Organic Letters, Год журнала: 2023, Номер 25(24), С. 4576 - 4580
Опубликована: Июнь 8, 2023
We report, herein, a photoinduced iron-catalyzed direct chlorination of aromatic sulfonyl chloride at room temperature. In this protocol, FeCl3-catalyzed has been realized temperature under the irradiation light (400–410 nm). During process, many commercially or readily available substituted chlorides could produce corresponding in moderate to good yields.
Язык: Английский
Organic Chemistry Frontiers, Год журнала: 2024, Номер 11(14), С. 4024 - 4040
Опубликована: Янв. 1, 2024
This review provides a comprehensive overview of metal catalysis in photo-electrochemical systems, discussing reaction mechanisms and offering prospects for this triadic catalytic mode.
Язык: Английский
Процитировано
13
Environmental Science & Technology, Год журнала: 2023, Номер 57(49), С. 20915 - 20928
Опубликована: Ноя. 28, 2023
Mixed metal oxide (MMO) anodes are commonly used for electrochlorination of ammonium (NH4+) in wastewater treatment, but they suffer from low efficiency due to inadequate chlorine generation at Cl– concentrations and sluggish reaction kinetics between free NH4+ under acidic pH conditions. To address this challenge, we develop a straightforward wet chemistry approach synthesize BiOCl-functionalized MMO electrodes using the as an efficient Ohmic contact electron transfer. Our study demonstrates that BiOCl@MMO anode outperforms pristine anode, exhibiting higher (24.6–60.0 mg Cl2 L–1), increased Faradaic (75.5 vs 31.0%), improved rate constant oxidation (2.41 0.76 L–1 min–1) 50 mM concentration. Characterization techniques including paramagnetic resonance situ transient absorption spectra confirm production radicals (Cl• Cl2•–) by BiOCl/MMO anode. Laser flash photolysis reveals significantly apparent second-order constants ((4.3–4.9) × 106 M–1 s–1 2.0–4.0) Cl•, compared undetectable Cl2•–, well slower (102 < 4.0) within same range, emphasizing significance Cl• enhancing oxidation. Mechanistic studies provide compelling evidence capacity BiOCl adsorption, facilitating evolution generation. Importantly, exhibits excellent long-term stability high catalytic activity NH4+-N removal real landfill leachate. These findings offer valuable insights into rational design improve electrocatalytic abatement, which holds great promise treatment applications.
Язык: Английский
Процитировано
19
ACS Catalysis, Год журнала: 2025, Номер 15(3), С. 2212 - 2221
Опубликована: Янв. 23, 2025
Despite recent advances in enantioselective radical coupling with strained cyclic rings, asymmetric reactions triggered by unstrained motifs remain rare. Herein, we report a mild and general strategy for activating diverse set of readily available alcohols the remote site-specific allylic alkylation ketones through combination photoredox-mediated proton-coupled electron transfer chiral chromium catalysis. This newly developed dual catalytic system exhibits extensive applicability, operates under conditions, offers straightforward operation, demonstrates tolerance to functional groups. The open-shell has also been applied late-stage modification complex drug natural product derivatives high levels enantioselectivity.
Язык: Английский
Процитировано
1
Advanced Synthesis & Catalysis, Год журнала: 2024, Номер 366(7), С. 1595 - 1605
Опубликована: Фев. 3, 2024
Abstract Herein, we present a photoinduced deconstructive alkoxyamination of alkyl alcohols catalyzed by iron salts. This transformation involves the initiation alkoxy radicals through chlorine radical‐induced radical formation, followed β ‐scission and trapping resulting carbon with 2,2,6,6‐tetramethylpiperidin‐1‐yl (TEMPO). reaction exhibits broad substrate scope (40 examples), including primary secondary that are prone to oxidation combination TEMPO iron. Mechanistic investigations have revealed enhanced coordination chloride ion center inhibits OH process, thereby enabling tolerance alcohols.
Язык: Английский
Процитировано
6
Journal of Chemical Information and Modeling, Год журнала: 2025, Номер unknown
Опубликована: Фев. 6, 2025
The mechanisms for the C(sp3)-H activation and addition reactions between acetonitrile (or acetone) alkynes have been investigated with M06-2X-D3/ma-def2-TZVP method basis set. SMD (solvation model based on solute electron density) was applied to simulate solvent effect. In first second reactions, 2-phenylbut-3-yn-2-ol reacted acetone, respectively. First, activations of acetone could be achieved by PhCOO• t-BuO• radicals. Then, converted into final products P1 P2. Gibbs free energy surfaces these two suggest that blue lines would favorable paths lower barriers, terminal C atom C≡C bond is best reactive site. Moreover, analysis IRI (Interaction Region Indicator) reveals Z- E-configuration transformations. While in third fourth methyl(2-(phenylethynyl)phenyl)sulfane has interactions via some paths, profiles show C10 atom, rather than C11 priority, are favorable. Furthermore, action mode Na2HPO4 reduce barrier benefit reaction. vdW (van der Waals) play an important role choice fifth sixth) reaction, it happened 1-(2-(methylthio)phenyl)-3-phenylprop-2-yn-1-one acetontrile yield product P5 P6). computational results uncovered line path, site depends interactions, which origin selectivity. addition, investigation byproducts carried out, can explain reason only main produced. Both those agree experimental results. localized orbital locator (LOL) isosurfaces, Laplacian order (LBO), density critical point (ρBCP), spin isosurface graphs, graphs used analyze structure reveal reaction substances.
Язык: Английский
Процитировано
0
Chemical Engineering Journal, Год журнала: 2023, Номер 481, С. 148353 - 148353
Опубликована: Дек. 25, 2023
Язык: Английский
Процитировано
5
Advanced Synthesis & Catalysis, Год журнала: 2023, Номер 365(15), С. 2524 - 2529
Опубликована: Июль 3, 2023
Abstract We present here an iron‐catalyzed oxidative C sp 3 −C bond cleavage of unstrained tertiary alkyl aromatics to provide a range synthetically useful arylketones even with H 2 O as the oxidant. This method is operationally simple, scalable, and eco‐friendly, well suitable for late‐stage oxidation complex molecules bearing hydroxy groups, making it valuable tool in organic synthesis.
Язык: Английский
Процитировано
3
Chinese Chemical Letters, Год журнала: 2023, Номер 35(1), С. 108835 - 108835
Опубликована: Июль 29, 2023
Язык: Английский
Процитировано
3
Organic Letters, Год журнала: 2023, Номер 25(24), С. 4576 - 4580
Опубликована: Июнь 8, 2023
We report, herein, a photoinduced iron-catalyzed direct chlorination of aromatic sulfonyl chloride at room temperature. In this protocol, FeCl3-catalyzed has been realized temperature under the irradiation light (400–410 nm). During process, many commercially or readily available substituted chlorides could produce corresponding in moderate to good yields.
Язык: Английский
Процитировано
2