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Title: Uncovering Structural Opportunities for Zirconium Metal–Organic Frameworks via Linker Desymmetrization

Abstract

The discovery of metal–organic frameworks (MOFs) mimicking inorganic minerals with intricate topologies requires elaborate linker design guidelines. Herein, the concept of linker desymmetrization into the design of tetratopic linker based Zr-MOFs is applied. A series of bent tetratopic linkers with various substituents are utilized to construct Zr-MOFs with distinct cluster connectivities and topologies. For example, the assembly between a bent linker L-SO2 with C2v symmetry and an 8-connected Zr6 cluster leads to the formation of an scu topology, while another flu topology can be obtained by the combination of a novel 8-connected Zr6 cluster and a bent linker L-O with C1 symmetry. Further utilization of restricted bent linker [(L-(CH3)6)] gives rise to a fascinating (4, 6)-c cor net, originated from the corundum lattice, with an unprecedented 6-c Zr6 cluster. In addition, the removal of toxic selenite ions in aqueous solution is performed by PCN-903-(CH3)6 which exhibits rapid and efficient detoxification. This work uncovers new structural opportunities for Zr-MOFs via linker desymmetrization and provides novel design strategies for the discovery of sophisticated topologies for practical applications.

Authors:
 [1];  [2];  [1];  [2];  [1];  [1];  [1];  [1];  [3];  [1]; ORCiD logo [4]
+ Show Author Affiliations
  1. College of Science School of Materials Science and Engineering China University of Petroleum (East China) Qingdao Shandong 266580 China
  2. Department of Chemistry Texas A&,M University College Station TX 77843 USA
  3. Xi'an Institute of Flexible Electronics Northwestern Polytechnical University Xi'an 710072 China
  4. Department of Chemistry Texas A&,M University College Station TX 77843 USA, Department of Materials Science and Engineering Texas A&,M University College Station TX 77843‐3003 USA
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Center for Gas Separations Relevant to Clean Energy Technologies (CGS); Univ. of California, Oakland, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Natural Science Foundation of China (NSFC); Taishan Scholar Foundation; Welch Foundation
OSTI Identifier:
1567891
Alternate Identifier(s):
OSTI ID: 1567893; OSTI ID: 1623480
Grant/Contract Number:  
SC0001015; 21875285; 21571187; ts201511019
Resource Type:
Published Article
Journal Name:
Advanced Science
Additional Journal Information:
Journal Name: Advanced Science Journal Volume: 6 Journal Issue: 23; Journal ID: ISSN 2198-3844
Publisher:
Wiley Blackwell (John Wiley & Sons)
Country of Publication:
Germany
Language:
English
Subject:
Chemistry; Science & Technology - Other Topics; Materials Science

Citation Formats

Wang, Yutong, Feng, Liang, Zhang, Kai, Wang, Kun‐Yu, Fan, Weidong, Wang, Xiaokang, Guo, Bingbing, Dai, Fangna, Zhang, Liangliang, Sun, Daofeng, and Zhou, Hong‐Cai. Uncovering Structural Opportunities for Zirconium Metal–Organic Frameworks via Linker Desymmetrization. Germany: N. p., 2019. Web. doi:10.1002/advs.201901855.
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Wang, Yutong, Feng, Liang, Zhang, Kai, Wang, Kun‐Yu, Fan, Weidong, Wang, Xiaokang, Guo, Bingbing, Dai, Fangna, Zhang, Liangliang, Sun, Daofeng, & Zhou, Hong‐Cai. Uncovering Structural Opportunities for Zirconium Metal–Organic Frameworks via Linker Desymmetrization. Germany. https://doi.org/10.1002/advs.201901855
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Wang, Yutong, Feng, Liang, Zhang, Kai, Wang, Kun‐Yu, Fan, Weidong, Wang, Xiaokang, Guo, Bingbing, Dai, Fangna, Zhang, Liangliang, Sun, Daofeng, and Zhou, Hong‐Cai. Mon . "Uncovering Structural Opportunities for Zirconium Metal–Organic Frameworks via Linker Desymmetrization". Germany. https://doi.org/10.1002/advs.201901855.
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@article{osti_1567891,
title = {Uncovering Structural Opportunities for Zirconium Metal–Organic Frameworks via Linker Desymmetrization},
author = {Wang, Yutong and Feng, Liang and Zhang, Kai and Wang, Kun‐Yu and Fan, Weidong and Wang, Xiaokang and Guo, Bingbing and Dai, Fangna and Zhang, Liangliang and Sun, Daofeng and Zhou, Hong‐Cai},
abstractNote = {The discovery of metal–organic frameworks (MOFs) mimicking inorganic minerals with intricate topologies requires elaborate linker design guidelines. Herein, the concept of linker desymmetrization into the design of tetratopic linker based Zr-MOFs is applied. A series of bent tetratopic linkers with various substituents are utilized to construct Zr-MOFs with distinct cluster connectivities and topologies. For example, the assembly between a bent linker L-SO2 with C2v symmetry and an 8-connected Zr6 cluster leads to the formation of an scu topology, while another flu topology can be obtained by the combination of a novel 8-connected Zr6 cluster and a bent linker L-O with C1 symmetry. Further utilization of restricted bent linker [(L-(CH3)6)] gives rise to a fascinating (4, 6)-c cor net, originated from the corundum lattice, with an unprecedented 6-c Zr6 cluster. In addition, the removal of toxic selenite ions in aqueous solution is performed by PCN-903-(CH3)6 which exhibits rapid and efficient detoxification. This work uncovers new structural opportunities for Zr-MOFs via linker desymmetrization and provides novel design strategies for the discovery of sophisticated topologies for practical applications.},
doi = {10.1002/advs.201901855},
journal = {Advanced Science},
number = 23,
volume = 6,
place = {Germany},
year = {Mon Sep 30 00:00:00 EDT 2019},
month = {Mon Sep 30 00:00:00 EDT 2019}
}
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https://doi.org/10.1002/advs.201901855
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