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

Abstract

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 CO 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.