Year: 2023
Type: article
Abstract: 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 CO 2 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.
Source: Nature Catalysis
Institutions: City University of Hong Kong, State Key Laboratory of Marine Pollution, California Institute of Technology, Hong Kong Polytechnic University, East China University of Science and Technology, State Key Laboratory of Chemical Engineering, National Taiwan University, Chinese University of Hong Kong, Shenzhen, Centre National de la Recherche Scientifique, Université Paris Cité, Laboratoire d'Electrochimie Moléculaire, City University of Hong Kong, Shenzhen Research Institute
Language: English
Field: Energy
Domain: Physical Sciences
Open Access status: hybrid
Estimated APC paid: $11,690
OpenAlex ID: W4385805408