尉犁水黑云母的间层结构和层间域性质研究
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摘要
新疆尉犁且干布拉克蛭石矿主要由蛭石-云母的规则间层矿物(即水黑云母)所构成。本文在前人对尉犁水黑云母的研究基础上，着重研究了尉犁水黑云母的间层结构特征、不同热处理方法中水黑云母结构的变化、水黑云母的无机阳离子交换性能、有机水黑云母的制备及其特征，以及在有机污染物处理中的应用前景等。这些研究一方面弥补了前人理论研究方面的不足之处，另一方面又为合理开发尉犁水黑云母矿物资源提供理论依据。
对尉犁水黑云母主要红外吸收谱带的归属进行了确认。研究了水黑云母经不同温度热处理后其产物的结构和性质变化。在500℃～600℃，水黑云母失去再水化能力，同时层间阳离子失去可交换性。在800℃～900℃，水黑云母脱去与八面体铁有关的羟基。在900℃～1000℃，水黑云母脱去与八面体镁有关的羟基。在1100℃时，水黑云母开始解体为镁橄榄石等矿物相。通过对不同温度下膨胀水黑云母的体积膨胀倍数的测定、IR和SEM的研究，得出800℃左右的瞬间加热法是制备膨胀水黑云母的最佳条件。
尉犁水黑云母通常含有蛭石和云母分凝相。尉犁水黑云母的X射线衍射特征总体上与国外确定的水黑云母相似，但其d值、变异系数CV、半高宽和衍射强度与完全规则的水黑云母有所差别。本文第一次将图解法运用于蛭石-云母间层结构的研究，指出尉犁水黑云母存在完全规则的水黑云母层与蛭石或云母层不规则间层的现象。用一维傅里叶转换法验证了图解法所得结论的正确性。
对尉犁水黑云母的无机和有机阳离子交换性质进行了研究。研究表明，水黑云母中蛭石晶层的Na~+、Ca~(2+)是可交换的，而云母晶层的K~+基本上是不可交换的。研究了不同层间阳离子对水黑云母层间水赋存状态的影响。随着层间阳离子离子势的增大，其层间水脱失温度增高，层间水的对称伸缩振动频率降低，弯曲振动频率提高。Al~(3+)不遵从上述规律，是因为Al~(3+)的离子势极大，在进入水黑云母层间后发生水解作用所致。
用十六烷基三甲基铵(HDTMA)制备了有机水黑云母。研究了有机水黑云母的基本特征，特别是利用定向片X射线衍射确定了HDTMA在水黑云母层间以倾斜立式方式排列。水黑云母与HDTMA反应存在离子交换和分子吸附两种机制。由于HDTMA以紧密排列方式进入水黑云母层间，因此虽然撑大了水黑云母的层间距，但没有增大其比表面积。
水黑云母对苯酚和氯苯两种非离子型环境污染物没有吸附作用，但经表面活性剂处理后其吸附能力大大增强。有机水黑云母的吸附能力与表面活性剂的类型和层间有机碳含量的多少有关。有机水黑云母对苯酚和氯苯的吸附实际上是苯酚和氯苯在水相与有机水黑云母中有机相之间的一种分配过程，其吸附等温线为直线型。苯酚和氯苯的竞争吸附并未减弱有机水黑云母的吸附能力，反而由于它们同时存在产生协同效应，使有机水黑云母总的吸附能力有所提高。有机水黑云母的这种性质对于处理废水中的多种有机污染物具有重要的实用价值。
Tseganbrark vermiculite deposit in Weili, Xinjiang, is mainly composed of hydrobiotite, a vermiculite-phlogopite interstratified mineral. Following the previous studies on hydrobiotite in Weili, the characteristics of interstratified structure, the variation of structure to different thermal treatment, ion-exchange, preparation and properties of organic-hydrobiotite and the potential of organic polutants disposal are discussed in this paper.
The main IR bands of Weili hydrobiotite has been classified in this paper. The structure and nature of heated hydrobiotite at different temperatures have been studied. At 500℃~600℃, hydrobiotite loses its rehydration property, and the interlayer cations become unexchangeable. The hydroxyls banded to octahedral Fe and Mg dehydrate at 800℃ -900℃ and 900℃ ~ 1000℃ respectively. Hydrobiotite is destroyed to forsterite at 1100℃. According to volume expansion times, IR and SEM study, the most suitable condition in which hydrobiotite expands is sudden thermal treatment at about 800 ℃.
The segregated phases of vermiculite and phlogopite have been found in Weili hydrobiotite. The characteristics of XRD pattern of Weili hydrobiotite is similar to that found in other countries. However, the coefficient of variation of basal spacing, the breadths at half-maximum intensity and peak intensities differentiate Weili hydrobiotite from strictly ordered hydrobiotite. The graphical technique, first used for the interstratified structure of vermiculite and mica in this paper, indicates the presence of random mixing of strictly ordered hydrobiotite layer and vermiculite or mica layer. The Fourier transform demonstrates the efficiency of the graphical technique proposed.
The inorganic and organic ion-exchange have been studied. The Na+ and Ca2+ in the vermiculite interlayer is exchangeable, and K+ in the phlogopite interlayer is unexchangeable. The effects of interlayer cation on the nature of interlayer water have been studied. With the increase of ionic potential, the dehydrated temperature and the bending vibration frequency of interlayer water increase, and strength vibration frequency decreases. Owing to the hydrolysis in the hydrobiotite interlayer, Al3* doesn't abide by the above rule.
The organic-hydrobiotite has been obtained by the treatment of hexatrimethylammonium (HDTMA). The basic characteristics of organic-hydrobiotite have been studied in this paper. Alkylammonium ions form paraffin-type structure in the hydrobiotite interlayer. The interaction of HDTMA with hydrobiotite includes ion-exchange and molecular uptake. As a result of contact arrangement of HDTMA in the interlayer, the BET Specific Surface Area of organic-hydrobiotite doesn't increase although hydrobiotite is expanded by HDTMA.
Hydrobiotite has no adsorption to non-ionic organic contaminants such as phenol and chlorobenzene. However, the HDTMA-modified hydrobiotite has great adsorption to phenol and chlorobenzene. The adsorption depends on the content of organic carbon and the type of surfactant. The adsorption of phenol and chlorobenzene by organic-hydrobiotite is a partition
mechanism between water phase and organic phase in organic-hydrobiotite, and the adsorption isotherm is a linear type. The adsorptive ability of organic-hydrobiotite has been strengthened, not weakened, by the competitive uptake of phenol and chlorobenzene. This property has the practical value when organic-hydrobiotite is used in removal of more than one contaminants from waste water.
对尉犁水黑云母主要红外吸收谱带的归属进行了确认。研究了水黑云母经不同温度热处理后其产物的结构和性质变化。在500℃～600℃，水黑云母失去再水化能力，同时层间阳离子失去可交换性。在800℃～900℃，水黑云母脱去与八面体铁有关的羟基。在900℃～1000℃，水黑云母脱去与八面体镁有关的羟基。在1100℃时，水黑云母开始解体为镁橄榄石等矿物相。通过对不同温度下膨胀水黑云母的体积膨胀倍数的测定、IR和SEM的研究，得出800℃左右的瞬间加热法是制备膨胀水黑云母的最佳条件。
尉犁水黑云母通常含有蛭石和云母分凝相。尉犁水黑云母的X射线衍射特征总体上与国外确定的水黑云母相似，但其d值、变异系数CV、半高宽和衍射强度与完全规则的水黑云母有所差别。本文第一次将图解法运用于蛭石-云母间层结构的研究，指出尉犁水黑云母存在完全规则的水黑云母层与蛭石或云母层不规则间层的现象。用一维傅里叶转换法验证了图解法所得结论的正确性。
对尉犁水黑云母的无机和有机阳离子交换性质进行了研究。研究表明，水黑云母中蛭石晶层的Na~+、Ca~(2+)是可交换的，而云母晶层的K~+基本上是不可交换的。研究了不同层间阳离子对水黑云母层间水赋存状态的影响。随着层间阳离子离子势的增大，其层间水脱失温度增高，层间水的对称伸缩振动频率降低，弯曲振动频率提高。Al~(3+)不遵从上述规律，是因为Al~(3+)的离子势极大，在进入水黑云母层间后发生水解作用所致。
用十六烷基三甲基铵(HDTMA)制备了有机水黑云母。研究了有机水黑云母的基本特征，特别是利用定向片X射线衍射确定了HDTMA在水黑云母层间以倾斜立式方式排列。水黑云母与HDTMA反应存在离子交换和分子吸附两种机制。由于HDTMA以紧密排列方式进入水黑云母层间，因此虽然撑大了水黑云母的层间距，但没有增大其比表面积。
水黑云母对苯酚和氯苯两种非离子型环境污染物没有吸附作用，但经表面活性剂处理后其吸附能力大大增强。有机水黑云母的吸附能力与表面活性剂的类型和层间有机碳含量的多少有关。有机水黑云母对苯酚和氯苯的吸附实际上是苯酚和氯苯在水相与有机水黑云母中有机相之间的一种分配过程，其吸附等温线为直线型。苯酚和氯苯的竞争吸附并未减弱有机水黑云母的吸附能力，反而由于它们同时存在产生协同效应，使有机水黑云母总的吸附能力有所提高。有机水黑云母的这种性质对于处理废水中的多种有机污染物具有重要的实用价值。
Tseganbrark vermiculite deposit in Weili, Xinjiang, is mainly composed of hydrobiotite, a vermiculite-phlogopite interstratified mineral. Following the previous studies on hydrobiotite in Weili, the characteristics of interstratified structure, the variation of structure to different thermal treatment, ion-exchange, preparation and properties of organic-hydrobiotite and the potential of organic polutants disposal are discussed in this paper.
The main IR bands of Weili hydrobiotite has been classified in this paper. The structure and nature of heated hydrobiotite at different temperatures have been studied. At 500℃~600℃, hydrobiotite loses its rehydration property, and the interlayer cations become unexchangeable. The hydroxyls banded to octahedral Fe and Mg dehydrate at 800℃ -900℃ and 900℃ ~ 1000℃ respectively. Hydrobiotite is destroyed to forsterite at 1100℃. According to volume expansion times, IR and SEM study, the most suitable condition in which hydrobiotite expands is sudden thermal treatment at about 800 ℃.
The segregated phases of vermiculite and phlogopite have been found in Weili hydrobiotite. The characteristics of XRD pattern of Weili hydrobiotite is similar to that found in other countries. However, the coefficient of variation of basal spacing, the breadths at half-maximum intensity and peak intensities differentiate Weili hydrobiotite from strictly ordered hydrobiotite. The graphical technique, first used for the interstratified structure of vermiculite and mica in this paper, indicates the presence of random mixing of strictly ordered hydrobiotite layer and vermiculite or mica layer. The Fourier transform demonstrates the efficiency of the graphical technique proposed.
The inorganic and organic ion-exchange have been studied. The Na+ and Ca2+ in the vermiculite interlayer is exchangeable, and K+ in the phlogopite interlayer is unexchangeable. The effects of interlayer cation on the nature of interlayer water have been studied. With the increase of ionic potential, the dehydrated temperature and the bending vibration frequency of interlayer water increase, and strength vibration frequency decreases. Owing to the hydrolysis in the hydrobiotite interlayer, Al3* doesn't abide by the above rule.
The organic-hydrobiotite has been obtained by the treatment of hexatrimethylammonium (HDTMA). The basic characteristics of organic-hydrobiotite have been studied in this paper. Alkylammonium ions form paraffin-type structure in the hydrobiotite interlayer. The interaction of HDTMA with hydrobiotite includes ion-exchange and molecular uptake. As a result of contact arrangement of HDTMA in the interlayer, the BET Specific Surface Area of organic-hydrobiotite doesn't increase although hydrobiotite is expanded by HDTMA.
Hydrobiotite has no adsorption to non-ionic organic contaminants such as phenol and chlorobenzene. However, the HDTMA-modified hydrobiotite has great adsorption to phenol and chlorobenzene. The adsorption depends on the content of organic carbon and the type of surfactant. The adsorption of phenol and chlorobenzene by organic-hydrobiotite is a partition
mechanism between water phase and organic phase in organic-hydrobiotite, and the adsorption isotherm is a linear type. The adsorptive ability of organic-hydrobiotite has been strengthened, not weakened, by the competitive uptake of phenol and chlorobenzene. This property has the practical value when organic-hydrobiotite is used in removal of more than one contaminants from waste water.
引文
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