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Title: Cation-Dependent Intrinsic Electrical Conductivity in Isostructural Tetrathiafulvalene-Based Microporous Metal–Organic Frameworks

Abstract

Isostructural metal-organic frameworks (MOFs) M2(TTFTB) (M = Mn, Co, Zn, and Cd; H4TTFTB = tetrathiafulvalene tetrabenzoate) exhibit a striking correlation between their single-crystal conductivities and the shortest S···S interaction defined by neighboring TTF cores, which inversely correlates with the ionic radius of the metal ions. The larger cations cause a pinching of the S···S contact, which is responsible for better orbital overlap between pz orbitals on neighboring S and C atoms. Density functional theory calculations show that these orbitals are critically involved in the valence band of these materials, such that modulation of the S···S distance has an important effect on band dispersion and, implicitly, on the conductivity. The Cd analogue, with the largest cation and shortest S···S contact, shows the largest electrical conductivity, σ = 2.86 (±0.53) × 10-4 S/cm, which is also among the highest in microporous MOFs. These results describe the first demonstration of tunable intrinsic electrical conductivity in this class of materials and serve as a blueprint for controlling charge transport in MOFs with π-stacked motifs.

Authors:
 [1];  [1];  [1];  [2];  [2];  [1];  [1]
  1. Department of Chemistry, Massachusetts Institute of Technology, 77 Massachusetts Avenue, Cambridge, Massachusetts 02139, United States
  2. Department of Chemistry, University of Bath, Claverton Down, Bath BA2 7AY, United Kingdom
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Center for Excitonics (CE)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1170238
Alternate Identifier(s):
OSTI ID: 1385577
Grant/Contract Number:  
SC0001088; SC0006937
Resource Type:
Published Article
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Name: Journal of the American Chemical Society Journal Volume: 137 Journal Issue: 5; Journal ID: ISSN 0002-7863
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
14 SOLAR ENERGY; 36 MATERIALS SCIENCE; solar (photovoltaic), solid state lighting, photosynthesis (natural and artificial), charge transport, optics, synthesis (novel materials), synthesis (self-assembly), synthesis (scalable processing)

Citation Formats

Park, Sarah S., Hontz, Eric R., Sun, Lei, Hendon, Christopher H., Walsh, Aron, Van Voorhis, Troy, and Dincă, Mircea. Cation-Dependent Intrinsic Electrical Conductivity in Isostructural Tetrathiafulvalene-Based Microporous Metal–Organic Frameworks. United States: N. p., 2015. Web. doi:10.1021/ja512437u.
Park, Sarah S., Hontz, Eric R., Sun, Lei, Hendon, Christopher H., Walsh, Aron, Van Voorhis, Troy, & Dincă, Mircea. Cation-Dependent Intrinsic Electrical Conductivity in Isostructural Tetrathiafulvalene-Based Microporous Metal–Organic Frameworks. United States. doi:10.1021/ja512437u.
Park, Sarah S., Hontz, Eric R., Sun, Lei, Hendon, Christopher H., Walsh, Aron, Van Voorhis, Troy, and Dincă, Mircea. Mon . "Cation-Dependent Intrinsic Electrical Conductivity in Isostructural Tetrathiafulvalene-Based Microporous Metal–Organic Frameworks". United States. doi:10.1021/ja512437u.
@article{osti_1170238,
title = {Cation-Dependent Intrinsic Electrical Conductivity in Isostructural Tetrathiafulvalene-Based Microporous Metal–Organic Frameworks},
author = {Park, Sarah S. and Hontz, Eric R. and Sun, Lei and Hendon, Christopher H. and Walsh, Aron and Van Voorhis, Troy and Dincă, Mircea},
abstractNote = {Isostructural metal-organic frameworks (MOFs) M2(TTFTB) (M = Mn, Co, Zn, and Cd; H4TTFTB = tetrathiafulvalene tetrabenzoate) exhibit a striking correlation between their single-crystal conductivities and the shortest S···S interaction defined by neighboring TTF cores, which inversely correlates with the ionic radius of the metal ions. The larger cations cause a pinching of the S···S contact, which is responsible for better orbital overlap between pz orbitals on neighboring S and C atoms. Density functional theory calculations show that these orbitals are critically involved in the valence band of these materials, such that modulation of the S···S distance has an important effect on band dispersion and, implicitly, on the conductivity. The Cd analogue, with the largest cation and shortest S···S contact, shows the largest electrical conductivity, σ = 2.86 (±0.53) × 10-4 S/cm, which is also among the highest in microporous MOFs. These results describe the first demonstration of tunable intrinsic electrical conductivity in this class of materials and serve as a blueprint for controlling charge transport in MOFs with π-stacked motifs.},
doi = {10.1021/ja512437u},
journal = {Journal of the American Chemical Society},
number = 5,
volume = 137,
place = {United States},
year = {2015},
month = {1}
}

Journal Article:
Free Publicly Available Full Text
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DOI: 10.1021/ja512437u

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Cited by: 84 works
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Figures / Tables:

Figure 1 Figure 1: (a) Calculated band structure and projected density of states of Zn2(TTFTB). The work function, ϕ, and absolute energy scale are aligned to vacuum according to ref 20. The coordinates of the reciprocal space points are Γ = (0, 0, 0) and A = (0, 0, 1/2). Corresponding pictorialmore » representation of the valence band orbitals in Zn2(TTFTB) (b) and one of the TTF cores (c). Zn atoms and their coordination sphere are represented by black polyhedra. Gold, red, black, and white spheres represent S, O, C, and H atoms, respectively.« less

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journal, January 2016

  • Sun, Lei; Campbell, Michael G.; Dincă, Mircea
  • Angewandte Chemie International Edition, Vol. 55, Issue 11
  • DOI: 10.1002/anie.201506219

Metal-Organic Frameworks Containing Missing-Linker Defects Leading to High Hydroxide-Ion Conductivity
journal, December 2015

  • Montoro, Carmen; Ocón, Pilar; Zamora, Félix
  • Chemistry - A European Journal, Vol. 22, Issue 5
  • DOI: 10.1002/chem.201503951

The Design of Water Oxidation Electrocatalysts from Nanoscale Metal–Organic Frameworks
journal, July 2018

  • Shao, Qi; Yang, Jian; Huang, Xiaoqing
  • Chemistry – A European Journal, Vol. 24, Issue 57
  • DOI: 10.1002/chem.201801572

Anion‐Coordination‐Assisted Assembly of Supramolecular Charge‐Transfer Complexes Based on Tris(urea) Ligands
journal, January 2020

  • Zhang, Dan; Hou, Le‐Kai; Zhang, Qiang
  • Chemistry – A European Journal, Vol. 26, Issue 6
  • DOI: 10.1002/chem.201905021

Recent Development and Application of Conductive MOFs
journal, August 2018


Electroactive Metalorganic Frameworks
journal, October 2018

  • Medina, Dana D.; Mähringer, Andre; Bein, Thomas
  • Israel Journal of Chemistry, Vol. 58, Issue 9-10
  • DOI: 10.1002/ijch.201800110

Mechano-regulated metal–organic framework nanofilm for ultrasensitive and anti-jamming strain sensing
journal, September 2018


Microbial reduction of metal-organic frameworks enables synergistic chromium removal
journal, November 2019

  • Springthorpe, Sarah K.; Dundas, Christopher M.; Keitz, Benjamin K.
  • Nature Communications, Vol. 10, Issue 1
  • DOI: 10.1038/s41467-019-13219-w

Electron delocalization and charge mobility as a function of reduction in a metal–organic framework
journal, June 2018


Modulating the rate of charge transport in a metal–organic framework thin film using host:guest chemistry
journal, January 2016

  • Hod, Idan; Farha, Omar K.; Hupp, Joseph T.
  • Chemical Communications, Vol. 52, Issue 8
  • DOI: 10.1039/c5cc09695b

Exploiting redox activity in metal–organic frameworks: concepts, trends and perspectives
journal, January 2016


An updated roadmap for the integration of metal–organic frameworks with electronic devices and chemical sensors
journal, January 2017

  • Stassen, Ivo; Burtch, Nicholas; Talin, Alec
  • Chemical Society Reviews, Vol. 46, Issue 11
  • DOI: 10.1039/c7cs00122c

Emerging crystalline porous materials as a multifunctional platform for electrochemical energy storage
journal, January 2017

  • Zhou, Junwen; Wang, Bo
  • Chemical Society Reviews, Vol. 46, Issue 22
  • DOI: 10.1039/c7cs00283a

Magnetic functionalities in MOFs: from the framework to the pore
journal, January 2018

  • Mínguez Espallargas, Guillermo; Coronado, Eugenio
  • Chemical Society Reviews, Vol. 47, Issue 2
  • DOI: 10.1039/c7cs00653e

Is iron unique in promoting electrical conductivity in MOFs?
journal, January 2017

  • Sun, Lei; Hendon, Christopher H.; Park, Sarah S.
  • Chemical Science, Vol. 8, Issue 6
  • DOI: 10.1039/c7sc00647k

The role of redox hopping in metal–organic framework electrocatalysis
journal, January 2018

  • Lin, Shaoyang; Usov, Pavel M.; Morris, Amanda J.
  • Chemical Communications, Vol. 54, Issue 51
  • DOI: 10.1039/c8cc01664j

Conductive two-dimensional metal–organic frameworks as multifunctional materials
journal, January 2018

  • Ko, Michael; Mendecki, Lukasz; Mirica, Katherine A.
  • Chemical Communications, Vol. 54, Issue 57
  • DOI: 10.1039/c8cc02871k

Functionalised tetrathiafulvalene- (TTF-) macrocycles: recent trends in applied supramolecular chemistry
journal, January 2018

  • Jana, Atanu; Bähring, Steffen; Ishida, Masatoshi
  • Chemical Society Reviews, Vol. 47, Issue 15
  • DOI: 10.1039/c8cs00035b

A porous, electrically conductive hexa-zirconium( iv ) metal–organic framework
journal, January 2018

  • Goswami, Subhadip; Ray, Debmalya; Otake, Ken-ichi
  • Chemical Science, Vol. 9, Issue 19
  • DOI: 10.1039/c8sc00961a

Interdigitated conducting tetrathiafulvalene-based coordination networks
journal, January 2020

  • Bechu, Damien; Xie, Lilia S.; Le Breton, Nolwenn
  • Chemical Communications, Vol. 56, Issue 16
  • DOI: 10.1039/c9cc09960c

Rational modifications of PCN-700 to induce electrical conductivity: a computational study
journal, January 2020

  • Chong, Sanggyu; Kim, Jihan
  • Dalton Transactions, Vol. 49, Issue 1
  • DOI: 10.1039/c9dt03865e

Switchable electrical conductivity in a three-dimensional metal–organic framework via reversible ligand n-doping
journal, January 2020

  • Wentz, Hanna C.; Skorupskii, Grigorii; Bonfim, Ana B.
  • Chemical Science, Vol. 11, Issue 5
  • DOI: 10.1039/c9sc06150a

Coordination polymer-based conductive materials: ionic conductivity vs. electronic conductivity
journal, January 2019

  • Wang, Hai-Ning; Meng, Xing; Dong, Long-Zhang
  • Journal of Materials Chemistry A, Vol. 7, Issue 42
  • DOI: 10.1039/c9ta08253k

Emergence of electrical conductivity in a flexible coordination polymer by using chemical reduction
journal, January 2020

  • Fuku, Kentaro; Miyata, Momoka; Takaishi, Shinya
  • Chemical Communications, Vol. 56, Issue 61
  • DOI: 10.1039/d0cc03062g

Development of multi-metallic complexes using metal-salen complexes as building blocks
journal, November 2019


Prospects for electroactive and conducting framework materials
journal, May 2019

  • Murase, Ryuichi; Ding, Bowen; Gu, Qinyi
  • Philosophical Transactions of the Royal Society A: Mathematical, Physical and Engineering Sciences, Vol. 377, Issue 2149
  • DOI: 10.1098/rsta.2018.0226

On/off switchable electronic conduction in intercalated metal-organic frameworks
journal, August 2017

  • Ogihara, Nobuhiro; Ohba, Nobuko; Kishida, Yoshihiro
  • Science Advances, Vol. 3, Issue 8
  • DOI: 10.1126/sciadv.1603103

Charge-transfer interactions between fullerenes and a mesoporous tetrathiafulvalene-based metal–organic framework
journal, January 2019

  • Souto, Manuel; Calbo, Joaquín; Mañas-Valero, Samuel
  • Beilstein Journal of Nanotechnology, Vol. 10
  • DOI: 10.3762/bjnano.10.183

    Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.