Robust removal of thallium(I) from water with nano-MnO2 implanted zwitterionic porous hydrogel

IF 6.1 1区化学 Q1 CHEMISTRY, ANALYTICAL

Talanta Pub Date : 2025-06-18 DOI:10.1016/j.talanta.2025.128484

Hongjie Wu , Dirong Gong , Xiaoyu Jia

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Abstract

The uncontrolled disposal of Tl(I) waste comes at a significant economic and environmental cost because of the acute toxicity and high mobility. To resolve the aggregation problem for most reported MnO₂ based adsorbent materials which significantly affected the adsorption efficiency, porous zwitterionic ammonium propyl sulfonate (zw) polyacrylamide hydrogel (PAAm) has been fabricated to disperse nano-MnO₂ as a support. The developed nano-MnO₂@PAAm-zw exhibited a specific surface area of 5.06 m²/g and a pore diameter of 23.8 nm. particularly amenable to removal of Tl(I) for environmental remediation. The factors, including adsorbent MnO₂ incorporation, feeding amount, adsorption time, pH of the solution, Tl(I) initial concentration and existence of competing cations that governing the adsorption performances were fully elucidated. The maximal removal capacity Q_e reaches up to 336.5 mg (Tl) g⁻¹(MnO₂) with 99.92 % elimination efficiency and a low residue of 4.5 μg L⁻¹. The materials exhibit an astonishing robustness against nature matrix and high concentration of cations with adsorption capacity being 928.6–41.43 times larger than various competing counterparts for lab-made and mineral samples, representing the state-of-the-art level of adsorbents. The adsorbent can be regenerated at least five times retaining 86.0 % of original efficiency. A novel concerted mechanistic pathway of retention mainly associated with re-dox reaction is possible. These features offer great potentials for selective and deep elimination of total thallium in water samples.

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纳米二氧化锰注入两性离子多孔水凝胶对水中铊的强力去除

由于毒性大、流动性高，不加控制地处置放射性放射性废物将付出巨大的经济和环境代价。为解决目前报道的二氧化锰基吸附剂的聚集问题，制备了多孔两性离子丙基磺酸铵（zw）聚丙烯酰胺水凝胶（PAAm）来分散纳米二氧化锰作为载体。制备的nano-MnO2@PAAm-zw比表面积为5.06 m2/g，孔径为23.8 nm。特别适合移除Tl(I)以进行环境修复。研究了吸附剂MnO2掺入量、投料量、吸附时间、溶液pH、Tl(I)初始浓度和竞争阳离子的存在等因素对吸附性能的影响。最大去除率Qe可达336.5 mg (Tl) g−1(MnO2)，去除率为99.92%，残留量为4.5 μg−1。该材料对天然基质和高浓度阳离子表现出惊人的鲁棒性，吸附容量比各种竞争对手的实验室制造和矿物样品大928.6-41.43倍，代表了最先进的吸附剂水平。该吸附剂可再生5次以上，吸附剂的回收率为86.0%。一种主要与氧化还原反应相关的新的协同机制途径是可能的。这些特性为选择性和深度去除水样中的总铊提供了巨大的潜力。

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来源期刊

Talanta 化学-分析化学

CiteScore

12.30

自引率

4.90%

发文量

861

审稿时长

29 days

期刊介绍： Talanta provides a forum for the publication of original research papers, short communications, and critical reviews in all branches of pure and applied analytical chemistry. Papers are evaluated based on established guidelines, including the fundamental nature of the study, scientific novelty, substantial improvement or advantage over existing technology or methods, and demonstrated analytical applicability. Original research papers on fundamental studies, and on novel sensor and instrumentation developments, are encouraged. Novel or improved applications in areas such as clinical and biological chemistry, environmental analysis, geochemistry, materials science and engineering, and analytical platforms for omics development are welcome. Analytical performance of methods should be determined, including interference and matrix effects, and methods should be validated by comparison with a standard method, or analysis of a certified reference material. Simple spiking recoveries may not be sufficient. The developed method should especially comprise information on selectivity, sensitivity, detection limits, accuracy, and reliability. However, applying official validation or robustness studies to a routine method or technique does not necessarily constitute novelty. Proper statistical treatment of the data should be provided. Relevant literature should be cited, including related publications by the authors, and authors should discuss how their proposed methodology compares with previously reported methods.