INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2015
·
IF 2.587
Ye He,Zhiqian Guo,Pengwei Jin,Changhong Jiao,He Tian,Weihong Zhu
α-Ketoglutarate (α-KA) can convert to 2-hydroxyglutarate (2-HG), which is confirmed to be associated with many diseases, especially with acute myeloid leukemia (AML). In this paper, a novel reaction-based chemosensor DT based on the typical Schiff-base reaction was designed for sensing the biomarker of α-KA, in which a diazanyl group as the recognition group was linked with a benzothiadiazole unit as the fluorophore moiety. Considering the typical Schiff-base reaction to generate hydrazones suffering from slow kinetics, particularly under neutral conditions, a series of parallel experiments was conducted for optimizing the chemical recognition process, including varying the solvent, reaction temperature, reactant concentration, and reaction rate. The optimum condition was established as a pH value, temperature, α-KA concentration, and response time of 5.7, 30 °C, 100 μM, and 20 min, respectively. Notably, in contrast with the initial 6.3-fold fluorescence enhancement, the remarkable 75-fold fluorescence enhancement ((I – I0)/I0 at 560 nm) was observed by optimizing the chemical recognition process of DT and α-KA. Finally, DT was carried out for the chemical recognition processing of α-KA in serum. We demonstrated that DT is selective for α-KA over other potential biologically interferences with similar structures and thus is suitable for detecting α-KA in serum. On the basis of the optimized chemical recognition process, DT shows high potential application for sensing α-KA with remarkable fluorescence enhancement. This work provided a potential method that is quick and convenient for sensing biomarker α-KA in serum. It is worth noting that without complicated pretreatment, utilizing a novel reaction-based fluorescent chemosensor may establish a new promising platform for clinical diagnosis biomarker.
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Polymer Chemistry
·
2016
·Vol. 7
·期 14
·2511-2520
·
IF 5.687
Jiahui Su,Hong Huang,Yanyan Cui,Yingyin Chen,Xiaoxuan Liu
Two types of photoactive polymers with an alkoxyphenyl ketone moiety at their backbone centers were synthesized through atom transfer radical polymerization. A facile protocol for preparing α,ω-heterotelechelic polymers was developed, employing nitroxide with different functional groups (e.g., hydroxyl, propargyl, glycidyl, and polyethylene glycol) coupled with macromolecular radicals generated via the Norrish-type I photoreaction under mild UV irradiation from the said polymers. Experimental conditions such as solvent effects and irradiaton time were investigated to optimize the efficiency of reaction functionality. The number-average molecular weights of the photoactive polymers and α,ω-heterotelechelic polymers were determined by gel permeation chromatography. Material structures were further confirmed by 1H NMR and FT-IR spectroscopy. The end group activity of α,ω-heterotelechelic polymers obtained from this reaction was further demonstrated using the Cu-catalyzed azide–alkyne click reactions between PS-N3 and polystyrene capped with a propargyl group.
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Polymer Chemistry
·
2016
·Vol. 7
·期 47
·7216-7222
·
IF 5.687
Yan Li,Cheng Chen,Jinlong Wu,Xiangxiang Jia,Yufan Lu,Fangjuan Chen,Lijian Liu
Copolymerization between alkyl diazoacetates and α,β-unsaturated aldehydes, which is a one-pot, one-step and catalyst-free reaction, is presented. The product is a ternary copolymer composed of an alkyl diazoacetate, an α,β-unsaturated aldehyde and an α-carbalkoxy carbene, which is derived from the alkyl diazoacetate by the release of N2. Thus, the reaction is named as the C1N2/C2/C1 copolymerization. Various diazoacetates and α,β-unsaturated aldehydes were utilized to establish the methodology. The products are down-/up-conversion fluorescence molecules that can significantly enhance cell imaging through the synchronized excitation of near-ultraviolet and near-infrared light and may be widely used in other optical fields. The up-conversion fluorescence is the result of a two-photon excitation process.
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Food & Function
·
2016
·Vol. 7
·期 9
·3953-3963
·
IF 2.686
Li Zeng,Guowen Zhang,Yijing Liao,Deming Gong
It is important to investigate the inhibition of α-glucosidase due to its correlation with type 2 diabetes. Morin was found to exert significant inhibition activity on α-glucosidase in a reversible mixed-type manner with an IC50 value of (4.48 ± 0.04) μM. Analyses of fluorescence and circular dichroism spectra indicated that the formation of the morin-α-glucosidase complex was driven mainly by hydrophobic forces and hydrogen bonding, and caused the conformational changes of α-glucosidase. The phase diagrams of fluorescence showed that the conformational change process was monophasic without intermediates. Molecular docking indicated that morin mainly interacted with amino acid residues located close to the active site of α-glucosidase, which may move to cover the active pocket to reduce the binding of the substrate and then inhibit the catalytic activity. Morin was also found to exhibit inhibition in the generation of advanced glycation end products which was related to the long term complications of diabetes.
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Catalysis Science & Technology
·
2016
·Vol. 6
·期 20
·7429-7436
·
IF 5.287
Xiuquan Jia,Jiping Ma,Min Wang,Xiaofang Li,Jin Gao,Jie Xu
The tandem reaction is a growing field to yield important advances toward green and sustainable chemistry. Herein, we report a bifunctional manganese oxide catalyst with an interface binding redox phase (α-MnO2) and a basic phase (NaxMnO2). The molar ratio of NaOH/Mn plays a great role in the formation of α-MnO2/NaxMnO2. The sodium cation is essential for the formation of a basic NaxMnO2 phase while the potassium cation promotes the formation of a redox-active α-MnO2 phase. The interface structure of α-MnO2/NaxMnO2 geometrically favors the ammoxidation–Pinner tandem reaction to synthesize imidates in a 58–96% yield from aldehydes. Thus a phase collaborative effect is observed. In the ammoxidation process, the redox cycle of MnIV/MnIII is involved and the lattice oxygen in the α-MnO2 phase acts as an active oxygen species. The O–H in methanol is activated and dissociated on the basic sites of NaxMnO2 to the adsorbed methoxyl species to facilitate the Pinner synthesis. This approach bypasses the conventional synthesis of imidates, which suffer from harsh reaction conditions and the requirement for multiple steps.
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POLYHEDRON
·
2016
·
IF 2.108
Jingquan Sha,Xiya Yang,Longjiang Sun,Xiumei Zhang,Shuxian Li,Jisen Li,Ning Sheng
An assembly of cyclodextrin metal-organic frameworks (CD-MOFs) has aroused extensive research interests due to their excellent encapsulation capacity and biocompatibility. In this work, starting from the chiral building block α-cyclodextrin (α-CD), a novel α-CD-MOF compound with left-handed chiral helices, [Na(H 2 O)(C 36 H 60 O 30 )]·H 2 O (Na-α-CD-MOF), was synthesized through changing the diffusion solvent, and then structurally characterized. Single crystal X-ray diffraction analysis reveals that Na-α-CD-MOF exhibits a 3D left-handed helical chiral framework with large cavities (740 Å 3 ). The result of a drug adsorption assay shows Na-α-CD-MOF possesses a more efficient drug adsorption capacity than α-CD matrix, and the solubility of the drug adsorbed in Na-α-CD-MOF can be greatly enhanced. All the results, including the lower cytotoxicity, indicate that Na-α-CD-MOF is an excellent kind of renewable, environmental friendly and biocompatibility drug carrier material.
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CHINESE JOURNAL OF CATALYSIS
·
2024
·
IF 15.7
Changpo Ma,Ying Lai,Tiange Zhao,Xiaoxuan Zhang,Haichao Liu,Weiran Yang
α,ω-Dicarboxylic acids are important intermediates for the preparation of polyamides , polyesters and polyurethanes . However, their production pathways are limited and usually suffer from low efficiency and environmental problems. Here, we report an innovative approach to synthesize C+2 dicarboxylic acids directly from cyclic ethers by dicarbonylation. Different from the general findings that C+1 monocarboxylic acids are produced by carbonylation of cyclic ethers involving alkene intermediates, in this work, by manipulating the reaction system with RhCl 3 and iodine in acetic acid, diiodide-substituted intermediates were selectively formed and subsequently converted to dicarboxylic acids in the presence of H 2 and CO. As high as 84% yield of adipic acid was obtained directly from tetrahydrofuran. This catalytic system is applicable not only to a wide variety of cyclic ethers but also to different primary diols to synthesize C2-elongated α,ω-dicarboxylic acids. This work provides a novel dicarbonylation strategy for the efficient synthesis of adipic acid, glutaric acid and other important α,ω-dicarboxylic acids (such as 1,7-heptanedioic acid and 1,8-octanedioic acid) that are still not easily synthesized by other methods.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2024
·
IF 7.7
Nana Li,Liangqiang Chen,Wanqiu Huang,Mengdi Hao,Huabin Tu,Hao Shen,Fan Yang,Shaoning Yu
As one of the most important industrial enzymes, α-amylase is widely used in food processing, such as starch sugar and fermentation, bringing high added value to industry of more than a trillion dollars. We developed a multi-enzyme system (Glu&Gox@Cu-MOF-74) prepared by embedding α-glucosidase (Glu) and glucose oxidase (Gox) into the biomimetic metal-organic framework Cu-MOF-74 using in situ encapsulation within 15 min at room temperature for efficient and sensitive detection of α-amylase activity. Benefitting from the remarkable peroxidase-mimicking property and rigid skeleton of Cu-MOF-74, the biocatalytic platform exhibited excellent cascade activity and tolerance in various extremely harsh environments compared to natural enzymes. On this basis, a cascade biocatalytic platform was constructed for the detection of α-amylase activity with wide linear range (5–100 U/L) and low limit of detection (1.45 U/L). The colorimetric cascade scheme is important for the sensitive and selective determination of α-amylase in complex fermentation samples, and the detection time is short (∼0.5 h). This work provides new ideas for the detection of α-amylase based on the cascade amplification method.
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JOURNAL OF MOLECULAR LIQUIDS
·
2024
·
IF 5.3
Caixia Deng,Shuang Li,JiaYu Wang,Qiang Yang,Hui Chen,Fenglin Tang,Xiupei Yang
In this work, flower-like TiO 2 (TiO 2 -F) was first prepared by modulating the morphology of TiO 2 , and then, α-Fe 2 O 3 was loaded onto TiO 2 -F to successfully prepare α-Fe 2 O 3 /TiO 2 -F heterojunction materials. The material showed excellent degradation properties of doxycycline hydrochloride under visible light. The photocatalytic degradation efficiency of α-Fe 2 O 3 /TiO 2 -F2 for doxycycline hydrochloride under visible light reached 95.76 % in 120 min, and its pseudo-first-order degradation rate constant was 0.02647 min −1 , which was 3.68 and 2.01 times higher than those of α-Fe 2 O 3 and TiO 2 alone, respectively. This good photocatalytic performance is attributed mainly to the introduction of α-Fe 2 O 3 to form a Type II heterojunction with floral TiO 2 (TiO 2 -F), which is capable of promoting the separation of electron–hole pairs of photocatalysts and exhibiting a stronger redox capacity. The material exhibits notable stability and maintains high degradation efficiency even after undergoing multiple cycles. Furthermore, free radical trapping experiments and electron spin resonance (ESR) characterization revealed that hydroxyl radicals play a dominant role in this system. Finally, the degradation pathways were analyzed, and relevant toxicological analyses were performed, indicating that the toxicity of doxycycline hydrochloride gradually decreased during the photocatalytic degradation process.
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Nano Research
·
2024
·
IF 9.5
Zhao Yuan,Wang Qingshuang,Yin Dongming,Wang Xiaoli,Li Shouliang,Wang Chunli,Liang Long,Zhao Shaolei,Wang Limin,Cheng Yong
α-AlH 3 is regarded as one of the most promising hydrogen storage materials due to its high hydrogen storage capacity (10.1 wt.%, 148 kg·m −3 ). However, in practical applications, the associated hydrogen release temperature remains relatively high. To effectively address this issue, hollow structured Fe@C nanorods derived from Fe-MOF are introduced as highly efficient catalyst to optimize the dehydrogenation properties of α-AlH 3 . Comparatively, the initial hydrogen release temperature of α-AlH 3 + 3 wt.% Fe@C is reduced to 94.2 °C, which is significantly lower than that of pure α-AlH 3 (137.8 °C). At 100 and 120 °C, it exhibits hydrogen capacities of 5.38 wt.% and 7.47 wt.%, respectively, whereas pure α-AlH 3 only delivers hydrogen capacities of 0.24 wt.% and 5.94 wt.% under the same temperatures. The density functional theory (DFT) calculations further indicate that the existence of Fe@C catalyst can make the length of Al–H bond increase, which is more conducive to the release of hydrogen. The results show that the synergistic effect of Fe and porous carbon in Fe@C nanorods can improve the hydrogen desorption kinetics of α-AlH 3 , providing a good prospect for the application of α-AlH 3 in hydrogen storage fields.
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MOLECULES
·
2024
·Vol. 29
·期 23
·5604
·
IF 4.2
Zhiqiang Yu,Qingcheng Wang,Jinhao Jia,Wenbo Kang,Meilian Ou,Zhimou Xu
Among the transition metal oxides, hematite (α-Fe2O3) has been widely used in the preparation of memristors because of its excellent physical and chemical properties. In this paper, α-Fe2O3nanowire arrays with a preferred orientation along the [110] direction were prepared by a facile hydrothermal method and annealing treatment on the FTO substrate, and then α-Fe2O3nanowire array-based Au/α-Fe2O3/FTO memristors were obtained by plating the Au electrodes on the as-prepared α-Fe2O3nanowire arrays. The as-prepared α-Fe2O3nanowire array-based Au/α-Fe2O3/FTO memristors have demonstrated stable nonvolatile bipolar resistive switching behaviors with a high resistive switching ratio of about two orders of magnitude, good resistance retention (up to 103s), and ultralow set voltage (Vset= +2.63 V) and reset voltage (Vreset= −2 V). In addition, the space charge-limited conduction (SCLC) mechanism has been proposed to be in the high resistance state, and the formation and destruction of the conductive channels modulated by oxygen vacancies have been suggested to be responsible for the nonvolatile resistive switching behaviors of the Au/α-Fe2O3/FTO memristors. Our results show the potential of the Au/α-Fe2O3/FTO memristors in nonvolatile memory applications.
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ACS Applied Energy Materials
·
2024
·
IF 5.4
Yining Pan,Qiang Zeng,Linhong Li,Mingxin Deng,Xiang Liao,Mingjun Zhang,Wei Wang,Feng Xie,Fangyang Liu
Integrating cesium (Cs) into perovskite layers significantly enhances the stability of perovskite solar cells (PSCs), which is a critical aspect for achieving high efficiency. However, the elemental and phase segregation, caused by the inhomogeneous distribution of Cs within the perovskite film, poses a risk to the device’s lifetime. To address this issue, we present an innovative aqueous synthesis method for CsxFA1–xPbI3 (CsFA) microcrystals as precursors to perovskite thin films. These synthesized microcrystals ensure uniform cesium distribution across the perovskite grains, acting as a 3D scaffold for the crystallization process. This scaffold serves as a template, facilitating a homogeneous Cs distribution within the perovskite film. Utilizing these CsFA microcrystals, we achieved a maximum power conversion efficiency (PCE) of 23.70%, with the devices maintaining 96% of their initial PCE after 600 h in ambient conditions. Our innovative approach facilitates the mass production of high-purity CsFA microcrystals from cost-effective, low-purity starting materials, which is conducive to facile application for further commercialization.
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