Tuning Mass Transport in Electrocatalysis Down to Sub-5 nm through Nanoscale Grade Separation

Angew Chem Int Ed Engl. 2023 Jan 16;62(3):e202212653. doi: 10.1002/anie.202212653. Epub 2022 Dec 12.

Abstract

Nano and single-atom catalysis open new possibilities of producing green hydrogen (H2 ) by water electrolysis. However, for the hydrogen evolution reaction (HER) which occurs at a characteristic reaction rate proportional to the potential, the fast generation of H2 nanobubbles at atomic-scale interfaces often leads to the blockage of active sites. Herein, a nanoscale grade-separation strategy is proposed to tackle mass-transport problem by utilizing ordered three-dimensional (3d) interconnected sub-5 nm pores. The results reveal that 3d criss-crossing mesopores with grade separation allow efficient diffusion of H2 bubbles along the interconnected channels. After the support of ultrafine ruthenium (Ru), the 3d mesopores are on a superior level to two-dimensional system at maximizing the catalyst performance and the obtained Ru catalyst outperforms most of the other HER catalysts. This work provides a potential route to fine-tuning few-nanometer mass transport during water electrolysis.

Keywords: Hydrogen Evolution Reaction; Mass Transport; Nanocatalysis; Ordered Mesoporous Structure; Single-Atom Catalysis.