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Mechanochemical Urea Synthesis Using Ammonia–Water and Carbon Dioxide Under Mild Conditions: An Experimental and Theoretical Study

Yichun Lou,Haoyu Chen,Linrui Wang,Shengpeng Chen,Yameng Song,Yifei Ding,Zixiang Hao,Chengli He,Dong Qiu,Hui Li,Junjian Wang,Duanyang Liu,Xiaoli Cui

The production of urea predominantly relies on the energy-intensive Bosch–Meiser process, which operates at temperatures ranging from 150 to 200 °C and pressures of approximately 150 to 250 bar. More sustainable approaches to urea synthesis under milder conditions remain a significant challenge. Herein, we demonstrate that urea can be synthesized via a mechanochemical method using ammonia–water and CO2 under an ambient environment. Without extra catalysts, the ZrO2 texture of the jar and grinding balls has a crucial mechanocatalytic effect on direct urea synthesis. Experimental data coupled with theoretical calculation results indicate that the mechano-induced oxygen vacancies (OV) within the (101) crystal plane of ZrO2 play a pivotal role in urea formation. These vacancies notably reduce the energy barrier for the generation of *NH2 and the subsequent decomposition of NH2COOH, thereby facilitating a more energy-efficient urea synthesis process. This work presents a novel method for synthesizing urea under mild conditions, offering potential cost-effective alternatives to urea production.