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From 1D Coordination Polymers to Metal Organic Frameworks by the Use of 2-Pyridyl Oximes.

ABSTRACT: The synthesis and characterization of coordination polymers and metal-organic frameworks (MOFs) has attracted a significant interest over the last decades due to their fascinating physical properties, as well as their use in a wide range of technological, environmental, and biomedical applications. The initial use of 2-pyridyl oximic ligands such as pyridine-2 amidoxime (H2pyaox) and 2-methyl pyridyl ketoxime (Hmpko) in combination with 1,2,4,5-benzene tetracarboxylic acid (pyromellitic acid), H4pma, provided access to nine new compounds whose structures and properties are discussed in detail. Among them, [Zn2(pma)(H2pyaox)2(H2O)2]n (3) and [Cu4(OH)2(pma)(mpko)2]n (9) are the first MOFs based on a 2-pyridyl oxime with 9 possessing a novel 3,4,5,8-c net topology. [Zn2(pma)(H2pyaox)2]n (2), [Cu2(pma)(H2pyaox)2(DMF)2]n (6), and [Cu2(pma)(Hmpko)2(DMF)2]n (8) join a small family of coordination polymers containing an oximic ligand. 9 exhibits selectivity for FeIII ions adsorption, as was demonstrated by a variety of techniques including UV-vis, EDX, and magnetism. DC magnetic susceptibility studies in 9 revealed the presence of strong antiferromagnetic interactions between the metal centers, which lead to a diamagnetic ground state; it was also found that the magnetic properties of 9 are affected by the amount of the encapsulated Fe3+ ions, which is a very desirable property for the development of magnetism-based sensors.

SUBMITTER: Mylonas-Margaritis I

PROVIDER: S-EPMC7560365 | biostudies-literature | 2020 Sep

REPOSITORIES: biostudies-literature

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From 1D Coordination Polymers to Metal Organic Frameworks by the Use of 2-Pyridyl Oximes.

Mylonas-Margaritis Ioannis I Gérard Auban A Skordi Katerina K Mayans Julia J Tasiopoulos Anastasios A McArdle Patrick P Papatriantafyllopoulou Constantina C

Materials (Basel, Switzerland) 20200914 18

The synthesis and characterization of coordination polymers and metal-organic frameworks (MOFs) has attracted a significant interest over the last decades due to their fascinating physical properties, as well as their use in a wide range of technological, environmental, and biomedical applications. The initial use of 2-pyridyl oximic ligands such as pyridine-2 amidoxime (H<sub>2</sub>pyaox) and 2-methyl pyridyl ketoxime (Hmpko) in combination with 1,2,4,5-benzene tetracarboxylic acid (pyromellit ...[more]

PMID: 32937938

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Project description:In recent studies, porphyrin derivatives have been frequently used as building blocks for the fabrication of metal-organic coordination networks (MOCNs) on metal surfaces under ultrahigh vacuum conditions (UHV). The porphyrin core can host a variety of 3d transition metals, which are usually incorporated in solution. However, the replacement of a pre-existing metal atom in the porphyrin core by a different metallic species has been rarely reported under UHV. Herein, we studied the influence of cyanophenyl and pyridyl functional endgroups in the self-assembly of structurally different porphyrin-based MOCNs by the deposition of Fe atoms on tetracyanophenyl (Co-TCNPP) and tetrapyridyl-functionalized (Zn-TPPyP) porphyrins on Au(111) by means of scanning tunneling microscopy (STM). A comparative analysis of the influence of the cyano and pyridyl endgroups on the formation of different in-plane coordination motifs is performed. Each porphyrin derivative formed two structurally different Fe-coordinated MOCNs stabilized by three- and fourfold in-plane coordination nodes, respectively. Interestingly, the codeposited Fe atoms did not only bind to the functional endgroups but also reacted with the porphyrin core of the Zn-substituted porphyrin (Zn-TPyP), i.e., an atom exchange reaction took place in the porphyrin core where the codeposited Fe atoms replaced the Zn atoms. This was evidenced by the appearance of molecules with an enhanced (centered) STM contrast compared with the appearance of Zn-TPyP, which suggested the formation of a new molecular species, i.e., Fe-TPPyP. Furthermore, the porphyrin core of the Co-substituted porphyrin (Co-TCNPP) displayed an off-centered STM contrast after the deposition of Fe atoms, which was attributed to the binding of the Fe atoms on the top site of the Co-substituted porphyrin core. In summary, the deposition of metal atoms onto organic layers can steer the formation of structurally different MOCNs and may replace pre-existing metal atoms contained in the porphyrin core.

Dataset Information

From 1D Coordination Polymers to Metal Organic Frameworks by the Use of 2-Pyridyl Oximes.

Publications

From 1D Coordination Polymers to Metal Organic Frameworks by the Use of 2-Pyridyl Oximes.

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