NDLI: Can self-assembly of copper(II) picolinamide building blocks be controlled?

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Can self-assembly of copper(II) picolinamide building blocks be controlled?

Content Provider	Semantic Scholar
Author	Đaković, Marijana Vila-Viçosa, Diogo Bandeira, Nuno A. G. Calhorda, Maria José Kozlevčar, Bojan Jagličič, Zvonko Popović, Zora
Copyright Year	2013
Abstract	Four copper(II) derivatives with picolinamide (piaH), [Cu(N3)2(piaH)2] (1), [Cu(NCO)2(piaH)2] (2), [Cu(pia)2]·2H2O (3) and [Cu(pia)(piaH)(ClO4)]2 (4) are reported. 1 and 2 were isolated as powders shortly after precipitation, becoming crystalline (3) after prolonged standing in mother liquor. The single crystal X-ray analysis revealed the deprotonation of the amide nitrogen (pia) in both 3 (mononuclear square planar [Cu(pia-N,N)2] building blocks) and 4 (pia acting as a bridge between copper(II) ions within the dimer). MAGSUS χMT versus T curves suggest only weak magnetic interactions between the copper(II) species in 3 and 4, though 4 is dinuclear. The magnetic coupling was reproduced by DFT calculations on the experimentally determined structures. The mechanism of formation of compounds 3 and 4 was analyzed by DFT calculations. Models of 1 and 2 underwent transfer of two hydrogen atoms from the piaH ligands to the two axial ligands N3− or NCO− that were released yielding 3. In the reaction leading to 4, the perchlorate is a very weak base that cannot deprotonate the piaH ligand and after the first hydrogen transfer to acetate the dimer 4 is formed. This reactivity, favoring alternative pathways, may switch off an expected self-assembly process.
Starting Page	8074
Ending Page	8087
Page Count	14
File Format	PDF HTM / HTML
DOI	10.1039/C3CE41011K
Volume Number	15
Alternate Webpage(s)	http://www.rsc.org/suppdata/ce/c3/c3ce41011k/c3ce41011k.pdf
Alternate Webpage(s)	https://doi.org/10.1039/C3CE41011K
Language	English
Access Restriction	Open
Content Type	Text
Resource Type	Article

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