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- Title
Highly Efficient and Selective N‐Formylation of Amines with CO<sub>2</sub> and H<sub>2</sub> Catalyzed by Porous Organometallic Polymers.
- Authors
Shen, Yajing; Zheng, Qingshu; Chen, Zhe‐Ning; Wen, Daheng; Clark, James H.; Xu, Xin; Tu, Tao
- Abstract
The valorization of carbon dioxide (CO2) to fine chemicals is one of the most promising approaches for CO2 capture and utilization. Herein we demonstrated a series of porous organometallic polymers could be employed as highly efficient and recyclable catalysts for this purpose. Synergetic effects of specific surface area, iridium content, and CO2 adsorption capability are crucial to achieve excellent selectivity and yields towards N‐formylation of diverse amines with CO2 and H2 under mild reaction conditions even at 20 ppm catalyst loading. Density functional theory calculations revealed not only a redox‐neutral catalytic pathway but also a new plausible mechanism with the incorporation of the key intermediate formic acid via a proton‐relay process. Remarkably, a record turnover number (TON=1.58×106) was achieved in the synthesis of N,N‐dimethylformamide (DMF), and the solid catalysts can be reused up to 12 runs, highlighting their practical potential in industry.
- Subjects
FORMYLATION; ORGANOMETALLIC polymers; POROUS polymers; CATALYSTS recycling; TURNOVER frequency (Catalysis); DENSITY functional theory
- Publication
Angewandte Chemie, 2021, Vol 133, Issue 8, p4171
- ISSN
0044-8249
- Publication type
Article
- DOI
10.1002/ange.202011260