D301苯乙烯树脂固载Dawson型杂多酸催化剂的制备及性能研究
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摘要
以D301苯乙烯树脂作为载体,采用加热回流的方法,制备了固载Dawson型杂多酸H9[P2Mo16V2O62]催化剂,并用傅里叶变换红外光谱、X-射线衍射、扫描电镜和电子能谱仪进行表征.将此催化剂用于环己醇选择性氧化,考察了温度、时间、催化剂用量和双氧水用量对反应的影响以及催化剂的重复使用性能.实验结果表明,催化剂可使环己醇高选择性生成环己酮,在环己醇0.05 mol,反应温度为80oC,反应时间5 h,催化剂用量3.2 g,ω(H2O2)=30%H2O222 ml条件下,环己醇的转化率为78.6%,环己酮的选择性为87.3%,催化剂易于回收再用,在较优条件下,固载催化剂重复使用四次,仍保持较高的催化活性.
A Dawson H9[P2Mo16V2O62] supported on D301 styrene exchange resin by heating reflux methed is prepared and characterized by Fourier transform infrared spectroscopy(FTIR),x-ray diffraction(XRD),scanning electron microscopy(SEM) and electron spectrometer(ES).This catalyst is applied to selective oxidation of cyclohexanol.The effects on the oxidation of cyclohexanol are investigated in details including the amount of catalyst and H2O2,the temperature,the time and the catalytic activity of recycling.Experiment results show cyclohexanone could be selectively synthesized from cyclohexanol upon catalysis.The transformation of cyclohexanol is 78.6% and the selective of cyclohexanone is 87.3% when using 3.2 g catalyst and 22 ml ω(H2O2)=30%H2O2,at 80oC and reacting 5 h.The high catalytic activity is retained after repeating four times.
A Dawson H9[P2Mo16V2O62] supported on D301 styrene exchange resin by heating reflux methed is prepared and characterized by Fourier transform infrared spectroscopy(FTIR),x-ray diffraction(XRD),scanning electron microscopy(SEM) and electron spectrometer(ES).This catalyst is applied to selective oxidation of cyclohexanol.The effects on the oxidation of cyclohexanol are investigated in details including the amount of catalyst and H2O2,the temperature,the time and the catalytic activity of recycling.Experiment results show cyclohexanone could be selectively synthesized from cyclohexanol upon catalysis.The transformation of cyclohexanol is 78.6% and the selective of cyclohexanone is 87.3% when using 3.2 g catalyst and 22 ml ω(H2O2)=30%H2O2,at 80oC and reacting 5 h.The high catalytic activity is retained after repeating four times.
引文
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[4]贾太轩,张继昌,赵凌,等.(CTAB)9[Sb1.00W9O33]催化氧化环己醇制备环己酮[J].石油化工,2011,40(6):594-597.
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[9]李贵贤,赵军龙,余华,等.Keggin型多元杂多酸催化合成苯乙酮环乙二缩酮[J].分子催化,2010,24(2):129-134.
[10]毛志红,王洁,李贵贤,等.硅烷化凹凸棒石负载H5PMo10V2O40催化合成苯甲醛乙二醇缩醛[J].分子催化,2010,25(5):393-398.
[11]王恩波,高丽华,刘景福,等.具有Dawson结构的钼钒磷杂多酸的制备和性质研究[J].化学学报,1988,46(8):757-762.
[12]李家其,尹笃林,郭军,等.Dawson型钒代磷钼酸在酮/醇缩合中的催化性能[J].分子催化,2009,23(6):511-515.
[13]刘霞,赵军,冯长根,等.三钒取代的Dawson型磷钼钒甘氨酸杂多化合物的合成及光谱研究[J].光谱学与光谱分析,2006,26(12):2226-2228.
[2]谢文莲,田爱国.环己酮生产工艺及研究进展[J].化工进展,2003,22(4):420-423.
[3]谭钦文,尹光志,李斗.环己酮生产废水处理工程技术改造[J].水处理技术,2008,34(6):82-86.
[4]贾太轩,张继昌,赵凌,等.(CTAB)9[Sb1.00W9O33]催化氧化环己醇制备环己酮[J].石油化工,2011,40(6):594-597.
[5]于克生,冯豫川,刘承秀.Dawson型磷钼钒杂多酸催化H2O2氧化醇类化合物的研究[J].西南民族大学学报:自然科学版,2011,1:107-110.
[6]于克生,冯豫川,周永恒,等.Dawson型磷钼酸及钒修饰Dawson型磷钼酸的制备及其活性研究[J].西南民族大学学报:自然科学版,2011,2:257-262.
[7]冯豫川,于克生,苗计生,等.高含量钒修饰Dawson型磷钼酸的制备及性能研究[J].西南民族大学学报:自然科学版,2011,3:431-436.
[8]王俊,李天全,秦玉楠.含钼杂多酸型催化剂在有机合成中的应用[J].中国铝业,2005,29(2):34-36.
[9]李贵贤,赵军龙,余华,等.Keggin型多元杂多酸催化合成苯乙酮环乙二缩酮[J].分子催化,2010,24(2):129-134.
[10]毛志红,王洁,李贵贤,等.硅烷化凹凸棒石负载H5PMo10V2O40催化合成苯甲醛乙二醇缩醛[J].分子催化,2010,25(5):393-398.
[11]王恩波,高丽华,刘景福,等.具有Dawson结构的钼钒磷杂多酸的制备和性质研究[J].化学学报,1988,46(8):757-762.
[12]李家其,尹笃林,郭军,等.Dawson型钒代磷钼酸在酮/醇缩合中的催化性能[J].分子催化,2009,23(6):511-515.
[13]刘霞,赵军,冯长根,等.三钒取代的Dawson型磷钼钒甘氨酸杂多化合物的合成及光谱研究[J].光谱学与光谱分析,2006,26(12):2226-2228.