几种高效除氟吸附剂的颗粒化方法与吸附效果研究
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摘要
论文以实用化的颗粒除氟吸附剂制备为目的,以吸附剂的吸附容量与机械强度为研究目标,通过颗粒海藻酸镧、颗粒铁-镧复合氧化物吸附剂的制备,研究了不同吸附材料与颗粒化方法制备的颗粒吸附剂的除氟作用效果,并对颗粒吸附剂的作用机理进行了系统研究。
通过滴球-交联法制备颗粒海藻酸镧吸附剂,并应用其进行除氟研究,结果显示,颗粒吸附剂的吸附速率快,动力学过程符合拟二级反应方程；其吸附等温线符合Langmuir模型,吸附过程受pH值及SO42-离子干扰较大,最佳吸附pH值为4.0,最大吸附容量可达197.2 mg/g；机理研究显示,该颗粒吸附剂的除氟机理为离子交换作用。该颗粒吸附剂具有很好的机械强度,同时存在较严重的溶胀现象。
对铁镧复合氧化物吸附剂进行了两种颗粒化方法研究。采用挤出法制备的铁镧复合氧化物颗粒吸附剂呈柱状,该颗粒吸附速率较快,动力学过程符合拟一级反应方程；其吸附等温线符合Langmuir模型；pH优化范围5-7；HCO3-与HPO4-对吸附除氟的干扰较大；优化条件下最大吸附量12.1mg/g。连续试验表明,其吸附穿透时间大大高于活性氧化铝,动态吸附量为活性氧化铝的3倍以上。该颗粒吸附剂在水中浸泡后机械强度较差。
采用滴球-交联法制备的铁镧复合氧化物颗粒吸附剂呈球形,颗粒吸附剂的吸附速率快,动力学过程符合拟二级反应方程；其吸附等温线符合Freundlich模型,吸附过程受pH及HPO42-离子干扰较大,最佳吸附pH=4,优化条件下最大吸附容量达30.1mg/g。该吸附剂连续动态吸附效果佳,穿透体积达2326倍,是颗粒活性氧化铝的8-10倍；间歇再生效果较好；同时该吸附剂具有较好的机械强度。
比较研究发现,尽管颗粒海藻酸镧具有很高的吸附容量,但镧元素的含量高,因价格昂贵而应用受到限制；挤出法制备的柱状铁-镧复合氧化物吸附剂,吸附能力尚可,但机械强度较差；而滴球法制备的球形铁-镧复合氧化物颗粒吸附剂,在吸附性能及机械性能等方面均有较好的表现,并通过连续试验运行考核,证明了该吸附剂的有效性。
This paper focuses on the production of practical granular adsorbents for fluoride removal. Adsorption capacity and mechanical strength of granular adsorbent were taken into objective function. Granulation methods, fluoride removal performance as well as the adsorption mechanism of the adsorbent were researched for granular lanthanum alginate and granular iron-lanthanum complex hydroxides adsorbent.
Granular lanthanum alginate was prepared by cross-link method. It was applied in fluoride removal and the results showed that the adsorption rate is fast and the adsorption kinetics was in accordance with second order reaction rate equation; the adsorption isotherm fitted Langmuir equation well; the adsorption process was mainly affected by pH and SO42-; the optimal pH was 4.0 and the maximum adsorption capacity was 197.2 mg/g. The adsorption mechanism of lanthanum alginate was ion exchange as seen from the studies. These adsorbents had good mechanical strength but could cause significant swelling.
Granular iron-lanthanum complex hydroxides adsorbent was prepared using two methods, namely:extrusion and dropping method. Granular iron-lanthanum complex hydroxides adsorbent prepared by extrusion method was in bar shape. It adsorption rate was fast and the adsorption kinetics was in accordance with first order reaction rate equation; the adsorption isotherm fitted Langmuir equation well; the optimal pH range was 5-7, the maximum adsorption capacity was 12.1 mg/g at the optimal conditions. HCO3- and HPO42-affected the adsorption process largely. In column test the breakthrough volume of our adsorbent was much higher than that of activated alumina; the dynamic adsorption capacity was over 3 times of that of activated alumina. But the adsorbent's mechanical strength reduced a lot when soaked in water for a long time.
Granular iron-lanthanum complex hydroxides adsorbent prepared by dropping method was in ball shape. Its adsorption rate was fast and the adsorption kinetics was in accordance with second order reaction rate equation; the adsorption isotherm fitted Langmuir equation well; adsorption process was maily affected by pH and SO42-, the optimal pH was 4, the maximum adsorption capacity was 30.1 mg/g on the optimal conditions. In column test breakthrough volume was 2326, which is 8-10 times of that of activated alumina. The adsorbent had good mechanical strength.
Studies showed that granular lanthanum alginate had high adsorption capacity, but with high lanthanum element content, which lead to high application price. Granular iron-lanthanum complex hydroxides adsorbent prepared by extrusion method wasn't suitable for application because of its poor mechanical strength. Granular iron-lanthanum complex hydroxides adsorbent prepared by dropping method had good adsorption capacity and mechanical strength, so it had the potential of application.
通过滴球-交联法制备颗粒海藻酸镧吸附剂,并应用其进行除氟研究,结果显示,颗粒吸附剂的吸附速率快,动力学过程符合拟二级反应方程；其吸附等温线符合Langmuir模型,吸附过程受pH值及SO42-离子干扰较大,最佳吸附pH值为4.0,最大吸附容量可达197.2 mg/g；机理研究显示,该颗粒吸附剂的除氟机理为离子交换作用。该颗粒吸附剂具有很好的机械强度,同时存在较严重的溶胀现象。
对铁镧复合氧化物吸附剂进行了两种颗粒化方法研究。采用挤出法制备的铁镧复合氧化物颗粒吸附剂呈柱状,该颗粒吸附速率较快,动力学过程符合拟一级反应方程；其吸附等温线符合Langmuir模型；pH优化范围5-7；HCO3-与HPO4-对吸附除氟的干扰较大；优化条件下最大吸附量12.1mg/g。连续试验表明,其吸附穿透时间大大高于活性氧化铝,动态吸附量为活性氧化铝的3倍以上。该颗粒吸附剂在水中浸泡后机械强度较差。
采用滴球-交联法制备的铁镧复合氧化物颗粒吸附剂呈球形,颗粒吸附剂的吸附速率快,动力学过程符合拟二级反应方程；其吸附等温线符合Freundlich模型,吸附过程受pH及HPO42-离子干扰较大,最佳吸附pH=4,优化条件下最大吸附容量达30.1mg/g。该吸附剂连续动态吸附效果佳,穿透体积达2326倍,是颗粒活性氧化铝的8-10倍；间歇再生效果较好；同时该吸附剂具有较好的机械强度。
比较研究发现,尽管颗粒海藻酸镧具有很高的吸附容量,但镧元素的含量高,因价格昂贵而应用受到限制；挤出法制备的柱状铁-镧复合氧化物吸附剂,吸附能力尚可,但机械强度较差；而滴球法制备的球形铁-镧复合氧化物颗粒吸附剂,在吸附性能及机械性能等方面均有较好的表现,并通过连续试验运行考核,证明了该吸附剂的有效性。
This paper focuses on the production of practical granular adsorbents for fluoride removal. Adsorption capacity and mechanical strength of granular adsorbent were taken into objective function. Granulation methods, fluoride removal performance as well as the adsorption mechanism of the adsorbent were researched for granular lanthanum alginate and granular iron-lanthanum complex hydroxides adsorbent.
Granular lanthanum alginate was prepared by cross-link method. It was applied in fluoride removal and the results showed that the adsorption rate is fast and the adsorption kinetics was in accordance with second order reaction rate equation; the adsorption isotherm fitted Langmuir equation well; the adsorption process was mainly affected by pH and SO42-; the optimal pH was 4.0 and the maximum adsorption capacity was 197.2 mg/g. The adsorption mechanism of lanthanum alginate was ion exchange as seen from the studies. These adsorbents had good mechanical strength but could cause significant swelling.
Granular iron-lanthanum complex hydroxides adsorbent was prepared using two methods, namely:extrusion and dropping method. Granular iron-lanthanum complex hydroxides adsorbent prepared by extrusion method was in bar shape. It adsorption rate was fast and the adsorption kinetics was in accordance with first order reaction rate equation; the adsorption isotherm fitted Langmuir equation well; the optimal pH range was 5-7, the maximum adsorption capacity was 12.1 mg/g at the optimal conditions. HCO3- and HPO42-affected the adsorption process largely. In column test the breakthrough volume of our adsorbent was much higher than that of activated alumina; the dynamic adsorption capacity was over 3 times of that of activated alumina. But the adsorbent's mechanical strength reduced a lot when soaked in water for a long time.
Granular iron-lanthanum complex hydroxides adsorbent prepared by dropping method was in ball shape. Its adsorption rate was fast and the adsorption kinetics was in accordance with second order reaction rate equation; the adsorption isotherm fitted Langmuir equation well; adsorption process was maily affected by pH and SO42-, the optimal pH was 4, the maximum adsorption capacity was 30.1 mg/g on the optimal conditions. In column test breakthrough volume was 2326, which is 8-10 times of that of activated alumina. The adsorbent had good mechanical strength.
Studies showed that granular lanthanum alginate had high adsorption capacity, but with high lanthanum element content, which lead to high application price. Granular iron-lanthanum complex hydroxides adsorbent prepared by extrusion method wasn't suitable for application because of its poor mechanical strength. Granular iron-lanthanum complex hydroxides adsorbent prepared by dropping method had good adsorption capacity and mechanical strength, so it had the potential of application.
引文
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