Synergistic Physicochemical Effect of Neighboring Atoms in Nano Hollow Multishelled Structure: A Platform for Breaking the Activity-Stability Imbalance

Abstract

Modulation of surface curvature and intershell neighboring-atom physicochemical synergy empowers nano hollow multishelled structure (HoMS) curved-surface single-atom catalysts (CS SACs) to overcome the inherent activity-stability trade-off of conventional SACs. This mini-review summarizes three fabrication strategies for curved carbon supports, focusing on in-situ templated HoMS construction and multishelled neighbor atomic synergy. Different from classic single-layer curved single-atom catalysts, the hierarchical curved interfaces of HoMS realize cooperative regulation between inner single atoms and neighbor outer-shell heteroatoms via electrostatic repulsion, breaking Gibbs free-energy scaling relations and adsorption/desorption limitation to simultaneously optimize catalytic activity and durability. Recent progress of CS SACs in oxygen reduction reaction (ORR), nitrogen reduction reaction (NRR), carbon dioxide reduction reaction (CO₂RR) and hydrogen evolution reaction (HER) is overviewed. We elaborate that substrate curvature optimizes intermediate adsorption behaviors via modulating the electronic configuration, lattice strain and local interfacial electric field surrounding isolated metal active sites. Most importantly, existing limitations and future directions targeting precise HoMS engineering are highlighted to guide the rational design of high-performance single-atom electrocatalysts.

Keywords

Hollow multishelled structure / Single-atom catalyst / Curvature effect / Structure-activity relationship / Adsorption/desorption limitation

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