Sulfhydryl-modified zeolite A with exceptional strontium adsorption selectivity

IF 10.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Lingyi Li, Lanxing Ren, Dong Wang, Junchang Chen, Qi Guo, Yuting Zhao, Fuqiang Zhao, Linwei He, Jie Li, Wenqi Zhang, Lijuan Song, Long Chen, Lixi Chen, Bin Wang, Lin Zhu, Tao Duan, Zhifang Chai, Shuao Wang
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Abstract

Efficient removal of trace radiostrontium from contaminated highly saline wastewater, such as seawater, remains a critical but challenging task due to the coexistence of large excess of hard cations like Na+, K+, Mg2+ and particularly Ca2+, which shares similar physicochemical properties with Sr2+. Herein, we successfully boosted the selectivity by a sulfhydryl-functionalized NaA zeolite (SH-NaA) via ion exchange coupled with reinforced soft-soft interactions between sulfhydryl groups and Sr2+. Remarkably, SH-NaA achieved a 99.8% removal efficiency of Sr2+ in the presence of a tenfold excess of Ca2+, with a distribution coefficient (Kd) of 4.98×105 mL/g. The effectiveness of SH-NaA in accurately capturing Sr2+ was further validated by its superior dynamic adsorption performance in natural seawater compared to pristine NaA zeolite. Batch experiments highlighted SH-NaA’s exceptional Sr2+ removal efficiency (qm = 233.36 mg/g), rapid adsorption kinetics (1 min), superior decontamination depth (Kd = 6.71×105 mL/g), and robust irradiation stability (400 kGy γ-ray). X-ray photoelectron spectroscopy (XPS) and in situ Fourier-transform infrared (FTIR) analyses underscored the pivotal role of sulfhydryl groups in Sr2+ capture. Density functional theory (DFT) calculations revealed that the sulfhydryl-functionalized NaA zeolite exhibits the best selectivity toward Sr2+, with an interaction energy of −2.55 eV. These findings demonstrate that organic group functionalized zeolites hold significant promise for environmental remediation applications.

巯基改性A型沸石具有优异的锶吸附选择性
由于与Sr2+具有相似物理化学性质的Na+、K+、Mg2+、特别是Ca2+等大量过量的硬阳离子共存,从污染的高盐废水(如海水)中有效去除痕量放射性锶仍然是一项关键但具有挑战性的任务。本文中,我们通过离子交换与巯基与Sr2+之间增强的软软相互作用,成功地提高了巯基功能化NaA分子筛(SH-NaA)的选择性。值得注意的是,在Ca2+过量10倍的情况下,SH-NaA对Sr2+的去除率达到99.8%,分配系数(Kd)为4.98×105 mL/g。与原始NaA沸石相比,SH-NaA沸石在天然海水中具有更优越的动态吸附性能,进一步验证了其准确捕获Sr2+的有效性。批量实验表明,SH-NaA具有优异的Sr2+去除效率(qm = 233.36 mg/g),快速吸附动力学(1 min),优越的去污深度(Kd = 6.71×105 mL/g)和强大的辐照稳定性(400 kGy γ射线)。x射线光电子能谱(XPS)和原位傅立叶变换红外(FTIR)分析强调了巯基在Sr2+捕获中的关键作用。密度泛函理论(DFT)计算表明,巯基官能化NaA分子筛对Sr2+的选择性最好,其相互作用能为- 2.55 eV。这些发现表明,有机基团功能化沸石在环境修复应用中具有重要的前景。
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来源期刊
Science China Chemistry
Science China Chemistry CHEMISTRY, MULTIDISCIPLINARY-
CiteScore
14.40
自引率
7.30%
发文量
3787
审稿时长
2.2 months
期刊介绍: Science China Chemistry, co-sponsored by the Chinese Academy of Sciences and the National Natural Science Foundation of China and published by Science China Press, publishes high-quality original research in both basic and applied chemistry. Indexed by Science Citation Index, it is a premier academic journal in the field. Categories of articles include: Highlights. Brief summaries and scholarly comments on recent research achievements in any field of chemistry. Perspectives. Concise reports on thelatest chemistry trends of interest to scientists worldwide, including discussions of research breakthroughs and interpretations of important science and funding policies. Reviews. In-depth summaries of representative results and achievements of the past 5–10 years in selected topics based on or closely related to the research expertise of the authors, providing a thorough assessment of the significance, current status, and future research directions of the field.
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