Amidoxime modified polyacrylonitrile fiber based uranium chelation from wastewater containing uranium in presence of fluoride and chlorine with high concentration

doi:10.11949/j.issn.0438-1157.20171175

CIESC Journal ›› 2018, Vol. 69 ›› Issue (5): 2263-2271.DOI: 10.11949/j.issn.0438-1157.20171175

Amidoxime modified polyacrylonitrile fiber based uranium chelation from wastewater containing uranium in presence of fluoride and chlorine with high concentration

CHENG Yanxia^1,2,3, DONG Faqin², HE Ping¹, NIE Xiaoqin³, CHENG Wencai³, LI Caixia¹, DING Congcong³, HUANG Wenbo³, TAN Zhaoyi⁴, XIAO Xiangzhu⁴

1. School of Materials Science and Engineering, Southwest University of Science and Technology, Mianyang 621010, Sichuan, China;
2. Key Laboratory of Solid Waste Treatment and Resource Recycle, Ministry of Education, Southwest University of Science and Technology, Mianyang 621010, Sichuan, China;
3. Fundamental Science on Nuclear Wastes and Environmental Safety Laboratory, Southwest University of Science and Technology, Mianyang 621010, Sichuan, China;
4. Institute of Nuclear Physics and Chemistry, China Academy of Engineering Physics, Mianyang 621900, Sichuan, China

Received:2017-08-28 Revised:2017-11-29 Online:2018-05-05 Published:2018-05-05
Supported by:
supported by the National Natural Science Foundation of China (41502316), the Post-Doctor Foundation of China and Southwest University of Science and Technology (2017M612991, 16zxy7167), the Military and Civilian Integration of China Academy of Engineering Physics (JM201503) and the Graduate Innovation Foundation of Southwest University of Science and Technology (18ycx064).

高氟高氯含铀废水中偕胺肟基改性聚丙烯腈纤维螯合铀的研究

程艳霞^1,2,3, 董发勤², 何平¹, 聂小琴³, 程文财³, 李彩霞¹, 丁聪聪³, 黄文波³, 谭昭怡⁴, 肖湘竹⁴

1. 西南科技大学材料科学与工程学院, 四川绵阳 621010;
2. 西南科技大学固体废物处理与资源化教育部重点实验室, 四川绵阳 621010;
3. 西南科技大学核废物与环境安全国防重点科学实验室, 四川绵阳 621010;
4. 中国工程物理研究院核物理与化学研究所, 四川绵阳 621900

通讯作者: 董发勤, 何平, 聂小琴
基金资助:
国家自然科学基金项目（41502316）；中国博士后科学基金（2017M612991）；西南科技大学博士后基金（16zxy7167）；中国工程物理研究院军民融合项目基金（JM201503）；西南科技大学研究生创新基金（18ycx064）。

Abstract

Abstract:

Amidoxime modified polyacrylonitrile fiber (AO-PANF) was prepared by reacting polyacrylonitrile fiber (PANF) as fundamental materials with hydroxylamine hydrochloride. The chelation behavior of AO-PANF to uranium from wastewater containing uranium in the presence of fluoride and chlorine with high concentration was investigated by Scanning Electron Microscopy, Fourier Transform Infrared Spectra and batch adsorption. The results showed that nitrile groups were successfully transformed into amidoxime groups by the amidoximation reaction. The conversion rate of nitrile groups increased with the increasing concentration of hydroxylamine hydrochloride. The adsorption quantity of uranium reached up the largest value when the conversion rate of nitrile group was 22.34%. The adsorption quantity of AO-PANF to uranium increased and then decreased with increasing pH, and the maximum adsorption quantity was obtained at pH 5. The concentrations of both F^- and Cl^- have little effect on the adsorption quantity of AO-PANF to uranium. The maximum adsorption quantity of AO-PANF (22.34% conversion rate of nitrile groups) to uranium in 100 ml wastewater (100 mg·L^-1 initial concentration of uranium) was 19.53 mg·g^-1 under the condition of pH 5, 45℃ and 0.40 g adsorbent dose, and the adsorption experiment reached equilibrium after 3 h. AO-PANF adsorbed uranium through chelation between the -NH₂ of amidoxime groups and UO₂F₄^2- of wastewater. The adsorption process conformed to Freundlich isothermal adsorption model and pseudo-second order kinetic equation. It was shown that AO-PANF can effectively extract uranium from wastewater containing uranium in the presence of fluoride and chlorine with high concentration, and has a promising application prospect.

Key words: uranium wastewater, fluoride, chlorine, modification, AO-PANF, chelation

摘要：

以聚丙烯腈纤维（PANF）为基体与盐酸羟胺反应制得偕胺肟基改性纤维（AO-PANF），并通过扫描电镜、红外光谱和批次吸附，探究了AO-PANF对高氟高氯含铀废水中铀的螯合行为。结果表明，偕胺肟化反应将PANF中的氰基成功转化为偕胺肟基团，转化率随盐酸羟胺浓度增加而增大，氰基转化率为22.34%时，AO-PANF对铀的吸附量最大。随废水pH增加，AO-PANF对铀的吸附量先增大后减小，pH为5时，其值最大。F^-和Cl^-浓度变化对AO-PANF的吸附量影响较小。当处理100 ml铀初始浓度为100 mg·L^-1，pH为5的废水，温度为45℃，吸附剂投加量为0.40 g时，转化率为22.34%的AO-PANF对铀的吸附量为19.53 mg·g^-1，3 h左右吸附达到平衡。AO-PANF通过偕胺肟基团中—NH₂与废水中UO₂F₄^2-螯合实现对铀的吸附。该吸附过程符合Freundlich等温吸附模型和准二级动力学方程。研究表明AO-PANF可以有效地螯合高氟高氯含铀废水中的铀，具有良好的应用前景。

关键词: 含铀废水, 氟, 氯, 改性, 偕胺肟基纤维, 螯合

CLC Number:

O642

CHENG Yanxia, DONG Faqin, HE Ping, NIE Xiaoqin, CHENG Wencai, LI Caixia, DING Congcong, HUANG Wenbo, TAN Zhaoyi, XIAO Xiangzhu. Amidoxime modified polyacrylonitrile fiber based uranium chelation from wastewater containing uranium in presence of fluoride and chlorine with high concentration[J]. CIESC Journal, 2018, 69(5): 2263-2271.

程艳霞, 董发勤, 何平, 聂小琴, 程文财, 李彩霞, 丁聪聪, 黄文波, 谭昭怡, 肖湘竹. 高氟高氯含铀废水中偕胺肟基改性聚丙烯腈纤维螯合铀的研究[J]. 化工学报, 2018, 69(5): 2263-2271.

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Amidoxime modified polyacrylonitrile fiber based uranium chelation from wastewater containing uranium in presence of fluoride and chlorine with high concentration

高氟高氯含铀废水中偕胺肟基改性聚丙烯腈纤维螯合铀的研究

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