Herein, the decontamination performance and likelihood
of a shift
in the reaction mechanism of CuO-activated percarbonate (SPC) in the
presence of ascorbic acid (AA) (i.e., CuO/SPC/AA process) under varying
pH conditions were explored. Experimental results revealed that sulfamethazine
(SMT) could be well degraded over a wide pH range (3.0–9.0).
Mechanistic investigations suggested that the hydroxyl radical (•OH) was the major reactive oxygen species (ROS) at
acidic pH, whereas Cu(III) played a dominant role in SMT degradation
at neutral and alkaline pHs. Alternatively, •OH
was determined to be the secondary reactive species generated from
the hydrolysis of Cu(III) at neutral and alkaline pHs. Moreover, the
role of AA and coexisting Na2CO3 was explored.
It was concluded that the regeneration of Cu(I) played an important
role in mediating the copper redox cycle under all of the studied
pHs, which mainly benefited from reductive AA, and the available superoxide
radical (O2
•–) and deprotonated
form of H2O2 could also contribute to this process
at neutral and alkaline pHs. The coexisting Na2CO3 exerted a negligible impact on SMT degradation at acidic and neutral
pHs, while a slight inhibitive effect was observed at alkaline pH.
Simultaneously, the potential practicability of the CuO/SPC/AA process
was evaluated. This work deepens the understanding of copper-catalyzed
heterogeneous activation of percarbonate, widening the application
of the reductant for water decontamination.