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Dr. Na Sheng Ye Ma Qianwen Zhu Xin Hong Juan Zhang Prof. Jun Xu Feng Deng Prof. Junliang Sun Prof. Zhaochi Feng Prof. Liang Wang Prof. Xiangju Meng Prof. Feng-Shou Xiao 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(50):11408-11411
Unlike conventional aluminosilicate zeolites synthesized in alkaline media, aluminophosphate molecular sieves (AlPOs) have always been prepared under acidic conditions in the past three decades; this has been regarded as one of essential factors for synthesis, except for the case of silica-substituted analogues (SAPOs). For the first time, we demonstrate herein a simple and generalized route for synthesizing various types of aluminophosphate molecular sieves in alkaline media. A series of aluminophosphate sieves and their analogues have been prepared with different quaternary ammonium cations as structure-directing agents in this manner. The above successes have extended the systematic media from acidic or neutral to alkaline for the preparation of a series of aluminophosphate molecular sieves, which possibly open an alternative route for the synthesis of aluminophosphate molecular sieves. 相似文献
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Furio Corà Maria Alfredsson Carolyn M Barker Rob G Bell Martin D Foster Iman Saadoune Alexandra Simperler C.Richard A Catlow 《Journal of solid state chemistry》2003,176(2):496-529
We present a thorough computational study of transition metal-doped zeolite and aluminophosphate (AlPO) frameworks. The structural and electronic chemistry of the dopants is examined with ab initio quantum mechanical calculations, and the results correlated with the Brønsted and Lewis acid strength, and with the redox potential of the dopant ions in the framework. The energetics of doping is provided, and is employed to analyze the mode of dopant incorporation, and its site ordering in the microporous framework. In total, 23 dopant ions are examined in the isostructural framework of chabasite and AlPO-34. These cover most of the isomorphous framework replacements known to occur experimentally, but also framework replacements that have not yet been achieved. In this case, ab initio modeling techniques are employed in a predictive way. Finally, we present a computational study of the alkene epoxidation on titanosilicates, that covers the whole catalytic cycle. 相似文献
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Daniel M. Dawson Robert F. Moran Scott Sneddon Sharon E. Ashbrook 《Magnetic resonance in chemistry : MRC》2019,57(5):176-190
The 31P chemical shift anisotropy (CSA) offers a potential source of new information to help determine the structures of aluminophosphate (AlPO) framework materials. We investigate how to measure the CSAs, which are small (span of ~20–30 ppm) for AlPOs, demonstrating the need for CSA-amplification experiments (often in conjunction with 27Al and/or 1H decoupling) at high magnetic field (20.0 T) to obtain accurate values. We show that the most shielded component of the chemical shift tensor, δ33, is related to the length of the shortest P─O bond, whereas the more deshielded components, δ11 and δ22 can be related more readily to the mean P─O bond lengths and P─O─Al angles. Using the case of Mg-doped STA-2 as an example, the CSA is shown to be much larger for P(OAl)4–n(OMg)n environments, primarily owing to a much shorter P─O(Mg) bond affecting δ33, however, because the mean P─O bond lengths and P─O─T (T = Al, Mg) bond angles do not change significantly between P(OAl)4 and P(OAl)4–n(OMg)n sites, the isotropic chemical shifts for these species are similar, leading to overlapped spectral lines. When the CSA information is included, spectral assignment becomes unambiguous, therefore, although the specialist conditions required might preclude the routine measurement of 31P CSAs in AlPOs, in some cases (particularly doped materials), the experiments can still provide valuable additional information for spectral assignment. 相似文献
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Large pore aluminophosphate-based molecular sieves like AlPO4-5, MAPO-5, MnAPO-5 and ZAPO-5 were synthesised hydrothermally using triethylamine as a structure directing agent. These materials
were characterised by X-ray diffraction (XRD),27A1 and31P MAS-NMR, ICP-MS,n-butylamine-TPD, BET and SEM. The catalytic performance of these materials was tested for isopropylation of benzene with 2-propanol
at 250, 300, 350 and 400°C. The products were cumene,p-DIPB (p-diisopropylbenzene) andm-DIPB (m-diisopropylbenzene). MnAPO-5 was found to be more active than the other catalysts. Maximum conversion (20%) was noted at
350°C over MnAPO-5. The selectivity to DIPB was found to decrease with time on stream but the selectivity to cumene showed
an increase after 3 h of time on stream 相似文献
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