Photocatalytic C-N coupling from stable and transient intermediates for gram-scale acetamide synthesis DOI Creative Commons
Xin Li,

Weiping Yang,

Jun‐Ping Yue

et al.

Nature Communications, Journal Year: 2025, Volume and Issue: 16(1)

Published: April 15, 2025

Abstract Electro/photocatalytic C-N coupling acts as a key build-block to the next generation of chemicals like amides for wide applications in energy, pharmaceuticals and chemical industries. However, uncontrolled intermediates challenges efficient amide production regarding yield or selectivity. Here we propose photocatalytic radical addition route, where fundamental active species, including oxygen photogenerated electron-hole pairs, are regulated selective acetamide synthesis from mild co-oxidation CH 3 2 OH NH . Sufficient is provided accumulate stable intermediate (CH CHO). Meanwhile, limited concentration ensures controllable fast transient ( ● ) on CHO. Through directed stable-transient intermediates, rate pushed forward hundred-mmol level (105.61 ± 4.86 mmol·g cat −1 ·h with selectivity 99.17% 0.39%, reaching gram-scale (1.82 g) acetamide. These results illuminate valuable opportunities photocatalysis-driven synthetic industry.

Language: Английский

Artificial Photosynthesis of Formamide via an Oxidant‐Free Photoinduced Radical Coupling Route over Pt‐CdS DOI Open Access
Junyu Gao, Jinhu Wang, Dong Li

et al.

Angewandte Chemie International Edition, Journal Year: 2025, Volume and Issue: unknown

Published: March 9, 2025

Abstract Large‐scale manufacturing of formamide is always involved with the use carbon monoxide, hence developing a series eco‐friendly synthesis routes great significance. Alternative feedstock low‐cost methanol expected to fulfill this breakthrough due its green and renewable nature; however, overoxidation severely inhibits efficacious from ammonia through conventional catalytic route. Herein, we report successful development direct radical coupling route for converting into high‐selectivity hydrogen without extra oxidants under ambient conditions. The optimized Pt‐CdS photocatalysts offered an impressive production rate 1.45 mmol g −1 h , as well exceptional hole selectivity reaching up 63.5%. oxidant‐free mechanism high‐efficiency generation revealed by in situ characterizations (e.g., electron paramagnetic resonance transient absorption spectroscopy), stems photogenerated holes oxidizing hydroxymethyl subsequently C─N amino radical. This work demonstrates efficient photoinduced strategy promise acceptable alternative current technologies artificial photosynthesis using clean abundant solar energy.

Language: Английский

Citations

0
Interfacial Electron Transfer Induced Dual-Site Synergetic Effects Boosting Formamide Synthesis on Cuo/In2o3 Hollow Cubes DOI

Qiuyan Shen,

Wei‐Ren Chen,

Zixuan Wei

et al.

Published: Jan. 1, 2025

Language: Английский

Citations

0
Photocatalytic C-N coupling from stable and transient intermediates for gram-scale acetamide synthesis DOI Creative Commons
Xin Li,

Weiping Yang,

Jun‐Ping Yue

et al.

Nature Communications, Journal Year: 2025, Volume and Issue: 16(1)

Published: April 15, 2025

Abstract Electro/photocatalytic C-N coupling acts as a key build-block to the next generation of chemicals like amides for wide applications in energy, pharmaceuticals and chemical industries. However, uncontrolled intermediates challenges efficient amide production regarding yield or selectivity. Here we propose photocatalytic radical addition route, where fundamental active species, including oxygen photogenerated electron-hole pairs, are regulated selective acetamide synthesis from mild co-oxidation CH 3 2 OH NH . Sufficient is provided accumulate stable intermediate (CH CHO). Meanwhile, limited concentration ensures controllable fast transient ( ● ) on CHO. Through directed stable-transient intermediates, rate pushed forward hundred-mmol level (105.61 ± 4.86 mmol·g cat −1 ·h with selectivity 99.17% 0.39%, reaching gram-scale (1.82 g) acetamide. These results illuminate valuable opportunities photocatalysis-driven synthetic industry.

Language: Английский

Citations

0