Search Menu
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information
Search Scholarly Publications

Title: Rational Construction of Porous Metal–Organic Frameworks for Uranium(VI) Extraction: The Strong Periodic Tendency with a Metal Node

Abstract

Although metal-organic frameworks (MOFs) have been reported as important porous materials for the potential utility in metal ion separation, coordinating the functionality, structure, and component of MOFs remains a great challenge. Herein, a series of anionic rare earth MOFs (RE-MOFs) were synthesized via a solvothermal template reaction and for the first time explored for uranium(VI) capture from an acidic medium. The unusually high extraction capacity of UO22+ (e.g., 538 mg U per g of Y-MOF) was achieved through ion-exchange with the concomitant release of Me2NH2+, during which the uranium(VI) extraction in the series of isostructural RE-MOFs was found to be highly sensitive to the ionic radii of the metal nodes. That is, the uranium(VI) adsorption capacities continuously increased as the ionic radii decreased. Finally, in-depth mechanism insight was obtained from molecular dynamics simulations, suggesting that both the accessible pore volume of the MOFs and hydrogen-bonding interactions contribute to the strong periodic tendency of uranium(VI) extraction.

Authors:
ORCiD logo [1];  [2]; ORCiD logo [2];  [1];  [1];  [2];  [1];  [3]; ORCiD logo [4]; ORCiD logo [2]
+ Show Author Affiliations
  1. Changzhou Univ. (China)
  2. Chinese Academy of Sciences (CAS), Beijing (China)
  3. Chinese Academy of Sciences (CAS), Beijing (China); Chinese Academy of Sciences (CAS), Zhejiang (China)
  4. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Center for Actinide Science & Technology (CAST); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Natural Science Foundation of China (NSFC); Youth Innovation Promotion Association; Jiangsu Higher Education Institution
OSTI Identifier:
1642681
Grant/Contract Number:  
AC02-05CH11231; 11775037; 21777161; 21836001; 21806167; 19KJA150001; SC0016568
Resource Type:
Accepted Manuscript
Journal Name:
ACS Applied Materials and Interfaces
Additional Journal Information:
Journal Volume: 12; Journal Issue: 12; Journal ID: ISSN 1944-8244
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; periodic tendency; rare earth MOFs; adsorption; uranium; ionic radii

Citation Formats

Zhang, Zhi-Hui, Lan, Jian-Hui, Yuan, Li-Yong, Sheng, Pan-Pan, He, Ming-Yang, Zheng, Li-Rong, Chen, Qun, Chai, Zhi-Fang, Gibson, John K., and Shi, Wei-Qun. Rational Construction of Porous Metal–Organic Frameworks for Uranium(VI) Extraction: The Strong Periodic Tendency with a Metal Node. United States: N. p., 2020. Web. doi:10.1021/acsami.0c02121.
Copy to clipboard
Zhang, Zhi-Hui, Lan, Jian-Hui, Yuan, Li-Yong, Sheng, Pan-Pan, He, Ming-Yang, Zheng, Li-Rong, Chen, Qun, Chai, Zhi-Fang, Gibson, John K., & Shi, Wei-Qun. Rational Construction of Porous Metal–Organic Frameworks for Uranium(VI) Extraction: The Strong Periodic Tendency with a Metal Node. United States. https://doi.org/10.1021/acsami.0c02121
Copy to clipboard
Zhang, Zhi-Hui, Lan, Jian-Hui, Yuan, Li-Yong, Sheng, Pan-Pan, He, Ming-Yang, Zheng, Li-Rong, Chen, Qun, Chai, Zhi-Fang, Gibson, John K., and Shi, Wei-Qun. Fri . "Rational Construction of Porous Metal–Organic Frameworks for Uranium(VI) Extraction: The Strong Periodic Tendency with a Metal Node". United States. https://doi.org/10.1021/acsami.0c02121. https://www.osti.gov/servlets/purl/1642681.
Copy to clipboard
@article{osti_1642681,
title = {Rational Construction of Porous Metal–Organic Frameworks for Uranium(VI) Extraction: The Strong Periodic Tendency with a Metal Node},
author = {Zhang, Zhi-Hui and Lan, Jian-Hui and Yuan, Li-Yong and Sheng, Pan-Pan and He, Ming-Yang and Zheng, Li-Rong and Chen, Qun and Chai, Zhi-Fang and Gibson, John K. and Shi, Wei-Qun},
abstractNote = {Although metal-organic frameworks (MOFs) have been reported as important porous materials for the potential utility in metal ion separation, coordinating the functionality, structure, and component of MOFs remains a great challenge. Herein, a series of anionic rare earth MOFs (RE-MOFs) were synthesized via a solvothermal template reaction and for the first time explored for uranium(VI) capture from an acidic medium. The unusually high extraction capacity of UO22+ (e.g., 538 mg U per g of Y-MOF) was achieved through ion-exchange with the concomitant release of Me2NH2+, during which the uranium(VI) extraction in the series of isostructural RE-MOFs was found to be highly sensitive to the ionic radii of the metal nodes. That is, the uranium(VI) adsorption capacities continuously increased as the ionic radii decreased. Finally, in-depth mechanism insight was obtained from molecular dynamics simulations, suggesting that both the accessible pore volume of the MOFs and hydrogen-bonding interactions contribute to the strong periodic tendency of uranium(VI) extraction.},
doi = {10.1021/acsami.0c02121},
journal = {ACS Applied Materials and Interfaces},
number = 12,
volume = 12,
place = {United States},
year = {Fri Feb 28 00:00:00 EST 2020},
month = {Fri Feb 28 00:00:00 EST 2020}
}
Copy to clipboard
Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1021/acsami.0c02121
Copyright Statement
Other availability
Search WorldCat Search WorldCat to find libraries that may hold this journal
Citation Metrics:
Cited by: 36 works
Citation information provided by
Web of Science
Save / Share:
Export Metadata
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.

Works referenced in this record:

Systematic Design of Pore Size and Functionality in Isoreticular MOFs and Their Application in Methane Storage
journal, January 2002

  • Eddaoudi, Mohamed; Kim, Jaheon; Rosi, Nathaniel
  • Science, Vol. 295, Issue 5554, p. 469-472
  • DOI: 10.1126/science.1067208

Metal–Organic Frameworks for Analytical Chemistry: From Sample Collection to Chromatographic Separation
journal, January 2012

  • Gu, Zhi-Yuan; Yang, Cheng-Xiong; Chang, Na
  • Accounts of Chemical Research, Vol. 45, Issue 5
  • DOI: 10.1021/ar2002599

Dynamic Spacer Installation for Multirole Metal–Organic Frameworks: A New Direction toward Multifunctional MOFs Achieving Ultrahigh Methane Storage Working Capacity
journal, April 2017

  • Chen, Cheng-Xia; Wei, Zhang-Wen; Jiang, Ji-Jun
  • Journal of the American Chemical Society, Vol. 139, Issue 17
  • DOI: 10.1021/jacs.7b01320

UTSA-74: A MOF-74 Isomer with Two Accessible Binding Sites per Metal Center for Highly Selective Gas Separation
journal, April 2016

  • Luo, Feng; Yan, Changsheng; Dang, Lilong
  • Journal of the American Chemical Society, Vol. 138, Issue 17
  • DOI: 10.1021/jacs.6b02030

High Methane Storage Working Capacity in Metal–Organic Frameworks with Acrylate Links
journal, August 2016

  • Jiang, Juncong; Furukawa, Hiroyasu; Zhang, Yue-Biao
  • Journal of the American Chemical Society, Vol. 138, Issue 32
  • DOI: 10.1021/jacs.6b05261

CD-MOF: A Versatile Separation Medium
journal, February 2016

  • Hartlieb, Karel J.; Holcroft, James M.; Moghadam, Peyman Z.
  • Journal of the American Chemical Society, Vol. 138, Issue 7
  • DOI: 10.1021/jacs.5b12860

Separation of Hexane Isomers in a Metal-Organic Framework with Triangular Channels
journal, May 2013

Hydrocarbon Separations in a Metal-Organic Framework with Open Iron(II) Coordination Sites
journal, March 2012

Design and Synthesis of a Water-Stable Anionic Uranium-Based Metal-Organic Framework (MOF) with Ultra Large Pores
journal, July 2016

  • Li, Peng; Vermeulen, Nicolaas A.; Gong, Xirui
  • Angewandte Chemie International Edition, Vol. 55, Issue 35
  • DOI: 10.1002/anie.201605547

Ethane/ethylene separation in a metal-organic framework with iron-peroxo sites
journal, October 2018

Engineering Metal Organic Frameworks for Heterogeneous Catalysis
journal, August 2010

  • Corma, A.; García, H.; Llabrés i Xamena, F. X.
  • Chemical Reviews, Vol. 110, Issue 8, p. 4606-4655
  • DOI: 10.1021/cr9003924

Flexible Porous Metal-Organic Frameworks for a Controlled Drug Delivery
journal, May 2008

  • Horcajada, Patricia; Serre, Christian; Maurin, Guillaume
  • Journal of the American Chemical Society, Vol. 130, Issue 21
  • DOI: 10.1021/ja710973k

Lanthanide–organic frameworks for gas storage and as magneto-luminescent materials
journal, August 2014

  • Roy, Syamantak; Chakraborty, Anindita; Maji, Tapas Kumar
  • Coordination Chemistry Reviews, Vol. 273-274
  • DOI: 10.1016/j.ccr.2014.03.035

Lanthanide Metal-Organic Framework Microrods: Colored Optical Waveguides and Chiral Polarized Emission
journal, May 2017

  • Yang, Xiaogang; Lin, Xianqing; Zhao, Yibing
  • Angewandte Chemie International Edition, Vol. 56, Issue 27
  • DOI: 10.1002/anie.201703917

Anionic Lanthanide MOFs as a Platform for Iron-Selective Sensing, Systematic Color Tuning, and Efficient Nanoparticle Catalysis
journal, January 2017

Lanthanide based tuning of luminescence in MOFs and dense frameworks – from mono- and multimetal systems to sensors and films
journal, January 2014

  • Meyer, L. V.; Schönfeld, F.; Müller-Buschbaum, K.
  • Chemical Communications, Vol. 50, Issue 60
  • DOI: 10.1039/c4cc00848k

2D and 3D photoreactive lanthanide MOFs of trans,trans-muconic acid
journal, January 2013

  • Michaelides, Adonis; Skoulika, Stavroula; Siskos, Michael G.
  • Chem. Commun., Vol. 49, Issue 10
  • DOI: 10.1039/c2cc36356a

Flexible lanthanide MOFs as highly selective and reusable liquid MeOH sorbents
journal, January 2013

  • Efthymiou, Constantinos G.; Kyprianidou, Eleni J.; Milios, Constantinos J.
  • Journal of Materials Chemistry A, Vol. 1, Issue 16
  • DOI: 10.1039/c3ta00115f

Metal–Organic Frameworks assembled from tetraphosphonic ligands and lanthanides
journal, January 2018

  • Firmino, Ana D. G.; Figueira, Flávio; Tomé, João P. C.
  • Coordination Chemistry Reviews, Vol. 355
  • DOI: 10.1016/j.ccr.2017.08.001

Tuning Intrinsic and Extrinsic Proton Conduction in Metal–Organic Frameworks by the Lanthanide Contraction
journal, October 2017

  • Wong, Norman E.; Ramaswamy, Padmini; Lee, Andrew S.
  • Journal of the American Chemical Society, Vol. 139, Issue 41
  • DOI: 10.1021/jacs.7b07987

Ionic metal-organic frameworks (iMOFs): Design principles and applications
journal, January 2016

  • Karmakar, Avishek; Desai, Aamod V.; Ghosh, Sujit K.
  • Coordination Chemistry Reviews, Vol. 307
  • DOI: 10.1016/j.ccr.2015.08.007

Unique Proton Dynamics in an Efficient MOF-Based Proton Conductor
journal, February 2017

  • Wei, Yong-Sheng; Hu, Xiao-Peng; Han, Zhen
  • Journal of the American Chemical Society, Vol. 139, Issue 9
  • DOI: 10.1021/jacs.6b12847

Materials for the Recovery of Uranium from Seawater
journal, June 2017

Separation of actinides from spent nuclear fuel: A review
journal, November 2016

U6+ Minerals and Inorganic Compounds: Insights into an Expanded Structural Hierarchy of Crystal Structures
journal, December 2005

Opportunities of Porous Organic Polymers for Radionuclide Sequestration
journal, June 2019

Design Strategies to Enhance Amidoxime Chelators for Uranium Recovery
journal, August 2019

  • Aguila, Briana; Sun, Qi; Cassady, Harper
  • ACS Applied Materials & Interfaces, Vol. 11, Issue 34
  • DOI: 10.1021/acsami.9b09532

Bio-inspired nano-traps for uranium extraction from seawater and recovery from nuclear waste
journal, April 2018

Quaternary Phosphonium-Grafted Porous Aromatic Framework for Preferential Uranium Adsorption in Alkaline Solution
journal, September 2019

  • Shen, Yinglin; Chu, Nini; Yang, Suliang
  • Industrial & Engineering Chemistry Research, Vol. 58, Issue 39
  • DOI: 10.1021/acs.iecr.9b03580

Skeleton Engineering of Homocoupled Conjugated Microporous Polymers for Highly Efficient Uranium Capture via Synergistic Coordination
journal, December 2019

  • Zhang, Lei; Pu, Ning; Yu, Boxuan
  • ACS Applied Materials & Interfaces, Vol. 12, Issue 3
  • DOI: 10.1021/acsami.9b20944

Functionalized Porous Aromatic Framework for Efficient Uranium Adsorption from Aqueous Solutions
journal, March 2017

  • Li, Baiyan; Sun, Qi; Zhang, Yiming
  • ACS Applied Materials & Interfaces, Vol. 9, Issue 14
  • DOI: 10.1021/acsami.7b01711

p K a -Directed Incorporation of Phosphonates into MOF-808 via Ligand Exchange: Stability and Adsorption Properties for Uranium
journal, August 2019

  • Zhang, Wen; Bu, An; Ji, Qingyuan
  • ACS Applied Materials & Interfaces, Vol. 11, Issue 37
  • DOI: 10.1021/acsami.9b10920

Nano-MOF + Technique for Efficient Uranyl Remediation
journal, May 2019

  • Xu, Lin; Zhang, Duo; Ma, Fuyin
  • ACS Applied Materials & Interfaces, Vol. 11, Issue 24
  • DOI: 10.1021/acsami.9b06068

Cooperative Capture of Uranyl Ions by a Carbonyl-Bearing Hierarchical-Porous Cu-Organic Framework
journal, November 2019

  • Wang, Xiao-Feng; Chen, Yangyang; Song, Li-Ping
  • Angewandte Chemie International Edition, Vol. 58, Issue 52
  • DOI: 10.1002/anie.201909045

Facile construction of Fe@ zeolite imidazolate Framework-67 to selectively remove uranyl ions from aqueous solution
journal, October 2018

An anionic manganese( ii ) metal–organic framework for uranyl adsorption
journal, January 2019

  • Zhang, Tao; Ling, Bo-Kai; Hu, Yue-Qiao
  • CrystEngComm, Vol. 21, Issue 26
  • DOI: 10.1039/c9ce00603f

Synthesis of novel nanomaterials and their application in efficient removal of radionuclides
journal, June 2019

Metal–organic frameworks HKUST-1 for liquid-phase adsorption of uranium
journal, August 2013

  • Feng, Yafei; Jiang, Heng; Li, Songnan
  • Colloids and Surfaces A: Physicochemical and Engineering Aspects, Vol. 431
  • DOI: 10.1016/j.colsurfa.2013.04.032

MOF-76: from a luminescent probe to highly efficient UVI sorption material
journal, January 2013

  • Yang, Weiting; Bai, Zhi-Qiang; Shi, Wei-Qun
  • Chemical Communications, Vol. 49, Issue 88
  • DOI: 10.1039/c3cc44983a

A Combined Experimental and Theoretical Study on the Extraction of Uranium by Amino-Derived Metal–Organic Frameworks through Post-Synthetic Strategy
journal, November 2016

  • Li, Linnan; Ma, Wen; Shen, Sensen
  • ACS Applied Materials & Interfaces, Vol. 8, Issue 45
  • DOI: 10.1021/acsami.6b11332

U(VI) capture from aqueous solution by highly porous and stable MOFs: UiO-66 and its amine derivative
journal, April 2015

  • Luo, Bai-Cheng; Yuan, Li-Yong; Chai, Zhi-Fang
  • Journal of Radioanalytical and Nuclear Chemistry, Vol. 307, Issue 1
  • DOI: 10.1007/s10967-015-4108-3

Highly porous and stable metal–organic frameworks for uranium extraction
journal, January 2013

  • Carboni, Michaël; Abney, Carter W.; Liu, Shubin
  • Chemical Science, Vol. 4, Issue 6, p. 2396-2402
  • DOI: 10.1039/c3sc50230a

A Water-Stable Dual-Channel Luminescence Sensor for UO 2 2+ Ions Based on an Anionic Terbium(III) Metal-Organic Framework
journal, May 2017

  • Ye, Junwei; Bogale, Raji F.; Shi, Yangwei
  • Chemistry - A European Journal, Vol. 23, Issue 32
  • DOI: 10.1002/chem.201700713

Carboxylates of rare earth elements
journal, June 2017

  • Janicki, Rafał; Mondry, Anna; Starynowicz, Przemysław
  • Coordination Chemistry Reviews, Vol. 340
  • DOI: 10.1016/j.ccr.2016.12.001

Polymorphic Ln(iii) and BPTC-based porous metal–organic frameworks with visible, NIR photoluminescent and magnetic properties
journal, January 2014

  • Zhang, Liying; Song, Tianyou; Xu, Jianing
  • CrystEngComm, Vol. 16, Issue 12
  • DOI: 10.1039/c3ce42181c

UFF, a full periodic table force field for molecular mechanics and molecular dynamics simulations
journal, December 1992

  • Rappe, A. K.; Casewit, C. J.; Colwell, K. S.
  • Journal of the American Chemical Society, Vol. 114, Issue 25, p. 10024-10035
  • DOI: 10.1021/ja00051a040

Development and application of effective pairwise potentials for UO2n+, NpO2n+, PuO2n+, and AmO2n+ (n = 1, 2) ions with water
journal, January 2013

  • Pomogaev, Vladimir; Tiwari, Surya Prakash; Rai, Neeraj
  • Physical Chemistry Chemical Physics, Vol. 15, Issue 38
  • DOI: 10.1039/c3cp52444b

The missing term in effective pair potentials
journal, November 1987

  • Berendsen, H. J. C.; Grigera, J. R.; Straatsma, T. P.
  • The Journal of Physical Chemistry, Vol. 91, Issue 24
  • DOI: 10.1021/j100308a038

Numerical integration of the cartesian equations of motion of a system with constraints: molecular dynamics of n-alkanes
journal, March 1977

  • Ryckaert, Jean-Paul; Ciccotti, Giovanni; Berendsen, Herman J. C.
  • Journal of Computational Physics, Vol. 23, Issue 3
  • DOI: 10.1016/0021-9991(77)90098-5

A Chemical Route to Activation of Open Metal Sites in the Copper-Based Metal–Organic Framework Materials HKUST-1 and Cu-MOF-2
journal, July 2015

  • Kim, Hong Ki; Yun, Won Seok; Kim, Min-Bum
  • Journal of the American Chemical Society, Vol. 137, Issue 31
  • DOI: 10.1021/jacs.5b06637

Extending the Use of Highly Porous and Functionalized MOFs to Th(IV) Capture
journal, July 2017

  • Zhang, Nan; Yuan, Li-Yong; Guo, Wen-Lu
  • ACS Applied Materials & Interfaces, Vol. 9, Issue 30
  • DOI: 10.1021/acsami.7b04192

Efficient Removal and Recovery of Uranium by a Layered Organic–Inorganic Hybrid Thiostannate
journal, September 2016

  • Feng, Mei-Ling; Sarma, Debajit; Qi, Xing-Hui
  • Journal of the American Chemical Society, Vol. 138, Issue 38
  • DOI: 10.1021/jacs.6b07351
    Sort by:
    [ × clear filter / sort ]

    Similar Records in DOE PAGES and OSTI.GOV collections:

    Other research related to this record: