Ion incorporation into Cobalt(II)-organic framework for green and efficient synthesis of oxazolidinones via carbon dioxide fixation

Journal of Colloid and Interface Science, Год журнала: 2025, Номер 688, С. 32 - 43

Опубликована: Фев. 20, 2025

Язык: Английский

Tailored Engineering of Primary Catalytic Sites and Secondary Coordination Spheres in Metalloenzyme-Mimetic MOF Catalysts for Boosting Efficient CO₂ Conversion

Chemical Science, Год журнала: 2025, Номер unknown

Опубликована: Янв. 1, 2025

The fabrication of metalloenzyme-mimetic artificial catalyst is a promising approach to achieve maximum catalytic efficiency, but the rational integration sophisticatedly optimized primary sites (PCS) and secondary coordination spheres (SCS) for specific transformation poses grand challenge. Here in this work, we report tailored engineering Cu PCS perfluoroalkyl SCS onto zirconium-based framework [UiO-67-(BPY-Cu)-F x (x = 3, 5, 7, 11)] [BPY 2,2'-bipyridine-5,5'-dicarboxylate] that can be utilized highly efficient carboxylic cyclization reaction between propargylamines flue gas CO2. groups act as tunable facilely adjust surface electronegativity, hydrophobicity, well CO2 affinity water vapor-resistance by simply varying chain length. Meanwhile, synergy significantly facilitated step stabilizing critical transition state, leading fast oxazolidinone ring. Owing these features, UiO-67-(BPY-Cu)-F7 exhibited remarkable behavior greatly facilitating binding CO2, promoting stabilization state cyclization, boosting releasing oxazolidinones, which have been systematically investigated combination substrate adsorption tests, situ Fourier transform infrared spectra, canonical Monte Carlo simulations, density functional theory calculations, etc. Consequently, showed outstanding performance under ambient conditions, exhibiting 64 times higher turnover frequency (TOF) than homogeneous or other MOF catalysts, highest TOF similar conditions. present work not only provides an alternative strategy construction advanced systems, also paves new direction development conversion with exceptional activity through catalysts.

Язык: Английский

Cu(i)-based metal–organic framework-derived core–shell composites for carbon dioxide conversion to oxazolidinones

Catalysis Science & Technology, Год журнала: 2025, Номер unknown

Опубликована: Янв. 1, 2025

Encapsulation of Cu 2 O NPs in MOFs and construction core–shell composites not only protects Cu( i ) but also promotes CO localized enrichment, enhancing catalytic efficiency for the one-pot synthesis oxazolidinones.

Язык: Английский