层状前体法制备复合氧化物及其负载型固体碱催化剂的结构与性能研究
|
摘要
随着世界环保意识的加强以及绿色化学的发展,研制环境友好的固体碱催化剂越来越受到研究者的重视。本文采用层状前体法制备了复合氧化物及其负载型固体碱催化剂,对其结构和性能进行了详细的研究,并初步探讨了催化反应机理。本文的主要内容和创新点如下:
将3d金属作为剪裁催化剂酸碱性的元素制备了复合氧化物型固体碱催化剂。采用成核/晶化隔离法制备了催化剂前体MgAlFe-CO_3-LDHs和CoMgAlFe-CO_3-LDHs,静态空气气氛中,不同温度焙烧得到复合氧化物型固体碱催化剂,采用XRD、FT-IR、In situHTXRD、TG/DTA-MS、BET、CO_2-TPD、XPS和苯酚吸附等表征技术对催化剂前体的结构、热稳定性及催化剂的比表面积、孔径分布、表面性质、碱性进行了详细研究,并以Knoevenagel缩合反应为探针反应研究了催化性能,探讨了其反应机理。结果表明,催化剂前体的层板金属元素组成和焙烧温度是影响催化剂活性的两个主要因素。以MgAlFe-CO_3-LDHs前体经500℃焙烧得到的催化剂活性最好,催化剂表面碱性是影响催化剂活性的主要因素,而催化剂的比表面积和孔径分布影响较小。催化剂表面的中强碱性位(M~(n+)-O~(2-))是Knoevenagel缩合反应的活性中心。详细研究了Fe的摩尔含量的变化对催化活性的影响,由于Fe的电负性较Mg、Al强,发现当0.02≤Fe/(Mg+Al+Fe)＜0.06时,随着Fe含量的增加,Lewis酸性位有所增加,由于酸碱协同作用催化活性高于同等条件下合成的MgAl复合氧化物;Fe/(Mg+Al+Fe)≥0.06时,Fe含量增加,碱密度降低,催化活性降低。表明通过向层状前体中适当添加3d金属离子,可有效剪裁复合氧化物型催化剂的酸碱性,使其适应于不同酸碱强度要求的催化反应,从而为该类催化剂应用范围的拓宽提供了新思路。
首次将成核/晶化隔离法制备的MgAl复合氧化物作为载体,制备了负载KF固体碱催化剂,详细研究了催化剂结构、热分解性能和表面性质并用吸附CO_2后的原位红外和Hammett函数法研究了其酸碱性。采用碳酸乙烯酯(EC)和甲醇的酯交换反应为探针反应考察了其催化性能。研究表明,催化剂的活性中心是表面均匀分散的F~-。KF的负载量是影响催化活性的重要因素之一,负载11.8wt%KF催化活性最好,碳酸乙烯酯的转化率为94%,碳酸二甲酯(DMC)的选择性为81%,DMC的时空收率STY为0.75mmol/(g cat·min),是相同条件下,单纯MgAl复合氧化物的38倍,是文献报道Mg2.5Al-OH-LDHs催化剂活性的7倍。
With strengthen of people's environment protection consciousness and the development of green chemistry,employment of eco-friendly solid bases catalysis in the fine chemical industry is of topical interest.In present paper,mixed oxides and KF-supported mixed oxides solid base catalysts were synthesized based on layered double hydroxides(LDHs) precursors.The structure and physico-chemical properties of the prepared catalysts were studied systematically.The novelty and major content of the thesis were detailed as follows:
A kind of mixed metal oxide type solid base catalysts were obtained through calcining precursors of MgAlFe-CO_3-LDHs,CoMgAlFe -CO_3-LDH in which Fe~(3+)species were chosen as a tailoring element controlling acid-base property.The structural,thermal,textural and bases properties of the mixed oxids were examined by using XRD,FT-IR,in situ high temperature XRD,TG-MS,CO_2-TPD,phenol adsorption and Knoevenagel condensation reactivity.The results manifest that the compositions and calcined temperature significantly affect the catalytic activity.Fe-500 derived from MgAlFe-CO_3-LDHs have the highest activity.And the catalytic activity is majorly dependent on the basic strength and the quantity of the surface basic sites,but less on the surface area and pore size.The middle strength basic site is critical for Knoevenagel condensation.Moreover,the Fe content significantly affect the catalytic activity.With Fe molar fraction range of 0.02≤Fe/(Mg+Al+Fe)＜0.06,catalytic activity of MgAlFe oxides is higher than that of MgAl mixed oxides from MgAl-CO_3-LDH,probably because that surface segregation of Fe in the samples with lower Fe content moderately increases the number of Lewis acidic sites and thus activates the carbonyl group of benzaldehyde.When Fe/(Mg+Al+Fe)beyond 0.06, the number of acidic site is enhanced with increasing content of Fe, whereas the reduced number of base sites result in a lower catalytic activity.
A series of KF-supported MgAl mixed oxides was synthesized from the layered precursors for the first time.Their basicity character is revealed mainly by in situ FT-IR after adsorption of CO_2 and transesterification reaction of ethylene carbonate(EC)and methanol.The results manifest that the higher basicity and activity of catalysts is correlated to the highly dispersed F~-.The loading content of KF affects the catalytic activity.When the content of KF was 11.8 wt%,the EC conversion reaches 94%and the selectivity to dimethyl carbonate(DMC) is 81%.The corresponding space time yield(STY)is 0.75 DMC mmol/(g cat·min),which was 38 times to the as-prepared MgAl mixed oxides,and 7 times to Mg_(2.5)Al-OH-LDHs reported in literature.
The present eco-friendly catalyst is a potential alternative to soluble bases in the fine chemical industry.
将3d金属作为剪裁催化剂酸碱性的元素制备了复合氧化物型固体碱催化剂。采用成核/晶化隔离法制备了催化剂前体MgAlFe-CO_3-LDHs和CoMgAlFe-CO_3-LDHs,静态空气气氛中,不同温度焙烧得到复合氧化物型固体碱催化剂,采用XRD、FT-IR、In situHTXRD、TG/DTA-MS、BET、CO_2-TPD、XPS和苯酚吸附等表征技术对催化剂前体的结构、热稳定性及催化剂的比表面积、孔径分布、表面性质、碱性进行了详细研究,并以Knoevenagel缩合反应为探针反应研究了催化性能,探讨了其反应机理。结果表明,催化剂前体的层板金属元素组成和焙烧温度是影响催化剂活性的两个主要因素。以MgAlFe-CO_3-LDHs前体经500℃焙烧得到的催化剂活性最好,催化剂表面碱性是影响催化剂活性的主要因素,而催化剂的比表面积和孔径分布影响较小。催化剂表面的中强碱性位(M~(n+)-O~(2-))是Knoevenagel缩合反应的活性中心。详细研究了Fe的摩尔含量的变化对催化活性的影响,由于Fe的电负性较Mg、Al强,发现当0.02≤Fe/(Mg+Al+Fe)＜0.06时,随着Fe含量的增加,Lewis酸性位有所增加,由于酸碱协同作用催化活性高于同等条件下合成的MgAl复合氧化物;Fe/(Mg+Al+Fe)≥0.06时,Fe含量增加,碱密度降低,催化活性降低。表明通过向层状前体中适当添加3d金属离子,可有效剪裁复合氧化物型催化剂的酸碱性,使其适应于不同酸碱强度要求的催化反应,从而为该类催化剂应用范围的拓宽提供了新思路。
首次将成核/晶化隔离法制备的MgAl复合氧化物作为载体,制备了负载KF固体碱催化剂,详细研究了催化剂结构、热分解性能和表面性质并用吸附CO_2后的原位红外和Hammett函数法研究了其酸碱性。采用碳酸乙烯酯(EC)和甲醇的酯交换反应为探针反应考察了其催化性能。研究表明,催化剂的活性中心是表面均匀分散的F~-。KF的负载量是影响催化活性的重要因素之一,负载11.8wt%KF催化活性最好,碳酸乙烯酯的转化率为94%,碳酸二甲酯(DMC)的选择性为81%,DMC的时空收率STY为0.75mmol/(g cat·min),是相同条件下,单纯MgAl复合氧化物的38倍,是文献报道Mg2.5Al-OH-LDHs催化剂活性的7倍。
With strengthen of people's environment protection consciousness and the development of green chemistry,employment of eco-friendly solid bases catalysis in the fine chemical industry is of topical interest.In present paper,mixed oxides and KF-supported mixed oxides solid base catalysts were synthesized based on layered double hydroxides(LDHs) precursors.The structure and physico-chemical properties of the prepared catalysts were studied systematically.The novelty and major content of the thesis were detailed as follows:
A kind of mixed metal oxide type solid base catalysts were obtained through calcining precursors of MgAlFe-CO_3-LDHs,CoMgAlFe -CO_3-LDH in which Fe~(3+)species were chosen as a tailoring element controlling acid-base property.The structural,thermal,textural and bases properties of the mixed oxids were examined by using XRD,FT-IR,in situ high temperature XRD,TG-MS,CO_2-TPD,phenol adsorption and Knoevenagel condensation reactivity.The results manifest that the compositions and calcined temperature significantly affect the catalytic activity.Fe-500 derived from MgAlFe-CO_3-LDHs have the highest activity.And the catalytic activity is majorly dependent on the basic strength and the quantity of the surface basic sites,but less on the surface area and pore size.The middle strength basic site is critical for Knoevenagel condensation.Moreover,the Fe content significantly affect the catalytic activity.With Fe molar fraction range of 0.02≤Fe/(Mg+Al+Fe)＜0.06,catalytic activity of MgAlFe oxides is higher than that of MgAl mixed oxides from MgAl-CO_3-LDH,probably because that surface segregation of Fe in the samples with lower Fe content moderately increases the number of Lewis acidic sites and thus activates the carbonyl group of benzaldehyde.When Fe/(Mg+Al+Fe)beyond 0.06, the number of acidic site is enhanced with increasing content of Fe, whereas the reduced number of base sites result in a lower catalytic activity.
A series of KF-supported MgAl mixed oxides was synthesized from the layered precursors for the first time.Their basicity character is revealed mainly by in situ FT-IR after adsorption of CO_2 and transesterification reaction of ethylene carbonate(EC)and methanol.The results manifest that the higher basicity and activity of catalysts is correlated to the highly dispersed F~-.The loading content of KF affects the catalytic activity.When the content of KF was 11.8 wt%,the EC conversion reaches 94%and the selectivity to dimethyl carbonate(DMC) is 81%.The corresponding space time yield(STY)is 0.75 DMC mmol/(g cat·min),which was 38 times to the as-prepared MgAl mixed oxides,and 7 times to Mg_(2.5)Al-OH-LDHs reported in literature.
The present eco-friendly catalyst is a potential alternative to soluble bases in the fine chemical industry.
引文
[1]Tanabe K.Catalysis by Acids and Bases[J].Elsevier Amsterdam,1985,1:20-27.
[2]Brindlye G W,Kikkawa S.Thermal behavior of hydrotalcite and of anion-exchanged forms of hydrotalcite[J].Calys Caly Miner.,1980,28:87-91.
[3]Pines H,Stalick W M.Base-catalyzed Reactions of Hydrocarbons and Relatec Compounds[D].New York:Academic Press,1977
[4]Reichle W T.Catalytic reactions by thermally activated,synthetic,anionic clay minerals [J].J.Catal.,1985,94:547-557
[5]Cavani F,TrifirO F,Vaccari A.Hydrotalcite-type anionic clays:preparation,properties and applications[J].Catal.Today,1991,11(2):173-301
[6]田部浩三等.新固体酸和碱及其催化作用[M].北京:化学工业出版社,1992
[7]魏彤,王谋华,魏伟,孙予罕,钟炳.固体碱催化剂[J].化学通报,2002,9:594-600
[8]Pacheco M A,Marshall C L.Review of Dimethyl Carbonate(DMC)Manufacture and Its Characteristics as a Fuel Additive[J].Energy&Fuels,1997,11:2-29
[9]东北师范大学,华南师范大学等编.有机化学(下册)[M].北京:高等教育出版社,1992:88-89
[10]Lin X,Chuah G K,Jaenicka S.Base-functionalized MCM-41 as catalysts for the synthesis of monoglycerides[J].J.Mol.Catal.A:Chemical,1999,150:287-294
[11]朱洪法.催化剂载体制备及应用技术[MI.北京:石油工业出版社,2002
[12]Hattori H.Heterogeneous basic catalysis[J].Chem Rev,1995,95(3):537-558
[13]赵雷洪,郑小明,费金华.稀土氧化物固体碱催化剂的表面性质[J].催化学报,1996,17(3):227-231
[14]Zhang H,QI R,Duan X.,Evans D G.Synthesis and characterization of a novel nanoscale magnetic solid base catalyst involving a layered double hydroxide supported on a ferrite core[J].J.Solid State Chem.,2004,177:772-7801
[15]Climent M J,Corma A,Iborra S.Activated hydrotalcites as catalysts for the synthesis of chalcones of pharmaceutical interest[J].J.Catal.,2004,221(2):474-482
[16]Climent M J,Corma A,Iborra S.Base catalysis for fine chemicals production:Claisen-Schmidt condensationon zeolites and hydrotalcites for the production of chal-cones and flavanones of pharmaceutical interest[J].J.Catal.,1995,151(1):60-66
[17]Caldararu H,Caragheorgheopol A,Corma A.One eletron donor sites and their strength distribution on some hydrotalcite and MgO surfaces as studied by EPR spectroscopy[J].J.Chem.Soc.Faraday Trans.,1994,90,(1):213-218
[18]Corma A,Fornes V,Rey F.Hydrotalcites as base catalysts:influence of the chemical composition and synthesis conditions on the dehydrogenation of isopropanol[J].J.Catal.,1994,148(1):205-212
[19]Weitkamp J,Hunger M,Rymsa U.Base catalysis on microporous and mesoporous materials:recent progress and perspectives[J].Micro.Meso.Mater.,2001,48:255-270
[20]Vera R L.Constantino and Thomas J.Pinnavaia,Basic Properties of Mg~(2+)_(1-X)Al~(3+)_X Layered Double Hydroxides Intercalated by Carbonate Hydroxide,Chloride,and Sulfate Anions[J].Inorg.Chem.,1995,34:883-892.
[21]杨锡尧,任韶玲,何晖,王大庆.新型催化剂载体材料—镁铝复合氧化物的制备及 其物理化学性质[J].分子催化,1996,10(2):88-94.
[22]徐景士,王红明,吴志明.微波法制备的固体碱催化丁醛自缩合反应[J].精细化工,2002,19(11):644-646
[23]Weinstock L.M.,Stevenson J.M.,Tomellini S.A.,Pan S.,Utne T.,Jobson R.B.,Reinhold D.F.,Characterization of the actual catalytic agent in potassium fluoride on activated alumina systems[J].Tetrahedron Lett.,1986,27:3845-3848.
[24]Ando T,Clark J H,Cork D G,Hanafusa T,Ichihara J,Kimura T.Fluoride-alumina reagents:the active basic species[J].Tetrahedron Lett.,1987,28(13):1421-1424
[25]Kabashima H,Tsuji H,Nakata S,Tanaka Y,Hattori H.Activity for base-catalyzed reactions and characterization of alumina-supported KF catalysts[J].Appl.Catal.A,2000,227:194-195
[26]Handa H,Baba T,Sugisawa H,Ono Y.Highly efficient self-condensation of benzaldehyde to benzyl benzoate over KF-loaded alumina[J].J.Mol.Catal.A,1998,134:171-177.
[27]Ando T,Brown S J,Clark J H,Cork D G,Hanafusa T,Ichihara J,Miller J M,Robertson M.S.Alumina-supported fluoride reagents for organic synthesis:optimisation of reagent preparation and elucidation of the active species[J].J.Chem.Sot.,Perkin Trans.,1986,2:1133-1139.
[28]Clacens J,Genuit D,Delmotte L,Garcia-Ruiz A,Bergeret G,Montiel R,Lopez J,Figueras F.Effect of the support on the basic and catalytic properties of KF[J].J.catal.,2004,221:483-490
[29]Shailendra V,Bordawekar S.V.,Doskocil E.J.,Davis R.J.,Influence of support composition on the structure and reactivity of strontium base catalysts[J].Catal.Lett.,1997,44:193-199
[30]Ruckenstein E,Khan A Z.Effects of Superbasic Catalysts Prepared by Promoting MgO with Bialkali Metal Compounds on the Oxidative Coupling of Methane[J].J.Catal.,1993,141:628-647
[31]Shinzo K,Toshihilo S,Takafumi N.Polymerization of Propylene Oxide by Calcined Synthetic Hydrotalcite[J].Makromol.Chem,Rapid Commum,1981,2:231-233
[32]Matsuhashi H,Motoi H,Arata K.Determination of acid strength of solid superacids by temperature programmed desorption using pyridine[J].Catal.Lett.,1994,26(3-4):325-328
[33]Hama I,Sasamoto H,Okamoto T.Influence of Catalyst Structure on Direct Ethoxylation of Fatty Methyl Ester over Al-Mg Composite Oxide Catalyst[J].JAOCS,1997,74(7):817-822.
[34]Genin J-M R.,et.al.Thermodynamic equilibria in aqueous suspersions of synthesis and natural Fe(Ⅱ)-Fe(Ⅲ)green rusts:occurrences of the mineral in hydromorphic soils[J].Environ.Sci.Technol.,1998,32(8):1058-1068.
[35]Kooli F,Rives V,Ulibarri M A.Preparation and study of decavanadate-pillared hydrotalite -like anionic clays containing transition metal cations in the layers,2 Samples containing magnesium-chromium and nikel-chromium[J].Inorg.Chem.,1995,34:5122-5128
[36]Baltpurvins K A,Burns R C,Lawrance G A,Stuart A D.Effect of Ca~(2+),Mg~(2+),and anion type on the aging of iron hydroxide precipitates[J].Environ.Sci.Technol., 1997,31(4):1024-1032.
[37]L6pez-Salinas E,Garcia-Sanchez M,Llanos-Serrano M E,Navarrete-Bolanoz J.Formation of Base Sites on Calcined Mg-Ga Hydrotalcite-like [Mg_(1-x)Gax(OH)_2](CO_3)_(x/2)·mH_2O[J].J.Phys.Chem.B,1997,101:5112-5117
[38]Ogawa T.,Fire-resistant vinyl chloride resin compositions[P].JP 04/65,448,02 Mar 1992.
[39]Flame-retardent compositions[P],JP 62/22,839,31 Jan 1987
[40]Hydrotalcite-containing PVC films for agricultural uses[P],JP 63/118,374,23 May 1988
[41]辛勤.固体催化剂研究方法[M].北京:科学出版社,2004
[42]雷经新,石秋杰.固体碱催化剂在有机合成中的应用及进展[J].化工时刊,2005(19)2:49-53
[43]Jothi J T,Raja T,Streekumar K.Influence of acid-base properties of mixed oxides derived from hydrotalcite-like precursors in the transfer hydrogenation of propiophenone[J].J.Mol.Catal.,2000,157:193-201
[44]Yadav V K,Kapoor X K.Tetrabedron Lett,1994,35:94-81
[45]Yaday V K,Kapoor K K.Tetrahedron,1996,52:36-59
[46]Kakuno Y,Hattri H,Addition of amines to conjugated dienes catalyzed by solid base catalysts[J].J.Catal.,1984,85:509-518
[47]Imizu Y,Hattofi H,Tanabe K.Selective formation of trans-2-butene-1,4-d2 and (E)-2-methyl-2-butene-1,4-d2 in deuteration of 1,3-butadiene derivatives over thorium oxide catalyst[J].J.Catal.,1979,56:303-314
[48]Hattori H.Solid base catalysts:generation of basic sites and application to organic synthesis[J].Appl Catal A,2001,222:247-259
[49]Zahouily M,Salah M,Bahlaouane B.Solid catalysts for the production of fine chemicals:the use of natural phosphate alone and doped base catalysts for the synthesis of unsaturated arylsulfones[J].Tetrahedron,2004,60:1631-1635
[50]蒋绍亮,章福祥,关乃佳.固体碱催化剂在催化反应中的应用进展[J].石油化工,2006,35(1):1-10
[51]Bancquart S,Vanhove C,Pouilloux Y.Glycerol Transesterification with Methyl Stearate over Solid Basic Catalysts[J].Appl.Catal.A,2001,218:1-11
[52]Taylor H F W.,et.al.Crystal structures of some double hydroxide minerals[J].Mineral Mag.,1973,39:77-389.
[53]Giannelis E P,Nocera D J,Pinnavaia T J.Anionic photocatalysts supported in layered double hydroxides:intercalation and photophysical properties of a ruthenium complex anion in synthetic hydrotalcite[J].Inorg.Chem.,1987,26:203-205.
[54]Vaccari A.Preparation and catalytic properties of cationic and anionic clays[J].Catal.Today,1998,41:53-71.
[55]Vaccari A.Clays and catalysis:a promising future[J].Appl.Clay Sci.,1999,14:161-198.
[56]Pausch I H,Lohse H,Schurmann K,Allmann R.Syntheses of disordered and Al-rich hydrotalcite-like compounds[J].Clays Clay Miner.,1986,34:507-510.
[57]Brown G.Gastuche M C.Mixed magnetium-aluminium hydroxides[J].Clay Miner.,1967,7:193-201.
[58]Feitknecht W,et.al.Double hydroxides and basic double salts(Ⅲ)Mg-Al double hydroxides[J].Helv.Chim.Acta,1942,25:131-137.
[59]杜以波等.影响水滑石品体结构的因素[J].燃料化学学报,1997,5(25):449-453
[60]Roy De A,Besse J P.Evolution of protonic conduction in some synthetic anionic clays [J].Solid State Ionics,1991,46:95-101.
[61]Yamaoka T.,Abe,M.Tsuji M Mat Res Bull.1989,24:1183.
[62]谢鲜梅等.阴离子粘土的合成方法[J].太原理工大学学报,1997,2(28):58.
[63]Roy D M,Roy R,Osborn E F.The system MgO-Al_2O_3-H_2O and influence of carbonate and nitrate ions on the phase equilibria[J].Ameri.J.S ci.,1953,251:337-361
[64]Mascolo G,Marino O.A new synthesis and characterization of magnesium aluminium hydroxides[J].Mineral.Mag.,1980,43:619-621.
[65]谢晖,矫庆泽,段雪.镁铝型水滑石水热合成[J].应用化学,2001,18(1):70-72.
[66]杜以波,何静,李峰等.水滑石及柱撑水滑石的制备和表征[J].北京化工大学学报,1997,24(3):76-80.
[67]Malherbe F,Besse J P,Wade S R,Smith W J.Highly selective synthesis of 2-butoxy ethanol over Mg/Al/V mixed oxides catalysts derived from hydrotalcites[J].Catal.Lett,2000,67:197-202.
[68]Ogawa M,Kaiho H.Homogeneous Precipitation of Uniform Hydrotalcite Particles[J].Langmuir,2002,18:4240-4242.
[69]段雪,矫庆泽,李蕾.均分散超细阴离子层状材料的新合成方法[P].中国专利,CN99119385.1999-09-14.
[70]ZhaoY,Li F,Zhang R,Evans D G,Duan X.Preparation of Layered Double-Hydroxide Nanomaterials with a Uniform Crystallite Size Using a New Method Involving Separate Nucleation and Aging Steps[J].Chem.Mater.,2002,14:4286-4291.
[71]张慧,齐荣,刘丽娜,段雪.镁铁双羟基复合金属氧化物的可控合成及品面生长特征研究[J].化学物理学报.2003,16:45.
[72]杜以波,何静,李峰,D.G.Evans,段雪,王作新.微波技术在制备水滑石和柱撑水滑石中的应用[J].应用科学学报,1998,16(3):349-354.
[73]Rives V.Comment on "Direct observation of a metastable solid phase of Mg/Al/CO_3-layered double hydroxide by means of high-temperature in situ powder XRD and DTA/TG"[J].Inorg.Chem.,JAN,1999,38:406.
[74]Bera P,Rajamathi M,Hegde M S,Kamath P V.Thermal behavior of hydroxides,hydroxysalts and hydrotalcites[J].Bull.Mater.Sci.,(India)2000,23:141-145.
[75]Reichle WT,et al..The nature of the thermal decomposition of a catalytically active anionic clay minerals[J].J.Catal.,1986,101:352-359.
[76]Kanezak E i.Effect of Atomic Ratio Mg/Al in Layers of Mg and Al Layered Double Hydroxide on Thermal Stability of Hydrotalcite-Like Layered Structure BY Means of In Situ High Temperature Powder X-Ray Diffraction[J].Mater.Res.Bull.,1998,33(5):773-778.
[77]屠迈等.镍铁水滑石及其衍生混合氧化物的制备和表征[J].无机化学学报,1997,2(13):160-163.
[78]Kruissink E C,et al.Coprecipitated nickel-alumina catalyst for methanation at high temperature[J].J.Chem.Soc.Faraday Trans I.,1981,77:649-663.
[79]刘玉敏等.钴铜铝水滑石类化合物的合成及其催化氧化对甲酚:Ⅰ.水滑石的合成 及其表征[J].应用化学,1998,2(15):11-13.
[80]Hibino T,Tsunashima A.Calcination and rehydration behavior of Mg-Fe-CO_3hydrotalcite-like compounds[J].J.Mater.Sci.Lett,2000,19:1403-1405.
[81]张慧,齐荣,段雪.镁铁和镁铝双羟基复合金属氧化物的结构与性能差异[J].无机化学学报,2002,18:833-836.
[82]Rives V.,Kannan S.Layered double hydroxides with the hydrotalcite-type structure containing Cu~(2+),Ni~(2+)and Al~(3+)[J].J.Mater.Chem.,2000,10:489.
[83]Nijs H,del Bock M,Vansant E F.Comparative Study of the Synthesis and Properties of Polyoxometalate Pillared Layered Double Hydroxides(POM-LDHs)[J].J.Porous Mater.,1999,6:101-110.
[84]Labajos F M,Sastre M D,Trujillano R,Rives V.New layered double hydroxides with the hydrotalcite structure containing Ni(Ⅱ)and V(Ⅲ)[J].J.Mater.Chem.,1999,9:1033-1039.
[85]Di Cosimo J I,Diez V K,Xu M,Iglesia E,Apesteguia C R,Structure and Surface and Catalytic Properties of Mg-A1 Basic Oxides[J].J.Catal.,1998,178:499-510.
[86]Schaper H,Berg- slot J J,Storke W H.Stabilized magnesia:a novel catalyst(support)material[J].J.Appl.Catal.,1989,54:79-90.
[87]Mckenzie A L,et al.,Investigation of the surface structure and basic properties of calcined hydrotalcites[J].J.Catal.,1992,138:547-561.
[88]屠迈等,MgFeO氧化物催化剂酸碱性质的微量吸附量热研究[J].化学通报,1996,10:39-43.
[89]Shen J Y,et al.Synthesis and surface acid/base properties of Mg-Al mixed oxides obtained from hydrotalcites[J].Langmuir,1994,10:3902-3908.
[90]Casenave S,Martinez H,et al.Acid-base properties of Mg-Ni-Al mixed oxides using LDH as precursors[J].Thermochimica Acta,2001,379:85-93.
[91]Aramendia M A,Aviles Y,et al.Comparative study of Mg/Al and Mg/Ga layered double hydroxides[J],Micro.Meso.Mater.,1999,29:319-328.
[92]李大塘等.Mg-Al-O复合氧化物催化剂的表面酸碱性质(Ⅰ):强度与数量研究[J].湘潭师范学院学报,1999,20(3):10-12
[93]李大塘等.Mg-Al-O复合氧化物催化剂的表面酸碱性质(Ⅱ):酸碱种类研究[J].湘潭师范学院学报[J].1999,20(6):9-12.
[94]李大塘等.Mg-Al-O复合氧化物催化剂的表面酸碱性质(Ⅲ):体相结构研究[J].湘潭师范学院学报,2000,21(3):16-20.
[95]段雪,张法智等.插层组装与功能材料[M].北京:化学工业出版社,2007
[96]谢晖.层状结构阴离子型选择性红外吸收材料制备与性能研究[D].北京:北京化工大学近代化学研究所.2000
[97]Khan A I,Lei L,Norquist A J,O'Hare D.Intercalation and controlled release of pharmaceutically active compounds from a layered double hydroxide[J].Chem.Commun,2001,2342
[98]Zhu K,Liu C,Ye X,et al.Catalysis of hydrotalcibe-like compounds in liquid phase oxidation[1]:Phenol hydroxylation[J].Appl.Catal.A,1998,168:365-372
[99]Lebedeva O,Tichit D,Coq B.Influence of the compensating anions of Ni/Al and Ni/Mg/Al layered double hydroxides on their activation under oxidizing and reducing atmospheres[J].Appl.Catal.A:general,1999,183(I):61-71
[100]Coq B,Tichit D,Ribet S.Co/Ni/Mg/Al Layered Double Hydroxides as Precursors of Catalysts for the Hydrogenation of Nitriles:Hydrogenation of Acetonitrile[J].J.Catal.,2000,189(1):117-128
[101]李连生,马淑杰,惠健斌等.稀士水滑石催化合成邻苯二甲酸二戊酯的研究[J].高等学校化学学报,1995,16(8):1164-1167
[102]徐征,贺鹤鸣,蒋大振.低碳烃类在杂多酸柱水滑石上的烷基化[J].科技通报,1994,39,(15):1392-1395.
[103]Kaneda K,Yamaguchi K,et al.Catalyst design of hydrotalcite compounds for efficient oxidations[J].J.Catal.Surv Jpn,2000,4:31-38.
[104]Zoltan F,Zoltan H,et al.Mg-Al 3:1 hydrotalcite catalyst in the synthesis of cyclopropane carboxylic acid derivatives[J].J.Mole.Catal.A:Chemical,2000,161:149-155.
[105]Yamaguchi K,Ebitani K,Yoshida T,Yoshida T,Yoshida H,Kaneda K.Mg-Al Mixed Oxides as Highly Active Acid-Base Catalysts for Cycloaddition of Carbon Dioxide to Epoxides[J].J.Am.Chem.Soc.,1999,121:4526-4527
[106]Roelofs J C A A,Lensveld D J,Van Dillen A J,De Jong K P.On the Structure of Activated Hydrotalcites as Solid Base Catalysts for Liquid-Phase Aldol Condensation [J].J.Catal.,2001,203:184-191.
[107]Prinetto F,Tichit D,Teissier R,Coq B.Mg- and Ni-containing layered double hydroxides as soda substitutes in the aldol condensation of acetone[J].Catal.Today,2000,55:103-116.
[108]Tichit D,Bennani M N,Figueras F,Tessier R,Kervennal J.Aldol condensation of acetone over layered double hydroxides of the meixnerite type[J].Appl.Clay Sci.,1998,13:401-415.
[109]Ebitani K,Motokura K,Mori K,Mizugaki T,Kaneda K.Reconstructed Hydrotalcite as a Highly Active Heterogeneous Base Catalyst for Carbon-Carbon Bond Formations in the Presence of Water[J].J.Org.Chem.,2006,71(15):5440-5447
[110]Fernandez J M,Ulibarri M A,Labajos F M,Rives V.The effect of iron on the crystalline phases formed upon thermal decomposition of Mg-Al-Fe hydrotalcites[J].J.Mater.Chem.,1998,8:2507-2514
[111]Cantu M,L6pez-Salinas E,Valente J S.SOx Removal by Calcined MgAlFe Hydrotalcite-like Materials:Effect of the Chemical Composition and the Cerium Incorporation Method[J].Environ.Sci.Technol.,2005,39:9715-9720
[112]Cheng W P,Yu X Y,Wang W J,Liu L,Yang J G,He M Y.Synthesis,characterization and evaluation of Cu/MgAlFe as novel transfer catalyst for SOx removal[J].Catal.Comm.,2008,9:1505-1509
[113]陈银飞,葛忠华,吕德伟.MgAlFe复合氧化物氧化吸附SO_2的性质[J].环境科学学报,2001,21(3):307-311
[114]Kustrowski P,Rafalska-Lasocha A,Majda D,Tomaszewka D,Dziembaj R.Preparation and characterization of new Mg-Al-Fe oxide catalyst precursors for dehydrogenation of ethylbenzene in the presence of carbon dioxide[J].Solid State Ionics,2001,141-142:237-342
[115]Choudary B M,Kantam M L,Neeraja V,Rao K K,Figueras F,Delmottec L.Layered double hydroxide fluoride:a novel solid base catalyst for C-C bond formation[J].Green Chem.,2001.3:257-260
[116]段雪,矫庆泽,李蕾.均分散超细阴离子层状材料的新合成方法[P].中国专利,99119385.7,1999-9-14
[117]段雪,矫庆泽.全返混液膜反应器及其在制备超细阴离子层状材料中的应用[P].中国专利,00132145.5,2002-12-14
[118]Kazuya Y,Kohki E,Tomoko Y,Hisao Y,Kiyotomi K.MgoAl Mixed Oxides as Highly Active Acid-Base Catalysts for Cycloaddition of Carbon Dioxide to Epoxides[J].J.Am.Chem.Soc.1999,121:4526-4527
[119]Federica D,Giovanna G.Investigation of Acid-Base Properties of Catalysts Obtained from Layered Double Hydroxides[J].J.Phys.Chem.B,2000,104:11117-11426
[120]Abello S,Medina F,Tichit D,Perez-Ramirez J,Groen J C,Sueiras J E,Salagre P,Cesteros Y.Aldol Condensations Over Reconstructed Mg - Al Hydrotalcites:StructureActivity Relationships Related to the Rehydration Method[J].Chem.Eur.J.2005,11:728-739
[121]Hammond C.The Basics of Crystallography and Diffraction[M].Oxford University Press:Oxford,1997,p 145
[122]Yang W,Kim Y,Liu Paul K T,Sahimi M,Tsotsis T T.A study by in situ techniques of the thermal evolution of the structure of a Mg-Al-CO_3 layered double hydroxide[J].Chem.Eng.Sci.,2002,57:2945-2953.
[123]Radha A.V.,Thomas G.S.,Vishnu Kamath,P.,Shivakumara C.Suppression of Spinel Fornation to Induce Reversible Thermal Behavior in the Layered Double Hydroxides (LDHs)of Co with Al,Fe,Ga,and In[J].J.Phys.Chem B,2007,111:3384-3390
[124]Titulaer M K,Jansen J B H,Geus J W.The quantity of reduced nickel in synthetic takovite:effects of preparation conditions and calcination temperature[J].Clays Clay Miner.,1994,42:249-258.
[125]Dumitriu E,Hulea V,Chelaru C.Influence of the acid-base properties of solid catalysts derived from hydrotalcite-like compounds on the condensation of formaldehyde and acetaldehyde[J].Appl.Catal.A,1999,178:145-157.
[126]Rousselot I,Taviot-Gueho C,Besse J P.Synthesis and characterization of mixed Ga/Al-containing layered double hydroxides:study of their basic properties through the Knoevenagel condensation of benzaldehyde and ethyl cyanoacetate,and comparison to other LDHs[J].Int.J.Inorg.Mater.,1999,1:165-174
[127]J.A.迪安主编,尚久方等译.兰氏化学手册[M].北京:科学出版社,1991,115
[128]Lopez-Salinas E,Garcia-Sanchez M,Montoya J A,Acosta D R,Abasolo J A,Schifter I.Stuctural characterization of synthetic hydrotaleite-like[Mg_(1-x)Ga_x(OH)_2](CO_3)_(x/2)·2H_2O [J].Langmuir,1997,13(17):4748-4753
[129]Intissar M,Segnil R,Payen C,Besse J P,Lerouxn F.Trivalent cation substitution effect into layered double hydroxides Co_2Fe_yAl_(1-y)(OH)_6Cl·nH_2O:study of the local order ionic conductivity and magnetic properties[J].J.Solid State Chem.,2002,167:508-516
[130]Gregg S J,Sing K S W.Adsorption,Surface Area and Porosity[C].2nd ed.,Academic Press,New York,1982.
[131]Anillo A A,Villa-Carcia M A,Liavona R,Suarez M,Rodriguez J.Textural Properties of a-Titanium(IV)Phenylphosphonate:Influence of Preparation Conditions[J].Mater.Res.Bull.,1999,34(4):627-640.
[132] Rohrer C L, Rohrer G S. Monte Carlo simulations of Mg(Al)O solid solutions based on crystal chemical rules[J]. Chem. Mater., 1994,6:501-507
[133] Di Cosimo J I, Apestegui a C R, et al.. Structural Requirements and Reaction Pathways in CondensationReactions of Alcohols on MgyAlOx Catalysts [J]. J. Catal., 2000, 190:261-275
[134] Duke C V A, Miller J A, Clark J H, Kybett A P. F19 MAS NMR and FTIR analysis of the adsorption of alkali metal fluorides onto alumina [J]. J. Mol. Catal.l990,62:233-242
[135] Millange F, Walton R I, O_Hare D. Time-resolved in situ X-ray diffraction study of the liquid-phase reconstruction of Mg-Al carbonate hydrotalcite-like compounds [J].J.Mater. Chem. 2000, 10:1713-1720.
[136] Tundo P, Selva M. The Chemistry of Dimethyl Carbonate [J]. Acc. Chem. Res., 2002,35(9): 706-716.
[137] Pacheco M A, Marshall C L. Review of Dimethyl Carbonate (DMC) Manufacture and Its Characteristics as a Fuel Additive [J]. Energy Fuels, 1997, 11: 2—29.
[138] Joho F, Novak P. SNIFTIRS investigation of the oxidative decomposition of organic-carbonate-based electrolytes for lithium-ion cells [J]. Electrochimica Acta,2000,45:3589-3599
[139] Fukuoka S, Kawamura M, Komiya K, Tojo M, Hachiya H, Hasegawa K, Aminaka M,Okamoto H, Fukawa I, Konno S. A novel non-phosgene polycarbonate production process using by-product CO_2 as starting material, Green Chem.2003,5: 497—507
[140] Delledonne D, Rivetti F, Romano U. Developments in the production and application of dimethylcarbonate [J]. App. Catal. A: Gen. 2001, 221: 241—251
[141] Choi J-C, He L-N, Yasuda H, Sakakura T. Selective and high yield synthesis of dimethyl carbonate directly from carbon dioxide and methanol [J]. Green Chem.,2002,4:230-234
[142] Tomishige K, Ikeda Y, Sakaihori T, Fujimoto K. Catalytic Properties and Structure of Zirconia Catalysts for Direct Synthesis of Dimethyl Carbonate from Methanol and Carbon Dioxide [J]. J. Catal., 2000, 192: 355-362.
[143] Fujita S-i, Bhanage B M, Ikushima Y, Arai, M. Synthesis of dimethyl carbonate from carbon dioxide and methanol in the presence of methyl iodide and base catalysts under mild conditions: effect of reaction conditions and reaction mechanism [J]. Green Chem.,2001,3:87-91
[144] Bhanage B M, Fujita S-i, Ikushima Y, Arai M. Synthesis of dimethyl carbonate and glycols from carbon dioxide, epoxides, and methanol using heterogeneous basic metal oxide catalysts with high activity and selectivity [J]. Appl. Catal. A: Gen., 2001,219:259-266
[145] Chang Y, Han T J, Liu Z, Wu W, Gao L, Li J, Gao H, Zhao G, Huang J. One-pot synthesis of dimethyl carbonate and glycols from supercritical CO_2, ethylene oxide or propylene oxide, and methanol [J]. Appl. Catal. A: Gen. 2004, 263: 179—186.
[146] Li Y, Zhao X-q, Wang Y-j. Synthesis of dimethyl carbonate from methanol, propylene oxide and carbon dioxide over KOH/4A molecular sieve catalyst [J]. Appl. Catal. A:Gen., 2005, 279: 205-208.
[147] De J, Johannes P, Lange J-P [P]. US Patent 6,835,858, 2004
[148]Tatsumi T,Watanabe Y,Koyano K A.Synthesis of dimethyl carbonate from ethylene carbonate and methanol using TS-1 as solid base catalyst[J].Chem.Commun.,1996:2281-2282.
[149]Srivastava R,Srinivas D,Ratnasamy P.Synthesis of polycarbonate monomers by CO2insertion in epoxides over zeolite-based catalysts[J].Stud.Surf.Sci.Catal.,2004,154C:2703.
[150]Wei T,Wang M,Wei W,Sun Y,Zhong B.Synthesis of dimethyl carbonate by transesterification over CaO/carbon composites[J].Green Chem.,2003,5:343-346.
[151]Wei T,Wang M,Wei W,Sun Y,Zhong B,Morrell(Ed.)in:D.G.,Catalysis of Organic Reactions[M].Marcel Decker,New York,2003,p.659,chap.58.
[152]Watanabe Y,Tatsumi T.Hydrotalcite-type materials as catalysts for the synthesis of dimethyl carbonate from ethylene carbonate and methanol[J].Micro.Meso.Mater.,1998,22:399-407.
[153]Bhanage B M,Fujita S-i,He Y,Ikushima Y,Shirai M,Torii K,Arai M._Concurrent Synthesis of Dimethyl Carbonate and Ethylene Glycol via Transesterification of Ethylene Carbonate and Methanol Using Smectite Catalysts Containing Mg and/or Ni [J].Catal.Lett.,2002,83:137-141
[154]Srivastava R,Srinivas D,Ratnasamy P.Fe-Zn double-metal cyanide complexes as novel,solid transesterification catalysts[J].J.Catal.,2006,241:34-44.
[155]吕亮,吾国强等.水滑石的制备、表征及其在酯交换反应中的应用[J].精细石油化工,2001,(6):9-12
[156]吕亮,吾国强等.酯交换反应在皮革加脂剂合成中的应用[J].皮革化工,2000,16:19-22
[157]朱建华,淳远,王英,须沁华.强碱性沸石分子筛催化材料.科学通报,1999,44:897-902
[2]Brindlye G W,Kikkawa S.Thermal behavior of hydrotalcite and of anion-exchanged forms of hydrotalcite[J].Calys Caly Miner.,1980,28:87-91.
[3]Pines H,Stalick W M.Base-catalyzed Reactions of Hydrocarbons and Relatec Compounds[D].New York:Academic Press,1977
[4]Reichle W T.Catalytic reactions by thermally activated,synthetic,anionic clay minerals [J].J.Catal.,1985,94:547-557
[5]Cavani F,TrifirO F,Vaccari A.Hydrotalcite-type anionic clays:preparation,properties and applications[J].Catal.Today,1991,11(2):173-301
[6]田部浩三等.新固体酸和碱及其催化作用[M].北京:化学工业出版社,1992
[7]魏彤,王谋华,魏伟,孙予罕,钟炳.固体碱催化剂[J].化学通报,2002,9:594-600
[8]Pacheco M A,Marshall C L.Review of Dimethyl Carbonate(DMC)Manufacture and Its Characteristics as a Fuel Additive[J].Energy&Fuels,1997,11:2-29
[9]东北师范大学,华南师范大学等编.有机化学(下册)[M].北京:高等教育出版社,1992:88-89
[10]Lin X,Chuah G K,Jaenicka S.Base-functionalized MCM-41 as catalysts for the synthesis of monoglycerides[J].J.Mol.Catal.A:Chemical,1999,150:287-294
[11]朱洪法.催化剂载体制备及应用技术[MI.北京:石油工业出版社,2002
[12]Hattori H.Heterogeneous basic catalysis[J].Chem Rev,1995,95(3):537-558
[13]赵雷洪,郑小明,费金华.稀土氧化物固体碱催化剂的表面性质[J].催化学报,1996,17(3):227-231
[14]Zhang H,QI R,Duan X.,Evans D G.Synthesis and characterization of a novel nanoscale magnetic solid base catalyst involving a layered double hydroxide supported on a ferrite core[J].J.Solid State Chem.,2004,177:772-7801
[15]Climent M J,Corma A,Iborra S.Activated hydrotalcites as catalysts for the synthesis of chalcones of pharmaceutical interest[J].J.Catal.,2004,221(2):474-482
[16]Climent M J,Corma A,Iborra S.Base catalysis for fine chemicals production:Claisen-Schmidt condensationon zeolites and hydrotalcites for the production of chal-cones and flavanones of pharmaceutical interest[J].J.Catal.,1995,151(1):60-66
[17]Caldararu H,Caragheorgheopol A,Corma A.One eletron donor sites and their strength distribution on some hydrotalcite and MgO surfaces as studied by EPR spectroscopy[J].J.Chem.Soc.Faraday Trans.,1994,90,(1):213-218
[18]Corma A,Fornes V,Rey F.Hydrotalcites as base catalysts:influence of the chemical composition and synthesis conditions on the dehydrogenation of isopropanol[J].J.Catal.,1994,148(1):205-212
[19]Weitkamp J,Hunger M,Rymsa U.Base catalysis on microporous and mesoporous materials:recent progress and perspectives[J].Micro.Meso.Mater.,2001,48:255-270
[20]Vera R L.Constantino and Thomas J.Pinnavaia,Basic Properties of Mg~(2+)_(1-X)Al~(3+)_X Layered Double Hydroxides Intercalated by Carbonate Hydroxide,Chloride,and Sulfate Anions[J].Inorg.Chem.,1995,34:883-892.
[21]杨锡尧,任韶玲,何晖,王大庆.新型催化剂载体材料—镁铝复合氧化物的制备及 其物理化学性质[J].分子催化,1996,10(2):88-94.
[22]徐景士,王红明,吴志明.微波法制备的固体碱催化丁醛自缩合反应[J].精细化工,2002,19(11):644-646
[23]Weinstock L.M.,Stevenson J.M.,Tomellini S.A.,Pan S.,Utne T.,Jobson R.B.,Reinhold D.F.,Characterization of the actual catalytic agent in potassium fluoride on activated alumina systems[J].Tetrahedron Lett.,1986,27:3845-3848.
[24]Ando T,Clark J H,Cork D G,Hanafusa T,Ichihara J,Kimura T.Fluoride-alumina reagents:the active basic species[J].Tetrahedron Lett.,1987,28(13):1421-1424
[25]Kabashima H,Tsuji H,Nakata S,Tanaka Y,Hattori H.Activity for base-catalyzed reactions and characterization of alumina-supported KF catalysts[J].Appl.Catal.A,2000,227:194-195
[26]Handa H,Baba T,Sugisawa H,Ono Y.Highly efficient self-condensation of benzaldehyde to benzyl benzoate over KF-loaded alumina[J].J.Mol.Catal.A,1998,134:171-177.
[27]Ando T,Brown S J,Clark J H,Cork D G,Hanafusa T,Ichihara J,Miller J M,Robertson M.S.Alumina-supported fluoride reagents for organic synthesis:optimisation of reagent preparation and elucidation of the active species[J].J.Chem.Sot.,Perkin Trans.,1986,2:1133-1139.
[28]Clacens J,Genuit D,Delmotte L,Garcia-Ruiz A,Bergeret G,Montiel R,Lopez J,Figueras F.Effect of the support on the basic and catalytic properties of KF[J].J.catal.,2004,221:483-490
[29]Shailendra V,Bordawekar S.V.,Doskocil E.J.,Davis R.J.,Influence of support composition on the structure and reactivity of strontium base catalysts[J].Catal.Lett.,1997,44:193-199
[30]Ruckenstein E,Khan A Z.Effects of Superbasic Catalysts Prepared by Promoting MgO with Bialkali Metal Compounds on the Oxidative Coupling of Methane[J].J.Catal.,1993,141:628-647
[31]Shinzo K,Toshihilo S,Takafumi N.Polymerization of Propylene Oxide by Calcined Synthetic Hydrotalcite[J].Makromol.Chem,Rapid Commum,1981,2:231-233
[32]Matsuhashi H,Motoi H,Arata K.Determination of acid strength of solid superacids by temperature programmed desorption using pyridine[J].Catal.Lett.,1994,26(3-4):325-328
[33]Hama I,Sasamoto H,Okamoto T.Influence of Catalyst Structure on Direct Ethoxylation of Fatty Methyl Ester over Al-Mg Composite Oxide Catalyst[J].JAOCS,1997,74(7):817-822.
[34]Genin J-M R.,et.al.Thermodynamic equilibria in aqueous suspersions of synthesis and natural Fe(Ⅱ)-Fe(Ⅲ)green rusts:occurrences of the mineral in hydromorphic soils[J].Environ.Sci.Technol.,1998,32(8):1058-1068.
[35]Kooli F,Rives V,Ulibarri M A.Preparation and study of decavanadate-pillared hydrotalite -like anionic clays containing transition metal cations in the layers,2 Samples containing magnesium-chromium and nikel-chromium[J].Inorg.Chem.,1995,34:5122-5128
[36]Baltpurvins K A,Burns R C,Lawrance G A,Stuart A D.Effect of Ca~(2+),Mg~(2+),and anion type on the aging of iron hydroxide precipitates[J].Environ.Sci.Technol., 1997,31(4):1024-1032.
[37]L6pez-Salinas E,Garcia-Sanchez M,Llanos-Serrano M E,Navarrete-Bolanoz J.Formation of Base Sites on Calcined Mg-Ga Hydrotalcite-like [Mg_(1-x)Gax(OH)_2](CO_3)_(x/2)·mH_2O[J].J.Phys.Chem.B,1997,101:5112-5117
[38]Ogawa T.,Fire-resistant vinyl chloride resin compositions[P].JP 04/65,448,02 Mar 1992.
[39]Flame-retardent compositions[P],JP 62/22,839,31 Jan 1987
[40]Hydrotalcite-containing PVC films for agricultural uses[P],JP 63/118,374,23 May 1988
[41]辛勤.固体催化剂研究方法[M].北京:科学出版社,2004
[42]雷经新,石秋杰.固体碱催化剂在有机合成中的应用及进展[J].化工时刊,2005(19)2:49-53
[43]Jothi J T,Raja T,Streekumar K.Influence of acid-base properties of mixed oxides derived from hydrotalcite-like precursors in the transfer hydrogenation of propiophenone[J].J.Mol.Catal.,2000,157:193-201
[44]Yadav V K,Kapoor X K.Tetrabedron Lett,1994,35:94-81
[45]Yaday V K,Kapoor K K.Tetrahedron,1996,52:36-59
[46]Kakuno Y,Hattri H,Addition of amines to conjugated dienes catalyzed by solid base catalysts[J].J.Catal.,1984,85:509-518
[47]Imizu Y,Hattofi H,Tanabe K.Selective formation of trans-2-butene-1,4-d2 and (E)-2-methyl-2-butene-1,4-d2 in deuteration of 1,3-butadiene derivatives over thorium oxide catalyst[J].J.Catal.,1979,56:303-314
[48]Hattori H.Solid base catalysts:generation of basic sites and application to organic synthesis[J].Appl Catal A,2001,222:247-259
[49]Zahouily M,Salah M,Bahlaouane B.Solid catalysts for the production of fine chemicals:the use of natural phosphate alone and doped base catalysts for the synthesis of unsaturated arylsulfones[J].Tetrahedron,2004,60:1631-1635
[50]蒋绍亮,章福祥,关乃佳.固体碱催化剂在催化反应中的应用进展[J].石油化工,2006,35(1):1-10
[51]Bancquart S,Vanhove C,Pouilloux Y.Glycerol Transesterification with Methyl Stearate over Solid Basic Catalysts[J].Appl.Catal.A,2001,218:1-11
[52]Taylor H F W.,et.al.Crystal structures of some double hydroxide minerals[J].Mineral Mag.,1973,39:77-389.
[53]Giannelis E P,Nocera D J,Pinnavaia T J.Anionic photocatalysts supported in layered double hydroxides:intercalation and photophysical properties of a ruthenium complex anion in synthetic hydrotalcite[J].Inorg.Chem.,1987,26:203-205.
[54]Vaccari A.Preparation and catalytic properties of cationic and anionic clays[J].Catal.Today,1998,41:53-71.
[55]Vaccari A.Clays and catalysis:a promising future[J].Appl.Clay Sci.,1999,14:161-198.
[56]Pausch I H,Lohse H,Schurmann K,Allmann R.Syntheses of disordered and Al-rich hydrotalcite-like compounds[J].Clays Clay Miner.,1986,34:507-510.
[57]Brown G.Gastuche M C.Mixed magnetium-aluminium hydroxides[J].Clay Miner.,1967,7:193-201.
[58]Feitknecht W,et.al.Double hydroxides and basic double salts(Ⅲ)Mg-Al double hydroxides[J].Helv.Chim.Acta,1942,25:131-137.
[59]杜以波等.影响水滑石品体结构的因素[J].燃料化学学报,1997,5(25):449-453
[60]Roy De A,Besse J P.Evolution of protonic conduction in some synthetic anionic clays [J].Solid State Ionics,1991,46:95-101.
[61]Yamaoka T.,Abe,M.Tsuji M Mat Res Bull.1989,24:1183.
[62]谢鲜梅等.阴离子粘土的合成方法[J].太原理工大学学报,1997,2(28):58.
[63]Roy D M,Roy R,Osborn E F.The system MgO-Al_2O_3-H_2O and influence of carbonate and nitrate ions on the phase equilibria[J].Ameri.J.S ci.,1953,251:337-361
[64]Mascolo G,Marino O.A new synthesis and characterization of magnesium aluminium hydroxides[J].Mineral.Mag.,1980,43:619-621.
[65]谢晖,矫庆泽,段雪.镁铝型水滑石水热合成[J].应用化学,2001,18(1):70-72.
[66]杜以波,何静,李峰等.水滑石及柱撑水滑石的制备和表征[J].北京化工大学学报,1997,24(3):76-80.
[67]Malherbe F,Besse J P,Wade S R,Smith W J.Highly selective synthesis of 2-butoxy ethanol over Mg/Al/V mixed oxides catalysts derived from hydrotalcites[J].Catal.Lett,2000,67:197-202.
[68]Ogawa M,Kaiho H.Homogeneous Precipitation of Uniform Hydrotalcite Particles[J].Langmuir,2002,18:4240-4242.
[69]段雪,矫庆泽,李蕾.均分散超细阴离子层状材料的新合成方法[P].中国专利,CN99119385.1999-09-14.
[70]ZhaoY,Li F,Zhang R,Evans D G,Duan X.Preparation of Layered Double-Hydroxide Nanomaterials with a Uniform Crystallite Size Using a New Method Involving Separate Nucleation and Aging Steps[J].Chem.Mater.,2002,14:4286-4291.
[71]张慧,齐荣,刘丽娜,段雪.镁铁双羟基复合金属氧化物的可控合成及品面生长特征研究[J].化学物理学报.2003,16:45.
[72]杜以波,何静,李峰,D.G.Evans,段雪,王作新.微波技术在制备水滑石和柱撑水滑石中的应用[J].应用科学学报,1998,16(3):349-354.
[73]Rives V.Comment on "Direct observation of a metastable solid phase of Mg/Al/CO_3-layered double hydroxide by means of high-temperature in situ powder XRD and DTA/TG"[J].Inorg.Chem.,JAN,1999,38:406.
[74]Bera P,Rajamathi M,Hegde M S,Kamath P V.Thermal behavior of hydroxides,hydroxysalts and hydrotalcites[J].Bull.Mater.Sci.,(India)2000,23:141-145.
[75]Reichle WT,et al..The nature of the thermal decomposition of a catalytically active anionic clay minerals[J].J.Catal.,1986,101:352-359.
[76]Kanezak E i.Effect of Atomic Ratio Mg/Al in Layers of Mg and Al Layered Double Hydroxide on Thermal Stability of Hydrotalcite-Like Layered Structure BY Means of In Situ High Temperature Powder X-Ray Diffraction[J].Mater.Res.Bull.,1998,33(5):773-778.
[77]屠迈等.镍铁水滑石及其衍生混合氧化物的制备和表征[J].无机化学学报,1997,2(13):160-163.
[78]Kruissink E C,et al.Coprecipitated nickel-alumina catalyst for methanation at high temperature[J].J.Chem.Soc.Faraday Trans I.,1981,77:649-663.
[79]刘玉敏等.钴铜铝水滑石类化合物的合成及其催化氧化对甲酚:Ⅰ.水滑石的合成 及其表征[J].应用化学,1998,2(15):11-13.
[80]Hibino T,Tsunashima A.Calcination and rehydration behavior of Mg-Fe-CO_3hydrotalcite-like compounds[J].J.Mater.Sci.Lett,2000,19:1403-1405.
[81]张慧,齐荣,段雪.镁铁和镁铝双羟基复合金属氧化物的结构与性能差异[J].无机化学学报,2002,18:833-836.
[82]Rives V.,Kannan S.Layered double hydroxides with the hydrotalcite-type structure containing Cu~(2+),Ni~(2+)and Al~(3+)[J].J.Mater.Chem.,2000,10:489.
[83]Nijs H,del Bock M,Vansant E F.Comparative Study of the Synthesis and Properties of Polyoxometalate Pillared Layered Double Hydroxides(POM-LDHs)[J].J.Porous Mater.,1999,6:101-110.
[84]Labajos F M,Sastre M D,Trujillano R,Rives V.New layered double hydroxides with the hydrotalcite structure containing Ni(Ⅱ)and V(Ⅲ)[J].J.Mater.Chem.,1999,9:1033-1039.
[85]Di Cosimo J I,Diez V K,Xu M,Iglesia E,Apesteguia C R,Structure and Surface and Catalytic Properties of Mg-A1 Basic Oxides[J].J.Catal.,1998,178:499-510.
[86]Schaper H,Berg- slot J J,Storke W H.Stabilized magnesia:a novel catalyst(support)material[J].J.Appl.Catal.,1989,54:79-90.
[87]Mckenzie A L,et al.,Investigation of the surface structure and basic properties of calcined hydrotalcites[J].J.Catal.,1992,138:547-561.
[88]屠迈等,MgFeO氧化物催化剂酸碱性质的微量吸附量热研究[J].化学通报,1996,10:39-43.
[89]Shen J Y,et al.Synthesis and surface acid/base properties of Mg-Al mixed oxides obtained from hydrotalcites[J].Langmuir,1994,10:3902-3908.
[90]Casenave S,Martinez H,et al.Acid-base properties of Mg-Ni-Al mixed oxides using LDH as precursors[J].Thermochimica Acta,2001,379:85-93.
[91]Aramendia M A,Aviles Y,et al.Comparative study of Mg/Al and Mg/Ga layered double hydroxides[J],Micro.Meso.Mater.,1999,29:319-328.
[92]李大塘等.Mg-Al-O复合氧化物催化剂的表面酸碱性质(Ⅰ):强度与数量研究[J].湘潭师范学院学报,1999,20(3):10-12
[93]李大塘等.Mg-Al-O复合氧化物催化剂的表面酸碱性质(Ⅱ):酸碱种类研究[J].湘潭师范学院学报[J].1999,20(6):9-12.
[94]李大塘等.Mg-Al-O复合氧化物催化剂的表面酸碱性质(Ⅲ):体相结构研究[J].湘潭师范学院学报,2000,21(3):16-20.
[95]段雪,张法智等.插层组装与功能材料[M].北京:化学工业出版社,2007
[96]谢晖.层状结构阴离子型选择性红外吸收材料制备与性能研究[D].北京:北京化工大学近代化学研究所.2000
[97]Khan A I,Lei L,Norquist A J,O'Hare D.Intercalation and controlled release of pharmaceutically active compounds from a layered double hydroxide[J].Chem.Commun,2001,2342
[98]Zhu K,Liu C,Ye X,et al.Catalysis of hydrotalcibe-like compounds in liquid phase oxidation[1]:Phenol hydroxylation[J].Appl.Catal.A,1998,168:365-372
[99]Lebedeva O,Tichit D,Coq B.Influence of the compensating anions of Ni/Al and Ni/Mg/Al layered double hydroxides on their activation under oxidizing and reducing atmospheres[J].Appl.Catal.A:general,1999,183(I):61-71
[100]Coq B,Tichit D,Ribet S.Co/Ni/Mg/Al Layered Double Hydroxides as Precursors of Catalysts for the Hydrogenation of Nitriles:Hydrogenation of Acetonitrile[J].J.Catal.,2000,189(1):117-128
[101]李连生,马淑杰,惠健斌等.稀士水滑石催化合成邻苯二甲酸二戊酯的研究[J].高等学校化学学报,1995,16(8):1164-1167
[102]徐征,贺鹤鸣,蒋大振.低碳烃类在杂多酸柱水滑石上的烷基化[J].科技通报,1994,39,(15):1392-1395.
[103]Kaneda K,Yamaguchi K,et al.Catalyst design of hydrotalcite compounds for efficient oxidations[J].J.Catal.Surv Jpn,2000,4:31-38.
[104]Zoltan F,Zoltan H,et al.Mg-Al 3:1 hydrotalcite catalyst in the synthesis of cyclopropane carboxylic acid derivatives[J].J.Mole.Catal.A:Chemical,2000,161:149-155.
[105]Yamaguchi K,Ebitani K,Yoshida T,Yoshida T,Yoshida H,Kaneda K.Mg-Al Mixed Oxides as Highly Active Acid-Base Catalysts for Cycloaddition of Carbon Dioxide to Epoxides[J].J.Am.Chem.Soc.,1999,121:4526-4527
[106]Roelofs J C A A,Lensveld D J,Van Dillen A J,De Jong K P.On the Structure of Activated Hydrotalcites as Solid Base Catalysts for Liquid-Phase Aldol Condensation [J].J.Catal.,2001,203:184-191.
[107]Prinetto F,Tichit D,Teissier R,Coq B.Mg- and Ni-containing layered double hydroxides as soda substitutes in the aldol condensation of acetone[J].Catal.Today,2000,55:103-116.
[108]Tichit D,Bennani M N,Figueras F,Tessier R,Kervennal J.Aldol condensation of acetone over layered double hydroxides of the meixnerite type[J].Appl.Clay Sci.,1998,13:401-415.
[109]Ebitani K,Motokura K,Mori K,Mizugaki T,Kaneda K.Reconstructed Hydrotalcite as a Highly Active Heterogeneous Base Catalyst for Carbon-Carbon Bond Formations in the Presence of Water[J].J.Org.Chem.,2006,71(15):5440-5447
[110]Fernandez J M,Ulibarri M A,Labajos F M,Rives V.The effect of iron on the crystalline phases formed upon thermal decomposition of Mg-Al-Fe hydrotalcites[J].J.Mater.Chem.,1998,8:2507-2514
[111]Cantu M,L6pez-Salinas E,Valente J S.SOx Removal by Calcined MgAlFe Hydrotalcite-like Materials:Effect of the Chemical Composition and the Cerium Incorporation Method[J].Environ.Sci.Technol.,2005,39:9715-9720
[112]Cheng W P,Yu X Y,Wang W J,Liu L,Yang J G,He M Y.Synthesis,characterization and evaluation of Cu/MgAlFe as novel transfer catalyst for SOx removal[J].Catal.Comm.,2008,9:1505-1509
[113]陈银飞,葛忠华,吕德伟.MgAlFe复合氧化物氧化吸附SO_2的性质[J].环境科学学报,2001,21(3):307-311
[114]Kustrowski P,Rafalska-Lasocha A,Majda D,Tomaszewka D,Dziembaj R.Preparation and characterization of new Mg-Al-Fe oxide catalyst precursors for dehydrogenation of ethylbenzene in the presence of carbon dioxide[J].Solid State Ionics,2001,141-142:237-342
[115]Choudary B M,Kantam M L,Neeraja V,Rao K K,Figueras F,Delmottec L.Layered double hydroxide fluoride:a novel solid base catalyst for C-C bond formation[J].Green Chem.,2001.3:257-260
[116]段雪,矫庆泽,李蕾.均分散超细阴离子层状材料的新合成方法[P].中国专利,99119385.7,1999-9-14
[117]段雪,矫庆泽.全返混液膜反应器及其在制备超细阴离子层状材料中的应用[P].中国专利,00132145.5,2002-12-14
[118]Kazuya Y,Kohki E,Tomoko Y,Hisao Y,Kiyotomi K.MgoAl Mixed Oxides as Highly Active Acid-Base Catalysts for Cycloaddition of Carbon Dioxide to Epoxides[J].J.Am.Chem.Soc.1999,121:4526-4527
[119]Federica D,Giovanna G.Investigation of Acid-Base Properties of Catalysts Obtained from Layered Double Hydroxides[J].J.Phys.Chem.B,2000,104:11117-11426
[120]Abello S,Medina F,Tichit D,Perez-Ramirez J,Groen J C,Sueiras J E,Salagre P,Cesteros Y.Aldol Condensations Over Reconstructed Mg - Al Hydrotalcites:StructureActivity Relationships Related to the Rehydration Method[J].Chem.Eur.J.2005,11:728-739
[121]Hammond C.The Basics of Crystallography and Diffraction[M].Oxford University Press:Oxford,1997,p 145
[122]Yang W,Kim Y,Liu Paul K T,Sahimi M,Tsotsis T T.A study by in situ techniques of the thermal evolution of the structure of a Mg-Al-CO_3 layered double hydroxide[J].Chem.Eng.Sci.,2002,57:2945-2953.
[123]Radha A.V.,Thomas G.S.,Vishnu Kamath,P.,Shivakumara C.Suppression of Spinel Fornation to Induce Reversible Thermal Behavior in the Layered Double Hydroxides (LDHs)of Co with Al,Fe,Ga,and In[J].J.Phys.Chem B,2007,111:3384-3390
[124]Titulaer M K,Jansen J B H,Geus J W.The quantity of reduced nickel in synthetic takovite:effects of preparation conditions and calcination temperature[J].Clays Clay Miner.,1994,42:249-258.
[125]Dumitriu E,Hulea V,Chelaru C.Influence of the acid-base properties of solid catalysts derived from hydrotalcite-like compounds on the condensation of formaldehyde and acetaldehyde[J].Appl.Catal.A,1999,178:145-157.
[126]Rousselot I,Taviot-Gueho C,Besse J P.Synthesis and characterization of mixed Ga/Al-containing layered double hydroxides:study of their basic properties through the Knoevenagel condensation of benzaldehyde and ethyl cyanoacetate,and comparison to other LDHs[J].Int.J.Inorg.Mater.,1999,1:165-174
[127]J.A.迪安主编,尚久方等译.兰氏化学手册[M].北京:科学出版社,1991,115
[128]Lopez-Salinas E,Garcia-Sanchez M,Montoya J A,Acosta D R,Abasolo J A,Schifter I.Stuctural characterization of synthetic hydrotaleite-like[Mg_(1-x)Ga_x(OH)_2](CO_3)_(x/2)·2H_2O [J].Langmuir,1997,13(17):4748-4753
[129]Intissar M,Segnil R,Payen C,Besse J P,Lerouxn F.Trivalent cation substitution effect into layered double hydroxides Co_2Fe_yAl_(1-y)(OH)_6Cl·nH_2O:study of the local order ionic conductivity and magnetic properties[J].J.Solid State Chem.,2002,167:508-516
[130]Gregg S J,Sing K S W.Adsorption,Surface Area and Porosity[C].2nd ed.,Academic Press,New York,1982.
[131]Anillo A A,Villa-Carcia M A,Liavona R,Suarez M,Rodriguez J.Textural Properties of a-Titanium(IV)Phenylphosphonate:Influence of Preparation Conditions[J].Mater.Res.Bull.,1999,34(4):627-640.
[132] Rohrer C L, Rohrer G S. Monte Carlo simulations of Mg(Al)O solid solutions based on crystal chemical rules[J]. Chem. Mater., 1994,6:501-507
[133] Di Cosimo J I, Apestegui a C R, et al.. Structural Requirements and Reaction Pathways in CondensationReactions of Alcohols on MgyAlOx Catalysts [J]. J. Catal., 2000, 190:261-275
[134] Duke C V A, Miller J A, Clark J H, Kybett A P. F19 MAS NMR and FTIR analysis of the adsorption of alkali metal fluorides onto alumina [J]. J. Mol. Catal.l990,62:233-242
[135] Millange F, Walton R I, O_Hare D. Time-resolved in situ X-ray diffraction study of the liquid-phase reconstruction of Mg-Al carbonate hydrotalcite-like compounds [J].J.Mater. Chem. 2000, 10:1713-1720.
[136] Tundo P, Selva M. The Chemistry of Dimethyl Carbonate [J]. Acc. Chem. Res., 2002,35(9): 706-716.
[137] Pacheco M A, Marshall C L. Review of Dimethyl Carbonate (DMC) Manufacture and Its Characteristics as a Fuel Additive [J]. Energy Fuels, 1997, 11: 2—29.
[138] Joho F, Novak P. SNIFTIRS investigation of the oxidative decomposition of organic-carbonate-based electrolytes for lithium-ion cells [J]. Electrochimica Acta,2000,45:3589-3599
[139] Fukuoka S, Kawamura M, Komiya K, Tojo M, Hachiya H, Hasegawa K, Aminaka M,Okamoto H, Fukawa I, Konno S. A novel non-phosgene polycarbonate production process using by-product CO_2 as starting material, Green Chem.2003,5: 497—507
[140] Delledonne D, Rivetti F, Romano U. Developments in the production and application of dimethylcarbonate [J]. App. Catal. A: Gen. 2001, 221: 241—251
[141] Choi J-C, He L-N, Yasuda H, Sakakura T. Selective and high yield synthesis of dimethyl carbonate directly from carbon dioxide and methanol [J]. Green Chem.,2002,4:230-234
[142] Tomishige K, Ikeda Y, Sakaihori T, Fujimoto K. Catalytic Properties and Structure of Zirconia Catalysts for Direct Synthesis of Dimethyl Carbonate from Methanol and Carbon Dioxide [J]. J. Catal., 2000, 192: 355-362.
[143] Fujita S-i, Bhanage B M, Ikushima Y, Arai, M. Synthesis of dimethyl carbonate from carbon dioxide and methanol in the presence of methyl iodide and base catalysts under mild conditions: effect of reaction conditions and reaction mechanism [J]. Green Chem.,2001,3:87-91
[144] Bhanage B M, Fujita S-i, Ikushima Y, Arai M. Synthesis of dimethyl carbonate and glycols from carbon dioxide, epoxides, and methanol using heterogeneous basic metal oxide catalysts with high activity and selectivity [J]. Appl. Catal. A: Gen., 2001,219:259-266
[145] Chang Y, Han T J, Liu Z, Wu W, Gao L, Li J, Gao H, Zhao G, Huang J. One-pot synthesis of dimethyl carbonate and glycols from supercritical CO_2, ethylene oxide or propylene oxide, and methanol [J]. Appl. Catal. A: Gen. 2004, 263: 179—186.
[146] Li Y, Zhao X-q, Wang Y-j. Synthesis of dimethyl carbonate from methanol, propylene oxide and carbon dioxide over KOH/4A molecular sieve catalyst [J]. Appl. Catal. A:Gen., 2005, 279: 205-208.
[147] De J, Johannes P, Lange J-P [P]. US Patent 6,835,858, 2004
[148]Tatsumi T,Watanabe Y,Koyano K A.Synthesis of dimethyl carbonate from ethylene carbonate and methanol using TS-1 as solid base catalyst[J].Chem.Commun.,1996:2281-2282.
[149]Srivastava R,Srinivas D,Ratnasamy P.Synthesis of polycarbonate monomers by CO2insertion in epoxides over zeolite-based catalysts[J].Stud.Surf.Sci.Catal.,2004,154C:2703.
[150]Wei T,Wang M,Wei W,Sun Y,Zhong B.Synthesis of dimethyl carbonate by transesterification over CaO/carbon composites[J].Green Chem.,2003,5:343-346.
[151]Wei T,Wang M,Wei W,Sun Y,Zhong B,Morrell(Ed.)in:D.G.,Catalysis of Organic Reactions[M].Marcel Decker,New York,2003,p.659,chap.58.
[152]Watanabe Y,Tatsumi T.Hydrotalcite-type materials as catalysts for the synthesis of dimethyl carbonate from ethylene carbonate and methanol[J].Micro.Meso.Mater.,1998,22:399-407.
[153]Bhanage B M,Fujita S-i,He Y,Ikushima Y,Shirai M,Torii K,Arai M._Concurrent Synthesis of Dimethyl Carbonate and Ethylene Glycol via Transesterification of Ethylene Carbonate and Methanol Using Smectite Catalysts Containing Mg and/or Ni [J].Catal.Lett.,2002,83:137-141
[154]Srivastava R,Srinivas D,Ratnasamy P.Fe-Zn double-metal cyanide complexes as novel,solid transesterification catalysts[J].J.Catal.,2006,241:34-44.
[155]吕亮,吾国强等.水滑石的制备、表征及其在酯交换反应中的应用[J].精细石油化工,2001,(6):9-12
[156]吕亮,吾国强等.酯交换反应在皮革加脂剂合成中的应用[J].皮革化工,2000,16:19-22
[157]朱建华,淳远,王英,须沁华.强碱性沸石分子筛催化材料.科学通报,1999,44:897-902