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Title: Extraction of Lanthanide and Actinide Ions from Aqueous Mixtures Using a Carboxylic Acid-Functionalized Porous Aromatic Framework

Abstract

Porous aromatic frameworks (PAFs) incorporating a high concentration of acid functional groups possess characteristics that are promising for use in separating lanthanide and actinide metal ions, as required in the treatment of radioactive waste. These materials have been shown to be indefinitely stable to concentrated acids and bases, potentially allowing for multiple adsorption/stripping cycles. Additionally, the PAFs combine exceptional features from MOFs and inorganic/ activated carbons giving rise to tunable pore surfaces and maximum chemical stability. Herein, we present a study of the adsorption of selected metal ions, Sr2+, Fe3+, Nd3+, and Am3+, from aqueous solutions employing a carbon-based porous aromatic framework, BPP-7 (Berkeley Porous Polymer-7). This material displays high metal loading capacities together with excellent adsorption selectivity for neodymium over strontium based on Langmuir adsorption isotherms and ideal adsorbed solution theory (IAST) calculations. Based in part upon X-ray absorption spectroscopy studies, the stronger adsorption of neodymium is attributed to multiple metal ion and binding site interactions resulting from the densely functionalized and highly interpenetrated structure of BPP-7. Finally, recyclability and combustibility experiments demonstrate that multiple adsorption/stripping cycles can be completed with minimal degradation of the polymer adsorption capacity.

Authors:
; ; ; ;  [1]; ;  [2]; ; ;  [3];  [3];  [1];  [3]; ;
  1. Chemistry Department, Lomonosov Moscow State University, Leninskie Gory, Moscow 11991, Russia
  2. Radiochemistry Department, China Institute of Atomic Energy, Beijing 102413, China
  3. Actinide Chemistry Group, Energy and Environment Science Division, Quantum Beam Science Center, Japan Atomic Energy Agency, 1-1-1 Kouto, Sayo-cho, Sayo-gun, Hyogo 679-5148, Japan
Publication Date:
Research Org.:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1247030
Alternate Identifier(s):
OSTI ID: 1435066
Grant/Contract Number:  
AC02-05CH11231; SC0001015
Resource Type:
Journal Article: Published Article
Journal Name:
ACS Central Science
Additional Journal Information:
Journal Name: ACS Central Science Journal Volume: 2 Journal Issue: 4; Journal ID: ISSN 2374-7943
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE

Citation Formats

Demir, Selvan, Brune, Nicholas K., Van Humbeck, Jeffrey F., Mason, Jarad A., Plakhova, Tatiana V., Wang, Shuao, Tian, Guoxin, Minasian, Stefan G., Tyliszczak, Tolek, Yaita, Tsuyoshi, Kobayashi, Tohru, Kalmykov, Stepan N., Shiwaku, Hideaki, Shuh, David K., and Long, Jeffrey R. Extraction of Lanthanide and Actinide Ions from Aqueous Mixtures Using a Carboxylic Acid-Functionalized Porous Aromatic Framework. United States: N. p., 2016. Web. doi:10.1021/acscentsci.6b00066.
Demir, Selvan, Brune, Nicholas K., Van Humbeck, Jeffrey F., Mason, Jarad A., Plakhova, Tatiana V., Wang, Shuao, Tian, Guoxin, Minasian, Stefan G., Tyliszczak, Tolek, Yaita, Tsuyoshi, Kobayashi, Tohru, Kalmykov, Stepan N., Shiwaku, Hideaki, Shuh, David K., & Long, Jeffrey R. Extraction of Lanthanide and Actinide Ions from Aqueous Mixtures Using a Carboxylic Acid-Functionalized Porous Aromatic Framework. United States. https://doi.org/10.1021/acscentsci.6b00066
Demir, Selvan, Brune, Nicholas K., Van Humbeck, Jeffrey F., Mason, Jarad A., Plakhova, Tatiana V., Wang, Shuao, Tian, Guoxin, Minasian, Stefan G., Tyliszczak, Tolek, Yaita, Tsuyoshi, Kobayashi, Tohru, Kalmykov, Stepan N., Shiwaku, Hideaki, Shuh, David K., and Long, Jeffrey R. 2016. "Extraction of Lanthanide and Actinide Ions from Aqueous Mixtures Using a Carboxylic Acid-Functionalized Porous Aromatic Framework". United States. https://doi.org/10.1021/acscentsci.6b00066.
@article{osti_1247030,
title = {Extraction of Lanthanide and Actinide Ions from Aqueous Mixtures Using a Carboxylic Acid-Functionalized Porous Aromatic Framework},
author = {Demir, Selvan and Brune, Nicholas K. and Van Humbeck, Jeffrey F. and Mason, Jarad A. and Plakhova, Tatiana V. and Wang, Shuao and Tian, Guoxin and Minasian, Stefan G. and Tyliszczak, Tolek and Yaita, Tsuyoshi and Kobayashi, Tohru and Kalmykov, Stepan N. and Shiwaku, Hideaki and Shuh, David K. and Long, Jeffrey R.},
abstractNote = {Porous aromatic frameworks (PAFs) incorporating a high concentration of acid functional groups possess characteristics that are promising for use in separating lanthanide and actinide metal ions, as required in the treatment of radioactive waste. These materials have been shown to be indefinitely stable to concentrated acids and bases, potentially allowing for multiple adsorption/stripping cycles. Additionally, the PAFs combine exceptional features from MOFs and inorganic/ activated carbons giving rise to tunable pore surfaces and maximum chemical stability. Herein, we present a study of the adsorption of selected metal ions, Sr2+, Fe3+, Nd3+, and Am3+, from aqueous solutions employing a carbon-based porous aromatic framework, BPP-7 (Berkeley Porous Polymer-7). This material displays high metal loading capacities together with excellent adsorption selectivity for neodymium over strontium based on Langmuir adsorption isotherms and ideal adsorbed solution theory (IAST) calculations. Based in part upon X-ray absorption spectroscopy studies, the stronger adsorption of neodymium is attributed to multiple metal ion and binding site interactions resulting from the densely functionalized and highly interpenetrated structure of BPP-7. Finally, recyclability and combustibility experiments demonstrate that multiple adsorption/stripping cycles can be completed with minimal degradation of the polymer adsorption capacity.},
doi = {10.1021/acscentsci.6b00066},
url = {https://www.osti.gov/biblio/1247030}, journal = {ACS Central Science},
issn = {2374-7943},
number = 4,
volume = 2,
place = {United States},
year = {Tue Apr 12 00:00:00 EDT 2016},
month = {Tue Apr 12 00:00:00 EDT 2016}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record at https://doi.org/10.1021/acscentsci.6b00066

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Cited by: 97 works
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