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优先使用聚合物负载的 Mg/Al 层状双氢氧化物纳米片进行磷酸盐的吸附。

Preferable phosphate sequestration using polymer-supported Mg/Al layered double hydroxide nanosheets.

机构信息

School of Environmental Science and Engineering, Nanjing Tech University, Nanjing 211816, China.

School of Environmental Science and Engineering, Nanjing Tech University, Nanjing 211816, China.

出版信息

J Colloid Interface Sci. 2022 May 15;614:583-592. doi: 10.1016/j.jcis.2022.01.158. Epub 2022 Jan 29.

Abstract

The efficient removal of phosphate from waters is critical to mitigating eutrophication. Recently, layered double hydroxides (LDHs) have been believed to be promising adsorbents for phosphate removal. Nevertheless, the scaled-up application of LDHs is limited by the difficulties of separation, excessive pressure drops, and potential metal leaching. In this study, a millimeter-sized nanocomposite, MgAl-201, was fabricated by impregnating Mg/Al LDH nanosheets into a polystyrene anion exchanger D201. The resulting MgAl-201 combines the inherent affinity of Mg/Al LDH toward phosphate and the excellent hydrodynamic performance of the support material. Benefiting from the shielding effect from the cross-linked polymeric host, MgAl-201 exhibits satisfactory chemical stability in the range of pH 3-11 with a negligible metal release. Adsorption experiments show that MgAl-201 has superb applicability to neutral phosphate-contaminated waters. It reaches adsorption equilibrium within 270 min, and the maximum adsorption capacity calculated by the double Langmuir model is 52.0 mg/g. Meanwhile, MgAl-201 exhibits more preferable adsorption toward phosphate than D201 when coexisting anions are at relatively high levels. FTIR and XPS surveys revealed that two distinct adsorption interactions were involved in phosphate removal, that is, electrostatic interactions from the quaternary ammonium groups bonded on the host and the interlayer exchangeable anions in the encapsulated Mg/Al LDH, and specific inner-sphere complexation from the -OH groups in the Mg/Al LDH layers. For wastewater application, a satisfactory treatable volume of 580 BV was achieved to reduce the effluents from 2.0 mg/L to 0.5 mg/L, which was up to 8 times that of the traditional anion exchanger D201. Furthermore, MgAl-201 could be easily regenerated using the NaCO-NaCl binary solution and maintained good reusability without significant capacity loss after 5 adsorption-desorption cycles. The results suggest that MgAl-201 is of great application capability for preferable phosphate sequestration in advanced wastewater treatment.

摘要

从水中高效去除磷酸盐对于减轻富营养化至关重要。最近,层状双氢氧化物(LDHs)被认为是一种很有前途的磷酸盐去除吸附剂。然而,LDHs 的规模化应用受到分离困难、压降过大和潜在金属浸出等因素的限制。在这项研究中,通过将 Mg/Al LDH 纳米片浸渍到聚苯乙烯阴离子交换剂 D201 中,制备出毫米级的纳米复合材料 MgAl-201。所得到的 MgAl-201 结合了 Mg/Al LDH 对磷酸盐的固有亲和力和支撑材料的优异水动力性能。得益于交联聚合物主体的屏蔽效应,MgAl-201 在 pH 值为 3-11 的范围内表现出令人满意的化学稳定性,金属浸出可忽略不计。吸附实验表明,MgAl-201 对中性磷酸盐污染水具有极好的适用性。它在 270 分钟内达到吸附平衡,通过双朗缪尔模型计算的最大吸附容量为 52.0 mg/g。同时,当共存阴离子处于较高水平时,MgAl-201 对磷酸盐的吸附比 D201 更具优势。FTIR 和 XPS 调查表明,磷酸盐的去除涉及两种不同的吸附相互作用,即与主体结合的季铵基团的静电相互作用和封装在 Mg/Al LDH 中的层间可交换阴离子,以及 Mg/Al LDH 层中的 -OH 基团的特定内球络合。对于废水应用,实现了令人满意的 580 BV 处理量,可将废水中的磷酸盐从 2.0 mg/L 降低至 0.5 mg/L,是传统阴离子交换剂 D201 的 8 倍。此外,MgAl-201 可以使用 NaCO-NaCl 二元溶液很容易地再生,并在 5 次吸附-解吸循环后保持良好的可重复使用性,而没有明显的容量损失。结果表明,MgAl-201 在高级废水处理中对磷酸盐的优先螯合具有很大的应用潜力。

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