活性炭石墨烯钯纳米催化剂催化传质的模拟及实验研究-化学工程专业论文.docxVIP

万方数据 万方数据 中文摘要 活性炭具有发达的微观孔道，它的比表面积可达到 1000 m2/g，作为催化剂 载体可以有效分散活性颗粒。但正是由于活性炭的微观孔道，导致反应物在接触 催化活性位点时，扩散阻力较大，对催化活性起消极作用。自 2004 年石墨烯的 成功制备，其在催化领域的应用就受到大家重视。这是因为石墨烯和活性炭一样 都具有在高温、强酸强碱条件下的稳定性，同时石墨烯的比表面积高达 2630 m2/g 且为单片层结构。这些特点导致石墨烯作为催化剂载体在催化反应的过程中可以 更好的分散活性位点且反应过程不存在内扩散影响。本文研究了本征反应速率、 扩散速率、催化剂尺寸对活性炭/石墨烯基催化剂催化过程的影响，并用硼氢化钠 还原对硝基苯酚反应证明石墨烯基催化剂催化活性优于活性炭基催化剂。 本文利用 COMSOL Multiphysics 软件对催化反应过程进行模拟。对于活性 炭基催化剂，通过改变本征反应速率、扩散速率、催化剂尺寸三个因素研究其在 催化过程中沿半径方向反应物浓度变化。对于快速反应，减小反应物扩散速率或 增大催化剂尺寸均不利于活性炭颗粒内部活性位点的利用。对于石墨烯基催化剂， 通过改变本征反应速率因素研究在催化传质过程中石墨烯表面反应物浓度的变 化。对于快速反应，石墨烯表面几乎没有反应物积累，而对于慢速反应，石墨烯 表面反应物浓度与环境流体相同。同时，本文对活性炭/石墨烯基催化剂催化硼氢 化钠还原对硝基苯酚进行模拟，得到石墨烯基催化剂催化效率优于活性炭基催化 剂。 本文采用在活性炭/石墨烯载体上负载钯纳米颗粒催化剂催化硼氢化钠还原 对硝基苯酚实验证明模拟结果。控制反应平行进行，得到石墨烯基钯纳米颗粒催 化剂的催化效率优于活性炭基催化剂。 关键词：活性炭；石墨烯；COMSOL；内扩散；对硝基苯酚 ABSTRACT Activated carbon has developed micro channel and its specific surface area is as large as 1000 m2/g. As the catalyst carrier it can effectively disperse the active particles, but just because of its micro channel, the diffusion resistance is relatively large when reactants touch catalytic active site, which has a negative effect on catalytic activity. Since graphene was successfully prepared in 2004, its application in catalysis has attracted people’s attention. This is because graphene has good stability under the condition of high temperature, strong acid and strong alkali, while its specific area is 2630 m2/g with the single layer structure. Because of these characteristics graphene can disperse the active site better as the catalyst carrier in the reaction process without the effects of internal diffusion. In this work, the effect of intrinsic reaction rate, diffusion rate and catalyst size on activated carbon and graphene catalyst process has been investigated, and the reduction of p-nitrophenol by sodium borohydride indicated that the catalytic activity of graphene based catalysts in better than that of activated carbon based catalyst. In this work, the catalytic reaction process was simulated with C