Novel Topology in Semiconducting Tetrathiafulvalene Lanthanide Metal-Organic Frameworks

Xie, Lilia S.; Dincă, Mircea

doi:10.1002/ijch.201800068

Title: Novel Topology in Semiconducting Tetrathiafulvalene Lanthanide Metal-Organic Frameworks

Abstract

Abstract Tetrathiafulvalene tetrabenzoate (TTFTB) and several lanthanide ions self‐assemble into metal‐organic frameworks (MOFs) that exhibit a novel topology, a (3,3,3,6,6)‐coordinated net, which features an unusual ligand coordination mode and stacking motif. The Yb and Lu MOFs are electrically conductive, with pellet conductivity values of 9(7) × 10 ⁻⁷ and 3(2) × 10 ⁻⁷ S/cm, respectively. The crystallographically‐determined bond lengths indicate partial oxidation of the ligand, with close S ⋅ ⋅ ⋅ S contacts between ligands providing likely charge transport pathways in the material. Magnetometry reveals temperature‐independent paramagnetism, consistent with the presence of ligand‐based radicals, as well as weak antiferromagnetic coupling between Yb ³⁺ centers. These results illustrate the diversity of MOF structures and properties that are accessible with the TTFTB ligand owing to its electroactive nature, propensity for intermolecular interactions, and conformational flexibility.

Authors:

Xie, Lilia S. ^[1];

^[1]

Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)

Publication Date:: Thu Aug 09 00:00:00 EDT 2018

Research Org.:: Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)

OSTI Identifier:: 1612890

Alternate Identifier(s):: OSTI ID: 1463752

Grant/Contract Number:: SC0018235; 1122374

Resource Type:: Accepted Manuscript

Journal Name:: Israel Journal of Chemistry

Additional Journal Information:: Journal Volume: 58; Journal Issue: 9-10; Journal ID: ISSN 0021-2148

Publisher:: Wiley

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Chemistry; metal-organic frameworks; lanthanides; structure elucidation; π interactions; tetrathiafulvalene

Citation Formats


                    Xie, Lilia S., and Dincă, Mircea. Novel Topology in Semiconducting Tetrathiafulvalene Lanthanide Metal-Organic Frameworks.  United States: N. p., 2018. 
Web.  doi:10.1002/ijch.201800068.

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                    Xie, Lilia S., & Dincă, Mircea. Novel Topology in Semiconducting Tetrathiafulvalene Lanthanide Metal-Organic Frameworks.  United States.  https://doi.org/10.1002/ijch.201800068

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                    Xie, Lilia S., and Dincă, Mircea. Thu .  
"Novel Topology in Semiconducting Tetrathiafulvalene Lanthanide Metal-Organic Frameworks".  United States.  https://doi.org/10.1002/ijch.201800068.  https://www.osti.gov/servlets/purl/1612890.

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@article{osti_1612890,

  title        = {Novel Topology in Semiconducting Tetrathiafulvalene Lanthanide Metal-Organic Frameworks},

  author       = {Xie, Lilia S. and Dincă, Mircea},

  abstractNote = {Abstract Tetrathiafulvalene tetrabenzoate (TTFTB) and several lanthanide ions self‐assemble into metal‐organic frameworks (MOFs) that exhibit a novel topology, a (3,3,3,6,6)‐coordinated net, which features an unusual ligand coordination mode and stacking motif. The Yb and Lu MOFs are electrically conductive, with pellet conductivity values of 9(7) × 10 −7 and 3(2) × 10 −7 S/cm, respectively. The crystallographically‐determined bond lengths indicate partial oxidation of the ligand, with close S ⋅ ⋅ ⋅ S contacts between ligands providing likely charge transport pathways in the material. Magnetometry reveals temperature‐independent paramagnetism, consistent with the presence of ligand‐based radicals, as well as weak antiferromagnetic coupling between Yb 3+ centers. These results illustrate the diversity of MOF structures and properties that are accessible with the TTFTB ligand owing to its electroactive nature, propensity for intermolecular interactions, and conformational flexibility.},

  doi          = {10.1002/ijch.201800068},

  journal      = {Israel Journal of Chemistry},

  number       = 9-10,

  volume       = 58,

  place        = {United States},

  year         = {Thu Aug 09 00:00:00 EDT 2018},

  month        = {Thu Aug 09 00:00:00 EDT 2018}

}

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Works referencing / citing this record:

Electronic, Structural and Functional Versatility in Tetrathiafulvalene‐Lanthanide Metal–Organic Frameworks
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Title: Novel Topology in Semiconducting Tetrathiafulvalene Lanthanide Metal-Organic Frameworks

Abstract

Citation Formats

High Charge Mobility in a Tetrathiafulvalene-Based Microporous Metal–Organic Framework journal, July 2012

Cation-Dependent Intrinsic Electrical Conductivity in Isostructural Tetrathiafulvalene-Based Microporous Metal–Organic Frameworks journal, January 2015

Secondary building units, nets and bonding in the chemistry of metal–organic frameworks journal, January 2009

Supermolecular Building Blocks (SBBs) for the Design and Synthesis of Highly Porous Metal-Organic Frameworks journal, February 2008

The Reticular Chemistry Structure Resource (RCSR) Database of, and Symbols for, Crystal Nets journal, December 2008

Metal–organic framework materials as catalysts journal, January 2009

Systematic Design of Pore Size and Functionality in Isoreticular MOFs and Their Application in Methane Storage journal, January 2002

Selective Vapor Pressure Dependent Proton Transport in a Metal–Organic Framework with Two Distinct Hydrophilic Pores journal, February 2018

Topological Analysis of Metal–Organic Frameworks with Polytopic Linkers and/or Multiple Building Units and the Minimal Transitivity Principle journal, November 2013

From semiconductor-semiconductor transition (42 K) to the highest-Tc organic superconductor, .kappa.-(ET)2Cu[N(CN)2]Cl (Tc = 12.5 K) journal, September 1990

Applied Topological Analysis of Crystal Structures with the Program Package ToposPro journal, May 2014

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Metal–Organic Frameworks and Self-Assembled Supramolecular Coordination Complexes: Comparing and Contrasting the Design, Synthesis, and Functionality of Metal–Organic Materials journal, November 2012

Reticular synthesis and the design of new materials journal, June 2003

A new ambient-pressure organic superconductor, .kappa.-(ET)2Cu[N(CN)2]Br, with the highest transition temperature yet observed (inductive onset Tc = 11.6 K, resistive onset = 12.5 K) journal, July 1990

Hydrogen storage in metal–organic frameworks journal, January 2009

Metal–Organic Frameworks for Separations journal, September 2011

Hybrid Molecular Materials Based upon Organic π-Electron Donors and Metal Complexes. Radical Salts of Bis(ethylenethia)tetrathiafulvalene (BET-TTF) with the Octahedral Anions Hexacyanoferrate(III) and Nitroprusside. The First Kappa Phase in the BET-TTF Family journal, July 2001

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Metal–Organic Framework Materials as Chemical Sensors journal, September 2011

Tuning the structure and function of metal–organic frameworks via linker design journal, January 2014

A New Ambient Pressure Organic Superconductor Based on BEDT-TTF with T C Higher than 10 K (T C =10.4 K) journal, January 1988

The Organic Secondary Building Unit: Strong Intermolecular π Interactions Define Topology in MIT-25, a Mesoporous MOF with Proton-Replete Channels journal, March 2017

Crystal Structures, Gas Adsorption, and Electrochemical Properties of Electroactive Coordination Polymers Based on the Tetrathiafulvalene-Tetrabenzoate Ligand journal, February 2015

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The electronic, optical and magnetic consequences of delocalization in multifunctional donor–acceptor organic polymers journal, January 2015

Grid-Type Metal Ion Architectures: Functional Metallosupramolecular Arrays journal, July 2004

Measuring and Reporting Electrical Conductivity in Metal–Organic Frameworks: Cd 2 (TTFTB) as a Case Study journal, October 2016

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journal, July 2012

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journal, January 2015

Secondary building units, nets and bonding in the chemistry of metal–organic frameworks
journal, January 2009

Supermolecular Building Blocks (SBBs) for the Design and Synthesis of Highly Porous Metal-Organic Frameworks
journal, February 2008

The Reticular Chemistry Structure Resource (RCSR) Database of, and Symbols for, Crystal Nets
journal, December 2008

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Systematic Design of Pore Size and Functionality in Isoreticular MOFs and Their Application in Methane Storage
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From semiconductor-semiconductor transition (42 K) to the highest-Tc organic superconductor, .kappa.-(ET)2Cu[N(CN)2]Cl (Tc = 12.5 K)
journal, September 1990

Applied Topological Analysis of Crystal Structures with the Program Package ToposPro
journal, May 2014

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journal, January 1991

Metal–Organic Frameworks and Self-Assembled Supramolecular Coordination Complexes: Comparing and Contrasting the Design, Synthesis, and Functionality of Metal–Organic Materials
journal, November 2012

Reticular synthesis and the design of new materials
journal, June 2003

A new ambient-pressure organic superconductor, .kappa.-(ET)2Cu[N(CN)2]Br, with the highest transition temperature yet observed (inductive onset Tc = 11.6 K, resistive onset = 12.5 K)
journal, July 1990

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Hybrid Molecular Materials Based upon Organic π-Electron Donors and Metal Complexes. Radical Salts of Bis(ethylenethia)tetrathiafulvalene (BET-TTF) with the Octahedral Anions Hexacyanoferrate(III) and Nitroprusside. The First Kappa Phase in the BET-TTF Family
journal, July 2001

Redox-switchable breathing behavior in tetrathiafulvalene-based metal–organic frameworks
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Metal–Organic Framework Materials as Chemical Sensors
journal, September 2011

Tuning the structure and function of metal–organic frameworks via linker design
journal, January 2014

A New Ambient Pressure Organic Superconductor Based on BEDT-TTF with T _C Higher than 10 K (T _C =10.4 K)
journal, January 1988

The Organic Secondary Building Unit: Strong Intermolecular π Interactions Define Topology in MIT-25, a Mesoporous MOF with Proton-Replete Channels
journal, March 2017

Crystal Structures, Gas Adsorption, and Electrochemical Properties of Electroactive Coordination Polymers Based on the Tetrathiafulvalene-Tetrabenzoate Ligand
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journal, December 1963

The electronic, optical and magnetic consequences of delocalization in multifunctional donor–acceptor organic polymers
journal, January 2015

Grid-Type Metal Ion Architectures: Functional Metallosupramolecular Arrays
journal, July 2004

Measuring and Reporting Electrical Conductivity in Metal–Organic Frameworks: Cd ₂ (TTFTB) as a Case Study
journal, October 2016

Deconstructing the Crystal Structures of Metal–Organic Frameworks and Related Materials into Their Underlying Nets
journal, September 2011

Electronic, Structural and Functional Versatility in Tetrathiafulvalene‐Lanthanide Metal–Organic Frameworks
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journal, January 2020

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