A Strong Magnetic Field Alters the Activity and Selectivity of the CO₂RR by Restraining C–C Coupling

Abstract

As an external field, a magnetic field can change the electrocatalytic activity of catalysts through various effects. Among them, electron spin polarization on the catalyst surface has attracted much attention. Herein, we investigate the sensitive response behavior of a Cu2O nanocubes to an in situ magnetic field. Under a 3 T strong magnetic field, the total transferred electron quantity in IT test (−1.1 VRHE) and the current density in the polarization curve increase by 28.7% and 54.7%, respectively, while the onset potential decreases significantly by 114 mV. Moreover, it was found that product selectivity was also altered by the magnetic field. The Faraday efficiency of C1 increases substantially, along with the inhibition of C2+ reaction paths and the HER. Our experimental results and DFT calculation demonstrate that a hybrid magnetic effect accelerates the CO2RR kinetic and generates spin polarization of the catalyst surface. The polarized surface changes the binding energy of *OCHO/*COOH and inhibits singlet C–C coupling, which restrains the C2+ reduction path and thus more CO2 is reduced to HCOOH.

Keywords

• CO₂RR
• magnetic field effect
• Cu-based catalysts
• spin polarization