Design of highly efficient catalysts guided by redox of individual carbon supports

Abstract

The precise design of highly efficient nanocatalysts with traditional ensemble methodologies faces a challenge. Here, we demonstrate the first precise guidance of basic research on carbon supports at the single-particle level for designing Pt/C nanoelectrocatalysts. With single-molecule fluorescence microscopy to measure redox electron transfer (ET) rates on individual graphene sheets (GSs), we reveal that the reductive ET rate increases with the thickness decrease of GSs, while the oxidative ET increases with the thickness decrease first and reaches a constant on thinner GSs. Notably, O=C-OH accelerates reductive ET while slowing oxidative ET. All these insights are further confirmed on carbon nanospheres. Guided by these unprecedented insights, two high-efficiency Pt/C nanoelectrocatalysts for the hydrogen evolution reaction and hydrogen oxidation reaction are designed. Compared to traditional ensemble methods, our single-particle-level research on carbon supports provides a deeper understanding of the support effect, enabling precise nanocatalyst design and reducing unnecessary research and development costs.