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 CO and N 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, CO, 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.

中文翻译：

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铜基单原子合金上 CN 耦合电合成尿素的前景广阔


尿素的电化学合成在能源领域具有重要意义，然而，缺乏高效的电催化剂是主要瓶颈。在这项研究中，系统地研究了 40 种基于 Cu(100) 和 Cu(111) 表面的单原子合金 (SAA) 作为 CO 和 N 共还原生产尿素的电催化剂，利用第一原理计算。除了传统的 NCON、CO、COOH 和 CO 途径之外，在 Cu 基 SAA 上还发现了一种有前景的单一 N 和 C 偶联途径。 CuHf(100) 在 NN 分解、CN 偶联方面表现出高效率，并且反应极限电位低。此外，CuHf(100) 和 CuSc(100) 已被认为是高效尿素电合成的优质电催化剂。这项工作提供了特定单一氮物种的潜在反应机制，同时也为电催化尿素合成反应中过渡金属基催化剂的表面工程提供了通用策略。