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Enhanced photocatalytic synthesis of urea from co‐reduction of N2 and CO2 on Z‐schematic SrTiO3‐FeS‐CoWO4 heterostructure
Angewandte Chemie International Edition ( IF 16.1 ) Pub Date : 2024-11-19 , DOI: 10.1002/anie.202419628
Muhammad Irfan Ahmad, Yanming Liu, Yaqi Wang, Peike Cao, Hongtao Yu, Houfen Li, Shuo Chen, Xie Quan

The photocatalytic co‐reduction of CO2 and N2 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, SrTiO3‐FeS‐CoWO4, for boosting photocatalytic urea synthesis via enhancing the initial CO2 and N2 adsorption step and reducing the energy barrier for the C‐N coupling reaction. A high urea yield of 8054.2 μg·gcat−1·h‐1 was achieved on SrTiO3‐FeS‐CoWO4, which was significantly higher than the state‐of‐the‐art. The SrTiO3‐FeS‐CoWO4 Z‐scheme photocatalyst, with accelerated charge transfer by FeS, not only had dual active sites for the chemical adsorption and activation of CO2 and N2, 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.

中文翻译:


N2 和 CO2 在 Z 示意图 SrTiO3-FeS-CoWO4 异质结构上共还原增强光催化合成尿素



CO2 和 N2 的光催化共还原是在温和条件下合成尿素的可持续方法。然而,由于 C-N 偶联反应的动力学缓慢,尿素的高产率合成是一项挑战。在此,我们成功设计了一种 Z 型光催化剂 SrTiO3-FeS-CoWO4,用于通过增强初始 CO2 和 N2 吸附步骤和减少 C-N 耦合反应的能垒来促进光催化尿素合成。在 SrTiO3-FeS-CoWO4 上实现了 8054.2 μg·gcat-1·h-1 的高尿素产率,明显高于最先进的水平。SrTiO3‐FeS‐CoWO4 Z-型光催化剂通过 FeS 加速电荷转移,不仅具有化学吸附和活化 CO2 和 N2 的双活性位点,而且还保留了高导带 (-1.50 eV) 和电子和质子的加速供应,这是其良好的光还原活性和显著降低的 C-N 耦合反应速率决定步骤的能量势垒的原因。
更新日期:2024-11-19
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