The degradation of atrazine (ATZ),sulfamethoxazole (SMX) and metoprolol (MET) in flowthrough VUV/UV/H2O2reactors was investigated with a focus on the effects of H2O2dosage and reactor internal diameter (ID).Results sh...The degradation of atrazine (ATZ),sulfamethoxazole (SMX) and metoprolol (MET) in flowthrough VUV/UV/H2O2reactors was investigated with a focus on the effects of H2O2dosage and reactor internal diameter (ID).Results showed that the micropollutants were degraded efficiently in the flow-through VUV/UV/H2O2reactors following the pseudo first-order kinetics (R2>0.92).However,the steady-state assumption (SSA) kinetic model being vital in batch reactors was found invalid in flow-through reactors where fluid mixing was less sufficient.With the increase of H2O2dosage,the ATZ removal efficiency remained almost constant while the SMX and MET removal was enhanced to different extents,which could be explained by the different reactivities of the pollutants towards HO·.A larger reactor ID resulted in lower degradation rate constants for all the three pollutants on account of the lower average fluence rate,but the change in energy efficiency was much more complicated.In reality,the electrical energy per order (EEO) of the investigated VUV/UV/H2O2treatments ranged between 0.14–0.20,0.07–0.14 and 0.09–0.26 k Wh/m3/order for ATZ,SMX and MET,respectively,with the lowest EEOfor each pollutant obtained under varied H2O2dosages and reactor IDs.This study has demonstrated the efficiency of VUV/UV/H2O2process for micropollutant removal and the inadequacy of the SSA model in flow-through reactors,and elaborated the influential mechanisms of H2O2dosage and reactor ID on the reactor performances.展开更多
The problem of water and sulfur poisoning in flue gas atmosphere remains a significant obstacle for low-temperature deNO_(x) catalysts.This study investigated the sulfation mechanism of the CoMn_(2)O_(4)/CeTiO_(x)(CMC...The problem of water and sulfur poisoning in flue gas atmosphere remains a significant obstacle for low-temperature deNO_(x) catalysts.This study investigated the sulfation mechanism of the CoMn_(2)O_(4)/CeTiO_(x)(CMCT)catalyst during the selective catalytic reduction of NO_(x) with NH3 under conditions containing H2O and SO_(2) at 150℃.Employing a comprehensive suite of time-resolved analysis and characterization techniques,the evolution of sulfate species was systematically categorized into three stages:initial rapid surface sulfate accumulation,the transformation of surface sulfates to bulk metal sulfates,and partial sulfates decomposition after the removal of H2O and SO_(2).These findings indicate that bulk metal sulfates irreversibly deactivate the catalyst by distorting active component lattices and consuming oxygen vacancies,whereas surface sulfates(including ammonium sulfates and surface-coordinated metal sulfates)cause reversible performance loss through decomposition.Furthermore,the competitive adsorption of H2O and SO_(2) significantly influences the catalytic efficiency,with H2O suppressing SO_(2) adsorption while simultaneously enhancing the formation of Brönsted acid sites.This research underscores the critical role of sulfate dynamics on catalyst performance,revealing the enhanced SO_(2) resistance of the Eley-Rideal mechanism facilitated by the Ce-Ti support relative to the Langmuir-Hinshelwood pathway.Collectively,the study unravels the complex interplay of sulfate dynamics influencing catalyst performance and provides potential approaches to mitigate deactivation in demanding atmospheric conditions.展开更多
制备了负载在Na Y分子筛上的Fe Cu Mn Y复合催化剂,并对其在非均相UV Fe Cu Mn Y H2O2体系中催化氧化4BS染料废水进行了研究.结果表明,非均相UV Fe Cu Mn Y H2O2体系对4BS染料废水的处理具有很高的效率.在基准条件下,反应时间为20min时...制备了负载在Na Y分子筛上的Fe Cu Mn Y复合催化剂,并对其在非均相UV Fe Cu Mn Y H2O2体系中催化氧化4BS染料废水进行了研究.结果表明,非均相UV Fe Cu Mn Y H2O2体系对4BS染料废水的处理具有很高的效率.在基准条件下,反应时间为20min时,废水中4BS的去除率达到了93 7%.与均相UV Fenton体系不同,非均相UV Fe Cu Mn Y H2O2体系在碱性条件下(pH=10 5)仍可高效去除CODCr.动力学研究得到催化氧化4BS废水的模型方程,该模型可以为非均相UV Fe Cu Mn Y H2O2体系处理高色度的实际染料废水提供指导.展开更多
采用UV/H2O2技术对污染水体中的MTBE进行了氧化降解试验,考察了不同MTBE初始浓度,不同H2O2浓度,不同pH值,不同波长的紫外光对降解效果的影响,以及不同Cl-、HCO3-浓度的抑制作用.结果表明,在室温条件下,当紫外光波长为254 nm,H2O2为15 m ...采用UV/H2O2技术对污染水体中的MTBE进行了氧化降解试验,考察了不同MTBE初始浓度,不同H2O2浓度,不同pH值,不同波长的紫外光对降解效果的影响,以及不同Cl-、HCO3-浓度的抑制作用.结果表明,在室温条件下,当紫外光波长为254 nm,H2O2为15 m mol/L,pH为3.0时对起始浓度为1 m mol/L的MTBE具有较好的降解效果;反应60 min,MTBE去除率可达97.6%.实验证明,UV/H2O2氧化技术是降解MTBE的一种有效方法.展开更多
基金supported by the National Natural Science Foundation of China(No.51908536)the Ministry of Science and Technology of China(No.2018YFE0204103)。
文摘The degradation of atrazine (ATZ),sulfamethoxazole (SMX) and metoprolol (MET) in flowthrough VUV/UV/H2O2reactors was investigated with a focus on the effects of H2O2dosage and reactor internal diameter (ID).Results showed that the micropollutants were degraded efficiently in the flow-through VUV/UV/H2O2reactors following the pseudo first-order kinetics (R2>0.92).However,the steady-state assumption (SSA) kinetic model being vital in batch reactors was found invalid in flow-through reactors where fluid mixing was less sufficient.With the increase of H2O2dosage,the ATZ removal efficiency remained almost constant while the SMX and MET removal was enhanced to different extents,which could be explained by the different reactivities of the pollutants towards HO·.A larger reactor ID resulted in lower degradation rate constants for all the three pollutants on account of the lower average fluence rate,but the change in energy efficiency was much more complicated.In reality,the electrical energy per order (EEO) of the investigated VUV/UV/H2O2treatments ranged between 0.14–0.20,0.07–0.14 and 0.09–0.26 k Wh/m3/order for ATZ,SMX and MET,respectively,with the lowest EEOfor each pollutant obtained under varied H2O2dosages and reactor IDs.This study has demonstrated the efficiency of VUV/UV/H2O2process for micropollutant removal and the inadequacy of the SSA model in flow-through reactors,and elaborated the influential mechanisms of H2O2dosage and reactor ID on the reactor performances.
文摘The problem of water and sulfur poisoning in flue gas atmosphere remains a significant obstacle for low-temperature deNO_(x) catalysts.This study investigated the sulfation mechanism of the CoMn_(2)O_(4)/CeTiO_(x)(CMCT)catalyst during the selective catalytic reduction of NO_(x) with NH3 under conditions containing H2O and SO_(2) at 150℃.Employing a comprehensive suite of time-resolved analysis and characterization techniques,the evolution of sulfate species was systematically categorized into three stages:initial rapid surface sulfate accumulation,the transformation of surface sulfates to bulk metal sulfates,and partial sulfates decomposition after the removal of H2O and SO_(2).These findings indicate that bulk metal sulfates irreversibly deactivate the catalyst by distorting active component lattices and consuming oxygen vacancies,whereas surface sulfates(including ammonium sulfates and surface-coordinated metal sulfates)cause reversible performance loss through decomposition.Furthermore,the competitive adsorption of H2O and SO_(2) significantly influences the catalytic efficiency,with H2O suppressing SO_(2) adsorption while simultaneously enhancing the formation of Brönsted acid sites.This research underscores the critical role of sulfate dynamics on catalyst performance,revealing the enhanced SO_(2) resistance of the Eley-Rideal mechanism facilitated by the Ce-Ti support relative to the Langmuir-Hinshelwood pathway.Collectively,the study unravels the complex interplay of sulfate dynamics influencing catalyst performance and provides potential approaches to mitigate deactivation in demanding atmospheric conditions.
文摘制备了负载在Na Y分子筛上的Fe Cu Mn Y复合催化剂,并对其在非均相UV Fe Cu Mn Y H2O2体系中催化氧化4BS染料废水进行了研究.结果表明,非均相UV Fe Cu Mn Y H2O2体系对4BS染料废水的处理具有很高的效率.在基准条件下,反应时间为20min时,废水中4BS的去除率达到了93 7%.与均相UV Fenton体系不同,非均相UV Fe Cu Mn Y H2O2体系在碱性条件下(pH=10 5)仍可高效去除CODCr.动力学研究得到催化氧化4BS废水的模型方程,该模型可以为非均相UV Fe Cu Mn Y H2O2体系处理高色度的实际染料废水提供指导.
文摘采用UV/H2O2技术对污染水体中的MTBE进行了氧化降解试验,考察了不同MTBE初始浓度,不同H2O2浓度,不同pH值,不同波长的紫外光对降解效果的影响,以及不同Cl-、HCO3-浓度的抑制作用.结果表明,在室温条件下,当紫外光波长为254 nm,H2O2为15 m mol/L,pH为3.0时对起始浓度为1 m mol/L的MTBE具有较好的降解效果;反应60 min,MTBE去除率可达97.6%.实验证明,UV/H2O2氧化技术是降解MTBE的一种有效方法.
