Boosting CO₂ Electroreduction on Bismuth Nanoplates with a Three-Dimensional Nitrogen-Doped Graphene Aerogel Matrix

Electrochemical CO₂ reduction reaction (CO₂RR), which uses renewable electricity to produce high-value-added chemicals, offers an alternative clean path to the carbon cycle. However, bismuth-based catalysts show great potential for the conversion of CO₂ and water to formate, but their overall efficiency is still hampered by the weak CO₂ adsorption, low electrical conductivity, and slow mass transfer of CO₂ molecules. Herein, we report that a rationally modulated nitrogen-doped graphene aerogel matrix (NGA) can significantly enhance the CO₂RR performance of bismuth nanoplates (BiNPs) by both modulating the electronic structure of bismuth and regulating the interface for chemical reaction and mass transfer environments. In particular, the NGA prepared by reducing graphene oxide (GO) with hydrazine hydrate (denoted as NGA_hdrz) exhibits significantly enhanced strong metal–support interaction (SMSI), increased specific surface area, strengthened CO₂ adsorption, and modulated wettability. As a result, the Bi/NGA_hdrz exhibits significantly boosted CO₂RR properties, with a Faradaic efficiency (FE) of 96.4% at a current density of 51.4 mA cm^–2 for formate evolution at a potential of −1.0 V versus reversible hydrogen electrode (vs RHE) in aqueous solution under ambient conditions.