Curved interface-induced Jahn-Teller effect in single-atom catalysts for water purification

Area of Science:

• Catalysis
• Environmental Science
• Materials Science

Background:

• Single-atom catalysts (SACs) offer efficient water purification via advanced oxidation processes (AOPs).
• Understanding intrinsic mechanisms and interface effects in SACs remains a challenge for optimizing AOPs.
• Jahn-Teller (J-T) effects in metal-nitrogen-carbon (M-N4-C) sites influence catalytic activity.

Purpose of the Study:

• To precisely control the Jahn-Teller (J-T) effect in M-N4-C single-atom catalysts.
• To enhance the efficiency of advanced oxidation processes (AOPs) for water purification.
• To investigate the relationship between J-T effect modulation and reactive oxygen species production.

Main Methods:

• Synthesis and characterization of M-N4-C single-atom catalysts (M = Mn, Fe, Co, Ni).
• Experimental investigation of peroxymonosulfate activation and catalytic performance.
• Theoretical calculations (e.g., DFT) to elucidate reaction mechanisms and electronic structure.

Main Results:

• A volcano-fit-like relationship was observed between J-T effect intensity and AOP performance.
• Controlled J-T effects modulated the adsorption of peroxymonosulfate and weakened d-p orbital hybridization.
• Catalysts demonstrated stable activity for 100 hours in a 20 L flow reactor, indicating scalability.

Conclusions:

• Precise control of the J-T effect in M-N4-C SACs is a viable strategy to boost AOP efficiency.
• Tuning metal d-orbital interactions is crucial for designing effective SACs for sustainable environmental remediation.
• The findings support the potential of SACs for large-scale industrial wastewater treatment.