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分子筛MCM-48负载多金属氧酸盐的合成及其催化性能研究

Synthesis, Characterization and Catalytic Activity of Polyoxometalates on MCM-48 Molecular Sieve

【作者】 张义军

【导师】 杨水金;

【作者基本信息】 华中师范大学 , 分析化学, 2008, 硕士

【摘要】 制备了Keggin型多酸化合物磷钨酸、硅钨酸及其负载型H3PW12O40/MCM-48,H4SiW12O40/MCM-48并采用IR和XRD对其进行了表征。研究了H3PW12O40,H3PW12O40/MCM-48在可见光光照条件下,对模拟染料废水甲基橙溶液的光催化脱色性能,实验结果表明,光催化剂的投加量,甲基橙的初始浓度,光照强度,光照时间以及催化剂类型是影响甲基橙溶液脱色率的重要因素。以甲基丙烯酸和正丁醇为原料,探讨了应用H3PW12O40/MCM-48催化合成甲基丙烯酸正丁酯的条件,考察了原料量比,催化剂用量,反应时间诸因素对产品收率的影响。结果表明,H3PW12O40/MCM-48是合成甲基丙烯酸正丁酯的良好催化剂。分别考察了以H4SiW12O40/MCM-48为催化剂对以乙酰乙酸乙酯、环己酮、丁酮、苯甲醛和正丁醛与二元醇(乙二醇,1,2-丙二醇)为原料合成10种缩醛(酮)的反应条件,以及以H4SiW12O40/MCM-48为催化剂对丁酮和1,2-丙二醇为原料合成丁酮1,2-丙二醇缩酮的催化活性,较系统地考察了原料量比,催化剂用量,反应时间诸因素对产品收率的影响。结果表明,H4SiW12O40/MCM-48是合成缩醛(酮)的良好催化剂。

【Abstract】 In this paper,the Keggin unit polyoxometalate phosphotungstic acid(H3PW12O40), silicotungstic acid(H4SiW12O40),H3PW12O40/MCM-48,H4SiW12O40/MCM-48 were prepared,and they were characterized by IR and XRD.Both of H3PW12O40and H3PW12O40/MCM-48 were used as the photocatalysts to degradate the methyl orange solution under irradiated by visible light.It has been shown that the photocatalyst dosage, the initital concentration of methyl orange,intensity and time under irradiated by visible light are the important factors of decolorizing.With methacrylic acid and n-butyl alcohol as material,the synthesis of n-butyl methacrylate catalyzed by H3PW12O40/MCM-48 was studied.And effects of the rate of material,catalyst dosage and reaction time on yields of the products were investigated too.Experimental results showed that H3PW12O40/MCM-48 is an excellent catalyst.In addition,H4SiW12O40/MCM-48 as an environmental friendly catalysts,the catalytic activities of H4SiW12O40/MCM-48 in synthesizing 2-methyl-2-ethoxycarbonylmethyl-1, 3-dioxolane,2,4-dimethyl-2-ethoxycarbonyl-methyl-1,3-dioxolane, cyclohexanone ethylene ketal,cyclohexanone 1,2-propanediol ketal, butanoneethylene ketal,butanonel,2-propanediolketal,2-phenyl- 1,3-dioxolane, 4-methyl-2-phenyl-1,3-dioxolane,2-propyl-1,3-dioxolane and 4-methyl-2-propyl-1, 3-dioxolane were reported,while butanone 1,2-propanediol ketal was synthesized from butanone and 1,2-propanediol in the presence of H4SiW12O40/MCM-48. The factors influencing the synthesis were discussed and the optimum conditions were found out.The experimental results showed that H4SiW12O40/MCM-48 is an excellent catalyst.

【关键词】 多金属氧酸盐光催化剂降解甲基橙MCM-48缩醛缩酮催化
【Key words】 polyoxometalatephotocatalystdegradationmethyl orangeMCM-48acetalketalcatalys
  • 【分类号】O643.3
  • 【被引频次】1
  • 【下载频次】270
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