【作者】 张涛；

【导师】 董岁明；

【作者基本信息】 长安大学 ， 应用化学， 2018， 硕士

【摘要】 高氟水广泛分布于全球范围内,中国也是高氟水受害较为严重的国家之一,长期饮用高氟水对人体健康危害很大,在水资源日益短缺的今天,对高氟劣质水的处理就显得尤为重要。为探究对高氟劣质水中氟离子的去除方法和途径,本文制备了三种生物活性炭并对其进行了改性,制得了三种改性生物活性炭除氟材料,并对它们的除氟性能进行了研究。研究内容如下:（1）铁离子改性猪粪炭的制备及其除氟性能以猪粪为原材料,高温焙烧制得生物活性炭（ZC）,ZC浸渍Fe³⁺后制得铁改性生物活性炭（Fe-ZC）。并对Fe-ZC的结构和形貌进行了SEM和FTIR的表征,研究了Fe-ZC的除氟性能,并从理论上对其等温吸附的动力学特征进行了探讨。结果表明:吸附时间为120min、pH为7、投加量为24g/L时,对高氟劣质水中氟离子的去除率达到90%以上。其中,CO₃^2-、HCO₃^-、PO₄^3-对除氟效果的影响显著,影响大小为CO₃^2->HCO₃^->PO₄^3-。Fe-ZC对氟离子的吸附过程为准二级动力学方程,符合Langmuir型等温模型。（2）氧化铝改性猕猴桃枝炭的制备及其除氟性能以猕猴桃枝为原料,高温焙烧制得生物活性炭（MC）,MC浸渍三氯化铝溶液,然后300℃下加热2h制得载铝生物活性炭（Al-MC）。对Al-MC的结构和形貌进行了SEM和FTIR的表征。探讨了其制备条件。研究表明,当AlCl₃浓度为0.3mol/L,加热温度为300℃时制得的材料除氟效果最佳。同时,研究了投加量、初始浓度、pH值、时间以及共存离子对氟离子去除性能的影响。单因素试验表明:初始浓度和pH值对氟离子的去除率有较大影响,CO₃^2-、HCO₃^-、PO₄^3-对除氟效果的影响大小为CO₃^2->HCO₃^->PO₄^3-。响应面试验表明:氟离子的吸附量与因素之间的函数关系可以用回归方程拟合,因素影响大小为:初始浓度>pH值>投加量;优化得到氟离子吸附的最佳条件为Al-MC投加量为0.3g,初始浓度为15mg/L,pH值为7时,吸附量可达到18.83mg/g。（3）硝酸镧改性竹炭的制备及其除氟性能以竹屑为原料,高温焙烧制得生物活性炭（ZuC）,ZuC浸渍硝酸镧溶液制得载镧生物活性炭（La-ZuC）,对La-ZuC的结构和形貌进行了SEM和FTIR的表征。在室温下,研究了吸附时间、pH值、投加量及初始浓度对氟离子去除性能的影响。单因素试验表明:吸附平衡时间为120min,当含氟劣质水的浓度为5mg/L时,除氟率达到98.6%。25mg/L时除氟率下降到35.12%,而吸附量则增加到29.27 mg/g。HCO₃^-、CO₃^2-、PO₄^3-对除氟效果的影响大小为CO₃^2->HCO₃^->PO₄^3-。就投加量、初始浓度、pH值、时间4个因素对含氟劣质水中氟离子吸附量的影响进行正交试验。4个因素对氟离子吸附量的影响大小依次为初始浓度、投加量、pH值、时间。最佳吸附条件为:pH值为7,初始浓度为15mg/L,投加量为0.3g。在此条件下,La-ZuC对氟离子吸附量可达到12.65mg/g。更多还原

【Abstract】 High-fluorine water is widely distributed in the world,and china is also one of the countries where high-fluorine water is more seriously damaged.It is harmful to human health if people drink high-fluorine water for long time.In today’s increasingly scarce water resources,it is particularly important to treatment of high-fluorine water.In order to explore the treatment of fluoride ion in high-fluorine inferior water,the three biological activated carbons prepared were modified to obtain three modified biological fluoride removal materials,and their fluoride removal performance was studied.The specific research content is as follows:（1）Preparation of iron-modified pig manure and its fluoride removal performanceThe pig manure was used as raw material,biological activated carbon（ZC）was prepared by high-temperature calcination,and iron modified biological activated carbon（Fe-ZC）was prepared after ZC impregnated Fe³⁺.The SEM and FTIR were used to characterize the structure and morphology of Fe-ZC.The defluoridation performance of Fe-ZC was studied,and the kinetic characteristics of the isothermal adsorption were discussed theoretically.The results showed that when the adsorption time was 120min,the pH was 7 and the dosage was24g/L,the removal rate of fluoride ion in high-quality fluoride water was over 90%.Among them,CO₃^2-,HCO₃^-,PO₄^3-have a significant effect on the effect of fluoride removal,and the effect size is CO₃^2->HCO₃^->PO₄^3-.The adsorption process of Fe-ZC on fluoride ion is a quasi-second-order kinetic equation,which is in accordance with the Langmuir isothermal model.（2）Preparation of alumina modified kiwifruit carbon and its fluoride removal performanceUsing kiwifruit as raw material,high-temperature roasting to obtain biological activated carbon（MC）,MC was impregnated with aluminum chloride solution,and then heating at300°C for 2h to obtain aluminum-loaded biological activated carbon（Al-MC）.The structure and morphology of Al-MC were characterized by SEM and FTIR.The preparation conditions were discussed.The studies have shown that when the AlCl₃ concentration is 0.3mol/L and the heating temperature is 300°C,the obtained material has the best fluoride removal effect.At the same time,the effects of dosage,initial concentration,pH value,time and coexisting ions on fluoride ion removal performance were studied.Single factor tests showed that the initial concentration and pH value had a great influence on the removal rate of fluoride ions.The effects of HCO₃^-,CO₃^2-,and PO₄^3-on fluoride removal were CO₃^2->HCO₃^->PO₄^3-.The response surface test showed that the functional relationship between fluoride ion adsorption capacity and factors can be fitted by regression equation.The factors affecting size are:initial concentration>pH value>dosing amount;the optimal condition for obtaining fluoride ion adsorption is that when the amount of Al-MC added was 0.3 g,the initial concentration was15 mg/L,and the pH was 7,the amount of adsorption was 18.83 mg/g.（3）Preparation of cerium nitrate modified bamboo charcoal and its fluoride removal performanceBioactive activated carbon（ZuC）was prepared from bamboo shavings as a raw material by high-temperature calcination,and La-ZuC bioactive activated carbon（La-ZuC）was prepared by impregnating thorium nitrate with zirconium.The structure and morphology of La-ZuC were characterized by SEM and FTIR.At room temperature,the effects of adsorption time,pH value,dosage and initial concentration on the fluoride ion removal performance were studied.The single factor test showed that the adsorption equilibrium time was 120 minutes.When the concentration of fluorine-containing inferior water was 5 mg/L,the fluorine removal rate was 98.6%.At 25 mg/L,the fluorine removal rate decreased to 35.12%,while the adsorption capacity increased to 29.27 mg/g.The effects of HCO₃^-,CO₃^2-,and PO₄^3-on fluoride removal were CO₃^2->HCO₃^->PO₄^3-.The effects of four factors,such as dosage,initial concentration,pH,and time,on the adsorption capacity of fluoride ions in poor-quality water were orthogonally tested.The influence of the four factors on the amount of fluoride adsorption was the initial concentration,dosage,pH,and time.The optimum adsorption conditions was that:pH was 7,initial concentration was 15 mg/L,dosage was 0.3 g.Under this condition,the fluoride adsorption capacity of La-ZuC can reach 12.65mg/g.更多还原