Abstract
Electrochemical reduction of carbon dioxide (CO2) into chemicals and fuels has recently attracted much interest, but normally suffers from a high overpotential and low selectivity. In this work, single P atoms were introduced into a N-doped carbon supported single Fe atom catalyst (Fe-SAC/NPC) mainly in the form of P−C bonds for CO2 electroreduction to CO in an aqueous solution. This catalyst exhibited a CO Faradaic efficiency of ≈97 % at a low overpotential of 320 mV, and a Tafel slope of only 59 mV dec−1, comparable to state-of-the-art gold catalysts. Experimental analysis combined with DFT calculations suggested that single P atom in high coordination shells (n≥3), in particular the third coordination shell of Fe center enhanced the electronic localization of Fe, which improved the stabilization of the key *COOH intermediate on Fe, leading to superior CO2 electrochemical reduction performance at low overpotentials.
Original language | English |
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Pages (from-to) | 23614-23618 |
Journal | Angewandte Chemie - International Edition |
Volume | 60 |
Issue number | 44 |
Early online date | 31 Aug 2021 |
DOIs | |
Publication status | Published - 25 Oct 2021 |
Keywords
- CO electroreduction
- electron localization
- low overpotentials
- phosphorous
- single Fe atom