Cooperative adsorption of interfacial Ga-N dual-site in GaOOH@N-doped carbon nanotubes for enhanced electrocatalytic reduction of carbon dioxide

To reduce activation energy barrier and promote the kinetics of electrocatalytic CO₂ reduction reaction (eCO₂RR), the performance of CO₂ adsorption and activation on electrocatalysts should be optimized. Here, GaOOH is successfully coupled with N-doped carbon nanotubes (NC) via a facile self-assembly-calcination process. The obtained GaOOH@N-doped carbon nanotubes (Ga-NC) display the best CO faradaic efficiency of 96.1 % at −0.6 V (vs. reversible hydrogen electrode). Control-experiment and characterization results suggest Ga-N dual-site in interface between GaOOH and NC shows cooperative adsorption of CO₂. C atom in CO₂ is adsorbed on N site while O atom in CO₂ is adsorbed on Ga site. This cooperative adsorption efficiently promotes the CO₂ adsorption and activation performance, as well as the breaking of C[dbnd]O bond due to opposite attraction from Ga-N dual-site. Moreover, in-situ Fourier transform infrared spectroscopy confirms decreased reaction barrier for formation of *CO₂^– and *COOH intermediates. This work inspires us to construct interfacial dual-site structure with cooperative adsorption property for promoting eCO₂RR activity.