Flexible Zirconium Metal‐Organic Frameworks as Bioinspired Switchable Catalysts

Yuan, Shuai; Zou, Lanfang; Li, Haixia; Chen, Ying‐Pin; Qin, Junsheng; Zhang, Qiang; Lu, Weigang; Hall, Michael B.; Zhou, Hong‐Cai

doi:10.1002/anie.201604313

Title: Flexible Zirconium Metal‐Organic Frameworks as Bioinspired Switchable Catalysts

Abstract

Abstract Flexible metal–organic frameworks (MOFs) are highly desirable in host–guest chemistry owing to their almost unlimited structural/functional diversities and stimuli‐responsive pore architectures. Herein, we designed a flexible Zr‐MOF system, namely PCN‐700 series, for the realization of switchable catalysis in cycloaddition reactions of CO ₂ with epoxides. Their breathing behaviors were studied by successive single‐crystal X‐ray diffraction analyses. The breathing amplitudes of the PCN‐700 series were modulated through pre‐functionalization of organic linkers and post‐synthetic linker installation. Experiments and molecular simulations confirm that the catalytic activities of the PCN‐700 series can be switched on and off upon reversible structural transformation, which is reminiscent of sophisticated biological systems such as allosteric enzymes.

Authors:

Yuan, Shuai ^[1]; Zou, Lanfang ^[1]; Li, Haixia ^[1]; Chen, Ying‐Pin ^[1]; Qin, Junsheng ^[1]; Zhang, Qiang ^[1]; Lu, Weigang ^[2]; Hall, Michael B. ^[1];

^[1]

Department of Chemistry Texas A&,M University College Station TX 77843 USA
Department of Chemistry Blinn College Bryan TX 77805 USA

Publication Date:: Mon Jun 27 00:00:00 EDT 2016

Sponsoring Org.:: USDOE

OSTI Identifier:: 1400460

Grant/Contract Number:: SC0001015; EE-0007049

Resource Type:: Publisher's Accepted Manuscript

Journal Name:: Angewandte Chemie (International Edition)

Additional Journal Information:: Journal Name: Angewandte Chemie (International Edition) Journal Volume: 55 Journal Issue: 36; Journal ID: ISSN 1433-7851

Publisher:: Wiley Blackwell (John Wiley & Sons)

Country of Publication:: Germany

Language:: English

Citation Formats


                    Yuan, Shuai, Zou, Lanfang, Li, Haixia, Chen, Ying‐Pin, Qin, Junsheng, Zhang, Qiang, Lu, Weigang, Hall, Michael B., and Zhou, Hong‐Cai. Flexible Zirconium Metal‐Organic Frameworks as Bioinspired Switchable Catalysts.  Germany: N. p., 2016. 
Web.  doi:10.1002/anie.201604313.

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                    Yuan, Shuai, Zou, Lanfang, Li, Haixia, Chen, Ying‐Pin, Qin, Junsheng, Zhang, Qiang, Lu, Weigang, Hall, Michael B., & Zhou, Hong‐Cai. Flexible Zirconium Metal‐Organic Frameworks as Bioinspired Switchable Catalysts.  Germany.  https://doi.org/10.1002/anie.201604313

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                    Yuan, Shuai, Zou, Lanfang, Li, Haixia, Chen, Ying‐Pin, Qin, Junsheng, Zhang, Qiang, Lu, Weigang, Hall, Michael B., and Zhou, Hong‐Cai. Mon .  
"Flexible Zirconium Metal‐Organic Frameworks as Bioinspired Switchable Catalysts".  Germany.  https://doi.org/10.1002/anie.201604313.

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@article{osti_1400460,

  title        = {Flexible Zirconium Metal‐Organic Frameworks as Bioinspired Switchable Catalysts},

  author       = {Yuan, Shuai and Zou, Lanfang and Li, Haixia and Chen, Ying‐Pin and Qin, Junsheng and Zhang, Qiang and Lu, Weigang and Hall, Michael B. and Zhou, Hong‐Cai},

  abstractNote = {Abstract Flexible metal–organic frameworks (MOFs) are highly desirable in host–guest chemistry owing to their almost unlimited structural/functional diversities and stimuli‐responsive pore architectures. Herein, we designed a flexible Zr‐MOF system, namely PCN‐700 series, for the realization of switchable catalysis in cycloaddition reactions of CO 2 with epoxides. Their breathing behaviors were studied by successive single‐crystal X‐ray diffraction analyses. The breathing amplitudes of the PCN‐700 series were modulated through pre‐functionalization of organic linkers and post‐synthetic linker installation. Experiments and molecular simulations confirm that the catalytic activities of the PCN‐700 series can be switched on and off upon reversible structural transformation, which is reminiscent of sophisticated biological systems such as allosteric enzymes.},

  doi          = {10.1002/anie.201604313},

  journal      = {Angewandte Chemie (International Edition)},

  number       = 36,

  volume       = 55,

  place        = {Germany},

  year         = {Mon Jun 27 00:00:00 EDT 2016},

  month        = {Mon Jun 27 00:00:00 EDT 2016}

}

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Title: Flexible Zirconium Metal‐Organic Frameworks as Bioinspired Switchable Catalysts

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Diastereodivergent Asymmetric Sulfa-Michael Additions of α-Branched Enones using a Single Chiral Organic Catalyst journal, November 2011

Robust, Chiral, and Porous BINAP-Based Metal–Organic Frameworks for Highly Enantioselective Cyclization Reactions journal, September 2015

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Kinetic Resolution of Amines: A Highly Enantioselective and Chemoselective Acetylating Agent with a Unique Solvent-Induced Reversal of Stereoselectivity journal, June 2004

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How Linker’s Modification Controls Swelling Properties of Highly Flexible Iron(III) Dicarboxylates MIL-88 journal, November 2011

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journal, January 2012

Flexible metal–organic frameworks
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Superacidity in Sulfated Metal–Organic Framework-808
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Allosteric Supramolecular Receptors and Catalysts
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A Reversible Crystallinity-Preserving Phase Transition in Metal–Organic Frameworks: Discovery, Mechanistic Studies, and Potential Applications
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A New Zirconium Inorganic Building Brick Forming Metal Organic Frameworks with Exceptional Stability
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Kinetic Resolution of Amines: A Highly Enantioselective and Chemoselective Acetylating Agent with a Unique Solvent-Induced Reversal of Stereoselectivity
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