Heteroatom-doping of carbocatalysts has been a powerful strategy to remarkably enhance the catalytic performance.Herein,the underlying nature of N promotional effects on peroxymonosulfate(PMS)activation for phenol rem...Heteroatom-doping of carbocatalysts has been a powerful strategy to remarkably enhance the catalytic performance.Herein,the underlying nature of N promotional effects on peroxymonosulfate(PMS)activation for phenol removal is understood by combining kinetics analysis with multiple techniques.A strategy using mixed acid oxidation of carbon nanotube(CNT)followed by NH3 treatment is employed to yield a series of catalysts with different N-doping contents but similar fraction of sp^(2)-hybridized carbon and defective degree,endowing with a chance to discriminate the dominant N-containing active sites.The multi-sites kinetics analysis suggests the graphitic N-containing sites as the dominant active sites.The mechanism of the surface-bound reactive species is also discriminated as the dominant reaction mechanism.The insights reported here could provide the methodology to fundamentally understand the heteroatom-doping effects of carbocatalysis.展开更多
Aromatic compounds such as phenols presented widely in coal chemical industry wastewater(CCW)render the treatment facing great challenge due to their biorefractory characteristics and potential risks to the environmen...Aromatic compounds such as phenols presented widely in coal chemical industry wastewater(CCW)render the treatment facing great challenge due to their biorefractory characteristics and potential risks to the environment and human health.Ozone-based advanced oxidation processes show promising for these pollutants removal,but the mineralization via ozonation alone is unsatisfactory and not cost-effective.Herein,a hybrid peroxi-coagulation/ozonation process(denoted as PCO)was developed using sacrificial iron plate as an anode and carbon black modified carbon felt as cathode in the presence of ozonation.An enhanced phenol removal of∼100%within 20 min and phenol mineralization of∼80%within 60 min were achieved with a low energy consumption of 0.35 kWh/g TOC.In this novel process,synergistic effect between ozonation and peroxi-coagulation was observed,and beside O_(3) direct oxidation,peroxone played a dominant role for phenol removal.In the PCO process,the hydrolyzed Fe species enhanced the generation of reactive oxygen species(ROS),while•OH was dominantly responsible for pollutant degradation.This process also illustrated high resistance to high ionic strength and better performance for TOC removal in real wastewater when compared with ozonation and peroxi-coagulation process.Therefore,this process is more cost-effective,being very promising for CCW treatment.展开更多
There is an urgent demand for tuning the selectivity and activity of the photocatalysts to remove coexistent pollutants simultaneously.Herein,we introduced the surficial activity sites into the bismuth oxybromide(Bi O...There is an urgent demand for tuning the selectivity and activity of the photocatalysts to remove coexistent pollutants simultaneously.Herein,we introduced the surficial activity sites into the bismuth oxybromide(Bi OBr),including the Bi/Bi-O defects and hetero Cu atoms,and then the higher photocatalytic activity and selectivity of BiOBr were realized for degradation phenol and ciprofloxacin(CIP).It can be found that the Bi/Bi-O defects played more important role in enhancing the photocatalytic activity for degradation of phenol,while the Cu atoms significantly improved the photocatalytic activity for removing CIP.Moreover,the heterogeneous Cu atoms as the activity sites excited the reaction between phenol and CIP even under dark condition and were beneficial for synchronously removing phenol and CIP.This work provides a feasible way for BiOX photocatalyst to remove co-existent pollutants and may have a practical application.展开更多
基金supported by the Natural Science Foundation of China(21922803 and 21776077)the Shanghai Natural Science Foundation(17ZR1407300 and 17ZR1407500)+3 种基金the China Postdoctoral Science Foundation(BX20190116)the Program for Professor of Special Appointment(Eastern Scholar)at Shanghai Institutions of Higher Learning,the Shanghai Rising-Star Program(17QA1401200)the State Key Laboratory of Organic-Inorganic Composites(oic-201801007)the Open Project of State Key Laboratory of Chemical Engineering(SKLChe-15C03 and SKL-ChE-16C05).
文摘Heteroatom-doping of carbocatalysts has been a powerful strategy to remarkably enhance the catalytic performance.Herein,the underlying nature of N promotional effects on peroxymonosulfate(PMS)activation for phenol removal is understood by combining kinetics analysis with multiple techniques.A strategy using mixed acid oxidation of carbon nanotube(CNT)followed by NH3 treatment is employed to yield a series of catalysts with different N-doping contents but similar fraction of sp^(2)-hybridized carbon and defective degree,endowing with a chance to discriminate the dominant N-containing active sites.The multi-sites kinetics analysis suggests the graphitic N-containing sites as the dominant active sites.The mechanism of the surface-bound reactive species is also discriminated as the dominant reaction mechanism.The insights reported here could provide the methodology to fundamentally understand the heteroatom-doping effects of carbocatalysis.
基金supported by Natural Science Foundation of China(Nos.21976096 and 52170085)Key Project of Natural Science Foundation of Tianjin(No.21JCZDJC00320)+1 种基金National highlevel foreign experts project(Nos.QN20200002003,G2021125001 and G2021125002)Fundamental Research Funds for the Central Universities,Nankai University。
文摘Aromatic compounds such as phenols presented widely in coal chemical industry wastewater(CCW)render the treatment facing great challenge due to their biorefractory characteristics and potential risks to the environment and human health.Ozone-based advanced oxidation processes show promising for these pollutants removal,but the mineralization via ozonation alone is unsatisfactory and not cost-effective.Herein,a hybrid peroxi-coagulation/ozonation process(denoted as PCO)was developed using sacrificial iron plate as an anode and carbon black modified carbon felt as cathode in the presence of ozonation.An enhanced phenol removal of∼100%within 20 min and phenol mineralization of∼80%within 60 min were achieved with a low energy consumption of 0.35 kWh/g TOC.In this novel process,synergistic effect between ozonation and peroxi-coagulation was observed,and beside O_(3) direct oxidation,peroxone played a dominant role for phenol removal.In the PCO process,the hydrolyzed Fe species enhanced the generation of reactive oxygen species(ROS),while•OH was dominantly responsible for pollutant degradation.This process also illustrated high resistance to high ionic strength and better performance for TOC removal in real wastewater when compared with ozonation and peroxi-coagulation process.Therefore,this process is more cost-effective,being very promising for CCW treatment.
基金financially supported by the Chongqing Research Program of Basic Research and Frontier Technology(No.cstc2018jcyj AX0408)。
文摘There is an urgent demand for tuning the selectivity and activity of the photocatalysts to remove coexistent pollutants simultaneously.Herein,we introduced the surficial activity sites into the bismuth oxybromide(Bi OBr),including the Bi/Bi-O defects and hetero Cu atoms,and then the higher photocatalytic activity and selectivity of BiOBr were realized for degradation phenol and ciprofloxacin(CIP).It can be found that the Bi/Bi-O defects played more important role in enhancing the photocatalytic activity for degradation of phenol,while the Cu atoms significantly improved the photocatalytic activity for removing CIP.Moreover,the heterogeneous Cu atoms as the activity sites excited the reaction between phenol and CIP even under dark condition and were beneficial for synchronously removing phenol and CIP.This work provides a feasible way for BiOX photocatalyst to remove co-existent pollutants and may have a practical application.