在 Z 型 SrTiO3-FeS-CoWO4 异质结构上增强 N2 和 CO2 共同还原尿素的光催化合成。

IF 16.1 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Angewandte Chemie International Edition 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
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引用次数: 0

摘要

CO2 和 N2 的光催化共还原反应是在温和条件下合成尿素的一种可持续方法。然而,由于 C-N 偶联反应的动力学缓慢,高产合成尿素是一项挑战。在此,我们成功地设计了一种 Z 型光催化剂 SrTiO3-FeS-CoWO4 ,通过增强 CO2 和 N2 的初始吸附步骤并降低 C-N 偶联反应的能量障碍,促进光催化尿素合成。SrTiO3-FeS-CoWO4 的尿素产率高达 8054.2 μg-gcat-1-h-1,明显高于最先进的水平。由 FeS 加速电荷转移的 SrTiO3-FeS-CoWO4 Z 型光催化剂不仅具有化学吸附和活化 CO2 和 N2 的双重活性位点,而且保留了高导带(-1.50 eV)和电子与质子的加速供应,这是其具有良好光导活性和显著降低 C-N 偶联反应决定速率步骤能垒的原因。
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Enhanced photocatalytic synthesis of urea from co-reduction of N2 and CO2 on Z-schematic SrTiO3-FeS-CoWO4 heterostructure.

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.

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来源期刊
CiteScore
26.60
自引率
6.60%
发文量
3549
审稿时长
1.5 months
期刊介绍: Angewandte Chemie, a journal of the German Chemical Society (GDCh), maintains a leading position among scholarly journals in general chemistry with an impressive Impact Factor of 16.6 (2022 Journal Citation Reports, Clarivate, 2023). Published weekly in a reader-friendly format, it features new articles almost every day. Established in 1887, Angewandte Chemie is a prominent chemistry journal, offering a dynamic blend of Review-type articles, Highlights, Communications, and Research Articles on a weekly basis, making it unique in the field.
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