Engineering Pt‐Cu diatomics electrocatalysts enables highly efficient urea synthesis

• Published in: AIChE journal Vol. 70; no. 6
• Main Authors: Lu, Fei, Wang, Jingnan, Gao, Yuhang, Wang, Yan, Wang, Xi
• Format: Journal Article
• Language: English
• Published: Hoboken, USA John Wiley & Sons, Inc 01.06.2024; American Institute of Chemical Engineers
• Subjects: Carbon dioxide; Catalysts; Chemical reduction; Copper; C‐N coupling; Diatoms; Electrocatalysts; first‐principles design; Hydrogen evolution reactions; Platinum; Pt‐diatomics; suppressing the competitive reactions; Synthesis; Titanium dioxide; Urea; Ureas; urea‐synthesis electrocatalyst
• ISSN: 0001-1541; 1547-5905
• DOI: 10.1002/aic.18403

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 N2 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 (Pt1Cu1‐TiO2) for urea production based on theoretical predictions. Through rational screening of 8 Pt‐diatomics HUECs, we discovered that Pt1Cu1‐TiO2 can effectively suppress HER and NRR while promoting the adsorption of CO2 and N2. Subsequently, we experimentally fabricated Pt1Cu1‐TiO2 which exhibited optimal urea electrosynthesis activity of 51.71 molurea molPt+Cu−1 h−1. Pt1‐Cu1 diatomics in Pt1Cu1‐TiO2 could synergistically encourage the activation of *CO2/*N2 and crucial C‐N coupling with an optimal energy barrier (0.25 eV).