【作者】 刘南；

【导师】 刘淼；

【作者基本信息】 吉林大学 ， 环境科学， 2011， 博士

【摘要】 随着工业的高速发展,人类生活空间逐渐受到污染和影响。恶臭气体污染逐渐成为影响社会生活质量的重要环境问题之一,尤其是生产过程中排放的恶臭对人体健康已经形成严重威胁。近年来,随着恶臭污染治理社会需求的加大,促进了国内、外关于治理此类污染物应用技术的发展,出现较多的新兴净化技术如：臭氧处理法、等离子体处理法、光触媒催化降解法等,这些方法在实际操作过程中各有利弊,在一定时间内还无法进行普及和应用。吸附法由于其独特的物理化学特性和操作简便,始终是为全球比较广泛的环境治理技术,在广泛用于水质净化的同时,因其净化容量大,一些优质的吸附剂在空气环境治理中也得到了越来越广的应用,本文主要采用氧化铝和沸石进行吸附实验,并对其进行表面改性制备,以求获得更高效恶臭气体污染吸附材料。论文前半部概述了吸附剂组成及改性吸附的原理,因氧化铝本身性质稳定且具备较好的吸附能力,再通过硝酸锰和硝酸镧的高温浸渍改性,得到表面性能更优的氧化铝吸附剂,结合SEM、XRD对改性前后表面进行分析,首先证明了氧化铝在微结构上发生了有利于吸附的性能上的改变,比表面积增加的同时也促进了表面的高温热稳性。其次调整改性制备条件,考察对整体表面结构变化起的作用,在一定范围内增加焙烧温度、延长浸渍时间、增加浸渍液浓度都对吸附性能的发挥产生有利影响。在此基础之上,利用这两种改性氧化铝对硫化氢进行吸附研究,其吸附穿透效果与改性性能变化情况吻合,说明氧化铝比表面积大小直接影响吸附性能的强弱,Mn-Al2O3吸附能力总体优于La-Al2O3和原态Al2O3。在H2S吸附反应过程中,柱内温度升高对吸附结果产生不利影响,温度越高吸附性能力越低,La-Al2O3在高温下吸附性能相对稳定。此外,H2S与载气混合后的进口体积空速对总体吸附效率影响较大,在2h内空速越大吸附效率越高,对吸附数据进行拟合处理后发现氧化铝吸附反应适合用弗莱德利希形式表达。本文后半部分主要以沸石作为改性材料,研究改性工艺对吸附性能的影响。研究结果发现其改性作用主要依托于对沸石内部硅铝变化引发的骨架调整。本研究采用了酸化浸渍、过渡元素焙烧以及稀土金属焙烧法进行沸石改性制备,经过表面酸性基团的测定,证明酸溶液类型与浸煮强度是酸改性制备工艺中最重要的两个影响因素,而对金属浸渍焙烧影响较大的因素则与氧化铝改性单元相类似,主要区别是浸渍液选择氯化物进行掺杂,所有经过焙烧的沸石中,GZ-Co与GZ-La表面性能提高幅度最大,GZ-La在高温吸附过程中表现稳定。在利用GZ-La对氨气吸附的研究中,总结出空速与进气浓度对吸附穿透效果产生影响的结论,建立了离子交换吸附的微观模型。本文通过对氧化铝和沸石进行改性工艺制备,得到了物性较好的改性吸附剂,并通过对硫化氢和氨气的吸附研究,证明了改性工艺在固体吸附剂领域可以取得更好的发展,在吸附恶臭气体处理方面上提供了新的见解和思路,其研究结果可能在未来在气态污染物治理方向上能够得到更广泛的认可。更多还原

【Abstract】 Human habit has been increasingly polluted and influenced with a rapidly development of industry. Obnoxious gases has gradually become an serious problem which pose a threat to social life quality and public health, especially those emitted from industrial production.In recent years, the increasingly social demand for treatment of oders promoted the development of technologies of control, many noval techniques springs up:ozonization, palsma technology, photocatalytic degradation and so on.Adsorption has been widely used all over the world as its unique physical-chemical feature and simplified operation. Also, some adsorbents are used in treatment of air pollution as its large adsorption capacity.But none of these can carry out with a popuarity in a short time because of the deficiencies. This article introduced Al2O3 and zeolite into adsorption tests as adsorbent, surface modified samples are prepared to remove orders with a higher efficiency.The former half of the article summarizes the composition of adsorbent and the theory of modified adsorption. Modified sample with a better surface Stability, self-adsorb feature, high-temperature impregnation by Mn(NO3)2 and La(NO3)3 are contribute to the better adsorbing performance.SEM and XRD test first shows that modification in micro-structure and increase of specific surface area promote a better adsorption ability and a higher thermo-stability respectively.Secondly, single-factor tests shows that increase in roasting temperature, impregnation time and concentration of impregnation solution in a reasonably extent lead to a advance on adsorption.Based on these, H2S adsorption tests illustrated that adsorption breakthrough effect fits right in with the modification treatment, which further shows that adsorbing functionality is directly attributed to the specific area.High column temperature leads to a negative effect in adsorption while La-Al2O3 perform more steadily in high temperature window.Besides, weight hour space velocity, of mixture of H2S and carrier gas, leads to a higher efficiency with its increase in a 2h extent. Friedrich model can satisfactorily interpret the fitted curve.The later half of this article discusses the influence on adsorption as the modified zeolite is used as a adsorbent Surface acid functional group determination illustrated that the style of acid solution and the strength of digestion plays the most important role in preparation such as acidified impregnation, transition metal digestion and rare metal digestion, using zeolite as the base material.The influence factor on metal- impregnation is similar to the unit of modified Al2O3 while the main difference is caused by chloride in the digestion solution.Preparation by GZ-Co and GZ-La zeolite strengthen the adsorption function mostly while GZ-La perform more steadily in high temperature adsorption.Micro-model of inter-ion exchange adsorption is established through NH3 adsorption by GZ-La, which gives.H2S and NH3 adsorption by satisfied adsorbent, which are prepared by modification of Al2O3 and zeolite, demonstrated that modification can be widely used in the treatment of gases. New viewpoint and thought of gas physical treatment come true, which may be widely adopted.更多还原