Boosting photocatalytic water splitting of polymeric C$_{60}$ by reduced dimensionality from 2D monolayer to 1D chain

Recent synthesis of 2D fullerene networks [$Nature$ 606, 507 (2022) & $Nature$ 613, 71 (2023)] provides new opportunities for photovoltaics and photocatalysis because of their versatile crystal structures for further tailoring of electronic, optical and chemical function. To shed light on the structural aspects of photocatalytic water splitting performance of fullerene nanomaterials, we compare the photocatalytic properties of individual polymeric fullerene chains and monolayer fullerene networks from first principles calculations. It is found that the photocatalytic efficiency can be further optimised by reducing dimensionality from 2D to 1D. The conduction band edge of the polymeric C$_{60}$ chain provides a much higher external potential for the hydrogen reduction reaction than its monolayer counterparts over a wider range of pH values, and the surface active sites in the 1D chain are two times more than those in the 2D networks from a thermodynamic perspective. These observations render the 1D fullerene polymer a more promising candidate as a photocatalyst for the hydrogen evolution reaction than monolayer fullerene networks.