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脱砷离子筛的研制及机理初探
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摘要
本文着力于研究与开发对微量砷具有直接净化功能的一类新型生态环境材料即脱砷离子筛,包括:(1)开发两种具有特殊二维结构的新型无机非整比复合物,用化学制筛手段,赋予对特定离子的筛效应与键合能力,使之高效地捕获待净化的有害砷离子,材料具有筛取容量大、深度吸附的特点;(2)所制备材料既可用于饮用水深度脱砷过程,还可用于植物提取物溶液中脱砷过程,可有效脱除复杂体系中存在的微量砷,材料具有抗污染能力强的特点。
     本文对层柱化合物脱砷材料的制备、性能表征、外能注入促进和强化吸附过程及吸附分离微量砷过程中的材料表面物理化学行为进行了较为深入的探索。利用水解法、溶胶凝胶法制备了高吸附性能的钛柱撑蒙脱土和钛柱撑水滑石,分别结合铝镁水滑石、蒙脱土的性能和结构特征,对制备途径进行调变,开展结构设计和吸附性能研究。运用X光电能谱(XPS)、原位红外光谱(FT-IR)、X射线衍射分析(XRD)、透射电子显微镜分析(TEM)及差热分析(DTA)、固体核磁共振谱图分析(NMR)等手段对各种层柱材料的界面性质进行了表征。研究了不同制备条件对钛柱撑蒙脱土和钛柱撑水滑石的结构及对深度吸附水体系中痕、微量砷的影响,系统地研究了钛柱撑蒙脱土和钛柱撑水滑石具有特殊二维结构对微量砷吸附的机理以及不同外能注入强化吸附性能的影响。结果表明,紫外光照射可有效促进材料对微量砷的有效吸附。借助MD模拟手段,对蒙脱石-离子-水体系进行模拟,考察了层间含有不同补偿离子的蒙脱石的膨胀行为,进一步研究了层间物质的结构和运动行为,并探索了层间Na+和Mg2+形成不同扩散行为的原因。借助液相色谱-质谱联用仪等分析手段,对吸附过程前后三七主要成分的指纹图谱进行详细考察。结果表明,脱砷过程不仅有效分离去除有害砷,还可保证三七主要成分不变,实现了三七浸膏的质量控制。
This thesis focused on the investigation and development of the dearsenic ionic sieve, a novel ecotypic and environmental material, which has the function to decontaminate the trace arsenic directly. Two main aspects were included in the thesis. Firstly, two kinds of novel inorganic non-stoichiometric compounds with special planar structure were developed. By the chemical preparation method, the selective separation and bond combination capability of the sieve for the given ions was enhanced. Specially, the prepared sieve can effectively capture the deleterious arsenic ion with high separation capability and deep adsorption. Secondly, the prepared material can not only be used in the deep dearsenic process of the drinking water, but also can be used in the dearsenic process of the lixivium of vegetation. The trace arsenic in the complex systems can be decontaminated effectively and the material has very high resistant ability to the pollutant.
     The preparation of the pillared dearsenic materials, the performance characterization, the enhancement and intensify of the adsorption process by the external introduction of energy and the physical and chemical behaviors on the material surface during the adsorption and separation process of the trace arsenic were investigated systematically in this thesis. The TiO+_2-pillared montmorillonite and the TiO_2-pillared talcum with high adsorption capacity were prepared by hydrolysis and sol-gel methods respectively. According to the properties and the structure characteristic of the aluminium-magnesium talcum and montmorillonite, the preparation procedure and the pillared material were optimized and the relationship between the structure and the performance of the materials was explored. The interface properties of the pillared materials were characterized by XPS, FT-IR, SRD, TEM, DTA and solid NMR. The effects of the preparation conditions on the structures of the TiO2-pillared montmorillonite and the TiO2-pillared talcum and the deep adsorption of the trace arsenic in the water system were investigated. The adsorption mechanism of the trace arsenic for the TiO2-pillared montmorillonite and the TiO2-pillared talcum with special planar structures and the effects of the external introduction of energy on the enhancement of the adsorption were studied systematically. The experimental results indicate that the ultraviolet radiation can effectively enhance the adsorption of trace arsenic. The
引文
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