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Title: Rare earth separations by selective borate crystallization

Abstract

Lanthanides possess similar chemical properties rendering their separation from one another a challenge of fundamental chemical and global importance given their incorporation into many advanced technologies. New separation strategies combining green chemistry with low cost and high efficiency remain highly desirable. We demonstrate that the subtle bonding differences among trivalent lanthanides can be amplified during the crystallization of borates, providing chemical recognition of specific lanthanides that originates from Ln 3+ coordination alterations, borate polymerization diversity and soft ligand coordination selectivity. Six distinct phases are obtained under identical reaction conditions across lanthanide series, further leading to an efficient and cost-effective separation strategy via selective crystallization. As proof of concept, Nd/Sm and Nd/Dy are used as binary models to demonstrate solid/aqueous and solid/solid separation processes. Controlling the reaction kinetics gives rise to enhanced separation efficiency of Nd/Sm system and a one-step quantitative separation of Nd/Dy with the aid of selective density-based flotation.

Authors:
 [1];  [1];  [2];  [1];  [1];  [1];  [1];  [2];  [1];  [3];  [1]
  1. Soochow Univ. and Collaborative Innovation Center of Radiation Medicine of Jiangsu Higher Education Institutions, Suzhou (China). School for Radiological and Interdisciplinary Sciences
  2. Chinese Academy of Sciences (CAS), Beijing (China). Engineering Lab. of Specialty Fibers and Nuclear Energy Materials
  3. Florida State Univ., Tallahassee, FL (United States). Dept. of Chemistry and Biochemistry
Publication Date:
Research Org.:
Florida State Univ., Tallahassee, FL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1465711
Grant/Contract Number:  
FG02-13ER16414; SC0010677
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 8; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE

Citation Formats

Yin, Xuemiao, Wang, Yaxing, Bai, Xiaojing, Wang, Yumin, Chen, Lanhua, Xiao, Chengliang, Diwu, Juan, Du, Shiyu, Chai, Zhifang, Albrecht-Schmitt, Thomas E., and Wang, Shuao. Rare earth separations by selective borate crystallization. United States: N. p., 2017. Web. doi:10.1038/ncomms14438.
Yin, Xuemiao, Wang, Yaxing, Bai, Xiaojing, Wang, Yumin, Chen, Lanhua, Xiao, Chengliang, Diwu, Juan, Du, Shiyu, Chai, Zhifang, Albrecht-Schmitt, Thomas E., & Wang, Shuao. Rare earth separations by selective borate crystallization. United States. doi:10.1038/ncomms14438.
Yin, Xuemiao, Wang, Yaxing, Bai, Xiaojing, Wang, Yumin, Chen, Lanhua, Xiao, Chengliang, Diwu, Juan, Du, Shiyu, Chai, Zhifang, Albrecht-Schmitt, Thomas E., and Wang, Shuao. Tue . "Rare earth separations by selective borate crystallization". United States. doi:10.1038/ncomms14438. https://www.osti.gov/servlets/purl/1465711.
@article{osti_1465711,
title = {Rare earth separations by selective borate crystallization},
author = {Yin, Xuemiao and Wang, Yaxing and Bai, Xiaojing and Wang, Yumin and Chen, Lanhua and Xiao, Chengliang and Diwu, Juan and Du, Shiyu and Chai, Zhifang and Albrecht-Schmitt, Thomas E. and Wang, Shuao},
abstractNote = {Lanthanides possess similar chemical properties rendering their separation from one another a challenge of fundamental chemical and global importance given their incorporation into many advanced technologies. New separation strategies combining green chemistry with low cost and high efficiency remain highly desirable. We demonstrate that the subtle bonding differences among trivalent lanthanides can be amplified during the crystallization of borates, providing chemical recognition of specific lanthanides that originates from Ln3+ coordination alterations, borate polymerization diversity and soft ligand coordination selectivity. Six distinct phases are obtained under identical reaction conditions across lanthanide series, further leading to an efficient and cost-effective separation strategy via selective crystallization. As proof of concept, Nd/Sm and Nd/Dy are used as binary models to demonstrate solid/aqueous and solid/solid separation processes. Controlling the reaction kinetics gives rise to enhanced separation efficiency of Nd/Sm system and a one-step quantitative separation of Nd/Dy with the aid of selective density-based flotation.},
doi = {10.1038/ncomms14438},
journal = {Nature Communications},
issn = {2041-1723},
number = ,
volume = 8,
place = {United States},
year = {2017},
month = {3}
}

Journal Article:
Free Publicly Available Full Text
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Citation Metrics:
Cited by: 26 works
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Figures / Tables:

Figure 1 Figure 1: The periodic trend for the unary lanthanide borates from molten boric acid flux reactions. Chemical equations of boric acid flux reactions with six different groups of lanthanides showing the periodic trend for the formation of lanthanide borates.

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Works referenced in this record:

Generalized Gradient Approximation Made Simple
journal, October 1996

  • Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias
  • Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868
  • DOI: 10.1103/PhysRevLett.77.3865

Special points for Brillouin-zone integrations
journal, June 1976

  • Monkhorst, Hendrik J.; Pack, James D.
  • Physical Review B, Vol. 13, Issue 12, p. 5188-5192
  • DOI: 10.1103/PhysRevB.13.5188

Inhomogeneous Electron Gas
journal, November 1964


    Works referencing / citing this record:

    CCDC 1521493: Experimental Crystal Structure Determination
    dataset, January 2017


    CCDC 1521491: Experimental Crystal Structure Determination: LANQAV : Non-CSD Structure
    dataset, December 2016


    CCDC 1521492: Experimental Crystal Structure Determination: LANQEZ : catena-((μ-dihydrogen hexaborate)-diaqua-chloro-neodymium monohydrate)
    dataset, December 2016


    CCDC 1521494: Experimental Crystal Structure Determination: LANQOJ : catena-((μ-pentahydrogen hexaborate)-europium boric acid)
    dataset, December 2016


      Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.