期刊
ACS CENTRAL SCIENCE
卷 4, 期 6, 页码 739-747出版社
AMER CHEMICAL SOC
DOI: 10.1021/acscentsci.8b00223
关键词
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资金
- U.S. Department of Homeland Security [2012-DN-130-NF0001]
- U.S. Department of Energy, Office of Science, Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division
- Office of Science of the U.S. Department of Energy [DE-AC02-05CH11231]
- U.S. Department of Energy, Office of Science, Office of Workforce Development for Teachers and Scientists, Office of Science Graduate Student Research (SCGSR) program
- DOE [DESC0014664]
- United States Government
- Department of Energy
Fundamental understanding of the selective recognition and separation of f-block metal ions by chelating agents is of crucial importance for advancing sustainable energy systems. Current investigations in this area are mostly focused on the study of inner-sphere interactions between metal ions and donor groups of ligands, while the effects on the selectivity resulting from molecular interactions in the outer-sphere region have been largely overlooked. Herein, we explore the fundamental origins of the selectivity of the solvating extractant N,N,N',N'-tetraoctyl diglycolamide (TODGA) for adjacent lanthanides in a liquid-liquid extraction system, which is of relevance to nuclear fuel reprocessing and rare-earth refining technologies. Complementary investigations integrating distribution studies, quantum mechanical calculations, and classical molecular dynamics simulations establish a relationship between coextracted water and lanthanide extraction by TODGA across the series, pointing to the importance of the hydrogen-bonding interactions between outer-sphere nitrate ions and water clusters in a nonpolar environment. Our findings have significant implications for the design of novel efficient separation systems and processes, emphasizing the importance of tuning both inner-and outer-sphere interactions to obtain total control over selectivity in the biphasic extraction of lanthanides.
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