有机-无机杂化的钼砷酸盐的水热合成和性质（英文）
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摘要
通过水热法合成了由As-Mo-O簇和Cu~I有机单元构筑而成的钼砷酸盐{[Cu~I(2, 2′-bipy)_2]_3[As(OH)Mo_4O_(14)(OH)]·2H_2O}_(2 )(1)(bipy=bipyridine),并用元素分析、红外光谱和X射线单晶衍射对其进行了定性.1属于单斜晶系,P2(1)/c空间群.1中的多阴离子[As(OH)Mo_4O_(14)(OH)]~(3-)是有四个交替的共面的和共边的{MoO_6}八面体组成,在这些八面体上有一个{AsO_2(OH)}单元.
An organic-inorganic molybdenum arsenate constructed from the As-Mo-O cluster and Cu~I-organic units, namely, {[Cu~I(2, 2′-bipy)_2]_3[As(OH)Mo_4O_(14)(OH)]·2 H_2O}_(2 )(1)(bipy = bipyridine), were hydrothermally synthesized and characterized by IR spectroscopy, elemental analysis and single-crystal X-ray diffraction. 1 crystallizes in the monoclinic space group P2(1)/c.The polyanion [As(OH)Mo_4O_(14)(OH)]~(3-)of 1 is built from four alternately face-and edge-shared {MoO_6} octahedra capped by an {AsO_2(OH)} subunit.
An organic-inorganic molybdenum arsenate constructed from the As-Mo-O cluster and Cu~I-organic units, namely, {[Cu~I(2, 2′-bipy)_2]_3[As(OH)Mo_4O_(14)(OH)]·2 H_2O}_(2 )(1)(bipy = bipyridine), were hydrothermally synthesized and characterized by IR spectroscopy, elemental analysis and single-crystal X-ray diffraction. 1 crystallizes in the monoclinic space group P2(1)/c.The polyanion [As(OH)Mo_4O_(14)(OH)]~(3-)of 1 is built from four alternately face-and edge-shared {MoO_6} octahedra capped by an {AsO_2(OH)} subunit.
引文
[1] HABER J.The role of molybdenum in catalysis;climax molybdenum [M]:London,1981.
[2] CHEN C C,WANG Q,LEI P X,et al.Photodegradation of dye pollutants catalyzed by porous K3PW12O40 under visible irradiation [J].Environmental Science & Technology,2006,40(12):3965-3970.
[3] KOZHEVNIKOV I V.Catalysis by heteropoly acids and multicomponent polyoxometalates in liquid-phase reactions [J].Chemical Reviews,1998,98(1):171-198.
[4] DIMITRIS E K.A survey of applications of polyoxometalates[J].Chemical Reviews,1998,98(1):359-388.
[5] YAMASE T.Photo-and electrochromism of polyoxometalates and related materials [J].Chemical Reviews,1998,98(1):307-326.
[6] HAUSHALTER R C,STROHMAIER K G,LAI F W.Structure of a three-dimensional,microporous molybdenum phosphate with large cavities [J].Science,1989,246(4935):1289-1291.
[7] MATSUURA I,KIMURA N.In new developments in selective oxidation II;Corberán Cortés V,Vic Bellón S,Eds.;Elsevier:Amsterdam,1994,82:271-279.
[8] DATURI M,BUSCA G,GUESDON A,et al.Vibrational spectra study of Mo(V) phosphates as examples of different geometries of dimolybdenyl species [J].Journal of Materials Chemistry,2001,11(6):1726-1731.
[9] HE Q L,WANG E B.Hydrothermal synthesis and crystal structure of a new molybdenum(VI) arsenate(III),CoIII(en)3H3O[(CoIIO6)Mo■O18(As■O3)2]·2H2O [J].Inorganica Chimica Acta,1999,295(2):244-247.
[10] WIGGIN S B,WELLER M T.A chiral,16-ring channel framework and a layered caesium zincoarsenate [J].Chemical Communications,2006(10):1100-1102.
[11] LI L L,SHEN Q,XUE G L,et al.Two sandwich arsenomolybdates based on the new building block As(iii)Mo7O279-:[Cr2(AsMo7O27)2]12- and [Cu2(AsMo7O27)2]14- [J].Journal of Chemistry Society,Dalton Transactions,2008(42):5698-5700.
[12] SUN C Y,LI Y G,WANG E B,et al.A series of new organic-inorganic molybdenum arsenate complexes based on [(ZnO6)(As3O3)2Mo6O18]4- and [HxAs2Mo6O26](6-x)- clusters as SBUs [J].Inorganic Chemistry,2007,46:1563-1574.
[13] XU H S,LI L L,LIU B,et al.AsMo7O27- bridged dinuclear sandwich-type heteropolymolybdates of Cr(III) and Fe(III):magnetism of [MM′(AsMo7O27)2]12- with MM′ = FeFe,CrFe,and CrCr [J].Inorganic Chemistry,2009,48:10275-10280.
[14] BURKHOLDER E,WRIGHT S,GOLUB V,et al.Solid state coordination chemistry of oxomolybdenum organoarsonate materials [J].Inorganic Chemistry,2003,42(23):7460-7471.
[15] BURKHOLDER E,ZUBIETA J.Hydrothermal synthesis and structural characterization of a network oxide constructed from {Mo12O34(O3AsC6H5)4}4- clusters and {Cu(terpy)}2+ subunits [J].Inorganica Chimica Acta,2004,357(1):301-304.
[16] MüLLER A,PETERS F,POPE M T,et al.Polyoxometalates:very large clusters nanoscale magnets [J].Chemical Reviews,1998,98(1):239-272.
[17] SHELDRICK G M.SHELXS-97,Program for X-ray Crystal Structure Solution [CP].Germany:University of G?ttingen,1997.
[18] LAUDISE R A.Hydrothermal synthesis of crystals [J].Chemical & Engineering News,1987,65(39):30-43.
[19] HAGRMAN D,HAGRMAN P J,ZUBIETA J.The structural role of metal-organonitrogen subunits in the molecular manipulation of molybdenum oxides [J].Comments on Inorganic Chemistry,1999,21(4/6):225-261.
[20] HSU K F,WANG S L.Cs5Mo8O24(OH)2AsO4· 2H2O and Cs7Mo8O26AsO4:Two novel molybdenum(VI) arsenates containing heteropolyanions [AsMo8O30H2]5- and [AsMo8O30]7- [J].Inorganic Chemistry,1997,36(14):3049-3054.
[21] BRESE N E,O'KEEFFE M.Bond-valence parameters for solids [J].Acta Crystallographica,1991,B47:192-197.
[2] CHEN C C,WANG Q,LEI P X,et al.Photodegradation of dye pollutants catalyzed by porous K3PW12O40 under visible irradiation [J].Environmental Science & Technology,2006,40(12):3965-3970.
[3] KOZHEVNIKOV I V.Catalysis by heteropoly acids and multicomponent polyoxometalates in liquid-phase reactions [J].Chemical Reviews,1998,98(1):171-198.
[4] DIMITRIS E K.A survey of applications of polyoxometalates[J].Chemical Reviews,1998,98(1):359-388.
[5] YAMASE T.Photo-and electrochromism of polyoxometalates and related materials [J].Chemical Reviews,1998,98(1):307-326.
[6] HAUSHALTER R C,STROHMAIER K G,LAI F W.Structure of a three-dimensional,microporous molybdenum phosphate with large cavities [J].Science,1989,246(4935):1289-1291.
[7] MATSUURA I,KIMURA N.In new developments in selective oxidation II;Corberán Cortés V,Vic Bellón S,Eds.;Elsevier:Amsterdam,1994,82:271-279.
[8] DATURI M,BUSCA G,GUESDON A,et al.Vibrational spectra study of Mo(V) phosphates as examples of different geometries of dimolybdenyl species [J].Journal of Materials Chemistry,2001,11(6):1726-1731.
[9] HE Q L,WANG E B.Hydrothermal synthesis and crystal structure of a new molybdenum(VI) arsenate(III),CoIII(en)3H3O[(CoIIO6)Mo■O18(As■O3)2]·2H2O [J].Inorganica Chimica Acta,1999,295(2):244-247.
[10] WIGGIN S B,WELLER M T.A chiral,16-ring channel framework and a layered caesium zincoarsenate [J].Chemical Communications,2006(10):1100-1102.
[11] LI L L,SHEN Q,XUE G L,et al.Two sandwich arsenomolybdates based on the new building block As(iii)Mo7O279-:[Cr2(AsMo7O27)2]12- and [Cu2(AsMo7O27)2]14- [J].Journal of Chemistry Society,Dalton Transactions,2008(42):5698-5700.
[12] SUN C Y,LI Y G,WANG E B,et al.A series of new organic-inorganic molybdenum arsenate complexes based on [(ZnO6)(As3O3)2Mo6O18]4- and [HxAs2Mo6O26](6-x)- clusters as SBUs [J].Inorganic Chemistry,2007,46:1563-1574.
[13] XU H S,LI L L,LIU B,et al.AsMo7O27- bridged dinuclear sandwich-type heteropolymolybdates of Cr(III) and Fe(III):magnetism of [MM′(AsMo7O27)2]12- with MM′ = FeFe,CrFe,and CrCr [J].Inorganic Chemistry,2009,48:10275-10280.
[14] BURKHOLDER E,WRIGHT S,GOLUB V,et al.Solid state coordination chemistry of oxomolybdenum organoarsonate materials [J].Inorganic Chemistry,2003,42(23):7460-7471.
[15] BURKHOLDER E,ZUBIETA J.Hydrothermal synthesis and structural characterization of a network oxide constructed from {Mo12O34(O3AsC6H5)4}4- clusters and {Cu(terpy)}2+ subunits [J].Inorganica Chimica Acta,2004,357(1):301-304.
[16] MüLLER A,PETERS F,POPE M T,et al.Polyoxometalates:very large clusters nanoscale magnets [J].Chemical Reviews,1998,98(1):239-272.
[17] SHELDRICK G M.SHELXS-97,Program for X-ray Crystal Structure Solution [CP].Germany:University of G?ttingen,1997.
[18] LAUDISE R A.Hydrothermal synthesis of crystals [J].Chemical & Engineering News,1987,65(39):30-43.
[19] HAGRMAN D,HAGRMAN P J,ZUBIETA J.The structural role of metal-organonitrogen subunits in the molecular manipulation of molybdenum oxides [J].Comments on Inorganic Chemistry,1999,21(4/6):225-261.
[20] HSU K F,WANG S L.Cs5Mo8O24(OH)2AsO4· 2H2O and Cs7Mo8O26AsO4:Two novel molybdenum(VI) arsenates containing heteropolyanions [AsMo8O30H2]5- and [AsMo8O30]7- [J].Inorganic Chemistry,1997,36(14):3049-3054.
[21] BRESE N E,O'KEEFFE M.Bond-valence parameters for solids [J].Acta Crystallographica,1991,B47:192-197.