Dataset Information

Zn^II and Cu^II-Based Coordination Polymers and Metal Organic Frameworks by the of Use of 2-Pyridyl Oximes and 1,3,5-Benzenetricarboxylic Acid.

ABSTRACT: The simultaneous use of 2-pyridyl oximes (pyridine-2 amidoxime, H₂pyaox; 2-methyl pyridyl ketoxime, Hmpko) and 1,3,5-benzenetricarboxylic acid (H₃btc) provided access to five new compounds, namely [Zn(H₂btc)₂(H₂pyaox)₂]•2H₂O (1•2H₂O), [Zn(Hbtc)(H₂pyaox)₂]_n (2), [Cu(Hbtc)(H₂pyaox)]_n (3), [Cu(Hbtc)(HmpKo)]_n (4) and [Cu₂(Hbtc)₂(Hmpko)₂(H₂O)₂]•4H₂O (5•4H₂O). Among them, 3 is the first example of a metal-organic framework (MOF) containing H₂pyaox. Its framework can be described as a 3-c uninodal net of hcb topology with the layers being parallel to the (1,0,1) plane. Furthermore, 3 is the third reported MOF based on a 2-pyridyl oxime in general. 2 and 4 are new members of a small family of coordination polymers containing an oximic ligand. 1-5 form 3D networks through strong intermolecular interactions. Dc magnetic susceptibility studies were carried out in a crystalline sample of 3 and revealed the presence of weak exchange interactions between the metal centres; the experimental data were fitted to a theoretical model with the fitting parameters being J = -0.16(1) cm^-1 and g = 2.085(1). The isotropic g value was also confirmed by electronic paramagnetic resonance (EPR) spectroscopy. Reactivity studies were performed for 3 in the presence of metal ions; the reaction progress was studied and discussed for Fe(NO₃)₃ by the use of several characterization techniques, including single crystal X-ray crystallography and IR spectroscopy.

SUBMITTER: Mylonas-Margaritis I

PROVIDER: S-EPMC7831896 | biostudies-literature | 2021 Jan

REPOSITORIES: biostudies-literature

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Publications

ZnII and CuII-Based Coordination Polymers and Metal Organic Frameworks by the of Use of 2-Pyridyl Oximes and 1,3,5-Benzenetricarboxylic Acid.

Mylonas-Margaritis Ioannis I Mayans Julia J McArdle Patrick P Papatriantafyllopoulou Constantina C

Molecules (Basel, Switzerland) 20210118 2

The simultaneous use of 2-pyridyl oximes (pyridine-2 amidoxime, H2pyaox; 2-methyl pyridyl ketoxime, Hmpko) and 1,3,5-benzenetricarboxylic acid (H3btc) provided access to five new compounds, namely [Zn(H2btc)2(H2pyaox)2]•2H2O (1•2H2O), [Zn(Hbtc)(H2pyaox)2]n (2), [Cu(Hbtc)(H2pyaox)]n (3), [Cu(Hbtc)(HmpKo)]n (4) and [Cu ...[more]

PMID: 33477697

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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

Zn^II and Cu^II-Based Coordination Polymers and Metal Organic Frameworks by the of Use of 2-Pyridyl Oximes and 1,3,5-Benzenetricarboxylic Acid.

Publications

Zn<sup>II</sup> and Cu<sup>II</sup>-Based Coordination Polymers and Metal Organic Frameworks by the of Use of 2-Pyridyl Oximes and 1,3,5-Benzenetricarboxylic Acid.

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