Jieshan Qiu

Dalian University of Technology, Lü-ta-shih, Liaoning, China

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Publications (214)466.85 Total impact

  • [Show abstract] [Hide abstract]
    ABSTRACT: Novel 2-phenylquinoline-based cyclometalated PtII complexes are synthesized and fully characterized. 2-Phenylquinoline derivatives with a functional group at the 4-position of the phenyl ring are prepared through an efficient Pd-catalyzed ligand-free and aerobic Suzuki reaction of 2-bromoquinoline with arylboronic acids. The photophysical properties of the complexes demonstrate that the introduction of a diphenylamino group at the 4-position of the phenyl ring affects the HOMO level of the PtII complex significantly, resulting in a marked decrease in energy gap. The emission or energy gap is not influenced clearly by other substituents (methyl, cyano, fluoro, trifluoromethyl, methoxyl, carbazol-9-yl) at the 4-position of the phenyl ring. All the complexes show redshifted room-temperature phosphorescence emission (at 578–599 nm) relative to the model complex Pt(ppy)acac (at 486 nm). The oxygen sensitivity of the complexes is evaluated quantitatively in a polymer film. The films containing the PtII complexes are sensitive to O2, and the luminescence changes gradually and reversibly with O2 concentration. The PtII complex with a triphenylamino moiety exhibits the highest sensitivity (=0.020 Torr−1). The 2-phenylquinoline-based PtII complexes are potential candidates for efficient luminescent oxygen sensing. The present results provide a systematic study on the structure–property relationship between the 2-phenylquinoline-based PtII complexes and oxygen sensing.
    ChemPlusChem 07/2014;
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    ABSTRACT: The desired control of size, structure, and optical properties of fluorescent carbon dots (CDs) is critical for understanding the fluorescence mechanism and exploring their potential application. Herein, a top-down strategy to chemically tailor the inexpensive coal to fluorescent CDs by a combined method of carbonization and acidic oxidation etching is reported. The size and optical properties of the as-made CDs are tuned by controlling the structures of graphitic crystallites in the starting precursor. The coal-derived CDs exhibit two different distinctive emission modes, where the intensity of the short-wavelength emission is significantly enhanced by partial reduction treatment. The evolution of the electronic structure and the surface states analysis show that two different types of fluorescence centers, nano-sized sp2 carbon domains and surface defects, are responsible for the observed emission characteristics. The reduced CDs are demonstrated as an effective fluorescent sensing material for label-free and selective detection of Cu(II) ions with a detection limit as low as 2.0 nm, showing a great promise for real-world sensor applications.
    Small 07/2014; · 7.82 Impact Factor
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    ABSTRACT: Here we report the synthesis of ZnO@C coaxial gemel hexagonal microrods with a thin hydrothermal carbon (HTC) layer on their surface by a facile one-step hydrothermal method with furfural as the carbon precursor. The furfural has a unique dual role, which not only induces the nucleation of ZnO in the initial stage of hydrothermal process, but also forms a thin HTC layer deposited on the ZnO surface. The thickness of the surface HTC layer increases with the hydrothermal time till to 16 h under the conditions adopted in the present study. It has been found that the HTC layer has resulted in a significant improvement in the photocatalytic activities and photostabilities of the ZnO@C microrods for the UV-irradiated photodegradation of methylene blue solution. The mechanism involved in the process is proposed and discussed in terms of the photodegradation scheme and the properties of the ZnO@C microrods.
    ACS Applied Materials & Interfaces 04/2014; · 5.01 Impact Factor
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    ABSTRACT: Stable graphene oxide monoliths (GOMs) have been fabricated by exploiting epoxy groups on the surface of graphene oxide (GO) in a ring opening reaction with amine groups of poly(oxypropylene) diamines (D400). This method can rapidly form covalently bonded GOM with D400 within 60 s. FTIR and XPS analyses confirm the formation of covalent C-N bonds. Investigation of the GOM formation mechanism reveals that the interaction of GO with a diamine cross-linker can result in 3 different GO assemblies depending on the ratio of D400 to GO, which have been proven both by experiment and molecular dynamics calculations. Moreover, XRD results indicate that the interspacial distance between GO sheets can be tuned by varying the diamine chain length and concentration. We demonstrate that the resulting GOM can be moulded into various shapes and behaves like an elastic hydrogel. The fabricated GOM is non-cyctotoxic to L929 cell lines indicating a potential for biomedical applications. It could also be readily converted to graphene monolith upon thermal treatment. This new rapid and facile method to prepare covalently cross-linked GOM may open the door to the synthesis and application of next generation multifunctional 3D graphene structures.
    Advanced Functional Materials 04/2014; · 9.77 Impact Factor
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    ABSTRACT: Spilled oil represents a menace to the aquatic ecosystem and the whole environment in general and requires timely cleanup. Among all the avaliable technologies, oil sorption has attracted the most attention because of its simplicity and high level of effectiveness. The key for the development of this technology is convenient fabrication of high-performance oil sorbents that can be used repeatedly. In this work, a fast microwave irradiation-mediated approach has been proposed for manufacturing multiwall carbon nanotube (MWCNT)–graphene hybrid aerogels, in which MWCNTs are vertically anchored on the surface of cell walls of graphene aerogels. The hybrid monoliths show superhydrophobicity and superoleophilicity, a large pore volume, a large pore size, and excellent compressibility, demonstrating outstanding performance for recyclable oil sorption.
    Environmental Science & Technology Letters. 03/2014; 1(3):214–220.
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    ABSTRACT: A new ZIF-8 membrane architecture with high performance supported on vertically aligned ZnO nanorods was successfully prepared. The vertically aligned, single crystal ZnO nanorods were grown seamlessly from porous ceramic support to form an intermediate support layer for the ZIF-8 membrane. They provide multiple anchorages for the ZIF-8 membrane that are both strong and flexible. The nanorods were activated to induce a uniform nucleation of ZIF nuclei on their surface to initiate and guide the growth of a defect-free ZIF-8 membrane. Single gas permeations and binary separations carried out to investigate the transport properties of these new membrane architectures confirmed that the ZIF-8 membranes were free of defects and stable at a higher temperature (473 K).
    Chemistry of Materials. 02/2014; 26(5):1975–1981.
  • Haiqiu Fang, Chang Yu, Tingli Ma, Jieshan Qiu
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    ABSTRACT: Boron-doped graphene, synthesized by annealing a mixture of graphite oxide and B2O3, has shown a high conversion efficiency of 6.73% as a counter electrode (CE) for dye-sensitized solar cells, which is better than the Pt CE.
    Chemical Communications 02/2014; · 6.38 Impact Factor
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    ABSTRACT: The idea of extending functions of graphene aerogels and achieving specific applications has aroused wide attentions recently. A solution to this challenge is the formation of hybrid structure where the graphene aerogels are decorated with other functional nanostrucutres. An infiltration-evaporation-curing strategy has been proposed by formation of hybrid structure containing polydimethylsiloxane (PDMS) and compressible graphene aerogel (CGA) where the cellular walls of the CGA is coated uniformly with integrated polymer layer. The resulting composite shows enhanced compressive strength and a stable Young's modulus that is superior to those of pure CGAs. This unique structure combines the advantages of both components, giving rise to excellent electromechanical performance, where the bulk resistance repeatedly shows a synchronous and linear response to the variation of volume during compression at a wide range of compressed rates. Furthermore, the foam-like structure delivers a water droplet with "sticky" superhydrophobicity and a size as large as 32 μL, which remains tightly pinned to the composite, even when turning it upside-down. This is the first demonstration of the superhydrophobicity with strong adhesion on a foam-like structure. These outstanding properties qualify the PDMS/CGA composites developed here as promising candidates for a wide range of applications such as in sensors, actuators, and materials used for biochemical separation and tissue engineering.
    ACS Applied Materials & Interfaces 02/2014; · 5.01 Impact Factor
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    ABSTRACT: Transition metal oxide coupling with carbon is an effective method for improving electrical conductivity of battery electrodes and avoiding the degradation of their lithium storage capability due to large volume expansion/contraction and severe particle aggregation during the lithium insertion and desertion process. In our present work, we develop an effective approach to fabricate the nanocomposites of porous rod-shaped Fe3O4 anchored on reduced graphene oxide (Fe3O4/rGO) by controlling the in situ nucleation and growth of β-FeOOH onto the graphene oxide (β-FeOOH/GO) and followed by dielectric barrier discharge (DBD) hydrogen plasma treatment. Such well-designed hierarchical nanostructures are beneficial for maximum utilization of electrochemically active matter in lithium ion batteries and display superior Li uptake with high reversible capacity, good rate capability, and excellent stability, maintaining 890 mA h g(-1) capacity over 100 cycles at a current density of 500 mA g(-1).
    Nanoscale 01/2014; · 6.23 Impact Factor
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    ABSTRACT: Novel triphenylamine-based cyclometalated Pt(II) complexes containing a pyridyl moiety have been synthesized and fully characterized. The cyclometalating ligands were prepared via an efficient palladium-catalyzed ligand-free Suzuki reaction of 4-(diphenylamino)phenylboronic acid with 2-pyridyl bromides under aerobic and aqueous conditions. The photophysical properties of the complexes exhibited that introducing an electron-withdrawing group like trifluoromethyl or cyano group on the 5-position of the pyridine ring affected the LUMO level of the Pt(II) complex significantly, resulting in a marked decrease in energy gap. Moreover, the complex with a cyano group at the 5-position imparts a substantial red-shift up to 56 nm. The O2 sensitivity of the complexes was quantitatively evaluated in a polymer film. The results of the O2-sensing sensitivity of the Pt(II) complexes demonstrated that the complex with a nitrile ligand exhibited the highest sensitivity (KSVapp = 0.102 Torr−1). The triphenylamine-based cyclometalated Pt(II) complexes are potential candidates for efficient luminescent oxygen sensing.
    Dyes and Pigments 01/2014; 101:85–92. · 3.53 Impact Factor
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    ABSTRACT: Carbon nanotube supported ruthenium catalysts, assembled at the water/oil interfaces, show excellent activity and selectivity for the hydrodeoxygenation of the bio-oil model compound of vanillin under mild conditions (1 MPa, 150 °C). Based on a direct fluorescence image, the Ru/CNT catalysts are mainly distributed on the surface of the emulsion droplets, forming a Pickering emulsion. Simultaneous reaction and separation of the products are achieved in the constructed emulsions, which have great potential in the simplifications of the isolation and purification stages for bio-oil refining.
    Catalysis Communications 01/2014; 47:28–31. · 2.92 Impact Factor
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    ABSTRACT: Carbon/carbon composite membranes (CCMs) were made using the blend of polyimide with ordered mesoporous carbon (OMC) as precursor at a pyrolysis temperature of 650°C. The thermal stability of precursors, the structure evolution, and the morphology and gas separation performance of CCMs were investigated. The results have shown that the CCMs are one of the most attractive membrane materials for gas separation. The thermal stability of the precursor is improved by the addition of OMC. OMC can tightly embed in the membrane matrix due to the carbonaceous homology of matrix. As a result of the addition of OMC into carbon membranes, the gas permeability of O2 increases ten times, together with the O2/N2 selectivity significantly boosting from 10.3 to 12.9.
    Separation Science and Technology 01/2014; 49(2). · 1.16 Impact Factor
  • Min Ji, Suzhen Ren, Ce Hao, Huili Jin, Jieshan Qiu
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    ABSTRACT: This study investigates the interaction between X (X = H and F) and graphene C54H18 (D 6 h), and the potential energy surface of the graphene radical. The calculations on the structures and energies are further discussed thermodynamically and kinetically using the density function theory method at the B3LYP/6-31G (d) level. Our findings show that there are four distinct isomers of C54H18–X. C54H18–H2 and C54H18–F4 are the most stable isomers in their own systems. In addition, the transition states, as well as reaction pathways of H transferring between different key points on representative patch, are given to explore the possible reaction mechanism. Finally, the stability of C54H18–X2 is discussed through the density functional theory.
    Molecular Simulation 01/2014; 40(4). · 1.06 Impact Factor
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    ABSTRACT: Nanostructured activated carbons for electrochemical double-layer capacitors were synthesized from depleted fullerene soot (DFS) via KOH activation. The structural and textural properties of the activated DFS were studied using transmission electron microscopy, X-ray diffraction, and nitrogen sorption. Activated DFS with high specific surface areas (SSAs) of up to 2,153 m2 g−1 and narrow pore size distributions (PSDs) was obtained by controlling the KOH/DFS ratio. The activated DFS exhibited excellent capacitive behavior, with a high specific capacitance of 250 F g−1 at a current density of 50 mA g−1 in a 6 M KOH electrolyte, and a high rate performance, with a capacitance retention of up to 80 % at a high scan rate of 200 mV s−1. Moreover, the activated DFS samples exhibited good electrochemical stability; high capacitance retention ratios of >90 % were obtained at a current density of 2,000 mA g−1 for 5,000 cycles with cell voltages of 0.9 and 1.0 V in a two-electrode system. The high electrochemical performance can be attributed to high SSAs, narrow PSDs, and nanoscale particle sizes, which facilitate the formation of electrochemical double layers and rapid ion diffusion.
    Journal of Applied Electrochemistry 01/2014; · 1.84 Impact Factor
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    ABSTRACT: This work presents a facile and rapid approach for the preparation of graphene sheet (GS) decorated by nanometer scaled molybdenum disulfide (MoS2) with effective hydrodesulfurization activity for carbonyl sulfide conversion at low temperature (<300 °C). Using functionalized GS as microwave susceptor and ammonium tetrathiomolybdate as the precursor of MoS2, nanocomposites consisting of MoS2 nanoparticles and GS was prepared through a solvent-free microwave-assisted route. The synthesized MoS2 and GS hybrid (M-MoS2/GS) was characterized by X-ray diffraction, Fourier transform infrared spectrometry, Raman spectrometry, scanning and transmission electron microscopies as well as low temperature nitrogen adsorption. Compared to MoS2/GS and MoS2/activated carbon catalysts made by conventional thermal decomposition, the M-MoS2/GS composite shows excellent performance for the hydrodesulfurization of carbonyl sulfide. The high catalytic efficiency over M-MoS2/GS composite demonstrates that microwave irradiation is helpful for the preparation of graphene-based catalysts with enhanced catalytic activity. The low-cost synthesis procedure paves the way for the exploitation of the presented hybrid materials as catalysts for the hydrodesulfurization of coal-based gas.
    Fuel. 01/2014; 119:163–169.
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    ABSTRACT: Graphene-incorporated nitrogen-rich carbon composite with nitrogen content of ca. 10 wt.% has been synthesized by an effective yet simple hydrothermal reaction of glucosamine in the presence of graphene oxide (GO). The nitrogen content of carbon composite is nearly twice as high as that of hydrothermal carbon without graphene. GO is favorable for the high nitrogen doping in the carbon composite by the reaction between the glucosamine-released ammonia and GO. The hydrothermal carbon composite is further activated by KOH, and graphene in the activated carbon composite demonstrates a positive effect of increasing specific surface area, pore volume and electrical conductivity, resulting in superior electrochemical performance. The activated carbon composite with higher specific surface area and micropore volume possesses higher specific capacitance with a value of 300 F g−1 at 0.1 A g−1 in 6 M KOH aqueous solution in the two electrode cell. Larger mesopore volume and higher conductivity of the activated carbon composite will provide fast ion and electron transfer, thus leading to higher rate capacity with a capacitance retention of 76% at 8 A g−1 in comparison to the activated hydrothermal carbon without graphene.
    Carbon. 01/2014; 70:130–141.
  • Computational and Theoretical Chemistry. 01/2014;
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    ABSTRACT: Polychlorinated diphenyl ethers (PCDEs) are a focus of current environmental concern as a group of ubiquitous potential persistent organic pollutants. There are still significant gaps in our knowledge concerning the photolysis mechanisms of PCDEs. In this study, the direct photolysis mechanisms of PCDEs were investigated by density functional theory. The direct photolysis of PCDEs has three potential reaction pathways including photodechlorination, C−O bond photodissociation, and PCDFs formation. Taking a representative PCDE (i.e., CDE8) for example, we found that C−Cl bond dissociation is the rate-determining step for the photodechlorination. Chlorobenzene is predicted to be photoproduct of CDE8 through the photodissociation of the C−O bond. Furthermore, the calculated mean bond dissociation energies of both C−Cl and C−O bonds of 20 PCDEs decrease with the increased degree of chlorination. It is also found that the photoactivity of PCDEs increases with an increase of chlorination degree by evaluating the average charge of Cl atoms and mean bond dissociation energies of C−Cl and C−O bonds from reaction thermodynamics. Our findings provided a new insight into the mechanisms of direct photolysis of PCDEs, which may be useful in the future in utilizing quantum chemistry calculation in investigating the behavior and fate of organic pollutants in the environment.
    Chemosphere 01/2014; 111:7–12. · 3.14 Impact Factor
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    ABSTRACT: Here we report the finding of a new crumpled graphene structure – folded graphene belts (FGBs) – generated by means of shock cooling of an aqueous chemically converted graphene (CCG) dispersion. Unlike the traditional tubular hollow structures such as CNTs or CNSs, the as-made FGBs feature an accordion-like geometry in which the 2D graphene sheets were folded along multiple parallel axes. In situ scanning electron microscope (SEM) measurements revealed that the prepared FGBs were highly elastic and can keep their shape under repeated large strains. The formation and growth of ice crystals during the shock cooling step in liquid nitrogen are believed to be the driving force for the formation of such unique folded graphene structures.
    Carbon. 01/2014; 76:46–53.
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    ABSTRACT: Activated nitrogen-doped carbons (ANCs) were prepared by carbonization/activation approach using aminated polyvinyl chloride (PVC) as precursor. ANCs exhibit larger porosities and higher specific surface areas than those of their nitrogen-free counterparts for the same KOH/carbon ratio. The specific surface area of ANC-1 is up to 1,398 m2 g−1 even at a low KOH/carbon ratio of 1:1. Fourier transform infrared spectroscopy investigation of the nitrogen-enriched resin precursor indicates the efficient dehydrochlorination of PVC by ethylenediamine at a low temperature. The nitrogen content and the population of nitrogen functionalities strongly depend on the KOH/carbon ratios and decrease drastically after KOH activation as seen from the elemental and X-ray photoelectron spectroscopy analysis. The surface concentration of N-6 and N-Q almost disappears and the dominant nitrogen groups become N-5 after KOH activation. The highest specific capacitance of ANCs is up to 345 F g−1 at a current density of 50 mA g−1 in 6 M KOH electrolyte. ANCs also exhibit a good capacitive behavior at a high scan rate of 200 mV s−1 and an excellent cyclability with a capacitance retention ratio as high as ∼93 % at a current density of 2,000 mA g−1 for 5,000 cycles.
    Journal of Solid State Electrochemistry 01/2014; 18(1). · 2.28 Impact Factor

Publication Stats

1k Citations
466.85 Total Impact Points

Institutions

  • 1998–2014
    • Dalian University of Technology
      • • State Key Laboratory of Fine Chemicals
      • • Department of Environmental Science and Technology
      • • School of Environmental and Biological Science and Technology
      • • School of Chemical Engineering
      • • Department of Materials Science and Chemical Engineering
      Lü-ta-shih, Liaoning, China