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一种用于从天然水和实际废水中有效且选择性去除磷酸盐的铈(Ce)基氨化单宁/聚乙烯醇水凝胶。

A cerium (Ce) -based ammoniated tannin/polyvinyl alcohol hydrogel for effective and selective phosphate removal from natural water and real wastewater.

作者信息

Yang Zijun, Yin Xuexue, Wang Zixuan, Sha Bing, Miao Lingzhan, Wu Jun, You Guoxiang, Hou Jun

机构信息

College of Civil Engineering and Transportation, Hohai University, Nanjing 210098, China.

College of Environment, Hohai University, Nanjing 210098, China.

出版信息

Int J Biol Macromol. 2025 May;309(Pt 1):142756. doi: 10.1016/j.ijbiomac.2025.142756. Epub 2025 Apr 1.

DOI:10.1016/j.ijbiomac.2025.142756
PMID:40180099
Abstract

This paper presents the synthesis of a cost-effective, environmentally friendly, and highly efficient Cerium (Ce)-based polyvinyl alcohol/tannin hydrogel adsorbent modified with triethylene tetramine (Ce-PVA/TA/TETA). This material integrates components with exceptional phosphate affinity, making it ideal for phosphate removal applications. Specifically, the hydrogels were firstly prepared by using tannin and polyvinyl alcohol as raw materials. Subsequently, after HBO as crosslinking, the Ce was loaded into hydrogel by co-precipitation and Ce-PVA/TA was modified by triethylene tetramine amine to obtain Ce-PVA/TA/TETA with high adsorption efficiency and high selectivity. Triple modification with tannin hydrogelation, Ce loading and amination can significantly improve the affinity of the material to phosphate. This allows the Ce-PVA/TA/TETA hydrogel to maintain high phosphate adsorption capabilities across a wide pH range of 3.0-12.0. The Ce-PVA/TA/TETA hydrogel achieved a maximum phosphorus adsorption capacity of 110.88 mg/g within an equilibrium time of 120 min at 25 °C and pH = 3.0. The presence of co-existing ions had impact on phosphate adsorption. Both the pseudo-second-order model and the Langmuir model effectively described the kinetics and isotherms, respectively. The adsorption process was a monolayer chemical adsorption, which was dominated by the surface adsorption and particle internal diffusion. Besides electrostatic attraction, ligand exchange and internal diffusion mechanisms were involved in the phosphate adsorbing of Ce-PVA/TA/TETA based on Zeta potential, FTIR, and XPS analysis. Most importantly, the Ce-PVA/TA/TETA hydrogel can swiftly remove phosphate from natural water and wastewater at low doses, meeting regulatory standards. This underscores its promising potential for phosphate management and eutrophication control.

摘要

本文介绍了一种具有成本效益、环境友好且高效的铈(Ce)基聚乙烯醇/单宁水凝胶吸附剂的合成方法,该吸附剂用三亚乙基四胺(Ce-PVA/TA/TETA)改性。这种材料整合了具有优异磷酸盐亲和力的成分,使其成为去除磷酸盐应用的理想选择。具体而言,首先以单宁和聚乙烯醇为原料制备水凝胶。随后,以HBO作为交联剂,通过共沉淀法将Ce负载到水凝胶中,并通过三亚乙基四胺对Ce-PVA/TA进行改性,以获得具有高吸附效率和高选择性的Ce-PVA/TA/TETA。通过单宁水凝胶化、Ce负载和胺化的三重改性可以显著提高材料对磷酸盐的亲和力。这使得Ce-PVA/TA/TETA水凝胶在3.0-12.0的宽pH范围内保持高磷酸盐吸附能力。在25℃和pH=3.0的条件下,Ce-PVA/TA/TETA水凝胶在120分钟的平衡时间内实现了110.88mg/g的最大磷吸附容量。共存离子的存在对磷酸盐吸附有影响。准二级模型和朗缪尔模型分别有效地描述了动力学和等温线。吸附过程是单层化学吸附,主要由表面吸附和颗粒内扩散主导。基于Zeta电位、傅里叶变换红外光谱(FTIR)和X射线光电子能谱(XPS)分析,除了静电吸引外,配体交换和内扩散机制也参与了Ce-PVA/TA/TETA对磷酸盐的吸附。最重要的是,Ce-PVA/TA/TETA水凝胶可以在低剂量下迅速从天然水和废水中去除磷酸盐,符合监管标准。这突出了其在磷酸盐管理和富营养化控制方面的广阔前景。

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