exhibited a superior photocatalytic activity and stability for the reduction of 4-nitrophenol due to the abundant hydroxyl groups of sucrose and the synergistic effect between Au and Ag elements. The rate constant of 4-nitrophenol reduction could be linearly controlled by the composition of Au–Ag alloy NPs or their synthesis time. It was indicated that the photocatalytic activity of Au–Ag alloy NPs could be predetermined as early as their synthesis process. The above methods of controlling the rate constant provide promising routes for other photocatalytic reactions using bimetallic NPs as photocatalysts.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2018
·
IF 5.667
Yuan Tan,Mingshi Li,Xiaoxue Ye,Zhengguo Wang,Yanying Wang,Chunya Li
Ionic liquid functionalized tungsten disulfite nanosheets (IL-WS 2 ) were prepared by using 1-vinyl-3-(3-aminopropyl)-imidazolium bromide (VAPimBr) ionic liquid as an auxiliary reagent to exfoliate WS 2 bulk crystals in N-methyl pyrrolidone with ultrasonication. Hollow gold nanospheres (HGNs) were controllably synthesized by using 1,3-di(3-bromopropyl)-imidazolium bromide ionic liquid as the functional monomer. HGNs were integrated onto IL-WS 2 nanosheet surface to fabricate a HGNs/IL-WS 2 nanocomposite through the interaction between S and Au atoms. VAPimBr ionic liquid and HGNs can significantly enhance the photocurrent response of IL-WS 2 nanosheets. Human epididymis protein 4 antibody (anti-HE4) was immobilized onto the HGNs/IL-WS 2 nanocomposite modified glassy carbon electrode (GCE) surface. Followed by being treated with glutaraldehyde vapor and bovine serum albumin (BSA), a photoelectrochemical immunosensor for human epididymis protein 4 (HE4) was successfully constructed and denoted as anti-HE4/HGNs/IL-WS 2 /GCE. The photoelectrochemical variation upon interacting with HE4 was used for the quantitative assay. Experimental conditions including the exfoliation time, the amount of VAPimBr ionic liquid, HGNs size, ascorbic acid concentration, incubation time, incubation temperature have been optimized. Under optimal conditions, HE4 was determined by using the photoelectrochemical immunosensor in a dynamic linear range from 0.1 pg mL −1 to 10 ng mL −1 with a detection limit of 0.03 pg mL −1 (S/N = 3). HE4 in clinical serum samples were also accurately determined with satisfied results.
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ANALYTICA CHIMICA ACTA
·
2017
·
IF 4.95
Yaran Du,Xiqian Li,Haijiao Zheng,Xueju Lv,Qiong Jia
In the present work, a novel metal-organic framework (MOF) fluorescent probe was prepared by post-synthetic modification of MIL-53-NH 2 (Al) with carboxylatocalix[4]arene (CC[4]A). The introduced CC[4]A could not only enhance the fluorescence performance and the recognition ability of the probe, but also sustain the high stability under UV light and moisture conditions. A method based on the as-synthesized CC[4]A@MIL-53-NH 2 (Al) probe was established for sensing hippuric acid . The detection limit was determined to be as low as 3.7 μg mL −1 . Over the concentration range of 0.005–3 mg mL −1 , the calibration curve was obtained with a satisfactory linearity ( R 2 = 0.993). The method was successfully used for rapid and highly selective direct monitor of hippuric acid in human urine. The sensor had great potential to be used as a simple diagnostic tool for hippuric acid in human urine which is regarded as a biological index of toluene exposure.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2024
·
IF 4.9
Ting Zhou,Luyao Zang,Junjie Sun,Xia Zhang,Zijie Qu,Xia Liu,Guodong Zhang,Xiufeng Wang,Fang Wang,Zhiqing Zhang
Considering the severe hazard to health posed by nitrophenol (NP) isomers, especially 4-NP, reliable and selective detection strategies are urgently challenged. In this study, a fluorescence platform based on glutathione-stabilized gold/silver nanoclusters (GSH-Au/Ag NCs) and zeolite imidazolate framework material (ZIF-8) was developed for 4-NP detection. The synergistic effect of gold and silver makes the bimetallic nanoclusters (GSH-Au/Ag NCs) much better in optical properties than gold nanoclusters. Subsequently, GSH-Au/Ag NCs with aggregation-induced emission (AIE) effect was encapsulated into ZIF-8 to obtain GSH-Au/Ag NCs@ZIF-8 nanocomposite. Compared with GSH-Au NCs, the fluorescence signal was efficiently further improved nearly 7 times through the confinement effect of ZIF-8, and the fluorescence lifetime was increased from 1.2 μs to 6.9 μs. The addition of 4-NP effectively quenched the fluorescence emission peak of GSH-Au/Ag NCs@ZIF-8 at 600 nm, and the assay exhibited highly sensitivity to 4-NP with the detection limit of 1.11 μM from 2.0 μM to 35 μM. Especially, results showed that 4-NP could be easily discriminated from nitrophenol isomers (3-NP and 2-NP). The mechanism research demonstrated that the absorption curve of GSH-Au/Ag NCs@ZIF-8 + 4-NP overlapped greatly with the fluorescence excitation spectrum of GSH-Au/Ag NCs@ZIF-8, and the fluorescence lifetime of GSH-Au/Ag NCs@ZIF-8 did not change when 4-NP was present or not. Therefore, the mechanism of GSH-Au/Ag NCs@ZIF-8 for 4-NP detection was mainly attributed to the inner filter effect (IFE). Furthermore, the developed detection assay was applied to water sample with satisfactory recovery results, demonstrating its high potential in monitoring 4-NP in environment.
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