Xinhe Bao

Chinese Academy of Sciences, Peping, Beijing, China

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Publications (377)1334.32 Total impact

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    ABSTRACT: New Insight into Reaction Mechanisms of Ethanol Steam Reforming on Co/ZrO2 Junming Sun†,‡, Ayman M. Karim†, Donghai Mei†, Mark Engelhard†, Yong Wang†, ‡ * † Institute for Interfacial Catalysis, Pacific Northwest National Laboratory, Richland, Washington 99352, United States ‡ The Gene & Linda Voiland School of Chemical Engineering and Bioengineering, Washington State University, Pullman Washington 99164, United States Due to its low carbon footprint and renewable source, steam reforming of biomass-derived ethanol (ESR) has been extensively investigated to produce hydrogen for hydrotreating of biomass derived oxygenates or the potential fuel-cell application.1 Among the studied metals, cobalt based catalysts have been found to be promising in ESR due to its low-cost and high C-C cleavage activity.2-4 Previous work has shown that acetone act as mainly intermediate toward coking.5 In this work, a systematic investigation of ESR over Co/ZrO2 has been studied using a combination of catalytic evaluation and characterizations such as X-ray diffraction, nitrogen sorption, in situ X-ray photoelectron spectroscopy and transmission electron microscopy, as well as DFT calculations. We show that acetone is a major reaction intermediate which is steam reformed to selectively form H2 and CO2 on metallic cobalt at 450 C (Scheme 1, green highlighted path forward). In the newly discovered sequential reaction pathway, cobalt was found to play a bifunctional role in transforming ethanol to H2 and CO2 with high selectivity. For Co/ZrO2 catalysts, non-reducible cobalt (cobalt species strongly interact with ZrO2 support) passivates most of the strong acidic sites on ZrO2, suppresses the undesired dehydration of ethanol on the support, and favors the dehydrogenation and condensation/ketonization reaction pathway, resulting in acetone formation. Metallic cobalt (reducible cobalt) on carbon filament formed during the ESR was found to be mainly responsible for the subsequent acetone steam reforming reactions.6 The current study not only provides a fundamental new insight into the reaction mechanism of ESR on Co/ZrO2, but also sheds a light on how to design high selective and durable cobalt catalysts for steam reforming of bio-mass derived small oxygenates (e.g., ethanol, acetone and acetic acid). Scheme 1 Proposed main reaction pathway for ethanol steam reforming on Co/ZrO2 catalysts Key words: Ethanol steam reforming, Acetone steam reforming, Cobalt, Hydrogen production, Reaction mechanism, Nanoparticles References (1) Cortright, R. D.; Davda, R. R.; Dumesic, J. A. Nature 2002, 418, 964. (2) Song, H.; Ozkan, U. S. Journal of Catalysis 2009, 261, 66. (3) Lebarbier, V. M.; Karim, A. M.; Engelhard, M. H.; Wu, Y.; Xu, B. Q.; Petersen, E. J.; Datye, A. K.; Wang, Y. ChemSusChem 2011, 4, 1679. (4) Karim, A. M.; Su, Y.; Sun, J. M.; Yang, C.; Strohm, J. J.; King, D. L.; Wang, Y. Applied Catalysis B-Environmental 2010, 96, 441. (5) Mattos, L. V.; Jacobs, G.; Davis, B. H.; Noronha, F. B. Chem. Rev. 2012, 112, 4094. (6) Sun, J.; Mei, D.; Karim, A. M.; Datye, A. K.; Wang, Y. ChemCatChem 2013, 10.1002/cctc.201300041.
    Applied Catalysis B Environmental 01/2015; 162:141–148. · 5.83 Impact Factor
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    ABSTRACT: An increasing number of experimental studies have demonstrated that metal or metal oxide nanoparticles confined inside carbon nanotubes (CNTs) exhibit different catalytic activities with respect to the same metals deposited on the CNT exterior walls, with some reactions enhanced, whereas others hindered. In this article, we describe a concept of confinement energy, which enables prediction of the electronic effects on confined catalysis in different reactions. Combining density functional theory calculations and experiments by taking typical transition metals such as Fe, FeCo, RhMn, and Ru as models, we observed stronger strains and deformations within the CNT channels due to different electronic structures and spatial confinement. This leads to downshifted d-band states and consequently the adsorption of molecules such as CO, N2, and O2 is weakened. Thus, the confined space of CNTs provides essentially a unique microenvironment, which shifts the volcano curve of the catalytic activities towards the metals with higher binding energies. The extent of the shift depends on the specific metals and the CNT diameters. This concept generalizes the diverse effects observed in experiments for different reactions and it is anticipated to be applicable to an even broader range of reactions other than redox of metal species, CO hydrogenation, ammonia synthesis and decomposition discussed here.
    Journal of the American Chemical Society 12/2014; · 10.68 Impact Factor
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    ABSTRACT: Graphitic overlayers on metals have commonly been considered as inhibitors for surface reactions due to their chemical inertness and physical blockage of surface active sites. In this work, however, we find that surface reactions, for instance, CO adsorption/desorption and CO oxidation, can take place on Pt(111) surface covered by monolayer graphene sheets. Surface science measurements combined with density functional calculations show that the graphene overlayer weakens the strong interaction between CO and Pt and, consequently, facilitates the CO oxidation with lower apparent activation energy. These results suggest that interfaces between graphitic overlayers and metal surfaces act as 2D confined nanoreactors, in which catalytic reactions are promoted. The finding contrasts with the conventional knowledge that graphitic carbon poisons a catalyst surface but opens up an avenue to enhance catalytic performance through coating of metal catalysts with controlled graphitic covers.
    Proceedings of the National Academy of Sciences of the United States of America. 12/2014; 111(48):17023-8.
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    ABSTRACT: Controllable synthesis of large domain, high-quality monolayer MoS2 is the basic premise both for exploring some fundamental physical issues, and for engineering its applications in nanoelectronics, optoelectronics, etc. Herein, by introducing H2 as carrier gas, the successful synthesis of large domain monolayer MoS2 triangular flakes on Au foils, with the edge length approaching to 80 mm is reported. The growth process is proposed to be mediated by two competitive effects with H2 acting as both a reduction promoter for efficient sulfurization of MoO3 and an etching reagent of resulting MoS2 flakes. By using low-energy electron microscopy/diffraction, the crystal orientations and domain boundaries of MoS2 flakes directly on Au foils for the first time are further identified. These on-site and transfer-free characterizations should shed light on the initial growth and the aggregation of MoS2 on arbitrary substrates, further guiding the growth toward large domain flakes or monolayer films.
    Advanced Functional Materials 12/2014; · 10.44 Impact Factor
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    ABSTRACT: N-doped graphene used as an efficient electron donor of iron catalyst for CO hydrogenation can achieve a high selectivity of around 50% for light olefins, significantly superior to the selectivity of iron catalyst on conventional carbon materials, e.g. carbon black with a selectivity of around 30% at the same reaction conditions.
    Chemical Communications 10/2014; · 6.38 Impact Factor
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    ABSTRACT: Ring current is a fundamental concept to understand the nuclear magnetic resonance (NMR) properties and aromaticity for conjugated systems, such as carbon nanotubes (CNTs). Employing the recently developed gauge including projector augmented wave (GIPAW), we studied the ring currents of CNTs systematically and visualized their distribution. The ring current patterns are determined by the semiconducting or metallic properties of CNTs. The discrepancy is mainly caused by the axial component of external magnetic fields, whereas the radial component induced ring currents are almost independent on the electronic structures of CNTs, where the intensities of ring currents are linearly related to the diameters of CNTs. Although the ring currents induced by the radial component are more intense than the ones by the axial component, only the later determines the overall NMR responses and aromaticity of CNTs as well. Furthermore, the semiconducting CNTs are more aromatic than the metallic counterparts due to the existence of delocalized ring currents on the semiconducting CNTs. These fundamental features are of vital importance for development of CNT-based nanoelectronics and applications in magnetic fields.
    Chemical Science 08/2014; · 8.31 Impact Factor
  • Chinese Journal of Catalysis 08/2014; 32(8):1418-1423. · 1.30 Impact Factor
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    ABSTRACT: Silica supported Pt–Co and Au–Co nanoparticles (NPs) were subjected to various redox processes and characterized by X-ray diffraction, X-ray absorption near edge structure, and X-ray photoelectron spectroscopy. We found that most of the Co oxide (CoOx) species on Pt NPs can be reduced at 100 °C forming an alloy structure with Pt at elevated temperatures. Oxidation of Co in the reduced sample takes place gradually with increasing temperatures. In contrast, temperatures higher than 400 °C are needed to reduce CoOx on Au NPs and Co atoms hardly form an alloy with Au even at 600 °C. The Co species in the reduced Au–Co/SiO2 sample were quickly oxidized in an O2 atmosphere at room temperature. High CO oxidation activity was observed in the Pt–Co/SiO2 catalyst reduced below 300 °C; however this necessitated reduction at 600 °C of the Au–Co/SiO2 catalyst. The results illustrate a stronger interaction of Co (CoOx) with Pt than with Au. In both systems, the optimum treatment conditions are to produce a similar CoO-on-noble metal (NM) active structure and maximize the density of interface sites between the surface CoO structure and the NM support.
    Catal. Sci. Technol. 08/2014; 4(9).
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    ABSTRACT: Ammonium ferric citrate (AFC) was used as a single-source molecular precursor to prepare Fe/Fe3C nanoparticles encapsulated in nitrogen-doped carbon by pyrolysis in Ar atmosphere followed by acid-leaching. Comparative studies, using citric acid and ferric citrate as the precursors, indicated that the ammonia and ferric ion in AFC and the pyrolysis temperature affected the composition of iron species and the properties of carbon in AFC-derived materials. Above the pyrolysis temperature of 600 °C, the iron species were Fe/Fe3C, and the carbon had a hollow graphitic nanoshell structure in AFC-derived materials. The specific surface area and content of nitrogen element decreased with increasing pyrolysis temperature. The AFC-derived material pyrolyzed at 600 °C had the optimal graphitization degree, specific surface area (489 m2 g−1) and content of nitrogen (1.8 wt.%), thus resulted in the greatest activity for oxygen reduction reaction among the AFC-derived materials pyrolyzed at different temperatures. The AFC-derived material pyrolyzed at 600 °C exhibited improved methanol-resistance ability compared with Pt/C catalyst.
    Carbon 08/2014; 75:381–389. · 6.16 Impact Factor
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    ABSTRACT: Hydrogen is considered as an important clean energy carrier for the energy future and electrocatalytic splitting of water is one of the most efficient technologies for hydrogen production. As one potential alternative to Pt-based catalysts in hydrogen evolution reaction (HER), two-dimensional (2D) molybdenum sulfide (MoS2) nanomaterials have evoked enormous research interest while it remains a great challenge in the structure control for high-performance HER electrocatalysis due to the lack of efficient preparation techniques. Herein, we reported a one-pot chemical method to directly synthesize 2D MoS2 with controllable layers. Multiply-layer MoS2 (ML-MoS2), few-layer MoS2 (FL-MoS2) and single-layer MoS2 coating on carbon nanotubes (SL-MoS2-CNTs) can be efficiently prepared through the modulation of experimental conditions. The enhanced catalytic activity is demonstrated in HER with the layer number of MoS2 nanosheets reducing. Remarkably, the optimized SL-MoS2-CNTs sample showed long-term durability with an accelerated degradation experiment even more than 10,000 recycles, and high HER activity with an onset overpotential of only ~40 mV vs. RHE. This study introduces a novel, cheap and facile strategy to prepare layer-controlled 2D MoS2 nanosheets with a large quantity, and are expected to broaden the already widely energy applications for 2D MoS2 nanosheets.
    RSC Advances 07/2014; · 3.71 Impact Factor
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    ABSTRACT: Electrolyzers and fuel cells have been extensively investigated as a promising solution for renewable energy storage and conversion. Hydrogen evolution reaction (HER) and oxygen reduction reaction (ORR) are important electrocatalytic processes in electrolyzers and fuel cells. Exploring efficient non-precious metal catalysts for HER and ORR in acidic medium remains a great challenge. Herein, we report graphene-supported iron-based nanoparticles encapsulated in nitrogen-doped carbon (Fe@N-C) hybrid material act as an efficient HER and ORR catalyst. The hybrid material was synthesized by pyrolysis of graphene oxide and ammonia ferric citrate followed by acid-leaching. During the pyrolysis, nitrogen was doped into graphene lattice, and the carbon nanoshell grown on graphene effectively suppressed the stacking of graphene sheet, exposing more active sites to reactants. The hybrid material showed higher electrocatalytic activities than graphene sheet or Fe@N-C alone, which was probably attributed to the synergetic role of nitrogen-doped graphene and Fe@N-C towards the electrocatalytic reactions.
    Faraday Discussions 07/2014; · 3.82 Impact Factor
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    ABSTRACT: Diffusion dynamics of guest molecules in nanopores has been studied intensively because diffusion is center to a number of research fields such as separation, drug delivery, chemical reactions and sensing. In the present work, we report an experimental investigation on the self-diffusion of water inside the carbon nanotube (CNT) channels using pulsed field gradient (PFG) NMR method. Dispersion of CNTs homogeneously in water and cooling down to temperatures below the melting point of bulk water allow us to probe the translational motion of confined water molecules. The results demonstrate that the self-diffusion coefficient of water in CNTs is highly dependent on the diffusion time and CNT diameter. Particularly, the diffusivity of water in double-walled carbon nanotubes (DWNTs) with an average inner diameter of 2.3±0.3 nm is twice of that in multi-walled carbon nanotubes (MWNTs) with an average inner diameter of 6.7±0.8 nm in the temperature range of 263 ─ 223 K. In addition, the effective self-diffusion coefficient in DWNTs is one order of magnitude higher than that reported for mesoporous silica materials with a similar pore size. The faster diffusivity of water in CNTs could be attributed to the ordered hydrogen bonding formed between water molecules within the confined channels of CNTs, and the weak interaction between water and CNT walls.
    Langmuir : the ACS journal of surfaces and colloids. 06/2014;
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    ABSTRACT: Interlayer expanded zeolites are derived from layered zeolite precursors by inserting a tetrahedrally coordinated atom (T-atom) in between the precursor layers. To achieve this expansion, a Si source like dichlorodimethylsilane or diethoxydimethylsilane is typically used. In the interlayer expansion of the layered zeolite precursor RUB-36, an Fe salt instead of a silylating agent was used to fill up the linking sites in between the layers. The obtained material showed a shift of the first XRD reflection similar to that of RUB-36 interlayer expanded with dichlorodimethylsilane, indicating an increase in interlayer distance. Diffuse reflectance UV-vis spectra and EPR characterization proved the incorporation of isolated Fe sites. Using FTIR spectroscopy with pyridine and acetonitrile as probe molecules, it was found that the incorporation of Fe results in an increase in Lewis acidity. The material was successfully used as a catalyst in the acylation of anisole with acetic anhydride and in the alkylation of toluene with benzyl chloride. The Fe incorporation proved to be remarkably stable. In spite of the HCl production during the alkylation reaction, no leaching was observed and the catalyst could be reused after regeneration.
    J. Mater. Chem. A. 06/2014; 2(25).
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    ABSTRACT: Structural changes of FeOx nanostructures supported on Pt(111) and Pt foil with response to oxidation and reduction treatments in O2 and H2 atmospheres upto 1.0 bar have been investigated by using X-ray photoelectron spectroscopy and scanning tunneling microscopy. We show that submonolayer O–Fe bilayer (FeO) structure on Pt(111) can be transformed to O–Fe–O trilayer (FeO2) upon oxidation in 5.0 × 10−6 mbar O2, while the FeO to FeO2 transformation happens over the full FeO film only with the O2 partial pressure above 1.0 × 10−3 mbar. Reduction of the submonolayer FeO2 structure back to the FeO structure occurs when exposed to 1.0 mbar H2 at room temperature (RT). In contrast, the full FeO2 structure can be kept even under 1.0 bar H2 exposure condition. The FeOx coverage and FeOx/Pt boundary play a critical role in the redox behavior of the supported FeOx nanostructures. Furthermore, we show that the FeOx nanostructures supported on Pt foil can be oxidized in a similar way as those on the Pt(111) surface. However, the Pt foil supported FeO2 nanostructures can be more deeply reduced to the state close to metallic Fe in 1.0 mbar H2 at RT. The close-packed Pt(111) surface exhibits a stronger confinement effect on the FeO overlayer than the open polycrystalline Pt surface.
    Topics in Catalysis 06/2014; 57(10-13). · 2.61 Impact Factor
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    ABSTRACT: In heterogeneous catalysis, graphitic carbon formed on metal often poisons metal-catalyzed reactions through physical blockage of surface active sites. In materials science, recent works show that graphene overlayers can passivate metal surfaces acting as gas-impermeable protection coatings. However, here we show using in situ surface electron microscopy and photoemission spectroscopy that CO can be readily trapped inside the two-dimensional space between the graphene overlayer and Ru(0001) surface under near-ambient conditions. The intercalated CO molecules effectively decouple the graphene overlayer from the Ru substrate. Meanwhile, the graphene cover exerts a strong confinement effect on the surface chemistry of CO on Ru(0001), showing that a high-coverage CO adlayer can be kept at the graphene/Ru interface at room temperature which desorbs intensively and completely around 390 K. This finding challenges the traditional concept of graphene films as passivation layers, indicating that the surface graphitic carbon can be used to modify the surface chemistry of metals.
    The Journal of Physical Chemistry C 05/2014; 118(23):12391–12398. · 4.84 Impact Factor
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    ABSTRACT: The efficient use of natural gas will require catalysts that can activate the first C-H bond of methane while suppressing complete dehydrogenation and avoiding overoxidation. We report that single iron sites embedded in a silica matrix enable direct, nonoxidative conversion of methane, exclusively to ethylene and aromatics. The reaction is initiated by catalytic generation of methyl radicals, followed by a series of gas-phase reactions. The absence of adjacent iron sites prevents catalytic C-C coupling, further oligomerization, and hence, coke deposition. At 1363 kelvin, methane conversion reached a maximum at 48.1% and ethylene selectivity peaked at 48.4%, whereas the total hydrocarbon selectivity exceeded 99%, representing an atom-economical transformation process of methane. The lattice-confined single iron sites delivered stable performance, with no deactivation observed during a 60-hour test.
    Science 05/2014; 344(6184):616-9. · 31.20 Impact Factor
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    ABSTRACT: Podlike nitrogen-doped carbon nanotubes encapsulating FeNi alloy nanoparticles (Pod(N)-FeNi) were prepared by the direct pyrolysis of organometallic precursors. Cyclic voltammetry (CV), electrochemical impedance spectroscopy (EIS), and Tafel polarization measurements revealed their excellent electrocatalytic activities in the I−/I3− redox reaction of dye-sensitized solar cells (DSSCs). This is suggested to arise from the modification of the surface electronic properties of the carbon by the encapsulated metal alloy nanoparticles (NPs). Sequential scanning with EIS and CV further showed the high electrochemical stability of the Pod(N)-FeNi composite. DSSCs with Pod(N)-FeNi as the counter electrode (CE) presented a power conversion efficiency of 8.82 %, which is superior to that of the control device with sputtered Pt as the CE. The Pod(N)-FeNi composite thus shows promise as an environmentally friendly, low-cost, and highly efficient CE material for DSSCs.
    Angewandte Chemie International Edition 05/2014; · 11.34 Impact Factor
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    ABSTRACT: Podlike nitrogen-doped carbon nanotubes encapsulating FeNi alloy nanoparticles (Pod(N)-FeNi) were prepared by the direct pyrolysis of organometallic precursors. Cyclic voltammetry (CV), electrochemical impedance spectroscopy (EIS), and Tafel polarization measurements revealed their excellent electrocatalytic activities in the I−/I3− redox reaction of dye-sensitized solar cells (DSSCs). This is suggested to arise from the modification of the surface electronic properties of the carbon by the encapsulated metal alloy nanoparticles (NPs). Sequential scanning with EIS and CV further showed the high electrochemical stability of the Pod(N)-FeNi composite. DSSCs with Pod(N)-FeNi as the counter electrode (CE) presented a power conversion efficiency of 8.82 %, which is superior to that of the control device with sputtered Pt as the CE. The Pod(N)-FeNi composite thus shows promise as an environmentally friendly, low-cost, and highly efficient CE material for DSSCs.
    Angewandte Chemie 05/2014;
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    ABSTRACT: Employing a low-cost and highly efficient electrocatalyst to replace Pt-based catalysts for hydrogen evolution reaction (HER) has attracted increasing interest in renewable energy research. Earth-abundant transition metals such as Fe, Co and Ni have been investigated as promising alternatives in alkaline electrolytes. However, these non-precious-metal catalysts are not stable in acids, excluding their application in the acidic solid polymer electrolyte (SPE). Herein, we report a strategy to encapsulate 3d transition metals Fe, Co and the FeCo alloy into nitrogen-doped carbon nanotubes (CNTs) and investigated their HER activity in acidic electrolyte. The optimized catalysts exhibited long-term durability and high activity with only a textasciitilde70 mV onset overpotential vs. RHE which is quite close to that of commercial 40% Pt/C catalyst, demonstrating the potential for the replacement of Pt-based catalysts. Density function theory (DFT) calculations indicated that the introduction of metal and nitrogen dopants can synergistically optimize the electronic structure of the CNTs and the adsorption free energy of H atom on CNTs, and therefore promote the HER with a Volmer-Heyrovsky mechanism.
    Energy & Environmental Science 04/2014; · 11.65 Impact Factor
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    ABSTRACT: An asymmetrically doped bilayer graphene is grown by modulation-doped chemical vapor deposition, which consists of one intrinsic layer and one nitrogen-doped layer according to AB stacking. The asymmetrically doped bilayer crystalline profile is found to extend the identical registry as adjacent pristine bilayer region, thus forming single-crystalline bilayer graphene p-n junctions. Efficient photocurrent with responsivity as high as 0.2 mA/W is generated at the bilayer p-n junctions via a hot carrier-assisted mechanism.
    Small 03/2014; · 7.82 Impact Factor

Publication Stats

2k Citations
1,334.32 Total Impact Points


  • 1998–2014
    • Chinese Academy of Sciences
      • • State Key Laboratory of Catalysis
      • • Dalian Institute of Chemical Physics
      Peping, Beijing, China
    • Dalian Institute of Chemical Physics
      Lü-ta-shih, Liaoning, China
  • 2011–2013
    • Peking University
      • College of Chemistry and Molecular Engineering
      Peping, Beijing, China
    • State Key Laboratory of Medical Genetics of China
      Ch’ang-sha-shih, Hunan, China
  • 1999–2013
    • Northeast Institute of Geography and Agroecology
      • State Key Laboratory of Catalysis
      Beijing, Beijing Shi, China
    • Tianjin University
      T’ien-ching-shih, Tianjin Shi, China
  • 2010
    • Shandong University
      • Institute of Theoretical Chemistry
      Jinan, Shandong Sheng, China
    • Northeast Normal University
      Hsin-ching, Jilin Sheng, China
  • 1993–2010
    • Max Planck Society
      München, Bavaria, Germany
  • 2009
    • CUNY Graduate Center
      New York City, New York, United States
  • 2007
    • Northeast Forestry University
      • Key Laboratory of Plant Ecology, Ministry of Education
      Charbin, Heilongjiang Sheng, China
  • 1993–2007
    • Fritz Haber Institute of the Max Planck Society
      • Department of Inorganic Chemistry
      Berlin, Land Berlin, Germany
  • 2006
    • Tsinghua University
      Peping, Beijing, China
  • 2002–2006
    • University of Science and Technology of China
      • Department of Chemical Physics
      Hefei, Anhui Sheng, China
  • 2005
    • Universität Stuttgart
      Stuttgart, Baden-Württemberg, Germany
  • 1999–2005
    • Dalian University of Technology
      • • School of Chemical Engineering
      • • State Key Laboratory of Fine Chemicals
      Dalian, Liaoning, China
  • 2004
    • Liaoning Normal University
      Lü-ta-shih, Liaoning, China
  • 2001
    • National Academy of Sciences of Ukraine
      • Institute of Physics
      Kievo, Kyiv City, Ukraine
  • 1994
    • Fudan University
      • Department of Chemistry
      Shanghai, Shanghai Shi, China