活性炭吸附放射性废水中U(Ⅵ)的特性研究

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清华大学辅仁网/2017-07-07

于静^1,2, 王建龙^1,3, 蒋翼周²

1. 清华大学核能与新能源技术研究院, 先进核能技术协同创新中心, 北京 100084;
2. 西北核技术研究所, 西安 710024;
3. 清华大学放射性废物处理北京市重点实验室, 北京 100084

Adsorption of uranium (Ⅵ) by activated carbon from radioactive wastewater

YU Jing^1,2, WANG Jianlong^1,3, JIANG Yizhou²

1. Collaborative Innovation Center for Advanced Nuclear Energy Technology, Institute of Nuclear and New Energy Technology, Tsinghua University, Beijing 100084, China;
2. Northwest Institute of Nuclear Technology, Xi'an 710024, China;
3. Beijing Key Laboratory of Radioactive Waste Treatment, Tsinghua University, Beijing 100084, China

摘要:

输出: BibTeX | EndNote (RIS)

摘要该文研究了活性炭对放射性废水中铀的吸附特性, 所研究的影响因素包括接触时间、溶液的pH值pH_a、铀的初始浓度和实验温度。利用能谱扫描电镜(SEM)、透射电镜(TEM)、X射线能谱(EDS)和红外光谱(FTIR)对活性炭的表面物化性质和表面功能团进行了表征。结果表明, 活性炭表面存在羟基官能团并对吸附起重要作用; 吸附反应在30 min内可以达到平衡; pH_a在3~9对吸附影响较大, 在3< pH_a< 5时吸附容量和吸附率增大, 在5< pH_a< 7时吸附容量和吸附率减小, 在7< pH_a< 9时吸附容量和吸附率上升较快; U(Ⅵ)在活性炭上的吸附反应符合Tempkin、Slip和D-R等温模型及准一级动力学方程; 吸附反应是自发放热熵增过程。饱和吸附容量为62.50 mg·g^-1, 吸附率最大为99.23%。

关键词 ：活性炭,U(Ⅵ),吸附,放射性废水

Abstract：The adsorption of uranium from wastewater onto activated carbon was investigated in batch experiments. Four independent variables, the contact time, solution pH_a, initial uranium concentration and temperature, were varied to determine the influence of these parameters on the adsorption of the uranium from water. The activated carbon size were characterized by scanning electron microscopy (SEM) and transmission electron microscopy (TEM), with the element content characterized by energy dispersive X-ray spectrometer (EDS) and surface functional groups characterized by infrared spectrocopy (FTIR). The FTIR spectra indicated that hydroxyl groups are present on the surface of the activated carbon and affected the adsorption. The U(Ⅵ) adsorption onto activated carbon reached sorption equilibrium within 30 min. The adsorption of U(Ⅵ) on activated carbon was strongly dependent on the pH_a in the range of 3.0~9.0. The adsorption capacity and removal percent increase for pH_a from 3 to 5, decrease for pH_a=5~7, and then increase quickly for pH_a=7~9. The U(Ⅵ) adsorption on activated carbon is well described by a pseudo-second-order kinetic model and the Tempkin, Slip, and D-R isotherm models. The sorption reaction is spontaneous, exothermic and increases the entropy. The maxmium adsorption capacity is 62.50 mg·g^-1. The maxmium removal rate is 99.23%.

Key words：activated carbon U(Ⅵ)adsorption radioactive wastewater

收稿日期: 2015-09-14 出版日期: 2016-04-01

ZTFLH:

O615.2

通讯作者:王建龙,教授,E-mail:wangjl@tsinghua.edu.cnE-mail: wangjl@tsinghua.edu.cn

引用本文:

于静, 王建龙, 蒋翼周. 活性炭吸附放射性废水中U(Ⅵ)的特性研究[J]. 清华大学学报（自然科学版）, 2016, 56(3): 312-317.
YU Jing, WANG Jianlong, JIANG Yizhou. Adsorption of uranium (Ⅵ) by activated carbon from radioactive wastewater. Journal of Tsinghua University(Science and Technology), 2016, 56(3): 312-317.

链接本文:

http://jst.tsinghuajournals.com/CN/10.16511/j.cnki.qhdxxb.2016.21.022或 http://jst.tsinghuajournals.com/CN/Y2016/V56/I3/312

图表:

图1　活性炭的SEM 和FEM 照片

表1　活性炭吸附U(Ⅵ)前后的元素质量百分比的EDS测定结果

图2　活性炭吸附U(Ⅵ)前的红外谱图

图3　活性炭吸附U(Ⅵ)后的红外谱图

图4　接触时间对活性炭吸附U(Ⅵ)的影响 (C₀=20mg·L^-1,pH_a=5.0±0.2,T=25℃)

图5　活性炭吸附U(Ⅵ)的准一级、准二级、 Elovich和内扩散动力学模拟结果

表2　动力学模型拟合活性炭吸附U(Ⅵ)的参数值

图6　pHa 对活性炭吸附U(Ⅵ)的影响 (C0=20mg·L^-1,t=12h,T=25℃)

图7　C₀对活性炭吸附U(Ⅵ)的影响 (pH_a=5.0±0.2,t=12h,T=25℃)

图8　活性炭吸附U(Ⅵ)的Langmuir,Freundlich, Temkin,RＧP,Slips,DＧR 等温模式模拟结果

图9　温度对活性炭吸附U(Ⅵ)的影响 (pH_a=5.0±0.2,C₀＝20mg·L^-1,t=12h)

表3　活性炭吸附U(Ⅵ)的热力学拟合参数

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