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 NGAhdrz) exhibits significantly enhanced strong metal–support
interaction (SMSI), increased specific surface area, strengthened
CO2 adsorption, and modulated wettability. As a result,
the Bi/NGAhdrz 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.