Nanochanneling and Local Crystallization Engineering Accelerate Multiphase Single-Atom Catalysis for Rapid Water...

Area of Science:

• Materials Science
• Catalysis
• Environmental Chemistry

Background:

• Designing single-atom catalysts (SACs) with hierarchical structures for multiphase reactions is challenging.
• Optimizing the local chemical environment is crucial for efficient catalytic processes.

Purpose of the Study:

• To develop a universal strategy for synthesizing channel-digging microspherical SACs.
• To enhance gas-liquid-solid mass transfer and tune the thermodynamics of catalytic ozonation.

Main Methods:

• Catalytically graphitizing carbon microspheres and etching amorphous carbon via mild combustion.
• Fabricating cross-linked hierarchical graphitic nanochannels confining transition metal single atoms (TMCSs-Air).
• Investigating ozone (O3) adsorption configuration and activation barriers.

Main Results:

• Nanoenvironment engineering increased interfacial ozone mass transfer by 3.2-fold.
• Ozone adsorption shifted to a bidental "side-on" configuration, lowering activation barriers.
• CoCSs-Air catalyst showed 3.6-fold higher ozone utilization and 4.2-fold greater turnover frequency (1580 min⁻¹).

Conclusions:

• TMCSs-Air nanoreactors effectively enhance multiphase heterogeneous catalysis by overcoming gas diffusion limitations.
• The developed catalysts show significant potential for treating real-world petrochemical wastewater.
• This strategy offers a pathway for precise engineering of SACs for diverse catalytic applications.