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Formation of coordination polymers or discrete adducts via reactions of gadolinium(III)-copper(II) 15-metallacrown-5 complexes with polycarboxylates: synthesis, structures and magnetic properties.
Inorg Chem. 2014 Feb 03; 53(3):1320-30.IC

Abstract

Reactions of the copper(II)-gadolinium(III) 15-metallacrown-5 complex [GdCu5(Glyha)5(NO3)2(H2O)6](NO3) (Glyha(2-) = dianion of glycinehydroxamic acid) with different di/tricarboxylates (1,3-phthalate, 1,4-phthalate, biphenyl-4,4'-dicarboxylate, citrate) resulted in formation of different types of products: {[(GdCu5(Glyha)5(H2O)2)(GdCu5(Glyha)5(H2O)3)(1,3-bdc)3]·16H2O}n (1), {[(GdCu5(Glyha)5(H2O)3)2(1,4-bdc)2](1,4-bdc)·8H2O}n (2), {[(GdCu5(Glyha)5(H2O)4)2(1,4-bdc)3]·8H2O}n (3), [GdCu5(Glyha)5(Citr)(H2O)4]·7H2O (4), {[GdCu5(Glyha)5(H2O)5](μ2-CO3)[Cu(Fgg)]}·7H2O (5) and [Cu(Gly)2(H2O)]n (6) (where bdc(2-) is the corresponding phthalate (benzenedicarboxylate), Citr(3-) is citrate, Fgg(3-) is the trianion of [(N-formylaminoacetyl)amino]acetic acid and Gly(-) is glycinate). Complexes 1-5 contain the [GdCu5(Glyha)5](3+) cation. Complexes 2 and 3 possess the same composition but differ by the mode of p-phthalate coordination to the [GdCu5(Glyha)5](3+) unit. In compounds 1-3, metallacrown cations are linked by the corresponding phthalates in 1D, 1D and 2D polymers, respectively, whereas 4 and 5 are discrete molecules. Compound 5 is the product of a multistep reaction, which finally involves atmospheric CO2 capture. Hydrolysis of hydroxamate in this reaction is confirmed by isolation of a mononuclear copper glycine complex 6. The χMT vs T data for 1 were fitted using a model based on the Hamiltonian Ĥ (GdCu5) = -2J1(S1 × SGd + S2 × SGd + S3 × SGd + S4 × SGd + S5 × SGd) - 2J2(S1 × S2 + S2 × S3 + S3 × S4 + S4 × S1 + S5 × S1. The best fit corresponded to J1 = +0.60(2) cm(-1), J2 = -61.0(5) cm(-1) and zJ' = -0.035(4) cm(-1). Complex 1 is the first example of a 15-metallacrown-5 system, for which numerical values of exchange parameters have been reported. The isotherm for methanol absorption by compound 1 at 293 K was typical for microporous sorbents, whereas ethanol sorption was negligibly small.

Authors+Show Affiliations

Department of Chemistry, Taras Shevchenko National University of Kyiv , Volodymyrska Street 62, Kiev 01601, Ukraine.No affiliation info availableNo affiliation info availableNo affiliation info availableNo affiliation info available

Pub Type(s)

Journal Article

Language

eng

PubMed ID

24422476

Citation

Pavlishchuk, Anna V., et al. "Formation of Coordination Polymers or Discrete Adducts Via Reactions of gadolinium(III)-copper(II) 15-metallacrown-5 Complexes With Polycarboxylates: Synthesis, Structures and Magnetic Properties." Inorganic Chemistry, vol. 53, no. 3, 2014, pp. 1320-30.
Pavlishchuk AV, Kolotilov SV, Zeller M, et al. Formation of coordination polymers or discrete adducts via reactions of gadolinium(III)-copper(II) 15-metallacrown-5 complexes with polycarboxylates: synthesis, structures and magnetic properties. Inorg Chem. 2014;53(3):1320-30.
Pavlishchuk, A. V., Kolotilov, S. V., Zeller, M., Thompson, L. K., & Addison, A. W. (2014). Formation of coordination polymers or discrete adducts via reactions of gadolinium(III)-copper(II) 15-metallacrown-5 complexes with polycarboxylates: synthesis, structures and magnetic properties. Inorganic Chemistry, 53(3), 1320-30. https://doi.org/10.1021/ic401928m
Pavlishchuk AV, et al. Formation of Coordination Polymers or Discrete Adducts Via Reactions of gadolinium(III)-copper(II) 15-metallacrown-5 Complexes With Polycarboxylates: Synthesis, Structures and Magnetic Properties. Inorg Chem. 2014 Feb 3;53(3):1320-30. PubMed PMID: 24422476.
* Article titles in AMA citation format should be in sentence-case
TY - JOUR T1 - Formation of coordination polymers or discrete adducts via reactions of gadolinium(III)-copper(II) 15-metallacrown-5 complexes with polycarboxylates: synthesis, structures and magnetic properties. AU - Pavlishchuk,Anna V, AU - Kolotilov,Sergey V, AU - Zeller,Matthias, AU - Thompson,Laurence K, AU - Addison,Anthony W, Y1 - 2014/01/14/ PY - 2014/1/16/entrez PY - 2014/1/16/pubmed PY - 2014/1/16/medline SP - 1320 EP - 30 JF - Inorganic chemistry JO - Inorg Chem VL - 53 IS - 3 N2 - Reactions of the copper(II)-gadolinium(III) 15-metallacrown-5 complex [GdCu5(Glyha)5(NO3)2(H2O)6](NO3) (Glyha(2-) = dianion of glycinehydroxamic acid) with different di/tricarboxylates (1,3-phthalate, 1,4-phthalate, biphenyl-4,4'-dicarboxylate, citrate) resulted in formation of different types of products: {[(GdCu5(Glyha)5(H2O)2)(GdCu5(Glyha)5(H2O)3)(1,3-bdc)3]·16H2O}n (1), {[(GdCu5(Glyha)5(H2O)3)2(1,4-bdc)2](1,4-bdc)·8H2O}n (2), {[(GdCu5(Glyha)5(H2O)4)2(1,4-bdc)3]·8H2O}n (3), [GdCu5(Glyha)5(Citr)(H2O)4]·7H2O (4), {[GdCu5(Glyha)5(H2O)5](μ2-CO3)[Cu(Fgg)]}·7H2O (5) and [Cu(Gly)2(H2O)]n (6) (where bdc(2-) is the corresponding phthalate (benzenedicarboxylate), Citr(3-) is citrate, Fgg(3-) is the trianion of [(N-formylaminoacetyl)amino]acetic acid and Gly(-) is glycinate). Complexes 1-5 contain the [GdCu5(Glyha)5](3+) cation. Complexes 2 and 3 possess the same composition but differ by the mode of p-phthalate coordination to the [GdCu5(Glyha)5](3+) unit. In compounds 1-3, metallacrown cations are linked by the corresponding phthalates in 1D, 1D and 2D polymers, respectively, whereas 4 and 5 are discrete molecules. Compound 5 is the product of a multistep reaction, which finally involves atmospheric CO2 capture. Hydrolysis of hydroxamate in this reaction is confirmed by isolation of a mononuclear copper glycine complex 6. The χMT vs T data for 1 were fitted using a model based on the Hamiltonian Ĥ (GdCu5) = -2J1(S1 × SGd + S2 × SGd + S3 × SGd + S4 × SGd + S5 × SGd) - 2J2(S1 × S2 + S2 × S3 + S3 × S4 + S4 × S1 + S5 × S1. The best fit corresponded to J1 = +0.60(2) cm(-1), J2 = -61.0(5) cm(-1) and zJ' = -0.035(4) cm(-1). Complex 1 is the first example of a 15-metallacrown-5 system, for which numerical values of exchange parameters have been reported. The isotherm for methanol absorption by compound 1 at 293 K was typical for microporous sorbents, whereas ethanol sorption was negligibly small. SN - 1520-510X UR - https://www.unboundmedicine.com/medline/citation/24422476/Formation_of_coordination_polymers_or_discrete_adducts_via_reactions_of_gadolinium_III__copper_II__15_metallacrown_5_complexes_with_polycarboxylates:_synthesis_structures_and_magnetic_properties_ L2 - https://dx.doi.org/10.1021/ic401928m DB - PRIME DP - Unbound Medicine ER -
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