Zwitterionic Ru(III) Complexes: Stability of Metal-Ligand Bond
and Host-Guest Binding with Cucurbit[7]uril

J 2020

Zwitterionic Ru(III) Complexes: Stability of Metal-Ligand Bond and Host-Guest Binding with Cucurbit[7]uril

MALALI, Sanaz; Jan CHYBA; Michal KNOR; Michal HORNÍ; Marek NEČAS et. al.

Základní údaje

Originální název

Zwitterionic Ru(III) Complexes: Stability of Metal-Ligand Bond and Host-Guest Binding with Cucurbit[7]uril

Autoři

MALALI, Sanaz; Jan CHYBA ; Michal KNOR; Michal HORNÍ; Marek NEČAS; Jan NOVOTNÝ a Radek MAREK

Vydání

Inorganic Chemistry, American Chemical Society, 2020, 0020-1669

Další údaje

Jazyk

angličtina

Typ výsledku

Článek v odborném periodiku

Obor

10400 1.4 Chemical sciences

Stát vydavatele

Spojené státy

Utajení

není předmětem státního či obchodního tajemství

Odkazy

DOI: 10.1021/acs.inorgchem.0c01328

Impakt faktor

Impact factor: 5.165

Kód RIV

RIV/00216224:14740/20:00114221

Organizační jednotka

Středoevropský technologický institut

DOI

https://doi.org/10.1021/acs.inorgchem.0c01328

UT WoS

000552287100073

EID Scopus

2-s2.0-85088047805

Klíčová slova anglicky

ruthenium(III) compound;cucurbit[7]uril;host-guest complex;NMR spectroscopy;paramagnetic;hyperfine shift;spin-dipole contribution

Štítky

14313010, 143160, CF NMR, CF SAXS, rivok

Příznaky

Mezinárodní význam, Recenzováno

Změněno: 14. 10. 2024 15:33, Ing. Marie Švancarová

Anotace

V originále

A wide range of ruthenium-based coordination compounds have been reported to possess potential as metallodrugs with anticancer or antimetastatic activity. In this work, we synthesized a set of new zwitterionic Ru(III) compounds bearing ligands derived from N-alkyl (R) systems based on pyridine, 4,4'-bipyridine, or 1,4-diazabicyclo[2.2.2]octane (DABCO). The effects of the ligand(s) and their environment on the coordination stability have been investigated. Whereas the [DABCO-R]+ ligand is shown to be easily split out of a negative [RuCl4]- core, positively charged R-pyridine and R-bipyridine ligands form somewhat more stable Ru(III) complexes and can be used as supramolecular anchors for binding with macrocycles. Therefore, supramolecular host-guest assemblies between the stable zwitterionic Ru(III) guests and the cucurbit[7]uril host were investigated and characterized in detail by using NMR spectroscopy and single-crystal X-ray diffraction. Paramagnetic 1H NMR experiments supplemented by relativistic DFT calculations of the structure and hyperfine NMR shifts were performed to determine the host-guest binding modes in solution. In contrast to the intramolecular hyperfine shifts, dominated by the through-bond Fermi-contact mechanism, supramolecular hyperfine shifts were shown to depend on the “through-space” spin-dipole contributions with structural trends being satisfactorily reproduced by a simple point-dipole approximation.

Návaznosti

GA18-05421S, projekt VaV

Název: Rozvoj paramagnetické NMR spektroskopie pro supramolekulární systémy (Akronym: SUPRAMAG)

Investor: Grantová agentura ČR, Rozvoj paramagnetické NMR spektroskopie pro supramolekulární systémy

LQ1601, projekt VaV

Název: CEITEC 2020 (Akronym: CEITEC2020)

Investor: Ministerstvo školství, mládeže a tělovýchovy ČR, CEITEC 2020

90127, velká výzkumná infrastruktura

Název: CIISB II

Citovat

MALALI, Sanaz; Jan CHYBA; Michal KNOR; Michal HORNÍ; Marek NEČAS; Jan NOVOTNÝ a Radek MAREK. Zwitterionic Ru(III) Complexes: Stability of Metal-Ligand Bond and Host-Guest Binding with Cucurbit[7]uril. Inorganic Chemistry. American Chemical Society, 2020, roč. 59, č. 14, s. 10185-10196. ISSN 0020-1669. Dostupné z: https://doi.org/10.1021/acs.inorgchem.0c01328.

@article{1669308,
   author = {Malali, Sanaz and Chyba, Jan and Knor, Michal and Horní, Michal and Nečas, Marek and Novotný, Jan and Marek, Radek},
   article_number = {14},
   doi = {https://doi.org/10.1021/acs.inorgchem.0c01328},
   keywords = {ruthenium(III) compound;cucurbit[7]uril;host-guest complex;NMR spectroscopy;paramagnetic;hyperfine shift;spin-dipole contribution},
   language = {eng},
   issn = {0020-1669},
   journal = {Inorganic Chemistry},
   title = {Zwitterionic Ru(III) Complexes: Stability of Metal-Ligand Bond and Host-Guest Binding with Cucurbit[7]uril},
   url = {http://dx.doi.org/10.1021/acs.inorgchem.0c01328},
   volume = {59},
   year = {2020}
}

TY  - JOUR
ID  - 1669308
AU  - Malali, Sanaz - Chyba, Jan - Knor, Michal - Horní, Michal - Nečas, Marek - Novotný, Jan - Marek, Radek
PY  - 2020
TI  - Zwitterionic Ru(III) Complexes: Stability of Metal-Ligand Bond and Host-Guest Binding with Cucurbit[7]uril
JF  - Inorganic Chemistry
VL  - 59
IS  - 14
SP  - 10185-10196
EP  - 10185-10196
PB  - American Chemical Society
SN  - 00201669
KW  - ruthenium(III) compound;cucurbit[7]uril;host-guest complex;NMR spectroscopy;paramagnetic;hyperfine shift;spin-dipole contribution
UR  - http://dx.doi.org/10.1021/acs.inorgchem.0c01328
L2  - http://dx.doi.org/10.1021/acs.inorgchem.0c01328
N2  - A wide range of ruthenium-based coordination compounds have been reported to possess potential as metallodrugs with anticancer or antimetastatic activity. In this work, we synthesized a set of new zwitterionic Ru(III) compounds bearing ligands derived from N-alkyl (R) systems based on pyridine, 4,4'-bipyridine, or 1,4-diazabicyclo[2.2.2]octane (DABCO). The effects of the ligand(s) and their environment on the coordination stability have been investigated. Whereas the [DABCO-R]+ ligand is shown to be easily split out of a negative [RuCl4]- core, positively charged R-pyridine and R-bipyridine ligands form somewhat more stable Ru(III) complexes and can be used as supramolecular anchors for binding with macrocycles. Therefore, supramolecular host-guest assemblies between the stable zwitterionic Ru(III) guests and the cucurbit[7]uril host were investigated and characterized in detail by using NMR spectroscopy and single-crystal X-ray diffraction. Paramagnetic 1H NMR experiments supplemented by relativistic DFT calculations of the structure and hyperfine NMR shifts were performed to determine the host-guest binding modes in solution. In contrast to the intramolecular hyperfine shifts, dominated by the through-bond Fermi-contact mechanism, supramolecular hyperfine shifts were shown to depend on the “through-space” spin-dipole contributions with structural trends being satisfactorily reproduced by a simple point-dipole approximation.
ER  -

MALALI, Sanaz; Jan CHYBA; Michal KNOR; Michal HORNÍ; Marek NEČAS; Jan NOVOTNÝ a Radek MAREK. Zwitterionic Ru(III) Complexes: Stability of Metal-Ligand Bond and Host-Guest Binding with Cucurbit[7]uril. \textit{Inorganic Chemistry}. American Chemical Society, 2020, roč.~59, č.~14, s.~10185-10196. ISSN~0020-1669. Dostupné z: https://doi.org/10.1021/acs.inorgchem.0c01328.

Přehled o publikaci