Iron single atoms and nitrogen vacancies on graphitic carbon nitride synergically shallowing deep electron traps towards efficient photocatalytic ozonation

[Display omitted] •Fe-CNV catalysts demonstrate excellent performance in photocatalytic ozonation.•Nvs exhibit opposite effect to photocatalytic activity with or without iron SAs.•Iron SAs shallow deep electron traps caused by Nvs at atomic level.•Coupling iron SAs and adjacent Nvs enrich surface charges around active sites. The coupling of photocatalysis and ozonation has been approved a very efficient strategy for hydroxyl radicals (•OH) production and wastewater decontamination, yet it remains challenging to enrich surface-reaching charges around reaction centers to accelerate this process. This paper explored the strategy of single-atoms (SAs) modification and defects control, aiming to enhance the activity of graphite carbon nitride (CN) in the visible light photocatalytic ozonation. It was found that the presence of iron SAs on CN greatly altered the impact of nitrogen vacancies (NVs), which behaved as recombination centers of photogenerated charge carriers and deteriorated activity of CN, while positively promoting the separation and migration of photogenerated carriers in the case for Fe-CNV (consist of iron SAs and NVs) catalysts. Based on photoluminescence (PL) emission, time-resolved PL spectra, ultrafast transient absorption spectroscopy and first-principles calculations, we found that adjacent iron SAs revived electrons trapped at NVs by elevating their energy level and mediating their interfacial transfer, leading to the decreased loss during electron transfer. This finding demonstrates the feasible tailor of energy level alignment for defect states to shallow deep electron traps.