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Kojiro Nakai Yasunori Oumi Haruyuki Horie Tsuneji Sano Hideaki Yoshitake 《Microporous and mesoporous materials》2007,100(1-3):328-339
Bromination and subsequent ethylenediamine substitution of the CC double bond in mesoporous ethylenesilica were carried out to explore the characteristics of this periodic mesoporous organosilica. The structures of the products (BrPMO and EDA–BrPMO, respectively) were analysed by IR, Br K-edge EXAFS and NMR spectroscopies, as well as X-ray diffraction and nitrogen adsorption. We showed (1) that the formulae of the two products that formed were [CHBrSiO1.5]0.45[CHSiO1.5]0.55 and [NH2CH2CH2NHCHSiO1.5]0.05 [CHBrSiO1.5]0.40[CHSiO1.5]0.55, respectively, (2) that the addition of Br2 at room temperature occurred on the CC double bonds with disturbing the framework structure, (3) that IR absorption band of CC bonds that reacted with Br2 is significantly different from that of inactive CC bond, (4) that the length of the C–Br bond was considerably longer than in conventional alkyl bromides, and (5) that a large proportion of the ν(C–Br) band remained at the same position in the IR absorption spectrum after the ethylenediamine (EDA) substitution, while a new ν(C–Br) absorption also appeared. The mechanisms of these reactions are discussed at both the micro and mesoscopic levels.
Arsenate adsorption on EDA–BrPMO, in which the EDA is directly bound to the “surface” of the mesopores, was compared with adsorption on EDA–Pr–PMO, which was prepared by the direct synthesis of 3-chloropropyl-functionalized mesoporous ethanesilica followed by the substitution of Cl with EDA. The strength of the adsorption, as measured with the distribution coefficient, was greater for the former adsorbent than the latter. The origin of this difference was attributed to the distance between amino group and the surface. 相似文献
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Norihiro Moriyama Yuta Kawano Qing Wang Ryota Inoue Meng Guo Makoto Yokoji Hiroki Nagasawa Masakoto Kanezashi Toshinori Tsuru 《American Institute of Chemical Engineers》2021,67(7):e17223
Pervaporation (PV) is a membrane technology that holds great promise for industrial applications. To better understand the PV mechanism, PV dehydrations of various types of organic solvents (methanol, ethanol, iso-propanol, tert-butanol, and acetone) were performed on five types of organosilica and two types of silicon carbide-based membranes, all with different pore sizes. Water permeance was dependent on the types of organic aqueous solutions, which suggested that organic solvents penetrated the pores and hindered the permeation of water. In addition, water permeance of various types of membranes in PV was well correlated with hydrogen permeance in single-gas permeation. Furthermore, a clear correlation was obtained between the permeance ratio in PV and that in single-gas permeation, which was confirmed via the modified-gas translation model. These correlations make it possible to use single-gas permeation properties to predict PV performance. 相似文献
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Methylcyclohexane dehydrogenation for hydrogen production via a bimodal catalytic membrane reactor
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Lie Meng Xin Yu Takuya Niimi Hiroki Nagasawa Masakoto Kanezashi Tomohisa Yoshioka Toshinori Tsuru 《American Institute of Chemical Engineers》2015,61(5):1628-1638
The dehydrogenation of methylcyclohexane (MCH) to toluene (TOL) for hydrogen production was theoretically and experimentally investigated in a bimodal catalytic membrane reactor (CMR), that combined Pt/Al2O3 catalysts with a hydrogen‐selective organosilica membrane prepared via sol‐gel processing using bis(triethoxysilyl) ethane (BTESE). Effects of operating conditions on the membrane reactor performance were systematically investigated, and the experimental results were in good agreement with those calculated by a simulation model with a fitted catalyst loading. With H2 extraction from the reaction stream to the permeate stream, MCH conversion at 250°C was significantly increased beyond the equilibrium conversion of 0.44–0.86. Because of the high H2 selectivity and permeance of BTESE‐derived membranes, a H2 flow with purity higher than 99.8% was obtained in the permeate stream, and the H2 recovery ratio reached 0.99 in a pressurized reactor. A system that combined the CMR with a fixed‐bed prereactor was proposed for MCH dehydrogenation. © 2015 American Institute of Chemical Engineers AIChE J, 61: 1628–1638, 2015 相似文献
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Meng Guo Masakoto Kanezashi Hiroki Nagasawa Liang Yu Kazuki Yamamoto Takahiro Gunji Toshinori Tsuru 《American Institute of Chemical Engineers》2020,66(4):e16850
Fine-tuned, molecular-composite, organosilica membranes were fabricated via the co-condensation of organosilica precursors bis(triethoxysilyl)acetylene (BTESA) and bis(triethoxysilyl)benzene (BTESB). Fourier transform infrared and UV–vis spectra confirmed the co-condensation behaviors of BTESA and BTESB. The evolution of the network structure indicated that the incorporated BTESB decreased the membrane pore size, which was determined by a modified gas translation model according to the steric effect of the phenyl groups. The incorporation of BTESB to BTESA finely tuned the membrane structure and endowed the resultant composite membrane with improved separation properties. The BTESAB 9:1 membrane (molar ratio of BTESA/BTESB was 9:1) exhibited high C3H6 permeance at 4.5 × 10−8 mol m−2 s−1 Pa−1 and a C3H6/C3H8 permeance ratio of 33 at 50°C. One of the most important developments of this study involved clearly defining the relationship between membrane pore size and C3H6/C3H8 separation performance for organosilica membranes in single and binary separation systems. 相似文献
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《Journal of Industrial and Engineering Chemistry》2014,20(4):1703-1712
The efficiency of an ionic liquid based periodic mesoporous organosilica (PMO-IL) in the removal of sunset yellow from aqueous solutions using ultrasonic assisted adsorption method was investigated. The PMO-IL was first characterized by nitrogen sorption and TEM techniques. The optimized conditions (0.013 g of adsorbent, 32 mg L−1 of sunset yellow at 2 min of sonication time and pH 7) were obtained by central composite design (CCD). Fitting the equilibrium data show the suitability of the Langmuir model with second-order equation to control the kinetic of the adsorption process and good reusability (5 cycles) of PMO-IL for adsorption of dye. 相似文献
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Rong Xu Jinhui Wang Masakoto Kanezashi Tomohisa Yoshioka Toshinori Tsuru 《American Institute of Chemical Engineers》2013,59(4):1298-1307
Hybrid organosilica membranes were successfully prepared using bis(triethoxysilyl)ethane (BTESE) and applied to reverse osmosis (RO) desalination. The organosilica membrane calcined at 300°C almost completely rejected salts and neutral solutes with low‐molecular‐weight. Increasing the operating pressure led to an increase in water flux and salt rejection, while the flux and rejection decreased as salt concentration increased. The water permeation mechanism differed from the viscous flow mechanism. Observed activation energies for permeation were larger for membranes with a smaller pore size, and were considerably larger than the activation energy for water viscosity. The organosilica membranes exhibited exceptional hydrothermal stability in temperature cycles up to 90°C. The applicability of the generalized solution‐diffusion (SD) model to RO and pervaporation (PV) desalination processes were examined, and the quantitative differences in water permeance were accurately predicted by the application of generalized transport equations. © 2012 American Institute of Chemical Engineers AIChE J, 59: 1298–1307, 2013 相似文献
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Biodegradable Ethylene‐Bis(Propyl)Disulfide‐Based Periodic Mesoporous Organosilica Nanorods and Nanospheres for Efficient In‐Vitro Drug Delivery
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Lei Yu Panpan Pan Yu Zhang Yi Zhang Li Wan Xiaowei Cheng Yonghui Deng 《Small (Weinheim an der Bergstrasse, Germany)》2019,15(14)
Using interfacial reaction systems for biphasic catalytic reactions is attracting more and more attention due to their simple reaction process and low environmental pollution. Yolk–shell structured materials have broad applications in biomedicine, catalysis, and environmental remediation owing to their open channels and large space for guest molecules. Conventional methods to obtain yolk–shell mesoporous materials rely on costly and complex hard‐template strategies. In this study, a mild and convenient nonsacrificial self‐template strategy is developed to construct yolk–shell magnetic periodic mesoporous organosilica (YS‐mPMO) particles by using the unique swelling–deswelling property of low‐crosslinking density resorcinol formaldehyde (RF). The obtained YS‐mPMO microspheres possess an amphiphilic outer shell, high surface area (393 m2 g?1), uniform mesopores (2.58 nm), a tunable middle hollow space (50–156 nm), and high superparamagnetism (34.4–37.1 emu g?1). By tuning the synthesis conditions, heterojunction structured yolk–shell Fe3O4@RF@void@PMO particles with different morphologies can be produced. Owing to the amphipathy of PMO framworks, the YS‐mPMO particles show great emulsion stabilization ability and recyclability under a magnetic field. YS‐mPMO microspheres with immobilized Au nanoparticles (≈3 nm) act as both solid emulsifier for dispersing styrene (St) in water and interface catalysts for selective conversion of St into styrene oxide with a high selectivity of 86%, and yields of over 97%. 相似文献
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