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 (364 Írán, domácí), Jan CHYBA (203 Česká republika, domácí), Michal KNOR (203 Česká republika, domácí), Michal HORNÍ (203 Česká republika, domácí), Marek NEČAS (203 Česká republika, domácí), Jan NOVOTNÝ (203 Česká republika, domácí) a Radek MAREK (203 Česká republika, garant, domácí)

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

http://dx.doi.org/10.1021/acs.inorgchem.0c01328

UT WoS

000552287100073

Klíčová slova anglicky

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

Štítky

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://dx.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 = {http://dx.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://dx.doi.org/10.1021/acs.inorgchem.0c01328.

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