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MOFs在多相催化中的应用MOFs在多相催化中的应用Outline

About“MOFs”ⅱMOFsinHeterogeneousCatalysis

IntroductionRecentProgressandProspect

OutlineⅰAbout“MOFs”可调控的孔结构及表面功能基团高比表面多孔材料所属领域相关材料最大比表面积(m2g-1)有序结构沸石904无序碳结构2030MOFs金属有机骨架由含氧、氮等的多齿有机配体与过渡金属离子自组装而成的配位聚合物MOFs:metal-organicframeworksPCPs:porouscoordinationpolymersMOCNs:metal-organiccoordinationnetworks相互作用:配位键(CB)氢键(HB)金属键(MB)π-π键(PP)可调控的孔结构及表面功能基团多孔材料所属领域相关材Zn4O(BDC)3(DMF)8-(C6H5Cl)MOF-5----Zn4O(BDC)3所属领域相关--Yaghietal.Science2002,295,469.Zn4O(BDC)3(DMF)8-(C6H5Cl)MOF-所属领域相关合成方法:金属+有机配体+溶剂

扩散法均相条件控制多相(缓释)釜式自组装水热溶剂热离子热潜在应用:磁性材料、光学材料、吸附分离、气体存储催化材料所属领域相关合成方法:金属+有机配体+溶剂催化MOFsinHeterogeneousCatalysisCoordinativelyunsaturatedmetalcenters(UMCs)CatalysismaterialscompletelyisolatedanduniformArrangementofUMCsMOFssynthesisstrategyMOFsinHeterogeneousCatalysiMOFsinHeterogeneousCatalysis--Fujitaetal.J.Am.Chem.Soc.1994,116,115[Cd(4,4’-bpy)2](NO3)21994,Fujitaetal.firstreportedMOFsappliedinHeterogeneousCatalysis.Benzaldehyde+cyanotrimethylsilane

2-(trimethylsiloxy)phenylacetonitrile

Cat.Yield77%MOFsinHeterogeneousCatalysiMOFsinHeterogeneousCatalysisPapers20Patents10

reactions:oxidation,epoxidation,carbonylation,hydration,alkoxylation,dehydrogenation,hydrogenation,isomerization,acylation,oligo-/polymerization,photocatalysis,asymmetriccatalysis

role:

catalyst(Lewisacid、base)

supportMOFsinHeterogeneousCatalysiMOFsinHeterogeneousCatalysis--Kimetal.Nature2000,404,9821-phenyl-2-propanolee.8%MOFsinHeterogeneousCatalysiMOFsinHeterogeneousCatalysis--W.Linetal.J.Am.Chem.Soc.2005,127,8940[Cd3Cl6L3]·4DMF·6MeOH·3H2OMOFsinHeterogeneousCatalysiMOFsinHeterogeneousCatalysis--W.Linetal.J.Am.Chem.Soc.2005,127,8940MOFsinHeterogeneousCatalysiMOFsinHeterogeneousCatalysis--W.Linetal.J.Am.Chem.Soc.2005,127,8940MOFsinHeterogeneousCatalysiMOFsinHeterogeneousCatalysis[Cd(4-btapa)2(NO3)2]·6H2O·2DMF--Kitagawaetal.J.Am.Chem.Soc.2007,129(9),2607.MOFsinHeterogeneousCatalysiMOFsinHeterogeneousCatalysis--Kitagawaetal.J.Am.Chem.Soc.2007,129(9),2607.Knoevenagelcondensation

MOFsinHeterogeneousCatalysiMOFsinHeterogeneousCatalysis--Morietal.J.Catal.2005,232,186MOFsinHeterogeneousCatalysiMOFsinHeterogeneousCatalysisReactionmechanismprioritycoordinationofolefinsontometalloporphyrinsintramoleculartransferofhydrogenfromarhodiumcentertoaolefinmoleculecoordinatedontometalloporphyrin--Morietal.J.Catal.2005,232,186MOFsinHeterogeneousCatalysi

MOFs在多相催化中的应用MOFs在多相催化中的应用Outline

About“MOFs”ⅱMOFsinHeterogeneousCatalysis

IntroductionRecentProgressandProspect

OutlineⅰAbout“MOFs”可调控的孔结构及表面功能基团高比表面多孔材料所属领域相关材料最大比表面积(m2g-1)有序结构沸石904无序碳结构2030MOFs金属有机骨架由含氧、氮等的多齿有机配体与过渡金属离子自组装而成的配位聚合物MOFs:metal-organicframeworksPCPs:porouscoordinationpolymersMOCNs:metal-organiccoordinationnetworks相互作用:配位键(CB)氢键(HB)金属键(MB)π-π键(PP)可调控的孔结构及表面功能基团多孔材料所属领域相关材Zn4O(BDC)3(DMF)8-(C6H5Cl)MOF-5----Zn4O(BDC)3所属领域相关--Yaghietal.Science2002,295,469.Zn4O(BDC)3(DMF)8-(C6H5Cl)MOF-所属领域相关合成方法:金属+有机配体+溶剂

扩散法均相条件控制多相(缓释)釜式自组装水热溶剂热离子热潜在应用:磁性材料、光学材料、吸附分离、气体存储催化材料所属领域相关合成方法:金属+有机配体+溶剂催化MOFsinHeterogeneousCatalysisCoordinativelyunsaturatedmetalcenters(UMCs)CatalysismaterialscompletelyisolatedanduniformArrangementofUMCsMOFssynthesisstrategyMOFsinHeterogeneousCatalysiMOFsinHeterogeneousCatalysis--Fujitaetal.J.Am.Chem.Soc.1994,116,115[Cd(4,4’-bpy)2](NO3)21994,Fujitaetal.firstreportedMOFsappliedinHeterogeneousCatalysis.Benzaldehyde+cyanotrimethylsilane

2-(trimethylsiloxy)phenylacetonitrile

Cat.Yield77%MOFsinHeterogeneousCatalysiMOFsinHeterogeneousCatalysisPapers20Patents10

reactions:oxidation,epoxidation,carbonylation,hydration,alkoxylation,dehydrogenation,hydrogenation,isomerization,acylation,oligo-/polymerization,photocatalysis,asymmetriccatalysis

role:

catalyst(Lewisacid、base)

supportMOFsinHeterogeneousCatalysiMOFsinHeterogeneousCatalysis--Kimetal.Nature2000,404,9821-phenyl-2-propanolee.8%MOFsinHeterogeneousCatalysiMOFsinHeterogeneousCatalysis--W.Linetal.J.Am.Chem.Soc.2005,127,8940[Cd3Cl6L3]·4DMF·6MeOH·3H2OMOFsinHeterogeneousCatalysiMOFsinHeterogeneousCatalysis--W.Linetal.J.Am.Chem.Soc.2005,127,8940MOFsinHeterogeneousCatalysiMOFsinHeterogeneousCatalysis--W.Linetal.J.Am.Chem.Soc.2005,127,8940MOFsinHeterogeneousCatalysiMOFsinHeterogeneousCatalysis[Cd(4-btapa)2(NO3)2]·6H2O·2DMF--Kitagawaetal.

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