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1.
Clickable Periodic Mesoporous Organosilicas: Synthesis,Click Reactions,and Adsorption of Antibiotics
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Dr. Jinsuo Gao Xueying Zhang Dr. Shutao Xu Prof. Feng Tan Prof. Xinyong Li Prof. Yaobin Zhang Prof. Zhenping Qu Prof. Xie Quan Dr. Jian Liu 《Chemistry (Weinheim an der Bergstrasse, Germany)》2014,20(7):1957-1963
Pharmaceutical antibiotics are not easily removed from water by conventional water‐treatment technologies and have been recognized as new emerging pollutants. Herein, we report the synthesis of clickable azido periodic mesoporous organosilicas (PMOs) and their use as adsorbents for the adsorption of antibiotics. Ethane‐bridged PMOs, functionalized with azido groups at different densities, were synthesized by the co‐condensation of 1,2‐bis(trimethoxysilyl)ethane (BTME) and 3‐azidopropyltrimethoxysilane (AzPTMS), in the presence of nonionic‐surfactant triblock‐copolymer P123, in an acidic medium. Four different alkynes were conjugated to azide‐terminated PMOs by means of an efficient click reaction. The clicked PMOs showed improved adsorption capacity (241 μg g?1) for antibiotics (ciprofloxacin hydrochloride) compared with azido‐functionalized PMOs because of the enhanced π–π stacking interactions. These results indicate that click reactions can introduce multifunctional groups onto PMOs, thus demonstrating the great potential of PMOs for environmental applications. 相似文献
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A General Method for Preparing Bridged Organosilanes with Pendant Functional Groups and Functional Mesoporous Organosilicas
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Prof. Jana Hodačová Dr. Guillaume Toquer Dr. Xavier Cattoën Dr. Michel Wong Chi Man 《Chemistry (Weinheim an der Bergstrasse, Germany)》2014,20(33):10371-10382
New organosilica precursors containing two triethoxysilyl groups suitable for the organosilica material formation through the sol‐gel process were designed and synthesised. These precursors display alkyne or azide groups for attaching targeted functional groups by copper‐catalysed azide–alkyne cycloaddition (CuAAC) and can be used for the preparation of functional organosilicas following two strategies: 1) the functional group is first appended by CuAAC under anhydrous conditions, then the functional material is prepared by the sol‐gel process; 2) the precursor is first subjected to the sol‐gel process, producing porous, clickable bridged silsesquioxanes or periodic mesoporous organosilicas (PMOs), then the desired functional groups are attached by means of CuAAC. Herein, we show the feasibility of both approaches. A series of bridged bis(triethoxysilane)s with different pending organic moieties was prepared, demonstrating the compatibility of the first approach with many functional groups. In particular, we demonstrate that organic functional molecules bearing only one derivatisation site can be used to produce bridged organosilanes and bridged silsesquioxanes. In the second approach, clickable PMOs and porous bridged silsesquioxanes were prepared from the alkyne‐ or azide‐containing precursors, and thereafter, functionalised with complementary model azide‐ or alkyne‐containing molecules. These results confirmed the potential of this approach as a general methodology for preparing functional organosilicas with high loadings of functional groups. Both approaches give rise to a wide range of new functional organosilica materials. 相似文献
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S. Shylesh Prinson P. Samuel Sheetal Sisodiya A. P. Singh 《Catalysis Surveys from Asia》2008,12(4):266-282
Micelle-templated mesoporous and organic–inorganic hybrid mesoporous materials are important in many fields of material research,
especially for hosting catalysts in confined space. Among this class, the recent discovery of periodic mesoporous organosilicas
(PMOs) represent an exciting new group of organic–inorganic nanocomposites targeted for a broad range of applications ranging
from catalysis to microelectronics. Compared to the earlier generation of organic–inorganic hybrid mesoporous samples, obtained
by the cocondensation reaction or by the grafting reaction, PMOs represent the right combination of organic and inorganic
groups in the frame wall positions. This article reviews the current state of art in organic–inorganic hybrid mesoporous material
research with special emphasis over periodic mesoporous organosilica materials having various redox centers (Ti, V, Cr) suitable
for oxidation reactions as well as acidic sites (Al, –SO3H) for the organic transformation of bulky molecules. 相似文献
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分别采用1,4-(双乙氧基硅烷)苯(1,4-BTEB)和1,2-三乙氧基硅基乙烷(1,2-BTESE)作为有机硅源,正硅酸乙酯(TEOS)为无机硅源,钛酸四丁酯(TBOT)为钛源,以Pluronic EO20PO70EO20(P123)为模板剂在酸性环境下水热合成制备了Ti掺杂的有机-无机有序介孔有机硅材料Ti-SBA-15-ben和Ti-SBA-15-et.同时,在合成过程中加入H2O2作为配合剂调节钛源水解速度,制备得到Ti-SBA-15-ben-H和Ti-SBA-15-et-H.采用FT-IR、DR UV-Vis、N2物理吸附、XRD、TG-DSC、TEM等方法对制备的样品进行了表征.结果表明:合成过程中加入H2O2制备的苯基桥连有机硅杂化材料具有较好的疏水性能,其骨架中活性4价位钛含量高,结构有序性最好.在以叔丁基过氧化氢(TBHP)为氧源的环己烯氧化反应中对制备的催化材料进行了对比评价,结果表明:Ti-SBA-15-ben-H表现出最高的催化活性,其催化的反应以环氧化产物为主,环己烯的转化率为26.9%,环氧选择性为32.8%,T i-SBA-15-et催化的反应以烯丙位氧化产物2-环己烯-1-酮为主,环己烯的转化率为8.5%,2-环己烯-1-酮选择性为41.2%. 相似文献
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You-Kyong Seo 《Journal of solid state chemistry》2006,179(4):1285-1288
Mesoporous hybrid material containing urethane moieties in functionalized long chain organic group have been synthesized by using bis[3-(triethoxysilyl) propyl urethane]ethane (BTESPUE) and tetraethoxysilane as structural ingredients. The incorporation of BTESPUE within the framework of mesoporous material was confirmed by Fourier transform-infrared, X-ray photoelectron spectroscopy, solid-state NMR spectroscopy and thermogravimetric analysis. This material had a thick wall and uniform pore, which may be attributed to the hydrogen bonding inside framework due to urethane moieties. 相似文献
8.
《Ultrasonics sonochemistry》2014,21(1):387-394
Benzene-bridged periodic mesoporous organosilicas (PMOs) with the MCM-41 were synthesized by a rapid sonochemical process via co-condensation of tetraethoxysilane (TEOS) and 1,4-bis(triethoxysilyl) benzene (BTEB) under basic conditions within a few minutes using cetyltrimethylammoniumbromide (CTMABr) as a structure-directing agent. The molar ratio of the silicon precursors and the synthesis time were varied in order to investigate their influence on the structural ordering of the materials. The characteristics of the materials were evaluated by X-ray diffraction (XRD), N2-sorption, transmission electron microscopy (TEM) and solid-state NMR spectroscopy. The resultant materials exhibited well-ordered hexagonal mesostructures with surface areas in the range of 602–1237 m2/g, pore volumes of 0.37–0.68 cm3/g, and pore diameters in the range of 2.5–3.5 nm. Two dimensional 29Si{1H} heteronuclear correlation (HETCOR) NMR spectra confirmed the formation of a single mesophase with various Q (from TEOS) and T (from BTEB) silicon species located randomly within the pore walls due to the co-condensation of BTEB and TEOS, which excluded the possibility of formation of island or two separate phases within such a short synthesis time. The prime advantage of the present synthesis route is that it can effectively reduce the total synthesis time from days to a few minutes, much shorter than the conventional benzene-bridged PMOs synthesis methods. 相似文献
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YANG QiHua LIU Jian & ZHANG Lei State Key Laboratory of Catalysis Dalian Institute of Chemical Physics Chinese Academy of Sciences Dalian China 《中国科学:化学》2010,(2)
The integration of organic and inorganic fragments within the pore walls of the periodic mesoporous organosilicas (PMOs) represents one of the recent breakthroughs in material science. The resulting PMOs are promising materials for applications in such areas as catalysis, adsorption, separation and drug-delivery. We summarize here the recent progress made in the synthesis of PMOs with hierarchical structures and large functional groups, with special emphasis on the chiral mesoporous organosilicas and their ... 相似文献
10.
Two series of ordered mesoporous organosilica (OMO) SBA-15 materials with surface and bridging groups were fabricated by varying
the organic precursor addition at different synthesis stages. The consequence of the delayed introduction of organic precursor
on the structural and adsorption properties of the resulting OMOs was investigated. The OMOs studied were synthesized via
co-condensation of tetraethyl orthosilicate (TEOS) and ureidopropyltrimethoxysilane (UPS) as well as TEOS and bis(triethoxysilylpropyl)
disulfide (BTDS) in the presence of poly(ethylene oxide)-poly(propylene oxide)- poly(ethylene oxide) triblock copolymer Pluronic
P123 (EO20PO70EO20). The aforementioned OMOs were characterized by nitrogen adsorption-desorption isotherms at −196 °C and powder X-ray diffraction
(XRD). Nitrogen adsorption isotherms were used to estimate the pore volume, mesopore diameter and the BET specific surface
area, whereas the XRD data provided information about structural ordering and unit cell of the samples studied.
Ryan Felix, undergraduate student from Oberlin College (Oberlin, OH, USA) participating in the NSF-REU program during Summer
2006. 相似文献