Oxygen activation leading to the generation of reactive oxygen species(ROS)is essential for photocatalytic environmental remediation.The limited efficiency of O_(2)adsorption and reductive activation significantly lim...Oxygen activation leading to the generation of reactive oxygen species(ROS)is essential for photocatalytic environmental remediation.The limited efficiency of O_(2)adsorption and reductive activation significantly limits the production of ROS when employing C_(3)N_(4)for the degradation of emerging pollutants.Doping with metal single atoms may lead to unsatisfactory efficiency,due to the recombination of photogenerated electron-hole pairs.Here,Mn and S single atoms were introduced into C_(3)N_(4),resulting in the excellent photocatalytic performances.Mn/S-C_(3)N_(4)achieved 100%removal of bisphenol A,with a rate constant 11 times that of pristine C_(3)N_(4).According to the experimental results and theoretical simulations,Satoms restrict holes,facilitating the photo-generated carriers’separation.Single-atom Mn acts as the O_(2)adsorption site,enhancing the adsorption and activation of O_(2),resulting the generation of ROS.This study presents a novel approach for developing highly effective photocatalysts that follows a new mechanism to eliminate organic pollutants from water.展开更多
Advanced oxidation processes have been widely studied for organic pollutants treatment in water,but the degradation performance of radical-dominated pathway was severely inhibited by the side reactions between the ani...Advanced oxidation processes have been widely studied for organic pollutants treatment in water,but the degradation performance of radical-dominated pathway was severely inhibited by the side reactions between the anions and radicals,especially in high salinity conditions.Here,a singlet oxygen(^(1)O_(2))-dominated non-radical process was developed for organic pollutants degradation in high salinity wastewater,with layered crednerite(CuMnO_(2))as catalysts and peroxymonosulfate(PMS)as oxidant.Based on the experiments and density functional theory calculations,^(1)O_(2)was the dominating reactive species and the constructed Cu-O-Mn with electron-deficient Mn captured electron from PMS promoting the generation of^(1)O_(2).The rapid degradation of bisphenol A(BPA)was achieved by CuMnO_(2)/PMS system,which was 5-fold and 21-fold higher than that in Mn_(2)O_(3)/PMS system and Cu_(2)O/PMS system.The CuMnO_(2)/PMS system shown prominent BPA removal performance under high salinity conditions,prominent PMS utilization efficiency,outstanding total organic carbon removal rate,wide range of applicable pH and good stability.This work unveiled that the^(1)O_(2)-dominated non-radical process of CuMnO_(2)/PMS system overcame the inhibitory effect of anions in high salinity conditions,which provided a promising technique to remove organic pollutants from high saline wastewater.展开更多
基金supported by the Key Research&Developmental Programof Shandong Province(No.2021CXGC011202)the National Natural Science Foundation of China(Nos.22276110 and 22106088)the Fundamental Research Funds of Shandong University(No.zy202102).
文摘Oxygen activation leading to the generation of reactive oxygen species(ROS)is essential for photocatalytic environmental remediation.The limited efficiency of O_(2)adsorption and reductive activation significantly limits the production of ROS when employing C_(3)N_(4)for the degradation of emerging pollutants.Doping with metal single atoms may lead to unsatisfactory efficiency,due to the recombination of photogenerated electron-hole pairs.Here,Mn and S single atoms were introduced into C_(3)N_(4),resulting in the excellent photocatalytic performances.Mn/S-C_(3)N_(4)achieved 100%removal of bisphenol A,with a rate constant 11 times that of pristine C_(3)N_(4).According to the experimental results and theoretical simulations,Satoms restrict holes,facilitating the photo-generated carriers’separation.Single-atom Mn acts as the O_(2)adsorption site,enhancing the adsorption and activation of O_(2),resulting the generation of ROS.This study presents a novel approach for developing highly effective photocatalysts that follows a new mechanism to eliminate organic pollutants from water.
基金supported by the Open Fund of Guangdong Provincial Key Laboratory of Solid Wastes Pollution Control and Recycling (No.2020B121201003)the National Natural Science Foundation of China (Nos.21876099,22106088,and 22276110)+1 种基金the Key Research&Developmental Program of Shandong Province (No.2021CXGC011202)the Fundamental Research Funds of Shandong University (No.zy202102)。
文摘Advanced oxidation processes have been widely studied for organic pollutants treatment in water,but the degradation performance of radical-dominated pathway was severely inhibited by the side reactions between the anions and radicals,especially in high salinity conditions.Here,a singlet oxygen(^(1)O_(2))-dominated non-radical process was developed for organic pollutants degradation in high salinity wastewater,with layered crednerite(CuMnO_(2))as catalysts and peroxymonosulfate(PMS)as oxidant.Based on the experiments and density functional theory calculations,^(1)O_(2)was the dominating reactive species and the constructed Cu-O-Mn with electron-deficient Mn captured electron from PMS promoting the generation of^(1)O_(2).The rapid degradation of bisphenol A(BPA)was achieved by CuMnO_(2)/PMS system,which was 5-fold and 21-fold higher than that in Mn_(2)O_(3)/PMS system and Cu_(2)O/PMS system.The CuMnO_(2)/PMS system shown prominent BPA removal performance under high salinity conditions,prominent PMS utilization efficiency,outstanding total organic carbon removal rate,wide range of applicable pH and good stability.This work unveiled that the^(1)O_(2)-dominated non-radical process of CuMnO_(2)/PMS system overcame the inhibitory effect of anions in high salinity conditions,which provided a promising technique to remove organic pollutants from high saline wastewater.
