The remarkable influence of N, O-ligands in the assembly of a bis-calix[4]arene-supported [MnIV2MnIII10MnII8] cluster

Coletta, Marco; Sanz, Sergio; McCormick, Laura J.; Teat, Simon J.; Brechin, Euan K.; Dalgarno, Scott J.

doi:10.1039/c7dt04233g

Title: The remarkable influence of N, O-ligands in the assembly of a bis-calix[4]arene-supported [Mn^IV₂Mn^III₁₀Mn^II₈] cluster

Abstract

We report that calix[4]arenes are versatile ligands, capable of supporting the formation of a wide variety of polymetallic clusters comprising 3d, 4f or 3d-4f metal ions. Calixarene-based metal ion fragments act as both bridging and structure capping moieties in these systems, and this behaviour is systematically extended upon moving to bis-calix[4]arene, a relatively new ligand in which two calix[4]arenes are tethered at the methylene bridge position. N,O-Ligands greatly influence cluster formation with bis-calix[4]arene, affording a remarkable mixed-valence [Mn^IV₂Mn^III₁₀Mn^II₈] cluster that displays coordination chemistry typical of each ligand type, but also new structure capping behaviour for the latter.

Authors:

^[1];

^[2];

^[3]; Teat, Simon J. ^[3];

^[2];

^[1]

Heriot-Watt Univ., Riccarton, Edinburgh (United Kingdom)
Univ. of Edinburgh, Scotland (United Kingdom)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)

Publication Date:: Fri Nov 24 00:00:00 EST 2017

Research Org.:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

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

OSTI Identifier:: 1530277

Grant/Contract Number:: AC02-05CH11231

Resource Type:: Accepted Manuscript

Journal Name:: Dalton Transactions

Additional Journal Information:: Journal Volume: 46; Journal Issue: 48; Journal ID: ISSN 1477-9226

Publisher:: Royal Society of Chemistry

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats


                    Coletta, Marco, Sanz, Sergio, McCormick, Laura J., Teat, Simon J., Brechin, Euan K., and Dalgarno, Scott J. The remarkable influence of N, O-ligands in the assembly of a bis-calix[4]arene-supported [MnIV2MnIII10MnII8] cluster.  United States: N. p., 2017. 
Web.  doi:10.1039/c7dt04233g.

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                    Coletta, Marco, Sanz, Sergio, McCormick, Laura J., Teat, Simon J., Brechin, Euan K., & Dalgarno, Scott J. The remarkable influence of N, O-ligands in the assembly of a bis-calix[4]arene-supported [MnIV2MnIII10MnII8] cluster.  United States.  https://doi.org/10.1039/c7dt04233g

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                    Coletta, Marco, Sanz, Sergio, McCormick, Laura J., Teat, Simon J., Brechin, Euan K., and Dalgarno, Scott J. Fri .  
"The remarkable influence of N, O-ligands in the assembly of a bis-calix[4]arene-supported [MnIV2MnIII10MnII8] cluster".  United States.  https://doi.org/10.1039/c7dt04233g.  https://www.osti.gov/servlets/purl/1530277.

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@article{osti_1530277,

  title        = {The remarkable influence of N, O-ligands in the assembly of a bis-calix[4]arene-supported [MnIV2MnIII10MnII8] cluster},

  author       = {Coletta, Marco and Sanz, Sergio and McCormick, Laura J. and Teat, Simon J. and Brechin, Euan K. and Dalgarno, Scott J.},

  abstractNote = {We report that calix[4]arenes are versatile ligands, capable of supporting the formation of a wide variety of polymetallic clusters comprising 3d, 4f or 3d-4f metal ions. Calixarene-based metal ion fragments act as both bridging and structure capping moieties in these systems, and this behaviour is systematically extended upon moving to bis-calix[4]arene, a relatively new ligand in which two calix[4]arenes are tethered at the methylene bridge position. N,O-Ligands greatly influence cluster formation with bis-calix[4]arene, affording a remarkable mixed-valence [MnIV2MnIII10MnII8] cluster that displays coordination chemistry typical of each ligand type, but also new structure capping behaviour for the latter.},

  doi          = {10.1039/c7dt04233g},

  journal      = {Dalton Transactions},

  number       = 48,

  volume       = 46,

  place        = {United States},

  year         = {Fri Nov 24 00:00:00 EST 2017},

  month        = {Fri Nov 24 00:00:00 EST 2017}

}

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Figure 1: Single crystal X-ray structures of 1 (A),^2a 2 (B),^3b H₈L1 (C), ¹⁴ 3 (D),¹⁴ 4 (E),¹⁵ and 5 (F).¹⁶ Colour code C – grey, O – red, N – royal blue, Mn^II – pale blue, Mn^III – purple, Cu^II – light blue, Ln^III – green. Hydrogen atoms (exceptmore »

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Title: The remarkable influence of N, O-ligands in the assembly of a bis-calix[4]arene-supported [MnIV2MnIII10MnII8] cluster

Abstract

Citation Formats

Figures / Tables:

Polytopic ligand directed self-assembly—polymetallic [n×n] grids versus non-grid oligomers journal, January 2009

The Use of Calixarenes in Metal-Based Catalysis journal, December 2008

Synthesis, structure, and properties of a new representative of the family of calix[4]arene-containing [MnII 2MnIII 2]-clusters journal, February 2013

Transition metal and lanthanide cluster complexes constructed with thiacalix[n]arene and its derivatives journal, July 2007

Unusual Structural Types in Manganese Cluster Chemistry from the Use of N , N , N ‘, N ‘-Tetrakis(2-hydroxyethyl)ethylenediamine: Mn 8 , Mn 12 , and Mn 20 Clusters journal, January 2008

Calix[4]arene-Based Single-Molecule Magnets journal, September 2009

Supertetrahedral icosanuclear and ring-like decanuclear mixed valent manganese(ii/iii) triethanolamine clusters journal, January 2010

Calix[4]arene-supported rare earth octahedra journal, January 2012

Heterometallic 3d–4f Single-Molecule Magnets: Ligand and Metal Ion Influences on the Magnetic Relaxation journal, March 2015

Experimental and theoretical study of the influence of peripheral environment on magnetic properties of tetranuclear manganese skeleton in new representatives of calix[4]arene-containing [MnII2 MnIII2] clusters journal, February 2015

Calixarene-supported hexadysprosium cluster showing single molecule magnet behavior journal, April 2012

Complementary ligands direct the formation of a calix[8]arene-supported ferromagnetic MnIVMnIII dimer journal, January 2013

Synthesis of Single-molecule Magnets Using Metallocyanates book, January 2006

Metallocalixarene catalysts: α-olefin polymerization and ROP of cyclic esters journal, January 2016

A Mixed-Valence Polyoxovanadate(III,IV) Cluster with a Calixarene Cap Exhibiting Ferromagnetic V(III)−V(IV) Interactions journal, February 2008

Synthesis and characterization of a series of manganese phosphonate complexes with various valences and nuclearity journal, January 2009

Synthesis and reactions of a 2-chlorocalix[4]arene and a 2,2′-coupled dicalixarene journal, June 2013

Thiacalixarene-based nanoscale polyhedral coordination cages journal, September 2014

Core expansion of bis-calix[4]arene-supported clusters journal, January 2016

Linked Supramolecular Building Blocks for Enhanced Cluster Formation journal, January 2015

Calixarene supported enneanuclear Cu(ii) clusters journal, January 2010

Diol-type ligands as central ‘players’ in the chemistry of high-spin molecules and single-molecule magnets journal, January 2008

The coordination chemistry of pyridyl oximes journal, January 2006

Self-assembly of two high-nuclearity manganese calixarene-phosphonate clusters: diamond-like Mn 16 and drum-like Mn 14 journal, January 2015

[Mn III 4 Ln III 4 ] Calix[4]arene Clusters as Enhanced Magnetic Coolers and Molecular Magnets journal, September 2010

Elucidating the Ring Inversion Mechanism(s) for Biscalixarenes journal, August 2014

Self-assembly and decay of Mn(ii) pivalate–phosphonate complexes journal, January 2014

Syntheses and Properties of Metal-Centered Mixed-Valent [NEt4]{MnII?[MnII3MnIII3Cl6(L)6]} Manganese Wheels journal, March 2005

Design of magnetic coordination complexes for quantum computing journal, January 2012

Calix[4]arene-supported FeIII2LnIII2 clusters journal, January 2011

Phosphonate Ligands Stabilize Mixed-Valent {MnIII20−xMnIIx} Clusters with Large Spin and Coercivity journal, August 2005

Facile Interchange of 3d and 4f Ions in Single-Molecule Magnets: Stepwise Assembly of [Mn 4 ], [Mn 3 Ln] and [Mn 2 Ln 2 ] Cages within Calix[4]arene Scaffolds journal, June 2015

A Family of Calix[4]arene-Supported [MnIII2MnII2] Clusters journal, May 2011

A New Family of 3 d -4 f Bis-Calix[4]arene-Supported Clusters journal, September 2017

Lanthanide ion complexes of the calixarenes. Part 4. Double inclusion by p-t-butylcalix[4]arene (H4L). Crystal structures of [Eu2(HL)2(dmf)4].7dmf (dmf = dimethylformamide) and H4L.dmso (dmso = dimethyl sulphoxide) journal, January 1989

A new class of single-molecule magnets: mixed-valent [Mn4(O2CMe)2(Hpdm)6][ClO4]2 with an S = 8 ground state journal, January 1999

A Mn15 single-molecule magnet consisting of a supertetrahedron incorporated in a loop journal, January 2010

Coordination Cluster Nuclearity Decreases with Decreasing Rare Earth Ionic Radius in 1:1 Cr/Ln N -Butyldiethanolamine Compounds: A Journey across the Lanthanide Series from Cr 4 III La 4 –Cr 4 III Tb 4 via Cr 3 III Dy 3 and Cr 3 III Ho 3 to Cr 2 III Er 2 –Cr 2 III Lu 2 journal, March 2015

Heterometallic Rings: Their Physics and use as Supramolecular Building Blocks journal, October 2015

Calix[4]arene-Based Single-Molecule Magnets journal, September 2009

The Coordination Chemistry of Pyridyl Oximes journal, May 2006

Phosphonate Ligands Stabilize Mixed-Valent {MnIII20−xMnIIx} Clusters with Large Spin and Coercivity journal, August 2005

Title: The remarkable influence of N, O-ligands in the assembly of a bis-calix[4]arene-supported [Mn^IV₂Mn^III₁₀Mn^II₈] cluster

Polytopic ligand directed self-assembly—polymetallic [n×n] grids versus non-grid oligomers
journal, January 2009

The Use of Calixarenes in Metal-Based Catalysis
journal, December 2008

Synthesis, structure, and properties of a new representative of the family of calix[4]arene-containing [MnII 2MnIII 2]-clusters
journal, February 2013

Transition metal and lanthanide cluster complexes constructed with thiacalix[n]arene and its derivatives
journal, July 2007

Unusual Structural Types in Manganese Cluster Chemistry from the Use of N , N , N ‘, N ‘-Tetrakis(2-hydroxyethyl)ethylenediamine: Mn ₈ , Mn ₁₂ , and Mn ₂₀ Clusters
journal, January 2008

Calix[4]arene-Based Single-Molecule Magnets
journal, September 2009

Supertetrahedral icosanuclear and ring-like decanuclear mixed valent manganese(ii/iii) triethanolamine clusters
journal, January 2010

Calix[4]arene-supported rare earth octahedra
journal, January 2012

Heterometallic 3d–4f Single-Molecule Magnets: Ligand and Metal Ion Influences on the Magnetic Relaxation
journal, March 2015

Experimental and theoretical study of the influence of peripheral environment on magnetic properties of tetranuclear manganese skeleton in new representatives of calix[4]arene-containing [MnII2 MnIII2] clusters
journal, February 2015

Calixarene-supported hexadysprosium cluster showing single molecule magnet behavior
journal, April 2012

Complementary ligands direct the formation of a calix[8]arene-supported ferromagnetic MnIVMnIII dimer
journal, January 2013

Synthesis of Single-molecule Magnets Using Metallocyanates
book, January 2006

Metallocalixarene catalysts: α-olefin polymerization and ROP of cyclic esters
journal, January 2016

A Mixed-Valence Polyoxovanadate(III,IV) Cluster with a Calixarene Cap Exhibiting Ferromagnetic V(III)−V(IV) Interactions
journal, February 2008

Synthesis and characterization of a series of manganese phosphonate complexes with various valences and nuclearity
journal, January 2009

Synthesis and reactions of a 2-chlorocalix[4]arene and a 2,2′-coupled dicalixarene
journal, June 2013

Thiacalixarene-based nanoscale polyhedral coordination cages
journal, September 2014

Core expansion of bis-calix[4]arene-supported clusters
journal, January 2016

Linked Supramolecular Building Blocks for Enhanced Cluster Formation
journal, January 2015

Calixarene supported enneanuclear Cu(ii) clusters
journal, January 2010

Diol-type ligands as central ‘players’ in the chemistry of high-spin molecules and single-molecule magnets
journal, January 2008

The coordination chemistry of pyridyl oximes
journal, January 2006

Self-assembly of two high-nuclearity manganese calixarene-phosphonate clusters: diamond-like Mn ₁₆ and drum-like Mn ₁₄
journal, January 2015

[Mn ^III ₄ Ln ^III ₄ ] Calix[4]arene Clusters as Enhanced Magnetic Coolers and Molecular Magnets
journal, September 2010

Elucidating the Ring Inversion Mechanism(s) for Biscalixarenes
journal, August 2014

Self-assembly and decay of Mn(ii) pivalate–phosphonate complexes
journal, January 2014

Syntheses and Properties of Metal-Centered Mixed-Valent [NEt4]{MnII?[MnII3MnIII3Cl6(L)6]} Manganese Wheels
journal, March 2005

Design of magnetic coordination complexes for quantum computing
journal, January 2012

Calix[4]arene-supported FeIII2LnIII2 clusters
journal, January 2011

Phosphonate Ligands Stabilize Mixed-Valent {MnIII20−xMnIIx} Clusters with Large Spin and Coercivity
journal, August 2005

Facile Interchange of 3d and 4f Ions in Single-Molecule Magnets: Stepwise Assembly of [Mn ₄ ], [Mn ₃ Ln] and [Mn ₂ Ln ₂ ] Cages within Calix[4]arene Scaffolds
journal, June 2015

A Family of Calix[4]arene-Supported [MnIII2MnII2] Clusters
journal, May 2011

A New Family of 3 d -4 f Bis-Calix[4]arene-Supported Clusters
journal, September 2017

Lanthanide ion complexes of the calixarenes. Part 4. Double inclusion by p-t-butylcalix[4]arene (H4L). Crystal structures of [Eu2(HL)2(dmf)4].7dmf (dmf = dimethylformamide) and H4L.dmso (dmso = dimethyl sulphoxide)
journal, January 1989

A new class of single-molecule magnets: mixed-valent [Mn4(O2CMe)2(Hpdm)6][ClO4]2 with an S = 8 ground state
journal, January 1999

A Mn15 single-molecule magnet consisting of a supertetrahedron incorporated in a loop
journal, January 2010

Heterometallic Rings: Their Physics and use as Supramolecular Building Blocks
journal, October 2015

Calix[4]arene-Based Single-Molecule Magnets
journal, September 2009

The Coordination Chemistry of Pyridyl Oximes
journal, May 2006

Phosphonate Ligands Stabilize Mixed-Valent {MnIII20−xMnIIx} Clusters with Large Spin and Coercivity
journal, August 2005