https://scholars.lib.ntu.edu.tw/handle/123456789/635006
標題: | Strain enhances the activity of molecular electrocatalysts via carbon nanotube supports | 作者: | Su, Jianjun Musgrave, Charles B. Song, Yun Huang, Libei Liu, Yong Li, Geng Xin, Yinger Xiong, Pei Li, Molly Meng Jung Wu, Haoran Zhu, Minghui HAO MING CHEN Zhang, Jianyu Shen, Hanchen Tang, Ben Zhong Robert, Marc Goddard, William A. Ye, Ruquan |
公開日期: | 1-一月-2023 | 來源出版物: | Nature Catalysis | 摘要: | Support-induced strain engineering is useful for modulating the properties of two-dimensional materials. However, controlling strain of planar molecules is technically challenging due to their sub-2 nm lateral size. Additionally, the effect of strain on molecular properties remains poorly understood. Here we show that carbon nanotubes (CNTs) are ideal substrates for inducing optimum properties through molecular curvature. In a tandem-flow electrolyser with monodispersed cobalt phthalocyanine (CoPc) on single-walled CNTs (CoPc/SWCNTs) for CO2 reduction, we achieve a methanol partial current density of >90 mA cm−2 with >60% selectivity, surpassing wide multiwalled CNTs at 16.6%. We report vibronic and X-ray spectroscopies to unravel the distinct local geometries and electronic structures induced by the strong molecule–support interactions. Grand canonical density functional theory confirms that curved CoPc/SWCNTs improve *CO binding to enable subsequent reduction, whereas wide multiwalled CNTs favour CO desorption. Our results show the important role of SWCNTs beyond catalyst dispersion and electron conduction. [Figure not available: see fulltext.]. |
URI: | https://scholars.lib.ntu.edu.tw/handle/123456789/635006 | ISSN: | 2520-1158 | DOI: | 10.1038/s41929-023-01005-3 |
顯示於: | 化學系 |
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