采用水热法合成了一种新的3-氨基吡啶砷钼多金属氧酸盐配合物(C5H7N2)3(AsMo12O40)·3C5H6N2·2H2O.通过单晶X射线衍射、红外光谱、紫外光谱和差热-热重对其进行了表征.用催化消除丙酮的反应为模式反应,测试了配合物的催化性能.研究结果表明,标题配合物是由Keggin结构[AsMo12O40]3-杂多阴离子、[C5H7N2]+阳离子、[C5H6N2]分子和结晶水分子组成.配合物属于单斜晶系,P21/n空间群;晶胞参数a＝1.33820(12)nm,b＝2.2542(2)nm,c＝1.9848(2)nm,β＝100.27(3)°,V＝5.8912(10)nm3,Z＝4,Rgt(F)＝0.0590,wRref(F2)＝0.1882.配合物对催化消除丙酮具有较好的的活性,催化实验结果表明,160℃下,0.20 g的催化剂可将初始浓度均为1.3 g/m3,流速为4.5 mL/min的丙酮完全消除.
参考文献
| [1] | Clemente-Juan J M,Coronado E,Forment-Aliaga A,et al.A New Heptanuclear Cobalt(Ⅱ)Cluster Encapsulated in a Novel Heteropolyoxometalate Topology:Synthesis,Structure,and Magnetic Properties of[Co7(H2O)2(OH)2 P2W25O94]16-[J].Inorg Chem,2004,43:2689-2694. |
| [2] | Mal S S,Kortz U.The Wheel-Shaped Cu20 Tungstophosphate[Cu20C1(OH)24(H2O)12(P8W48Ot84)l25-Ion[J].Angew Chem Ira Ed,2005,44:3777-3780. |
| [3] | Zhao J W,Jia H P,Zhang J,et al.A Combination of Laeunary Polyoxometalatesand High-Nuclear Transition-Metal Clusters under Hydrothermal Conditions.Part Ⅱ:From Double Cluster,Dimer,and Tetramer to Three-Dimensional Frameworks[J].Chem Eur J,2007,13:10030-10045. |
| [4] | GUO Dongiie,DANG Dongbin,BO Yan,et al.Preparation of Polyoxmetalate Nanopartcles with Keggin Structure by Solidstate at Room Temperature[J].Chem Res,2002,13(1):11-14(in Chinese).郭东杰,党东宾,柏燕,等.Keggin结构钼硅酸铵、钨硅酸铵纳米颗粒的室温固相合成、结构及性能研究[J].化学研究,2002,13(1):11-14. |
| [5] | Luan G Y,Li Y G,Wang S T,et al.A new-geggln Type Polyoxometalate Coordinated to Four Silver Complex Moieties:{PW9V3O40[Ag(2,2-bipy)]2[Ag2(2,2-bipy)3]2}[J].J Chem Soc Dalton Tram,2003:233-235. |
| [6] | Hu C W,Hashimto M,Okuhara T,et al.Catalysis by Heteropoly compounds XXII.Reactions of Esters and Esterification Catalyzed by Heteroplyacids in a Homogeneous Liquid Phase-Effects of the Central Atom of Heteropolyanions Having Tungsten as the Addenda Atom[J].J Catal,1993,143:437-448. |
| [7] | Attansio D,Bonamico M,Fares V,et al.Weak Charge-transfer Polyoxoanion Salts:The Reaction of Quinolin-8-ol(Hquin)with Phosphotungstic Acid and the Crystal and Molecular Structure of[H2quin]3[PW12O40]·4EtOH·2H2O[J].J Chem Soc Dalton Trans,1990:3221-3228. |
| [8] | Hai X,Liu F F,Wang JJ.The Synthesis and Crystal Structure of(Hpy)3[PMo12O40]·2(py)[J].J Chem Crystallogr,2010,40:306-309. |
| [9] | Akutagawa T,Endo D,Imai H,et al.Forination of p-Phenylenediamine-Crown Ether-[PMo12O40]4-Salts[J].Inorg Chem,2006,45(21):8628-8637. |
| [10] | States Environmental Protection Agency.Chemical'S Toxicity,Law and Environmental Data Manual[M].Beijing:China Environmental Science Press,1992(in Chinese).国家环境保护局.化学品毒性、法规、环境数据手册[M].北京:中国环境科学出版社,1992. |
| [11] | Sheldriek G M,SHELXS-97 and SHELXL-97,Program for the Solution of Crystal Structures,Cottingen(Germany):University of Gottingen,1997. |
| [12] | Sheldrick G M.SHELXS-97 and SHELXL-97,Program for the Refinement of Crystal Structures,Gottingen(Germany):University of C,fittingen,1997. |
| [13] | Deheheff C R,Fournier M,Franck R,et al.Vibrational Investigations of Polyoxometalates.2.Evidence for Anion-Anion Interactions in Molybdenum(Ⅳ)and Tungsten(Ⅳ)Compounds Related to the Keggin Structu[J].Inorg Chem,1983,22:207-216. |
| [14] | WANG Enbo,HU C.hangwen,XU Lin.Introduction of Heteropoly Acid Chemistry[M].Beijing:Chemical Industry Press,1984:16(in Chinese).王恩波,胡长文,许林.多酸化学导论[M].北京:化学工业出版社,1984:16. |
| [15] | Ueda T,Wada K,Hojo M.Voltammetric and Raman Spectroscopic Study on the Formation of Keggin-type V(V)-Substituted Molybdoarsenate Complexes in Aqueous and Aqueous-organic Soluti[J].Polyhedron,2001,20:83-89. |
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