铀(Ⅵ)在氧化锌修饰聚丙烯腈纤维上的吸附行为

doi:10.11896/cldb.18040272

材料导报

2019, Vol. 33

Issue (14): 2436-2443 https://doi.org/10.11896/cldb.18040272

高分子与聚合基复合材料

铀(Ⅵ)在氧化锌修饰聚丙烯腈纤维上的吸附行为

黄国庆^1,2, 白震媛¹, 陈兆文², 刘琦¹, 王君¹

1 哈尔滨工程大学材料科学与化学工程学院,哈尔滨 150001;
2 中国船舶重工集团公司第七一八研究所,邯郸 056027

Adsorption Behavior of Uranium(Ⅵ) on Zinc Oxide-modified Polyacrylonitrile Fibers

HUANG Guoqing^1,2, BAI Zhenyuan¹, CHEN Zhaowen², LIU Qi¹, WANG Jun¹

1 College of Materials Science and Chemical Engineering, Harbin Engineering University, Harbin 150001;
2 The 718^th Research Institute of CSIC, Handan 056027

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摘要本研究通过溶剂热自组装将氧化锌(ZnO)纳米棒阵列原位生长在聚丙烯腈纤维(PANF)表面,成功合成ZnO/PANF复合材料。ZnO的引入有效地增加了PANF表面的活性位点,从而改善了纯PANF吸附容量小的问题。采用扫描电子显微镜对材料形貌进行表征,并开展一系列静态吸附实验,研究了铀溶液的pH值、初始浓度、吸附时间及温度等因素对U(Ⅵ)吸附的影响。ZnO/PANF复合材料对U(Ⅵ)的饱和吸附量可达248.14 mg·g^-1(298.15 K,pH=6.0,C₀=200 mg· L^-1,t=180 min),符合准二级动力学模型以及Langmuir等温吸附模型,且吸附是一个吸热、自发过程;通过离子竞争实验以及循环吸脱附实验,验证了ZnO/PANF复合材料具有良好的选择性和循环利用率。值得注意的是,ZnO/PANF复合材料对低浓度铀的去除率可达89%,在真实海水以及模拟受放射性废物污染的海水中,ZnO/PANF复合材料对铀的去除率也均能达到45%以上,证明该吸附剂在海水提铀领域的潜在能力。通过IR和XPS证明该复合材料主要是通过表面的-COOH以及Zn-O中的含氧基团实现对U(Ⅵ)的吸附。

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	黄国庆
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关键词: 低浓度铀氧化锌聚丙烯腈纤维吸附

Abstract: In this study, the ZnO/PANF adsorbent was successfully synthesized by solvothermal self-assembly. The zinc oxide (ZnO) nanorod arrays were grown in situ on polyacrylonitrile fiber (PANF) surface. Due to the introduction of ZnO, the adsorbent effectively increases the active sites on the PANF surface, thereby improving the adsorption capacity of pure PANF. The scanning electron microscopy was used to characterize the material morphology. A series of batch adsorption experiments were carried out to study the effects of pH value and initial concentration of uranium solution, contact time and temperature on the adsorption of U (Ⅵ). The results showed that the optimal adsorption amount of U(Ⅵ) of ZnO/PANF adsorbent was 248.14 mg· g^-1 at 298.15 K, pH=6, C₀=200 mg· L^-1, and t=180 min, which is consistent with the pseudo-se-cond-order kinetics model and the Langmuir isotherm model. The adsorption is an endothermic and spontaneous process. The adsorbent exhibits excellent ion selectivity and cycle reproducibility. It is worth noting that the removal efficiency of ZnO/PANF composites for low-concentration uranium is 89% and for real seawater and simulated seawater contaminated by radioactive waste can also reach more than 45%, demonstrating the potential of the adsorbent in the field of uranium extraction from seawater. Furthermore, the adsorption mechanisms of U(Ⅵ) by ZnO/PANF was detailed conducted by IR and XPS analysis, and could be ascribed to the oxygen-containing groups of -COOH and Zn-O.

Key words: low concentration uranium zinc oxide polyacrylonitrile fiber adsorption

发布日期: 2019-06-19

ZTFLH:

TQ424

基金资助: 国家自然科学基金(NSFC 51603053);黑龙江省应用技术研究与开发计划国家项目省级资助(GX16A009);哈尔滨市应用技术研究与开发基金(2015RAQXJ038)

通讯作者: zhqw1888@sohu.com

作者简介: 黄国庆,中船重工第七一八研究所高级工程师。2010年9月至2014年1月,在吉林大学获得微电子学与固体电子学博士,毕业后到中船重工第七一八研究所工作。以第一作者在国外期刊发表论文2篇,申请国家发明专利5篇,其中授权专利3项。研究工作主要围绕先进功能材料和海水提铀方面。王君,哈尔滨工程大学教授,博士研究生导师。1996年毕业于吉林大学化学系物理化学专业,获理学学士学位。2007年毕业于哈尔滨工程大学材料学专业,获工学博士学位。以第一/通讯作者在国际知名刊物发表SCI检索论文200余篇,其中6篇论文被评为ESI高被引论文,1篇被评为热点论文;获授权国家发明专利26项。其团队主要研究方向包括:海洋中低浓度铀富集与分离纯化;长效海洋防污涂料开发与工程化应用;仿生功能材料设计与性能研究。

引用本文:

黄国庆, 白震媛, 陈兆文, 刘琦, 王君. 铀(Ⅵ)在氧化锌修饰聚丙烯腈纤维上的吸附行为[J]. 材料导报, 2019, 33(14): 2436-2443.
HUANG Guoqing, BAI Zhenyuan, CHEN Zhaowen, LIU Qi, WANG Jun. Adsorption Behavior of Uranium(Ⅵ) on Zinc Oxide-modified Polyacrylonitrile Fibers. Materials Reports, 2019, 33(14): 2436-2443.

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http://www.mater-rep.com/CN/10.11896/cldb.18040272 或 http://www.mater-rep.com/CN/Y2019/V33/I14/2436

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