Combining Ruthenium(II) Complexes with Metal–Organic Frameworks to Realize Effective Two-Photon Absorption for Singlet Oxygen Generation
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Singlet oxygen ((1)O2), as a reactive oxygen species, has garnered serious attention in physical, chemical, and biological studies. In this paper, we designed and synthesized a new type of singlet-oxygen generation system by exchanging cationic ruthenium complexes (RCs) into anionic bio-MOF-1. The resulting bio-MOF-1&RCs can be used as effective photocatalysts for generation of singlet oxygen under both single-photon and two-photon excitation. Especially, the excellent two-photon absorption (TPA) behavior of bio-MOF-1&RCs aroused our interest greatly because their two-photon absorption band lies in the optical window of biological tissue. Here, we measured the ability of bio-MOF-1&RCs to generate (1)O2 by irradiation under both 490 and 800 nm wavelength light in DMF. 1,3-Diphenylisobenzofuran (DPBF) and 2',7'-dichlorofluorescein (DCFH) were used as typical (1)O2 traps to detect and evaluate the efficiency of generation of (1)O2 under single-photon and two-photon excitation, respectively. Results indicated that bio-MOF-1&[Ru(phen)3](2+) was able to effectively generate (1)O2 under both conditions. Our work creates a novel synergistic TPA system with the excellent photophysical properties of RCs and the unique microporous structure benefit of MOFs, which may open a new avenue for creation of a cancer treatment system with both photodynamic therapy and chemotherapy.Singlet oxygen plays a major role in photodynamic inactivation of tumor cells or bacteria. Its efficacy depends critically on the oxygen concentration [O(2)], which can decrease in case oxygen is consumed caused by oxidative reactions. When detecting singlet oxygen directly by its luminescence at 1270 nm, the course of the luminescence signal is critically affected by [O(2)]. Thus, it should be feasible to monitor oxygen consumption during photo-oxidative processes. Singlet oxygen was generated by exciting a photosensitizer (TMPyP) in aqueous solution (H(2)O or D(2)O) of albumin. Chromatography shows that most of the TMPyP molecules are unbound, and therefore singlet oxygen molecules can diffuse in the solution. A sensor device for oxygen concentration revealed a rapid decrease of [O(2)] (oxygen depletion) in the solution during irradiation. The extent of oxygen depletion in aqueous albumin solution depends on the radiant exposure and the solvent. When detecting the luminescence signal of singlet oxygen, the shape of the luminescence signal significantly changed with irradiation time. Thus, local oxygen consumption could be monitored during photodynamic action by evaluating the course of singlet oxygen luminescence.
Limiting oxygen concentration
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Stable up to 523 K, the bis(dinitrogen) ruthenium and carbonyldinitrogen ruthenium complexes are formed by reaction of N2 with a carbonyl ruthenium species fixed on dealuminated Y zeolite [Eq. (a)]. A stable trans-dicarbonyldinitrogen ruthenium complex is also formed in the presence of CO at 300 K.
Molecular nitrogen
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На основе анализа обзорных РФЭ спектров образцов катализаторов 3%Ru/AlO и 3%Ru/СПС, до и после каталитического теста был установлен качественный и количественный элементный состав поверхности этих образцов. Состояния для катализатора 3%Ru/AlO до каталитического теста гидратированного рутения (IV) составил 23% и оксида рутения (IV) ± 45%, соответственно, и после ± гидратированного рутения (IV) составил 21% и оксида рутения (IV) ± 37%, соответственно. Состояния для катализатора 3%Ru/СПС до каталитического теста гидратированного рутения (IV) составил 29% и оксида рутения (IV) ± 3%, соответственно, и после ± гидратированного рутения (IV) составил 22% и оксида рутения (IV) ± 2%, соответственно. Based on the analysis of survey XPS spectra of 3%Ru/AlO and 3%Ru/HPS catalyst samples before and after the catalytic test, the qualitative and quantitative elemental composition of the surface of these samples was established. Conditions for the 3% Ru/AlO catalyst before the catalytic test of hydrated ruthenium (IV) was 23% and ruthenium (IV) oxide ± 45%, respectively, and after ± hydrated ruthenium (IV) was 21% and ruthenium (IV) oxide ± 37 %, respectively. Conditions for the catalyst 3% Ru/HPS before the catalytic test hydrated ruthenium (IV) was 29% and ruthenium (IV) oxide ± 3%, respectively, and after ± hydrated ruthenium (IV) was 22% and ruthenium (IV) oxide ± 2 %, respectively.
Ruthenium oxide
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Abstract A highly selective, sensitive, and rapid method has been developed for the spectrophotometric determination of ruthenium with 5-chloro-2-hydroxythiobenzhydrazide after extraction into molten naphthalene. Ruthenium was determined in the range 1.2–4.5 ppm. The complex was stable for more than 12 h with molar absorptivity of 1.516 × 104 L mol−1 cm−1 and detection limit of 0.0066 ppm. The method was found to be selective for ruthenium in the presence of a large number of diverse ions. Ruthenium was determined in various synthetic mixtures. The method permits the sequential separation and determination of ruthenium, osmium, and platinum from their mixtures.
Osmium
Molar absorptivity
Platinum group
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Dichloromethane
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Stable up to 523 K, the bis(dinitrogen) ruthenium and carbonyldinitrogen ruthenium complexes are formed by reaction of N2 with a carbonyl ruthenium species fixed on dealuminated Y zeolite [Eq. (a)]. A stable trans-dicarbonyldinitrogen ruthenium complex is also formed in the presence of CO at 300 K.
Molecular nitrogen
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Abstract The preparations of the title complexes (III), (V), and (VII) are described.
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The ruthenium complexes are known for their anticancer property. Some ruthenium complexes can bind with protein that may be related to the anticancer activity. The protein binding features of few ruthenium complexes have been analyzed to understand the amino acid selectivity within protein sequences. The docking, Molecular mechanics and QM/MM methods are used to predict the binding sites of these ruthenium complexes. The fluorinated ruthenium pyridocarbazole is a protein binding complex. The cis-chlorodimethylsulphoxide-S-bis(1,10-phenanthroline) ruthenium (II) chloride [RuN(B)], trichlorodimethylsulphoxide-S-(1,10-phenanthroline) ruthenium (III) [RuN(C)] and cis-dichlorotetrakis(dimethylsulphoxide) ruthenium (II) [RuN(D)] complexes can bind perfectly within fluorinated ruthenium pyridocarbazole is binding region. The complexes are found selective of certain amino acids, and the formation hydrogen bonds within the complex bonded region are found.
Docking (animal)
Ruthenium red
Phenanthroline
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