Micellar Transfer Hydrogenation Catalysis in Water with Monocarbonyl Ruthenium(II)-poly(vinylphosphonate)-Containing Polymers: Achieving Reduction of Biomass-Derived Aldehydes DOI Creative Commons
Denise Lovison,

Philipp Weingarten,

Alexandra Sebeschuk

и другие.

ACS Applied Polymer Materials, Год журнала: 2024, Номер 6(22), С. 13855 - 13864

Опубликована: Ноя. 7, 2024

With the aim to build a supramolecular organometallic catalyst for transfer hydrogenation (TH) reactions of hydrophobic substrates, micellar architectures different sizes were obtained using amphiphilic diblock copolymers (BCPs) tethered Ru(II) monocarbonyl complex. An end-group functionalization strategy was employed incorporate bipyridyl end-group, used further coordinate cationic ruthenium fragment, poly(2-vinylpyridine)-b-poly(diethyl vinylphosphonate). Owing their character, polymers form spherical micelles in water, which characterized by spectroscopic and analytical methods at pH values temperatures. The most suitable core–shell system could level catalytic activity complex toward biomass-derived aldehydes, be successfully reduced corresponding alcohols water potassium formate as hydride source. Depending on substrate's hydrophobicity concentration, varied significantly. In addition, polymer's properties hardly changed during catalysis, facilitating effective recycling until third cycle.

Язык: Английский

Metals in Cancer Research: Beyond Platinum Metallodrugs DOI Creative Commons
Angela Casini, Alexander Pöthig

ACS Central Science, Год журнала: 2024, Номер 10(2), С. 242 - 250

Опубликована: Фев. 7, 2024

The discovery of the medicinal properties platinum complexes has fueled design and synthesis new anticancer metallodrugs endowed with unique modes action (MoA). Among various families experimental antiproliferative agents, organometallics have emerged as ideal platforms to control compounds' reactivity stability in a physiological environment. This is advantageous efficiently deliver novel prodrug activation strategies, well acting only via noncovalent interactions their pharmacological targets. Noteworthy, another justification for advance organometallic compounds therapy stems from ability catalyze bioorthogonal reactions cancer cells. When not yet drug leads, such can be used selective chemical tools that benefit advantages catalytic amplification either label target interest (e.g., proteins) or boost output biochemical signals. Examples so-called "catalysis cells" are considered this Outlook together other candidates. selected case studies discussed frame more general challenges field inorganic chemistry.

Язык: Английский

Процитировано

42
Synergy Between Metal and Molecular Catalysts for (Photo)electrocatalytic 1,4-NADH Regeneration DOI
Fengyuan Liu, Wenwen Shi,

Shujie Tian

и другие.

The Journal of Physical Chemistry C, Год журнала: 2024, Номер 128(14), С. 5927 - 5933

Опубликована: Апрель 2, 2024

(Photo)electrocatalytic NAD+ reduction provides a promising approach for 1,4-NADH regeneration, but it remains challenging to achieve both high activity and selectivity. Here, we found prominent synergetic effects between various metals (Cu, Fe, Co, Ni) Rh-based complexes (M M') electrocatalytic reduction, promoting the selectivity simultaneously. Typically, normalized of Cu M coupled system is 15.6 times that M, while alone shows negligible at same potential. Meanwhile, enhanced from 63.3% as 95.3% system. We transfer hydrogen atoms metal electrode complex accelerates formation metal-hydride active species, which catalyzes regioselective production 1,4-NADH. This work universal strategy coupling proton-reduction electrocatalysts molecular catalysts efficient (photo)electrocatalytic 1,4-NAD(P)H regeneration.

Язык: Английский

Процитировано

7
Electrochemical NADH Regeneration Mediated by Pyridine Amidate Iridium Complexes Interconverting 1,4- and 1,6-NADH DOI
Caterina Trotta, Gabriel Menendez Rodriguez, Cristiano Zuccaccia

и другие.

ACS Catalysis, Год журнала: 2024, Номер 14(13), С. 10334 - 10343

Опубликована: Июнь 25, 2024

Although there is a huge interest in redox mediators for the selective electrochemical regeneration of 1,4-NADH, only class rhodium compounds with bipyridine ligands, initially introduced by pioneering work Wienkamp and Steckhan (Wienkamp, R.; Steckhan, E. Angew. Chem. Int. Ed. Engl. 1982, 21, 782−783, 10.1002/anie.198207822), has been developed over last few decades. Here we report first two progenitors indirect NADH regeneration, namely [Cp*Ir(R′-pica)Cl] {pica = R′-picolinamidate κ2-R′-pyridine-2-carboxamide ion (−1), 1 R′ H 2 Me}, which exhibit high TOF values (0.51 1.34 s–1 2, respectively), production rate up to 3 μmol h–1 cm–2, faradaic efficiency 99% both complexes 0.1 M phosphate buffer (pH 7, 298 K). The reaction exclusively leads mixture desired product, 1,6-NADH always 91:9 molar ratio, independently mediator, degree conversion, applied potential. 1H EXSY NMR unequivocally shows that rapid equilibrium establishes between 1,4-NADH (Keq 10.1, ΔG0 −1.4 kcal mol–1, K), presence suggesting latter are capable rapidly interconverting regioisomers NADH, thus allowing utilization totality regenerated NADH.

Язык: Английский

Процитировано

6
Designing biomimetic catalytic systems for CO2 reduction to formate using NAD(P)H DOI
Chan-Woo Park,

Chul Han Kwon,

Young Hyun Hong

и другие.

Inorganic Chemistry Frontiers, Год журнала: 2025, Номер unknown

Опубликована: Янв. 1, 2025

This review article focuses on current achievements and identifies future research directions by designing biomimetic catalytic systems for CO 2 reduction to formate using NAD(P)H.

Язык: Английский

Процитировано

0
Organometallic Catalysis Catches up with Enzymatic in the Regeneration of NADH DOI Creative Commons
Caterina Trotta,

G. Fraschini,

Elena Tacchi

и другие.

ACS Catalysis, Год журнала: 2025, Номер unknown, С. 9417 - 9429

Опубликована: Май 19, 2025

Язык: Английский

Процитировано

0
Integrin-Specific Stimuli-Responsive Nanomaterials for Cancer Theranostics DOI Creative Commons
Zahra Taheri, Negin Mozafari,

Ghazal Moradian

и другие.

Pharmaceutics, Год журнала: 2024, Номер 16(11), С. 1441 - 1441

Опубликована: Ноя. 11, 2024

: Cancer is one of the leading causes death worldwide. The tumor microenvironment makes difficult to treat, favoring drug resistance and formation metastases, resulting in death.

Язык: Английский

Процитировано

1
Ir(III) Diamine Transfer Hydrogenation Catalysts in Cancer Cells DOI Creative Commons

M. Fry,

Sitah A. Alsaif,

Yasmin Khanom

и другие.

ChemCatChem, Год журнала: 2024, Номер unknown

Опубликована: Окт. 7, 2024

Abstract The development of catalytic metallodrugs is an emerging field that may offer new approaches to cancer chemotherapeutic design. By exploiting the unique properties transition metal complexes, in‐cell catalysis can be applied modulate cellular redox balance as part a multi‐targeting mechanism action. We describe synthesis and characterization six coordinatively unsaturated iridium(III) diamine catalysts are stable at physiological pH in aqueous solution. Reduction colorimetric substrate 2,6‐dichlorophenolindophenol by transfer hydrogenation under biologically compatible conditions achieved turnover frequencies up 63 ± 2 h −1 demonstrated source hydride (sodium formate) limiting reagent, despite being 1000‐fold excess catalyst. catalyst showed low vivo acute toxicity zebrafish embryos modest vitro potency towards cells. When administered alone, generated oxidative stress cells (an effect was conserved vivo), but co‐treatment with nontoxic dose sodium formate negated this effect. Co‐treatment significantly enhanced (A2780 ovarian MCF7 breast cells) drug‐resistant (A2780cis MCF7‐TAMR1) not non‐tumorigenic (MRC5), demonstrating redox‐targeting generate selectivity for

Язык: Английский

Процитировано

0
Electrochemistry of ruthenium solid-state surface: fabrication and application DOI Creative Commons

Mohammed M. Al Hinaai,

Rayya A. Al-Balushi

Electrochemistry, Год журнала: 2024, Номер unknown, С. 136 - 173

Опубликована: Ноя. 27, 2024

The requirement for energy, stokehole chemicals, quality controls, monitoring public health, and environmental pollution encouraged the investigation rate to develop compounds with distinctive properties special applications. Researchers have proven that ruthenium (Ru) solid-state substances possess potential characteristics such as conductivity, stability, catalytic activity, ability integrate many other compounds. Intensive research has led progression of novel technologies, these nanomaterials demonstrated their enormous in various industries, especially field chemical industrial catalysts. Ru surfaces demonstrate high effectiveness efficiency catalyzing large numbers reactions. recent trend involves nanoparticles, graphene, gold, bimetallic alloys. critical enhancements were stability improving active site numbers. based electronic devices capacitors show excellent performance terms current density charge/discharge recycling ability. Also, most progress Ru-complexes base electromigrated chemiluminescent sensor unlimited its analytical gradually, researchers enabled creation surface sensors an number analytes. In this chapter, electrochemistry applications attractive fields are explored, is synthesis properties.

Язык: Английский

Процитировано

0
Cyclometalated and NNN Terpyridine Ruthenium Photocatalysts and Their Cytotoxic Activity DOI Creative Commons
Maurizio Ballico, Dario Alessi, Eleonora Aneggi

и другие.

Molecules, Год журнала: 2024, Номер 29(9), С. 2146 - 2146

Опубликована: Май 5, 2024

The cyclometalated terpyridine complexes [Ru(η2-OAc)(NC-tpy)(PP)] (PP = dppb 1, (R,R)-Skewphos 4, (S,S)-Skewphos 5) are easily obtained from the acetate derivatives [Ru(η2-OAc)2(PP)] dppb, 2, 3) and tpy in methanol by elimination of AcOH. precursors 3 prepared [Ru(η2-OAc)2(PPh3)2] Skewphos cyclohexane. Conversely, NNN [Ru(η1-OAc)(NNN-tpy)(PP)]OAc 6, 7) synthesized a one pot reaction [Ru(η2-OAc)2(PPh3)2], PP methanol. neutral NC-tpy 5 cationic NNN-tpy 7 catalyze transfer hydrogenation acetophenone (S/C 1000) 2-propanol with NaOiPr under light irradiation at 30 °C. Formation (S)-1-phenylethanol has been observed 6 MeOH/iPrOH mixture, whereas R-enantiomer is 5, (50–52% ee). show cytotoxic activity against anaplastic thyroid cancer 8505C SW1736 cell lines (ED50 0.31–8.53 µM), displaying an ED50 0.31 µM, four times lower compared to enantiomer 6.

Язык: Английский

Процитировано

0
Light-enhancing ketone transfer hydrogenation catalyzed by diphosphine phenanthroline ruthenium complexes DOI
Gustavo Henrique Cicero Masson, Maurizio Ballico, Beatriz E. Goi

и другие.

Molecular Catalysis, Год журнала: 2024, Номер 564, С. 114337 - 114337

Опубликована: Июнь 27, 2024

Язык: Английский

Процитировано

0