Journal
ACS APPLIED MATERIALS & INTERFACES
Volume 15, Issue 46, Pages 53436-53445Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsami.3c11097
Keywords
electrocatalysis; acetamide synthesis; single-atomalloy catalyst; C-C coupling; C-Ncoupling
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This study investigates the catalytic performance of Cu-based single-atom alloys in the electrochemical synthesis of acetamide from CO2 and N2. It is found that the W/Cu(111) SAA demonstrates exceptional activity and selectivity, effectively producing acetamide while suppressing undesired side reactions. The results suggest that this catalyst system provides an efficient pathway for forming C-C and C-N bonds through CO2/N-2 reduction.
The electrochemical conversion of carbon dioxide into value-added compounds not only paves the way toward a sustainable society but also unlocks the potential for electrocatalytic synthesis of amides through the introduction of N atoms. However, it also poses one of the greatest challenges in catalysis: achieving simultaneous completion of C-C coupling and C-N coupling. Here, we have meticulously investigated the catalytic prowess of Cu-based single-atom alloys in facilitating the electrochemical synthesis of acetamide from CO2 and N-2. Through a comprehensive screening process encompassing catalyst stability, adsorption capability, and selectivity against the HER, W/Cu(111) SAA has emerged as an auspicious contender. The reaction entails CO2 reduction to CO, C-C coupling leading to the formation of a ketene intermediate *CCO, N-2 reduction, and C-N coupling between NH3 and *CCO culminating in the production of acetamide. The W/Cu(111) surface not only exhibits exceptional activity in the formation of acetamide, with a barrier energy of 0.85 eV for the rate-determining CO hydrogenation step, but also effectively suppresses undesired side reactions leading to various C-1 and C-2 byproducts during CO2 reduction. This work presents a highly effective approach for forming C-C and C-N bonds via coelectroreduction of CO2 and N-2, illuminating the reaction mechanism underlying acetamide synthesis from these two gases on single-atom alloy catalysts. The catalyst design strategy employed in this study has the potential to be extended to a range of amide chemicals, thereby broadening the scope of products that can be obtained through CO2/N-2 reduction.
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