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1.
  • Hu, Jiwen, et al. (author)
  • Rapid detection of mercury (II) ions and water content by a new rhodamine B-based fluorescent chemosensor
  • 2020
  • In: Spectrochimica Acta Part A - Molecular and Biomolecular Spectroscopy. - : PERGAMON-ELSEVIER SCIENCE LTD. - 1386-1425 .- 1873-3557. ; 241
  • Journal article (peer-reviewed)abstract
    • A rhodamine B-based sensor (RS) was designed and synthesized by a combination of the spirolacton rhodamine B (fluorophore) and multidentate chelates (ionophore) with high affinity towards Hg2+. In the presence of Hg2+, the resulting red-orange fluorescence (under UV light) and naked eye red color of IDS are supposed to be used for quantitative and qualitative measurement of Hg2+. Further fluorescent titration and analysis demonstrate that RS can selectively detect Hg2+ within 1 s with a low limit of detection (LOD) of 16 nM in acetonitrile media, meanwhile, the association constant (K-a) was calculated to be 0.32 x 10(5) M-1. More importantly, the resultant complex (RSHg) of RS and Hg2+ has also been successfully applied to detect limited water content in acetonitrile solution. (C) 2020 Published by Elsevier B.V.
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2.
  • Hu, Jiwen, et al. (author)
  • A logic gate-based fluorogenic probe for Hg2+ detection and its applications in cellular imaging
  • 2016
  • In: Analytica Chimica Acta. - : ELSEVIER SCIENCE BV. - 0003-2670 .- 1873-4324. ; 919, s. 85-93
  • Journal article (peer-reviewed)abstract
    • A new colorimetric and fluorogenic probe (RN3) based on rhodamine-B has been successfully designed and synthesized. It displays a selective response to Hg2+ in the aqueous buffer solution over the other competing metals. Upon addition of Hg2+, the solution of RN3 exhibits a naked eye observable color change from colorless to red and an intensive fluorescence with about 105-fold enhancement. The changes in the color and fluorescence are ascribed to the ring-opening of spirolactam in rhodamine fluorophore, which is induced by a binding of the constructed receptor to Hg2+ with the association and dissociation constants of 0.22 x 10(5) M-1 and 25.2 mM, respectively. The Jobs plot experiment determines a 1: 1 binding stoichiometry between RN3 and Hg2+. The resultant "turn-on" fluorescence in buffer solution, allows the application of a method to determine Hg2+ levels in the range of 4.0-15.0 mu M, with the limit of detection (LOD) calculated at 60.7 nM (3 sigma/slope). In addition, the fluorescence turn-off and color fading-out happen to the mixture of RN3-Hg2+ by further addition of I- or S2-. The reversible switching cycles of fluorescence intensity upon alternate additions of Hg2+ and S2- demonstrate that RN3 can perform as an INHIBIT logic gate. Furthermore, the potential of RN3 as a fluorescent probe has been demonstrated for cellular imaging. (C) 2016 Elsevier B.V. All rights reserved.
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3.
  • Hu, Jiwen, et al. (author)
  • A new ratiometric fluorescent chemodosimeter based on an ICT modulation for the detection of Hg2
  • 2016
  • In: Sensors and actuators. B, Chemical. - : ELSEVIER SCIENCE SA. - 0925-4005 .- 1873-3077. ; 230, s. 639-644
  • Journal article (peer-reviewed)abstract
    • We design and synthesize a new ratiometric fluorescent chemodosimeter (S1) for the selective and sensitive detection of Hg2+. Upon addition of Hg2+, the emission of the S1 exhibits a large bathochromic shift from 393 to 515 nm (up to 122 nm) which is ascribed to an intramolecular charge transfer process in the resultant. The Hg2+-induced dethioacetalization for sensing mechanism has been demonstrated by using high-performance liquid chromatography analysis of the sensing process. The interference experiments further demonstrate that S1 exhibits very high selectivity towards Hg2+ over other coexisting cations/anions. Subsequently, a good linearity of the concentrations of Hg2+ (0-15 mu M) vs the ratiometric signals (I-515/I-393) allows a fluorogenic method for the quantitative detection of Hg2+, with the limitation of detection determined to be 5.22 x 10(-7) M. (C) 2016 Elsevier B.V. All rights reserved.
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4.
  • Hu, Jiwen, et al. (author)
  • A rhodamine-based fluorescent probe for Hg2+ and its application for biological visualization
  • 2014
  • In: Sensors and actuators. B, Chemical. - : Elsevier. - 0925-4005 .- 1873-3077. ; 203, s. 452-458
  • Journal article (peer-reviewed)abstract
    • A new visible light excitable fluorescent probe (1) is synthesized by appending a hydroxymethyl-pyridine to rhodamine B hydrazide. The probe displays very specific Hg2+-induced colour change and fluorescent enhancement in the aqueous systems. The "turn-on" response of fluorescence is based on a binding-induced ring-opening process from the spirolactam (nonfluorescent) to acyclic xanthene (fluorescent) in rhodamine B. The coordinating atoms O-center dot-N-N-O-center dot from the hydroxymethyl-pyridine and rhodamine B hydrazide play dominant role in the formation of a complex with 1:1 stoichiometry of Hg2+ to 1. It exhibits a linear response in the range of 0.1-5 mu M with the limit of detection (LOD) of 15.7 nM (3 sigma/slope), while the calculated value of the association constant of Hg2+/1 is 0.70 x 10(5) M-1. Furthermore, confocal microscopy imaging experiment demonstrates the probe 1 can be applied as a fluorescent probe for visualization of Hg2+ in living HeLa cells.
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5.
  • Hu, Jiwen, et al. (author)
  • Ratiometric fluorogenic determination of endogenous hypochlorous acid in living cells
  • 2019
  • In: Spectrochimica Acta Part A - Molecular and Biomolecular Spectroscopy. - : PERGAMON-ELSEVIER SCIENCE LTD. - 1386-1425 .- 1873-3557. ; 219, s. 232-239
  • Journal article (peer-reviewed)abstract
    • Hypochlorous acid (HClO) is one of the most important ROS (reactive oxygen species) and common pollutant in tap-water. However, the determination of HClO with fast response and high sensitivity/selectivity is still an urgent demanding. Here we fabricated a ratiometric fluorescent probe RC based on TBET (through-bond energy transfer) on the platform of coumarin and rhodamine with the thiosemicarbazide group as the linker. This probe could display the characteristic fluorescence emission of coumarin. Upon addition of HClO, the linker was reacted into an oxadiazole, resulting in the opening of spiro-ring of rhodamine. The resultant then gives ratiometric fluorogenic changes. The probe exhibits fast response and high selectivity and sensitivity towards HClO with a low limit of detection (similar to 140 nM). Eventually, RC is successfully applicated for determining spiked HClO in water samples and imaging endogenous HClO in living cells. (C) 2019 Published by Elsevier B.V.
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6.
  • Hu, Jiwen, et al. (author)
  • Selective colorimetric detection of copper (II) by a protein-based nanoprobe
  • 2021
  • In: Spectrochimica Acta Part A - Molecular and Biomolecular Spectroscopy. - : PERGAMON-ELSEVIER SCIENCE LTD. - 1386-1425 .- 1873-3557. ; 252
  • Journal article (peer-reviewed)abstract
    • In this work, we report a novel protein-based nanoprobe (PNP) that can be employed for quantitative analysis of Cu2+ in pure water medium and real samples. Structurally, the proposed nanoprobe comprises a biofriendly protein (hen egg-white lysozyme (HEWL)) and a Cu2+-specific chromogenic agent, where HEWL acts as a nanocarrier encapsulating a structurally tailored rhodamine B derivate. The resulting PNP exhibits a hydrodynamic diameter of similar to 106 nm and efficiently disperses in water, enabling the detection of Cu2+ in pure aqueous systems without the aid of any organic co-solvents. The high sensitivity and selectivity of PNP allow the colorimetric detection of Cu2+ in the presence of other metal interferents with a low detection limit of 160 nM. The satisfying recovery of trace level Cu2+ in environmental samples demonstrate the great potential of employing PNP for the determination of Cu2+ in actual applications. Most importantly, the simple co-grinding method employing proteins and chromogenic agents provides a novel strategy to generate sensing systems that are useful detection of pollutants in aqueous samples. (C) 2021 Elsevier B.V. All rights reserved.
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7.
  • Hu, Jiwen, 1986-, et al. (author)
  • Selective detections of Hg2+ and F- by using tailor-made fluorogenic probes
  • 2018
  • In: Sensors and actuators. B, Chemical. - : Elsevier. - 0925-4005 .- 1873-3077. ; 269, s. 368-376
  • Journal article (peer-reviewed)abstract
    • By ingeniously using a (imino)coumarin-precursor, three reactive fluorogenic probes of MP, FP, and FMP have been fabricated in a single facile synthetic route. MP and FP are able to respectively act as selective "turn-on" fluorescent probes for detecting Hg2+ and F- in buffer solution via specific analyte-induced reactions. Linear ranges for the detection of Hg2+ and F- are 0-10 mu M and 0-100 mu M with the limits of detection (LODs) of 4.0 x 10(-8) M and 1.14 x 10(-6) M (3 delta/slope), respectively. FMP is able to work as a molecular "AND" logic gate-based fluorogenic probe for monitoring the coexistence of Hg2+ and F- via a multistep reaction cascade. The analytes-induced sensing mechanisms have been determined by using high-performance liquid chromatography analysis (HPLC). In addition, three probes show negligible toxicity under the experimental conditions, and are successfully used for monitoring Hg2+ and F- in living cells with good cell permeability. The success of the work demonstrates that ingenious utility of specific analyte-induced reactions and conventional concepts on the appropriate molecular scaffold can definitely deliver tailor-made probes for various intended sensing purposes. (C) 2018 Published by Elsevier B.V.
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8.
  • Hu, Zhang-Jun, et al. (author)
  • A facile "click" reaction to fabricate a FRET-based ratiometric fluorescent Cu2+ probe
  • 2014
  • In: Journal of materials chemistry. B. - : Royal Society of Chemistry. - 2050-750X .- 2050-7518. ; 2:28, s. 4467-4472
  • Journal article (peer-reviewed)abstract
    • A facile one-step Cu(I)-catalyzed "click" reaction, between a dansyl-azide and a propargyl-substituted rhodamine B hydrazide, is employed to fabricate a novel FRET ratiometric "off-on" fluorescent probe. The sensitive emission of the donor, a dansyl group, overlaps perfectly with the absorption of the acceptor, xanthene in the open-ring rhodamine. The proposed probe shows high selectivity towards Cu2+. The ratio of emission intensities at 568 and 540 nm (I-568/I-540) exhibits a drastic 28-fold enhancement upon addition of Cu2+. The probe shows an excellent linear relationship between emission ratios and the concentrations of Cu2+ from 10 to 50 mu M, with a detection limit (S/N = 3) of 0.12 mu M. The preliminary cellular studies demonstrated that the probe is cell membrane permeable and could be applied for ratiometric fluorescence imaging of intracellular Cu2+ with almost no cytotoxicity. The ingenuity of the probe design is to construct a FRET donor-acceptor interconnector and a selective receptor simultaneously by "click" reaction. The strategy was verified to have great potential for developing novel FRET probes for Cu2+.
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9.
  • Hu, Zhang-Jun, et al. (author)
  • A TPA-caged precursor of (imino)coumarin for "turn-on" fluorogenic detection of Cu
  • 2016
  • In: Analytica Chimica Acta. - : ELSEVIER SCIENCE BV. - 0003-2670 .- 1873-4324. ; 933, s. 189-195
  • Journal article (peer-reviewed)abstract
    • We strategize to utilize the precursors of (imino) coumarin fluorophores to deliver novel reactive Cu+ probes, where tris[(2-pyridyl)-methyl] amine (TPA) works as a reactive receptor towards Cu+. To verify this strategy, CP1, a representative probe and relevant sensing behaviors towards Cu+ are presented here. CP1 features good solubility and fast response for monitoring labile copper in aqueous solution and live cells. The sensing mechanism of CP1 is determined by HPLC titration and mass spectrometric analysis. The probe CP1 exhibits a 60-fold fluorescence enhancement and a detection limitation of 10.8 nM upon the detection of Cu+. CP1 is further applied for imaging labile copper in live cells. This work provides a starting point for future development of Cu+ probes, based on in situ formation of (imino) coumarin scaffolds, as well as their further investigations of copper signaling and biological events. (C) 2016 Elsevier B.V. All rights reserved.
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10.
  • Hu, Zhang-Jun, et al. (author)
  • Real-time visualizing the regulation of reactive oxygen species on Zn2+ release in cellular lysosome by a specific fluorescent probe
  • 2018
  • In: Sensors and actuators. B, Chemical. - : ELSEVIER SCIENCE SA. - 0925-4005 .- 1873-3077. ; 264, s. 419-425
  • Journal article (peer-reviewed)abstract
    • Reactive oxygen species (ROS) regulating the release of free zinc ions (Zn2+) in cellular lysosome is closely related to various pathways of cellular signal transduction, such as inflammation and oxidative stress. Directly visualizing Zn2+ release in lysosome is essential for in-depth understanding these physiological processes, and is still an atelic challenge. In this work, we successfully fabricate a lysosome-specific Zn2+ fluorescent probe and achieve the visualization of ROS-induced Zn2+ release in lysosome of inflammatory cells. The as-prepared probe combines a green fluorophore, an ionophore with five-dentate sites, and a morpholine as the lysosome-specific localization moiety. The fluorescence of the fluorophore in the free probe is suppressed by a photoinduced electron transfer (PET) process from nitrogen atoms in the ionophore. Upon the addition of Zn2+, the fluorescence can be promoted immediately, achieving the real-time detection. Meanwhile, the probe is sensitive and selective to Zn2+, which provides the capability to detect low-concentration of free Zn2+ in lysosomes. Accordingly, the Zn2+ release was clearly observed in lysosome with the increase of ROS levels when the inflammation occurred in living cells. (c) 2018 Published by Elsevier B.V.
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11.
  • Wang, Hong, et al. (author)
  • Real-time tracking of mitochondrial dynamics by a dual-sensitive probe
  • 2020
  • In: Sensors and actuators. B, Chemical. - : Elsevier. - 0925-4005 .- 1873-3077. ; 320
  • Journal article (peer-reviewed)abstract
    • Tracking of mitochondrial dynamic processes including their morphology, biogenesis and elimination is of significance to deeply understand mitochondrial physiology and related diseases, which requires simultaneous and discriminative labeling of both mitochondria themselves and correlated downstream organelles. However, the combination of multiple fluorescent probes will bring the large invasive effect that seriously impacts the normal physiological processes of mitochondria within live cells. To address this issue, we herein construct a single molecular probe through the combination of two pH-sensitive fluorogens, hydroxyl-coumarin and rhodamine B, enabling the detection of intracellular microenvironmental pH variations. Importantly, the as-synthesized probe not only accumulates into mitochondria, indicated by cyan emission from hydroxyl-coumarin but also can be delivered to the downstream acidic autolysosomes upon the occurrence of mitophagy, indicated by red emission from rhodamine B. Taking advantage of a two-channel confocal microscopy strategy, we have achieved to real-time track the processes of mitochondrial replication, merge and autophagy.
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12.
  • Yu, Weibin, et al. (author)
  • Facile preparation of sulfonated biochar for highly efficient removal of toxic Pb(II) and Cd(II) from wastewater
  • 2021
  • In: Science of the Total Environment. - : ELSEVIER. - 0048-9697 .- 1879-1026. ; 750
  • Journal article (peer-reviewed)abstract
    • Biochar is deemed as the ideal material for the effective removal of heavy metals in wastewater treatment. Herein, we developed a facile one-step solvothermal method for the preparation of sulfonated biochar (SBC) from Axonopus compressus under a low-temperature condition. FTIR and XPS analysis demonstrate that plenty of -OH, -COOH and -SO3H moieties are generated on the surface of SBC during the sulfonation process. Due to high electronegativity and strong complexation of these moieties, SBC can rapidly adsorb Pb(II) and Cd(II) with capacities of 191.07 and 85.76 mg/g respectively within 5 min. SBC can be reused for 5 cycles with a negligible loss of adsorption capacity. In addition, different biomass-based biochars are prepared under the identical experimental conditions, and they are successfully applied in the treatments of Pb(II) and Cd(II). The satisfying results indicate that one-step low-temperature sulfonation could be a universalmethod, and various types of biomass waste could be the abundant, effective, economical material source for the treatment of environmental heavy metal pollution in future. (C) 2020 Elsevier B.V. All rights reserved.
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13.
  • Zhang, Xin, et al. (author)
  • A ratiometric fluorogenic nanoprobe for real-time quantitative monitoring of lysosomal pH
  • 2021
  • In: Sensors and actuators. B, Chemical. - : Elsevier Science SA. - 0925-4005 .- 1873-3077. ; 345
  • Journal article (peer-reviewed)abstract
    • Lysosomes are known as key players in cellular signalling and act as terminal degradation stations involved in a multitude of cellular processes. Being a highly influential physiological factor, pH is essential in the regulation of lysosome-mediated physiological and pathological processes. Aberrant pH fluctuations are highly related to lysosomal dysfunction that correlates to lysosomal storage diseases and neurodegenerative disorders. As such, real-time quantitative monitoring of lysosomal pH (pHL) is crucial for gaining insight into lysosomal dysfunction but challenging by the lack of effective lysosome-specific probes with high signal fidelity. Toward this end, we have proposed a lysosomal fluorogenic nanoprobe (TR-MP) for reliable ratiometric measuring of pHL. It is fabricated by rational manipulation of fluorescence resonance energy transfer (FRET) in a tailorable nanoplatform. The nanoprobe consists of biocompatible silica nanoparticles assembled with a pH-sensitive rhodamine derivative (RDM-TEOS) as an acceptor and aggregation-induced emission (AIE) fluorophore (TPE-OMe) as a donor to ensure high energy transfer efficiency. Further equipped with cell-penetrating facilitator and morpholine to enable effective cell-internalization and high lysosome affinity of TR-MP. Results show that TR-MP can quantitatively measure pH in a range of 3.0 - 7.0 and detect pHL fluctuations in live cells under various stimuli, as well as real-time monitor pHL during apoptosis.
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14.
  • Zhang, Xin, et al. (author)
  • Light-Up Lipid Droplets Dynamic Behaviors Using a Red-Emitting Fluorogenic Probe
  • 2020
  • In: Analytical Chemistry. - : AMER CHEMICAL SOC. - 0003-2700 .- 1520-6882. ; 92:5, s. 3613-3619
  • Journal article (peer-reviewed)abstract
    • Intracellular lipid metabolism occurs in lipid droplets (LDs), which is critical to the survival of cells. Imaging LDs is an intuitive way to understand their physiology in live cells. However, this is limited by the availability of specific probes that can properly visualize LDs in vivo. Here, an LDs-specific red-emitting probe is proposed to address this need, which is not merely with an ultrahigh signal-to-noise (S/N) ratio and a large Stokes shift (up to 214 nm) but also with superior resistance to photobleaching. The probe has been successfully applied to real-time tracking of intracellular LDs behaviors, including fusion, migration, and lipophagy processes. We deem that the proposed probe here offers a new possibility for deeper understanding of LDs-associated behaviors, elucidation of their roles and mechanisms in cellular metabolism, and determination of the transition between adaptive lipid storage and lipotoxicity as well.
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15.
  • zhang, xin, 1990-, et al. (author)
  • Single-wavelength-excited fluorogenic nanoprobe for accurate real-time ratiometric analysis of broad pH fluctuations in mitophagy
  • 2022
  • In: Nano Reseach. - : Tsinghua University Press. - 1998-0124 .- 1998-0000. ; 15, s. 6515-6521
  • Journal article (peer-reviewed)abstract
    • Mitophagy has a critical role in maintaining cellular homeostasis through acidic lysosomes engulfing excess or impaired mitochondria, thereby pH fluctuation is one of the most significant indicators for tracking mitophagy. Then such precise pH tracking demands the fluorogenic probe that has tailored contemporaneous features, including mitochondrial-specificity, excellent biocompatibility, wide pH-sensitive range of 8.0-4.0, and especially quantitative ability. However, available molecular probes cannot simultaneously meet all the requirements since it is extremely difficult to integrate multiple functionalities into a single molecule. To fully address this issue, we herein integrate two fluorogenic pH sensitive units, a mitochondria-specific block, cell-penetrating facilitator, and biocompatible segments into an elegant silica nano scaffold, which greatly ensures the applicability for real-time tracking of pH fluctuations in mitophagy. Most significantly, at a single wavelength excitation, the integrated pH-sensitive units have spectra-distinguishable fluorescence towards alkaline and acidic pH in a broad range that covers mitochondrial and lysosomal pH, thus enabling a ratiometric analysis of pH variations during the whole mitophagy. This work also provides constructive insights into the fabrication of advanced fluorescent nanoprobes for diverse biomedical applications.
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16.
  • Zhang, Xin, et al. (author)
  • Tailorable Membrane-Penetrating Nanoplatform for Highly Efficient Organelle-Specific Localization
  • 2021
  • In: Small. - : Wiley-V C H Verlag GMBH. - 1613-6810 .- 1613-6829. ; 17:31
  • Journal article (peer-reviewed)abstract
    • Given the breadth of currently arising opportunities and concerns associated with nanoparticles for biomedical imaging, various types of nanoparticles have been widely exploited, especially for cellular/subcellular level probing. However, most currently reported nanoparticles either have inefficient delivery into cells or lack specificity for intracellular destinations. The absence of well-defined nanoplatforms remains a critical challenge hindering practical nano-based bio-imaging. Herein, the authors elaborate on a tailorable membrane-penetrating nanoplatform as a carrier with encapsulated actives and decorated surfaces to tackle the above-mentioned issues. The tunable contents in such a versatile nanoplatform offer huge flexibility to reach the expected properties and functions. Aggregation-induced emission luminogen (AIEgen) is applied to achieve sought-after photophysical properties, specific targeting moieties are installed to give high affinity towards different desired organelles, and critical grafting of cell-penetrating cyclic disulfides (CPCDs) to promote cellular uptake efficiency without sacrificing the specificity. Hereafter, to validate its practicability, the tailored nano products are successfully applied to track the dynamic correlation between mitochondria and lysosomes during autophagy. The authors believe that the strategy and described materials can facilitate the development of functional nanomaterials for various life science applications.
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