Role of N-Donor Sterics on the Coordination Environment and Dimensionality of Uranyl Thiophenedicarboxylate Coordination Polymers

Thangavelu, Sonia G.; Butcher, Ray J.; Cahill, Christopher L.

doi:10.1021/acs.cgd.5b00549

Role of N-Donor Sterics on the Coordination Environment and Dimensionality of Uranyl Thiophenedicarboxylate Coordination Polymers

Journal Article · Fri May 29 00:00:00 EDT 2015 · Crystal Growth and Design

DOI:https://doi.org/10.1021/acs.cgd.5b00549· OSTI ID:1370892

Thangavelu, Sonia G. ^[1]; Butcher, Ray J. ^[2]; Cahill, Christopher L. ^[1]

The George Washington Univ., Washington D.C. (United States)
Howard Univ., Washington D.C. (United States)

Thiophene 2,5-dicarboxylic acid (TDC) was reacted with uranyl acetate dihydrate and one (or none) of six N-donor chelating ligands (2,2'-bipyridine (BPY), 4,4'-dimethyl-2,2'-bipyridine (4-MeBPY), 5,5'-dimethyl-2,2'-bipyridine (5-MeBPY), 6,6'-dimethyl-2,2'-bipyridine (6-MeBPY), 4,4',6,6'-tetramethyl-2,2'-bipyridine (4,6-MeBPY), and tetrakis(2-pyridyl)pyrazine (TPPZ) to result in the crystallization of seven uranyl coordination polymers, which were characterized by their crystal structures and luminescence properties. The seven coordination polymers, Na₂[(UO₂)₂(C₆H₂O₄S)₃]·₄H₂O (1), [(UO₂)₄(C₆H₂O₄S)₅(C₁₀H₈N₂)₂]·C₁₀H₁₀N₂·3H₂O (2), [(UO₂)(C₆H₂O₄S)(C₁₂H₁₂N₃)] (3), [(UO₂)(C₆H₂O₄S)(C₁₂H₁₂N₃)]·H₂O (4), [(UO₂)₂(C₆H₂O₄S)₃]·(C₁₂H₁₄N₂)·5H₂O (5), [(UO₂)₃(CH₃CO₂)(C₆H₂O₄S)₄](C₁₄H₁₇N₂)₃·(C₁₄H₁₆N₂)·H₂O (6), and [(UO₂)₂(C₆H₂O₄S)₃](C₂₄H₁₈N₆) (7), consist of either uranyl hexagonal bipyramidal or pentagonal bipyramidal coordination geometries. In all structures, structural variations in the local and global structures of 1–7 are influenced by the positions (or number) of methyl groups or pyridyl rings on the N-donor species, thus resulting in a wide diversity of structures ranging from single chains, double chains, or 2-D sheets. Direct coordination of N-donor ligands to uranyl centers is observed in the chain structures of 2–4 using BPY, 4-MeBPY, and 5-MeBPY, whereas the N-donor species participate as guests (as either neutral or charge balancing species) in the chain and sheet structures of 5–7 using 6-MeBPY, 4,6-MeBPY, and TPPZ, respectively. Compound 1 is the only structure that does not contain any N-donor ligands and thus crystallizes as a 2-D interpenetrating sheet. The luminescent properties of 1–7 are influenced by the direct coordination or noncoordination of N-donor species to uranyl centers. Compounds 2–4 exhibit typical UO₂²⁺ emission upon direct coordination of N-donors, but its absence is observed in 1, 5, 6, and 7, when N-donor species participate as guest molecules. These results suggest that direct coordination of N-donor ligands participate as chromophores, thus resulting in possible UO₂²⁺ sensitization. Finally, the lack of emission in 1, 5, 6, and 7 may be explained by the extended conjugation of the TDC ligands within their structures.

View Accepted Manuscript (DOE)

Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Materials Science of Actinides (MSA)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: SC0001089

OSTI ID:: 1370892

Journal Information:: Crystal Growth and Design, Journal Name: Crystal Growth and Design Journal Issue: 7 Vol. 15; ISSN 1528-7483

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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In situ formed [M(CN) 9 ] (M = W, Mo) as a building block for the construction of two nona-cyanometalate-bridged heterometallic coordination polymers Qian, Jun; Yoshikawa, Hirofumi; Humphrey, Mark G. CrystEngComm, Vol. 21, Issue 29 https://doi.org/10.1039/c9ce00579j	journal	January 2019
Crystal structure and fluorescence properties of catena -poly[[(2,2′-bi-1 H -imidazole-κ ² N , N ′)cadmium]-di-μ-chlorido] Liu, Yang; Liu, Hai-Hui Acta Crystallographica Section E Crystallographic Communications, Vol. 72, Issue 10 https://doi.org/10.1107/s2056989016013736	journal	September 2016

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