{"title":"功能化二维多层MXene从实际废水基质中选择性连续回收稀土元素","authors":"Shuangyou Bao, Yingjun Wang, Weiwei Yang, Charlotte Skjold Qvist Christensen, Yanan Shang, Yongsheng Yu, Zongsu Wei","doi":"10.1016/j.jhazmat.2025.137277","DOIUrl":null,"url":null,"abstract":"Rare earth elements (REEs) are the “fuel” for high-tech industry, yet their selective recovery from complex waste matrices is challenging. Herein, we designed a 2D multilayered MXene Ti<sub>3</sub>C<sub>2</sub>T<sub>x</sub> adsorbent for selective extraction of REEs in a broad pH range. By establishing strong Lewis acid-base interactions, extraction capacities of Ti<sub>3</sub>C<sub>2</sub>T<sub>x</sub> to Eu(III) and Ho(III) reached 892.8 and 649.2<!-- --> <!-- -->mg/g, respectively, even at pH 2.0. Following the Valence Matching Principle, the Ti<sub>3</sub>C<sub>2</sub>T<sub>x</sub> adsorbent also demonstrated high selectivity for recovery of various REEs from real REEs processing wastewater and actual sludge from magnet manufacturing industry. To demonstrate the practical feasibility, a layer-stacked membrane of Ti<sub>3</sub>C<sub>2</sub>T<sub>x</sub> supported on polyethersulfone substrate was fabricated for continuous recovery of REEs and exhibited excellent removal of Eu(III) (99.1% at pH 5.0), showcasing its potential for large-scale applications. DFT calculations and material characterization demonstrated that chemisorption between Lewis acid (REEs cations) and Lewis base (F and O) sites is the main adsorption process involved in the uptake of Eu(III) and Ho(III). Finally, both the Ti<sub>3</sub>C<sub>2</sub>T<sub>x</sub> adsorbent and membrane were successfully regenerated and reused via simple acid wash. Overall, the results demonstrate the Ti<sub>3</sub>C<sub>2</sub>T<sub>x</sub>-based recovery as a promising path for sustainable harvesting of REEs.","PeriodicalId":361,"journal":{"name":"Journal of Hazardous Materials","volume":"140 1","pages":""},"PeriodicalIF":12.2000,"publicationDate":"2025-01-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Functionalized 2D Multilayered MXene for Selective and Continuous Recovery of Rare Earth Elements from Real Wastewater Matrix\",\"authors\":\"Shuangyou Bao, Yingjun Wang, Weiwei Yang, Charlotte Skjold Qvist Christensen, Yanan Shang, Yongsheng Yu, Zongsu Wei\",\"doi\":\"10.1016/j.jhazmat.2025.137277\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Rare earth elements (REEs) are the “fuel” for high-tech industry, yet their selective recovery from complex waste matrices is challenging. Herein, we designed a 2D multilayered MXene Ti<sub>3</sub>C<sub>2</sub>T<sub>x</sub> adsorbent for selective extraction of REEs in a broad pH range. By establishing strong Lewis acid-base interactions, extraction capacities of Ti<sub>3</sub>C<sub>2</sub>T<sub>x</sub> to Eu(III) and Ho(III) reached 892.8 and 649.2<!-- --> <!-- -->mg/g, respectively, even at pH 2.0. Following the Valence Matching Principle, the Ti<sub>3</sub>C<sub>2</sub>T<sub>x</sub> adsorbent also demonstrated high selectivity for recovery of various REEs from real REEs processing wastewater and actual sludge from magnet manufacturing industry. To demonstrate the practical feasibility, a layer-stacked membrane of Ti<sub>3</sub>C<sub>2</sub>T<sub>x</sub> supported on polyethersulfone substrate was fabricated for continuous recovery of REEs and exhibited excellent removal of Eu(III) (99.1% at pH 5.0), showcasing its potential for large-scale applications. DFT calculations and material characterization demonstrated that chemisorption between Lewis acid (REEs cations) and Lewis base (F and O) sites is the main adsorption process involved in the uptake of Eu(III) and Ho(III). Finally, both the Ti<sub>3</sub>C<sub>2</sub>T<sub>x</sub> adsorbent and membrane were successfully regenerated and reused via simple acid wash. Overall, the results demonstrate the Ti<sub>3</sub>C<sub>2</sub>T<sub>x</sub>-based recovery as a promising path for sustainable harvesting of REEs.\",\"PeriodicalId\":361,\"journal\":{\"name\":\"Journal of Hazardous Materials\",\"volume\":\"140 1\",\"pages\":\"\"},\"PeriodicalIF\":12.2000,\"publicationDate\":\"2025-01-20\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of Hazardous Materials\",\"FirstCategoryId\":\"93\",\"ListUrlMain\":\"https://doi.org/10.1016/j.jhazmat.2025.137277\",\"RegionNum\":1,\"RegionCategory\":\"环境科学与生态学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"ENGINEERING, ENVIRONMENTAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Hazardous Materials","FirstCategoryId":"93","ListUrlMain":"https://doi.org/10.1016/j.jhazmat.2025.137277","RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENGINEERING, ENVIRONMENTAL","Score":null,"Total":0}
Functionalized 2D Multilayered MXene for Selective and Continuous Recovery of Rare Earth Elements from Real Wastewater Matrix
Rare earth elements (REEs) are the “fuel” for high-tech industry, yet their selective recovery from complex waste matrices is challenging. Herein, we designed a 2D multilayered MXene Ti3C2Tx adsorbent for selective extraction of REEs in a broad pH range. By establishing strong Lewis acid-base interactions, extraction capacities of Ti3C2Tx to Eu(III) and Ho(III) reached 892.8 and 649.2 mg/g, respectively, even at pH 2.0. Following the Valence Matching Principle, the Ti3C2Tx adsorbent also demonstrated high selectivity for recovery of various REEs from real REEs processing wastewater and actual sludge from magnet manufacturing industry. To demonstrate the practical feasibility, a layer-stacked membrane of Ti3C2Tx supported on polyethersulfone substrate was fabricated for continuous recovery of REEs and exhibited excellent removal of Eu(III) (99.1% at pH 5.0), showcasing its potential for large-scale applications. DFT calculations and material characterization demonstrated that chemisorption between Lewis acid (REEs cations) and Lewis base (F and O) sites is the main adsorption process involved in the uptake of Eu(III) and Ho(III). Finally, both the Ti3C2Tx adsorbent and membrane were successfully regenerated and reused via simple acid wash. Overall, the results demonstrate the Ti3C2Tx-based recovery as a promising path for sustainable harvesting of REEs.
期刊介绍:
The Journal of Hazardous Materials serves as a global platform for promoting cutting-edge research in the field of Environmental Science and Engineering. Our publication features a wide range of articles, including full-length research papers, review articles, and perspectives, with the aim of enhancing our understanding of the dangers and risks associated with various materials concerning public health and the environment. It is important to note that the term "environmental contaminants" refers specifically to substances that pose hazardous effects through contamination, while excluding those that do not have such impacts on the environment or human health. Moreover, we emphasize the distinction between wastes and hazardous materials in order to provide further clarity on the scope of the journal. We have a keen interest in exploring specific compounds and microbial agents that have adverse effects on the environment.