以H2O2为氧化剂,以磷酸氢盐或磷酸二氢盐为添加剂,研究了反应控制相转移催化剂(磷钨杂多酸季铵盐)催化丙烯环氧化的反应性能. 结果表明,当体系中不存在添加剂时,产物环氧丙烷的水解情况严重; 加入适量的添加剂可有效抑制环氧丙烷的水解. 作为抑制环氧丙烷水解的添加剂,磷酸氢盐比磷酸二氢盐具有更优异的性能,且磷酸氢钾比磷酸氢钠效果更佳. 在没有丙烯的情况下,随着温度的升高,环氧丙烷水解反应加剧; 在相同的温度下,环氧丙烷浓度越低,其水解率越高; 当环氧丙烷浓度较低时,催化剂的存在促进其水解,但在较高的浓度下,催化剂的存在则可抑制其水解. 随着温度的升高, H2O2分解反应加剧,当温度超过60 ℃时,分解速度显著加快. 催化剂在油/水二相中的分配实验结果表明,在H2O2存在的情况下,于50 ℃达到平衡时, 85.0%以上的催化剂被转移至有机相.
参考文献
[1] | Yamamoto J;Tsuji J .[P].JP:2000/107604,2000. |
[2] | Yamamoto J;Tsuji J .[P].JP:2000/117101,2000. |
[3] | Yamamoto J;Tsuji J .[P].JP:2000/107605,2000. |
[4] | 王晓晗,卢冠忠.过氧化氢异丙苯催化氧化丙烯制环氧丙烷[J].催化学报,2000(05):407-410. |
[5] | 王新宏,卢冠忠,刘晓晖,郭杨龙,王筠松.在溶胶-凝胶法制备的MoO3/SiO2催化剂上丙烯的环氧化反应[J].催化学报,2002(06):498-502. |
[6] | Neri C;Anfossi B;Esposito A;Buonomo F .[P].EP:100119,1984. |
[7] | Neri C;Buonomo F;Anfossi B .[P].EP:100118,1984. |
[8] | Neri C;Buonomo F .[P].EP:102097,1984. |
[9] | Clerici M G;Bellussi G;Romano U .[J].Journal of Catalysis,1991,129(01):159. |
[10] | Notari B .[J].Catalysis Today,1993,18(02):163. |
[11] | 李钢,郭新闻,王祥生.钛硅分子筛的结构表征及催化性能研究[J].燃料化学学报,1998(02):119-124. |
[12] | 薛俊利,许锡恩.TS-1催化合成环氧丙烷[J].燃料化学学报,1998(06):569-574. |
[13] | 卢冠忠;张国斌;刘文孝;韩春国,史建公 .[J].分子催化,1997,11(03):191. |
[14] | 高焕新;曹静;卢巍然;陈庆龄 .[P].CN:1268400,2000. |
[15] | Cooker B;Gaffney A M;Jewson J D;Onimus W H .[P].US:5780657,1998. |
[16] | Lu G Zh;Zuo X B .[J].Catalysis Letters,1999,58(01):67. |
[17] | Lu JQ.;Luo MF.;Lei H.;Li C. .Epoxidation of propylene on NaCl-modified silver catalysts with air as the oxidant[J].Applied Catalysis, A. General: An International Journal Devoted to Catalytic Science and Its Applications,2002(1/2):11-19. |
[18] | Jin G J;Lu G Zh;Guo Y L et al.[J].Catalysis Letters,2003,87(3-4):249. |
[19] | Jin G J;Lu G Zh;Guo Y L et al.[J].Catalysis Today,2004,93-95:173. |
[20] | Pennington B T .[P].US:4885374,1989. |
[21] | Pennington B T;Fullington M C .[P].US:4943643,1990. |
[22] | Yoshida H;Tanaka T;Yamamoto M.[J].Chemical Communications,1996(18):2125. |
[23] | Yoshida H.;Yamamoto M.;Yoshida T.;Funabiki T.;Yoshida S.;Tanaka T. .EPOXIDATION OF PROPENE BY GASEOUS OXYGEN OVER SILICA AND MG-LOADED SILICA UNDER PHOTOIRRADIATION[J].Journal of Catalysis,1997(2):351-357. |
[24] | Xi Z W;Zhou N;Sun Y;Li K L .[J].Science,2001,292(5519):1139. |
[25] | Sun Y.;Cao GY.;Xi ZW. .Epoxidation of olefins catalyzed by [pi-C5H5NC16H33](3) [PW4O16] with molecular oxygen and a recyclable reductant 2-ethylanthrahydroquinone[J].Journal of molecular catalysis, A. Chemical,2001(2):219-224. |
[26] | Zhou N;Xi Z W;Cao G Y;Gao Sh .[J].Applied Catalysis A:General,2003,250(02):239. |
[27] | Li J;Gao Sh;Li M et al.[J].Journal of Molecular Catalysis A:Chemical,2004,218(02):247. |
[28] | Gao J B;Chen Y Y;Han B et al.[J].Journal of Molecular Catalysis A:Chemical,2004,210(1-2):197. |
[29] | Csanyi L J;Jaky K .[J].Journal of Molecular Catalysis,1990,61(01):75. |
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