The
discharge of organic pollutants threatens the environment and health
and is also a waste of organic energy. Here, the reduction state Cu
(RSC) species-doped carbon–nitrogen–oxygen polymer (RSC-CNOP)
is synthesized from high-temperature polymerization of a Cu-polyimide
precursor, which is used as a Fenton-like catalyst and exhibits excellent
performance for pollutant degradation, accompanied by the utilization
of the electron energy of the pollutants. Experiments and theoretical
calculations reveal the promotion mechanism. The formed Cu(RSC)–O–C(π)
electron-transfer bridges in RSC-CNOP induce the bidirectional electron
transfers from RSC to O and from C(π) to O (RSC → O ←
π), forming the polarized reaction micro-areas (reinforced electron-rich
O microcenters and electron-poor C(π) microcenters). The free
electrons in electron-rich centers of RSC-CNOP are as many as ∼8
times that of the pure CNOP sample from the electron paramagnetic
resonance measurement. Pollutants are oxidized by supplying electrons
to electron-poor microcenters, and H2O2 can
be selectively reduced to •OH (also destruct pollutants)
in the electron-rich microcenter over RSC-CNOP. This work reveals
that the energy and electrons of pollutants can be efficiently utilized
in the Fenton-like system through constructing and reinforcing the
polarized dual reaction microcenters.
Dual reaction centers are formed between C–O–Cu bonding bridges of Cu-MP NCs owing to cation–π interactions. H2O2 is reduced to ˙OH on electron-rich Cu centers, while pollutants are degraded on electron-deficient centers.
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