将Cr(salen)配合物分别嫁接于介孔SiO2,MCM-41和SBA-15上制备成非均相Schiff碱铬配合物,并用FT-IR,UV-Vis,XRD,N2吸附和元素分析等对非均相铬配合物进行了表征.以30%的H2O2为氧化剂,以非均相铬配合物为催化剂,在无有机溶剂、相转移催化剂和添加剂的条件下,研究了选择性催化氧化苯甲醇合成苯甲醛的反应.结果表明,非均相铬配合物都表现出较好的催化性能.选择不同的介孔载体对非均相铬配合物的催化性能有较大的影响,Cr(salen)/MCM-41配合物显示有最好的催化性能;在优化的反应条件下,苯甲醇转化率可达52.5%,苯甲醛选择性为100%,且该非均相铬配合物重复使用4次后仍保持较好的催化性能.
参考文献
[1] | Kroschwitz J I.Kirk-Othmer Encyclopedia of Chemical Technology[M].New York:wiley,1992:64. |
[2] | Choudhary V R;Dumbre D K;Narkhede V S;Jana S K .[J].Catalysis Letters,2003,86(04):229. |
[3] | Noyori R;oki M;ato K.[J].Chemical Communications,2003(16):1977. |
[4] | Weng Zh H;Liao G X;Wang J Y;Jian X G .[J].Catalysis Communications,2007,8(10):1493. |
[5] | Zhi Huan Weng,Jin Yan Wang,Xi Gao Jian.Efficient oxidation of benzyl alcohol with heteropolytungstate as reaction-controlled phase-transfer catalyst[J].中国化学快报(英文版),2007(08):936-938. |
[6] | Parvulescu V;Popa A;Davidescu C M;Valceanu R Vass M Luca C .[J].Reactive and Functional Polymers,1997,33(2-3):329. |
[7] | Esposito A;Neri C;Buonomo F .[P].US 4480135,1984. |
[8] | 杜建亮,刘丹,桂建舟,张晓彤,宋丽娟,孙兆林.Cu/SBA-15催化苯甲醇氧化制苯甲醛[J].石油化工高等学校学报,2006(01):13-16. |
[9] | Choudhary V R;Dumbre D K;Uphade B S;Narkhede V S .[J].Journal of Molecular Catalysis A:Chemical,2004,215(1-2):129. |
[10] | 袁淑军,吕春绪,蔡春.一种新型金属胶束模拟氧化酶的合成及其对苯甲醇的催化氧化作用[J].分子催化,2003(01):14-17. |
[11] | Demicheli G;Maggi R;Mazzacani A;Righi P Sartori G Bigi F .[J].Tetrahedron Letters,2001,42(12):2401. |
[12] | Singh U G;Williams R T;Hallam K R;Allen G C .[J].Journal of Solid State Chemistry,2005,178(11):3405. |
[13] | Abrantes M;Sakthivel A;Romao CC;Kuhn FE .A chiral menthyl cyclopentadienyl molybdenum tricarbonyl chloro complex: Synthesis, heterogenization on MCM-41/MCM-48 and application in olefin epoxidation catalysis[J].Journal of Organometallic Chemistry,2006(14):3137-3145. |
[14] | Baleizao C.;Gigante B.;Garcia H.;Corma A. .Chiral vanadyl Schiff base complex anchored on silicas as solid enantioselective catalysts for formation of cyanohydrins: optimization of the asymmetric induction by support modification[J].Journal of Catalysis,2003(2):199-207. |
[15] | Zhang HD;Xiang S;Li C .Enantioselective epoxidation of unfunctionalised olefins catalyzed by Mn(salen) complexes immobilized in porous materials via phenyl sulfonic group[J].Chemical communications,2005(9):1209-1211. |
[16] | 张雪红,管莲秀,李军平,魏伟,赵宁,董满祥,孙予罕.嫁接型席夫碱配合物的制备及其催化性能[J].化学学报,2006(24):2479-2485. |
[17] | Wang XL;Wu GD;Li JP;Zhao N;Wei W;Sun YH .Selective oxidation of benzyl alcohol catalyzed by Cr(salen) complexes immobilized on MCM-41[J].Journal of molecular catalysis, A. Chemical,2007(1/2):86-94. |
[18] | Kresge C T;Leonowicz M E;Roth W J;Vartuli J C Beck J S .[J].Nature,1992,359(6397):710. |
[19] | Zhao D Y;Feng J L;Huo Q S;Melosh N,Fredrickson G H,Chmelka B F,tucky G D .[J].Science,1998,279(5350):548. |
[20] | Carvalho W A;Wallau M;Schuchardt U .[J].Journal of Molecular Catalysis A:Chemical,1999,144(01):91. |
[21] | Zhou X G;Yu X Q;Huang J S;Li S G Li L S Che C M.[J].Chemical Communications,1999(18):1789. |
[22] | Dominguez I;Fornes V;Sabater MJ .Chiral manganese(III) salen catalysts immobilized on MCM-41 and delaminated zeolites ITQ-2 and ITQ-6 through new axial coordinating linkers[J].Journal of Catalysis,2004(1):92-99. |
[23] | Gigante B.;Garcia H.;Sabater MJ.;Corma A. .Assessment of the negative factors responsible for the decrease in the enantioselectivity for the ring opening of epoxides catalyzed by chiral supported Cr(III)-salen complexes[J].Catalysis Letters,2000(1/2):113-119. |
[24] | 霍涌前,李珺,王伟,弓亚琼,张逢星.MCM-41介孔分子筛组装过渡金属配合物的电子光谱[J].光谱学与光谱分析,2004(03):281-284. |
[25] | Kingma I E;Wiersma M;Van der Baan J L;Balt S,Bickelhaupt F,de Bolster M W G,Klumpp G W,Spek A L.[J].Journal of the Chemical Society,Chemical Communications,1993(10):832. |
[26] | Mukherjee S;Samanta S;Roy B C;Bhaumik A .[J].Applied Catalysis A:General,2006,301(01):79. |
[27] | Lim M H;Stein A .[J].CHEMISTRY OF MATERIALS,1999(11):3285. |
[28] | Sing K S W;Everett D H;Haul R A W;Moscow L Pierotti R A Rouquerol T Siemienewska T .[J].Pure and Applied Chemistry,1985,57(04):603. |
[29] | Brunel D;Bellocq N;Sutra P;Cauvel A Laspéras M Moreau P Di Renzo F Galarneau A Fajula F .[J].Coordination Chemistry Reviews,1998,180(02):1085. |
[30] | Belal R;Meunier B .[J].Journal of Molecular Catalysis,1988,44(02):165. |
[31] | Lau S H;Caps V;Yeung K W;Wong K Y Tsang S C .[J].Microporous and Mesoporous Materials,1999,32(03):279. |
[32] | Maldotti A;Molinari A;Varani G;Lenarda M Storaro L Bigi F Maggi R Mazzacani A Sartori G .[J].Journal of Catalysis,2002,209(01):210. |
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