As an active metabolite of venlafaxine and emerging antidepressant,Odesmethylvenlafaxine(ODVEN) was widely detected in different water bodies,which caused potential harm to human health and environmental safety.In thi...As an active metabolite of venlafaxine and emerging antidepressant,Odesmethylvenlafaxine(ODVEN) was widely detected in different water bodies,which caused potential harm to human health and environmental safety.In this study,the comparative work on the ODVEN degradation by UV(254 nm) and UV-LED(275 nm) activated sodium percarbonate(SPC) systems was systematically performed.The higher removal rate of ODVEN can be achieved under UV-LED direct photolysis(14.99%) than UV direct photolysis(4.57%) due to the higher values of photolysis coefficient at the wavelength 275nm.Significant synergistic effects were observed in the UV/SPC(80.38%) and UV-LED/SPC(53.57%) systems and the former exhibited better performance for the elimination of ODVEN.The degradation of ODVEN all followed the pseudo-first-order kinetics well in these processes,and the pseudo-first-order rate constant(kobs) increased with increasing SPC concentration.Radicals quenching experiments demonstrated that both ·OH and CO_(3)·-were involved in the degradation of ODVEN and the second-order rate constant of ODVEN with CO_(3)·-(1.58 × 10^(8)(mol/L)-1sec-1) was reported for the first time based on competitive kinetic method.The introduction of HA,Cl-,NO_(3)-and HCO_(3)-inhibited the ODVEN degradation to varying degrees in the both processes.According to quantum chemical calculation,radical addition at the ortho-position of the phenolic hydroxyl group was confirmed to be the main reaction pathways for the oxidation of ODVEN by·OH.In addition,the oxidation of ODVEN may involve the demethylation,H-abstraction,OH^(-)addition and C-N bond cleavage.Eventually,the UV-LED/SPC process was considered to be more cost-effective compared to the UV/SPC process,although the UV/SPC process possessed a higher removal rate of ODVEN.展开更多
A new process for the Pd/Cu co-catalyzed homocoupling reaction of terminal alkynes was developed. The reaction was carried out in aqueous media with sodium percarbonate as both a clean oxidant and a base. Meanwhile, a...A new process for the Pd/Cu co-catalyzed homocoupling reaction of terminal alkynes was developed. The reaction was carried out in aqueous media with sodium percarbonate as both a clean oxidant and a base. Meanwhile, a palladium complex immobilized on a synthetic PS-PEG400-PPh2 resin was used as the catalyst, which may be recovered by simple filtration and reused for several times with high activity.展开更多
The performance of sodium percarbonate （SPC） activated with ferrous ion （Fe（Ⅱ） with the addition of formic acid （FA） to stimulate the degradation of carbon tetrachloride （CT） was investigated. Results showed...The performance of sodium percarbonate （SPC） activated with ferrous ion （Fe（Ⅱ） with the addition of formic acid （FA） to stimulate the degradation of carbon tetrachloride （CT） was investigated. Results showed that CT could be entirely reduced within 15 min in the system at a variety of SPC/Fe（Ⅱ）/FA/CT molar ratios in experimental level. Scavenging tests indicated that carbon dioxide radical anion （CO2-） was the dominant reactive oxygen species responsible for CT degradation. CT degradation rate, to a large extent, increased with increasing dosages of chemical agents and the optimal molar ratio of SPC/Fe（Ⅱ）/FAJCT was set as 60/60/60/1. The initial concentration of CT can hardly affect the CT removal, while CT degradation was favorable in the pH range of 3.0-9.0, but apparently inhibited at pH 12. C1- and HCO3 of high concentration showed negative impact on CT removal. Cl- released from CT was detected and the results confirmed nearly complete mineralization ofCT. CT degradation was proposed by reductive C-C1 bond splitting. This study demonstrated that SPC activated with Fe（Ⅱ） with the addition of FA may be promising technique for CT remediation in contaminated groundwater.展开更多
基金supported by the National Natural Science Foundation of China (Nos.51978618,51878582)the Natural Science Foundation of Zhejiang Province (Nos.LY21E080018,LY18E080036)+1 种基金Guiding Project of Fujian Province of China (No.2021Y0041)Foundation of Key Laboratory of Yangtze River Water Environment and Ministry of Education (Tongji University),China (No.YRWEF201901)。
文摘As an active metabolite of venlafaxine and emerging antidepressant,Odesmethylvenlafaxine(ODVEN) was widely detected in different water bodies,which caused potential harm to human health and environmental safety.In this study,the comparative work on the ODVEN degradation by UV(254 nm) and UV-LED(275 nm) activated sodium percarbonate(SPC) systems was systematically performed.The higher removal rate of ODVEN can be achieved under UV-LED direct photolysis(14.99%) than UV direct photolysis(4.57%) due to the higher values of photolysis coefficient at the wavelength 275nm.Significant synergistic effects were observed in the UV/SPC(80.38%) and UV-LED/SPC(53.57%) systems and the former exhibited better performance for the elimination of ODVEN.The degradation of ODVEN all followed the pseudo-first-order kinetics well in these processes,and the pseudo-first-order rate constant(kobs) increased with increasing SPC concentration.Radicals quenching experiments demonstrated that both ·OH and CO_(3)·-were involved in the degradation of ODVEN and the second-order rate constant of ODVEN with CO_(3)·-(1.58 × 10^(8)(mol/L)-1sec-1) was reported for the first time based on competitive kinetic method.The introduction of HA,Cl-,NO_(3)-and HCO_(3)-inhibited the ODVEN degradation to varying degrees in the both processes.According to quantum chemical calculation,radical addition at the ortho-position of the phenolic hydroxyl group was confirmed to be the main reaction pathways for the oxidation of ODVEN by·OH.In addition,the oxidation of ODVEN may involve the demethylation,H-abstraction,OH^(-)addition and C-N bond cleavage.Eventually,the UV-LED/SPC process was considered to be more cost-effective compared to the UV/SPC process,although the UV/SPC process possessed a higher removal rate of ODVEN.
基金Project supported by the National Natural Science Foundation of China （Nos. 20332030, 20572027, 20625205）.
文摘A new process for the Pd/Cu co-catalyzed homocoupling reaction of terminal alkynes was developed. The reaction was carried out in aqueous media with sodium percarbonate as both a clean oxidant and a base. Meanwhile, a palladium complex immobilized on a synthetic PS-PEG400-PPh2 resin was used as the catalyst, which may be recovered by simple filtration and reused for several times with high activity.
文摘The performance of sodium percarbonate （SPC） activated with ferrous ion （Fe（Ⅱ） with the addition of formic acid （FA） to stimulate the degradation of carbon tetrachloride （CT） was investigated. Results showed that CT could be entirely reduced within 15 min in the system at a variety of SPC/Fe（Ⅱ）/FA/CT molar ratios in experimental level. Scavenging tests indicated that carbon dioxide radical anion （CO2-） was the dominant reactive oxygen species responsible for CT degradation. CT degradation rate, to a large extent, increased with increasing dosages of chemical agents and the optimal molar ratio of SPC/Fe（Ⅱ）/FAJCT was set as 60/60/60/1. The initial concentration of CT can hardly affect the CT removal, while CT degradation was favorable in the pH range of 3.0-9.0, but apparently inhibited at pH 12. C1- and HCO3 of high concentration showed negative impact on CT removal. Cl- released from CT was detected and the results confirmed nearly complete mineralization ofCT. CT degradation was proposed by reductive C-C1 bond splitting. This study demonstrated that SPC activated with Fe（Ⅱ） with the addition of FA may be promising technique for CT remediation in contaminated groundwater.
