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Title: Linked supramolecular building blocks for enhanced cluster formation

Abstract

Methylene-bridged calix[4]arenes have emerged as extremely versatile ligand supports in the formation of new polymetallic clusters possessing fascinating magnetic properties. Metal ion binding rules established for this building block allow one to partially rationalise the complex assembly process. The ability to covalently link calix[4]arenes at the methylene bridge provides significantly improved control over the introduction of different metal centres to resulting cluster motifs. Clusters assembled from bis-calix[4]arenes and transition metal ions or 3d-4f combinations display characteristic features of the analogous calix[4]arene supported clusters, thereby demonstrating an enhanced and rational approach towards the targeted synthesis of complex and challenging structures.

Authors:
 [1];  [2];  [3];  [3];  [4];  [2];  [1]
+ Show Author Affiliations
  1. Heriot–Watt University Riccarton, Edinburgh (Scotland)
  2. Univ. of Edinburgh, Scotland (United Kingdom)
  3. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  4. Univ. of Copenhagen (Denmark)
Publication Date:
Research Org.:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1213464
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Chemistry - A European Journal
Additional Journal Information:
Journal Volume: 21; Journal Issue: 7; Journal ID: ISSN 0947-6539
Publisher:
ChemPubSoc Europe
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; calixarenes; clusters; coordination chemistry; magnetism; supramolecular chemistry

Citation Formats

McLellan, Ross, Palacios, Maria A., Beavers, Christine M., Teat, Simon J., Piligkos, Stergios, Brechin, Euan K., and Dalgarno, Scott J. Linked supramolecular building blocks for enhanced cluster formation. United States: N. p., 2015. Web. doi:10.1002/chem.201405746.
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McLellan, Ross, Palacios, Maria A., Beavers, Christine M., Teat, Simon J., Piligkos, Stergios, Brechin, Euan K., & Dalgarno, Scott J. Linked supramolecular building blocks for enhanced cluster formation. United States. https://doi.org/10.1002/chem.201405746
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McLellan, Ross, Palacios, Maria A., Beavers, Christine M., Teat, Simon J., Piligkos, Stergios, Brechin, Euan K., and Dalgarno, Scott J. Fri . "Linked supramolecular building blocks for enhanced cluster formation". United States. https://doi.org/10.1002/chem.201405746. https://www.osti.gov/servlets/purl/1213464.
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@article{osti_1213464,
title = {Linked supramolecular building blocks for enhanced cluster formation},
author = {McLellan, Ross and Palacios, Maria A. and Beavers, Christine M. and Teat, Simon J. and Piligkos, Stergios and Brechin, Euan K. and Dalgarno, Scott J.},
abstractNote = {Methylene-bridged calix[4]arenes have emerged as extremely versatile ligand supports in the formation of new polymetallic clusters possessing fascinating magnetic properties. Metal ion binding rules established for this building block allow one to partially rationalise the complex assembly process. The ability to covalently link calix[4]arenes at the methylene bridge provides significantly improved control over the introduction of different metal centres to resulting cluster motifs. Clusters assembled from bis-calix[4]arenes and transition metal ions or 3d-4f combinations display characteristic features of the analogous calix[4]arene supported clusters, thereby demonstrating an enhanced and rational approach towards the targeted synthesis of complex and challenging structures.},
doi = {10.1002/chem.201405746},
journal = {Chemistry - A European Journal},
number = 7,
volume = 21,
place = {United States},
year = {Fri Jan 09 00:00:00 EST 2015},
month = {Fri Jan 09 00:00:00 EST 2015}
}
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Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1002/chem.201405746
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Citation Metrics:
Cited by: 15 works
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Figures / Tables:

Figure 1 Figure 1: Selected polymetallic TBC[4]-supported clusters and the related bridge-linked bis-TBC[4]. A) Clusters supported by two TBC[4]s with tailored metal composition (Mn4, Mn3Ln1, Mn2Ln2 and Ln6). B) Square within square MnIII4LnMIII 4 clusters supported by four TBC[4]s. C) Tricapped trigonal prismatic Cu9 cluster motif with anions and ligated solvent omittedmore » for clarity. D) Metallic skeletons of clusters shown in A–C with capping TBC[4]-TM/LnM moieties drawn as large spheres. E) Two views of bis-TBC[4] showing the antiparallel arrangement and hydrogen-bonding interactions at the TBC[4] lower-rims. Colour code: Mn, purple; Ln, green; Cu, pale blue; N, royal blue; C, grey; O, red; S, yellow; H atoms are omitted for clarity.« less
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Works referenced in this record:

A classification of spin frustration in molecular magnets from a physical study of large odd-numbered-metal, odd electron rings
journal, November 2012

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A Calix[4]arene 3d/4f Magnetic Cooler
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The Importance of Being Exchanged: [Gd III 4 M II 8 (OH) 8 (L) 8 (O 2 CR) 8 ] 4+ Clusters for Magnetic Refrigeration
journal, April 2012

  • Hooper, Thomas N.; Schnack, Jürgen; Piligkos, Stergios
  • Angewandte Chemie, Vol. 124, Issue 19
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Calix[4]arene-Based Single-Molecule Magnets
journal, September 2009

  • Karotsis, Georgios; Teat, Simon J.; Wernsdorfer, Wolfgang
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A Calix[4]arene 3d/4f Magnetic Cooler
journal, December 2009

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Calix[4]arene-supported rare earth octahedra
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Calix[4]arene-Based Single-Molecule Magnets
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Calix[4]arene-supported FeIII2LnIII2 clusters
journal, January 2011

  • Sanz, Sergio; Ferreira, Kerry; McIntosh, Ruaraidh D.
  • Chemical Communications, Vol. 47, Issue 32
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A New Polynuclear Coordination Type for (Salicylaldoxime)copper(II) Complexes: Structure and Magnetic Properties of an (Oxime)Cu 6 Cluster
journal, November 2009

  • Wenzel, Marco; Forgan, Ross S.; Faure, Anaëlle
  • European Journal of Inorganic Chemistry, Vol. 2009, Issue 31
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A Family of Calix[4]arene-Supported [MnIII2MnII2] Clusters
journal, May 2011

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A molecular pinwheel multicopper( i ) cluster, [(L S− ) 6 Cu I 13 (S 2− ) 2 ] 3+ with μ 4 -sulfido, μ 3 -thiolato and nitrogenligands
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A Mixed-Valence Polyoxovanadate(III,IV) Cluster with a Calixarene Cap Exhibiting Ferromagnetic V(III)−V(IV) Interactions
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The Importance of Being Exchanged: [Gd III 4 M II 8 (OH) 8 (L) 8 (O 2 CR) 8 ] 4+ Clusters for Magnetic Refrigeration
journal, April 2012

  • Hooper, Thomas N.; Schnack, Jürgen; Piligkos, Stergios
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A Family of Calix[4]arene-Supported [MnIII2MnII2] Clusters
journal, May 2011

  • Taylor, Stephanie M.; Karotsis, Georgios; McIntosh, Ruaraidh D.
  • Chemistry - A European Journal, Vol. 17, Issue 27
  • DOI: 10.1002/chem.201003327

A classification of spin frustration in molecular magnets from a physical study of large odd-numbered-metal, odd electron rings
journal, November 2012

  • Baker, M. L.; Timco, G. A.; Piligkos, S.
  • Proceedings of the National Academy of Sciences, Vol. 109, Issue 47
  • DOI: 10.1073/pnas.1213127109
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    Works referencing / citing this record:

    Bis-Calix[4]arenes: From Ligand Design to the Directed Assembly of a Metal-Organic Trigonal Antiprism
    journal, May 2016

    • Coletta, Marco; McLellan, Ross; Murphy, Paul
    • Chemistry - A European Journal, Vol. 22, Issue 26
    • DOI: 10.1002/chem.201600762

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

    • Coletta, Marco; McLellan, Ross; Sanz, Sergio
    • Chemistry - A European Journal, Vol. 23, Issue 56
    • DOI: 10.1002/chem.201703197

    Supramolecular fluorescence enhancement via coordination-driven self-assembly in bis-picolylcalixarene blue-emitting M 2 L 2 X n macrocycles
    journal, January 2015

    • Guzmán-Percástegui, Edmundo; Vonlanthen, Mireille; Quiroz-García, Beatriz
    • Dalton Transactions, Vol. 44, Issue 36
    • DOI: 10.1039/c5dt02058a

    Solid-state structure and antimicrobial and cytotoxicity studies of a cucurbit[6]uril-like Cu 6 L 4 constructed from 3,5-bis[(1 H -tetrazol-5-yl)methyl]-4 H -1,2,4-triazol-4-amine
    journal, October 2018

    • Vasylevskyi, Serhii; Holzheu, Anja; Fromm, Katharina M.
    • Acta Crystallographica Section C Structural Chemistry, Vol. 74, Issue 11
    • DOI: 10.1107/s2053229618013670
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