两性有机修饰土的表面特性、稳定性特征及其影响因素的研究
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摘要
土壤中有机、重金属的污染是土壤污染的主要形式,研究如何防止和控制有机污染物和重金属污染物在土壤中的迁移、转化,并对污染土壤进行修复已经成为研究的热点。两性表面修饰土由于其结构上的特殊性而具有同时修复土壤中有机、重金属的复合污染的能力,但当前的研究主要集中在对污染物吸附能力的研究上,而对于土壤与两性表面修饰剂反应及其效应的研究目前尚未见到报道。在当前有机物、重金属污染日趋严重的环境下,对两性修饰土进行理论和应用上的深入研究,对于保护生态环境和人体健康具有重要意义。
本文在前期研究工作基础上,以陕西关中地区塿土和广州市郊稻田红壤作为供试土样,系统地研究了两性修饰剂与土壤表面的反应特征,两性修饰土制备时各种因素对两性修饰土表面特性的影响规律,以及不同因素对有机修饰土稳定性的影响规律。本研究首次提出了两性修饰剂BS-12分子在土样表面上的吸附同时存在电荷引力和疏水胶团两种形式,且以疏水胶团吸附型式为主的机制;发现了土样制备时修饰比例是影响表面特性的最主要影响因素;揭示了不同影响因素对两性修饰土稳定性的影响规律。研究得到主要结论如下:
1在塿土和红壤土样中,BS-12吸附等温线均呈现L型,属于多层吸附型式。塿土中BS-12的吸附在低修饰比例阶段表现为温度的负效应,高修饰比例阶段表现为温度正效应。红壤中BS-12的吸附则表现为温度的正效应。在低修饰比例时,塿土表面BS-12以静电吸附为主,而红壤表面BS-12以化学吸附为主。在高修饰比例时,塿土和红壤表面均已形成BS-12分子胶束,以胶束形式吸附。
2两性修饰塿土和红壤的表观CEC、CEC8.2、CECp均小于相应的未修饰土样,随着修饰比例的增加和土壤制备温度的升高,两种修饰土样的表观CEC、CEC8.2、CECp逐渐下降,而CECv呈增加趋势,AEC则变化不大。土样制备时土壤粒径、离子强度对两种修饰土样的CEC影响不大。pH对修饰红壤表观CEC影响不大,但却使修饰塿土的表观CEC在pH6以前下降,pH>6后趋于不变。土样制备时土壤粒径、pH、离子强度均不影响修饰塿土的电荷特征,但pH、离子强度均使红壤的CEC8.2、CECp上升。塿土修饰土样的比表面均高于原土的比表面,并随修饰比例的增加呈现先增加后减小的趋势,红壤则相反;土样制备时温度、pH、离子强度对两种修饰土样的比表面影响不大,但土壤粒径具有较大影响,随土壤粒径的增加,修饰塿土的比表面呈减小的趋势,而修饰红壤则相反。
3 BS-12解吸量随修饰比例的增加而呈线性增加,BS-12相对解吸率受修饰比例的影响不大。随pH上升,修饰塿土BS-12的解吸量先下降而后趋于不变,而修饰红壤BS-12解吸量不受解吸液pH值的影响。解吸液浓度的增加,修饰塿土和红壤的BS-12解吸量均呈现先增加,而后当解吸液达到一定浓度时,BS-12解吸量与解吸液浓度无关的变化规律。
4 BS-12与两种土壤的反应机制、制备条件对两性修饰土样表面特征的影响规律以及不同影响因素对两性修饰土稳定性的影响的研究结果,共同证实了BS-12分子在土样表面上的吸附同时存在电荷引力和疏水胶团两种形式,且以疏水胶团吸附型式为主。
Using Lou soil in Shaanxi and Red soil in Guangdong as sample, the systematic studies on the surface characteristics, stability and their affecting factors of soil modified with Duodalkylbetaine (BS-12) were conducted. The conclusions are showed as follows:
1 The adsorption isotherm of BS-12 on both Lou soil and Red soil at 20℃and 40℃are L type, implied a multi-layer adsorption models is existed. The BET model is the best model for describing the BS-12 adsorption. In the region of low modification ratio of modified lou soil, temperature has the negative effect on the BS-12 adsorption amount, which are in the way of electrostatic abstraction. In the region of red modification ratio of modified red soil, BS-12 adsorption amount are in the way of chemical adsorption. In the high regin of modification ratio, the adsorption amount has the positive effect on the temperature, which are in the way of micelles forms adsorption.
2 All the CEC, CEC8.2 and CECp of modified lou and red soil are lower than that of original soil. With the increase of modified ratio, the CEC, and CEC8.2 and CECp decrease, while the CECv increase. When the pH is between 4 and 6, the pH has relation with modified Lou soil CEC, while the pH is between 4 and 8, pH has no effect on CEC of modified Red soil. The ionic strength and the particle size don’t affect the CEC of modified soil. The specific surface area(SSA) of modified lou soil is higher than that of original lou soil, while SSA of modified red soil is lower than that of original red soil. With an increase of particle size of modified soil, SSA of modified soil is decreased. In addition to particle size, other factors have little effect on the specific surface area. When the modified ratio and the temperature of preparing modified soil increase, the CEC8.2 and CECp decrease, but the CECv increase. The ionic strength, the temperature and pH have little effect on the AEC of modified Lou soil. The AEC of modified red soil decrease with the pH value increase.
3 The desorption isotherm of BS-12 show a linear relationship. The modified ratios have little effect on relative desorption retio of BS-12 on both modified lou and red soil. The temperature has the positive effect on the desorption of BS-12. When the concentration of CaCl2 is higher than 0.05mol·L-1,the ionic strength has no effect on the desorption of BS-12.
4 The results of the adsorption of BS-12 on soil show that there are two mechanisms, elecrostatics adsoption and micelles forms adsorption, in which the micelles forms adsorption is a controll mechanism.
本文在前期研究工作基础上,以陕西关中地区塿土和广州市郊稻田红壤作为供试土样,系统地研究了两性修饰剂与土壤表面的反应特征,两性修饰土制备时各种因素对两性修饰土表面特性的影响规律,以及不同因素对有机修饰土稳定性的影响规律。本研究首次提出了两性修饰剂BS-12分子在土样表面上的吸附同时存在电荷引力和疏水胶团两种形式,且以疏水胶团吸附型式为主的机制;发现了土样制备时修饰比例是影响表面特性的最主要影响因素;揭示了不同影响因素对两性修饰土稳定性的影响规律。研究得到主要结论如下:
1在塿土和红壤土样中,BS-12吸附等温线均呈现L型,属于多层吸附型式。塿土中BS-12的吸附在低修饰比例阶段表现为温度的负效应,高修饰比例阶段表现为温度正效应。红壤中BS-12的吸附则表现为温度的正效应。在低修饰比例时,塿土表面BS-12以静电吸附为主,而红壤表面BS-12以化学吸附为主。在高修饰比例时,塿土和红壤表面均已形成BS-12分子胶束,以胶束形式吸附。
2两性修饰塿土和红壤的表观CEC、CEC8.2、CECp均小于相应的未修饰土样,随着修饰比例的增加和土壤制备温度的升高,两种修饰土样的表观CEC、CEC8.2、CECp逐渐下降,而CECv呈增加趋势,AEC则变化不大。土样制备时土壤粒径、离子强度对两种修饰土样的CEC影响不大。pH对修饰红壤表观CEC影响不大,但却使修饰塿土的表观CEC在pH6以前下降,pH>6后趋于不变。土样制备时土壤粒径、pH、离子强度均不影响修饰塿土的电荷特征,但pH、离子强度均使红壤的CEC8.2、CECp上升。塿土修饰土样的比表面均高于原土的比表面,并随修饰比例的增加呈现先增加后减小的趋势,红壤则相反;土样制备时温度、pH、离子强度对两种修饰土样的比表面影响不大,但土壤粒径具有较大影响,随土壤粒径的增加,修饰塿土的比表面呈减小的趋势,而修饰红壤则相反。
3 BS-12解吸量随修饰比例的增加而呈线性增加,BS-12相对解吸率受修饰比例的影响不大。随pH上升,修饰塿土BS-12的解吸量先下降而后趋于不变,而修饰红壤BS-12解吸量不受解吸液pH值的影响。解吸液浓度的增加,修饰塿土和红壤的BS-12解吸量均呈现先增加,而后当解吸液达到一定浓度时,BS-12解吸量与解吸液浓度无关的变化规律。
4 BS-12与两种土壤的反应机制、制备条件对两性修饰土样表面特征的影响规律以及不同影响因素对两性修饰土稳定性的影响的研究结果,共同证实了BS-12分子在土样表面上的吸附同时存在电荷引力和疏水胶团两种形式,且以疏水胶团吸附型式为主。
Using Lou soil in Shaanxi and Red soil in Guangdong as sample, the systematic studies on the surface characteristics, stability and their affecting factors of soil modified with Duodalkylbetaine (BS-12) were conducted. The conclusions are showed as follows:
1 The adsorption isotherm of BS-12 on both Lou soil and Red soil at 20℃and 40℃are L type, implied a multi-layer adsorption models is existed. The BET model is the best model for describing the BS-12 adsorption. In the region of low modification ratio of modified lou soil, temperature has the negative effect on the BS-12 adsorption amount, which are in the way of electrostatic abstraction. In the region of red modification ratio of modified red soil, BS-12 adsorption amount are in the way of chemical adsorption. In the high regin of modification ratio, the adsorption amount has the positive effect on the temperature, which are in the way of micelles forms adsorption.
2 All the CEC, CEC8.2 and CECp of modified lou and red soil are lower than that of original soil. With the increase of modified ratio, the CEC, and CEC8.2 and CECp decrease, while the CECv increase. When the pH is between 4 and 6, the pH has relation with modified Lou soil CEC, while the pH is between 4 and 8, pH has no effect on CEC of modified Red soil. The ionic strength and the particle size don’t affect the CEC of modified soil. The specific surface area(SSA) of modified lou soil is higher than that of original lou soil, while SSA of modified red soil is lower than that of original red soil. With an increase of particle size of modified soil, SSA of modified soil is decreased. In addition to particle size, other factors have little effect on the specific surface area. When the modified ratio and the temperature of preparing modified soil increase, the CEC8.2 and CECp decrease, but the CECv increase. The ionic strength, the temperature and pH have little effect on the AEC of modified Lou soil. The AEC of modified red soil decrease with the pH value increase.
3 The desorption isotherm of BS-12 show a linear relationship. The modified ratios have little effect on relative desorption retio of BS-12 on both modified lou and red soil. The temperature has the positive effect on the desorption of BS-12. When the concentration of CaCl2 is higher than 0.05mol·L-1,the ionic strength has no effect on the desorption of BS-12.
4 The results of the adsorption of BS-12 on soil show that there are two mechanisms, elecrostatics adsoption and micelles forms adsorption, in which the micelles forms adsorption is a controll mechanism.
引文
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