Thermodynamically Guided Synthesis of Mixed-Linker Zr-MOFs with Enhanced Tunability

Yuan, Shuai; Qin, Jun-Sheng; Zou, Lanfang; Chen, Ying-Pin; Wang, Xuan; Zhang, Qiang; Zhou, Hong-Cai

doi:10.1021/jacs.6b03263

Title: Thermodynamically Guided Synthesis of Mixed-Linker Zr-MOFs with Enhanced Tunability

Journal Article · Fri May 06 00:00:00 EDT 2016 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.6b03263· OSTI ID:1470340

Yuan, Shuai ^[1]; Qin, Jun-Sheng ^[1]; Zou, Lanfang ^[1]; Chen, Ying-Pin ^[1]; Wang, Xuan ^[1]; Zhang, Qiang ^[1]; Zhou, Hong-Cai ^[1]

Texas A & M Univ., College Station, TX (United States)

Guided by thermodynamics, we have synthesized two mixed-linker zirconium-based metal–organic frameworks (Zr-MOFs), namely, PCN-133 and PCN-134. Both of them possess a layer-pillar structure, in which the connection between Zr₆ clusters and primary BTB linkers form a (3,6)-connected kdg layer that is further extended into 3D frameworks by auxiliary DCDPS/TCPP linkers (BTB = benzene tribenzoate, DCDPS = 4,4'-dicarboxydiphenyl sulfone, TCPP = tetrakis(4-carboxyphenyl)porphyrin). PCN-134 demonstrates high porosity (N₂ uptake of 717 cm³·g^–1 and BET surface area of 1946 cm²·g^–1) and excellent chemical stability in aqueous solutions with pH values ranging from 0 to 13. More importantly, PCN-134 tolerates the partial absence of auxiliary linkers leading to structural defects during the assembly process while preserving its framework integrity. Furthermore, the defect density can be systematically controlled by tuning the occupancy of the auxiliary linker, which in turn affects the MOF properties. For instance, the dichromate uptake of PCN-134 is tuned by adjusting the BTB/TCPP ratios, which gives rise to an efficient dichromate absorbent when the TCPP molar ratio in linkers is set as 22%. Additionally, the photocatalytic reduction of Cr(VI) in aqueous solution was also performed by PCN-134–22%TCPP which exhibits excellent catalytic activity. This work not only opens up a new synthetic route toward mixed-linker MOFs, but also provides tunable control of MOF defects and, in turn, the properties.

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Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Center for Gas Separations Relevant to Clean Energy Technologies (CGS)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); ConocoPhillips

Grant/Contract Number:: SC0001015; EE0007049

OSTI ID:: 1470340

Journal Information:: Journal of the American Chemical Society, Vol. 138, Issue 20; Related Information: CGS partners with University of California, Berkeley; University of California, Davis; Lawrence Berkeley National Laboratory; University of Minnesota; National Energy Technology Laboratory; Texas A&M University; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 181 works

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Tunability of fluorescent metal–organic frameworks through dynamic spacer installation with multivariate fluorophores Chen, Cheng-Xia; Qiu, Qian-Feng; Pan, Mei Chemical Communications, Vol. 54, Issue 97 https://doi.org/10.1039/c8cc07441k	journal	January 2018
Construction of unprecedented pillar-layered metal organic frameworks via a dual-ligand strategy for dye degradation Tang, Yu-Huan; Wang, Fei; Zhang, Jian Dalton Transactions, Vol. 47, Issue 12 https://doi.org/10.1039/c7dt04484d	journal	January 2018
Specific detection of hypochlorite based on the size-selective effect of luminophore integrated MOF-801 synthesized by a one-pot strategy Ye, Yunxi; Zhao, Liwei; Hu, Shuanggang Dalton Transactions, Vol. 48, Issue 8 https://doi.org/10.1039/c8dt04692a	journal	January 2019
Pore-Environment Engineering with Multiple Metal Sites in Rare-Earth Porphyrinic Metal-Organic Frameworks Zhang, Liangliang; Yuan, Shuai; Feng, Liang Angewandte Chemie, Vol. 130, Issue 18 https://doi.org/10.1002/ange.201802661	journal	March 2018
Supramolecular frameworks based on 5,10,15,20-tetra(4-carboxyphenyl)porphyrins Morshedi, Mahbod; Ward, Jas S.; Kruger, Paul E. Dalton Transactions, Vol. 47, Issue 3 https://doi.org/10.1039/c7dt04162d	journal	January 2018
Ionic liquid accelerates the crystallization of Zr-based metal–organic frameworks Sang, Xinxin; Zhang, Jianling; Xiang, Junfeng Nature Communications, Vol. 8, Issue 1 https://doi.org/10.1038/s41467-017-00226-y	journal	August 2017
Topology-guided functional multiplicity of iron( iii )-based metal–organic frameworks Virmani, Erika; Beyer, Ole; Lüning, Ulrich Materials Chemistry Frontiers, Vol. 1, Issue 10 https://doi.org/10.1039/c7qm00263g	journal	January 2017
Recent Advances in Photocatalysis over Metal–Organic Frameworks‐Based Materials Zhang, Yijun; Mao, Fangxin; Wang, Lijie Solar RRL, Vol. 4, Issue 5 https://doi.org/10.1002/solr.201900438	journal	December 2019
Dynamic Coordination Chemistry of Fluorinated Zr‐MOFs: Synthetic Control and Reassembly/Disassembly Beyond de Novo Synthesis to Tune the Structure and Property Chen, Cheng‐Xia; Fan, Yan‐Zhong; Cao, Chen‐Chen Chemistry – A European Journal, Vol. 26, Issue 37 https://doi.org/10.1002/chem.202001052	journal	June 2020
A new route to triphenylpyridines utilizing ketoximes as building blocks via cascade reactions under iron-organic framework catalysis: VNU-20 was used as catalyst to achieve triphenylpyridines Nguyen, Vu H. H.; Doan, Son H.; Van, Tram T. Applied Organometallic Chemistry, Vol. 33, Issue 4 https://doi.org/10.1002/aoc.4841	journal	February 2019
Mixed-linker strategy for the construction of multifunctional metal–organic frameworks Qin, Jun-Sheng; Yuan, Shuai; Wang, Qi Journal of Materials Chemistry A, Vol. 5, Issue 9 https://doi.org/10.1039/c6ta10281f	journal	January 2017
A flexible thioether-based MOF as a crystalline sponge for structural characterization of liquid organic molecules Yang, Xin-Yu; Yuan, Shuai; Qin, Jun-Sheng Materials Chemistry Frontiers, Vol. 1, Issue 9 https://doi.org/10.1039/c7qm00152e	journal	January 2017
Pore-Environment Engineering with Multiple Metal Sites in Rare-Earth Porphyrinic Metal-Organic Frameworks Zhang, Liangliang; Yuan, Shuai; Feng, Liang Angewandte Chemie International Edition, Vol. 57, Issue 18 https://doi.org/10.1002/anie.201802661	journal	March 2018
A Stimuli-Responsive Zirconium Metal-Organic Framework Based on Supermolecular Design Krause, Simon; Bon, Volodymyr; Stoeck, Ulrich Angewandte Chemie, Vol. 129, Issue 36 https://doi.org/10.1002/ange.201702357	journal	July 2017
Covalent Organic Frameworks with Chirality Enriched by Biomolecules for Efficient Chiral Separation Zhang, Sainan; Zheng, Yunlong; An, Hongde Angewandte Chemie International Edition, Vol. 57, Issue 51 https://doi.org/10.1002/anie.201810571	journal	November 2018
Stable Metal–Organic Frameworks with Group 4 Metals: Current Status and Trends Yuan, Shuai; Qin, Jun-Sheng; Lollar, Christina T. ACS Central Science, Vol. 4, Issue 4 https://doi.org/10.1021/acscentsci.8b00073	journal	February 2018
Ligand-Rearrangement-Induced Transformation from a 3D Supramolecular Network to a Discrete Octanuclear Cluster: A Good Detector for Pb²⁺ and Cr₂O₇^2– Yang, Dan-Dan; Liu, Yue; Li, ShuangShuang ACS Omega, Vol. 4, Issue 7 https://doi.org/10.1021/acsomega.9b00680	journal	July 2019
Ultrahigh adsorption and singlet-oxygen mediated degradation for efficient synergetic removal of bisphenol A by a stable zirconium-porphyrin metal-organic framework Meng, Ai-Na; Chaihu, Ling-Xiao; Chen, Huan-Huan Scientific Reports, Vol. 7, Issue 1 https://doi.org/10.1038/s41598-017-06194-z	journal	July 2017

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
membrane
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CCDC 1470597: Experimental Crystal Structure Determination Yuan, Shuai; Qin, Jun-Sheng; Zou, Lanfang https://doi.org/10.5517/ccdc.csd.cc1lc8mv The current record is supplemented by this dataset	dataset	January 2016
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