Photoelectrocatalytic Cl-mediated C(sp3)–H aminomethylation of hydrocarbons by BiVO4 photoanodes

Nature Communications, Год журнала: 2025, Номер 16(1)

Опубликована: Март 8, 2025

Interfacial photoelectrochemistry at photoanodes has been extensively researched for solar energy conversion, but its application the production of high-value-added chemical compounds in organic chemistry still presents challenges. Herein, we report photoelectrocatalytic Cl-mediated C(sp3)–H aminomethylation alkanes with self-developed and reusable BiVO4 photoanodes. The swift condensation aniline aldehydes, along decrease electricity input by photogenerated holes photoanodes, work together to prevent excessive oxidation aniline, leading high yields desired product. Mechanistic experiments demonstrate that Cl- ions, as key mediators, could be attracted oxidized form Cl2. This is followed light-promoted homolytic cleavage Cl2, generating Cl radicals efficiently abstract hydrogen atoms from hydrocarbons. opens an avenue interfacial photoelectrochemical synthesis demonstrates a potential method optimizing conversion into fuels. A stable recyclable photoelectrode material was developed efficient hydrocarbons cell, which provides promising fuel conversion.

Язык: Английский

DABCO‐Mediated Photoelectrochemical Three‐Component Sulfonocyclization of 3‐Aza‐1,5‐dienes

Chinese Journal of Chemistry, Год журнала: 2024, Номер unknown

Опубликована: Дек. 2, 2024

Comprehensive Summary Herein, we report a rare example of three‐component net‐oxidative sulfonylation SO 2 surrogate with an oxidatively activated radical precursor under mild and metal‐ external‐oxidant‐free conditions. The mildness sustainability the reaction are enabled by photoelectrocatalysis, 3‐aza‐1,5‐dienes, organotrifluoroborates 1,4‐diazabicyclo[2.2.2]octane bis(sulfur dioxide) adduct (DABSO) undergo sulfonylative cyclization to afford sulfono 4‐pyrrolin‐2‐ones in atom‐economical manner broad substrate scope good functional‐group tolerance. protocol is amenable late‐stage diversification complex molecular architectures as well gram‐scale synthesis. Sunlight could be used light source, conducted all‐solar mode using commercially available photovoltaic panel generate electricity situ . Mechanistic studies reveal that generated (DABCO), which was generally innocent previous reactions, functions electron shuttle between photocatalytic cycle reactants.

Язык: Английский