Vacuum ultraviolet(VUV) photolysis is recognized as an environmental-friendly treatment process. Nitrate(NO-3) and natural organic matter(NOM) are widely present in water source.We investigated trichloronitromethane(T...Vacuum ultraviolet(VUV) photolysis is recognized as an environmental-friendly treatment process. Nitrate(NO-3) and natural organic matter(NOM) are widely present in water source.We investigated trichloronitromethane(TCNM) formation during chlorination after VUV photolysis, because TCNM is an unregulated highly toxic disinfection byproduct. In this study:(1) we found reactive nitrogen species that is generated under VUV photolysis of NO-3react with organic matter to form nitrogen-containing compounds and subsequently form TCNM during chlorination;(2) we found the mere presence of 0.1 mmol/L NO-3can result in the formation of up to 63.96 μg/L TCNM;(3) we found the changes in pH(6.0-8.0), chloride(1-4 mmol/L), and bicarbonate(1-4 mmol/L) cannot effectively diminish TCNM formation;and,(4) we established the quantitative structure-activity relationship(QSAR) model,which indicated a linear relationship between TCNM formation and the Hammett constant(σ) of model compounds;and,(5) we characterized TCNM precursors in water matrix after VUV photolysis and found 1161 much more nitrogen-containing compounds with higher aromaticity were generated. Overall, this study indicates more attention should be paid to reducing the formation risk of TCNM when applying VUV photolysis process at scale.展开更多
Hierarchical carbon material is used as a star cocatalyst in the field of photocatalysis due to its excellent catalytic properties. In this work, mesoporous carbon nitride sheet(MCNS) photocatalyst introduced nitrogen...Hierarchical carbon material is used as a star cocatalyst in the field of photocatalysis due to its excellent catalytic properties. In this work, mesoporous carbon nitride sheet(MCNS) photocatalyst introduced nitrogen-doped hollow carbon spheres assembled with cobalt nanoparticles(Co@NHC) is synthesized by electrostatic adsorption. A series of characterizations are analyzed to display the structures, morphologies and optical properties of as-prepared materials. The photocatalytic activity of Co@NHC/MCNS material is evaluated with hydrogen evolution under visible light irradiation. The results indicate that 5 wt%Co@NHC/MCNS material reveals higher photocatalytic activity of hydrogen evolution rate of 3675 μmol/g with 4 h reaction time, which is 159 times than that of pure MCNS material. The carbon material with excellent charge transport properties can effectively accelerate the charge transfer from ultrathin MCNS to cobalt nanoparticles. The goal of improving the photocatalytic performance of Co@NHC/MCNS material is achieved. As a result, it provides a feasible and promised approach for doping transition metals to enhance photocatalytic activity.展开更多
Pre-oxidation has been reported to be an effective way to remove algal cells in water, but the released algal organic matter (AOM) could be oxidized and lead to the increment in disinfection by-product (DBP) formation...Pre-oxidation has been reported to be an effective way to remove algal cells in water, but the released algal organic matter (AOM) could be oxidized and lead to the increment in disinfection by-product (DBP) formation. The relationship between pre-oxidation and AOM-derived DBP formation needs to be approached more precisely. This study compared the impact of four pre-oxidants, ozone (O), chlorine dioxide (ClO), potassium permanganate(KMnO) and sodium hypochlorite (NaClO), on the formation of nitrogenous (N-) and carbonaceous (C-) DBPs in AOM chlorination. The characterization (fluorescent properties,molecular weight distribution and amino acids concentration) on AOM samples showed that the characterization properties variations after pre-oxidation were highly dependent on the oxidizing ability of oxidants. The disinfection experiments showed that Oincreased DBP formation most significantly, which was consistent with the result of characterization properties variations. Then canonical correspondent analysis (CCA) and Pearson’s correlation analysis were conducted based on the characterization data and DBP formation. CCA indicated that C-DBPs formation was highly dependent on fluorescent data. The formation of haloacetic acids (HAAs) had a positive correlation with aromatic protein-like component while trichloromethane (TCM) had a positive correlation with fulvic acid-like component.Pearson’s correlation analysis showed that low molecular weight fractions were favorable to form N-DBPs. Therefore, characterization data could provide the advantages in the control of DBP formation, which further revealed that KMnOand ClOwere better options for removing algal cells as well as limiting DBP formation.展开更多
基金supported by Natural Science Foundation of Hunan Province (No. 2021JJ40066)National Natural Science Foundation (Nos. 51878257 and 52100007).
文摘Vacuum ultraviolet(VUV) photolysis is recognized as an environmental-friendly treatment process. Nitrate(NO-3) and natural organic matter(NOM) are widely present in water source.We investigated trichloronitromethane(TCNM) formation during chlorination after VUV photolysis, because TCNM is an unregulated highly toxic disinfection byproduct. In this study:(1) we found reactive nitrogen species that is generated under VUV photolysis of NO-3react with organic matter to form nitrogen-containing compounds and subsequently form TCNM during chlorination;(2) we found the mere presence of 0.1 mmol/L NO-3can result in the formation of up to 63.96 μg/L TCNM;(3) we found the changes in pH(6.0-8.0), chloride(1-4 mmol/L), and bicarbonate(1-4 mmol/L) cannot effectively diminish TCNM formation;and,(4) we established the quantitative structure-activity relationship(QSAR) model,which indicated a linear relationship between TCNM formation and the Hammett constant(σ) of model compounds;and,(5) we characterized TCNM precursors in water matrix after VUV photolysis and found 1161 much more nitrogen-containing compounds with higher aromaticity were generated. Overall, this study indicates more attention should be paid to reducing the formation risk of TCNM when applying VUV photolysis process at scale.
基金financially supported by the National Natural Science Foundation of China (Nos. 22008095, 22108106, 22075113, 22108110)the Special China Postdoctoral Science Foundation (Nos. 2020TQ0127, 2020M680065)+4 种基金Jiangsu Province Postdoctoral Science Foundation (No. 2021K396C)Key Laboratory of Electrochemical Energy Storage and Energy Conversion of Hainan Province (No. KFKT2021006)Jiangsu Funds for Distinguished Young Scientists (No. BK20190045)Natural Science Foundation of Jiangsu Province (No. BK20190981)Basic and Applied Basic Research Fund Project of Guangdong Province (No. 2019A1515111020)。
文摘Hierarchical carbon material is used as a star cocatalyst in the field of photocatalysis due to its excellent catalytic properties. In this work, mesoporous carbon nitride sheet(MCNS) photocatalyst introduced nitrogen-doped hollow carbon spheres assembled with cobalt nanoparticles(Co@NHC) is synthesized by electrostatic adsorption. A series of characterizations are analyzed to display the structures, morphologies and optical properties of as-prepared materials. The photocatalytic activity of Co@NHC/MCNS material is evaluated with hydrogen evolution under visible light irradiation. The results indicate that 5 wt%Co@NHC/MCNS material reveals higher photocatalytic activity of hydrogen evolution rate of 3675 μmol/g with 4 h reaction time, which is 159 times than that of pure MCNS material. The carbon material with excellent charge transport properties can effectively accelerate the charge transfer from ultrathin MCNS to cobalt nanoparticles. The goal of improving the photocatalytic performance of Co@NHC/MCNS material is achieved. As a result, it provides a feasible and promised approach for doping transition metals to enhance photocatalytic activity.
基金supported by the National Natural Science Foundation (Nos. 51878257, 52100007)the Natural Science Foundation of Hunan Province (No. 2021JJ40066) and the Natural Science Foundation of Hunan Province (No. 2021JJ40106)。
文摘Pre-oxidation has been reported to be an effective way to remove algal cells in water, but the released algal organic matter (AOM) could be oxidized and lead to the increment in disinfection by-product (DBP) formation. The relationship between pre-oxidation and AOM-derived DBP formation needs to be approached more precisely. This study compared the impact of four pre-oxidants, ozone (O), chlorine dioxide (ClO), potassium permanganate(KMnO) and sodium hypochlorite (NaClO), on the formation of nitrogenous (N-) and carbonaceous (C-) DBPs in AOM chlorination. The characterization (fluorescent properties,molecular weight distribution and amino acids concentration) on AOM samples showed that the characterization properties variations after pre-oxidation were highly dependent on the oxidizing ability of oxidants. The disinfection experiments showed that Oincreased DBP formation most significantly, which was consistent with the result of characterization properties variations. Then canonical correspondent analysis (CCA) and Pearson’s correlation analysis were conducted based on the characterization data and DBP formation. CCA indicated that C-DBPs formation was highly dependent on fluorescent data. The formation of haloacetic acids (HAAs) had a positive correlation with aromatic protein-like component while trichloromethane (TCM) had a positive correlation with fulvic acid-like component.Pearson’s correlation analysis showed that low molecular weight fractions were favorable to form N-DBPs. Therefore, characterization data could provide the advantages in the control of DBP formation, which further revealed that KMnOand ClOwere better options for removing algal cells as well as limiting DBP formation.