Qiang Xu

National Institute of Advanced Industrial Science and Technology, Tsukuba, Ibaraki, Japan

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Publications (299)1081.63 Total impact

  • Qi‐Long Zhu, Qiang Xu
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    ABSTRACT: Review: recent progress in designing and fabricating metal—organic framework composites for diverse functional applications; 419 refs.
    ChemInform 10/2014; 45(43).
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    ABSTRACT: a b s t r a c t In this paper, we report fabrication of hollow silica–zirconia composite spheres by polystyrene (PS) tem-plate method and control of wall thickness of the hollow spheres in nanoscale. Both the hollow spheres before and after calcination were characterized by scanning electron microscopy (SEM), transmission electron microscopy (TEM), Fourier transform infrared spectroscopy (FTIR), elemental analysis, and pow-der X-ray diffraction analysis (XRD). Morphology of the hollow spheres does not significantly change after calcination from the results of SEM and TEM images, while the amount of residual PS templates drastically decreases via the calcination procedure from the results of FTIR and elemental analysis. The sample after calcination mainly includes amorphous silica from the results of XRD, indicating that the hollow silica–zirconia composite spheres consist of amorphous phases and/or fine particles. Wall thick-nesses of the samples after calcination are controlled by adjusting the amount of PS template suspension, and hollow silica–zirconia composite spheres with the wall thicknesses of 17.5, 15.0, 10.0, and 2.0 nm are obtained using the PS template suspension of 25.0, 33.5, 100.0, and 400.0 g, respectively. The activities of the hollow spheres for hydrolytic dehydrogenation of ammonia borane (NH 3 BH 3) were compared. The evolutions of 2.0, 3.1, 5.0, and 8.0 mL hydrogen from aqueous NH 3 BH 3 solution were finished in about 4, 5, 3, and 7 min in the presence of the hollow spheres with wall thicknesses of 17.5, 15.0, 10.0, and 2.0 nm, respectively. The molar ratios of the hydrolytically generated hydrogen to the initial NH 3 BH 3 in the presence of the hollow spheres with wall thicknesses of 17.5, 15.0, 10.0, and 2.0 nm are 0.5, 0.8, 1.4, and 2.0, respectively. The results indicate that the activity of hollow silica–zirconia composite spheres for hydrolytic dehydrogenation of NH 3 BH 3 improves with decrease of wall thickness of the hol-low spheres. From the results of BET adsorption measurements, specific surface area of the hollow spheres increases with decrease of wall thickness of the hollow spheres. The results of activity, specific surface area, and XRD profiles suggest that the primary particles form layer-like structure in the wall of hollow silica–zirconia composite spheres and the number of the layers depends on the wall thickness. Ó 2014 Elsevier B.V. All rights reserved.
    Journal of Alloys and Compounds; 09/2014
  • Jun Li, Qi-Long Zhu, Qiang Xu
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    ABSTRACT: Non-noble bimetallic CuCo alloy nanoparticles (NPs) were successfully encapsulated in the pores of MIL-101 by using the double solvents method combined with the overwhelming reduction approach. Compared with their monometallic counterparts, the bimetallic CuCo alloy NPs present much higher catalytic activity for hydrolytic dehydrogenation of ammonia borane (AB) to generate a stoichiometric amount of hydrogen at room temperature for chemical hydrogen storage. The synergistic effect between copper and cobalt species plays an important role for the improved performance in the catalytic hydrolysis of AB.
    Catal. Sci. Technol. 09/2014;
  • Jian-Ke Sun, Qiang Xu
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    ABSTRACT: For the first time, MOF-derived hierarchically porous carbons with controlled pore structures for on-demand applications have been achieved by a double-templates approach.
    Chemical Communications 09/2014; · 6.38 Impact Factor
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    ABSTRACT: We study the effect of solvents on morphological and/or structural properties and catalytic activity of hollow nickel-silica composite spheres for hydrolytic dehydrogenation of ammonia borane. Nickel-silica composite shells were coated on polystyrene (PS) templates via sol-gel reaction with L(+)-arginine as the promoter of the sol-gel reaction followed or in parallel with the dissolution of the PS templates in the same medium to form hollow spheres. From the transmission electron microscopy (TEM) images, nickel-silica composite shells were formed for 1.5 h, and the surface roughness of the shells increases with the increase of aging time in methyl alcohol, while the shells were formed via the formation of aggregates of irregular shape in ethyl alcohol and 2-propyl alcohol. From the angle attenuated total reflectance infrared (ATR-IR) spectra, the order of dissolution rate of PS templates is 2-propyl alcohol > ethyl alcohol > methyl alcohol. These results indicate that the shells are formed before the dissolution of PS templates in methyl alcohol, while in ethyl alcohol and 2-propyl alcohol, nickel-silica composite shells was formed in parallel with dissolution of PS templates via the formation of aggregates of irregular shape. From the results of N 2 adsorption/desorption isotherm analysis, the order of BET surface area is samples prepared in ethyl alcohol > methyl alcohol ≈ 2-propyl alcohol. The catalytic activity for hydrolytic dehydrogenation from aqueous NaBH 4/ NH 3BH3 solution in the presence of the hollow spheres prepared in ethyl alcohol was much higher than those in the presence of the hollow spheres prepared in methyl alcohol and 2-propyl alcohol. Consequently, the solvents were mainly influenced in morphological homogeneity and BET surface area of hollow nickel-silica composite spheres, and these structural properties affected the catalytic activity.
    Journal of the Japan Institute of Energy 08/2014; 93(8):703-709.
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    ABSTRACT: The rigid and angular tetracarboxylic acid, 1,3-bis-(3,5-dicarboxyphenyl)imidazolium (H4L+), incorporating imidazolium group, has been used with different pyridine based linkers to construct a series of non-interpenetrated cationic frameworks, {[Zn2(L)(bpy)2]•(NO3)•(DMF)6•(H2O)9}n (1), {[Zn2(L)(dpe)2]•(NO3)•(DMF)3•(H2O)2}n (2) & {[Zn2(L)(bpb)2]•(NO3)•(DMF)3•(H2O)4}n (3) (L = L-3, DMF = N,N′-dimethylformamide, bpy = 4,4′-bipyridine, dpe = 1,2-di(4-pyridyl) ethylene, bpb = 1,4-bis(4-pyridyl)benzene). The frameworks consist of {[Zn2(L)]+}n 2D layers that are further pillared by the linker ligands to form 3D bipillared-layer porous structures. While the choice of the bent carboxylic acid ligand and formation of double-pillars are major factors in achieving charged non-interpenetrated frameworks, lengths of the pillar linkers direct the pore modulation. Accordingly, N2 gas adsorption capacity of the activated frameworks (1a, 2a, 3a) increases with increasing pillar length. Moreover, variation in the electronic environment and marked difference in frameworks’ pore sizes permit selective CO2 adsorption over N2, where 3a divulges highest selectivity. In contrast, the selectivity of CO2 over CH4 is reversed and follow the order 1a>2a>3a. These results demonstrate that even though the pore sizes of the frameworks are large enough compared to the kinetic diameters of the excluded gas molecules, electronic environment is crucial for the selective sorption of CO2.
    Inorganic Chemistry 06/2014; · 4.59 Impact Factor
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    ABSTRACT: Highly photoluminescent carbon nanodots (CNDs) were synthesized for the first time from metal–organic framework (MOF, ZIF-8) nanoparticles. Coupled with fluorescence and non-toxic characteristics, these carbon nanodots could potentially be used in biosafe color patterning.
    Chemistry 05/2014; · 5.93 Impact Factor
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    ABSTRACT: For the first time, high surface area uniformly nitrogen (N)- and boron-nitrogen (BN)-decorated nanoporous carbons have been successfully fabricated by impregnation of ionic liquids (ILs) within a metal-organic framework (MOF), MIL-100(Al), followed by carbonization, which exhibit remarkable CO2 and H2 adsorption capacities.
    Chemical Communications 05/2014; · 6.38 Impact Factor
  • Ashish Kumar Singh, Qiang Xu
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    ABSTRACT: a b s t r a c t Highly-dispersed surfactant-free bimetallic NiePt nanoparticles (NPs) with a particle size as small as 2.4 nm were successfully synthesized using NaBH 4 as reducing agent in the presence of NaOH, which exhibit excellent catalytic performance with very fast kinetics for selective decomposition of hydrous hydrazine to hydrogen at room temperature. NaOH plays an important role in the formation of highly-dispersed NiePt nanoparticles. The present results bring light to new opportunities in the development of high-performance metal nanoparticle catalysts and encourage the effective application of hydrous hydra-zine as a promising hydrogen storage material.
    International Journal of Hydrogen Energy 05/2014; · 3.55 Impact Factor
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    ABSTRACT: The influence of particle size of hollow silica-alumina composite spheres on their activity for hydrolytic dehydrogenation of ammonia borane (NH3BH3) was investigated. A silica-alumina composite shell was coated onto polystyrene (PS) template particles, before the removal of PS template particle by calcination. The diameter of the PS template particles decreased with an increase in the amount of poly (vinyl pyrrolidone) and the centrifugation speed, and the diameter of the obtained PS template particles was controlled between 150 and 400 nm. Hollow silica-alumina composite spheres with diameters of 180, 230, and 430 nm were prepared using these PS template particles; the shell thickness was controlled 15 nm by adjusting the amount of PS suspension and coating time. The hydrolytic dehydrogenation of NH3BH3 evolved 9.5, 9.0, and 7.0 mL hydrogen in the presence of hollow spheres with diameters of 180, 230, and 430 nm, respectively; the molar ratios of the generated hydrogen to the initial NH3BH3 in the presence of the hollow spheres were 2.5, 2.3, and 1.8, respectively. The results indicate that the activity increases with a decrease in the diameter of hollow spheres
    Journal of the Japan Institute of Energy 05/2014; 93(5):511-516.
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    ABSTRACT: High surface area nitrogen-decorated (N-decorated) nanoporous carbons have been successfully synthesized using nitrogen-rich metal-organic framework ZIF-8 as a template and precursor along with furfuryl alcohol and NH4OH as the secondary carbon and nitrogen sources, respectively. These carbons exhibited remarkable CO2 adsorption capacities, and CO2/N2 and CO2/CH4 selectivities. N-decorating in these carbons resulted in excellent activity for oxygen reduction reaction (ORR). Samples NC900 and NC1000, having moderate N contents, large surface areas and large amounts of mesopores, favored the four electron reduction pathway, while sample NC800, having a high N content, a moderate surface area and a large amount of micropores, favored the two electron reduction process.
    Journal of the American Chemical Society 04/2014; · 10.68 Impact Factor
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    ABSTRACT: Hollow nickel-silica spheres were synthesized by sol-gel method followed by in-situ activation in aqueous sodium borohydride (NaBH4) /ammonia borane (NH3BH3) solutions. The evolution of 38, 58, and 41 mL hydrogen was finished in about 125, 90, and 30 min from aqueous NaBH4/NH3BH3 solution in the presence of nickel-silica spheres precursor activated with the amount of NaBH4 = 5, 10, and 20 mg, respectively. Morphology of in-situ synthesized samples depends on the amount of NaBH4, and the hollow spheres were obtained with the medium amount of NaBH4. Particle size and wall thickness of the hollow spheres were controlled by adjusting ratio of ethyl alcohol to water, and the particle size and wall thickness decrease with increase of the ratio. The evolution of 44, 49, and 58 mL hydrogen from aqueous NaBH4/NH3BH3 solution was finished in about 45, 35, and 90 min in the presence of the in-situ synthesized hollow spheres obtained from the precursors prepared with ratio of ethyl alcohol to water = 3.3, 10, and 20, respectively. The results indicate that the amount of hydrogen evolution increases with increase of ratio of ethyl alcohol to water. Otherwise, the amount of hydrogen evolution was related with reducibility of the precursors.
    Journal of the Japan Institute of Energy 04/2014; 93(4):323-327.
  • Jun Li, Qi-Long Zhu, Qiang Xu
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    ABSTRACT: Ultrafine AuCo alloy nanoparticles were successfully encapsulated in the pores of MIL-101 by using the double solvents method combined with the overwhelming reduction approach, which exert excellent catalytic activity for hydrolytic dehydrogenation of ammonia borane.
    Chemical Communications 04/2014; · 6.38 Impact Factor
  • Arshad Aijaz, Qiang Xu
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    ABSTRACT: Metal–organic frameworks (MOFs) are highly ordered crystalline porous materials prepared by the self-assembly of metal ions and organic linkers having low-density framework structures of diversified topologies with tunable pore sizes and exceptionally large surface areas. Other than outstanding gas/molecule storage properties, loading of metal nanoparticles (MNPs) into the pores of MOFs could afford heterogeneous catalysts having advantages of controlling the particle growth to a nanosize region, resulting in highly active sites and enhanced catalytic performances, and these entrapped MNPs within MOF pores could be accessed by reactants for chemical transformations. This is a rapidly developing research area, and this Perspective addresses current achievements and future challenges for diverse MOF-immobilized MNPs within their pores, focusing especially on their preparation, characterization, and application as heterogeneous catalysts.
    Journal of Physical Chemistry Letters 04/2014; 5(8):1400–1411. · 6.59 Impact Factor
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    Materials Research Bulletin 04/2014; 52:117–121. · 1.97 Impact Factor
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    Qi-Long Zhu, Qiang Xu
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    ABSTRACT: Metal-organic frameworks (MOFs), also known as porous coordination polymers (PCPs), synthesized by assembling metal ions with organic ligands have recently emerged as a new class of crystalline porous materials. The amenability to design as well as fine-tunable and uniform pore structures makes them promising materials for a variety of applications. Controllable integration of MOFs and functional materials is leading to the creation of new multifunctional composites/hybrids, which exhibit new properties that are superior to those of the individual components through the collective behavior of the functional units. This is a rapidly developing interdisciplinary research area. This review provides an overview of the significant advances in the development of diverse MOF composites reported till now with special emphases on the synergistic effects and applications of the composites. The most widely used and successful strategies for composite synthesis are also presented.
    Chemical Society Reviews 03/2014; · 24.89 Impact Factor
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    ABSTRACT: Dendrimer-encapsulated Co nanoparticles (G6-OH(Co60)) have been synthesized through the complexation of Co2+ cations to the internal tertiary amine of sixth-generation hydroxyl-terminated poly(amidoamine) dendrimers followed by reduction by both sodium borohydride and ammonia borane in aqueous solution. The highly dispersed G6-OH(Co60), in which the average diameter of Co nanoparticles is approximately 1.6±0.4 nm, have been confirmed by TEM analysis. The catalytic activity of G6-OH(Co60) for the hydrolysis of ammonia borane has been studied in aqueous solution at different reaction temperatures, demonstrating a high catalytic performance.
    ChemCatChem 03/2014; · 5.18 Impact Factor
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    ABSTRACT: Hollow silica–nickel composite spheres L(+)-arginine Hydrolytic dehydrogenation Ammonia borane a b s t r a c t In this paper, we investigated influence of preparation conditions of hollow silica–nickel composite spheres on their morphology and catalytic activity for hydrolytic dehydrogenation of ammonia borane. In the preparation method of this study, when silica–nickel composite shells were coated on polystyrene templates by the sol–gel method using L(+)-arginine as the promoter for the reaction to form silica–nickel composite shell, the polystyrene templates were dissolved subsequently, even synchronously, in the same medium to form hollow spheres. The as-prepared silica–nickel composite spheres were character-ized by transmission electron microscopy and scanning electron microscopy. The effects of Si+Ni content on the morphology were systematically evaluated. All the as-prepared hollow silica–nickel composite spheres have the similar morphology as identified by SEM and TEM measurement. Homogeneity of the hollow silica–nickel composite spheres increases with the increase in the Si+Ni content as shown by the laser diffraction particle size analysis. The catalytic activities of the hollow silica–nickel composite spheres for hydrolytic dehydrogenation of ammonia borane prepared with different Si+Ni contents were compared. The catalytic activity for the hydrogen evolution in the presence of the hollow spheres increases with the increase of Si+Ni content. The results of FTIR spectra of the hollow silica–nickel com-posite spheres indicate that a certain amount of residual PS templates exists in hollow silica–nickel com-posite spheres. The residual PS templates was able to be reduced by procedure of as-prepared samples with toluene solvent. The catalytic activity of hollow silica–nickel composite spheres increases with decrease in the amount of residual PS templates. Ó 2013 Elsevier B.V. All rights reserved.
    Journal of Alloys and Compounds 03/2014; 588:615-621. · 2.73 Impact Factor
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    ABSTRACT: In an effort towards the rational design of porous MOFs with a functionalized channel surface, 3,3',5,5'-tetracarboxydiphenylmethane () has been used in combination with two different bipyridine ligands of similar lengths as linkers, and Zn(ii) ions as nodes. Under solvothermal conditions, two Zn(ii) coordination polymers, {[Zn()()]·DMF·2H2O}n () and {[Zn2()()(DMF)2]·DMF·4H2O}n () (DMF = dimethyl formamide, = 3,6-di-pyridin-4-yl-[1,2,4,5]tetrazine, = 4,4'-bispyridylphenyl) are formed in moderate yields. The obvious kink in the central methylene spacer of induces either C2v or Cs symmetry in the ligand, allowing different architectures in the resulting frameworks. Single crystal X-ray analysis shows that compound is a one-dimensional (1D) double chain architecture with rhombus voids, linked by Zn2(CO2)4 paddle-wheel secondary building units (SBUs). The tetrazine and pyridine moieties of the co-ligand and free carboxylic acid groups are lined along the voids of the framework. Compound , on the other hand, crystallizes as an infinite two-dimensional corrugated sheet structure, where individual sheets are stacked in -ABAB- patterns along the crystallographic b-axis. Thermogravimetric analysis (TGA) and variable temperature powder X-ray diffraction (VTPXRD) studies reveal high thermal stability for but collapses soon after desolvation. The desolvated framework shows selective CO2 adsorption over N2, H2, and CH4 at 273 K, with an isosteric heat of CO2 adsorption of 21.3 kJ mol(-1), suggesting an interaction of the CO2 molecules with the channel walls.
    Dalton Transactions 02/2014; · 3.81 Impact Factor
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Publication Stats

2k Citations
1,081.63 Total Impact Points

Institutions

  • 2001–2014
    • National Institute of Advanced Industrial Science and Technology
      • Research Institute for Ubiquitous Energy Devices
      Tsukuba, Ibaraki, Japan
  • 2008–2013
    • Banaras Hindu University
      • Department of Chemistry
      Benares, Uttar Pradesh, India
    • Hokkaido University
      • Division of Chemistry
      Sapporo, Hokkaidō, Japan
  • 2011
    • Northeast Normal University
      • Department of Chemistry
      Hsin-ching, Jilin Sheng, China
  • 2000–2010
    • Nankai University
      • Department of Chemistry
      Tianjin, Tianjin Shi, China
  • 2006–2009
    • Kobe University
      Kōbe, Hyōgo, Japan
    • Tianjin Normal University
      • College of Chemistry and Life Science
      Tianjin, Tianjin Shi, China
  • 2003–2006
    • Northeast Institute of Geography and Agroecology
      • State Key Laboratory of Organometallic Chemistry
      Beijing, Beijing Shi, China
  • 2002–2006
    • Fudan University
      • Department of Chemistry
      Shanghai, Shanghai Shi, China