OALib Journal期刊
ISSN: 2333-9721
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(TEAH)nH3-nPW12O40催化苯甲醇选择氧化及其反应机理
DOI: 10.1016/S1872-2067(14)60097-8, PP. 1224-1234
Keywords: 苯甲醇,选择氧化,磷钨酸盐,机理
Abstract:
?以Keggin结构的磷钨酸和三乙胺(TEA)为原料,通过简单的酸碱反应合成了磷钨酸的TEA盐.并以它们为催化剂,考察了以H2O2为氧化剂、以水为溶剂的体系中苯甲醇选择氧化制备苯甲醛的反应性能.结果表明,(TEAH)nH3-nPW12O40(n=1,2,3)系列催化剂对苯甲醇的选择氧化反应有很高的活性和选择性,且可被分离和循环使用.在适宜的反应条件下,最佳催化剂(TEAH)H2PW12O40上,苯甲醇的转化率可达99.6%,苯甲醛的选择性为100%.还采用IR,31PNMR谱和元素分析技术,对催化剂和反应过程中催化剂物种的转化和分布进行了考察,进而导出了反应机理.在这个水--油两相反应中,(PW12O40)3-首先在H2O2的作用下,氧化降解为溶于水的小分子过氧物种(PO4(WO(O2)2)4)3-和自由W物种.(PO4(WO(O2)2)4)3-是真正的活性物种,可将部份溶于水层的苯甲醇氧化为苯甲醛,自身转变为失去活性氧的反应后物种(SAR).而SAR又可与自由W物种一起聚合为前驱体状态的(PW12O40)3-,完成催化循环.
References
[1] | Salles L, Aubry C, Thouvenot R, Robert F, Dorémieux-Morin C, Chottard G, Ledon H, Jeannin Y, Brégeault J-M. Inorg Chem, 1994, 33: 871
|
[2] | Ishii Y, Yamawaki K, Yoshida T, Ura T, Ogawa M. J Org Chem, 1987, 52: 1868
|
[3] | Kozhevnikov I V, Mulder G P, Steverink-de Zoete M C, Oostwal M G. J Mol Catal A, 1998, 134: 223
|
[4] | Tundo P, Romanelli G P, Vázquez P G, Aricò F. Catal Commun, 2010, 11: 1181
|
[5] | Zhang F M, Guo M P, Ge H Q, Wang J. Chin J Chem Eng, 2007, 15: 895
|
[6] | Ma B C, Zhang Y S, Ding Y, Zhao W. Catal Commun, 2010, 11: 853
|
[7] | Liu C, Tan R, Sun W Q, Yin D H. Chin J Catal (刘成, 谭蓉, 孙文庆, 银董红. 催化学报), 2012, 33: 1032
|
[8] | Leng Y, Liu J, Jiang P P, Wang J. RSC Adv, 2012, 2: 11653
|
[9] | Duncan D C, Chambers R C, Hecht E, Hill C L. J Am Chem Soc, 1995, 117: 681
|
[10] | Aubry C, Chottard G, Platzer N, Brégeault J-M, Thouvenot R, Chauveau F, Huet C, Ledon H. Inorg Chem, 1991, 30: 4409
|
[11] | Fan C L, Liu W M. Chem Ind Tmies (樊春玲, 刘文明. 化工时刊), 2008, 22(9): 61
|
[12] | Wu X G, Yin J J, Hu Z J. Special Petrochem (吴鑫干, 尹娟娟, 胡在君. 精细石油化工), 2002, (4): 57
|
[13] | Kholdeeva O A, Maksimchuk N V, Maksimov G M. Catal Today, 2010, 157: 107
|
[14] | Ishii Y, Yamawaki K, Ura T, Yamada H, Yoshida T, Ogawa M. J Org Chem, 1988, 53: 3587
|
[15] | Zhang S J, Zhao G D, Gao S, Xi Z W, Xu J. J Mol Catal A, 2008, 289: 22
|
[16] | Zhao P P, Wang J, Chen G J, Zhou Y, Huang J. Catal Sci Technol, 2013, 3: 1394
|
[17] | Zhao W, Ding Y, Ma B C, Qiu W Y. Synth Commun, 2012, 42: 554
|
[18] | Weng Z H, Wang J Y, Zhang S H, Yan C, Jian X G. Catal Commun, 2008, 10: 125
|
[19] | Manyar H G, Chaure G S, Kumar A. J Mol Catal A, 2006, 243: 244
|
[20] | Weng Z H, Liao G X, Wang J Y, Jian X G. Catal Commun, 2007, 8: 1493
|
[21] | Weng Z H, Wang J Y, Jian X G. Catal Commun, 2008, 9: 1688
|
[22] | Leng Y, Zhao P P, Zhang M J, Wang J. J Mol Catal A, 2012, 358: 67
|
[23] | Zhao M T, Zhou J W, Li Z, Chen J, Xia C G. J Mol Catal (China) (赵美廷, 周剑伟, 李臻, 陈静, 夏春谷. 分子催化), 2011, 25: 97
|
[24] | Tan R, Liu C, Feng N D, Xiao J, Zheng W G, Zheng A M, Yin D H. Microporous Mesoporous Mater, 2012, 158: 77
|
[25] | Venturello C, D'Aloisio R, Bart J C J, Ricci M. J Mol Catal, 1985, 32: 107
|
[26] | Dengel A C, Griffith W P, Parkin B C. J Chem Soc, Dalton Trans, 1993: 2683
|
[27] | Yadav G D, Mistry C K. J Mol Catal A, 2001, 172: 135
|
[28] | Gao J B, Chen Y Y, Han B, Feng Z C, Li C, Zhou N, Gao S, Xi Z W. J Mol Catal A, 2004, 210: 197
|
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