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Title: Retrosynthesis of multi–component metal-organic frameworks

Abstract

Crystal engineering of metal–organic frameworks (MOFs) has allowed the construction of complex structures at atomic precision, but has yet to reach the same level of sophistication as organic synthesis. The synthesis of complex MOFs with multiple organic and/or inorganic components is ultimately limited by the lack of control over framework assembly in one-pot reactions. Herein, we demonstrate that multi-component MOFs with unprecedented complexity can be constructed in a predictable and stepwise manner under simple kinetic guidance, which conceptually mimics the retrosynthetic approach utilized to construct complicated organic molecules. Four multi-component MOFs were synthesized by the subsequent incorporation of organic linkers and inorganic clusters into the cavity of a mesoporous MOF, each composed of up to three different metals and two different linkers. Furthermore, we demonstrated the utility of such a retrosynthetic design through the construction of a cooperative bimetallic catalytic system with two collaborative metal sites for three-component Strecker reactions.

Authors:
 [1];  [1];  [1]; ORCiD logo [1];  [1];  [1];  [1];  [1];  [1]; ORCiD logo [2]; ORCiD logo [3];  [1]; ORCiD logo [4]
  1. Texas A & M Univ., College Station, TX (United States)
  2. Shandong Univ., Jinan (China)
  3. King Saud Univ., Riyadh (Saudi Arabia)
  4. Texas A & M Univ., College Station, TX (United States); King Saud Univ., Riyadh (Saudi Arabia)
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC), Washington, D.C. (United States). Center for Gas Separations Relevant to Clean Energy Technologies (CGS)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1470209
Grant/Contract Number:  
SC0001015
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 9; Journal Issue: 1; 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 2041-1723
Publisher:
Nature Publishing Group
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)

Citation Formats

Yuan, Shuai, Qin, Jun-Sheng, Li, Jialuo, Huang, Lan, Feng, Liang, Fang, Yu, Lollar, Christina, Pang, Jiandong, Zhang, Liangliang, Sun, Di, Alsalme, Ali, Cagin, Tahir, and Zhou, Hong-Cai. Retrosynthesis of multi–component metal-organic frameworks. United States: N. p., 2018. Web. doi:10.1038/s41467-018-03102-5.
Yuan, Shuai, Qin, Jun-Sheng, Li, Jialuo, Huang, Lan, Feng, Liang, Fang, Yu, Lollar, Christina, Pang, Jiandong, Zhang, Liangliang, Sun, Di, Alsalme, Ali, Cagin, Tahir, & Zhou, Hong-Cai. Retrosynthesis of multi–component metal-organic frameworks. United States. doi:10.1038/s41467-018-03102-5.
Yuan, Shuai, Qin, Jun-Sheng, Li, Jialuo, Huang, Lan, Feng, Liang, Fang, Yu, Lollar, Christina, Pang, Jiandong, Zhang, Liangliang, Sun, Di, Alsalme, Ali, Cagin, Tahir, and Zhou, Hong-Cai. Fri . "Retrosynthesis of multi–component metal-organic frameworks". United States. doi:10.1038/s41467-018-03102-5. https://www.osti.gov/servlets/purl/1470209.
@article{osti_1470209,
title = {Retrosynthesis of multi–component metal-organic frameworks},
author = {Yuan, Shuai and Qin, Jun-Sheng and Li, Jialuo and Huang, Lan and Feng, Liang and Fang, Yu and Lollar, Christina and Pang, Jiandong and Zhang, Liangliang and Sun, Di and Alsalme, Ali and Cagin, Tahir and Zhou, Hong-Cai},
abstractNote = {Crystal engineering of metal–organic frameworks (MOFs) has allowed the construction of complex structures at atomic precision, but has yet to reach the same level of sophistication as organic synthesis. The synthesis of complex MOFs with multiple organic and/or inorganic components is ultimately limited by the lack of control over framework assembly in one-pot reactions. Herein, we demonstrate that multi-component MOFs with unprecedented complexity can be constructed in a predictable and stepwise manner under simple kinetic guidance, which conceptually mimics the retrosynthetic approach utilized to construct complicated organic molecules. Four multi-component MOFs were synthesized by the subsequent incorporation of organic linkers and inorganic clusters into the cavity of a mesoporous MOF, each composed of up to three different metals and two different linkers. Furthermore, we demonstrated the utility of such a retrosynthetic design through the construction of a cooperative bimetallic catalytic system with two collaborative metal sites for three-component Strecker reactions.},
doi = {10.1038/s41467-018-03102-5},
journal = {Nature Communications},
number = 1,
volume = 9,
place = {United States},
year = {2018},
month = {2}
}

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    Systematic Ligand Modulation Enhances the Moisture Stability and Gas Sorption Characteristics of Quaternary Metal–Organic Frameworks
    journal, March 2015

    • Liu, Lujia; Telfer, Shane G.
    • Journal of the American Chemical Society, Vol. 137, Issue 11
    • DOI: 10.1021/jacs.5b00365

    Tunable Catalytic Activity of Solid Solution Metal–Organic Frameworks in One-Pot Multicomponent Reactions
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    journal, October 2015

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    • Journal of the American Chemical Society, Vol. 137, Issue 42
    • DOI: 10.1021/jacs.5b07687

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    journal, March 2016

    • Nguyen, Ha L.; Gándara, Felipe; Furukawa, Hiroyasu
    • Journal of the American Chemical Society, Vol. 138, Issue 13
    • DOI: 10.1021/jacs.6b01233

    Thermodynamically Guided Synthesis of Mixed-Linker Zr-MOFs with Enhanced Tunability
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    • Yuan, Shuai; Qin, Jun-Sheng; Zou, Lanfang
    • Journal of the American Chemical Society, Vol. 138, Issue 20
    • DOI: 10.1021/jacs.6b03263

    Linker Installation: Engineering Pore Environment with Precisely Placed Functionalities in Zirconium MOFs
    journal, July 2016

    • Yuan, Shuai; Chen, Ying-Pin; Qin, Jun-Sheng
    • Journal of the American Chemical Society, Vol. 138, Issue 28
    • DOI: 10.1021/jacs.6b04501

    Deciphering the Spatial Arrangement of Metals and Correlation to Reactivity in Multivariate Metal–Organic Frameworks
    journal, October 2016

    • Liu, Qi; Cong, Hengjiang; Deng, Hexiang
    • Journal of the American Chemical Society, Vol. 138, Issue 42
    • DOI: 10.1021/jacs.6b08724

    Modular and Stepwise Synthesis of a Hybrid Metal–Organic Framework for Efficient Electrocatalytic Oxygen Evolution
    journal, January 2017

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    • Journal of the American Chemical Society, Vol. 139, Issue 5
    • DOI: 10.1021/jacs.6b12353

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