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Metallosupramolecular Functional Helicates
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Metallosupramolecular Functional Helicates

A special issue of Molecules (ISSN 1420-3049). This special issue belongs to the section "Inorganic Chemistry".

Deadline for manuscript submissions: closed (31 December 2023) | Viewed by 7724

Special Issue Editor

Dr. Feng Li

E-Mail Website
Guest Editor
School of Science, Western Sydney University, Penrith, Sydney, NSW 2751, Australia
Interests: metallo-supramolecular; host-guest; molecular recognition; spin crossover; coordination cages; transition metals; metallo-ligand

Special Issue Information

Dear Colleagues,

The construction and investigation of metallo-supramolecular helicates continues to be a fast-growing and fascinating field of current research, with significant attention being paid to inorganic, organic, and biological areas. Metallo-supramolecular helical assemblies can be readily prepared by judicious choice between selected metal ions and suitably designed multidentate ligand components. Different synthetic strategies permit rational control of synergies over both the helix’s structure and its function. Furthermore, metallo-supramolecular helicates have continued to provide interesting avenues of study due to their potential applications in host–guest, photoactive, magnetic, redox-active, conductive, catalytic, ion-transport, non-linear optic and bioactive areas. In particular, the synthesis of functional metallo-supramolecular helicates has been motivated by their use as models for metalloproteins. The bulk research of homometallic metallo-supramolecular helicate motifs has been well documented. However, the search for increasingly complex and multifunctional materials has drawn researchers towards heterometallic and multifunctional helicates.

This Special Issue primarily focuses on the design and synthesis of functional metallo-supramolecular helicates, with emphasis on the unique properties arising from their helicity.

Dr. Feng Li
Guest Editor

Manuscript Submission Information

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Keywords

  • metallo-supramolecular
  • helicates
  • coordination chemistry
  • self-assembly
  • host–guest chemistry
  • molecular recognition

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Published Papers (3 papers)

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Research

15 pages, 3002 KiB  
Article
Study of the Counter Cation Effects on the Supramolecular Structure and Electronic Properties of a Dianionic Oxamate-Based {NiII2} Helicate
by Cintia A. Simosono, Rafaela M. R. da Silva, Nathália R. De Campos, Marye Agnes R. Silva, Antônio C. Doriguetto, Leonã S. Flores, Charlane C. Correa, Tatiana R. G. Simões, Ana Karoline S. M. Valdo, Felipe T. Martins, Flávio Garcia, Guilherme P. Guedes, Breno R. L. Galvão, Juliana Cancino-Bernardi, Ricardo D. dos Reis, Humberto O. Stumpf, Danielle D. Justino, Paulo F. R. Ortega, Walace D. do Pim, Miguel Julve and Maria Vanda Marinhoadd Show full author list remove Hide full author list
Molecules 2023, 28(5), 2086; https://doi.org/10.3390/molecules28052086 - 23 Feb 2023
Cited by 5 | Viewed by 2419
Abstract
Herein, we describe the synthesis, crystal structure, and electronic properties of {[K2(dmso)(H2O)5][Ni2(H2mpba)3]·dmso·2H2O}n (1) and [Ni(H2O)6][Ni2(H2mpba)3]·3CH3 [...] Read more.
Herein, we describe the synthesis, crystal structure, and electronic properties of {[K2(dmso)(H2O)5][Ni2(H2mpba)3]·dmso·2H2O}n (1) and [Ni(H2O)6][Ni2(H2mpba)3]·3CH3OH·4H2O (2) [dmso = dimethyl sulfoxide; CH3OH = methanol; and H4mpba = 1,3-phenylenebis(oxamic acid)] bearing the [Ni2(H2mpba)3]2− helicate, hereafter referred to as {NiII2}. SHAPE software calculations indicate that the coordination geometry of all the NiII atoms in 1 and 2 is a distorted octahedron (Oh) whereas the coordination environments for K1 and K2 atoms in 1 are Snub disphenoid J84 (D2d) and distorted octahedron (Oh), respectively. The {NiII2} helicate in 1 is connected by K+ counter cations yielding a 2D coordination network with sql topology. In contrast to 1, the electroneutrality of the triple-stranded [Ni2(H2mpba)3] 2− dinuclear motif in 2 is achieved by a [Ni(H2O)6]2+ complex cation, where the three neighboring {NiII2} units interact in a supramolecular fashion through four R22(10) homosynthons yielding a 2D array. Voltammetric measurements reveal that both compounds are redox active (with the NiII/NiI pair being mediated by OH– ions) but with differences in formal potentials that reflect changes in the energy levels of molecular orbitals. The NiII ions from the helicate and the counter-ion (complex cation) in 2 can be reversibly reduced, resulting in the highest faradaic current intensities. The redox reactions in 1 also occur in an alkaline medium but at higher formal potentials. The connection of the helicate with the K+ counter cation has an impact on the energy levels of the molecular orbitals; this experimental behavior was further supported by X-ray absorption near-edge spectroscopy (XANES) experiments and computational calculations. Full article
(This article belongs to the Special Issue Metallosupramolecular Functional Helicates)
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12 pages, 2818 KiB  
Article
Investigating the Conformations of a Family of [M2L3]4+ Helicates Using Single Crystal X-ray Diffraction
by Matthew J. Wallis, Hyunsung Min, Leonard F. Lindoy and Feng Li
Molecules 2023, 28(3), 1404; https://doi.org/10.3390/molecules28031404 - 1 Feb 2023
Cited by 9 | Viewed by 2180
Abstract
We present five new dinuclear triple helicate compounds of types [Mn2L3](ClO4)4, [Co2L3](BF4)4, [Ni2L3](BF4)4, [Cu2L3](BF4 [...] Read more.
We present five new dinuclear triple helicate compounds of types [Mn2L3](ClO4)4, [Co2L3](BF4)4, [Ni2L3](BF4)4, [Cu2L3](BF4)4, and [Zn2L3](BF4)4, where L is a previously reported semi-rigid ligand incorporating two α-diimine primary donor groups and two secondary 4-pyridyl donor groups. All complexes have been characterized in both solution and the solid state. Single crystal X-ray diffraction studies were used to probe the variation in the respective helical structures as the coordinated metal ion was altered, including the effect on the orientations of the secondary binding domains. The influence of the metal ion size, the spin state in the case of Fe(II), and the presence of Jahn-Teller distortions on the overall helical structure has been investigated. These results form a basis for the design and construction of new large metallosupramolecular architectures which manifest properties associated with the constituent helical metalloligand units. Full article
(This article belongs to the Special Issue Metallosupramolecular Functional Helicates)
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14 pages, 5511 KiB  
Article
pH and Salt-Assisted Macroscopic Chirality Inversion of Gadolinium Coordination Polymer
by Ting Hou, Lan-Qing Wu, Yan Xu, Song-Song Bao and Li-Min Zheng
Molecules 2023, 28(1), 163; https://doi.org/10.3390/molecules28010163 - 25 Dec 2022
Cited by 7 | Viewed by 2257
Abstract
The precise adjustment of handedness of helical architectures is important to regulate their functions. Macroscopic chirality inversion has been achieved in organic supramolecular systems by pH, metal ions, solvents, chiral and non-chiral additives, temperature, and light, but rarely in coordination polymers (CPs). In [...] Read more.
The precise adjustment of handedness of helical architectures is important to regulate their functions. Macroscopic chirality inversion has been achieved in organic supramolecular systems by pH, metal ions, solvents, chiral and non-chiral additives, temperature, and light, but rarely in coordination polymers (CPs). In particular, salt-assisted macroscopic chirality inversion has not been reported. In this work, we carried out a systematic investigation on the role of pH and salt in regulating the morphology of CPs based on Gd(NO3)3 and R-(1-phenylethylamino)methylphosphonic acid (R-pempH2). Without extra NO3−, the chirality inversion from the left-handed superhelix R-M to the right-handed superhelix R-P can be achieved by pH modulation from 3.2 to 3.8. The addition of NaNO3 (2.0 eq) at pH 3.8 results in an inversion of chiral sense from R-P to R-M as a pure phase. To our knowledge, this is the first example of salt-assisted macroscopic helical inversion in artificial systems. Full article
(This article belongs to the Special Issue Metallosupramolecular Functional Helicates)
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