稀土掺杂阳极氧化金属丝网VOCs处理催化剂的制备及性能研究
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摘要
挥发性有机化合物(VOCs)对环境和人体的严重危害已经引起了人们的广泛关注。目前国内外已开发的多种处理VOCs的技术中催化燃烧法因其高效、无二次污染的特点,是一种有效的处理技术。
稀土催化材料应用于工业废气的处理显示出非常优越的性质,有关这方面的研究有了很大的进展。近年来已有大量文献报导了稀土具有良好的助催化性能和储氧性能,多数研究发现将稀土元素作为助剂或添加剂与贵金属组合使用,可以有效地提高催化剂的活性、耐久性和高温稳定性。
本论文首先介绍了新型阳极氧化膜贵金属催化剂。通过改变阳极氧化工艺中电流强度、电解质种类、电解质浓度等影响阳极氧化膜形成的因素,筛选出阳极氧化的最佳工艺制备了阳极氧化膜不锈钢丝网载体。在所制备的载体上负载贵金属制备了阳极氧化膜不锈钢丝网贵金属催化剂,并对还原时间、焙烧温度等催化剂制备中的影响因素进行了考察。催化活性较好的0.1%Pt-0.5%Pd/不锈钢丝网催化剂对甲苯、丙酮和乙酸乙酯的完全转化温度分别为220℃、260℃和280℃。并采用SEM,XPS,EDX等表征技术对该催化剂的表面形貌及组成进行了测试。
在此基础上我们又引入稀土铈制备了稀土—贵金属不锈钢阳极氧化膜催化剂。考察了各反应条件变化对催化剂催化活性的影响,同时对该催化剂进行了耐热性和稳定性实验。结果表明,0.75%CeO_2-0.1%Pt-0.5%Pd/不锈钢丝网催化剂具有良好的催化活性,甲苯、丙酮和乙酸乙酯的完全转化温度分别为160℃、220℃和250℃,且该催化剂具有一定的稳定性。并运用多种实验技术(如:SEM,XPS,TPO,TPR,EDX等)对该催化材料的结构和性能进行了表征。
Nowadays, volatile organic compounds (VOCs) from chemical and petrochemical plants have given rise to comprehensive attention for their hazardous to the environment and human health. There are many different techniques used for elimination of VOCs. Among them, catalytic combustion is regarded as up-to-date feasible methods, for its high efficiency and no formation of by-products.
Rare earth materials showed very excellent characters in the industrial exhaust gas. It was reported that the rare earth elements appeared as good associate catalysts, and they have excellent oxygen storage capacity. There are a lot of literatures focused on adding rare earth elements into noble or transition metal materials, on which showed good catalytic activity. In addition, the catalysts also showed good stability and good resistance.
At first, we developed a noble metal catalyst, in which using stainless steel material as support by anodic oxidation treatment. We systematically investigated different conditions of anodic oxidation treatment, such as electrolyte concentrations and current intensity. At the same time, the influences of reductive time, calcined temperature and space velocity were also tested. The results indicated that 0.1%Pt-0.5%Pd/stainless steel wire mesh catalyst held the better catalytic performance for VOCs, on which the total conversion of toluene, acetone and ethyl acetate is at 220℃, 260℃and 280℃. The physical properties and surface structure of the catalysts were analyzed and characterized by SEM, XPS and EDX.
On the basis of the results mentioned above, the study of introduce rare earth element of Ce was performed. The factors of Ce-Pt-Pd/stainless steel wire mesh catalyst for VOCs were also investigated, such as current intensity, reductive time, calcined temperature, and so on. Then the thermal stability and the catalytic activity of VOCs oxidation over the catalysts were tested. The results revealed that 0.75%CeO_2-0.1%Pt-0.5%Pd/stainless steel wire mesh catalyst had the best performance for VOCs, on which the total conversion of toluene, acetone and ethyl acetate is at 160℃, 220℃and 250℃, respectively. The structure and catalytic properties of the catalysts were investigated by means of SEM, XPS, TPR, EDX technologies.
稀土催化材料应用于工业废气的处理显示出非常优越的性质,有关这方面的研究有了很大的进展。近年来已有大量文献报导了稀土具有良好的助催化性能和储氧性能,多数研究发现将稀土元素作为助剂或添加剂与贵金属组合使用,可以有效地提高催化剂的活性、耐久性和高温稳定性。
本论文首先介绍了新型阳极氧化膜贵金属催化剂。通过改变阳极氧化工艺中电流强度、电解质种类、电解质浓度等影响阳极氧化膜形成的因素,筛选出阳极氧化的最佳工艺制备了阳极氧化膜不锈钢丝网载体。在所制备的载体上负载贵金属制备了阳极氧化膜不锈钢丝网贵金属催化剂,并对还原时间、焙烧温度等催化剂制备中的影响因素进行了考察。催化活性较好的0.1%Pt-0.5%Pd/不锈钢丝网催化剂对甲苯、丙酮和乙酸乙酯的完全转化温度分别为220℃、260℃和280℃。并采用SEM,XPS,EDX等表征技术对该催化剂的表面形貌及组成进行了测试。
在此基础上我们又引入稀土铈制备了稀土—贵金属不锈钢阳极氧化膜催化剂。考察了各反应条件变化对催化剂催化活性的影响,同时对该催化剂进行了耐热性和稳定性实验。结果表明,0.75%CeO_2-0.1%Pt-0.5%Pd/不锈钢丝网催化剂具有良好的催化活性,甲苯、丙酮和乙酸乙酯的完全转化温度分别为160℃、220℃和250℃,且该催化剂具有一定的稳定性。并运用多种实验技术(如:SEM,XPS,TPO,TPR,EDX等)对该催化材料的结构和性能进行了表征。
Nowadays, volatile organic compounds (VOCs) from chemical and petrochemical plants have given rise to comprehensive attention for their hazardous to the environment and human health. There are many different techniques used for elimination of VOCs. Among them, catalytic combustion is regarded as up-to-date feasible methods, for its high efficiency and no formation of by-products.
Rare earth materials showed very excellent characters in the industrial exhaust gas. It was reported that the rare earth elements appeared as good associate catalysts, and they have excellent oxygen storage capacity. There are a lot of literatures focused on adding rare earth elements into noble or transition metal materials, on which showed good catalytic activity. In addition, the catalysts also showed good stability and good resistance.
At first, we developed a noble metal catalyst, in which using stainless steel material as support by anodic oxidation treatment. We systematically investigated different conditions of anodic oxidation treatment, such as electrolyte concentrations and current intensity. At the same time, the influences of reductive time, calcined temperature and space velocity were also tested. The results indicated that 0.1%Pt-0.5%Pd/stainless steel wire mesh catalyst held the better catalytic performance for VOCs, on which the total conversion of toluene, acetone and ethyl acetate is at 220℃, 260℃and 280℃. The physical properties and surface structure of the catalysts were analyzed and characterized by SEM, XPS and EDX.
On the basis of the results mentioned above, the study of introduce rare earth element of Ce was performed. The factors of Ce-Pt-Pd/stainless steel wire mesh catalyst for VOCs were also investigated, such as current intensity, reductive time, calcined temperature, and so on. Then the thermal stability and the catalytic activity of VOCs oxidation over the catalysts were tested. The results revealed that 0.75%CeO_2-0.1%Pt-0.5%Pd/stainless steel wire mesh catalyst had the best performance for VOCs, on which the total conversion of toluene, acetone and ethyl acetate is at 160℃, 220℃and 250℃, respectively. The structure and catalytic properties of the catalysts were investigated by means of SEM, XPS, TPR, EDX technologies.
引文
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