Abstract

The electrocatalytic reduction of CO2 to produce formic acid is gaining prominence as a critical technology in the pursuit of carbon neutrality. Nonetheless, it remains challenging to attain both substantial formic acid production and high stability across a wide voltage range, particularly when utilizing bismuth-based catalysts. Herein, we present a novel graphene quantum dot-mediated synthetic strategy to achieve the uniform deposition of highly dispersed bismuth nanoparticles on porous graphene. This innovative design achieves an elevated faradaic efficiency for formate of 87.0% at -1.11 V vs. RHE with high current density and long-term stability. When employing a flow cell, a maximum FEformate of 80.0% was attained with a total current density of 156.5 mA cm-2. The exceptional catalytic properties can be primarily attributed to the use of porous graphene as the support and the auxiliary contribution of graphene quantum dots, which enhance the dispersion of bismuth nanoparticles. This improved dispersion, in turn, has a significantly positive impact on CO2 activation and the generation of *HCOO intermediates to facilitate the formation of formate. This work presents a straightforward technique to create uniform metal nanoparticles on carbon materials for advancing various electrolytic applications.

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