Year: 2025
Type: article
Abstract: High Resolution Image Download MS PowerPoint Slide Direct hydrogenation of N 2 at ambient conditions lags behind the recent advances in molecular N 2 (electro-)fixation. In fact, molecular platforms that couple N 2 and H 2 activation remain rare. Inspired by recent photocatalytic approaches, we report here the photochemical hydrogenation of an N 2 -derived rhenium(V) benzoylimido complex. Self-sensitized photolysis with sacrificial 1,4-cyclohexadiene gave benzamide in a high yield. In turn, a new iridium(III) porphyrinato hydrido photocatalyst allowed for quantitative photohydrogenation via light-driven net hydride transfer. Transient absorption spectroscopy and computations support a light-driven, stepwise hydride transfer mechanism that is enabled by relativistic effects. This approach provides a new strategy for the reductive transformation of N 2 into nitrogenous products beyond ammonia.
Source: JACS Au
Language: English
Subfield: Organic Chemistry
Field: Chemistry
Domain: Physical Sciences
Open Access status: gold
Estimated APC paid: $3,500
OpenAlex ID: W4414577345