The ubiquity of refractory organic matter in aquatic environments necessitates innovative removal strategies.Sulfate radical-based advanced oxidation has emerged as an attractive solution,offering high selectivity,end...The ubiquity of refractory organic matter in aquatic environments necessitates innovative removal strategies.Sulfate radical-based advanced oxidation has emerged as an attractive solution,offering high selectivity,enduring efficacy,and anti-interference ability.Among many technologies,sulfite activation,leveraging its cost-effectiveness and lower toxicity compared to conventional persulfates,stands out.Yet,the activation process often relies on transition metals,suffering from low atom utilization.Here we introduce a series of single-atom catalysts(SACs)employing transition metals on g-C_(3)N_(4)substrates,effectively activating sulfite for acetaminophen degradation.We highlight the superior performance of Fe/CN,which demonstrates a degradation rate constant significantly surpassing those of Ni/CN and Cu/CN.Our investigation into the electronic and spin polarization characteristics of these catalysts reveals their critical role in catalytic efficiency,with oxysulfur radical-mediated reactions predominating.Notably,under visible light,the catalytic activity is enhanced,attributed to an increased generation of oxysulfur radicals and a strengthened electron donation-back donation dynamic.The proximity of Fe/CN's d-band center to the Fermi level,alongside its high spin polarization,is shown to improve sulfite adsorption and reduce the HOMO-LUMO gap,thereby accelerating photo-assisted sulfite activation.This work advances the understanding of SACs in environmental applications and lays the groundwork for future water treatment technologies.展开更多
基金Financial support from the National Natural Science Foundation of China(52270068)the open Project of the State Key Laboratory of Urban Water Resource and Environment,Harbin Institute of Technology(QG202225)+1 种基金the Heilongjiang Touyan Innovation Team Program was highly appreciatedWe would also like to thank Dr.Shibo Xi of Singapore Synchrotron Light Source for his help in catalyst characterization.
文摘The ubiquity of refractory organic matter in aquatic environments necessitates innovative removal strategies.Sulfate radical-based advanced oxidation has emerged as an attractive solution,offering high selectivity,enduring efficacy,and anti-interference ability.Among many technologies,sulfite activation,leveraging its cost-effectiveness and lower toxicity compared to conventional persulfates,stands out.Yet,the activation process often relies on transition metals,suffering from low atom utilization.Here we introduce a series of single-atom catalysts(SACs)employing transition metals on g-C_(3)N_(4)substrates,effectively activating sulfite for acetaminophen degradation.We highlight the superior performance of Fe/CN,which demonstrates a degradation rate constant significantly surpassing those of Ni/CN and Cu/CN.Our investigation into the electronic and spin polarization characteristics of these catalysts reveals their critical role in catalytic efficiency,with oxysulfur radical-mediated reactions predominating.Notably,under visible light,the catalytic activity is enhanced,attributed to an increased generation of oxysulfur radicals and a strengthened electron donation-back donation dynamic.The proximity of Fe/CN's d-band center to the Fermi level,alongside its high spin polarization,is shown to improve sulfite adsorption and reduce the HOMO-LUMO gap,thereby accelerating photo-assisted sulfite activation.This work advances the understanding of SACs in environmental applications and lays the groundwork for future water treatment technologies.
