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使用异硫脲盐功能化的埃洛石作为有机/无机杂化吸附剂去除铀(VI)离子。

The use of halloysite functionalized with isothiouronium salts as an organic/inorganic hybrid adsorbent for uranium(VI) ions removal.

作者信息

Gładysz-Płaska A, Majdan M, Tarasiuk B, Sternik D, Grabias E

机构信息

Maria Curie Skłodowska University, Faculty of Chemistry, 2 M. Curie Skłodowska Sq., 20-031 Lublin, Poland.

Maria Curie Skłodowska University, Faculty of Chemistry, 2 M. Curie Skłodowska Sq., 20-031 Lublin, Poland.

出版信息

J Hazard Mater. 2018 Jul 15;354:133-144. doi: 10.1016/j.jhazmat.2018.03.057. Epub 2018 Apr 21.

DOI:10.1016/j.jhazmat.2018.03.057
PMID:29747148
Abstract

Elimination of U(VI) from nuclear wastes and from the underground water near the uranium mines is the serious problem. Therefore search for new sorbents for U(VI) is still a big challenge for the scientists. This paper investigates of U(VI) ions sorption on halloysite modified with the isothiouronium salts: S-dodecaneisothiouronium bromide (ligand 1), S,S'-dodecane-1,12-diylbis(isothiouronium bromide) (ligand 2), S-hexadecaneisothiouronium chloride (ligand 3), S,S'-naphthalene-1,4-diylbis(methylisothiouronium) dichloride (ligand 4), and S,S'-2,5-dimethylbenzene-1,4-diylbis(methylisothiouronium) dichloride (ligand 5). It was established that halloysite modified by the ligands with four nitrogen atoms in their structure (ligand-5, 2 and 4) was characterized by higher sorption capacity compared with that modified by the ligands with two donor nitrogens (ligand-1 and 3). The maximum sorption capacity of halloysite-5 toward U(VI) was 157 mg U/g and this places the modified mineral among the most effective sorbents for U(VI) removal from wastes. As follows from ATR, XPS and thermal degradation spectra of the sorption products R-S-C(NH)(NH) complexes are formed on the external surface of the halloysite whereas oligomeric hydroxy complexes (UO)(OH) and (UO)(OH) are present in the interior of halloysite structure and interact predominantly with aluminols.

摘要

从核废料以及铀矿附近的地下水中去除U(VI)是一个严峻的问题。因此,寻找新型U(VI)吸附剂对科学家来说仍然是一个巨大的挑战。本文研究了用异硫脲鎓盐改性的埃洛石对U(VI)离子的吸附作用:S-十二烷基异硫脲溴化物(配体1)、S,S'-十二烷-1,12-二基双(异硫脲溴化物)(配体2)、S-十六烷基异硫脲氯化物(配体3)、S,S'-萘-1,4-二基双(甲基异硫脲)二氯化物(配体4)以及S,S'-2,5-二甲基苯-1,4-二基双(甲基异硫脲)二氯化物(配体5)。结果表明,结构中含有四个氮原子的配体(配体-5、2和4)改性的埃洛石,与含有两个供体氮的配体(配体-1和3)改性的埃洛石相比,具有更高的吸附容量。埃洛石-5对U(VI)的最大吸附容量为157 mg U/g,这使得这种改性矿物成为从废物中去除U(VI)最有效的吸附剂之一。从吸附产物的ATR、XPS和热降解光谱可以看出,R-S-C(NH)(NH)络合物在埃洛石外表面形成,而低聚羟基络合物(UO)(OH)和(UO)(OH)存在于埃洛石结构内部,主要与铝醇相互作用。

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