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Title: Overcoming the crystallization and designability issues in the ultrastable zirconium phosphonate framework system

Abstract

Metal-organic frameworks (MOFs) based on zirconium phosphonates exhibit superior chemical stability suitable for applications under harsh conditions. These compounds mostly exist as poorly crystallized precipitates, and precise structural information has therefore remained elusive. Furthermore, a zero-dimensional zirconium phosphonate cluster acting as secondary building unit has been lacking, leading to poor designability in this system. We overcome these challenges and obtain single crystals of three zirconium phosphonates that are suitable for structural analysis. Furthermore, these compounds are built by previously unknown isolated zirconium phosphonate clusters and exhibit combined high porosity and ultrastability even in fuming acids. SZ-2 possesses the largest void volume recorded in zirconium phosphonates and SZ-3 represents the most porous crystalline zirconium phosphonate and the only porous MOF material reported to survive in aqua regia. SZ-2 and SZ-3 can effectively remove uranyl ions from aqueous solutions over a wide pH range, and we have elucidated the removal mechanism.

Authors:
ORCiD logo [1]; ORCiD logo [2];  [2];  [2];  [2];  [2];  [2];  [3];  [2];  [2];  [2];  [2];  [2];  [3]; ORCiD logo [4];  [2];  [5];  [2]
+ Show Author Affiliations
  1. Soochow Univ., Jiangsu (China). Collaborative Innovation Center of Radiation Medicine of Jiangsu Higher Education Institutions; Nanjing Univ. of Science and Technology (China). School of Environment and Biological Engineering
  2. Soochow Univ., Jiangsu (China). Collaborative Innovation Center of Radiation Medicine of Jiangsu Higher Education Institutions
  3. Chinese Academy of Sciences (CAS), Beijing (China). Shanghai Inst. of Applied Physics and Key Lab. of Nuclear Radiation and Nuclear Energy Technology
  4. Soochow Univ., Jiangsu (China). Collaborative Innovation Center of Radiation Medicine of Jiangsu Higher Education Institutions; IBM Thomas J. Watson Research Center, Yorktown Heights, NY (United States). Computational Biology Center; Columbia Univ., New York, NY (United States). Dept. of Chemistry
  5. Florida State Univ., Tallahassee, FL (United States). Dept. of Chemistry and Biochemistry
Publication Date:
Research Org.:
Florida State Univ., Tallahassee, FL (United States); Energy Frontier Research Centers (EFRC) (United States). Center for Actinide Science & Technology (CAST)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1389275
Grant/Contract Number:  
SC0016568
Resource Type:
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; metal-organic frameworks; solid-state chemistry

Citation Formats

Zheng, Tao, Yang, Zaixing, Gui, Daxiang, Liu, Zhiyong, Wang, Xiangxiang, Dai, Xing, Liu, Shengtang, Zhang, Linjuan, Gao, Yang, Chen, Lanhua, Sheng, Daopeng, Wang, Yanlong, Diwu, Juan, Wang, Jianqiang, Zhou, Ruhong, Chai, Zhifang, Albrecht-Schmitt, Thomas E., and Wang, Shuao. Overcoming the crystallization and designability issues in the ultrastable zirconium phosphonate framework system. United States: N. p., 2017. Web. doi:10.1038/ncomms15369.
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Zheng, Tao, Yang, Zaixing, Gui, Daxiang, Liu, Zhiyong, Wang, Xiangxiang, Dai, Xing, Liu, Shengtang, Zhang, Linjuan, Gao, Yang, Chen, Lanhua, Sheng, Daopeng, Wang, Yanlong, Diwu, Juan, Wang, Jianqiang, Zhou, Ruhong, Chai, Zhifang, Albrecht-Schmitt, Thomas E., & Wang, Shuao. Overcoming the crystallization and designability issues in the ultrastable zirconium phosphonate framework system. United States. https://doi.org/10.1038/ncomms15369
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Zheng, Tao, Yang, Zaixing, Gui, Daxiang, Liu, Zhiyong, Wang, Xiangxiang, Dai, Xing, Liu, Shengtang, Zhang, Linjuan, Gao, Yang, Chen, Lanhua, Sheng, Daopeng, Wang, Yanlong, Diwu, Juan, Wang, Jianqiang, Zhou, Ruhong, Chai, Zhifang, Albrecht-Schmitt, Thomas E., and Wang, Shuao. Tue . "Overcoming the crystallization and designability issues in the ultrastable zirconium phosphonate framework system". United States. https://doi.org/10.1038/ncomms15369. https://www.osti.gov/servlets/purl/1389275.
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@article{osti_1389275,
title = {Overcoming the crystallization and designability issues in the ultrastable zirconium phosphonate framework system},
author = {Zheng, Tao and Yang, Zaixing and Gui, Daxiang and Liu, Zhiyong and Wang, Xiangxiang and Dai, Xing and Liu, Shengtang and Zhang, Linjuan and Gao, Yang and Chen, Lanhua and Sheng, Daopeng and Wang, Yanlong and Diwu, Juan and Wang, Jianqiang and Zhou, Ruhong and Chai, Zhifang and Albrecht-Schmitt, Thomas E. and Wang, Shuao},
abstractNote = {Metal-organic frameworks (MOFs) based on zirconium phosphonates exhibit superior chemical stability suitable for applications under harsh conditions. These compounds mostly exist as poorly crystallized precipitates, and precise structural information has therefore remained elusive. Furthermore, a zero-dimensional zirconium phosphonate cluster acting as secondary building unit has been lacking, leading to poor designability in this system. We overcome these challenges and obtain single crystals of three zirconium phosphonates that are suitable for structural analysis. Furthermore, these compounds are built by previously unknown isolated zirconium phosphonate clusters and exhibit combined high porosity and ultrastability even in fuming acids. SZ-2 possesses the largest void volume recorded in zirconium phosphonates and SZ-3 represents the most porous crystalline zirconium phosphonate and the only porous MOF material reported to survive in aqua regia. SZ-2 and SZ-3 can effectively remove uranyl ions from aqueous solutions over a wide pH range, and we have elucidated the removal mechanism.},
doi = {10.1038/ncomms15369},
journal = {Nature Communications},
number = ,
volume = 8,
place = {United States},
year = {2017},
month = {5}
}
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Figures / Tables:

Figure 1 Figure 1: Crystal structure and network topology of SZ-1. The Tppm ligand (a) is connected to four 8-connected Zr5P8 clusters (b) to generate a 3D network with a sieve-like layered structure in the bc plane (c–e). Colour scheme: Zr, green; P, purple; C, grey.
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    • Zhao, Shilei; Yuan, Yihui; Yu, Qiuhan
    • Angewandte Chemie International Edition, Vol. 58, Issue 42
    • DOI: 10.1002/anie.201908762

    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

    A Bio‐inspired Nano‐pocket Spatial Structure for Targeting Uranyl Capture
    journal, January 2020

    • Yuan, Yihui; Feng, Shiwei; Feng, Lijuan
    • Angewandte Chemie International Edition, Vol. 59, Issue 11
    • DOI: 10.1002/anie.201916450

    Ionothermal Synthesis of Hollow Aluminophosphate Molecular Sieves
    journal, May 2018

    • Feng, Jie; Wang, Jianfeng; Wang, Zheng
    • Particle & Particle Systems Characterization, Vol. 35, Issue 7
    • DOI: 10.1002/ppsc.201800125

    Synthesis of Some Di- and Tetraphosphonic Acids by Suzuki Cross-Coupling: Synthesis of Some Di- and Tetraphosphonic Acids by Suzuki Cross-Coupling
    journal, July 2018

    • Schütrumpf, Alexandra; Duthie, Andrew; Lork, Enno
    • Zeitschrift für anorganische und allgemeine Chemie, Vol. 644, Issue 19
    • DOI: 10.1002/zaac.201800197

    Phosphonate modified MoS2 composite material for effective adsorption of uranium(VI) in aqueous solution
    journal, December 2019

    • Kou, Ying; Zhang, Ling; Liu, Bo
    • Journal of Radioanalytical and Nuclear Chemistry, Vol. 323, Issue 1
    • DOI: 10.1007/s10967-019-06970-3

    Synthesis of ordered mesoporous carbonaceous materials and their highly efficient capture of uranium from solutions
    journal, December 2017

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

    Crystalline and permanently porous porphyrin-based metal tetraphosphonates
    journal, January 2018

    • Rhauderwiek, Timo; Wolkersdörfer, Konrad; Øien-Ødegaard, Sigurd
    • Chemical Communications, Vol. 54, Issue 4
    • DOI: 10.1039/c7cc07766a

    Insight into selectivity: uptake studies of radionuclides 90 Sr 2+ , 137 Cs + , and 233 UO 2 2+ with bis-amidoxime polymers
    journal, January 2018

    • Piechowicz, Marek; Chiarizia, R.; Soderholm, L.
    • Dalton Transactions, Vol. 47, Issue 15
    • DOI: 10.1039/c7dt04935h

    Constructing semiconductive crystalline microporous materials by Coulomb interactions
    journal, January 2017

    • Wang, Guan-E; Yao, Ming-Shui; Cai, Min-Lan
    • Journal of Materials Chemistry A, Vol. 5, Issue 35
    • DOI: 10.1039/c7ta05805e

    An easily synthesized microporous framework material for the selective capture of radioactive Cs + and Sr 2+ ions
    journal, January 2018

    • Gao, Yu-Jie; Feng, Mei-Ling; Zhang, Bo
    • Journal of Materials Chemistry A, Vol. 6, Issue 9
    • DOI: 10.1039/c7ta11208d

    Destabilization of DNA through interstrand crosslinking by UO 2 2+
    journal, January 2019

    • Rossberg, André; Abe, Takaya; Okuwaki, Koji
    • Chemical Communications, Vol. 55, Issue 14
    • DOI: 10.1039/c8cc09329f

    A uranyl phosphonate framework with a temperature-induced order–disorder transition and temperature-correlated photoluminescence
    journal, January 2018

    • Wang, Yi; Wang, Xiangxiang; Zhang, Dongya
    • CrystEngComm, Vol. 20, Issue 23
    • DOI: 10.1039/c8ce00450a

    Single-crystal-to-single-crystal desolvation in a Ti 32 nanoring cluster
    journal, January 2018

    • Wang, Xiangxiang; Gui, Daxiang; Zhai, Fuwan
    • CrystEngComm, Vol. 20, Issue 44
    • DOI: 10.1039/c8ce00717a

    Metal–organic framework as an efficient filter for the removal of heavy metal cations in water
    journal, January 2018

    • Gu, Zonglin; Song, Wei; Yang, Zaixing
    • Physical Chemistry Chemical Physics, Vol. 20, Issue 48
    • DOI: 10.1039/c8cp05129a

    An ingenious one-dimensional zirconium phosphonate with efficient strontium exchange capability and moderate proton conductivity
    journal, January 2018

    • Zhang, Jiarong; Chen, Lanhua; Gui, Daxiang
    • Dalton Transactions, Vol. 47, Issue 15
    • DOI: 10.1039/c8dt00508g

    Core–shell hierarchical C@Na 2 Ti 3 O 7 ·9H 2 O nanostructures for the efficient removal of radionuclides
    journal, January 2018

    • Tan, Xiaoli; Fang, Ming; Tan, Liqiang
    • Environmental Science: Nano, Vol. 5, Issue 5
    • DOI: 10.1039/c8en00149a

    Retracted Article: Plasma-grafted amidoxime/metal–organic framework composites for the selective sequestration of U( vi )
    journal, January 2018

    • Li, Fengbo; Li, Xiaoyu; Cui, Pu
    • Environmental Science: Nano, Vol. 5, Issue 8
    • DOI: 10.1039/c8en00583d

    Retracted Article: Mutual effect of Cs( i ) and Sr( ii ) sorption on nano-talc investigated by EXAFS, modeling and theoretical calculations
    journal, January 2019

    • Sun, Yubing; Song, Wencheng; Liu, Yang
    • Environmental Science: Nano, Vol. 6, Issue 2
    • DOI: 10.1039/c8en01313f

    A water-stable Ni( ii ) diphosphonate exhibiting water vapor adsorption and water-assisted high proton conductivity
    journal, January 2019

    • Xu, Hailong; Feng, Lu; Huang, Wentao
    • New Journal of Chemistry, Vol. 43, Issue 2
    • DOI: 10.1039/c8nj04776f

    Highly efficient Pb( ii ) and Cu( ii ) removal using hollow Fe 3 O 4 @PDA nanoparticles with excellent application capability and reusability
    journal, January 2018

    • Wang, Ning; Yang, Dongxu; Wang, Xiangxue
    • Inorganic Chemistry Frontiers, Vol. 5, Issue 9
    • DOI: 10.1039/c8qi00541a

    Highly stable and porous porphyrin-based zirconium and hafnium phosphonates – electron crystallography as an important tool for structure elucidation
    journal, January 2018

    • Rhauderwiek, Timo; Zhao, Haishuang; Hirschle, Patrick
    • Chemical Science, Vol. 9, Issue 24
    • DOI: 10.1039/c8sc01533c

    Metal–organic framework technologies for water remediation: towards a sustainable ecosystem
    journal, January 2018

    • Mon, Marta; Bruno, Rosaria; Ferrando-Soria, Jesus
    • Journal of Materials Chemistry A, Vol. 6, Issue 12
    • DOI: 10.1039/c8ta00264a

    Zinc-diphosphonates with extended dipyridine units: synthesis, structures, in situ reactions, and photochromism
    journal, January 2019

    • Liu, Hao-Hao; Ma, Yu-Juan; Han, Song-De
    • Dalton Transactions, Vol. 48, Issue 12
    • DOI: 10.1039/c9dt00081j

    Selective Th( iv ) capture from a new metal–organic framework with O − groups
    journal, January 2020

    • Guo, Xiang-Guang; Su, Jia; Xie, Wen-Qi
    • Dalton Transactions, Vol. 49, Issue 13
    • DOI: 10.1039/c9dt04912f

    Construction of novel phosphonate-based MOF/P–TiO 2 heterojunction photocatalysts: enhanced photocatalytic performance and mechanistic insight
    journal, January 2020

    • Zeng, Tianyu; Shi, Dajun; Cheng, Qingrong
    • Environmental Science: Nano, Vol. 7, Issue 3
    • DOI: 10.1039/c9en01180c

    Metal–organic framework-based materials for the recovery of uranium from aqueous solutions
    journal, January 2019

    • Yang, Weiting; Pan, Qinhe; Song, Shuyan
    • Inorganic Chemistry Frontiers, Vol. 6, Issue 8
    • DOI: 10.1039/c9qi00386j

    Interaction of U( vi ) with α-MnO 2 @layered double hydroxides by combined batch experiments and spectroscopy studies
    journal, January 2020

    • Ma, Junping; Wang, Chen; Zhao, Qiuyu
    • Inorganic Chemistry Frontiers, Vol. 7, Issue 2
    • DOI: 10.1039/c9qi01316d

    Fabrication of magnetic functionalised calix[4]arene composite for highly efficient and selective adsorption towards uranium(VI)
    journal, January 2019

    • Xiao, Fang-Zhu; Wang, Cheng; Yu, Li-Mei
    • Environmental Chemistry, Vol. 16, Issue 8
    • DOI: 10.1071/en19014

    New Directions in Metal Phosphonate and Phosphinate Chemistry
    journal, May 2019

    • Shearan, Stephen J. I.; Stock, Norbert; Emmerling, Franziska
    • Crystals, Vol. 9, Issue 5
    • DOI: 10.3390/cryst9050270

    Extraction of Metal Ions with Metal–Organic Frameworks
    journal, December 2019

    • Manousi, Natalia; Giannakoudakis, Dimitrios A.; Rosenberg, Erwin
    • Molecules, Vol. 24, Issue 24
    • DOI: 10.3390/molecules24244605

    Remarkable Acid Stability of Polypyrrole-MoS 4 : A Highly Selective and Efficient Scavenger of Heavy Metals Over a Wide pH Range
    journal, March 2018

    • Xie, Linxia; Yu, Zihuan; Islam, Saiful M.
    • Advanced Functional Materials, Vol. 28, Issue 20
    • DOI: 10.1002/adfm.201800502

    Photoinduced Multiple Effects to Enhance Uranium Extraction from Natural Seawater by Black Phosphorus Nanosheets
    journal, November 2019

    Flexible Metal-Organic Framework-Based Mixed-Matrix Membranes: A New Platform for H 2 S Sensors
    journal, July 2018

    A phase transformable ultrastable titanium-carboxylate framework for photoconduction
    journal, April 2018

    Metal–organic framework-based materials: superior adsorbents for the capture of toxic and radioactive metal ions
    journal, January 2018

    • Li, Jie; Wang, Xiangxue; Zhao, Guixia
    • Chemical Society Reviews, Vol. 47, Issue 7
    • DOI: 10.1039/c7cs00543a

    Two novel organic phosphorous-based MOFs: synthesis, characterization and photocatalytic properties
    journal, January 2019

    • Zeng, Tianyu; Wang, Liwen; Feng, Lu
    • Dalton Transactions, Vol. 48, Issue 2
    • DOI: 10.1039/c8dt04106g

    Superhydrophilic phosphate and amide functionalized magnetic adsorbent: a new combination of anti-biofouling and uranium extraction from seawater
    journal, January 2018

    • Guo, Xuejie; Chen, Rongrong; Liu, Qi
    • Environmental Science: Nano, Vol. 5, Issue 10
    • DOI: 10.1039/c8en00545a

    Retracted Article: The influence of nanoscale size on the adsorption–desorption of U( vi ) on nano-Al oxides
    journal, January 2018

    • Wan, Tian; Cheng, Wen; Ren, Jiehui
    • Environmental Science: Nano, Vol. 5, Issue 11
    • DOI: 10.1039/c8en00912k

    Macroscopic and microscopic investigation of uranium elimination by Ca–Mg–Al-layered double hydroxide supported nanoscale zero valent iron
    journal, January 2018

    • Pang, Hongwei; Wu, Yihan; Huang, Shuyi
    • Inorganic Chemistry Frontiers, Vol. 5, Issue 10
    • DOI: 10.1039/c8qi00779a

    Aqueous-phase detection of antibiotics and nitroaromatic explosives by an alkali-resistant Zn-MOF directed by an ionic liquid
    journal, January 2020

    • Qin, Jian-Hua; Huang, Ya-Dan; Shi, Ming-Yu
    • RSC Advances, Vol. 10, Issue 3
    • DOI: 10.1039/c9ra08733h

    Ammoniating Covalent Organic Framework (COF) for High‐Performance and Selective Extraction of Toxic and Radioactive Uranium Ions
    journal, June 2019

    A Dual‐Surface Amidoximated Halloysite Nanotube for High‐Efficiency Economical Uranium Extraction from Seawater
    journal, September 2019

    Photoinduced Multiple Effects to Enhance Uranium Extraction from Natural Seawater by Black Phosphorus Nanosheets
    journal, December 2019

    • Yuan, Yihui; Niu, Biye; Yu, Qiuhan
    • Angewandte Chemie International Edition, Vol. 59, Issue 3
    • DOI: 10.1002/anie.201913644

    Phosphatidyl-assisted fabrication of graphene oxide nanosheets with multiple active sites for uranium( vi ) capture
    journal, January 2018

    • Yang, Peipei; Liu, Qi; Zhang, Hongsen
    • Environmental Science: Nano, Vol. 5, Issue 7
    • DOI: 10.1039/c8en00401c

    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, Vol. 131, Issue 52
    • DOI: 10.1002/ange.201909045

    Regenerable and stable sp2 carbon-conjugated covalent organic frameworks for selective detection and extraction of uranium
    journal, January 2020

    Hollow cobalt sulfide for highly efficient uranium adsorption from aqueous solutions
    journal, January 2019

    • Dou, Weixin; Yang, Weiting; Zhao, Xiaojun
    • Inorganic Chemistry Frontiers, Vol. 6, Issue 11
    • DOI: 10.1039/c9qi00737g

    Highly Sensitive Determination of Bisphenol A in Bottled Water Samples by HPLC after Its Extraction by a Novel Th-MOF Pipette-Tip Micro-SPE
    journal, December 2019

    • Kaykhaii, Massoud; Yavari, Eilnaz; Sargazi, Ghasem
    • Journal of Chromatographic Science, Vol. 58, Issue 4
    • DOI: 10.1093/chromsci/bmz111

    A Bio‐inspired Nano‐pocket Spatial Structure for Targeting Uranyl Capture
    journal, March 2020

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