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Title: Facile and Efficient Decontamination of Thorium from Rare Earths Based on Selective Selenite Crystallization

Abstract

The coexistence of radioactive contaminants (e.g., thorium, uranium, and their daughters) in rare earth minerals introduces significant environmental, economic, and technological hurdles in modern rare earth production. Capable, low cost, and green decontamination strategies are therefore desired to ameliorate this problem. In this work, we report a single-step and quantitative decontamination strategy of thorium from rare earths based on a unique periodic trend in the formation of crystalline selenite compounds across the lanthanide series, where Ce(III) is fully oxidized in situ to Ce(IV). This gives rise to a crystallization system that is highly selective to trap tetravalent f-blocks while all other trivalent lanthanides completely remain in solution when coexist. These findings are bolstered by first-principles calculations of lattice energies and an examination of bonding in these compounds. This system is contrasted with typical natural and synthetic systems, where trivalent and tetravalent f-block elements often cocrystallize. The separation factors after one round of crystallization were determined from binary systems of Th(IV)/La(III), Th(IV)/Eu(III), and Th(IV)/Yb(III) to reach 2.1 × 10 5, 1.2 × 10 5, and 9 × 10 4, respectively. Selective crystallization of thorium from a simulated monazite composite yields a separation factor of 1.9 × 10 3 with nearly quantitativemore » removal of thorium.« less

Authors:
ORCiD logo [1];  [2];  [2];  [3];  [4];  [2];  [2];  [2];  [2]; ORCiD logo [4]; ORCiD logo [2];  [2]; ORCiD logo [5];  [6]; ORCiD logo [2]
  1. Sichuan Univ., Chengdu (China); Soochow Univ., Suzhou (China)
  2. Soochow Univ., Suzhou (China)
  3. Southwest Univ. of Science and Technology, Mianyang (China)
  4. Chinese Academy of Sciences (CAS), Ningbo (China)
  5. Florida State Univ., Tallahassee, FL (United States)
  6. Sichuan Univ., Chengdu (China)
Publication Date:
Research Org.:
Florida State Univ., Tallahassee, FL (United States). Energy Frontier Research Center (EFRC) Center for Actinide Science & Technology (CAST)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1470227
Grant/Contract Number:  
SC0016568
Resource Type:
Accepted Manuscript
Journal Name:
Inorganic Chemistry
Additional Journal Information:
Journal Volume: 57; Journal Issue: 4; Journal ID: ISSN 0020-1669
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY

Citation Formats

Wang, Yaxing, Lu, Huangjie, Dai, Xing, Duan, Tao, Bai, Xiaojing, Cai, Yawen, Yin, Xuemiao, Chen, Lanhua, Diwu, Juan, Du, Shiyu, Zhou, Ruhong, Chai, Zhifang, Albrecht-Schmitt, Thomas E., Liu, Ning, and Wang, Shuao. Facile and Efficient Decontamination of Thorium from Rare Earths Based on Selective Selenite Crystallization. United States: N. p., 2018. Web. doi:10.1021/acs.inorgchem.7b02681.
Wang, Yaxing, Lu, Huangjie, Dai, Xing, Duan, Tao, Bai, Xiaojing, Cai, Yawen, Yin, Xuemiao, Chen, Lanhua, Diwu, Juan, Du, Shiyu, Zhou, Ruhong, Chai, Zhifang, Albrecht-Schmitt, Thomas E., Liu, Ning, & Wang, Shuao. Facile and Efficient Decontamination of Thorium from Rare Earths Based on Selective Selenite Crystallization. United States. doi:10.1021/acs.inorgchem.7b02681.
Wang, Yaxing, Lu, Huangjie, Dai, Xing, Duan, Tao, Bai, Xiaojing, Cai, Yawen, Yin, Xuemiao, Chen, Lanhua, Diwu, Juan, Du, Shiyu, Zhou, Ruhong, Chai, Zhifang, Albrecht-Schmitt, Thomas E., Liu, Ning, and Wang, Shuao. Fri . "Facile and Efficient Decontamination of Thorium from Rare Earths Based on Selective Selenite Crystallization". United States. doi:10.1021/acs.inorgchem.7b02681. https://www.osti.gov/servlets/purl/1470227.
@article{osti_1470227,
title = {Facile and Efficient Decontamination of Thorium from Rare Earths Based on Selective Selenite Crystallization},
author = {Wang, Yaxing and Lu, Huangjie and Dai, Xing and Duan, Tao and Bai, Xiaojing and Cai, Yawen and Yin, Xuemiao and Chen, Lanhua and Diwu, Juan and Du, Shiyu and Zhou, Ruhong and Chai, Zhifang and Albrecht-Schmitt, Thomas E. and Liu, Ning and Wang, Shuao},
abstractNote = {The coexistence of radioactive contaminants (e.g., thorium, uranium, and their daughters) in rare earth minerals introduces significant environmental, economic, and technological hurdles in modern rare earth production. Capable, low cost, and green decontamination strategies are therefore desired to ameliorate this problem. In this work, we report a single-step and quantitative decontamination strategy of thorium from rare earths based on a unique periodic trend in the formation of crystalline selenite compounds across the lanthanide series, where Ce(III) is fully oxidized in situ to Ce(IV). This gives rise to a crystallization system that is highly selective to trap tetravalent f-blocks while all other trivalent lanthanides completely remain in solution when coexist. These findings are bolstered by first-principles calculations of lattice energies and an examination of bonding in these compounds. This system is contrasted with typical natural and synthetic systems, where trivalent and tetravalent f-block elements often cocrystallize. The separation factors after one round of crystallization were determined from binary systems of Th(IV)/La(III), Th(IV)/Eu(III), and Th(IV)/Yb(III) to reach 2.1 × 105, 1.2 × 105, and 9 × 104, respectively. Selective crystallization of thorium from a simulated monazite composite yields a separation factor of 1.9 × 103 with nearly quantitative removal of thorium.},
doi = {10.1021/acs.inorgchem.7b02681},
journal = {Inorganic Chemistry},
number = 4,
volume = 57,
place = {United States},
year = {2018},
month = {2}
}

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