Refining the Distinct Cu–N₄ Coordination in Mesoporous N-Doped Carbon to Boost Selective Deuteration under Mild Conditions

ACS Applied Materials & Interfaces, Год журнала: 2025, Номер unknown

Опубликована: Янв. 17, 2025

Deuterated compounds have broad applications across various fields, with dehalogenative deuteration serving as an efficient method to obtain these molecules. However, the diverse electronic structures of active sites in heterogeneous system and limited recyclability homogeneous significantly hinder advancement deuteration. In this study, we present a catalyst composed copper single-atom anchored within ordered mesoporous nitrogen-doped carbon matrix, synthesized via mesopore confinement method. The Cu1/OMNC-1100 catalyst, characterized by Cu-N4 sites, demonstrates exceptional performance, high functional group tolerance, remarkable durability 2-bromo-6-methoxynaphthalene under relatively mild conditions (80 °C, 2 MPa CO). Experimental results combined X-ray absorption fine structure analysis reveal that Cu-N3 can be converted into more stable counterparts at higher pyrolysis temperatures, resulting enhanced catalytic activity. This work strategy for designing site catalysts tunable coordination environments, providing promising approach improving performance selective reactions conditions.

Язык: Английский

Metal‐free, Selective Ortho‐Deuteration of N‐heterocyclic Oxides

Advanced Synthesis & Catalysis, Год журнала: 2025, Номер unknown

Опубликована: Фев. 1, 2025

Abstract Replacing hydrogen with deuterium raises the activation energy for C−D bond cleavage. This approach has gained attention in drug design, especially to protect ortho ‐position of pyridines, which are susceptible enzymatic oxidation. Until now, direct isotope exchange been largely restricted use reactive organolithium reagents or metal‐catalysed deuteration methods. In this work, we present a metal‐free, selective ‐deuteration N ‐heterocycles starting from their ‐oxides, proceeding at room temperature just 5 minutes. method achieves high incorporation across broad range ‐heterocycles, including bioactive compounds. Experimental and computational studies have elucidated mechanism reaction, showing that regioselectivity is driven by successful increase acidity ‐position, enabling deprotonation in‐situ generated dimsyl anion.

Язык: Английский

Base-driven dehydrohalogenation coupled with catalytic hydrodehalogenation as a novel strategy for rapid dehalogenation of halogenated organic compounds containing aliphatic C-X bonds

Journal of environmental chemical engineering, Год журнала: 2024, Номер 12(6), С. 114983 - 114983

Опубликована: Ноя. 29, 2024

Язык: Английский