近日，天津大学邓意达团队报道了电化学尿素合成单原子催化剂的高通量理论筛选。2025年11月4日出版的《德国应用化学》杂志发表了这项成果。

电化学尿素合成技术为可持续利用氮、碳资源提供了前景广阔的路径，但其发展受到反应机理不明确和有效催化剂设计原则缺失的制约。

研究组通过对40余种MN₄C型单原子催化剂进行高通量筛选，成功遴选出适用于电化学尿素合成的优势候选材料。该策略相较传统方法筛选效率提升94.8%。理论分析表明，Ti─、V─、Nb─、Mo─及Hf–N₄C催化剂能同时满足多项关键要求：热力学稳定性、小分子吸附优势、竞争反应抑制能力，以及氢化与C–N耦合过程的低能垒。

机理研究揭示出两种不同的C–N耦合路径，并证实N物种的氢化是后续耦合的必要前提。值得注意的是，研究组发现了NO₃^-还原与尿素全合成极限电势之间的线性关联，确立了NO₃→ *N转化活性作为催化剂筛选的有效描述符。该研究为理性设计高效尿素电催化剂提供了机理认知与预测框架。

附：英文原文

Title: High-Throughput Theoretical Screening of Single-Atom Catalysts for Electrochemical Urea Synthesis

Author: Yuan Liu, Zihan Shen, Zexiang Yin, Heng Zhao, Jiayi Qin, Yang Wang, Yaqiong Su, Haozhi Wang, Wenbin Hu, Zhichuan J. Xu, Yida Deng

Issue&Volume: 2025-11-04

Abstract: Electrochemical urea synthesis offers a promising approach for sustainable nitrogen and carbon utilization, yet its progress is hindered by the unclear reaction mechanism and the lack of effective catalyst design principles. Here, we conduct a high-throughput screening of over 40 MN4C-type single-atom catalysts (SACs) to identify promising candidates for electrochemical urea synthesis. This strategy improves screening efficiency by 94.8% compared to conventional methods. Our analysis demonstrates that Ti─, V─, Nb─, Mo─, and Hf–N4C catalysts concurrently fulfill the essential criteria, including thermodynamic stability, favorable adsorption of small molecules, suppression of competing reactions, and low energy barriers for both hydrogenation and C–N coupling. Mechanistic investigations reveal two distinct C–N coupling pathways and demonstrate that hydrogenation of *N species is a prerequisite for subsequent coupling. Notably, we reveal a linear correlation between the limiting potentials of NO3 reduction and overall urea synthesis, establishing *NO3 → *N activity as a reliable descriptor for catalyst screening. This work provides mechanistic insights and a predictive framework for the rational design of efficient urea electrocatalysts.

DOI: 10.1002/anie.202516299

Source: https://onlinelibrary.wiley.com/doi/10.1002/anie.202516299