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Achieving selective synthesis of N-benzylformamide via one-step electrocatalytic C-N coupling of CO2 and benzylamine
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DOI：10.1039/D6GC01435F.png)
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Abstract
En 中文
The pressing demands of CO2 emission reduction and organic amine pollutant treatment motivate the development of electrocatalytic C-N coupling toward resource recovery and green synthesis. The key challenge lies in co-activating both reactants while suppressing CO2 excessive reduction. Herein; we report the first efficient one-step electrocatalytic synthesis of N‑benzylformamide from CO2 and benzylamine under mild conditions over a bridging‑oxygen coordinated tin phthalocyanine catalyst (C-O-SnPc). At –3.8 V; it achieved a current density of 32 mA·cm–2; a Faradaic efficiency of 33.4%; and a yield of 53 mmol·L–1·h–1. In situ experiments identified key intermediates *COOH and *PhCH2NHCOOH; confirming a *COOH-mediated pathway. Theoretical calculations revealed oxygen coordination created a multifunctional electron-deficient Sn center. It polarized N-H bond and initiated an electron‑withdrawing chain that enhanced *COOH electrophilicity; facilitating the nucleophilic attack (C-N bonding). It also reduced the hydrogenation barrier from *PhCH2NHCOOH to *PhCH2NHCH2O2. This work provides a green strategy for resource recovery and upgrading CO2 and amines into high-value amides.
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