Structure Activity Relationship Approach toward the Improved Separation of Rare-Earth Elements Using Diglycolamides

Stamberga, Diana; Healy, Mary; Bryantsev, Vyacheslav; Albisser, Camille A.; Karslyan, Yana; Reinhart, Benjamin; Paulenova, Alena; Foster, Mackenzie; Lyon, Kevin; Moyer, Bruce A.; Popovs, Ilja; Jansone-Popova, Santa

doi:10.1021/acs.inorgchem.0c02861

Title: Structure Activity Relationship Approach toward the Improved Separation of Rare-Earth Elements Using Diglycolamides

Journal Article · Fri Nov 13 00:00:00 UTC 2020 · Inorganic Chemistry

DOI: https://doi.org/10.1021/acs.inorgchem.0c02861 · OSTI ID:1720238

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^[1]; Albisser, Camille A. ^[2]; Karslyan, Yana ^[3]; Reinhart, Benjamin ^[4]; Paulenova, Alena ^[5]; Foster, Mackenzie ^[6];

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Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Merck KGaA, Darmstadt (Germany)
Oregon State Univ., Corvallis, OR (United States); Argonne National Lab. (ANL), Argonne, IL (United States)
Argonne National Lab. (ANL), Argonne, IL (United States)
Oregon State Univ., Corvallis, OR (United States)
Marshallton Research Labs., King, NC (United States)
Idaho National Lab. (INL), Idaho Falls, ID (United States)

The separation of adjacent lanthanides continues to be a challenge worldwide because of the similar physical and chemical properties of these elements and a necessity to advance the use of clean-energy applications. In this paper, a systematic structure–performance relationship approach toward understanding the effect of N-alkyl group characteristics in diglycolamides (DGAs) on the separation of lanthanides(III) from a hydrochloric acid medium is presented. In addition to the three most extensively studied DGA complexants [N,N,N',N'-tetra(n-octyl)diglycolamide, TODGA; N,N,N',N'-tetra(2-ethylhexyl)diglycolamide, TEHDGA; N,N'-dimethyl-N,N'-di(n-octyl)diglycolamide, DMDODGA], 12 new extracting agents with varying substitution patterns were designed to study the interplay of steric and electronic effects that control rare-earth element extraction. Subtle changes in the structure around diglycolamide carbonyl oxygen atoms result in dramatic shifts in the lanthanide extraction strength and selectivity. The effects of the chain length and branching position of N-alkyl substituents in DGAs are elaborated on with the use of experimental, computational, and solution-structure characterization techniques.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-05CH11231; AC02-06CH11357; AC05-00OR22725

OSTI ID:: 1720238

Journal Information:: Inorganic Chemistry, Journal Name: Inorganic Chemistry Journal Issue: N/A Vol. TBD; ISSN 0020-1669

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
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rare earth element separations
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solution structure

Title: Structure Activity Relationship Approach toward the Improved Separation of Rare-Earth Elements Using Diglycolamides

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