Yue Li , Jiewen Tian , Yao Li , Hongxing He , Xiujun Deng , Haidong Ju , Rao Tao , Wen-Tong Chen , Guangzhi Hu
{"title":"A DFT-designed neodymium ion-imprinted membrane with fouling resistance and high flux","authors":"Yue Li , Jiewen Tian , Yao Li , Hongxing He , Xiujun Deng , Haidong Ju , Rao Tao , Wen-Tong Chen , Guangzhi Hu","doi":"10.1016/j.memsci.2024.123047","DOIUrl":null,"url":null,"abstract":"<div><p>The rare earth metal neodymium (Nd) is widely used in advanced industries such as hybrid cars and aerospace. Therefore, recovering neodymium from wastewater presents valuable opportunities for secondary recycling. The recovery of Nd<sup>3+</sup> from wastewater using ion imprinting technology (IIT) for efficient selective separation holds significant importance. In this study, hydrophilic Nd(III) ion-imprinted membranes, termed Nd(III)–P/P/TIIM, were synthesized using the IIT technique. Nd(III)–P/P/TIIM exhibited efficient and selective separation capabilities for Nd<sup>3+</sup> with a remarkable retention rate of 95.68 % and a high water flux reaching up to 636.94 L·m<sup>−2</sup>·h<sup>−1</sup>. Additionally, its relative selectivity coefficients for interfering ions (<span><math><mrow><msub><mi>K</mi><mtext>La</mtext></msub></mrow></math></span>, <span><math><mrow><msub><mi>K</mi><mtext>Eu</mtext></msub></mrow></math></span>, <span><math><mrow><msub><mi>K</mi><mtext>Cu</mtext></msub></mrow></math></span>) were 3.9, 29.5, and 37.9, respectively. Various analyses, including DFT calculations, HOMO and LUMO calculations, MEP images, and XPS spectroscopy, confirm that the mechanism of selective retention of Nd<sup>3+</sup> by Nd(III)–P/P/TIIM in solution is due to Coulombic adsorption between the –COO<sup>−</sup> anion and Nd<sup>3+</sup> as well as an imprint memory effect. Even after undergoing three water-BSA cycles, the membrane maintained a water flux of 357.96 L·m<sup>−2</sup>·h<sup>−1</sup>. The antifouling principle of Nd(III)–P/P/TIIM was investigated by XDLVO theory, attributed to the increase of electron donor tension (γ<sup>−</sup>) and Lewis acid-base interactions (<span><math><mrow><msup><mrow><mo>Δ</mo><mi>G</mi></mrow><mtext>AB</mtext></msup></mrow></math></span>) at the membrane surface. This work provides an insightful guidance for engineering high-performance membranes and has the potential to provide an alternative method for recycling neodymium.</p></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":null,"pages":null},"PeriodicalIF":8.4000,"publicationDate":"2024-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Membrane Science","FirstCategoryId":"5","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0376738824006410","RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENGINEERING, CHEMICAL","Score":null,"Total":0}
引用次数: 0
Abstract
The rare earth metal neodymium (Nd) is widely used in advanced industries such as hybrid cars and aerospace. Therefore, recovering neodymium from wastewater presents valuable opportunities for secondary recycling. The recovery of Nd3+ from wastewater using ion imprinting technology (IIT) for efficient selective separation holds significant importance. In this study, hydrophilic Nd(III) ion-imprinted membranes, termed Nd(III)–P/P/TIIM, were synthesized using the IIT technique. Nd(III)–P/P/TIIM exhibited efficient and selective separation capabilities for Nd3+ with a remarkable retention rate of 95.68 % and a high water flux reaching up to 636.94 L·m−2·h−1. Additionally, its relative selectivity coefficients for interfering ions (, , ) were 3.9, 29.5, and 37.9, respectively. Various analyses, including DFT calculations, HOMO and LUMO calculations, MEP images, and XPS spectroscopy, confirm that the mechanism of selective retention of Nd3+ by Nd(III)–P/P/TIIM in solution is due to Coulombic adsorption between the –COO− anion and Nd3+ as well as an imprint memory effect. Even after undergoing three water-BSA cycles, the membrane maintained a water flux of 357.96 L·m−2·h−1. The antifouling principle of Nd(III)–P/P/TIIM was investigated by XDLVO theory, attributed to the increase of electron donor tension (γ−) and Lewis acid-base interactions () at the membrane surface. This work provides an insightful guidance for engineering high-performance membranes and has the potential to provide an alternative method for recycling neodymium.
期刊介绍:
The Journal of Membrane Science is a publication that focuses on membrane systems and is aimed at academic and industrial chemists, chemical engineers, materials scientists, and membranologists. It publishes original research and reviews on various aspects of membrane transport, membrane formation/structure, fouling, module/process design, and processes/applications. The journal primarily focuses on the structure, function, and performance of non-biological membranes but also includes papers that relate to biological membranes. The Journal of Membrane Science publishes Full Text Papers, State-of-the-Art Reviews, Letters to the Editor, and Perspectives.