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

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

doi:10.1038/ncomms15369

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

Journal Article · Tue May 30 00:00:00 EDT 2017 · Nature Communications

DOI: https://doi.org/10.1038/ncomms15369 · OSTI ID:1389275

^[1];

^[2]; Gui, Daxiang ^[2]; Liu, Zhiyong ^[2]; Wang, Xiangxiang ^[2]; Dai, Xing ^[2]; Liu, Shengtang ^[2]; Zhang, Linjuan ^[3]; Gao, Yang ^[2]; Chen, Lanhua ^[2]; Sheng, Daopeng ^[2]; Wang, Yanlong ^[2]; Diwu, Juan ^[2]; Wang, Jianqiang ^[3];

^[4]; Chai, Zhifang ^[2]; Albrecht-Schmitt, Thomas E. ^[5]; Wang, Shuao ^[2]

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; IBM Thomas J Watson Research Center, Yorktown Heights, New York
Soochow Univ., Jiangsu (China). Collaborative Innovation Center of Radiation Medicine of Jiangsu Higher Education Institutions
Chinese Academy of Sciences (CAS), Beijing (China). Shanghai Inst. of Applied Physics and Key Lab. of Nuclear Radiation and Nuclear Energy Technology
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
Florida State Univ., Tallahassee, FL (United States). Dept. of Chemistry and Biochemistry

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.

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Research Organization:: Florida State Univ., Tallahassee, FL (United States); Energy Frontier Research Centers (EFRC) (United States). Center for Actinide Science & Technology (CAST)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: SC0016568

OSTI ID:: 1389275

Journal Information:: Nature Communications, Journal Name: Nature Communications Vol. 8; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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Metal–organic framework-based materials for the recovery of uranium from aqueous solutions Yang, Weiting; Pan, Qinhe; Song, Shuyan Inorganic Chemistry Frontiers, Vol. 6, Issue 8 https://doi.org/10.1039/c9qi00386j	journal	January 2019
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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
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CCDC 1450121: Experimental Crystal Structure Determination: BARLEO : catena-[tetrakis(1-butyl-1-methylpyrrolidin-1-ium) (μ-[methanetetrayltetrakis(4,1-phenylene)]tetrakis(phosphonato))-octafluoro-tri-zirconium(iv) dodecahydrate] Zheng, Tao; Yang, Zaixing; Gui, Daxiang https://doi.org/10.5517/ccdc.csd.cc1knz39 The current record is supplemented by this dataset	dataset	January 2016
CCDC 1450122: Experimental Crystal Structure Determination: BARLIS : octaethyl (methanetetrayltetra-4,1-phenylene)tetrakis(phosphonate) tetrahydrate Zheng, Tao; Yang, Zaixing; Gui, Daxiang https://doi.org/10.5517/ccdc.csd.cc1knz4b The current record is supplemented by this dataset	dataset	January 2016
CCDC 1450123: Experimental Crystal Structure Determination: DURPEN02 : (methanetetrayltetra-4,1-phenylene)tetrakis(phosphonic acid) Space Group: I 4 (82), Cell: a 13.2646(7)Å b 13.2646(7)Å c 7.5238(5)Å, α 90° β 90° γ 90° Zheng, Tao; Yang, Zaixing; Gui, Daxiang https://doi.org/10.5517/ccdc.csd.cc1knz5c The current record is supplemented by this dataset	dataset	January 2016
CCDC 1450124: Experimental Crystal Structure Determination: BARMAL : catena-[bis(1-butyl-1-methylpyrrolidin-1-ium) bis(μ-trihydrogen [methanetetrayltetrakis(4,1-phenylene)]tetrakis(phosphonato))-dodecafluoro-penta-zirconium(iv) pentahydrate] Zheng, Tao; Yang, Zaixing; Gui, Daxiang https://doi.org/10.5517/ccdc.csd.cc1knz6d The current record is supplemented by this dataset	dataset	October 2016
CCDC 1531836: Experimental Crystal Structure Determination: BARMEP : catena-[tetrakis(N-ethylpyridinium) bis(μ-hydrogen [tricyclo[3.3.1.13,7]decane-1,3,5,7-tetrayltetrakis(4,1-phenylene)]tetrakis(phosphonato))-octadecafluoro-hepta-zirconium(iv) tridecahydrate] Zheng, Tao; Yang, Zaixing; Gui, Daxiang https://doi.org/10.5517/ccdc.csd.cc1nf025 The current record is supplemented by this dataset	dataset	February 2017