Strain enhances the activity of molecular electrocatalysts via carbon nanotube supports

Abstract Support-induced strain engineering is useful for modulating the properties of two-dimensional materials. However, controlling planar molecules technically challenging due to their sub-2 nm lateral size. Additionally, effect on molecular remains poorly understood. Here we show that carbon nanotubes (CNTs) are ideal substrates inducing optimum through curvature. In a tandem-flow electrolyser with monodispersed cobalt phthalocyanine (CoPc) single-walled CNTs (CoPc/SWCNTs) CO 2 reduction, achieve methanol partial current density >90 mA cm −2 >60% selectivity, surpassing wide multiwalled at 16.6%. We report vibronic and X-ray spectroscopies unravel distinct local geometries electronic structures induced by strong molecule–support interactions. Grand canonical functional theory confirms curved CoPc/SWCNTs improve *CO binding enable subsequent whereas favour desorption. Our results important role SWCNTs beyond catalyst dispersion electron conduction.