General synthesis of single-atom catalysts with high metal loading using graphene quantum dots

Transition-metal single-atom catalysts present extraordinary activity per metal atomic site, but suffer from low metal-atom densities (typically less than 5 wt% or 1 at.%), which limits their overall catalytic performance. Here we report a general method for the synthesis of single-atom catalysts with high transition-metal-atom loadings of up to 40 wt% or 3.8 at.%, representing several-fold improvements compared to benchmarks in the literature. Graphene quantum dots, later interweaved into a carbon matrix, were used as a support, providing numerous anchoring sites and thus facilitating the generation of high densities of transition-metal atoms with sufficient spacing between the metal atoms to avoid aggregation. A significant increase in activity in electrochemical CO2 reduction (used as a representative reaction) was demonstrated on a Ni single-atom catalyst with increased Ni loading.

Automated summary

A general method was reported for synthesizing single-atom catalysts with high transition-metal-atom loadings, showing significant improvements compared to benchmarks in the literature. The use of graphene quantum dots interwoven into a carbon matrix provided anchoring sites for high densities of transition-metal atoms without aggregation. An increase in activity was demonstrated in electrochemical CO2 reduction on a Ni single-atom catalyst with increased Ni loading.