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摘要：本实验通过制备Fe3O4@SiO2@Cu2O磁性纳米材料并将其作为催化剂催化O3降解苯胺。通过实验比较了不同体系对苯胺的降解情况，并考察了pH、催化剂用量、O3浓度对苯胺降解反应的影响；同时，通过加入羟基自由基抑制剂(叔丁醇TBA)和超氧阴离子自由基抑制剂(对苯醌BQ)来确定活性中间产物，从而推测其可能的反应机理。结果表明，Fe3O4@SiO2@Cu2O磁性纳米材料对O3有较好的活化作用，反应20 min，苯胺能够被完全降解，在实验所选的pH范围内，pH=7时最有利于苯胺的去除。在实验因素控制范围内，随着催化剂用量或O3浓度的增加，苯胺的降解速率越快。通过向反应体系中投加自由基抑制剂实验，可推测Fe3O4@SiO2@Cu2O磁性纳米材料的加入促进了O3分解产生了超氧自由基(O2•-)，而非通常所认为的羟基自由基(•OH)。26385
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毕业论文关键词：Fe3O4@SiO2@Cu2O；O3；苯胺；降解；超氧自由基
Preparation of Fe3O4@SiO2@Cu2O and the Degradation of Aniline by Ozone Catalyzed with Fe3O4@SiO2@Cu2O Catalyst
Abstract: In this study, a magnetic nanomaterial (Fe3O4@SiO2@Cu2O) was prepared and used as a catalyst to catalyze O3 to degrade aniline, an organic pollutant which is carcinogenic, teratogenic and mutagenic. The degradation of aniline in different catalytic systems was compared in batch experiments. Meanwhile, the effects of solution pH, Fe3O4@SiO2@Cu2O dosage and the concentration of ozone on the degradation of aniline were investigated in this study. To reveal the active intermediates and the free radicals in the degradation of aniline by ozone activated by Fe3O4@SiO2@Cu2O, free radical inhibitors (tert-butanol, p-benzoquinone) were introduced into the degradation system, and the possible reaction mechanism was deduced. The results of the experiments indicated that Fe3O4@SiO2@Cu2O magnetic nanomaterial dramaticlly has a catalysis on the ozonation of aniline. When the reaction was carried out for 20 min, the aniline can be completely degraded. In the range of pH conducted in this study, the removal of aniline is most favorable at pH 7. During the range of the experimental factors, the degradation rate of aniline became faster with the increase of catalyst dosage or the concentration of O3. It can be concluded that the addition of Fe3O4@SiO2@Cu2O magnetic nanomaterial promotes the decomposition of O3 to produce superoxide free radicals (O2•-) to degrade aniline rather than hydroxyl free radicals (•OH) which were commonly considered as the main active intermediate via adding different free radical inhibitors to the catalytic system.
Key words: Fe3O4@SiO2@Cu2O; ozone; aniline; degradation; superoxide free radicals
目 录
摘要 1
关键词 1
Abstract 1
Key words 1
引言 1
1 材料与方法 2
1.1 实验原料及仪器 2
1.2 溶液配制 2
1.3 实验过程与方法 4
1.3.1 催化剂Fe3O4@SiO2@Cu2O的制备 4
1.3.2 实验装置 4
1.3.3 实验方法 5
1.4 分析方法 5
1.4.1 苯胺分析方法 5
1.4.2 气相中臭氧浓度测定方法 6
1.4.3 溶液pH值测定方法 6
1.4.4 水中TOC浓度测定方法 6
2 结果与讨论 6
2.1 不同反应体系对苯胺的降解 6
2.2 反应条件对Fe3O4@SiO2@Cu2O活化O3降解苯胺的影响 7
2.2.1 溶液pH对苯胺降解的影响 7