In this study,a practical process for ozonization of benzyl alcohols to ketones and aldehydes in a rotating packed bed(RPB-O3)reactor has been developed.Using 1-phenylethanol as a model reactant,the performance of RPB...In this study,a practical process for ozonization of benzyl alcohols to ketones and aldehydes in a rotating packed bed(RPB-O3)reactor has been developed.Using 1-phenylethanol as a model reactant,the performance of RPB-O3 process in different solvents has been compared with the commonly used stirred tank reactor(STR-O3).Ethyl acetate was the optimum solvent for the conversion of 1-phenylenthanol to acetophenone in RPB-O3 process,with 78%yield after 30 min.In a parallel STR-O3 experiment,the yield of acetophenone was50%.Other experimental variables,i.e.O3 concentration,reaction time,high-gravity factor and liquid flow rate were also optimized.The highest yield of acetophenone was obtained using O3 concentration of 80 mg·L-1,reaction time of 30 min,high gravity factor of 40 and liquid flow rate of 120 L·h-1.Under the optimized reaction conditions,a series of structurally diverse primary and secondary alcohols was oxidized with(19%–92%)yield.The ozonization mechanism was studied by Electron Paramagnetic Resonance(EPR)spectroscopy,monitoring the radical species formed upon self-decomposition of O3.The characteristic quadruple peak with the 1:2:2:1 intensity ratio that corresponds to hydroxyl radicals(·OH)was observed in the electron paramagnetic resonance(EPR)spectrum,indicating an indirect oxidation mechanism of alcohols via·OH radical.展开更多
Comprehensive Air Quality Model with extensions(CAMx)-Decoupled Direct Method(DDM)simulations of first-order ozone(O_(3))sensitivity to nitrogen oxides(NO_(x))and volatile organic compounds(VOCs)emissions were perform...Comprehensive Air Quality Model with extensions(CAMx)-Decoupled Direct Method(DDM)simulations of first-order ozone(O_(3))sensitivity to nitrogen oxides(NO_(x))and volatile organic compounds(VOCs)emissions were performed and combined with modelled P_(H_(2)O_(2))/P_(HNO_(3))ratios to obtain a range of thresholds for determining O_(3)-sensitivity regimes for different areas of China.Utilising the new threshold ranges for photochemical indicators,the method for determining O_(3)formation in the Ozone Source Apportionment Technology(OSAT)module within CAMx was improved by a dynamically varied threshold of P_(H_(2)O_(2))/P_(HNO_(3))ratio.The O_(3)concentration contributions in the newly added transition regime were apportioned to NO_(x)and VOCs emissions in proportion to the relationship between the P_(H_(2)O_(2))/P_(HNO_(3))ratio and first-order O_(3)sensitivity.The source contributions of O_(3)concentrations from different emission sectors from June to September 2019 were compared using the original and improved CAMx-OSAT.The results showed that the O_(3)concentration contributions changed significantly in the NO_(x)-limited regime,with a maximum decrease of 21.89%,while the contributions increased by up to 7.57%in the VOC-limited regime,and were within 15μg/m^(3)in the transition regime.The modified OSAT module enabled a more sophisticated attribution of O_(3)to precursor emissions and may have far-reaching implications for informing O_(3)pollution control policy.展开更多
Catalytic technologies have been paid increasing attention in refractory pollutants abatement due to its practical and potential values in water purification. As effective and efficient approaches for water purificati...Catalytic technologies have been paid increasing attention in refractory pollutants abatement due to its practical and potential values in water purification. As effective and efficient approaches for water purification, Fenton＇s reagent, ozonation, electrochemical and photocatalytic methods have been widely studied and applied in different aspects and have been reviewed by several articles. In recent years, some novel catalytic processes based on above processes have been developed for enhancing the efficiency of removing the organics from water. This review emphasized on the recent development of heterogeneous catalytic ozonation, electrocatalysis in respect of novel electrodes and electro-Fenton method, photoelectrocatalysis process and photoelectron-Fenton in water purification. It was also an attempt to propose general ideas about mechanism and principle enhancing the catalytic efficiency for the degradation and the mineralization of organics in water.展开更多
The electro-peroxone technology,a novel type of advanced oxidation technology,is widely used in wastewater treatment.Herein,this paper reviews the advantages and problems of the electro-peroxone technology compared wi...The electro-peroxone technology,a novel type of advanced oxidation technology,is widely used in wastewater treatment.Herein,this paper reviews the advantages and problems of the electro-peroxone technology compared with electrochemical oxidation technology,ozonation technology,and traditional peroxone technology.Due to the high kinetics of pollutant degradation,the electro-peroxone process can reduce the reaction time and energy consumption of pollutant treatment in wastewater.The electroperoxone technology can promote pollutant degradation and mineralization,which shows obvious synergistic effects of electrochemical oxidation and ozonation for wastewater treatment.Most importantly,the research mechanism of the electro-peroxone technology is systematically introduced from two aspects of cathode reaction and bulk reaction.The influence of experimental parameters on the wastewater treatment effect is also discussed.Finally,the potential applications and future research directions of the electro-peroxone technology in the wastewater field are proposed.The electro-peroxone process can offer a highly efficient and energy saving water treatment method to improve the performance of existing ozonation and electrochemical systems and has therefore become a promising electrochemical advanced oxidation process for wastewater treatment.展开更多
基金supported by the Specialized Research Fund for Sanjin Scholars Program of Shanxi Province(201707)Key Research&Development Plan of Shanxi Province(201903D321059)+1 种基金Shanxi Scholarship Council of China(2019032)Shanxi Graduate Education Innovation Project(2019BY106)。
文摘In this study,a practical process for ozonization of benzyl alcohols to ketones and aldehydes in a rotating packed bed(RPB-O3)reactor has been developed.Using 1-phenylethanol as a model reactant,the performance of RPB-O3 process in different solvents has been compared with the commonly used stirred tank reactor(STR-O3).Ethyl acetate was the optimum solvent for the conversion of 1-phenylenthanol to acetophenone in RPB-O3 process,with 78%yield after 30 min.In a parallel STR-O3 experiment,the yield of acetophenone was50%.Other experimental variables,i.e.O3 concentration,reaction time,high-gravity factor and liquid flow rate were also optimized.The highest yield of acetophenone was obtained using O3 concentration of 80 mg·L-1,reaction time of 30 min,high gravity factor of 40 and liquid flow rate of 120 L·h-1.Under the optimized reaction conditions,a series of structurally diverse primary and secondary alcohols was oxidized with(19%–92%)yield.The ozonization mechanism was studied by Electron Paramagnetic Resonance(EPR)spectroscopy,monitoring the radical species formed upon self-decomposition of O3.The characteristic quadruple peak with the 1:2:2:1 intensity ratio that corresponds to hydroxyl radicals(·OH)was observed in the electron paramagnetic resonance(EPR)spectrum,indicating an indirect oxidation mechanism of alcohols via·OH radical.
基金supported by the the National Key Research and Development Project(Nos.2022YFC3701105,2018YFC0213504,2017YFC0213003)the National Natural Science Foundation of China(No.42005112)。
文摘Comprehensive Air Quality Model with extensions(CAMx)-Decoupled Direct Method(DDM)simulations of first-order ozone(O_(3))sensitivity to nitrogen oxides(NO_(x))and volatile organic compounds(VOCs)emissions were performed and combined with modelled P_(H_(2)O_(2))/P_(HNO_(3))ratios to obtain a range of thresholds for determining O_(3)-sensitivity regimes for different areas of China.Utilising the new threshold ranges for photochemical indicators,the method for determining O_(3)formation in the Ozone Source Apportionment Technology(OSAT)module within CAMx was improved by a dynamically varied threshold of P_(H_(2)O_(2))/P_(HNO_(3))ratio.The O_(3)concentration contributions in the newly added transition regime were apportioned to NO_(x)and VOCs emissions in proportion to the relationship between the P_(H_(2)O_(2))/P_(HNO_(3))ratio and first-order O_(3)sensitivity.The source contributions of O_(3)concentrations from different emission sectors from June to September 2019 were compared using the original and improved CAMx-OSAT.The results showed that the O_(3)concentration contributions changed significantly in the NO_(x)-limited regime,with a maximum decrease of 21.89%,while the contributions increased by up to 7.57%in the VOC-limited regime,and were within 15μg/m^(3)in the transition regime.The modified OSAT module enabled a more sophisticated attribution of O_(3)to precursor emissions and may have far-reaching implications for informing O_(3)pollution control policy.
文摘Catalytic technologies have been paid increasing attention in refractory pollutants abatement due to its practical and potential values in water purification. As effective and efficient approaches for water purification, Fenton＇s reagent, ozonation, electrochemical and photocatalytic methods have been widely studied and applied in different aspects and have been reviewed by several articles. In recent years, some novel catalytic processes based on above processes have been developed for enhancing the efficiency of removing the organics from water. This review emphasized on the recent development of heterogeneous catalytic ozonation, electrocatalysis in respect of novel electrodes and electro-Fenton method, photoelectrocatalysis process and photoelectron-Fenton in water purification. It was also an attempt to propose general ideas about mechanism and principle enhancing the catalytic efficiency for the degradation and the mineralization of organics in water.
基金the financial support provided by the National Natural Science Foundation of China(No.21306175)the Zhejiang Provincial Natural Science Foundation of China(No.LGJ18E080001)+1 种基金the Project of Science and Technology Department of Jiashan(Nos.2020D02 and 2022A23)Zhejiang Province(No.2015C03017)。
文摘The electro-peroxone technology,a novel type of advanced oxidation technology,is widely used in wastewater treatment.Herein,this paper reviews the advantages and problems of the electro-peroxone technology compared with electrochemical oxidation technology,ozonation technology,and traditional peroxone technology.Due to the high kinetics of pollutant degradation,the electro-peroxone process can reduce the reaction time and energy consumption of pollutant treatment in wastewater.The electroperoxone technology can promote pollutant degradation and mineralization,which shows obvious synergistic effects of electrochemical oxidation and ozonation for wastewater treatment.Most importantly,the research mechanism of the electro-peroxone technology is systematically introduced from two aspects of cathode reaction and bulk reaction.The influence of experimental parameters on the wastewater treatment effect is also discussed.Finally,the potential applications and future research directions of the electro-peroxone technology in the wastewater field are proposed.The electro-peroxone process can offer a highly efficient and energy saving water treatment method to improve the performance of existing ozonation and electrochemical systems and has therefore become a promising electrochemical advanced oxidation process for wastewater treatment.
