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表面稳定二氮烯的光生和可视化

Photogeneration and Visualization of a Surface-Stabilized Dinitrene.

作者信息

Frezza Federico, Sánchez-Grande Ana, Canola Sofia, Nacci Christophe, Klívar Jiří, Mutombo Pingo, Chen Qifan, Gómez-Fernandez José María, Sánchez-Sánchez Carlos, Berger Jan, Ernst Karl-Heinz, Stará Irena G, Martín-Gago José Ángel, Starý Ivo, Grill Leonhard, Jelínek Pavel

机构信息

Institute of Physics, Czech Academy of Sciences, Cukrovarnická 10, 16200, Prague 6, Czech Republic.

Faculty of Nuclear Sciences and Physical Engineering, Czech Technical University in Prague, Břehová 78/7, 11519, Prague 1, Czech Republic.

出版信息

Angew Chem Int Ed Engl. 2025 May 12;64(20):e202502640. doi: 10.1002/anie.202502640. Epub 2025 Mar 6.

DOI:10.1002/anie.202502640
PMID:39989376
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC12070354/
Abstract

Nitrenes are known as key intermediates in various chemical reactions. Nitrene transfer reactions are particularly effective for synthesizing nitrogen-containing compounds, where metal catalysts play a crucial role in controlling nitrene reactivity and selectivity. In this study, we demonstrate the formation of a stable surface-supported dinitrene on Au(111) through UV irradiation of its diazide precursor, characterized by scanning probe techniques. The photoreaction mechanism is elucidated with wavelength-dependent experiments and time-dependent density functional theory calculations. Our findings present the first real-space visualization of a metal nitrene adsorbed on a surface, highlighting its potential in catalysis and surface functionalization.

摘要

氮宾是各种化学反应中的关键中间体。氮宾转移反应在合成含氮化合物方面特别有效,其中金属催化剂在控制氮宾的反应活性和选择性方面起着至关重要的作用。在本研究中,我们通过对其重氮化合物前体进行紫外线照射,证明了在Au(111)上形成了稳定的表面负载二氮宾,并通过扫描探针技术对其进行了表征。通过波长相关实验和含时密度泛函理论计算阐明了光反应机理。我们的研究结果首次实现了吸附在表面的金属氮宾的实空间可视化,突出了其在催化和表面功能化方面的潜力。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/654c/12070354/3e99bba211f8/ANIE-64-e202502640-g004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/654c/12070354/b7f38966ba7d/ANIE-64-e202502640-g002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/654c/12070354/df774125cb17/ANIE-64-e202502640-g001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/654c/12070354/1ffbf4ebcf3d/ANIE-64-e202502640-g003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/654c/12070354/3e99bba211f8/ANIE-64-e202502640-g004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/654c/12070354/b7f38966ba7d/ANIE-64-e202502640-g002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/654c/12070354/df774125cb17/ANIE-64-e202502640-g001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/654c/12070354/1ffbf4ebcf3d/ANIE-64-e202502640-g003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/654c/12070354/3e99bba211f8/ANIE-64-e202502640-g004.jpg

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本文引用的文献

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