Browsing by Author "Wu, H"
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- ItemMetal-organic frameworks with exceptionally high methane uptake: where and how is methane stored?(Wiley-VCH Verlag Berlin, 2010-05-03) Wu, H; Simmons, JM; Liu, Y; Brown, CM; Wang, XS; Ma, S; Peterson, VK; Southon, PD; Kepert, CJ; Zhou, HC; Yildirim, T; Zhou, WMetal–organic frameworks (MOFs) are a novel family of physisorptive materials that have exhibited great promise for methane storage. So far, a detailed understanding of their methane adsorption mechanism is still scarce. Herein, we report a comprehensive mechanistic study of methane storage in three milestone MOF compounds (HKUST-1, PCN-11, and PCN-14) the CH4 storage capacities of which are among the highest reported so far among all porous materials. The three MOFs consist of the same dicopper paddlewheel secondary building units, but contain different organic linkers, leading to cagelike pores with various sizes and geometries. From neutron powder diffraction experiments and accurate data analysis, assisted by grand canonical Monte Carlo (GCMC) simulations and DFT calculations, we anambiguously revealed the exact locations of the stored methane molecules in these MOF materials. We found that methane uptake takes place primarily at two types of strong adsorption site: 1) the open Cu coordination sites, which exhibit enhanced Coulomb attraction toward methane, and 2) the van der Waals potential pocket sites, in which the total dispersive interactions are enhanced due to the molecule being in contact with multiple “surfaces”. Interestingly, the enhanced van der Waals sites are present exclusively in small cages and at the windows to these cages, whereas large cages with relatively flat pore surfaces bind very little methane. Our results suggest that further, rational development of new MOF compounds for methane storage applications should focus on enriching open metal sites, increasing the volume percentage of accessible small cages and channels, and minimizing the fraction of large pores. © 2010, Wiley-VCH Verlag Berlin
- ItemOn line neutron flux mapping in fuel coolant channels of a research reactor(IEEE, 2014-01-30) Barbot, L; Domergue, C; Villard, JF; Destouches, C; Braoudakis, G; Wassink, D; Sinclair, B; Osborn, JC; Wu, H; Blandin, C; Thévenin, M; Corre, G; Normand, SThis work deals with the on-line neutron flux mapping of the OPAL research reactor. A specific irradiation device has been set up to investigate fuel coolant channels using subminiature fission chambers to get thermal neutron flux profiles. Experimental results are compared to first neutronic calculations and show good agreement (C/E ~0.97). © 2022 IEEE
- ItemOPAL Reactor: calculation/experiment comparison of neutron flue mapping in fuel coolant channels(International Group On Research Reactors, 2013-10-13) Barbot, L; Domergue, C; Villard, JF; Destouches, C; Braoudakis, G; Wassink, D; Sinclair, B; Osborn, JC; Wu, HThe measurement and calculation of the neutron flux mapping of the OPAL research reactor are presented. Following an investigation of fuel coolant channels using sub-miniature fission chambers to measure thermal neutron flux profiles, neutronic calculations were performed. Comparison between calculation and measurement shows very good agreement. © The Authors
- ItemQuantified zero thermal expansion in magnetic R2Fe17-based intermetallic compounds (R = rare earth)(American Chemical Society, 2023-06-13) Cao, YL; Matsukawa, T; Gibbs, A; Avdeev, M; Wang, CW; Wu, H; Huang, QZ; Ohoyama, K; Ishigaki, T; Zhou, H; Li, Q; Miao, J; Lin, K; Xing, XRZero thermal expansion (ZTE) has been a fascinating task for the past few decades due to its great scientific and practical merits. To realize ZTE, negative thermal expansion is typically employed by chemical substitutions on tuning structure features, which often relies on trial and error. Here, we report on exploring quantification of thermal expansion with magnetic ordering in an intermetallic class of R2Fe17 (R = rare earth), which can accurately determine the ZTE composition using a documented database. It demonstrates that the magnetic ordering of the Fe-sublattice contributes to the thermal expansion anomaly through simultaneous examinations of magnetization and neutron powder diffraction. Alternative elements can be manipulated on a Fe-sublattice to control both the total ordered magnetic moments of the Fe-sublattice and Curie temperature, which tailors the temperature variation of the magnetic contributions on thermal expansion. The current work might point to a future for ZTE high throughput searches, anticipated to benefit applications. © 2023 American Chemical Society
- ItemStructure and lateral Iiteraction in mixed monolayers of dioctadecyldimethylammonium chloride (DOAC) and stearyl alcohol(American Chemical Society, 2013-05-07) Ge, A; Wu, H; Darwish, TA; James, M; Osawa, M; Ye, Sπ-A isotherms, atomic force microscopy (AFM), and sum frequency generation (SFG) vibrational spectroscopy are employed to investigate the molecular structure and lateral interactions in mixed monolayers of dioctadecyldimethylammonium chloride (DOAC) and stearyl alcohol (SA) at air/water and air/solid interfaces. To avoid possible interference between the two molecules in the SFG spectroscopic measurements, perprotonated DOAC and perdeuterated SA (dSA) were used. The thermodynamic analyses for the π-A isotherms show that DOAC is miscible with dSA. SFG observations reveal that DOAC molecules become conformationally ordered as dSA molecules are introduced into the monolayer. AFM observations demonstrate coexistence of DOAC-rich and dSA-rich domains in the mixed monolayer with ratios different from their initial composition in the subphase. The present study suggests that DOAC molecules in the mixed monolayer are condensed by mixing with dSA in which the repulsive interactions between positively charged head groups of the DOAC molecules are largely reduced along with an increase of van der Waals interactions with dSA.© 2013, American Chemical Society.