Mingyu Cheng, Shao Wang, Zechuan Dai, Prof. Jing Xia, Bocheng Zhang, Pingyi Feng, Yin Zhu, Yangyang Zhang, Prof. Genqiang Zhang
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引用次数: 0
Abstract
Electrocatalytic C−N coupling for urea synthesis from carbon dioxide (CO2) and nitrate (NO3−) offers a sustainable alternative to the traditional Bosch-Meiser method. However, the complexity of intermediates in co-reduction hampers simultaneous improvement in urea yield and Faradaic efficiency (FE). Herein, we developed a Cu/Cu2O Mott–Schottky catalyst with nanoscale rectifying heterointerfaces through precise controllable in situ electroreduction of Cu2O nanowires, achieving notable FE (32.6–47.0 %) and substantial yields (6.08–30.4 μmol h−1 cm−2) across a broad range of ultralow applied potentials (0 to −0.3 V vs. RHE). Operando synchrotron radiation-Fourier transform infrared spectroscopy (SR-FTIR) confirmed the formation of *CO intermediates and C−N bonds, subsequently density functional theory (DFT) calculations deciphered that the Cu/Cu2O rectifying heterointerface modulated *CO adsorption, significantly enhancing subsequent C−N coupling dynamics between *CO and *NOH intermediates. This work not only provides a groundbreaking and advanced pathway for C−N coupling, but also offers deep insights into copper-based heterointerface catalysts for urea synthesis.
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.