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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY · 2021 · IF 4.098

The pH and mercury ion stimuli-responsive supramolecular assemblies of cucurbit[7]uril and Hoechst 33342

Qin Wang,Li-Bing Lü,Zhu Tao,Tao Sun,Qing Tang,Ying Huang

In the present work, we have investigated the effect of pH and mercury ions on the host–guest complex formed between cucurbit[7]uril (Q[7]) and Hoechst 33342 (H33342). 1 H NMR, UV–vis and fluorescence spectroscopy revealed that acid/base stimulation could change the binding stoichiometry between Q[7] and H33342. The results suggest that two complexation equilibria (1:1 and 2:1) may exist between H33342 and Q[7] at pH 2.0 and 4.5, respectively. However, a 1:1 host–guest complex was formed between H33342 and Q[7] at pH 7.0 and 10.0. Q[7] shows differential affinities for the protonated and neutral forms of H33342 dye. Moreover, the switching between H33342∙2H + @2Q[7](1:2) at pH 4.5 and H33342∙H + @Q[7](1:1) at pH 7.0 was reversible. Furthermore, as a metal stimulus, Hg 2+ ions could push (i) Q[7] from the piperazine ring to the benzimidazole position with a 1:1 guest–host ratio and (ii) a second Q[7] onto the ethyl position with a 1:2 guest–host stoichiometry. This stimulus response system will have potential applications in the field of molecular switch design.

研究领域: 超分子化学 · 分析化学
✓ 已验证 DOI PubMed 高影响因子
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ENVIRONMENTAL POLLUTION · 2020 · IF 6.793

Isolation of Trametes hirsuta La-7 with high laccase-productivity and its application in metabolism of 17β-estradiol

Kai Sun,Xing Cheng,Jialin Yu,Luojian Chen,Jiajun Wei,Wenjun Chen,Jun Wang,Shunyao Li,Qingzhu Liu,Youbin Si

Estrogens, which are extensive in the eco-environments, are a category of high-toxic emerging contaminants that induce metabolic disorders and even carcinogenic risks in wildlife and humans. Here we investigate whether fungus-secreted laccase can be used as a green catalyst to eliminate a representative estrogen, 17 β -estradiol (E2). A white-rot fungus Trametes hirsuta La-7 with high laccase-productivity, was isolated from pig manure-contaminated soil. Extracellular laccase activity expressed by strain La-7 was 65.4 U·mL −1 for a 3 d inoculation under the optimal fermentation parameters. The concentrated-crude laccase from Trametes hirsuta La-7 (CC- Th Lac) was capable of effectively metabolizing E2 at pH 4–6, and the apparent pseudo first-order reaction rate constant and half-life values were respectively 0.027–0.055 min −1 and 25.86–12.67 min ( R 2  > 0.98). The mass measurement of high-resolution mass spectrometry in combination with 13 C-isotope labeling identified that the main by-products of E2 metabolism were dimers, trimers , and tetramers, which are consistent with radical-driven C–C and/or C–O–C covalent coupling pathway, involving the initial enzymatic production of phenoxy radical intermediates and then the successive oxidative-oligomerization of radical intermediates. The formation of oligomers dramatically reduced the estrogenic activity of E2. Additionally, CC- Th Lac also exhibited high-efficiency metabolism capability toward E2 in the natural water and pig manure, with more than 94.4% and 91.0% of E2 having been metabolized, respectively. These findings provide a broad prospect for the clean biotechnological applications of Trametes hirsuta La-7 in estrogen-contaminated ecosystems.

CAS / MDL: 90-05-1 1401-55-4
研究领域: 环境生物学 · 生物化学 · 生态学
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Journal of Functional Foods · 2015 · IF 3.574

Biotransformed product, genistein 7-O-phosphate, enhances the oral bioavailability of genistein

Shang-Ta Wang,Ting-Fang Fang,Chen Hsu,Chia-Hao Chen,Chun-Jung Lin,Nan-Wei Su

Research has indicated the health beneficial effects of soyfoods. Genistein, one of the primary bioactive agents in soybeans, has a number of pharmacological and biological activities; however, its low water solubility and low intestinal permeability may lead to the depletion of genistein absorption from dietary intake and contribute to its poor oral bioavailability. Previous study revealed a water-soluble phosphate conjugate of genistein, genistein 7-O-phosphate (G7P), generated by biotransformation of Bacillus subtilis var. natto BCRC80517 with genistein. This study aimed to investigate the dissolution profile, intestinal permeability and oral bioavailability of genistein and G7P. G7P improved water solubility and also enhanced intestinal permeability in vitro and in situ , and greatly increased plasma exposure to genistein after oral administration in rats. The aqueous solubility of genistein is the absorption barrier to its oral bioavailability. G7P may be a promising and efficient alternative to genistein.

CAS / MDL: 446-72-0
研究领域: 药理学 · 营养学 · 生物转化
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MICROPOROUS AND MESOPOROUS MATERIALS · 2020 · IF 4.551

Functionalized ZIF-7/Pebax® 2533 mixed matrix membranes for CO2/N2 separation

Jie Gao,Haizhuo Mao,Hua Jin,Chen Chen,Armin Feldhoff,Yanshuo Li

Membrane-based separation technology has evolved as a competitive approach for CO 2 capture from flue gas (mainly N 2 ). To achieve high separation performance, three partially NH 2 -, OH- and CH 3 OH- functionalized mixed-linker-ZIF-7 were successfully synthesized, and incorporated into polyether-block-amide (Pebax® 2533) polymer to form mixed-matrix membranes (MMMs). As evidenced by the CO 2 adsorption isotherms , introducing functional groups in the ZIF-7 framework was indeed beneficial for CO 2 adsorption. All MMMs composed of ZIF-7-NH 2 , ZIF-7-OH and ZIF-7-CH 3 OH offered better CO 2 /N 2 separation performance than the parent ZIF-7-Pebax® 2533 membrane, suggesting the positive effect of functionalized ZIF-7 fillers on the gas separation performance. Among the three functionalized ZIF-7 based MMMs, the ZIF-7-OH-Pebax MMMs exhibited the best performance for CO 2 /N 2 separation, which might be ascribed to the highest adsorption selectivity of CO 2 over N 2 predicted by ideal adsorbed solution theory (IAST) for ZIF-7-OH fillers. The 14% ZIF-7-OH-Pebax MMM showed high CO 2 permeability of 273 Barrer and CO 2 /N 2 separation factor of 38, which increased by 60% and 145% as compared with the neat Pebax membrane. The strategy of preparing functionalized MOFs with strong affinity for CO 2 provides an effective method to develop MMMs for highly efficient CO 2 separation.

研究领域: 材料科学 · 环境工程
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Separations · 2023 ·Vol. 10 ·期 2 ·111 · IF 2.6

β-Diketone-Driven Deep Eutectic Solvent for Ultra-Efficient Natural Stable Lithium-7 Isotope Separation

Zexing Xie,Meiying Xie,Tingting Tang,Fan Yang,Liyan Xue,Zhengming Jiang

6Li and7Li are strategic resources. Because Li+ions have no outermost electrons and the radii of6Li and7Li differ by only one neutron, the separation of the naturally stable isotopes of Li, especially by solvent extraction, is recognized as a difficult problem worldwide. Therefore, in this paper, an advancedβ-diketone-driven deep eutectic solvent (DES) extraction system containing 2-thenoyltrifluoroacetone (HTTA) and tri-n-octyl phosphine oxide (TOPO) is introduced to the extraction and separation of6Li+and7Li+ions. Compared with those of reported HTTA extraction systems and crown ether extraction systems, the separation coefficient (β7Li/6Li) of theβ-diketone-driven DES extraction system can reach the best value of 1.068, which is now the highest knownβ-value reported in the extraction system. From the intramolecular hydrogen bond of HTTA to the intermolecular hydrogen bond of DES, the bond energy increases by 47.8%. Because the active site of the proton in DES provides a higher energy barrier for the separation of7Li, theβ7Li/6Liis significantly increased. The extractions were characterized by spectrum, using1H nuclear magnetic resonance (NMR) spectroscopy, Fourier-transform infrared (FT-IR) spectroscopy, and X-ray photoelectron spectroscopy (XPS). The mechanism was determined on the basis of the reaction kinetics and density functional theory (DFT). The DES extractant shows excellent cycle performance with regard to stripping and reusability. In conclusion, the highly efficient, economical, and stableβ-diketone-driven DES extraction system can be used for the separation of naturally stable Li isotopes, which provides good industrial application prospects.Keywords:β-diketone;Lithium-7;separation of isotopes;deep eutectic solvent (DES);solvent extraction

研究领域: 化学 · 材料科学
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Biotechnology Journal · 2023 · IF 4.7

Secretory Production of 7-dehydrocholesterol by Engineered Saccharomyces cerevisiae

Xia Ke,Zi-Hao Pan,Hong-Fei Du,Yi Shen,Ji-Dong Shen,Zhi-Qiang Liu,Yu-Guo Zheng

Background 7-dehydrocholesterol (7-DHC) can be directly converted to vitamin D 3 by UV irradiation and d e novo synthesis of 7-DHC in engineered Saccharomyces cerevisiae has been recognized as an attractive substitution to traditional chemical synthesis. Introduction of sterol extracellular transport pathway for the secretory production of 7-DHC is a promising approach to achieve higher titer and simplify the downstream purification processing. Methods and results A series of genes involved in ergosterol pathway were combined reinforced and reengineered in S. cerevisiae . A Biphasic fermentation system was introduced and 7-DHC was found to be enriched in oil-phase with an increased titer by 1.5-folds. Quantitative PCR revealed that say1, atf2, pdr5, pry1-3 involved in sterol storage and transport were all significantly induced in sterol overproduced strain. To enhance the secretion capacity, lipid transporters of Pry (Pathogen-related yeast proteins), NPC2(Niemann-Pick disease type C2), ABC(ATP-binding cassette)-family and their homologues were screened. Both individual and synergetic overexpression of Pr-1 (Plant pathogenesis Related protein-1) and St1 (Sterol transport1) largely increased the de novo biosynthesis and secretory productivity of 7-DHC, and the final titer reached 28.2 mg/g with a secretion ratio of 41.4%, which was 26.5-folds higher than the original strain. In addition, the cooperation between Pr-1 and St1 in sterol transport was further confirmed by confocal microscopy, molecular docking and directed site-mutation. Conclusion Selective secretion of different sterol intermediates was characterized in sterol over-produced strain and the extracellular export of 7-DHC developed in present study significantly improved the cell biosynthetic capacity, which offered a novel modification idea for 7-DHC de novo biosynthesis by S. cerevisiae cell factory. This article is protected by copyright. All rights reserved

CAS / MDL: 112-40-3
研究领域: 生物技术 · 微生物学 · 代谢工程 · 生物化学
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CHEMICAL ENGINEERING JOURNAL · 2024 · IF 13.3

Chameleon-inspired supramolecular materials based on cucurbit[7]uril and viologens exhibiting full-color tunable photochromic behavior

Dong-Xue Xia,Xin Wang,Wen-Qi Sun,Rui-Lian Lin,Jing-Xin Liu,Ying-Wei Yang

Inspired by Chameleons' skin color tuning in response to environmental changes, we design and prepare three inclusion complexes based on the cucurbit[7]uril (Q[7]) host and three viologen guests. Upon light irradiation, the colors of these inclusion complexes in the solid state turn from light colors to vivid three primary colors, i.e., red, green, and blue, respectively. Ultraviolet–visible (UV–vis) diffuse reflectance and electron spin resonance (ESR) spectra reveal that the photochromism can be attributed to the generation of viologen radicals, originating from the photoinduced electron transfer. The results of quantum chemical calculation indicate that Q[7] in the inclusion complexes acts as the electron donor in the photoinduced electron transfer process. Using a color mixing approach and finely manipulating the proportions of the three inclusion complexes, a series of composite photochromic materials (CPMs) can be manufactured, covering a full-color gamut in visible light. On the other hand, due to the ignorable size and shape change of CPMs during the photochromatic processes, the CPMs-based reversible photochromic “printing” and photofading “erase” properties were also used for quick response (QR) code. Therefore, these prominent intelligent features of CPMs open new avenues to explore optical regulated nano-platforms for multiple anti-counterfeiting, biomimetics, and military camouflage applications.

研究领域: 材料科学 · 化学 · 仿生学
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MICROCHEMICAL JOURNAL · 2022 · IF 5.304

High sensitivity electrochemiluminescence sensor based on the synergy of ZIF-7 and CdTe for determination of glucose

Xin Zhang,Li Tian,Kexin Wu,Zhuo Sun,Qian Wu,Xiangyu Shan,Yingjie Zhao,Ruizhan Chen,Juan Lu

An electrochemical luminescence (ECL) sensor for the detection of glucose was constructed by covering CdTe nanomaterials, ZIF-7 and glucose oxidase (GOD) on the electrode surface, respectively. CdTe and ZIF-7, as co-reaction promoters, could amplify ECL signals through synergy effect. The results demonstrated that ECL intensity increased when the concentration of glucose increased. Based on the change of ECL intensity, a method for the determination of glucose was established. Possible response mechanisms were also studied. The parameters of measurement conditions were optimized. The linear range of glucose was 2.0 × 10 −10  ∼ 2.0 × 10 −5  mol L −1 and the detection limit was 6.7 × 10 −11  mol L −1 under the optimal conditions. The constructed sensor had high sensitivity and selectivity. The results were satisfactory for the determination of glucose in real human serum samples.

研究领域: 分析化学 · 生物医学工程
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES · 2024 · IF 7.7

Enhanced activity of enzymes encapsulated in spheres metal azolate framework-7 with defects

Cai Cheng,Xiaoliang Guo,Yu Feng,Jie Yu,Shi Huang,Liexiong Zhang,Yu Wu,Linna Shao,Xuehan Xu,Lingling Feng

Developing metal-organic frameworks (MOFs) with specific structures is critical for improving the activity of embedded enzymes, and defects may be one of the effective methods. Several methods have been demonstrated to be effective in creating defects in MOFs, including post-synthetic treatments, the use of acid as a modulator, and the use of ordinary or thermally sensitive linkers. However, these methods necessitate the utilization of additional substances. Metal azolate framework-7 (MAF-7) is a kind of MOF that was formed by the coordination of Zn 2+ with 3-methyl-1,2,4-triazole (Hmtz). This paper presents a method for the preparation of defect MAF-7 by changing the sequence of reactants without the introduction of additional substances. The defects were characterized by a range of techniques, including scanning electron microscopy, transmission electron microscopy, Brunauer-Emmett-Teller, X-ray photoelectron spectroscopy, and powder X-ray diffraction. The activity of microcystinase A (MlrA) encapsulated in defective MAF-7 (CMlrA@DMAF-7) was found to be significantly increased in comparison to non-porous MAF-7 (NMAF-7), and was largely unaffected by alterations in synthesis conditions. It is also noteworthy that lysozyme (LZ) and horseradish peroxidase (HRP), which are commonly used in industry, also demonstrated enhanced activity when encapsulated in DMAF-7. It was therefore anticipated that modifying the sequence of reactant addition would be a straightforward and simple method of introducing defects into MAF-7, thereby improving enzyme utilization.

CAS / MDL: 868-77-9
研究领域: 生物化学 · 材料科学
✓ 已验证 产品关联 DOI PubMed 高影响因子
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TALANTA · 2018 · IF 4.244

Carbon nanosphere-based fluorescence aptasensor for targeted detection of breast cancer cell MCF-7

Dandan Yang,Mei Liu,Jing Xu,Chao Yang,Xiaoxiao Wang,Yongbing Lou,Nongyue He,Zhifei Wang

In this work, carbon nanosphere (CNS)-based fluorescence “turn off/on” aptasensor was developed for targeted detection of breast cancer cell MCF-7 by conjugation with FAM (a dye)-labeled mucin1 (MUC1) aptamer P0 (P0-FAM), which can recognize MUC1 protein overexpressed on the surface of MCF-7. Different from other carbon based fluorescence quenching materials, CNSs prepared by the carbonization of glucose not only have the high fluorescence quenching efficiency (98.8%), but also possess negligible cytotoxicity (in the concentration range of 0–1 mg/mL, which is 10 times higher than that of traditional carbon nanotubes or graphene oxide (0–100 µg/mL)). As for the detection of the mimic of the tumor antigen MUC1, the resulting fluorescence intensity increases nearly linearly in the range of 0–6 μM with the limit of detection (LOD) of 25 nM.

CAS / MDL: 9002-98-6
研究领域: 生物化学 · 医学诊断 · 纳米材料科学
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ACS Applied Materials & Interfaces · 2022 · IF 10.383

Inorganic Pillar Center-Facilitated Counterdiffusion Synthesis for Highly H2 Perm-Selective KAUST-7 Membranes

Jinyin Lv,Yanwen Cui,Jianhua Yang,Liangqing Li,Xuerong Zhou,Jinming Lu,Gaohong He

Fluorinated metal–organic framework materials (NbOFFIVE-1-Ni, also referred to as KAUST-7) have attracted widespread attention because of their high chemical stability and thermal stability, outstanding tolerance with water and H2S, and high CO2-adsorption selectivity over H2 and CH4. KAUST-7 was expected to be a new membrane material candidate for H2/CO2 separation because of the hindered permeation of CO2 resulting from the interaction between CO2 and (NbOF5)2– of the KAUST-7 framework. A highly H2 perm-selective KAUST-7 membrane was first achieved using a novel strategy of inorganic pillar center-facilitated counterdiffusion (IPCFCD) proposed by us. The IPCFCD method not only effectively avoided the corrosion of hydrofluoric acid to α-Al2O3 tubes in the process of preparing KAUST-7 membranes, but also better reduced grain boundary defects because of the faster nucleation rate and resultant high crystallinity. The KAUST-7 membrane exhibited a high H2/CO2 separation factor (SF) of 27.30 for the 1:1 H2/CO2 binary gas mixture with a high H2 permeance of 5.30 × 10–7 mol m–2 s–1 Pa–1 under ambient conditions and a slight decrease of the H2/CO2 SF with increasing operation temperature and presence of steam. This study highlighted the importance of pre-synthesizing inorganic pillar centers (NiNbOF5 intermediate) and the innovation of a membrane formation process for synthesizing polycrystalline KAUST-7 membranes. Most important of all, our study provided a novel approach to overcome the challenge in fabricating metal–organic framework membranes containing corrosive reactants for the corresponding supports.

CAS / MDL: 1313-99-1
研究领域: 材料科学 · 化学工程
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INTERNATIONAL JOURNAL OF PHARMACEUTICS · 2021 · IF 5.875

Redox responsive 7-ethyl-10-hydroxycamptothecin (SN38) lysophospholipid conjugate: synthesis, assembly and anticancer evaluation

Wei He,Yawei Du,Tao Wang,Ji Wang,Lei Cheng,Xinsong Li

7-Ethyl-10-hydroxycamptothecin (SN38), a potent camptothecin derivative specifically targeting DNA topoisomerase I cleavage complexes, has shown great potential in the treatment of solid tumors . Because of its poor solubility and chemical and metabolic stability, the clinical application of SN38 is highly limited. To address these problems, a novel redox-responsive SN38 conjugate based liposomal formulation is developed in this report. First, SN38 was conjugated with lysophospholipid by using a cleavable disulfide bond linker. After that, the conjugate (SN38-SS-PC) was assembled into liposomes by thin film method. Dynamic light   scattering   (DLS) characterization indicated that SN38-SS-PC liposomes possessed a narrow size distribution (172.8 ± 10.5 nm) and negative charged zeta potential (-8.9 ± 0.3 mV). The results of storage and physiological stabilities showed that SN38-SS-PC liposomes was stable under different conditions. More importantly, a reduction responsive release of parent drug SN38 was observed in the medium containing glutathione (GSH). In addition, SN38-SS-PC liposomes had a much more rapid cellular uptake behavior against cancer cells. The enhanced anti-cancer efficacy of SN38-SS-PC liposomes was further demonstrated by in vitro cytotoxicity assay against MCF-7 and A549 cells. Under in vivo evaluation in 4 T1 xenograft tumor model, SN38-SS-PC liposomes were observed to have lower systemic toxicity and higher tumor inhibition rate of 53.3% compared with the commercialized SN38 prodrug Irinotecan (Ir). In summary, SN38-SS-PC liposomes could be a promising redox responsive delivery system of SN38 for cancer therapy.

研究领域: 药学 · 肿瘤学 · 药物递送系统 · 生物药剂学
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