The distribution of Fe and the adsorption of NH3 in H-[Fe]MOR （mordenite） were investigated using dispersion corrected density functional theory （DFT-D2）.Based on the results,it can be found that the most favorabl...The distribution of Fe and the adsorption of NH3 in H-[Fe]MOR （mordenite） were investigated using dispersion corrected density functional theory （DFT-D2）.Based on the results,it can be found that the most favorable site for the distribution of Fe is T1O6,followed by T2O5,T4O2 and T3O1,and energy differences for Fe in different T sites are less than 0.09 eV,indicating that Fe atoms may distribute in all kinds of T sites in MOR.In addition,the adsorption energies for NH3 at each crystallographic position of H-[Fe]MOR were also determined.Finally,it can be concluded that the Br（o）nsted acid site at T2O5 is stronger than the other acid sites,and the adsorption of NH3 on Br（o）nsted acid sites is more stable than on Lewis acid sites.展开更多
A series of WO3/CeO2 （WOx/CeO2） catalysts were synthesized by wet impregnation of ammonium metatungstate on a CeO2 support. The resulting solid acid catalysts were characterized by X-ray diffraction （XRD）, UV-Vis ...A series of WO3/CeO2 （WOx/CeO2） catalysts were synthesized by wet impregnation of ammonium metatungstate on a CeO2 support. The resulting solid acid catalysts were characterized by X-ray diffraction （XRD）, UV-Vis spectroscopy （UV-Vis）, Raman spectroscopy （Raman）, in-situ Fourier transform infrared spectroscopy （in-situ FT-IR） of ammonia adsorption, NH3-TPD, H2 temperature- programmed reduction （H2-TPR）, NH3/NO oxidation and activity measurements for NOx reduction by NH3 （NH3-SCR）. The results show that polytungstate （WOx） species are the main species of tungsten oxide on the surface of ceria. The addition of tungsten oxide enhances the BriSnsted acidity of ceria catalysts remarkably and decreases the amount of surface oxygen on celia, with strong interaction between CeO2 and WOx. As a result, the N2 selectivity of NH3 oxidation and NH3-SCR at high temperatures （〉 300℃） is enhanced. Therefore, a wide working temperature window in which NOx conversion exceeds 80% （NOx conversion 〉 80%） from 200 to 450℃, is achieved over 10 wt.% WOx/CeO2 catalyst. A tentative model of the NH3-SCR reaction route on WOx/CeO2 catalysts is presented.展开更多
Motivated by the recent realization ofgraphene sensor to detect gas molecules that are harmful to the environment, the ammonia adsorption on graphene or graphene oxide （GO） was investigated using first-princi- ples ...Motivated by the recent realization ofgraphene sensor to detect gas molecules that are harmful to the environment, the ammonia adsorption on graphene or graphene oxide （GO） was investigated using first-princi- ples calculation. The optimal adsorption and orientation of the NH3 molecules on the graphene surfaces were determined, and the adsorption energies （Eb） as well as the Mulliken charge transfers ofNH3 were calculated. The Eb for the graphene are small and seem to be independent of the sites and orientations. The surface epoxy or hydroxyl groups can promote the adsorption of NH3 on the GO; the enhancement of the Eb for the hydroxyl groups is greater than that for the epoxy groups on the surface. The charge transfers from the molecule to the surfaces also exhibit the same trend. The Brōnsted acid sites and Lewis acid sites could stably exist on the GO with surface hydroxyl groups and on the basal, respectively.展开更多
Vertically aligned γ-AlOOH nanosheets （NSs） have been successfully fabricated on flexible Al foils via a solvothermal route without morphology-directing agents. Three different reaction temperature （25, 80, and 1...Vertically aligned γ-AlOOH nanosheets （NSs） have been successfully fabricated on flexible Al foils via a solvothermal route without morphology-directing agents. Three different reaction temperature （25, 80, and 120 ℃） and time （30 min, 45 min, and 24 h） are discussed for the growth period, which efficiently tune the density and size of theγ-AlOOH NSs. Meanwhile, the growth speed of the nanosheets confirms that dominant growth stage is seen in the initial 45 min. Furthermore, the interlayer of the γ-AlOOH NSs displays an average height of 140 nm and superhydrophilicity. By dynamic adsorption, the as- synthesized γ-AlOOH NSs exhibit an outstanding NH3 adsorption capacity of up to 146 mg/g and stably excellent regeneration for 5 cycles. The mechanism of NH3 adsorption on the in-plane of the γ-AlOOH NSs is explained by the Lewis acid/base theory. The H-bond interactions among the NH3 molecules and the edge groups （-OH） further improve the capture ability of the nanosheets.展开更多
基金Computational Chemistry Laboratory of School of Chemical Engineering and EnvironmentNatural Science Foundationof Shanxi Province(No.2009011014)Shenzhen Strategic Emerging Industries Special Fund Program of China(No.GGJS20120619101655715)
文摘The distribution of Fe and the adsorption of NH3 in H-[Fe]MOR （mordenite） were investigated using dispersion corrected density functional theory （DFT-D2）.Based on the results,it can be found that the most favorable site for the distribution of Fe is T1O6,followed by T2O5,T4O2 and T3O1,and energy differences for Fe in different T sites are less than 0.09 eV,indicating that Fe atoms may distribute in all kinds of T sites in MOR.In addition,the adsorption energies for NH3 at each crystallographic position of H-[Fe]MOR were also determined.Finally,it can be concluded that the Br（o）nsted acid site at T2O5 is stronger than the other acid sites,and the adsorption of NH3 on Br（o）nsted acid sites is more stable than on Lewis acid sites.
基金the Ministry of Science and Technology, PR China for financial support of Project 2010CB732304Science and Technology Department of Zhejiang Province Project 2011C31010
文摘A series of WO3/CeO2 （WOx/CeO2） catalysts were synthesized by wet impregnation of ammonium metatungstate on a CeO2 support. The resulting solid acid catalysts were characterized by X-ray diffraction （XRD）, UV-Vis spectroscopy （UV-Vis）, Raman spectroscopy （Raman）, in-situ Fourier transform infrared spectroscopy （in-situ FT-IR） of ammonia adsorption, NH3-TPD, H2 temperature- programmed reduction （H2-TPR）, NH3/NO oxidation and activity measurements for NOx reduction by NH3 （NH3-SCR）. The results show that polytungstate （WOx） species are the main species of tungsten oxide on the surface of ceria. The addition of tungsten oxide enhances the BriSnsted acidity of ceria catalysts remarkably and decreases the amount of surface oxygen on celia, with strong interaction between CeO2 and WOx. As a result, the N2 selectivity of NH3 oxidation and NH3-SCR at high temperatures （〉 300℃） is enhanced. Therefore, a wide working temperature window in which NOx conversion exceeds 80% （NOx conversion 〉 80%） from 200 to 450℃, is achieved over 10 wt.% WOx/CeO2 catalyst. A tentative model of the NH3-SCR reaction route on WOx/CeO2 catalysts is presented.
文摘Motivated by the recent realization ofgraphene sensor to detect gas molecules that are harmful to the environment, the ammonia adsorption on graphene or graphene oxide （GO） was investigated using first-princi- ples calculation. The optimal adsorption and orientation of the NH3 molecules on the graphene surfaces were determined, and the adsorption energies （Eb） as well as the Mulliken charge transfers ofNH3 were calculated. The Eb for the graphene are small and seem to be independent of the sites and orientations. The surface epoxy or hydroxyl groups can promote the adsorption of NH3 on the GO; the enhancement of the Eb for the hydroxyl groups is greater than that for the epoxy groups on the surface. The charge transfers from the molecule to the surfaces also exhibit the same trend. The Brōnsted acid sites and Lewis acid sites could stably exist on the GO with surface hydroxyl groups and on the basal, respectively.
文摘Vertically aligned γ-AlOOH nanosheets （NSs） have been successfully fabricated on flexible Al foils via a solvothermal route without morphology-directing agents. Three different reaction temperature （25, 80, and 120 ℃） and time （30 min, 45 min, and 24 h） are discussed for the growth period, which efficiently tune the density and size of theγ-AlOOH NSs. Meanwhile, the growth speed of the nanosheets confirms that dominant growth stage is seen in the initial 45 min. Furthermore, the interlayer of the γ-AlOOH NSs displays an average height of 140 nm and superhydrophilicity. By dynamic adsorption, the as- synthesized γ-AlOOH NSs exhibit an outstanding NH3 adsorption capacity of up to 146 mg/g and stably excellent regeneration for 5 cycles. The mechanism of NH3 adsorption on the in-plane of the γ-AlOOH NSs is explained by the Lewis acid/base theory. The H-bond interactions among the NH3 molecules and the edge groups （-OH） further improve the capture ability of the nanosheets.
