To achieve efficient urea formation via electrocatalytic C–N coupling, we proposed a new route for synthesizing urea on 2D metal borides (MBenes) by theoretical prediction. It has been reported that inert CO₂ and N₂ molecules can be converted into urea via electrocatalytic C–N bond coupling, which is a promising alternative method to industrial processes. However, due to the weak adsorption of and difficulty in activating CO₂ and N₂ molecules, the reaction of C–N coupling is challenging to achieve. To ensure C–N bond coupling between *NN* and *CO to form *NCON intermediates, which act as the key precursor to urea formation, the utilization of sustainable energy (solar energy) can be helpful in addressing the challenge of electrochemically synthesizing urea. Furthermore, computational screening provides an effective way to gain insight into the mechanisms of the C–N coupling and protonation steps. It is also beneficial for guiding the development of the sustainable synthesis of carbon nitride chemicals via C–N coupling, and we believe it will attract full attention in the future. A new theoretical strategy was used to screen efficient catalysts for urea electrosynthesis based on coupling CO₂ and N₂ to generate H₂NCONH₂. We established the Gibbs free energy landscape and calculated the limiting potential based on the rate-determining step, and a volcano plot was constructed as a function of ΔG(*NCON) to predict MBenes for urea formation. It included the kinetic stability, CO₂ and N₂ adsorbability, catalytic activity, and urea synthesis selectivity. It is demonstrated that Mo₂B₂ and Ru₂B₄ are suitable urea electrosynthesis catalysts with high activity and selectivity. This work can contribute to the application of C–N coupling electrochemical reactions.

为了通过电催化 C-N 偶联实现有效的尿素形成，我们提出了一种通过理论预测在二维金属硼化物 (MBenes) 上合成尿素的新途径。据报道，惰性CO ₂和N ₂分子可以通过电催化C-N键偶联转化为尿素，这是一种很有前途的工业过程替代方法。然而，由于CO ₂和N ₂分子吸附较弱且难以活化，C-N偶联反应难以实现。确保*N之间的C-N键耦合N* 和 *CO 形成 *NCON 中间体，作为尿素形成的关键前体，可持续能源（太阳能）的利用有助于解决电化学合成尿素的挑战。此外，计算筛选提供了一种深入了解 C-N 耦合和质子化步骤机制的有效方法。这也有利于指导通过C-N耦合可持续合成氮化碳化学品的发展，我们相信它会在未来引起充分的关注。基于CO ₂和N ₂偶联生成H ₂ NCONH _{2的新型理论策略筛选尿素电合成高效催化剂}. 我们建立了吉布斯自由能图谱，并基于速率确定步骤计算了极限势，并构建了一个火山图作为 ΔG(*NCON) 的函数来预测尿素形成的 MBenes。它包括动力学稳定性、CO ₂和N ₂吸附性、催化活性和尿素合成选择性。证明Mo ₂ B ₂和Ru ₂ B ₄是合适的具有高活性和选择性的尿素电合成催化剂。这项工作有助于 C-N 耦合电化学反应的应用。