Ahmad Muhammad Irfan, Liu Yanming, Wang Yaqi, Cao Peike, Yu Hongtao, Li Houfen, Chen Shuo, Quan Xie
Key Laboratory of Industrial Ecology and Environmental Engineering (Ministry of Education), School of Environmental Science and Technology, Dalian University of Technology, Dalian, 116024, China.
College of Environment Science and Engineering, Taiyuan University of Technology, Taiyuan, 030024, China.
Angew Chem Int Ed Engl. 2025 Feb 10;64(7):e202419628. doi: 10.1002/anie.202419628. Epub 2024 Nov 27.
The photocatalytic co-reduction of CO and N is a sustainable method for urea synthesis under mild conditions. However, high-yield synthesis of urea is a challenge due to the sluggish kinetics of the C-N coupling reaction. Herein, we have successfully engineered a Z-scheme photocatalyst, SrTiO-FeS-CoWO, for boosting photocatalytic urea synthesis via enhancing the initial CO and N adsorption step and reducing the energy barrier for the C-N coupling reaction. A high urea yield of 8054.2 μg ⋅ g ⋅ h was achieved on SrTiO-FeS-CoWO, which was significantly higher than the state-of-the-art. The SrTiO-FeS-CoWO Z-scheme photocatalyst, with accelerated charge transfer by FeS, not only had dual active sites for the chemical adsorption and activation of CO and N, but also retained the high conduction band (-1.50 eV) and accelerated supply of electrons and protons, which are responsible for its good photoreduction activity and significantly reduced energy barrier for the rate-determining step of C-N coupling reaction.
在温和条件下,光催化共还原CO和N是一种可持续的尿素合成方法。然而,由于C-N偶联反应动力学缓慢,高产率合成尿素是一项挑战。在此,我们成功设计了一种Z型光催化剂SrTiO-FeS-CoWO,通过增强初始CO和N吸附步骤并降低C-N偶联反应的能垒来促进光催化尿素合成。在SrTiO-FeS-CoWO上实现了8054.2 μg·g⁻¹·h的高尿素产率,这显著高于目前的先进水平。具有通过FeS加速电荷转移的SrTiO-FeS-CoWO Z型光催化剂,不仅具有用于CO和N化学吸附与活化的双活性位点,还保留了高导带(-1.50 eV)并加速了电子和质子的供应,这使其具有良好的光还原活性,并显著降低了C-N偶联反应速率决定步骤的能垒。