【作者】 王楠；

【导师】 冯威；

【作者基本信息】 吉林大学 ， 海洋地质， 2022， 硕士

【摘要】 实施“海洋强国”战略,需要保持海洋生态环境的持续、健康发展。海洋石油污染这类的环境问题对海洋渔业、水产养殖业以及海洋的生态环境有着严重危害,因此,海洋石油类污染物的降解和处理仍然是一个亟待解决的问题。本文为有效降解海水中石油类污染物,选取钛酸四丁酯作为钛源,采用溶胶-凝胶法（sol-gol）制备了TiO₂催化剂的前驱体,以密度均小于水的空心玻璃微珠（HGM）和活性炭微球为载体,运用浸渍焙烧的方法成功地将催化剂薄膜负载到空心玻璃微珠和活性炭微球上,再用水热法掺杂MoS₂量子点（MoS₂QDs）进行修饰,得到负载型光催化剂分别为MoS₂QDs/TiO₂@HGM?MoS₂QDs/TiO₂@活性炭微球。并以石油醚溶液为模拟污染物,并对其光催化氧化性能进行了研究,探究制备催化剂的最佳条件以及光催化剂对海水中石油醚类污染物的降解效率。利用X射线衍射分析（XRD）、扫描电子显微镜（SEM）、能谱仪表面元素分析法（EDX）、X射线光电子能谱仪（XPS）等技术对所制得的负载型纳米光催化剂样品的组成、形貌、结构等属性进行了表征。通过表征分析可知,空心玻璃微珠、活性炭微球载体上均成功地负载了MoS₂QDs/TiO₂光催化剂,当TiO₂@HGM?TiO₂@活性炭微球的焙烧温度为450℃,负载2次时为此催化剂最佳制备条件。掺杂MoS₂QDs后通过以石油醚为模拟污染物的海水溶液光催化反应2h,测定其降解率,考察了溶胶焙烧时间、负载次数对负载效果的影响,以及催化剂投加量、石油醚初始浓度和MoS₂QDs的掺杂量对目标污染物光催化活性的影响。实验表明:MoS₂QDs/TiO₂@HGM?MoS₂QDs/TiO₂@活性炭微球两种不同载体负载的催化剂都具有高效催化活性。当石油醚初始浓度为100mg/L时,适当调节溶液的p H,在此条件下,当掺杂量为2wt%的MoS₂QDs/TiO₂@HGM光催化剂在投加量为0.4g时,其降解率可达97%,催化性能最优;在此基础上继续探究载体为活性炭微球的光催化剂的催化性能,其最佳条件为当掺杂量为4wt%的MoS₂QDs/TiO₂@活性炭微球光催化剂在投加量为0.4 g时,降解率可达99.3%,经过5次循环实验后降解率仍可达到89%,证明此体系催化剂的结构稳定性强可重复回收利用。更多还原

【Abstract】 To implement the"maritime power"strategy,we need to maintain the sustainable and healthy development of the Marine ecological environment.The environmental problem of Marine oil pollution has brought serious harm to Marine fishery,aquaculture and Marine environment.Therefore,the degradation and treatment of Marine oil pollutants is still an urgent problem to be solved.In this paper for effective degradation of water pollutants,full selection of tetrabutyl titanate as titanium source,using the sol-gel method(sol gol TiO₂catalyst precursor was prepared,with hollow glass beads（HGM）and activated carbon microspheres as the carrier,using the method of impregnation calcination successfully load catalyst film on the hollow glass beads and activated carbon microspheres,The supported photocatalysts were MoS₂QDs/TiO₂@HGM and MoS₂QDs/TiO₂@activated carbon microspheres,respectively.Petroleum ether solution was used as the simulated pollutant,and its photocatalytic oxidation performance was studied to explore the optimum conditions for the preparation of catalysts and the degradation efficiency of petroleum ether pollutants in seawater.The effects of controllable conditions on supported MoS₂QDs/TiO₂@HGM and MoS₂QDs/TiO₂@activated carbon microspheres were studied.X-ray diffraction（XRD）,scanning electron microscopy（SEM）,energy spectrum instrument surface element analysis（EDX）,X-ray photoelectron spectroscopy（XPS）and other techniques were used to characterize the composition,morphology and structure of the supported nano-photocatalyst samples.Through characterization analysis,MoS₂QDs/TiO₂photocatalyst was successfully supported on hollow glass microspheres and activated carbon microspheres.When the calcination temperature of TiO₂@HGM and TiO₂@activated carbon microspheres was 450℃,the optimal preparation conditions for the catalyst were supported twice.After doping MoS₂QDs,the photocatalytic reaction of seawater solution with petroleum ether as the simulated pollutant was 2h,and the degradation rate was measured.The influence of sol roasting time and loading times on the loading effect was investigated,as well as the influence of catalyst dosage,initial concentration of petroleum ether,and the doping amount of MoS₂QDs on the photocatalytic activity of the target pollutant.The results show that MoS₂QDs/TiO₂@HGM and MoS₂QDs/TiO₂@activated carbon microspheres have high catalytic activity.When the initial concentration of petroleum ether is 100mg/L,the p H of the solution is properly adjusted.Under these conditions,when the doping amount of 2wt%MoS₂QDs/TiO₂@HGM photocatalyst is 0.4 g,the degradation rate can reach 97%,and the catalytic performance is the best.On this basis,the catalytic performance of the photocatalyst with activated carbon microspheres as the carrier was further explored.The optimal condition was that when the doping amount of MoS₂QDs/TiO₂@activated carbon microspheres was 0.4 g,the degradation rate could reach 99.3%,and the degradation rate could still reach 89%after 5 cycles of experiments.It is proved that the catalyst has strong structural stability and can be reused.更多还原