Promising urea electrosynthesis by C-N coupling on copper-based single-atom alloys

Abstract

Electrochemical synthesis of urea holds a significant importance in the energy landscape, however, the lack of efficient electrocatalysts is the main bottleneck. In this study, 40 single-atom alloys (SAAs) based on Cu(100) and Cu(111) surfaces have been systematically investigated as electrocatalysts for CO2 and N2 co-reduction to produce urea utilizing first-principles calculations. A promising single N and C coupling pathway is uncovered on Cu-based SAAs, besides conventional NCON, CO2, COOH, and CO pathways. CuHf(100) displays a high efficiency in N-N decomposition, C-N coupling, and low reaction limiting potential. Furthermore, CuHf(100) and CuSc(100) have been identified as superior electrocatalysts for efficient urea electrosynthesis. This work provides potential reaction mechanisms with specific single N species, but also a universal strategy for the surface engineering of transition metal-based catalysts in electrocatalytic urea synthesis reactions.