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中压紫外/甲酸盐还原体系对硝酸盐的去除效能及机制

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研究了中压紫外/甲酸盐(MPUV/HCOO)还原体系对硝酸盐(NO3-)的去除效能和机制.结果表明,MPUV/HCOO-体系的NO3-去除效果显著高于单独MPUV光解.当NO3-初始浓度为0.1 mmol·L-1,HCOO-投加量为1 mmol·L-1 时,MPUV/HCOO-体系中 NO3-的伪一级动力学降解速率(5.7×10-3 min-1)是单独 MPUV(1.0×10-3 min-1)光解的5.7倍,且HCOO-的投加使得120 min后NO3-还原率由13.7%提升至44.1%.增大紫外光强和弱碱性pH环境均有利于NO3-降解.该研究认为,中压紫外直接光解NO3-以及由HCOO-转化生成的二氧化碳阴离子自由基(CO2·-)介导的还原过程被认为共同促进了 NO3-的还原效率.利用激光闪光光解技术,首次定量了 CO2ˉ-与NO3-和NO2-的二级反应速率常数分别为1.57×106 L·(mol·s)-1和9.12×107 L·(mol·s)-1.MPUV/HCOO-体系将硝酸盐转化为亚硝酸盐,补充投加过氧化氢促进CO2-的生成,CO2-与亚硝酸盐反应进一步生成气态氮(氮气、氧化亚氮等)从水中脱除.在污水处理中,借助中压紫外消毒和生物处理系统中剩余碳源甲酸盐构建中压紫外/甲酸盐体系,有望强化污水深度脱氮,具有良好的应用前景.
Removal efficiency and mechanism of nitrate in the medium pressure ultraviolet/formate system
In this study,the nitrate removal efficiency and mechanism in the combination of medium pressure ultraviolet and formate(MPUV/HCOO-)system was investigated.The results showed that the nitrate removal efficiency in the MPUV/HCOO-system was significantly higher than that of MPUV photolysis alone.When the initial NO3-concentration was 0.1 mmol·L-1 and the HCOO-dosage was 1 mmol·L-1,the pseudo-first-order degradation rate of NO3-in the MPUV/HCOO-system(5.7×10-3 min-1)was 5.7 times higher than that of MPUV photolysis alone(1.0×10-3 min-1).The addition of HCOO-increased the NO3-reduction efficiency from 13.7%to 44.1%after 120 minutes.Increasing MPUV intensity and weakly alkaline pH condition were conducive to nitrate degradation.This study indicated that the reduction efficiency of NO3-was collectively enhanced by the direct photolysis of NO3-by MPUV and the reduction process mediated by carbon dioxide radical anion(CO2-)generated from HCOO-.Using the laser flash photolysis technology,the second order rate constants of the reaction between CO2-and nitrate or CO2-and nitrite were first quantified as 1.57×106 L·(mol·s)-1 or 9.12×107 L·(mol·s)-1,respectively.The MPUV/HCOO-system could lead to the transformation from NO3-to NO2-,supplemental hydrogen peroxide promoted the formation of CO2-,which could react with NO2-and produce gaseous nitrogen(such as nitrogen gas and nitrous oxide)discharged from water.In wastewater treatment,the MPUV/HCOO-system could be constructed with the medium pressure ultraviolet disinfection and the residual formate as the carbon source of biological treatment,which is expected to strengthen the deep denitrification of sewage and has a good application prospect.

nitratedeep denitrificationmedium pressure ultravioletformatecarbon dioxide radical anion(CO2)

任鹏飞、周建华、张锐、陈贻龙、张欣然

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广州市市政工程设计研究总院有限公司,广州 510006

中山大学环境科学与工程学院,广州 510006

硝酸盐 深度脱氮 中压紫外 甲酸盐 二氧化碳阴离子自由基(CO2)

2024

环境工程学报
中国科学院生态环境研究中心

环境工程学报

CSTPCD北大核心
影响因子:0.804
ISSN:1673-9108
年,卷(期):2024.18(9)