文献类型：期刊文献

英文题名：Strain enhances the activity of molecular electrocatalysts via carbon nanotube supports

作者：Su, Jianjun[1];Musgrave, Charles B.[2];Song, Yun[1];Huang, Libei[1];Liu, Yong[1];Li, Geng[1];Xin, Yinger[1];Xiong, Pei[3];Li, Molly Meng-Jung[3];Wu, Haoran[4];Zhu, Minghui[4];Chen, Hao Ming[5];Zhang, Jianyu[6];Shen, Hanchen[6];Tang, Ben Zhong[6];Robert, Marc[7];Goddard, William A., III[2];Ye, Ruquan[1,8]

机构：[1]City Univ Hong Kong, Dept Chem, State Key Lab Marine Pollut, Hong Kong, Peoples R China;[2]CALTECH, Mat & Proc Simulat Ctr, Pasadena, CA 91125 USA;[3]Hong Kong Polytech Univ, Dept Appl Phys, Hong Kong, Peoples R China;[4]East China Univ Sci & Technol, State Key Lab Chem Engn, Shanghai, Peoples R China;[5]Natl Taiwan Univ, Dept Chem, Taipei, Taiwan;[6]Chinese Univ Hong Kong Shenzhen CUHK Shenzhen, Shenzhen Inst Aggregate Sci & Technol, Sch Sci & Engn, Shenzhen, Peoples R China;[7]Univ Paris Cite, Lab Electrochim Mol, CNRS, Paris, France;[8]City Univ, Hong Kong Shenzhen Res Inst, Shenzhen, Peoples R China

年份：2023

卷号：6

期号：9

起止页码：818

外文期刊名：NATURE CATALYSIS

收录：;EI(收录号：20233414582989);WOS:【SCI-EXPANDED(收录号:WOS:001048827200001)】；

基金：R.Y. acknowledges support from the Guangdong Basic and Applied Basic Research Fund (2022A1515011333), the Hong Kong Research Grant Council (21300620, 11307120, 11309723), the State Key Laboratory of Marine Pollution (SKLMP/IRF/0029) and the Shenzhen Science and Technology Program (JCYJ20220818101204009 and 2021Szvup129). C.B.M. and W.A.G. acknowledge support from the Liquid Sunlight Alliance, which is supported by the US Department of Energy, Office of Science, Office of Basic Energy Sciences, Fuels from Sunlight Hub under award number DE-SC0021266. B.Z.T. acknowledges support from the Shenzhen Key Laboratory of Functional Aggregate Materials (ZDSYS20211021111400001) and the Science Technology Innovation Commission of Shenzhen Municipality (KQTD20210811090142053, JCYJ20220818103007014). We thank W. Zhai and L. Wang for help with Raman characterization, and W. Li for his assistance with high-resolution TEM imaging.

语种：英文

外文关键词：Density functional theory - Electrocatalysts - Molecules - Multiwalled carbon nanotubes (MWCN) - Photoelectron spectroscopy - X ray spectroscopy

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.