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Polymers
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Coordination Polymers: New Materials for Multiple Applications
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Coordination Polymers: New Materials for Multiple Applications

A special issue of Polymers (ISSN 2073-4360).

Deadline for manuscript submissions: closed (20 December 2015) | Viewed by 86044

Special Issue Editors

Prof. Dr. Félix Zamora

E-Mail Website
Guest Editor
1. Departamento de Química Inorgánica, Universidad Autónoma de Madrid, 28049 Madrid, Spain
2. Institute for Advanced Research in Chemical Sciences (IAdChem), Universidad Autónoma de Madrid, 28049 Madrid, Spain
3. Condensed Matter Physics Center (IFIMAC), Universidad Autónoma de Madrid, 28049 Madrid, Spain
Interests: nanomaterials; 2D materials; porous materials
Special Issues, Collections and Topics in MDPI journals
Dr. Guillermo Mínguez Espallargas

E-Mail Website
Guest Editor
Instituto de Ciencia Molecular (ICMol), Universidad de Valencia, 46980 Paterna, Spain
Interests: coordination polymers; MOFs; molecular magnetism; crystal engineering; responsive materials

Special Issue Information

Dear Colleagues,

Coordination polymers complement the fascinating covalent polymer world and enhance the fabrication of technological materials. The last 30 years have witnessed the expansion of the study of coordination polymers, which is now at the forefront of research in many laboratories around the world. The combination of organic ligands with metal centers via coordination bonds provides a plethora of materials with versatile architectures and extensive ranges of properties and applications. Some of these materials have been devoted to the preparation of multifunctional and/or stimuli-responsive materials. Although most research efforts have been focused on porous coordination polymers, also known as metal-organic frameworks (MOFs), there is at present a new renaissance of interest towards non-porous coordination polymers.
Additionally, coordination polymers are a current source of materials at the nanoscale level with valuable properties and potential applications ranging from molecular wires to drug-delivery.
This Special Issue aims to showcase the versatility of coordination polymers with examples of the large variety of potential applications, which include gas adsorption and separation, conductivity, magnetism, drug delivery, luminescence, etc.

Dr. Félix Zamora
Dr. Guillermo Mínguez Espallargas
Guest Editors

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Keywords

  • coordination polymers
  • metal-organic frameworks
  • multifunctional materials
  • porous materials
  • stimuli-responsive materials

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Published Papers (11 papers)

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4006 KiB  
Article
Single-Crystal-to-Single-Crystal Anion Exchange in a Gadolinium MOF: Incorporation of POMs and [AuCl4]−
by Javier López-Cabrelles, Guillermo Mínguez Espallargas and Eugenio Coronado
Polymers 2016, 8(5), 171; https://doi.org/10.3390/polym8050171 - 26 Apr 2016
Cited by 8 | Viewed by 6595
Abstract
The encapsulation of functional molecules inside porous coordination polymers (also known as metal-organic frameworks, MOFs) has become of great interest in recent years at the field of multifunctional materials. In this article, we present a study of the effects of size and charge [...] Read more.
The encapsulation of functional molecules inside porous coordination polymers (also known as metal-organic frameworks, MOFs) has become of great interest in recent years at the field of multifunctional materials. In this article, we present a study of the effects of size and charge in the anion exchange process of a Gd based MOF, involving molecular species like polyoxometalates (POMs), and [AuCl4]−. This post-synthetic modification has been characterized by IR, EDAX, and single crystal diffraction, which have provided unequivocal evidence of the location of the anion molecules in the framework. Full article
(This article belongs to the Special Issue Coordination Polymers: New Materials for Multiple Applications)
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3905 KiB  
Article
Hg(II) Coordination Polymers Based on N,N’-bis(pyridine-4-yl)formamidine
by Wayne Hsu, Xiang-Kai Yang, Pradhumna Mahat Chhetri and Jhy-Der Chen
Polymers 2016, 8(4), 137; https://doi.org/10.3390/polym8040137 - 11 Apr 2016
Cited by 11 | Viewed by 5955
Abstract
Reactions of N,N’-bis(pyridine-4-yl)formamidine (4-Hpyf) with HgX2 (X = Cl, Br, and I) afforded the formamidinate complex {[Hg(4-pyf)2]·(THF)}n, 1, and the formamidine complexes {[HgX2(4-Hpyf)]·(MeCN)}n (X = Br, 2; I, 3), which have been structurally characterized [...] Read more.
Reactions of N,N’-bis(pyridine-4-yl)formamidine (4-Hpyf) with HgX2 (X = Cl, Br, and I) afforded the formamidinate complex {[Hg(4-pyf)2]·(THF)}n, 1, and the formamidine complexes {[HgX2(4-Hpyf)]·(MeCN)}n (X = Br, 2; I, 3), which have been structurally characterized by X-ray crystallography. Complex 1 is a 2D layer with the {44·62}-sql topology and complexes 2 and 3 are helical chains. While the helical chains of 2 are linked through N–H···Br hydrogen bonds, those of 3 are linked through self-complementary double N–H···N hydrogen bonds, resulting in 2D supramolecular structures. The 4-pyf- ligands of 1 coordinate to the Hg(II) ions through one pyridyl and one adjacent amine nitrogen atoms and the 4-Hpyf ligands of 2 and 3 coordinate to the Hg(II) ions through two pyridyl nitrogen atoms, resulting in new bidentate binding modes. Complexes 1–3 provide a unique opportunity to envisage the effect of the halide anions of the starting Hg(II) salts on folding and unfolding the Hg(II) coordination polymers. Density function theory (DFT) calculation indicates that the emission of 1 is due to intraligand π→π * charge transfer between two different 4-pyf- ligands, whereas those of 2 and 3 can be ascribed to the charge transfer from non-bonding p-type orbitals of the halide anions to π * orbitals of the 4-pyf- ligands (n→π *). The gas sorption properties of the desolvated product of 1 are compared with the Cu analogues to show that the nature of the counteranion and the solvent-accessible volume are important in determining their adsorption capability. Full article
(This article belongs to the Special Issue Coordination Polymers: New Materials for Multiple Applications)
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2899 KiB  
Article
A Heterobimetallic Anionic 3,6-Connected 2D Coordination Polymer Based on Nitranilate as Ligand
by Samia Benmansour and Carlos J. Gómez-García
Polymers 2016, 8(3), 89; https://doi.org/10.3390/polym8030089 - 16 Mar 2016
Cited by 25 | Viewed by 6715
Abstract
In order to synthesize new coordination polymers with original architectures and interesting magnetic properties, we used the nitranilate ligand (C6O4(NO2)22− = C6N2O82−), derived from the dianionic ligand dhbq [...] Read more.
In order to synthesize new coordination polymers with original architectures and interesting magnetic properties, we used the nitranilate ligand (C6O4(NO2)22− = C6N2O82−), derived from the dianionic ligand dhbq2− (2,5-dihydroxy-1,4-benzoquinone = H2C6O42−). The use of this bis-bidentate bridging ligand led to [(DAMS)2{FeNa(C6N2O8)3}·CH3CN]n (1) (DAMS+ = C16H17N2+ = 4-[4-(dimethylamino)-α-styryl]-1-methylpyridinium), a 2D heterometallic coordination polymer presenting an unprecedented structure for any anilato-based compound. This structural type is a 3,6-connected 2D coordination polymer derived from the well-known honeycomb hexagonal structure, where Fe(III) ions alternate with Na+ dimers (as Na2O12 units) in the vertices of the hexagons and with an additional [Fe(C6N2O8)3]3− anion located in the center of the hexagons connecting the three Na+ dimers. The magnetic properties of compound 1 show the presence of paramagnetic isolated high spin Fe(III) complexes with a zero field splitting, |D| = 8.5 cm−1. Full article
(This article belongs to the Special Issue Coordination Polymers: New Materials for Multiple Applications)
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4890 KiB  
Article
Synthesis, Structures and Luminescence Properties of Metal-Organic Frameworks Based on Lithium-Lanthanide and Terephthalate
by Mohammed S. M. Abdelbaky, Zakariae Amghouz, Santiago García-Granda and José R. García
Polymers 2016, 8(3), 86; https://doi.org/10.3390/polym8030086 - 16 Mar 2016
Cited by 12 | Viewed by 8676
Abstract
Metal-organic frameworks assembled from Ln(III), Li(I) and rigid dicarboxylate ligand, formulated as [LiLn(BDC)2(H2O)·2(H2O)] (MS1-6,7a) and [LiTb(BDC)2] (MS7b) (Ln = Tb, Dy, Ho, Er, Yb, Y0.96Eu0.04, Y0.93Tb0.07, and [...] Read more.
Metal-organic frameworks assembled from Ln(III), Li(I) and rigid dicarboxylate ligand, formulated as [LiLn(BDC)2(H2O)·2(H2O)] (MS1-6,7a) and [LiTb(BDC)2] (MS7b) (Ln = Tb, Dy, Ho, Er, Yb, Y0.96Eu0.04, Y0.93Tb0.07, and H2BDC = terephthalic acid), were obtained under hydrothermal conditions. The isostructural MS1-6 crystallize in monoclinic P21/c space group. While, in the case of Tb3+ a mixture of at least two phases was obtained, the former one (MS7a) and a new monoclinic C2/c phase (MS7b). All compounds have been studied by single-crystal and powder X-ray diffraction, thermal analyses (TGA), vibrational spectroscopy (FTIR), and scanning electron microscopy (SEM-EDX). The structures of MS1-6 and MS7a are built up of inorganic-organic hybrid chains. These chains constructed from unusual four-membered rings, are formed by edge- and vertex-shared {LnO8} and {LiO4} polyhedra through oxygen atoms O3 (vertex) and O6-O7 (edge). Each chain is cross-linked to six neighboring chains through six terephthalate bridges. While, the structure of MS7b is constructed from double inorganic chains, and each chain is, in turn, related symmetrically to the adjacent one through the c glide plane. These chains are formed by infinitely alternating {LiO4} and {TbO8} polyhedra through (O2-O3) edges to create Tb–O–Li connectivity along the c-axis. Both MS1-6,7a and MS7b structures possess a 3D framework with 1D trigonal channels running along the a and c axes, containing water molecules and anhydrous, respectively. Topological studies revealed that MS1-6 and MS7a have a new 2-nodal 3,10-c net, while MS7b generates a 3D net with unusual β-Sn topology. The photoluminescence properties Eu- and Tb-doped compounds (MS5-6) are also investigated, exhibiting strong red and green light emissions, respectively, which are attributed to the efficient energy transfer process from the BDC ligand to Eu3+ and Tb3+. Full article
(This article belongs to the Special Issue Coordination Polymers: New Materials for Multiple Applications)
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3480 KiB  
Article
Tris(bipyridine)Metal(II)-Templated Assemblies of 3D Alkali-Ruthenium Oxalate Coordination Frameworks: Crystal Structures, Characterization and Photocatalytic Activity in Water Reduction
by Alla Dikhtiarenko, Pedro Villanueva-Delgado, Rafael Valiente, José R. García and José Gimeno
Polymers 2016, 8(2), 48; https://doi.org/10.3390/polym8020048 - 15 Feb 2016
Cited by 19 | Viewed by 9379
Abstract
A series of 3D oxalate-bridged ruthenium-based coordination polymers with the formula of {[ZII(bpy)3][MIRu(C2O4)3]}n (ZII = Zn2+ (1), Cu2+ (3, 4), Ru2+ [...] Read more.
A series of 3D oxalate-bridged ruthenium-based coordination polymers with the formula of {[ZII(bpy)3][MIRu(C2O4)3]}n (ZII = Zn2+ (1), Cu2+ (3, 4), Ru2+ (5, 6), Os2+ (7, 8); MI = Li+, Na+; bpy = 2,2’-bipyridine) and {[ZnII(bpy)3](H2O)[LiRu(C2O4)3]}n (2) has been synthesized at room temperature through a self-assembly reaction in aqueous media and characterized by single-crystal and powder X-ray diffraction, elemental analysis, infrared and diffuse reflectance UV–Vis spectroscopy and thermogravimetric analysis. The crystal structures of all compounds comprise chiral 3D honeycomb-like polymeric nets of the srs-type, which possess triangular anionic cages where [ZII(bpy)3]2+ cationic templates are selectively embedded. Structural analysis reveals that the electronic configuration of the cationic guests is affected by electrostatic interaction with the anionic framework. Moreover, the MLCT bands gaps values for 1–8 can be tuned in a rational way by judicious choice of [ZII(bpy)3]2+ guests. The 3D host-guest polymeric architectures can be used as self-supported heterogeneous photocatalysts for the reductive splitting of water, exhibiting photocatalytic activity for the evolution of H2 under UV light irradiation. Full article
(This article belongs to the Special Issue Coordination Polymers: New Materials for Multiple Applications)
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5164 KiB  
Article
Self-Assembly of Discrete Metallocycles versus Coordination Polymers Based on Cu(I) and Ag(I) Ions and Flexible Ligands: Structural Diversification and Luminescent Properties
by Javier Vallejos, Iván Brito, Alejandro Cárdenas, Michael Bolte, Sergio Conejeros, Pere Alemany and Jaime Llanos
Polymers 2016, 8(2), 46; https://doi.org/10.3390/polym8020046 - 15 Feb 2016
Cited by 16 | Viewed by 6799
Abstract
Three new Ag(I) and one Cu(I) coordination compounds with two different positional isomers, propane-1,3-diyl bis(pyridine-4-carboxylate) (L1) and propane-1,3-diyl bis(pyridine-3-carboxylate) (L2), of a bis-(pyridyl-carboxylate) ligand have been synthesized. X-ray diffraction analysis revealed that the self-assembly of L1 with AgCF3SO3 and AgClO [...] Read more.
Three new Ag(I) and one Cu(I) coordination compounds with two different positional isomers, propane-1,3-diyl bis(pyridine-4-carboxylate) (L1) and propane-1,3-diyl bis(pyridine-3-carboxylate) (L2), of a bis-(pyridyl-carboxylate) ligand have been synthesized. X-ray diffraction analysis revealed that the self-assembly of L1 with AgCF3SO3 and AgClO4 salts leads to the formation of discrete binuclear metallocycles {Ag(L1)CF3SO3}2 (1) and {Ag(L1)ClO4}2 (2), respectively. However, self-assembly of the other ligand, L2, with AgCF3SO3 and CuCl salts, results in a 1-D zig-zag chain {Ag(L2)CF3SO3}∞ (3) and a 1-D double-stranded helical chain {Cu2Cl2(L2)2}∞ (4) coordination polymers, respectively. Solid emission spectra recorded at room temperature show interesting luminescence properties for all four compounds in the range from 438 to 550 nm, especially for compound 4 that was found to change its emission color when the wavelength of the excitation radiation is switched from 332 to 436 nm. Full article
(This article belongs to the Special Issue Coordination Polymers: New Materials for Multiple Applications)
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6057 KiB  
Article
New URJC-1 Material with Remarkable Stability and Acid-Base Catalytic Properties
by Pedro Leo, Fernando Martínez, Guillermo Calleja, David Briones, Lukasz Wojtas and Gisela Orcajo
Polymers 2016, 8(2), 44; https://doi.org/10.3390/polym8020044 - 5 Feb 2016
Cited by 12 | Viewed by 6545
Abstract
Emerging new metal-organic structures with tunable physicochemical properties is an exciting research field for diverse applications. In this work, a novel metal-organic framework Cu(HIT)(DMF)0.5, named URJC-1, with a three-dimensional non-interpenetrated utp topological network, has been synthesized. This material exhibits a microporous [...] Read more.
Emerging new metal-organic structures with tunable physicochemical properties is an exciting research field for diverse applications. In this work, a novel metal-organic framework Cu(HIT)(DMF)0.5, named URJC-1, with a three-dimensional non-interpenetrated utp topological network, has been synthesized. This material exhibits a microporous structure with unsaturated copper centers and imidazole–tetrazole linkages that provide accessible Lewis acid/base sites. These features make URJC-1 an exceptional candidate for catalytic application in acid and base reactions of interest in fine chemistry. The URJC-1 material also displays a noteworthy thermal and chemical stability in different organic solvents of different polarity and boiling water. Its catalytic activity was evaluated in acid-catalyzed Friedel–Crafts acylation of anisole with acetyl chloride and base-catalyzed Knoevenagel condensation of benzaldehyde with malononitrile. In both cases, URJC-1 material showed very good performance, better than other metal organic frameworks and conventional catalysts. In addition, a remarkable structural stability was proven after several consecutive reaction cycles. Full article
(This article belongs to the Special Issue Coordination Polymers: New Materials for Multiple Applications)
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2714 KiB  
Article
Luminescence and Magnetic Properties of Two Three-Dimensional Terbium and Dysprosium MOFs Based on Azobenzene-4,4′-Dicarboxylic Linker
by Belén Fernández, Itziar Oyarzabal, José M. Seco, Eider San Sebastián, David Fairen-Jiménez, Santiago Gómez-Ruiz, Alfonso Salinas-Castillo, Antonio J. Calahorro and Antonio Rodríguez-Diéguez
Polymers 2016, 8(2), 39; https://doi.org/10.3390/polym8020039 - 2 Feb 2016
Cited by 10 | Viewed by 7684
Abstract
We report the in situ formation of two novel metal-organic frameworks based on terbium and dysprosium ions using azobenzene-4,4′-dicarboxylic acid (H2abd) as ligand, synthesized by soft hydrothermal routes. Both materials show isostructural three-dimensional networks with channels along a axis [...] Read more.
We report the in situ formation of two novel metal-organic frameworks based on terbium and dysprosium ions using azobenzene-4,4′-dicarboxylic acid (H2abd) as ligand, synthesized by soft hydrothermal routes. Both materials show isostructural three-dimensional networks with channels along a axis and display intense photoluminescence properties in the solid state at room temperature. Textural properties of the metal-organic frameworks (MOFs) have been fully characterized although no appreciable porosity was obtained. Magnetic properties of these materials were studied, highlighting the dysprosium material displays slightly frequency-dependent out of phase signals when measured under zero external field and under an applied field of 1000 Oe. Full article
(This article belongs to the Special Issue Coordination Polymers: New Materials for Multiple Applications)
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1634 KiB  
Article
Aerogels of 1D Coordination Polymers: From a Non-Porous Metal-Organic Crystal Structure to a Highly Porous Material
by Adrián Angulo-Ibáñez, Garikoitz Beobide, Oscar Castillo, Antonio Luque, Sonia Pérez-Yáñez and Daniel Vallejo-Sánchez
Polymers 2016, 8(1), 16; https://doi.org/10.3390/polym8010016 - 15 Jan 2016
Cited by 13 | Viewed by 11031
Abstract
The processing of an originally non-porous 1D coordination polymer as monolithic gel, xerogel and aerogel is reported as an alternative method to obtain novel metal-organic porous materials, conceptually different to conventional crystalline porous coordination polymer (PCPs) or metal-organic frameworks (MOFs). Although the work [...] Read more.
The processing of an originally non-porous 1D coordination polymer as monolithic gel, xerogel and aerogel is reported as an alternative method to obtain novel metal-organic porous materials, conceptually different to conventional crystalline porous coordination polymer (PCPs) or metal-organic frameworks (MOFs). Although the work herein reported is focused upon a particular kind of coordination polymer ([M(μ-ox)(4-apy)2]n, M: Co(II), Ni(II)), the results are of interest in the field of porous materials and of MOFs, as the employed synthetic approach implies that any coordination polymer could be processable as a mesoporous material. The polymerization conditions were fixed to obtain stiff gels at the synthesis stage. Gels were dried at ambient pressure and at supercritical conditions to render well shaped monolithic xerogels and aerogels, respectively. The monolithic shape of the synthesis product is another remarkable result, as it does not require a post-processing or the use of additives or binders. The aerogels of the 1D coordination polymers are featured by exhibiting high pore volumes and diameters ranging in the mesoporous/macroporous regions which endow to these materials the ability to deal with large-sized molecules. The aerogel monoliths present markedly low densities (0.082–0.311 g·cm−3), an aspect of interest for applications that persecute light materials. Full article
(This article belongs to the Special Issue Coordination Polymers: New Materials for Multiple Applications)
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5146 KiB  
Article
Construction of Four Zn(II) Coordination Polymers Used as Catalysts for the Photodegradation of Organic Dyes in Water
by Lei-Lei Liu, Cai-Xia Yu, Wei Zhou, Qi-Gui Zhang, Shi-Min Liu and Yun-Feng Shi
Polymers 2016, 8(1), 3; https://doi.org/10.3390/polym8010003 - 6 Jan 2016
Cited by 20 | Viewed by 7369
Abstract
Hydrothermal reactions of Zn(OAc)2·2H2O with flexible bipyridyl benzene ligand and three dicarboxylic derivatives gave rise to four new coordination polymers, [Zn7(μ4-O)2(OAc)10(bpmb)]n (1), [Zn(5-OH-1,3-BDC)(bpmb)]n (2), [Zn(1,2-BDC)(bpmb)] [...] Read more.
Hydrothermal reactions of Zn(OAc)2·2H2O with flexible bipyridyl benzene ligand and three dicarboxylic derivatives gave rise to four new coordination polymers, [Zn7(μ4-O)2(OAc)10(bpmb)]n (1), [Zn(5-OH-1,3-BDC)(bpmb)]n (2), [Zn(1,2-BDC)(bpmb)]n (3) and [Zn2(ADB)2(bpmb)]n (4) (bpmb = 1,4-bis(pyridine-3-ylmethoxy)benzene, 5-OH-1,3-H2BDC = 5-hydroxy-1,3-benzenedicarboxylic acid, 1,2-H2BDC = 1,2-benzenedicarboxylic acid, H2ADB = 2,2’-azodibenzoic acid). Their structures were characterized by single-crystal X-ray diffraction, elemental analyses, IR spectra, powder X-ray diffraction (PXRD) and thermogravimetric analyses (TGA). Compound 1 features a one-dimensional (1D) chain structure based on the rare heptanuclear [Zn7(μ4-O)(μ3-OAc)2(μ2-OAc)8] units. Compound 2 exhibits a novel 2D bilayer structure built from the two parallel 2D (4,4) layers. Compound 3 holds a 2D structure in which the 1,2-BDC ligands work as lockers interlocking 1D [Zn(bpmb)]n chain. Compound 4 comprises a 3D framework constructed by 2D wrinkled [Zn2(ADB)4]n networks and bpmb linkers with a six-connected pcu net. These results suggest that the motifs of the dicarboxylic ligands have significant effect on the final structures. These compounds exhibited relatively good photocatalytic activity towards the degradation of methylene blue (MB) in aqueous solution under a Xe lamp irradiation. Full article
(This article belongs to the Special Issue Coordination Polymers: New Materials for Multiple Applications)
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5122 KiB  
Article
Self-Assembly of 1D/2D Hybrid Nanostructures Consisting of a Cd(II) Coordination Polymer and NiAl-Layered Double Hydroxides
by Gonzalo Abellán, Pilar Amo-Ochoa, José Luis G. Fierro, Antonio Ribera, Eugenio Coronado and Félix Zamora
Polymers 2016, 8(1), 5; https://doi.org/10.3390/polym8010005 - 29 Dec 2015
Cited by 9 | Viewed by 7536
Abstract
The preparation and characterization of a novel hybrid material based on the combination of a 2D-layered double hydroxide (LDH) nanosheets and a 1D-coordination polymer (1D-CP) has been achieved through a simple mixture of suspensions of both building blocks via an exfoliation/restacking approach. The [...] Read more.
The preparation and characterization of a novel hybrid material based on the combination of a 2D-layered double hydroxide (LDH) nanosheets and a 1D-coordination polymer (1D-CP) has been achieved through a simple mixture of suspensions of both building blocks via an exfoliation/restacking approach. The hybrid material has been thoroughly characterized demonstrating that the 1D-CP moieties are intercalated as well as adsorbed on the surface of the LDH, giving rise to a layered assembly with the coexistence of the functionalities of their initial constituents. This hybrid represents the first example of the assembly of 1D/2D nanomaterials combining LDH with CP and opens the door for a plethora of different functional hybrid systems. Full article
(This article belongs to the Special Issue Coordination Polymers: New Materials for Multiple Applications)
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