A Universal Fenton‐Like Strategy for Selective Generation of 1 O 2 in Mixed Industrial Wastewater Treatment and Green Chemical Synthesis

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Abstract
Sustained and selective generation of singlet oxygen ( 1 O 2 ) in Fenton‐like catalytic systems is highly desirable for diverse applications, from freshwater resource management to green chemical synthesis. Despite advances in advanced oxidation processes, there remains a lack of generalizable methods that reliably modulate 1 O 2 selectivity. Here, we propose a descriptor‐assisted coordination modulation strategy, in which machine‐learning analysis identifies the d‐band center as an important electronic descriptor associated with 1 O 2 selectivity. Through N‐coordination modulation, the CoN 5 catalyst exhibited near‐complete 1 O 2 selectivity among the quantified reactive oxygen species (ROS) with a steady‐state concentration of 394 µM, outperforming recent reports. As an internal‐circulation pre‐oxidation module, the CoN 5 /peroxymonosulfate (CoN 5 /PMS) system continuously raised wastewater biochemical oxygen demand/chemical oxygen demand (BOD/COD) to above 0.5 over 192 h, increased bioavailable dissolved organic matter (DOM), and showed high microbiome compatibility, evidenced by reduced Vibrio fischeri inhibition and microbial diversity ordination clustering near the background with greater shared‐taxa overlap. This system also enabled selective thioanisole oxidation, achieving 90.6% conversion and 99.5% selectivity, with green synthesis potential demonstrated in a three‐chamber continuous single‐pass reactor. These results establish a generalizable coordination principle for steering ROS pathways and provide a deployable, low‐ecological‐risk route for both mixed wastewater treatment and green chemical synthesis.
Funding Information
  • National Natural Science Foundation of China (22225604)
  • National Natural Science Foundation of China (U24A20518)
  • National Natural Science Foundation of China (22422605)

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