Porosity-Triggered Efficient Single-Atom Catalysis in Two-Dimensional Materials

Area of Science:

• Materials Science
• Catalysis
• Nanotechnology

Background:

• Single-atom catalysts (SACs) offer high atom utilization and activity but suffer from thermal instability and sintering.
• Conventional 3D frameworks like MOFs have limitations in pore control and conductivity, impacting catalytic efficiency.

Purpose of the Study:

• To introduce a novel lattice confinement strategy using engineered 2D porous monolayers for stabilizing SACs.
• To design and identify stable 2D hosts with intrinsic sub-nanometer pores for enhanced quantum confinement effects.

Main Methods:

• Utilized first-principles calculations to screen 224 candidate materials.
• Designed 2D porous monolayers based on the "superatom" concept.
• Evaluated catalytic performance for the hydrogen evolution reaction.

Main Results:

• Identified stable 2D hosts with diverse electronic properties capable of strong quantum confinement.
• Demonstrated superior catalytic performance for SACs anchored on 2D monolayers compared to conventional doped architectures.
• Showcased precise electronic control over catalytic properties through active-site charge redistribution.

Conclusions:

• Established a viable and electronically robust strategy for designing next-generation single-atom catalysts.
• Highlighted the potential of engineered 2D porous monolayers for overcoming SAC instability and enhancing catalytic efficiency.
• Emphasized the role of quantum confinement and localized electronic control in tailoring catalyst performance.