Pair-Resolved Fe-M Dual-Atom Catalysts for Programmed PMS Activation: Mechanisms, Membrane Confinement, and...

Area of Science:

• Advanced oxidation processes
• Catalysis
• Environmental chemistry

Background:

• Peroxymonosulfate (PMS) activation is crucial for water remediation.
• Fe-based dual-atom catalysts (Fe-M DACs) offer tunable catalytic properties.
• Controlling radical vs. non-radical pathways is key for efficient pollutant degradation.

Purpose of the Study:

• To review recent advancements in Fe-M DACs for PMS activation.
• To elucidate the structure-activity relationships governing pathway selectivity.
• To provide design principles for targeting diverse pollutants in complex water matrices.

Main Methods:

• Pair-resolved analysis of Fe-M DACs (Fe-Co, Fe-Mo, Fe-Fe, Fe-Ni).
• Investigation of µ-peroxo bridging and spin/electronic coupling effects.
• Case study using Bisphenol A (BPA) degradation and membrane-confined systems.

Main Results:

• Fe-M DACs enable programmable switching between radical and non-radical PMS activation routes.
• Metal identity dictates pathway bifurcation (e.g., phenoxy-radical/ETP vs. hydroxylation).
• Membrane confinement enhances catalyst stability and separation in challenging effluents.

Conclusions:

• Fe-M DACs establish an atom-level "catalyst-co-catalyst" paradigm for advanced oxidation.
• Design rules are proposed for targeting specific pollutants like antibiotics and emerging contaminants.
• Future strategies should focus on halogenated pollutants and complex contaminant mixtures.