Fabrication of ion imprinted diethylenetriamine pentaacetic acid-polyethylenimine modified magnetic graphene oxide for selective adsorption of Ce(III)

IF 9.7 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Journal of Cleaner Production Pub Date : 2024-10-30 DOI:10.1016/j.jclepro.2024.144104
Ting Guo , Chaoke Bulin , Rongxiang Zheng
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Abstract

Selective recovery of rare earth elements is essential for both sustainable exploitation of rare earth resources and environmental remediation. Herein, Ce(Ⅲ) imprinted diethylenetriamine pentaacetic acid-polyethylenimine modified magnetic graphene oxide (IIP-DTPA-PEI-MGO) was fabricated for selective adsorption of Ce(Ⅲ). Adsorption efficiency and selectivity performance of IIP-DTPA-PEI-MGO towards Ce(Ⅲ) were evaluated via batch adsorption targeted at single and mixed solution, respectively. Adsorption mechanism was elucidated based on versatile adsorption fittings (isotherms, kinetics, thermodynamics) and spectroscopic tests (XPS, FTIR). Result presents, maximum adsorption efficiency of IIP-DTPA-PEI-MGO for Ce(III) is reached at pH = 5 in 30 min, demonstrating superior efficiency. The maximum mono layer adsorption capacity determined by the Langmuir model is 281.69 mg g−1. After adsorption, 75.65 % of original Ce(Ⅲ) is transferred into Ce(Ⅳ), while 24.35 % remain as Ce(Ⅲ). Furthermore, by virtue of its paramagnetic property, IIP-DTPA-PEI-MGO can be easily recovered for cyclic adsorption, thereby keeping adsorption quantity 90.44 mg g−1 on Ce(Ⅲ) in five consecutive cycles. Owing to ion imprinting sites, IIP-DTPA-PEI-MGO exhibits selectivity coefficient 1.34, 1.69, 2.32, 2.96, 15.24, 10.51 towards Ce(III) for binary solution Ce/La, Ce/Nd, Ce/Eu, Ce/Dy, Ce/Cu, Ce/Cr, respectively. In terms of adsorption mechanism, versatile functional groups O-H, C-N, C-O in IIP-DTPA-PEI-MGO provide heterogeneous affinity for Ce(Ⅲ), inducing chemical adsorption. This work provides a novel approach towards fabricating magnetic bio adsorbent for selective recovery of Ce(Ⅲ).

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制备离子印迹二乙烯三胺五醋酸-聚乙烯亚胺修饰的磁性石墨烯氧化物以选择性吸附 Ce(III)
稀土元素的选择性回收对于稀土资源的可持续开发和环境修复都至关重要。本文制备了用于选择性吸附 Ce(Ⅲ)的二乙烯三胺五醋酸-聚乙烯亚胺修饰磁性氧化石墨烯(IIP-DTPA-PEI-MGO)。通过针对单一溶液和混合溶液的批量吸附,分别评估了 IIP-DTPA-PEI-MGO 对 Ce(Ⅲ)的吸附效率和选择性。根据多种吸附配件(等温线、动力学、热力学)和光谱测试(XPS、傅立叶变换红外光谱)阐明了吸附机理。结果表明,IIP-DTPA-PEI-MGO 对 Ce(III)的最大吸附效率在 pH = 5 时于 30 分钟内达到,显示出卓越的吸附效率。根据 Langmuir 模型确定的最大单层吸附容量为 281.69 mg-g-1。吸附后,75.65% 的原始 Ce(Ⅲ) 转化为 Ce(Ⅳ),24.35% 仍为 Ce(Ⅲ)。此外,IIP-DTPA-PEI-MGO 还具有顺磁性,很容易被回收进行循环吸附,因此在 Ce(Ⅲ)上的吸附量在连续五个循环中保持在 90.44 mg-g-1。由于离子印迹位点的存在,IIP-DTPA-PEI-MGO 对二元溶液 Ce/La、Ce/Nd、Ce/Eu、Ce/Dy、Ce/Cu、Ce/Cr 的 Ce(Ⅲ)选择性系数分别为 1.34、1.69、2.32、2.96、15.24、10.51。从吸附机理来看,IIP-DTPA-PEI-MGO 中的多功能官能团 O-H、C-N、C-O 为 Ce(Ⅲ)提供了异质亲和力,诱导了化学吸附。这项工作为制造磁性生物吸附剂选择性回收铈(Ⅲ)提供了一种新方法。
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来源期刊
Journal of Cleaner Production
Journal of Cleaner Production 环境科学-工程:环境
CiteScore
20.40
自引率
9.00%
发文量
4720
审稿时长
111 days
期刊介绍: The Journal of Cleaner Production is an international, transdisciplinary journal that addresses and discusses theoretical and practical Cleaner Production, Environmental, and Sustainability issues. It aims to help societies become more sustainable by focusing on the concept of 'Cleaner Production', which aims at preventing waste production and increasing efficiencies in energy, water, resources, and human capital use. The journal serves as a platform for corporations, governments, education institutions, regions, and societies to engage in discussions and research related to Cleaner Production, environmental, and sustainability practices.
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