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<p>The spin-forbidden effect and high bond energy of molecular oxygen (O<sub>2</sub>) pose a fundamental challenge for its activation in wastewater treatment. We address this by constructing an atomically dispersed Fe-Mn dual-site catalyst (Fe<sub>0.1</sub>-Mn-350), which overcomes the sluggish O<sub>2</sub> kinetics of monometallic oxides and the aqueous instability of conventional single-atom catalysts. This catalyst enables complete degradation of 20 mg/L parachlormetaxylenol (PCMX) within 15 minutes, with a reaction rate (0.2205 min<sup>−1</sup>) 25 times greater than MnO<sub>2</sub> and surpassing benchmark catalysts. Experimental and theoretical analyses reveal that the preferential side-on O<sub>2</sub> adsorption at Fe sites of Fe<sub>0.1</sub>-Mn-350 significantly reduces activation barriers by 38% (versus Fe-CNTs by 15%, Co-MnO<sub>2</sub> by 25%), and triggers a dual-pathway mechanism involving both radical (<sup>•</sup>OH, O<sub>2</sub><sup>•−</sup>) and non-radical (<sup>1</sup>O<sub>2</sub>, Fe(IV)) species. Crucially, the Fe<sub>0.1</sub>-Mn-350/O<sub>2</sub> system demonstrates robust practicality, maintaining 98% efficiency in real hospital wastewater, stable operation in a 12-h continuous-flow reactor, and a low operational cost of 0.28 USD/m<sup>3</sup>. The technology’s environmental sustainability is further validated by a remarkable 80% recovery of zebrafish embryo hatchability and a 93% reduction in developmental toxicity. This work provides a green and economically viable strategy for the destructive treatment of persistent halogenated contaminants in water.</p>

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Molecular oxygen activation by atomic Fe-moieties on MnO2 for enhanced remediation of parachlormetaxylenol wastewater

  • 期刊论文

  • 发表日期：

    2026年3月25日

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  • Huiji Xiao,
  • Wenli Zhang,
  • Chenxi Zhu,
  • Kewei Lv,
  • Yun Wang,
  • Bing Xie,
  • Xiaoming Zou,
  • Xubiao Luo,
  • Yanbo Zhou

摘要

The spin-forbidden effect and high bond energy of molecular oxygen (O2) pose a fundamental challenge for its activation in wastewater treatment. We address this by constructing an atomically dispersed Fe-Mn dual-site catalyst (Fe0.1-Mn-350), which overcomes the sluggish O2 kinetics of monometallic oxides and the aqueous instability of conventional single-atom catalysts. This catalyst enables complete degradation of 20 mg/L parachlormetaxylenol (PCMX) within 15 minutes, with a reaction rate (0.2205 min−1) 25 times greater than MnO2 and surpassing benchmark catalysts. Experimental and theoretical analyses reveal that the preferential side-on O2 adsorption at Fe sites of Fe0.1-Mn-350 significantly reduces activation barriers by 38% (versus Fe-CNTs by 15%, Co-MnO2 by 25%), and triggers a dual-pathway mechanism involving both radical (•OH, O2•−) and non-radical (1O2, Fe(IV)) species. Crucially, the Fe0.1-Mn-350/O2 system demonstrates robust practicality, maintaining 98% efficiency in real hospital wastewater, stable operation in a 12-h continuous-flow reactor, and a low operational cost of 0.28 USD/m3. The technology’s environmental sustainability is further validated by a remarkable 80% recovery of zebrafish embryo hatchability and a 93% reduction in developmental toxicity. This work provides a green and economically viable strategy for the destructive treatment of persistent halogenated contaminants in water.