贺鹤勇
从事多相催化、固体核磁共振和多孔材料的合成和结构表征研究
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- 姓名:贺鹤勇
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学术头衔:
博士生导师
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学科领域:
勘查地质学
- 研究兴趣:从事多相催化、固体核磁共振和多孔材料的合成和结构表征研究
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11
【期刊论文】Evidence for strong acidity of the molecular sieve cloverite
贺鹤勇, Tery L. Barr*, ‡, Jacek Klinowski*, Heyong He*, Klaus AlberU*, Georg Miiller‡ & Johannes A. Lercher
NATURE VOL 365 30 SEPTEMBEF 1993,-0001,():
-1年11月30日
ZEOLITES derive their catalytic activity from the strong acidity of protons attached to the negatively charged aluminosilicate frame-work, which makes the materials excellent proton donors. Unlike zeolites, the aluminophosphate molecular sieves1,2 are built from alternating AIO4 and PO tetrahedra and are thus electrically neutral. Much attention has therefore been devoted to the genera-tion of Br0nsted acidity in these materials by introducing het-eroatoms, such as Si, Mg, Fe, Co or Zn, to produce negatively charged frameworks3-6. Similar arguments apply to gallophos-phate molecular sieves7-10, of which cioverite9,to is a remarkable example. This extra-large-pore material contains pore openings in the form of a four-leafed clover, defined by a ring of 20 gallium and phosphorus atoms, some of which are linked to terminal hydroxyl groups. Here we use NMR, X-ray photoelectron spectroscopy (ESCA) and infrared spectroscopy to show that the P-OH groups in cloverite are localized versions of those in solid phosphoric acid, H3PO4. Cloverite is thus a strong Br0nsted acid even though no heteroatoms are present in its framework.
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贺鹤勇, Heyong He a, Paul Barnes b, Juliet Munn b, Xavier Turrillas b and Jacek Klinowski a
Volume 196, number 3,4,-0001,():
-1年11月30日
The synthesis of DPA-VPI-5 and TBA-VPI-5 and their phase transformation to AIPO4-8 have been studied by X-ray diffraction in situ. The synchrotron radiation-energy dispersive diffraction is shown to be able to monitor these two fast reactions in real time. The results indicate that nucleation may occur already during the aging of the synthesis gel. The different rates oftransformtion of DPA-VPI-5 and TBA-VPI-5 show that the microstructure of the two materials is different.
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【期刊论文】Solid-State NMR Studies of Fullerene C60/Benzene Solvates
贺鹤勇, Heyong He, † Jamie Barras, †, ‡ John Foulkes, § and Jacek Klinowski *
118 J. Phys. Chem. B, Vol. 101, No.2, 1997,-0001,():
-1年11月30日
Stable van der Waals-bonded C60/benzene solvates were prepared using a novel crystallization technique. Solid-state NMR measurements on highly crystalline solvate under liquid benzene show that there is very little interaction between benzene and the C60 molecules and that the rotation of C60 at room temperature is not hindered. The magnetization transfer between benzene protons and local C60 molecules is highly inefficient. Three benzene species have been found in the solvate: two, nearly freely mobile, in wide and narrow porous structures, and the third constrained by C60 molecules in lattice defects. Premelting of deuterated benzene within the C60 solvate has been observed at Tm-10.5 K.
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【期刊论文】Synthesis of TBA-VPI-5 and DPA-VPI-5
贺鹤勇, Heyong He and Jacek Klinowski*
J. Phys. Chem. 1994,98, 1192-1197,-0001,():
-1年11月30日
The synthesis of TBA-and DPA-VPI-5 has been studied in detail. Optimal synthesis conditions have been established using ternary composition diagrams for TBA-Al203-PzOs and DPA-Al203-PzO. Gel samples at different aging times have been examined using chemical analysis, X-ray diffraction, FT-IR, and solid-state NMR. Two reactions occur between H3P04 and pseudo-boehmite during gel aging. Interaction between the acid and the OH groups linking the pseudo-boehmite layers leads to the formation of an AI-0-P species in which A1 is 6-coordinated. A further reaction between the acid and the AI-O-P species results in the formation of a 4-coordinated A1 species. Because of the different aging conditions, the latter reaction begins much earlier in the TBA system than in the DPA system. The behavior of DPA in the synthesis gel is different from that of TBA. There is evidence that crystallization of VPI-5 proceedsvia a solid-state mechanism, and that nucleation in both systems occurs already during the aging of the gels.
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【期刊论文】Solid-State NMR Studies of the Structure of Graphite Oxide
贺鹤勇, Heyong He, † Thomas Riedl, ‡ Anton Lerf, ‡ and Jacek Klinowski *, †
J. Phys. Chem. 1996, 100, 19954-19958,-0001,():
-1年11月30日
Graphite oxide (GO) and its derivatives have been studied using 13C and 1H NMR. The 13C NMR lines at 60, 70, and 130 ppm are assigned to C-OH, C-O-C, and>CdC<groups in the bulk of the material, respectively. The>CdC<double bonds are relatively stable, while C-OH groups may condense to form C-O-C (ether) linkages. There are at least two magnetically inequivalent C-OH sites, and the structure does not necessarily possess long-range order. Water molecules interact very strongly with the structure. The results reveal a number of new structural features.
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【期刊论文】Effects of support modification on Nb2O5/-Al2O3 catalyst for ethylene oxide hydration
贺鹤勇, Yingcheng Li a, b, Shirun Yan a, *, Weimin Yang b, Zaiku Xie b, Qingling Chen b, Bin Yue a, Heyong He a, ∗
Journal of Molecular Catalysis A: Chemical 226(2005)285-290,-0001,():
-1年11月30日
Effect of MgAl2O4 on the structure, acidity as well as the catalytic performance of Nb2O5/-Al2O3 catalyst for ethylene oxide hydration was studied using IR, XRD, NH3-TPD, CO2-TPD and catalytic reaction. Modification of Al2O3 support with MgAl2O4 led to an increase in both basicity and mechanical strength of the support. As a result, the density and strength of the acidity of the niobium oxide catalyst supported on the MgAl2O4 modified -Al2O3 reduced in comparison with that supported on the pure -Al2O3. The acidity of 10% Nb2O5/MgAl2O4/-Al2O3 decreased with increasing loading of MgAl2O4. Catalytic test showed that EO conversion decreased monotonously with increasing MgAl2O4 loading, whereas the selectivity to MEG exhibited a maximum of 90.6% at MgAl2O4 loading of 2.23%. In terms of MEG yield, optimal MgAl2O4 loading should be around 2%. Durability test emonstrated that 10% Nb2O5/MgAl2O4/-Al2O3 catalyst exhibited excellent stability within 1000 h time-on-stream.
Ethylene oxide, Hydration, Niobia, MgAl2O4, Support, Modification
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贺鹤勇, Xueying Chen, Shuai Wang, Jihua Zhuang, Minghua Qiao ∗, Kangnian Fan, Heyong He ∗
Journal of Catalysis 227(2004)419-427,-0001,():
-1年11月30日
The effects of pore structure on the reaction rates and selectivities in the liquid-phase hydrogenation of 2-ethylanthraquinone over Ni-B amorphous alloy catalysts prepared by the reductant-impregnation method were studied using regular (HMS, MCM-41, and SBA-15) and commercial mesoporous silicas as supports. The composition, particle size, and location of the Ni-B particles were profoundly influenced by the pore structure of the supports. It is found that the location of the Ni-B particles depended on the pore size of the supports, whereas the uniformity of particle size was related to the interaction between the Ni-B particles and the supports. The hydrogenation rate was much faster on Ni-B catalysts with pore diameters exceeding 5 nm than on the narrow-pore catalysts, whereas the selectivity to 2-ethyldihydroanthraquinone, the carbonyl group hydrogenation product, was higher on Ni-B catalysts supported on regular mesoporous silicas. The best activity and selectivity were achieved when using SBA-15 as the support, which is attributable to the formation of more uniform active sites due to the unique pore structure of SBA-15.
Ni-B amorphous alloy, Mesoporous silica, 2-Ethylanthraquinone, Hydrogenation, H2-O2
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【期刊论文】Selective catalytic hydration of ethylene oxide over niobium oxide supported on -alumina
贺鹤勇, Yingcheng Li a, b, Shirun Yan a, *, Bin Yue a, Weimin Yang b, Zaiku Xie b, Qingling Chen b, Heyong He a,
Applied Catalysis A: General 272(2004)305-310,-0001,():
-1年11月30日
Niobium oxide (Nb2O5) supported on alumina (-Al2O3) prepared by impregnation was studied for hydration of ethylene oxide. The effects of niobium oxide loadings, calcination temperature and molar ratio of water to ethylene oxide (EO) on the reaction performance were investigated. The structure and acidity of the catalysts were characterized by using X-ray diffraction (XRD), differential thermal analysis (DTA)-thermogravimetric (TG) and infrared (IR) of pyridine adsorption. A durability test of niobic acid and Nb2O5/-Al2O3 catalyst was carried out over a period of 1000h. It was found that Nb2O5/-Al2O3 demonstrated very high activity and selectivity for hydration of ethylene oxide to monoethylene glycol (MEG) under mild conditions. Compared with the result of non-catalytic reactions, the conversion of ethylene oxide was increased from 34 to 99.8% on keeping monoethylene glycol selectivity almost unchanged when the hydration was carried out over 10wt.%Nb2O5/-Al2O3 catalyst. The yield of monoethylene glycol over Nb2O5/-Al2O3 was higher than that obtained over other solid acid catalysts. Moreover, the supported niobia catalyst demonstrated excellent stability and no deactivation was observed within 1000h of time-on-stream.
Niobium oxide, Ethylene oxide, Monoethylene glycol, Hydration, Stability
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【期刊论文】n-Butane isomerization over Cs-salts of H3 PW12 O40: a mechanistic study by 1C MAS NMR
贺鹤勇, Zhuona Ma, Weiming Hua, Yu Ren, Heyong He, Zi Gao
Applied Catalysis A: General 256(2003)243-250,-0001,():
-1年11月30日
Reaction mechanism of skeletal isomerization of n-butane over Cs2.5H0.5P W12O40 catalyst was studied using 13C MAS NMR.The reaction proceeds mainly via a monomolecular mechanism at 80℃. The contribution of the bimolecular mechanism becomes more significant as the reaction temperature is increased to 150℃. Hydrogen suppresses the bimolecular mechanism, in particular on Pt-promoted Cs2. 5H0. 5P W12 O40 catalyst. The latter catalyst is highly selective to isobutane in the presence of H2 even at 220℃. The kinetics of the monomolecular isomerization reaction and the reaction schemes of 13C scrambling and n-butane isomerization are discussed.
Cs salts of H3 PW12O40, n-Butane isomerization, Reaction mechanism, 13C MAS NMR
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【期刊论文】A new structural model for graphite oxide
贺鹤勇, Heyong He a, Jacek Klinowski a, *, Michael Forster b, Anton Lerf b
Chemical Physics Letters 287 1998.53-56,-0001,():
-1年11月30日
Solid-state 13C NMR spectra of graphite oxide GO. and its derivatives prompt us to propose a new structural model. The spectra of GO treated with KI and the course of the thermal decomposition of GO reveal the presence of epoxide groups, responsible for the oxidating nature of the material. GO is built of aromatic'islands' of variable size which have not been oxidized, and are separated from each other by aliphatic 6-membered rings containing C-OH, epoxide groups and double bonds. The carbon grid is nearly flat; a small degree of warping is caused by the carbons attached to OH groups, which are in a slightly distorted tetrahedral configuration.
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