Abstract Heterogeneous catalysts with convenient recyclability and reusability are vitally important to reduce the cost of catalysts as well as to avoid complex separation and recovery operations. In this regard, magn...Abstract Heterogeneous catalysts with convenient recyclability and reusability are vitally important to reduce the cost of catalysts as well as to avoid complex separation and recovery operations. In this regard, magnetic MIL-100 （Fe）@SiO2@Fe3O4 microspheres with a novel core-shell structure were fabricated by the in-situ self-assembly of a metal-organic MIL- 100（Fe） framework around pre-synthesized magnetic SiO2@Fe3O4 particles under relatively mild and environmentally benign conditions. The catalytic activity of the MIL-100（Fe）@SiO2@Fe3O4 catalyst was tested for the liquid-phase acetalization of benzaldehyde and glycol. The MIL-100（Fe）@SiO2@Fe3O4 catalyst has a significant amount of accessible Lewis acid sites and therefore exhibited good acetalization catalytic activity. Moreover, due to its superparamagnetism properties, the heterogeneous MIL-100（Fe）@SiO2@Fe3O4 catalyst can be easily isolated from the reaction system within a few seconds by simply using an external magnet. The catalyst could then be reused at least eight times without significant loss in catalytic efficiency.展开更多
通过等体积浸渍法制备了金属有机骨架材料MIL-53(Al)(MIL:Materials of Institut Lavoisier)负载纳米Pd催化剂.采用X射线衍射(XRD)、透射电子显微镜(TEM)和X射线光电子能谱(XPS)等手段对催化剂的结构进行了表征.催化剂在反应前后XRD衍...通过等体积浸渍法制备了金属有机骨架材料MIL-53(Al)(MIL:Materials of Institut Lavoisier)负载纳米Pd催化剂.采用X射线衍射(XRD)、透射电子显微镜(TEM)和X射线光电子能谱(XPS)等手段对催化剂的结构进行了表征.催化剂在反应前后XRD衍射峰保持不变,说明载体MIL-53(Al)具有良好的稳定性.采用TEM对催化剂进行表征,结果表明,MIL-53(Al)的多孔晶体结构有助于形成高度分散的纳米Pd颗粒,样品2.7%(w)Pd/MIL-53中Pd颗粒的平均粒径为2.21 nm.该催化剂在CO氧化反应中表现出较高的催化活性,115°C达到完全转化.同时催化剂可循环使用,多次反应后催化活性和催化剂结构都保持稳定.展开更多
Heteropoly acids(HPA) are well known for their versatile solid acid catalysis in diverse chemical reactions, however they suffer from low surface area(<10 m^2/g) and leaching into the reactions media, which reduce ...Heteropoly acids(HPA) are well known for their versatile solid acid catalysis in diverse chemical reactions, however they suffer from low surface area(<10 m^2/g) and leaching into the reactions media, which reduce their prospects as industrial catalyst.Herein, a novel hybrid material HPW@Zr-BTC,composed of 12-tungstophoric acid(HPW) and Zr^(Ⅳ)-benzene tri-carboxylate(Zr-BTC) metal-organic framework(MOF), was prepared via one-pot solvothermal method. Excellent HPW loading up to 32.3 wt% was achieved, and HPW@Zr-BTC composite proved to be highly stable, besides the crystalline morphology of Zr-BTC was intact. The catalytic activity of the hybrid composite was explored via Friedel-Crafts acylation of anisole with benzoyl chloride.The 28.2 wt% HPW@Zr-BTC showed excellent catalytic performance, with 99.4% anisole conversion and 97.6% yield(pmethoxybenzophenone) under solvent free conditions. Excellent retention of catalytic activity was achieved after at least five consecutive runs due to non-observable HPW leaching. The promising activity and stability of the catalyst forecasted its potential industrial applications.展开更多
Nanosized MCM-41-SO3H based on ordered mesoporous silica material with a covalent sulfonic acid group was synthesized and used as acid catalyst for the new, simple, convenient and green synthesis of 2,4,5-trisubstitut...Nanosized MCM-41-SO3H based on ordered mesoporous silica material with a covalent sulfonic acid group was synthesized and used as acid catalyst for the new, simple, convenient and green synthesis of 2,4,5-trisubstituted and 1,2,4,5-tetra-substituted imidazoles. Also some of synthesis products are new. Echo-friendly protocol, short reaction times, easy and quick isolation of the products and excellent yields are the main advantages of this procedure.展开更多
A variety of terminal arylacetylenes have been conveniently synthesized in good to high yields via Sonogashira coupling of aryl iodides with （trimethylsilyl）acetylene catalyzed by MCM-41-supported mercapto palladium...A variety of terminal arylacetylenes have been conveniently synthesized in good to high yields via Sonogashira coupling of aryl iodides with （trimethylsilyl）acetylene catalyzed by MCM-41-supported mercapto palladium（0） complex, followed by desilylation under mild conditions. This polymeric palladium catalyst can be reused many times without any decrease in activity.展开更多
基金Acknowledgements This work was supported by the National Natural Science Foundation of China （Grant No. 21576243） and the Public Project of Zhejiang Province of China （2016C37057）.
文摘Abstract Heterogeneous catalysts with convenient recyclability and reusability are vitally important to reduce the cost of catalysts as well as to avoid complex separation and recovery operations. In this regard, magnetic MIL-100 （Fe）@SiO2@Fe3O4 microspheres with a novel core-shell structure were fabricated by the in-situ self-assembly of a metal-organic MIL- 100（Fe） framework around pre-synthesized magnetic SiO2@Fe3O4 particles under relatively mild and environmentally benign conditions. The catalytic activity of the MIL-100（Fe）@SiO2@Fe3O4 catalyst was tested for the liquid-phase acetalization of benzaldehyde and glycol. The MIL-100（Fe）@SiO2@Fe3O4 catalyst has a significant amount of accessible Lewis acid sites and therefore exhibited good acetalization catalytic activity. Moreover, due to its superparamagnetism properties, the heterogeneous MIL-100（Fe）@SiO2@Fe3O4 catalyst can be easily isolated from the reaction system within a few seconds by simply using an external magnet. The catalyst could then be reused at least eight times without significant loss in catalytic efficiency.
基金The project was supported by the National Natural Science Foundation of China(21073235,21173270,21177160)National High-Tech Research and Development Program of China(863)(2013AA061902)~~
文摘通过等体积浸渍法制备了金属有机骨架材料MIL-53(Al)(MIL:Materials of Institut Lavoisier)负载纳米Pd催化剂.采用X射线衍射(XRD)、透射电子显微镜(TEM)和X射线光电子能谱(XPS)等手段对催化剂的结构进行了表征.催化剂在反应前后XRD衍射峰保持不变,说明载体MIL-53(Al)具有良好的稳定性.采用TEM对催化剂进行表征,结果表明,MIL-53(Al)的多孔晶体结构有助于形成高度分散的纳米Pd颗粒,样品2.7%(w)Pd/MIL-53中Pd颗粒的平均粒径为2.21 nm.该催化剂在CO氧化反应中表现出较高的催化活性,115°C达到完全转化.同时催化剂可循环使用,多次反应后催化活性和催化剂结构都保持稳定.
基金supported by the National Key Research and Development Program of China(2016YFB0601303)the National Natural Science Foundation of China(51374193,21676278)+1 种基金Key Program of National Natural Science Foundation of China(9143420)Chinese Academy of Sciences,State Administration of Foreign Experts Affairs(CAS/SAFEA)International Partnership Program for Creative Research Teams(20140491518)
文摘Heteropoly acids(HPA) are well known for their versatile solid acid catalysis in diverse chemical reactions, however they suffer from low surface area(<10 m^2/g) and leaching into the reactions media, which reduce their prospects as industrial catalyst.Herein, a novel hybrid material HPW@Zr-BTC,composed of 12-tungstophoric acid(HPW) and Zr^(Ⅳ)-benzene tri-carboxylate(Zr-BTC) metal-organic framework(MOF), was prepared via one-pot solvothermal method. Excellent HPW loading up to 32.3 wt% was achieved, and HPW@Zr-BTC composite proved to be highly stable, besides the crystalline morphology of Zr-BTC was intact. The catalytic activity of the hybrid composite was explored via Friedel-Crafts acylation of anisole with benzoyl chloride.The 28.2 wt% HPW@Zr-BTC showed excellent catalytic performance, with 99.4% anisole conversion and 97.6% yield(pmethoxybenzophenone) under solvent free conditions. Excellent retention of catalytic activity was achieved after at least five consecutive runs due to non-observable HPW leaching. The promising activity and stability of the catalyst forecasted its potential industrial applications.
文摘Nanosized MCM-41-SO3H based on ordered mesoporous silica material with a covalent sulfonic acid group was synthesized and used as acid catalyst for the new, simple, convenient and green synthesis of 2,4,5-trisubstituted and 1,2,4,5-tetra-substituted imidazoles. Also some of synthesis products are new. Echo-friendly protocol, short reaction times, easy and quick isolation of the products and excellent yields are the main advantages of this procedure.
基金the National Natural Science Foundation of China (No.20462002)Natural Science Foundation of Jiangxi Province (No.0420015)for financial support.
文摘A variety of terminal arylacetylenes have been conveniently synthesized in good to high yields via Sonogashira coupling of aryl iodides with （trimethylsilyl）acetylene catalyzed by MCM-41-supported mercapto palladium（0） complex, followed by desilylation under mild conditions. This polymeric palladium catalyst can be reused many times without any decrease in activity.
