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

Abstract

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 routemore » toward mixed-linker MOFs, but also provides tunable control of MOF defects and, in turn, the properties.« less

Authors:
 [1];  [1];  [1];  [1];  [1];  [1];  [1]
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  1. Texas A & M Univ., College Station, TX (United States)
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Center for Gas Separations Relevant to Clean Energy Technologies (CGS)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); ConocoPhillips
OSTI Identifier:
1470340
Grant/Contract Number:  
SC0001015; EE0007049
Resource Type:
Accepted Manuscript
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 138; Journal 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; Journal ID: ISSN 0002-7863
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; membrane; carbon capture; materials and chemistry by design; synthesis (novel materials); synthesis (self-assembly); synthesis (scalable processing); layers; metal organic frameworks; defects; cluster chemistry; stability

Citation Formats

Yuan, Shuai, Qin, Jun-Sheng, Zou, Lanfang, Chen, Ying-Pin, Wang, Xuan, Zhang, Qiang, and Zhou, Hong-Cai. Thermodynamically Guided Synthesis of Mixed-Linker Zr-MOFs with Enhanced Tunability. United States: N. p., 2016. Web. doi:10.1021/jacs.6b03263.
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Yuan, Shuai, Qin, Jun-Sheng, Zou, Lanfang, Chen, Ying-Pin, Wang, Xuan, Zhang, Qiang, & Zhou, Hong-Cai. Thermodynamically Guided Synthesis of Mixed-Linker Zr-MOFs with Enhanced Tunability. United States. https://doi.org/10.1021/jacs.6b03263
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Yuan, Shuai, Qin, Jun-Sheng, Zou, Lanfang, Chen, Ying-Pin, Wang, Xuan, Zhang, Qiang, and Zhou, Hong-Cai. Fri . "Thermodynamically Guided Synthesis of Mixed-Linker Zr-MOFs with Enhanced Tunability". United States. https://doi.org/10.1021/jacs.6b03263. https://www.osti.gov/servlets/purl/1470340.
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@article{osti_1470340,
title = {Thermodynamically Guided Synthesis of Mixed-Linker Zr-MOFs with Enhanced Tunability},
author = {Yuan, Shuai and Qin, Jun-Sheng and Zou, Lanfang and Chen, Ying-Pin and Wang, Xuan and Zhang, Qiang and Zhou, Hong-Cai},
abstractNote = {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.},
doi = {10.1021/jacs.6b03263},
journal = {Journal of the American Chemical Society},
number = 20,
volume = 138,
place = {United States},
year = {Fri May 06 00:00:00 EDT 2016},
month = {Fri May 06 00:00:00 EDT 2016}
}
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https://doi.org/10.1021/jacs.6b03263
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Scheme 1 Scheme 1: The thermodynamically controlled strategy for the synthesis of mixed-linker Zr-MOFs
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    journal, January 2018

    • Qin, Jun-Sheng; Yuan, Shuai; Lollar, Christina
    • Chemical Communications, Vol. 54, Issue 34
    • DOI: 10.1039/c7cc09173g

    Framework disorder and its effect on selective hysteretic sorption of a T-shaped azole-based metal–organic framework
    journal, January 2019

    van der Waals Epitaxial Growth of 2D Metal-Porphyrin Framework Derived Thin Films for Dye-Sensitized Solar Cells
    journal, September 2018

    • Wang, Yan-Yue; Chen, Shu-Mei; Haldar, Ritesh
    • Advanced Materials Interfaces, Vol. 5, Issue 21
    • DOI: 10.1002/admi.201800985

    An ultrastable Zr-MOF for fast capture and highly luminescence detection of Cr 2 O 7 2− simultaneously in an aqueous phase
    journal, January 2018

    • Sun, Xiaodong; Yao, Shuo; Yu, Chengyang
    • Journal of Materials Chemistry A, Vol. 6, Issue 15
    • DOI: 10.1039/c8ta01060a

    NH 2 -UiO-66/ g -C 3 N 4 /CdTe composites for photocatalytic CO 2 reduction under visible light
    journal, October 2019

    • Yu, Fengyang; Chen, Liyong; Shen, Xiaoshuang
    • APL Materials, Vol. 7, Issue 10
    • DOI: 10.1063/1.5120528

    Zirconium-Porphyrin PCN-222: pH-responsive Controlled Anticancer Drug Oridonin
    journal, December 2018

    • Leng, Xin; Huang, Hongliang; Wang, Wenping
    • Evidence-Based Complementary and Alternative Medicine, Vol. 2018
    • DOI: 10.1155/2018/3249023

    Construction of hierarchically porous metal–organic frameworks through linker labilization
    journal, May 2017

    • Yuan, Shuai; Zou, Lanfang; Qin, Jun-Sheng
    • Nature Communications, Vol. 8, Issue 1
    • DOI: 10.1038/ncomms15356

    One-Step Synthesis of Hybrid Core-Shell Metal-Organic Frameworks
    journal, March 2018

    Tunability of fluorescent metal–organic frameworks through dynamic spacer installation with multivariate fluorophores
    journal, January 2018

    • Chen, Cheng-Xia; Qiu, Qian-Feng; Pan, Mei
    • Chemical Communications, Vol. 54, Issue 97
    • DOI: 10.1039/c8cc07441k

    Construction of unprecedented pillar-layered metal organic frameworks via a dual-ligand strategy for dye degradation
    journal, January 2018

    • Tang, Yu-Huan; Wang, Fei; Zhang, Jian
    • Dalton Transactions, Vol. 47, Issue 12
    • DOI: 10.1039/c7dt04484d

    Specific detection of hypochlorite based on the size-selective effect of luminophore integrated MOF-801 synthesized by a one-pot strategy
    journal, January 2019

    • Ye, Yunxi; Zhao, Liwei; Hu, Shuanggang
    • Dalton Transactions, Vol. 48, Issue 8
    • DOI: 10.1039/c8dt04692a

    Pore-Environment Engineering with Multiple Metal Sites in Rare-Earth Porphyrinic Metal-Organic Frameworks
    journal, March 2018

    • Zhang, Liangliang; Yuan, Shuai; Feng, Liang
    • Angewandte Chemie, Vol. 130, Issue 18
    • DOI: 10.1002/ange.201802661

    Supramolecular frameworks based on 5,10,15,20-tetra(4-carboxyphenyl)porphyrins
    journal, January 2018

    • Morshedi, Mahbod; Ward, Jas S.; Kruger, Paul E.
    • Dalton Transactions, Vol. 47, Issue 3
    • DOI: 10.1039/c7dt04162d

    Ionic liquid accelerates the crystallization of Zr-based metal–organic frameworks
    journal, August 2017

    Topology-guided functional multiplicity of iron( iii )-based metal–organic frameworks
    journal, January 2017

    • Virmani, Erika; Beyer, Ole; Lüning, Ulrich
    • Materials Chemistry Frontiers, Vol. 1, Issue 10
    • DOI: 10.1039/c7qm00263g

    Recent Advances in Photocatalysis over Metal–Organic Frameworks‐Based Materials
    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
    journal, June 2020

    • Chen, Cheng‐Xia; Fan, Yan‐Zhong; Cao, Chen‐Chen
    • Chemistry – A European Journal, Vol. 26, Issue 37
    • DOI: 10.1002/chem.202001052

    Mixed-linker strategy for the construction of multifunctional metal–organic frameworks
    journal, January 2017

    • Qin, Jun-Sheng; Yuan, Shuai; Wang, Qi
    • Journal of Materials Chemistry A, Vol. 5, Issue 9
    • DOI: 10.1039/c6ta10281f

    A flexible thioether-based MOF as a crystalline sponge for structural characterization of liquid organic molecules
    journal, January 2017

    • Yang, Xin-Yu; Yuan, Shuai; Qin, Jun-Sheng
    • Materials Chemistry Frontiers, Vol. 1, Issue 9
    • DOI: 10.1039/c7qm00152e

    Pore-Environment Engineering with Multiple Metal Sites in Rare-Earth Porphyrinic Metal-Organic Frameworks
    journal, March 2018

    • Zhang, Liangliang; Yuan, Shuai; Feng, Liang
    • Angewandte Chemie International Edition, Vol. 57, Issue 18
    • DOI: 10.1002/anie.201802661

    A Stimuli-Responsive Zirconium Metal-Organic Framework Based on Supermolecular Design
    journal, July 2017

    • Krause, Simon; Bon, Volodymyr; Stoeck, Ulrich
    • Angewandte Chemie, Vol. 129, Issue 36
    • DOI: 10.1002/ange.201702357

    Covalent Organic Frameworks with Chirality Enriched by Biomolecules for Efficient Chiral Separation
    journal, November 2018

    • Zhang, Sainan; Zheng, Yunlong; An, Hongde
    • Angewandte Chemie International Edition, Vol. 57, Issue 51
    • DOI: 10.1002/anie.201810571

    Stable Metal–Organic Frameworks with Group 4 Metals: Current Status and Trends
    journal, February 2018

    Ionic liquid accelerates the crystallization of Zr-based metal–organic frameworks
    journal, August 2017

    Improving MOF stability: approaches and applications
    journal, January 2019

    • Ding, Meili; Cai, Xuechao; Jiang, Hai-Long
    • Chemical Science, Vol. 10, Issue 44
    • DOI: 10.1039/c9sc03916c

    Zirconium-Porphyrin PCN-222: pH-responsive Controlled Anticancer Drug Oridonin
    journal, December 2018

    • Leng, Xin; Huang, Hongliang; Wang, Wenping
    • Evidence-Based Complementary and Alternative Medicine, Vol. 2018
    • DOI: 10.1155/2018/3249023
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