Engineering Pt‐Cu diatomics electrocatalysts enables highly efficient urea synthesis

Abstract The rational design of novel heterogeneous urea‐synthesis electrocatalysts (HUECs) poses an immense challenge due to their inherent complexity. Moreover, the ideal HUECs must also possess the ability to suppress two major competitive reactions: hydrogen evolution reaction (HER) and N 2 reduction reaction (NRR). However, this daunting task can be made feasible with the use of heterogeneous diatomic catalysts that have been supported by unambiguous theoretical models. Herein, we report a design for an efficient platinum‐copper diatomic electrocatalyst (Pt 1 Cu 1 ‐TiO 2 ) for urea production based on theoretical predictions. Through rational screening of 8 Pt‐diatomics HUECs, we discovered that Pt 1 Cu 1 ‐TiO 2 can effectively suppress HER and NRR while promoting the adsorption of CO 2 and N 2 . Subsequently, we experimentally fabricated Pt 1 Cu 1 ‐TiO 2 which exhibited optimal urea electrosynthesis activity of 51.71 mol urea mol Pt+Cu −1 h −1 . Pt 1 ‐Cu 1 diatomics in Pt 1 Cu 1 ‐TiO 2 could synergistically encourage the activation of *CO 2 /*N 2 and crucial C‐N coupling with an optimal energy barrier (0.25 eV).