Publications by authors named "Zhangjun Hu"

37 Publications

Tailorable Membrane-Penetrating Nanoplatform for Highly Efficient Organelle-Specific Localization.

Small 2021 Aug 25;17(31):e2101440. Epub 2021 Jun 25.

Department of Physics, Chemistry, and Biology (IFM), Linköping University, Linköping, SE581 83, Sweden.

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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http://dx.doi.org/10.1002/smll.202101440DOI Listing
August 2021

Impact of Amine Additives on Perovskite Precursor Aging: A Case Study of Light-Emitting Diodes.

J Phys Chem Lett 2021 Jul 17;12(25):5836-5843. Epub 2021 Jun 17.

Department of Physics Chemistry and Biology (IFM), Linköping University, Linköping SE-58183, Sweden.

Amines are widely employed as additives for improving the performance of metal halide perovskite optoelectronic devices. However, amines are well-known for their high chemical reactivity, the impact of which has yet to receive enough attention from the perovskite light-emitting diode community. Here, by investigating an unusual positive aging effect of CHNHI/CsI/PbI precursor solutions as an example, we reveal that amines gradually undergo N-formylation in perovskite precursors over time. This reaction is initialized by hydrolysis of dimethylformamide in the acidic chemical environment. Further investigations suggest that the reaction products collectively impact perovskite crystallization and eventually lead to significantly enhanced external quantum efficiency values, increasing from ∼2% for fresh solutions to ≳12% for aged ones. While this case study provides a positive aging effect, a negative aging effect is possible in other perovksite systems. Our findings pave the way for more reliable and reproducible device fabrication and call for further attention to underlying chemical reactions within the perovskite inks once amine additives are included.
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http://dx.doi.org/10.1021/acs.jpclett.1c01349DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC8256416PMC
July 2021

Hierarchical CoFe LDH/MOF nanorods array with strong coupling effect grown on carbon cloth enables efficient oxidation of water and urea.

Nanotechnology 2021 Jul 2;32(38). Epub 2021 Jul 2.

School of Environmental and Chemical Engineering, Shanghai University, Shanghai 200444, People's Republic of China.

Oxygen evolution reaction (OER) and urea oxidation reaction (UOR) play important roles in the fields of hydrogen energy production and pollution treatment. Herein, a facile one-step chemical etching strategy is provided for fabricating one-dimensional hierarchical nanorods array composed of CoFe layered double hydroxide (LDH)/metal-organic frameworks (MOFs) supported on carbon cloth as efficient and stable OER and UOR catalysts. By precisely controlling the etching rate, the ligands from Co-MOFs are partially removed, the corresponding metal centers then coordinate with hydroxyl ions to generate ultrathin amorphous CoFe LDH nanosheets. The resultant CoFe LDH/MOFs catalyst possesses large active surface area, enhanced conductivity and extended electron/mass transfer channels, which are beneficial for catalytic reactions. Additionally, the intimate contact between CoFe LDH and MOFs modulates the local electronic structure of the catalytic active site, leading to enhanced adsorption of oxygen-containing intermediates to facilitate fast electrocatalytic reaction. As a result, the optimized CoFe LDH/MOF-0.06 exhibits superior OER activity with a low overpotential of 276 at a current density of 10 mA cmwith long-term durability. Additionally, it merely requires a voltage of 1.45 V to obtain 10 mA cmin 1 M KOH solution with 0.33 urea and is 56 mV lower than the one in pure KOH. The work presented here may hew out a brand-new route to construct multi-functional electrocatalysts for water splitting, COreduction, nitrogen reduction reactions and so on.
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http://dx.doi.org/10.1088/1361-6528/ac0b65DOI Listing
July 2021

Selective colorimetric detection of copper (II) by a protein-based nanoprobe.

Spectrochim Acta A Mol Biomol Spectrosc 2021 May 13;252:119462. Epub 2021 Jan 13.

Department of Physics, Chemistry and Biology, Linköping University, Linköping 58183, Sweden.

In this work, we report a novel protein-based nanoprobe (PNP) that can be employed for quantitative analysis of Cu in pure water medium and real samples. Structurally, the proposed nanoprobe comprises a biofriendly protein (hen egg-white lysozyme (HEWL)) and a Cu-specific chromogenic agent, where HEWL acts as a nanocarrier encapsulating a structurally tailored rhodamine B derivate. The resulting PNP exhibits a hydrodynamic diameter of ~ 106 nm and efficiently disperses in water, enabling the detection of Cu in pure aqueous systems without the aid of any organic co-solvents. The high sensitivity and selectivity of PNP allow the colorimetric detection of Cu in the presence of other metal interferents with a low detection limit of 160 nM. The satisfying recovery of trace level Cu in environmental samples demonstrate the great potential of employing PNP for the determination of Cu 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.
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http://dx.doi.org/10.1016/j.saa.2021.119462DOI Listing
May 2021

Facile preparation of sulfonated biochar for highly efficient removal of toxic Pb(II) and Cd(II) from wastewater.

Sci Total Environ 2021 Jan 6;750:141545. Epub 2020 Aug 6.

College of Environmental Science and Engineering, Tongji University, Shanghai 200092, China.

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 -SOH 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 universal method, and various types of biomass waste could be the abundant, effective, economical material source for the treatment of environmental heavy metal pollution in future.
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http://dx.doi.org/10.1016/j.scitotenv.2020.141545DOI Listing
January 2021

Efficient and High-Luminance Perovskite Light-Emitting Diodes Based on CsPbBr Nanocrystals Synthesized from a Dual-Purpose Organic Lead Source.

Small 2020 Nov 26;16(46):e2003939. Epub 2020 Oct 26.

School of Materials and Energy, University of Electronic Science and Technology of China, Chengdu, 611731, P. R. China.

Rational engineering of the surface properties of perovskite nanocrystals (PeNCs) is critical to obtain light emitters with simultaneous high photoluminescence efficiency and excellent charge transport properties for light-emitting diodes (LEDs). However, the commonly used lead halide sources make it hard to rationally optimize the surface compositions of the PeNCs. In addition, previously developed ligand engineering strategies for conventional inorganic nanocrystals easily deteriorate surface properties of the PeNCs, bringing additional difficulties in optimizing their optoelectronic properties. In this work, a novel strategy of employing a dual-purpose organic lead source for the synthesis of highly luminescent PeNCs with enhanced charge transport property is developed. Lead naphthenate (Pb(NA) ), of which the metal ions work as lead sources while the naphthenate can function as the surface ligands afterward, is explored and the obtained products under different synthesis conditions are comprehensively investigated. Monodispersed cesium lead bromide (CsPbBr ) with controllable size and excellent optical properties, showing superior photoluminescence quantum yields up to 80%, is obtained. Based on the simultaneously enhanced electrical properties of the Pb(NA) -derived PeNCs, the resultant LEDs demonstrate a high peak external quantum efficiency of 8.44% and a superior maximum luminance of 31 759 cd cm .
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http://dx.doi.org/10.1002/smll.202003939DOI Listing
November 2020

Rapid detection of mercury (II) ions and water content by a new rhodamine B-based fluorescent chemosensor.

Spectrochim Acta A Mol Biomol Spectrosc 2020 Nov 30;241:118657. Epub 2020 Jun 30.

School of Environmental and Chemical Engineering, Shanghai University, Shanghai 200444, PR China; Division of Molecular Surface Physics & Nanoscience, Department of Physics, Chemistry and Biology, Linköping University, Linköping 58183, Sweden. Electronic address:

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 Hg. In the presence of Hg, the resulting red-orange fluorescence (under UV light) and naked eye red color of RS are supposed to be used for quantitative and qualitative measurement of Hg. Further fluorescent titration and analysis demonstrate that RS can selectively detect Hg within 1 s with a low limit of detection (LOD) of 16 nM in acetonitrile media, meanwhile, the association constant (K) was calculated to be 0.32 × 10 M. More importantly, the resultant complex (RSHg) of RS and Hg has also been successfully applied to detect limited water content in acetonitrile solution.
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http://dx.doi.org/10.1016/j.saa.2020.118657DOI Listing
November 2020

A Multi-responsive Fluorescent Probe Reveals Mitochondrial Nucleoprotein Dynamics with Reactive Oxygen Species Regulation through Super-resolution Imaging.

Angew Chem Int Ed Engl 2020 09 13;59(37):16154-16160. Epub 2020 Jul 13.

School of Chemistry and Chemical Engineering and Institute of Physical Science and Information Technology, Anhui University, Hefei, Anhui, 230601, China.

Understanding the biomolecular interactions in a specific organelle has been a long-standing challenge because it requires super-resolution imaging to resolve the spatial locations and dynamic interactions of multiple biomacromolecules. Two key difficulties are the scarcity of suitable probes for super-resolution nanoscopy and the complications that arise from the use of multiple probes. Herein, we report a quinolinium derivative probe that is selectively enriched in mitochondria and switches on in three different fluorescence modes in response to hydrogen peroxide (H O ), proteins, and nucleic acids, enabling the visualization of mitochondrial nucleoprotein dynamics. STED nanoscopy reveals that the proteins localize at mitochondrial cristae and largely fuse with nucleic acids to form nucleoproteins, whereas increasing H O level leads to disassociation of nucleic acid-protein complexes.
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http://dx.doi.org/10.1002/anie.202005959DOI Listing
September 2020

Integrated Design of Hierarchical [email protected]@[email protected] Nanobox as Anode Material for Enhanced Lithium Storage Performance.

ACS Appl Mater Interfaces 2020 Apr 17;12(17):19768-19777. Epub 2020 Apr 17.

Shanghai Applied Radiation Institute, School of Environmental and Chemical Engineering, Shanghai University, Shanghai 200444, China.

Transition-metal oxides (TMOs) are potential candidates for anode materials of lithium-ion batteries (LIBs) due to their high theoretical capacity (∼1000 mA h/g) and enhanced safety from suppressing the formation of lithium dendrites. However, the poor electron conductivity and the large volume expansion during lithiation/delithiation processes are still the main hurdles for the practical usage of TMOs as anode materials. In this work, the [email protected]@[email protected] hierarchical nanobox (CNMN) is then proposed and fabricated to solve those issues. The as-prepared nanobox contains hollow cubic CoSnO as a core and dual N-doped carbon-"sandwiched" MnO particles as a shell. As anode materials of LIBs, the hollow and carbon interlayer structures effectively accommodate the volume expansion while dual active TMOs of CoSnO and MnO efficiently increase the specific capacity. Notably, the dual-layer structure of N-doped carbons plays a critical functional role in the incorporated composites, where the inner layer serves as a reaction substrate and a spatial barrier and the outer layer offers electron conductivity, enabling more effective involvement of active anode materials in lithium storage, as well as maintaining their high activity during lithium cycling. Subsequently, the as-prepared CNMN exhibits a high specific capacity of 1195 mA h/g after the 200th cycle at 0.1C and an excellent stable reversible capacity of about 876 mA h/g after the 300th cycle at 0.5C with only 0.07 mA h/g fade per cycle after 300 cycles. Even after a 250 times fast charging/discharging cycle both at 5C, it still retains a reversible capacity of 422.6 mA h/g. We ascribe the enhanced lithium storage performances to the novel hierarchical architectures achieved from the rational design.
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http://dx.doi.org/10.1021/acsami.9b22368DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7304665PMC
April 2020

Perovskite-molecule composite thin films for efficient and stable light-emitting diodes.

Nat Commun 2020 Feb 14;11(1):891. Epub 2020 Feb 14.

Department of Physics, Chemistry, and Biology (IFM), Linköping University, Linköping, 58183, Sweden.

Although perovskite light-emitting diodes (PeLEDs) have recently experienced significant progress, there are only scattered reports of PeLEDs with both high efficiency and long operational stability, calling for additional strategies to address this challenge. Here, we develop perovskite-molecule composite thin films for efficient and stable PeLEDs. The perovskite-molecule composite thin films consist of in-situ formed high-quality perovskite nanocrystals embedded in the electron-transport molecular matrix, which controls nucleation process of perovskites, leading to PeLEDs with a peak external quantum efficiency of 17.3% and half-lifetime of approximately 100 h. In addition, we find that the device degradation mechanism at high driving voltages is different from that at low driving voltages. This work provides an effective strategy and deep understanding for achieving efficient and stable PeLEDs from both material and device perspectives.
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http://dx.doi.org/10.1038/s41467-020-14747-6DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7021679PMC
February 2020

Light-Up Lipid Droplets Dynamic Behaviors Using a Red-Emitting Fluorogenic Probe.

Anal Chem 2020 03 24;92(5):3613-3619. Epub 2020 Feb 24.

Department of Physics, Chemistry and Biology, Linköping University, Linköping 58183, Sweden.

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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http://dx.doi.org/10.1021/acs.analchem.9b04410DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7307831PMC
March 2020

Well-defined [email protected] hollow heterostructured nanocubes with enhanced dissociation kinetics for overall water splitting.

Nanoscale 2020 Jan 11;12(1):326-335. Epub 2019 Dec 11.

Shanghai Electrochemical Energy Devices Research Center, School of Chemistry and Chemical Engineering and State Key Laboratory of Metal Matrix Composites, Shanghai Jiao Tong University, Shanghai, 200240, China.

Hollow heterostructures have tremendous advantages in electrochemical energy storage and conversion areas due to their unique structure and composition characteristics. Here, we report the controlled synthesis of hollow CoSe nanocubes decorated with ultrathin MoSe nanosheets ([email protected]) as an efficient and robust bifunctional electrocatalyst for overall water splitting in a wide pH range. It is found that integrating ultrathin MoS nanosheets with hollow CoSe nanocubes can provide abundant active sites, promote electron/mass transfer and bubble release and facilitate the migration of charge carriers. Additionally, the surface electron coupling in the heterostructures enables it to serve as a source of sites for H and/or OH adsorption, thus reducing the activation barrier for water molecules adsorption and dissociation. As a result, the title compound, [email protected] hollow heterostructures, exhibits an overpotential of 183 mV and 309 mV at a current density of 10 mA cm toward hydrogen evolution reactions and oxygen evolution reactions in 1.0 M KOH, respectively. When applied as both cathode and anode for overall water splitting, a low battery voltage of 1.524 V is achieved along with excellent stability for at least 12 h. This work provides a new idea for the design and synthesis of high-performance catalysts for electrochemical energy storage and conversion.
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http://dx.doi.org/10.1039/c9nr08751fDOI Listing
January 2020

High-Quality Ruddlesden-Popper Perovskite Films Based on In Situ Formed Organic Spacer Cations.

Adv Mater 2019 Oct 28;31(41):e1904243. Epub 2019 Aug 28.

Department of Physics, Chemistry, and Biology (IFM), Linköping University, Linköping, SE-58183, Sweden.

Ruddlesden-Popper perovskites (RPPs), consisting of alternating organic spacer layers and inorganic layers, have emerged as a promising alternative to 3D perovskites for both photovoltaic and light-emitting applications. The organic spacer layers provide a wide range of new possibilities to tune the properties and even provide new functionalities for RPPs. However, the preparation of state-of-the-art RPPs requires organic ammonium halides as the starting materials, which need to be ex situ synthesized. A novel approach to prepare high-quality RPP films through in situ formation of organic spacer cations from amines is presented. Compared with control devices fabricated from organic ammonium halides, this new approach results in similar (and even better) device performance for both solar cells and light-emitting diodes. High-quality RPP films are fabricated based on different types of amines, demonstrating the universality of the approach. This approach not only represents a new pathway to fabricate efficient devices based on RPPs, but also provides an effective method to screen new organic spacers with further improved performance.
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http://dx.doi.org/10.1002/adma.201904243DOI Listing
October 2019

Porous ZnO/CoO/N-doped carbon nanocages synthesized via pyrolysis of complex metal-organic framework (MOF) hybrids as an advanced lithium-ion battery anode.

Acta Crystallogr C Struct Chem 2019 Jul 18;75(Pt 7):969-978. Epub 2019 Jun 18.

School of Environmental and Chemical Engineering, Shanghai University, Shangda Road 99, Shanghai 200444, People's Republic of China.

Metal oxides have a large storage capacity when employed as anode materials for lithium-ion batteries (LIBs). However, they often suffer from poor capacity retention due to their low electrical conductivity and huge volume variation during the charge-discharge process. To overcome these limitations, fabrication of metal oxides/carbon hybrids with hollow structures can be expected to further improve their electrochemical properties. Herein, ZnO-CoO nanocomposites embedded in N-doped carbon ([email protected]) nanocages with hollow dodecahedral shapes have been prepared successfully by the simple carbonizing and oxidizing of metal-organic frameworks (MOFs). Benefiting from the advantages of the structural features, i.e. the conductive N-doped carbon coating, the porous structure of the nanocages and the synergistic effects of different components, the as-prepared [email protected] not only avoids particle aggregation and nanostructure cracking but also facilitates the transport of ions and electrons. As a result, the resultant [email protected] shows a discharge capacity of 2373 mAh g at the first cycle and exhibits a retention capacity of 1305 mAh g even after 300 cycles at 0.1 A g. In addition, a reversible capacity of 948 mAh g is obtained at a current density of 2 A g, which delivers an excellent high-rate cycle ability.
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http://dx.doi.org/10.1107/S2053229619008222DOI Listing
July 2019

Unveiling the synergistic effect of precursor stoichiometry and interfacial reactions for perovskite light-emitting diodes.

Nat Commun 2019 Jun 27;10(1):2818. Epub 2019 Jun 27.

Department of Physics, Chemistry and Biology (IFM), Linköping University, Linköping, SE-58183, Sweden.

Metal halide perovskites are emerging as promising semiconductors for cost-effective and high-performance light-emitting diodes (LEDs). Previous investigations have focused on the optimisation of the emissive perovskite layer, for example, through quantum confinement to enhance the radiative recombination or through defect passivation to decrease non-radiative recombination. However, an in-depth understanding of how the buried charge transport layers affect the perovskite crystallisation, though of critical importance, is currently missing for perovskite LEDs. Here, we reveal synergistic effect of precursor stoichiometry and interfacial reactions for perovskite LEDs, and establish useful guidelines for rational device optimization. We reveal that efficient deprotonation of the undesirable organic cations by a metal oxide interlayer with a high isoelectric point is critical to promote the transition of intermediate phases to highly emissive perovskite films. Combining our findings with effective defect passivation of the active layer, we achieve high-efficiency perovskite LEDs with a maximum external quantum efficiency of 19.6%.
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http://dx.doi.org/10.1038/s41467-019-10612-3DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC6597563PMC
June 2019

Construction of SnS-SnO heterojunctions decorated on graphene nanosheets with enhanced visible-light photocatalytic performance.

Acta Crystallogr C Struct Chem 2019 Jun 29;75(Pt 6):812-821. Epub 2019 May 29.

School of Environmental and Chemical Engineering, Shanghai University, ShangDa Road 99, Shanghai 200444, People's Republic of China.

Heterostructures formed by the growth of one kind of nanomaterial in/on another have attracted increasing attention due to their microstructural characteristics and potential applications. In this work, SnS-SnO heterostructures were successfully prepared by a facile hydrothermal method. Due to the enhanced visible-light absorption and efficient separation of photo-generated holes and electrons, the SnS-SnO heterostructures display excellent photocatalytic performance for the degradation of rhodamine (RhB) under visible-light irradiation. Additionally, it is found that the introduction of graphene into the heterostructures further improved photocatalytic activity and stability. In particular, the optimized SnS-SnO/graphene photocatalyst can degrade 97.1% of RhB within 60 min, which is about 1.38 times greater than that of SnS-SnO heterostructures. This enhanced photocatalytic activity could be attributed to the high surface area and the excellent electron accepting and transporting properties of graphene, which served as an acceptor of the generated electrons to suppress charge recombination. These results provide a new insight for the design and development of hybrid photocatalysts.
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http://dx.doi.org/10.1107/S2053229619006399DOI Listing
June 2019

Ratiometric fluorogenic determination of endogenous hypochlorous acid in living cells.

Spectrochim Acta A Mol Biomol Spectrosc 2019 Aug 15;219:232-239. Epub 2019 Apr 15.

School of Environmental and Chemical Engineering, Shanghai University, Shanghai, 200444, PR China; Division of Molecular Surface Physics & Nanoscience, Department of Physics, Chemistry and Biology, Linköping University, Linköping 58183, Sweden. Electronic address:

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 (~140 nM). Eventually, RC is successfully applicated for determining spiked HClO in water samples and imaging endogenous HClO in living cells.
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http://dx.doi.org/10.1016/j.saa.2019.04.024DOI Listing
August 2019

Hybrid Rhodamine Fluorophores in the Visible/NIR Region for Biological Imaging.

Angew Chem Int Ed Engl 2019 10 11;58(40):14026-14043. Epub 2019 Jun 11.

Key Laboratory of Flexible Electronics (KLOFE) & Institute of Advanced Materials (IAM), Jiangsu National Synergetic Innovation Center for Advanced Materials (SICAM), Nanjing Tech University, Nanjing, 211816, P. R. China.

Fluorophores and probes are invaluable for the visualization of the location and dynamics of gene expression, protein expression, and molecular interactions in complex living systems. Rhodamine dyes are often used as scaffolds in biological labeling and turn-on fluorescence imaging. To date, their absorption and emission spectra have been expanded to cover the entire near-infrared region (650-950 nm), which provides a more suitable optical window for monitoring biomolecular production, trafficking, and localization in real time. This review summarizes the development of rhodamine fluorophores since their discovery and provides strategies for modulating their absorption and emission spectra to generate specific bathochromic-shifts. We also explain how larger Stokes shifts and dual-emissions can be obtained from hybrid rhodamine dyes. These hybrid fluorophores can be classified into various categories based on structural features including the alkylation of amidogens, the substitution of the O atom of xanthene, and hybridization with other fluorophores.
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http://dx.doi.org/10.1002/anie.201901061DOI Listing
October 2019

Environmentally benign synthesis of CoO-SnO heteronanorods with efficient photocatalytic performance activated by visible light.

J Colloid Interface Sci 2019 Apr 22;542:460-468. Epub 2019 Jan 22.

School of Environmental and Chemical Engineering, Shanghai University, Shanghai 200444, People's Republic of China. Electronic address:

One-dimensional (1D) heterostructured photocatalysts with controllable texture properties and compositions have attracted increasing interest owing to their unique optical, structural, and electronic advantages. Herein, 1D CoO-SnO heteronanorods were rationally designed and synthesized through a facile solution-based approach. Benefiting from both of their heterostructural and compositional characteristics, the resulting CoO-SnO heteronanorods exhibit high photocatalytic performance for the degradation of Rhodamine B (RhB) under visible-light irridation. In particular, the photocatalyst with a CoO/SnO mass ratio of 1:1 provides the best photocatalytic performance, which can degrade 90% RhB within 120 min. Besides, several reaction parameters affecting RhB degradation, such as churning time, calcination temperature and pH value, are investigated in detail. The enhanced photocatalytic activity can be attributed to the broadening of absorption spectrum to visible-light regions and the efficient charge separation of photogenerated electron-hole pairs due to the formed p-n heterojunctions. The strategy reported here can be able to expand to fabricate other heterostructured photocatalysts for practical applications in the fields of photocatalysis, water splitting, and solar cells.
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http://dx.doi.org/10.1016/j.jcis.2019.01.089DOI Listing
April 2019

Construction of Ni-doped SnO-SnS heterojunctions with synergistic effect for enhanced photodegradation activity.

J Hazard Mater 2019 Apr 7;368:204-213. Epub 2019 Jan 7.

School of Environmental and Chemical Engineering, Shanghai University, Shanghai 200444, People's Republic of China. Electronic address:

Construction of heterostructures with proper band alignment and effective transport and separation of photogenerated charges is highly expected for photocatalysis. In this work, Ni-doped SnO-SnS heterostructures (NiSnSO) are simply prepared by thermal oxidation of Ni-doped hierarchical SnS microspheres in the air. When applied for the photodegradation of organic contaminants, these NiSnSO exhibit excellent catalytic performance and stability due to the following advantages: (1) Ni doping leads to the enhancement of light harvesting of SnS in the visible light regions; (2) the formed heterojunctions promote the transport and separation of photogenerated electrons from SnS to SnO; (3) Ni-SnO quantum dots facilitate the enrichment of reactants, provide more reactive centers and accelerate product diffusion in the reactive centers; (4) the SnS hierarchical microspheres constituted by nanoplates provide abundant active sites, high structural void porosity and accessible inner surface to faciliate the catalytic reactions. As a result, the optimized NiSnSO can photodegrade 92.7% methyl orange within 80 min under the irradiation of simulated sunlight, greatly higher than those of pure SnS (29.8%) and Ni-doped SnS (52.1%). These results reveal that the combination of heteroatom doping and heterostructure fabrication is a very promising strategy to deliver nanomaterials for effectively photocatalytic applications.
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http://dx.doi.org/10.1016/j.jhazmat.2019.01.009DOI Listing
April 2019

Gasotransmitter Regulation of Phosphatase Activity in Live Cells Studied by Three-Channel Imaging Correlation.

Angew Chem Int Ed Engl 2019 02 21;58(8):2261-2265. Epub 2019 Jan 21.

School of Chemistry and Chemical Engineering, and, Institute of Physical Science and Information Technology, Anhui University, Hefei, Anhui, 230601, China.

Enzyme activity in live cells is dynamically regulated by small-molecule transmitters for maintaining normal physiological functions. A few probes have been devised to measure intracellular enzyme activities by fluorescent imaging, but the study of the regulation of enzyme activity via gasotransmitters in situ remains a long-standing challenge. Herein, we report a three-channel imaging correlation by a single dual-reactive fluorescent probe to measure the dependence of phosphatase activity on the H S level in cells. The two sites of the probe reactive to H S and phosphatase individually produce blue and green fluorescent responses, respectively, and resonance energy transfer can be triggered by their coexistence. Fluorescent analysis based on the three-channel imaging correlation shows that cells have an ideal level of H S to promote phosphatase activity up to its maximum. Significantly, a slight deviation from this H S level leads to a sharp decrease of phosphatase activity. The discovery further strengthens our understanding of the importance of H S in cellular signaling and in various human diseases.
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http://dx.doi.org/10.1002/anie.201811391DOI Listing
February 2019

A water-soluble "turn-on" fluorescent probe for specifically imaging mitochondria viscosity in living cells.

Spectrochim Acta A Mol Biomol Spectrosc 2018 Oct 30;203:127-131. Epub 2018 May 30.

Division of Molecular Surface Physics & Nanoscience, Department of Physics, Chemistry and Biology (IFM), Linköping University, 58183 Linköping, Sweden.

Rational design of water-soluble probes for mitochondrial viscosity in practical biological applications remains a challenge. Herein, we described a novel hydro soluble benzothiazole salt derivative MitoSN, which exhibits specifically response and singular sensitivity to the mitochondria viscosity in living Hela cells. MitoSN displays an excellent fluorescence enhancement (ca. 35-fold) with the increase of the viscosity in the water-glycerol system. Moreover, confocal microscopy indicates that MitoSN is sensitive to the local viscosity and selectively stains mitochondria, the body of zebrafish as well. Importantly, MitoSN is capable to identify the viscosity difference of mitochondria in normal and nystatin treated Hela cells. The work provides a useful tool to monitor the changes of viscosity in the mitochondrial microenvironment.
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http://dx.doi.org/10.1016/j.saa.2018.05.121DOI Listing
October 2018

Cerium oxide nanoparticles with antioxidant capabilities and gadolinium integration for MRI contrast enhancement.

Sci Rep 2018 05 3;8(1):6999. Epub 2018 May 3.

Division of Molecular Surface Physics and Nanoscience, Department of Physics, Chemistry and Biology (IFM), Linköping University, SE-581 83, Linköping, Sweden.

The chelating gadolinium-complex is routinely used as magnetic resonance imaging (MRI) -contrast enhancer. However, several safety issues have recently been reported by FDA and PRAC. There is an urgent need for the next generation of safer MRI-contrast enhancers, with improved local contrast and targeting capabilities. Cerium oxide nanoparticles (CeNPs) are designed with fractions of up to 50% gadolinium to utilize the superior MRI-contrast properties of gadolinium. CeNPs are well-tolerated in vivo and have redox properties making them suitable for biomedical applications, for example scavenging purposes on the tissue- and cellular level and during tumor treatment to reduce in vivo inflammatory processes. Our near edge X-ray absorption fine structure (NEXAFS) studies show that implementation of gadolinium changes the initial co-existence of oxidation states Ce and Ce of cerium, thereby affecting the scavenging properties of the nanoparticles. Based on ab initio electronic structure calculations, we describe the most prominent spectral features for the respective oxidation states. The as-prepared gadolinium-implemented CeNPs are 3-5 nm in size, have r-relaxivities between 7-13 mM s and show clear antioxidative properties, all of which means they are promising theranostic agents for use in future biomedical applications.
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http://dx.doi.org/10.1038/s41598-018-25390-zDOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC5934375PMC
May 2018

A novel Schiff base derivative: Synthesis, two-photon absorption properties and application for bioimaging.

Spectrochim Acta A Mol Biomol Spectrosc 2018 Jun 13;198:304-308. Epub 2018 Mar 13.

Division of Molecular Surface Physics & Nanoscience, Department of Physics, Chemistry and Biology (IFM), Linköing University, 58183 Linköing, Sweden. Electronic address:

A novel donor-π-acceptor-π-donor type (D-π-A-π-D') Schiff base derivative (L) has been designed and synthesized. The structure of L is confirmed by single-crystal X-ray diffraction analysis as well. The photophysical properties of compound L were comprehensively investigated by using both experimental and theoretical methods. The results indicate that L exhibits large Stokes shift and moderate two-photon action (2PA) cross-section in the near infrared (NIR) region. Furthermore, the confocal microscopy imaging study demonstrates that compound L could penetrate into cells and target the cellular mitochondria compartment. Due to its low cytotoxicity, compound L provides a promising tool for directly lighting up the mitochondria compartment in living HepG2 cells.
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http://dx.doi.org/10.1016/j.saa.2018.03.039DOI Listing
June 2018

Encapsulating CoS-CoSe heterostructured nanocrystals in N-doped carbon nanocubes as highly efficient counter electrodes for dye-sensitized solar cells.

Dalton Trans 2018 Apr;47(15):5236-5244

School of Environmental and Chemical Engineering, Shanghai University, Shanghai 200444, China.

Designing low-cost electrocatalysts combining the features of outstanding catalytic activity, excellent electrical conductivity, and high chemical stability remains a critical challenge for the large-scale fabrication of dye-sensitized solar cells (DSSCs). Here we report the controlled synthesis of CoS2-CoSe2 heterostructured nanocrystals encapsulated in N-doped carbon hollow nanocubes ([email protected]) through simultaneous sulfurization and selenization of polydopamine coated Prussian blue analogs. Benefiting from both structural and compositional characteristics, namely, the synergistic effect of CoS2-CoSe2 heterojunctions, the conductive N-doped carbon coating and the porous structure of the nanocubes, the resultant [email protected] nanocubes exhibit excellent electrocatalytic activity and cycling stability toward the generation of I3- ions in DSSCs. A typical device achieves a high power conversion efficiency (PCE) of 8.45% under AM1.5G illumination (100 mW cm-2), superior to that of a standard Pt-based device (8.07%). These results demonstrate that the as-synthesized [email protected] nanocubes are promising alternatives to Pt in DSSCs. The work represented here not only provides a promising strategy to design efficient and robust CE catalysts, but also can be extended for synthesizing other novel metal sulfide/selenide hybrid materials for applications in the fields of energy conversion and storage.
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http://dx.doi.org/10.1039/c8dt00067kDOI Listing
April 2018

A reversible and highly selective two-photon fluorescent "on-off-on" probe for biological Cu detection.

Org Biomol Chem 2018 03;16(13):2264-2268

Department of Chemistry, Anhui Provincial Engineering Research Center for Polysaccharide Drugs, Wannan Medical college, Wuhu, 241002, P.R. China.

A two-photon active probe for physiological copper (Cu2+) detection is expected to play an important role in monitoring biological metabolism. Herein, a novel Schiff base derivative (E)-2,2'-((4-((4-(diethylamino)-2-hydroxybenzylidene)amino)phenyl)azanediyl)bis(ethan-1-ol) (L) with remarkable two-photon activity was developed and synthetically investigated. L presents high selectivity and sensitivity for Cu2+ sensing in ethanol/HEPES buffer (v/v, 1 : 1), which is accompanied by the fluorescence switching "off" and subsequently "on" with the addition of EDTA. The mechanism for the detection of Cu2+ is further analyzed using 1H NMR titration, mass spectra and theoretical calculations. Furthermore, since the probe L possesses good photophysical properties, excellent biocompatibility and low cytotoxicity, it is successfully applied to track Cu2+ in the cellular endoplasmic reticulum by two-photon fluorescence imaging, showing its potential value for practical applications in biological systems.
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http://dx.doi.org/10.1039/c8ob00257fDOI Listing
March 2018

Synergistically Enhanced Electrochemical Performance of NiS-PtX (X = Fe, Ni) Heteronanorods as Heterogeneous Catalysts in Dye-Sensitized Solar Cells.

ACS Appl Mater Interfaces 2017 Aug 11;9(33):27607-27617. Epub 2017 Aug 11.

Shanghai Electrochemical Energy Devices Research Center, School of Chemistry and Chemical Engineering and State Key Laboratory of Metal Matrix Composites, Shanghai Jiao Tong University , Shanghai 200240, China.

Platinum (Pt)-based alloys are considerably promising electrocatalysts for the reduction of I/I and Co/Co redox couples in dye-sensitized solar cells (DSSCs). However, it is still challenging to minimize the dosage of Pt to achieve comparable or even higher catalytic efficiency. Here, by taking full advantages of the Mott-Schottky (M-S) effect at the metal-semiconductor interface, we successfully strategize a low-Pt-based M-S catalyst with enhanced electrocatalytic performance and stability for the large-scale application of DSSCs. The optimized M-S electrocatalyst of NiS-PtX (X = Fe, Ni) heteronanorods is constructed by rationally controlling the ratio of Pt to transition metal in the hybrids. It was found that the electrons transferred from NiS to PtX at their interface under the Mott-Schottky effect result in the concentration of electrons onto PtX domains, which subsequently accelerates the regeneration of both I/I and Co/Co redox shuttles in DSSCs. As a result, the DSSC with NiS-PtFe manifests an impressive power conversion efficiency (PCE) of 8.79% and 5.56% for iodine and cobalt-based electrolyte under AM1.5G illumination, respectively. These PCEs are obviously superior over those with NiS-Pt, PtFe, NiS, and pristine Pt electrodes. The strategy reported here is able to be further expanded to fabricate other low-Pt-alloyed M-S catalysts for wider applications in the fields of photocatalysis, water splitting, and heterojunction solar cells.
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http://dx.doi.org/10.1021/acsami.7b05418DOI Listing
August 2017

Two-Photon Active Organotin(IV) Carboxylate Complexes for Visualization of Anticancer Action.

ACS Biomater Sci Eng 2017 May 3;3(5):836-842. Epub 2017 Apr 3.

State Key Laboratory of Coordination Chemistry, Nanjing University, Nanjing 210093, P. R. China.

It is still a challenge that organotin(IV) carboxylate complexes with high-performance two-photon activity for cancer therapy. At present work, two novel organotin carboxylate complexes and , containing coumarin moiety, were rationally designed for two-photon fluorescent imaging and anticancer purpose. The complexes possessed large two-photon action cross-sections and high quantum yields. Living cells evaluation revealed that complexes and exhibited good biocompatibility and deep-tissue penetration over femtosecond laser with wavelength of 840 nm. Furthermore, the antitumor active and as well as possible mechanism of complexes and have been investigated systematically. The results indicated that complexes and could induce apoptotic cell death through a mitochondrial dysfunction and ROS elevation pathway. The present work provides a strategy for rationally designing organotin(IV) carboxylate complexes with two-photon activity and antitumor activity.
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http://dx.doi.org/10.1021/acsbiomaterials.6b00786DOI Listing
May 2017

A TPA-caged precursor of (imino)coumarin for "turn-on" fluorogenic detection of Cu(.).

Anal Chim Acta 2016 Aug 1;933:189-95. Epub 2016 Jun 1.

Division of Molecular Surface Physics & Nanoscience, Department of Physics, Chemistry and Biology, Linköping University, Linköping 58183, Sweden.

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.
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http://dx.doi.org/10.1016/j.aca.2016.05.031DOI Listing
August 2016

A logic gate-based fluorogenic probe for Hg(2+) detection and its applications in cellular imaging.

Anal Chim Acta 2016 May 19;919:85-93. Epub 2016 Mar 19.

Division of Molecular Surface Physics & Nanoscience, Department of Physics, Chemistry and Biology, Linköping University, Linköping, 58183, Sweden.

A new colorimetric and fluorogenic probe (RN3) based on rhodamine-B has been successfully designed and synthesized. It displays a selective response to Hg(2+) in the aqueous buffer solution over the other competing metals. Upon addition of Hg(2+), 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 Hg(2+) with the association and dissociation constants of 0.22 × 10(5) M(-1) and 25.2 μM, respectively. The Job's plot experiment determines a 1:1 binding stoichiometry between RN3 and Hg(2+). The resultant "turn-on" fluorescence in buffer solution, allows the application of a method to determine Hg(2+) levels in the range of 4.0-15.0 μM, with the limit of detection (LOD) calculated at 60.7 nM (3σ/slope). In addition, the fluorescence 'turn-off' and color 'fading-out' happen to the mixture of RN3-Hg(2+) by further addition of I(-) or S(2-). The reversible switching cycles of fluorescence intensity upon alternate additions of Hg(2+) and S(2-) 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.
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http://dx.doi.org/10.1016/j.aca.2016.03.017DOI Listing
May 2016
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