Ultra–selective and sustainable extraction of trace Cr(VI) from real waters using a thermally regenerable MOF composite of pDMAEMA-DUT-5

IF 8.1 1区 工程技术 Q1 ENGINEERING, CHEMICAL Separation and Purification Technology Pub Date : 2025-03-18 DOI:10.1016/j.seppur.2025.132601
Yilei Fang, Mengyu Tang, Xu Wu, Jiajie Zhang, Qian Guan, Yinzhou Luo, Xin Yu, Ranwen Ou
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Abstract

Trace amount of Cr(VI) in water still threatens human health and ecology. Several reported amine-based adsorbents can remove trace Cr(VI) in acidic solutions of pH 2–5, but perform badly at neutral and alkaline conditions, which is insufficient for treating natural waters. Also, the chemical eluate leads to secondary pollution. Here, the amine-rich thermo-responsive poly(dimethylaminoethyl methacrylate) (pDMAEMA) was selected based on its high pKa value and introduced into MOFs to produce pDMAEMA-DUT-5 for effective removal of trace Cr(VI) from natural waters. The composite with a polymer loading of 23.4 wt% achieved the highest adsorption capacity of 182.2 mg g−1 under an optimized condition, that is, at pH 3 and 25 °C. Besides, this material effectively reduced trace Cr(VI) content in natural waters from 100 to 1 μg L−1 by one filtration in a column. Its high selectivity was verified and further confirmed by the strong adsorption energy of Cr(VI) and −N(CH3)2. Furthermore, the composite could be fully regenerated in 45 °C water within 10 min, concentrating Cr(VI) for 270 folds in one adsorption–desorption cycle and maintaining over 99 % performance after five cycles. It demonstrated excellent removal efficiency, high selectivity, and thermal regeneration stability. This work presents a simple strategy to design highly selective and sustainable ion adsorbents for effective removal of toxic ions or resource recovery, while its thermal regeneration function largely simplifies further treatments.

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水中的微量六价铬仍然威胁着人类健康和生态环境。已报道的几种胺类吸附剂可以去除 pH 值为 2-5 的酸性溶液中的痕量六价铬,但在中性和碱性条件下性能较差,不足以处理天然水体。此外,化学洗脱物还会导致二次污染。在此,我们根据富胺热响应性聚(甲基丙烯酸二甲胺基乙酯)(pDMAEMA)的高 pKa 值,将其引入 MOF 中,制备出 pDMAEMA-DUT-5,用于有效去除天然水体中的痕量六价铬。在 pH 值为 3、温度为 25 ℃ 的优化条件下,聚合物负载量为 23.4 wt% 的复合材料的吸附容量最高,达到 182.2 mg g-1。此外,这种材料通过柱过滤一次就能有效地将天然水中的痕量六价铬含量从 100 μg L-1 降至 1 μg L-1。六价铬和-N(CH3)2的强吸附能验证并进一步证实了它的高选择性。此外,该复合材料可在 45 °C 的水中于 10 分钟内完全再生,在一次吸附-解吸循环中可浓缩 270 倍的 Cr(VI),并在五次循环后保持 99% 以上的性能。它表现出卓越的去除效率、高选择性和热再生稳定性。这项工作为设计高选择性和可持续的离子吸附剂提供了一种简单的策略,可用于有效去除有毒离子或回收资源,而其热再生功能在很大程度上简化了进一步的处理。
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来源期刊
Separation and Purification Technology
Separation and Purification Technology 工程技术-工程:化工
CiteScore
14.00
自引率
12.80%
发文量
2347
审稿时长
43 days
期刊介绍: Separation and Purification Technology is a premier journal committed to sharing innovative methods for separation and purification in chemical and environmental engineering, encompassing both homogeneous solutions and heterogeneous mixtures. Our scope includes the separation and/or purification of liquids, vapors, and gases, as well as carbon capture and separation techniques. However, it's important to note that methods solely intended for analytical purposes are not within the scope of the journal. Additionally, disciplines such as soil science, polymer science, and metallurgy fall outside the purview of Separation and Purification Technology. Join us in advancing the field of separation and purification methods for sustainable solutions in chemical and environmental engineering.
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