Transition
metal catalysts are known to activate persulfate, but
the properties that govern the intrinsic activity of these catalysts
are still unknown. Here, we developed a series of catalysts with transition
metals anchored on carbon nanotubes (denoted M–N–CNTs,
where M = Co, Fe, Mn, or Ni) containing single-atom M–N moieties,
to activate peroxymonosulfate for the efficient nonradical oxidation
of sulfamethoxazole. The spin state of M–N–CNTs strongly
determined their catalytic activity. A large effective magnetic moment
with a high spin state (e.g., Co–N) favored the overlap of
d orbitals with oxygen-containing adsorbates (such as peroxo species)
on metal active sites and promoted electron transfer, which facilitated
peroxymonosulfate adsorption and enhanced the oxidation capacity of
the reactive species. These findings advance the mechanistic understanding
of transition metal-mediated persulfate activation and inform the
development of efficient spintronic catalysts for environmental applications.
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