Dalton Transactions, Год журнала: 2024, Номер unknown
Опубликована: Янв. 1, 2024
Starting from ClSbR
Язык: Английский
Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(31)
Опубликована: Май 11, 2024
The use of noncovalent interactions based on electrophilic halogen, chalcogen, pnictogen, or tetrel centers in organocatalysis has gained noticeable attention. Herein, we provide an overview the most important developments last years with a clear focus experimental studies and catalysts which act via such non-transient interactions.
Язык: Английский
Процитировано
28
Journal of the American Chemical Society, Год журнала: 2023, Номер 145(50), С. 27167 - 27184
Опубликована: Дек. 8, 2023
Nature embeds some of its molecular machinery, including ion pumps, within lipid bilayer membranes. This has inspired chemists to attempt develop synthetic analogues exploit membrane confinement and transmembrane potential gradients, much like their biological cousins. In this perspective, we outline the various strategies by which machines─molecular systems in a nanomechanical motion is exploited for function─have been designed be incorporated membranes utilized mediate transport. We survey machines spanning both switches motors, those that act as mobile carriers or are anchored membrane, mechanically interlocked molecules, examples activated response external stimuli.
Язык: Английский
Процитировано
24
Chemical Science, Год журнала: 2024, Номер 15(37), С. 15006 - 15022
Опубликована: Янв. 1, 2024
Synthetic anion receptors based on sigma-hole interactions are increasingly used to transport anions across membranes. This article discusses the progress in field and prospects for biological applications.
Язык: Английский
Процитировано
9
Journal of the American Chemical Society, Год журнала: 2024, Номер 146(11), С. 7146 - 7151
Опубликована: Март 11, 2024
Our growing interest in the design of pnictogen-based strategies for anion transport has prompted an investigation into properties three simple triarylcatecholatostiboranes (1–3) general formula (o-C6Cl4O2)SbAr3 with Ar = Ph (1), o-tolyl (2), and o-xylyl (3) complexation hydroxide across phospholipid bilayers. A modified hydroxypyrene-1,3,6-trisulfonic acid (HPTS) assay carried out artificial liposomes shows that 1 2 are potent transporters while 3 is inactive. These results indicate steric hindrance imposed by groups prevents access to antimony center. Supporting this interpretation, quickly react TBAOH·30 H2O ([TBA]+ [nBu4N]+) form corresponding hydroxoantimonate salts [nBu4N][1-OH] [nBu4N][2-OH], whereas resists coordination remains unperturbed. Moreover, activities correlated +V oxidation state atom as parent trivalent stibines show no activity.
Язык: Английский
Процитировано
6
Inorganic Chemistry, Год журнала: 2024, Номер 63(32), С. 14943 - 14957
Опубликована: Июль 27, 2024
Cocrystallizations of
Язык: Английский
Процитировано
6
Chemical Communications, Год журнала: 2023, Номер 60(2), С. 192 - 195
Опубликована: Ноя. 16, 2023
The search for alternative gold catalyst activators has led us to consider the design of platforms in which a phosphine chloride moiety could be activated via formation pnictogen bond with neighboring antimony unit. Here, we describe that such system can accessed from 4-(diphenylphosphino)-5-(diphenylstibino)-2,7-di-tert-butyl-9,9-dimethylxanthene, by oxidation stibine 3,5-di-tert-butyl-o-benzoquinone and coordination an AuCl unit phosphine. This strategy affords complex Lewis acidic or pnictogen-bond donor catecholatostiborane flanks adjacent moiety. impacts catalytic reactivity center, as reflected ability this catalyze propargyl amide cyclization reactions. Comparisons phosphinostiborane ferrocene analog computations point intramolecular Au-Cl → Sb(V) interaction responsible observed activity.
Язык: Английский
Процитировано
10
Helvetica Chimica Acta, Год журнала: 2024, Номер 107(5)
Опубликована: Март 6, 2024
Abstract It is often said that pnictogen‐bonding catalysis, and σ ‐hole catalysis in general, would not work aqueous systems because the solvent interfere as an overcompetitive pnictogen‐bond acceptor. In this study, we show transfer of from hydrophobic solvents to possible by replacing only with hydrophilic substrates, without changing catalyst or reaction. This differs conventional covalent Lewis acid catalysts, which are instantaneously destroyed ligand exchange. With their water‐proof substituents place exchangeable ligands, supramolecular counterpart evinced catalyze hydrogenation quinolines neutral systems. To secure these results, introduce a water‐soluble fluorogenic substrate releases coumarin upon reduction instead activated quinolidiniums, stiborane catalysts deepened holes. They demonstrate can operate higher‐order architectures for under biologically relevant conditions, provide operational assay high‐throughput screening fluorescence imaging, situ conditions.
Язык: Английский
Процитировано
4
Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(45)
Опубликована: Июль 5, 2024
Abstract The objective of this study was to create artificial enzymes that capitalize on pnictogen bonding, a σ‐hole interaction is essentially absent in biocatalysis. For purpose, stibine catalysts were equipped with biotin derivative and combined streptavidin mutants identify an efficient transfer hydrogenation catalyst for the reduction fluorogenic quinoline substrate. Increased catalytic activity from wild‐type best coincides depth σ hole Sb(V) center, emergence saturation kinetic behavior. Michaelis–Menten analysis reveals transition‐state recognition low micromolar range, more than three orders magnitude stronger millimolar substrate recognition. Carboxylates preferred by contribute hydrogen‐bonded ion pairing anion‐π interactions emerging pyridinium product. challenging stereoselectivity aqueous systems further emphasizes compatibility bonding higher order catalysis.
Язык: Английский
Процитировано
4
Dalton Transactions, Год журнала: 2024, Номер 53(20), С. 8524 - 8534
Опубликована: Янв. 1, 2024
The synthetic strategies employed to isolate monomeric stibinidene chalcogenides (RSbCh) and stibine (R 3 SbCh) are discussed, a perspective on the outcomes future directions of this exciting area is provided.
Язык: Английский
Процитировано
3
Organometallics, Год журнала: 2024, Номер 43(11), С. 1246 - 1255
Опубликована: Май 29, 2024
With an interest in chalcogen bonding, we use a rigid indazolium backbone to install formally zero-valent Se center next divalent Te center, allowing us investigate the effects of oxidation on observed Te···Se interaction. Through spectroscopic and computational comparison Se(0) species with its Se(II) counterpart their monochalcogen analogues, experimentally computationally effect modulating basicity resulting Comparison well-studied naphthalene acenaphthene variants indicates that increased allows for comparably strong interaction despite longer peri distances larger splay angle. Finally, our study illuminates potential non-innocence cationic organic substituents chalcogen-bonding catalysis transfer hydrogenation quinolines.
Язык: Английский
Процитировано
3