引用本文: | 庞素艳,王强,鲁雪婷,江进,刘波,马军.中间价态锰强化KMnO4氧化降解三氯生[J].哈尔滨工业大学学报,2015,47(2):87.DOI:10.11918/j.issn.0367-6234.2015.02.016 |
| PANG Suyan,WANG Qiang,LU Xueting,JIANG Jin,LIU Bo,MA Jun.Oxidative removal of triclosan by potassium permanganate enhanced with manganese intermediates[J].Journal of Harbin Institute of Technology,2015,47(2):87.DOI:10.11918/j.issn.0367-6234.2015.02.016 |
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中间价态锰强化KMnO4氧化降解三氯生 |
庞素艳1, 王强1, 鲁雪婷1, 江进2,3, 刘波1, 马军2,3
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(1. 哈尔滨理工大学 化学与环境工程学院,绿色化工技术黑龙江省高校重点实验室,150040 哈尔滨;2. 城市水资源与 水环境国家重点实验室(哈尔滨工业大学),150090哈尔滨;3. 哈尔滨工业大学 市政环境工程学院,150090 哈尔滨)
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摘要: |
为验证中间价态锰在KMnO4氧化降解广谱杀菌剂三氯生过程中的强化作用,在不同pH假一级动力学实验条件下,研究KMnO4氧化降解三氯生的动力学规律,考察外加络合剂对KMnO4氧化降解三氯生的影响,评价还原剂Mn(II)在KMnO4氧化降解三氯生过程中的作用.结果表明,KMnO4氧化降解三氯生符合假一级动力学规律,且假一级速率常数Kobs(s-1) 随KMnO4浓度的增加呈线性增加. 通过KMnO4浓度与Kobs得到的二级反应速率常数k(L·mol-1·s-1)随pH先升高后降低,在三氯生pKa=8.1附近时最大.络合剂和天然水体的背景成分通过其配位作用,使得KMnO4氧化过程中产生的中间价态锰稳定性增强,强化KMnO4氧化降解三氯生.紫外-可见光谱扫描结果进一步表明,络合剂的强化作用主要是KMnO4氧化过程中生成具有强氧化性Mn(III)的贡献,同时络合剂存在条件下,Mn(II)能够催化KMnO4氧化降解三氯生. |
关键词: 高锰酸钾 三氯生 中间价态锰 络合剂 强化作用 |
DOI:10.11918/j.issn.0367-6234.2015.02.016 |
分类号:X703 |
基金项目:国家自然科学基金(51208159); 中国博士后科学基金(2013M541402). |
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Oxidative removal of triclosan by potassium permanganate enhanced with manganese intermediates |
PANG Suyan1, WANG Qiang1, LU Xueting1, JIANG Jin2,3, LIU Bo1, MA Jun2,3
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(1. Key Laboratory of Green Chemical Engineering and Technology of College of Heilongjiang Province, College of Chemical and Environmental Engineering, Harbin University of Science and Technology, 150040 Harbin, China; 2. State Key Laboratory of Urban Water Resource and Environment(Harbin Institute of Technology), 150090 Harbin, China; 3. School of Municipal and Environmental Engineering, Harbin Institute of Technology, 150090 Harbin, China)
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Abstract: |
To investigate the effect of manganese intermediates in situ formed on the oxidation of anti-biocide triclosan by potassium permanganate, experiments were conducted to examine the effects of some ligands as well as Mn(II) on the oxidation of triclosan by potassium permanganate under the condition with potassium permanganate in excess over a wide pH range. The results showed that the degradation of triclosan followed the second-order kinetics and the rate constants increased with the increase of pH and reached the maximum near the pKa (8.1) of triclosan, after which they decreased gradually. Both selected ligands and the background matrices of nature waters could significantly enhance the oxidation dynamics of triclosan by potassium permanganate via the involvement of stabilized manganese intermediates. The analysis by the UV-vis spectrophotometer scanning confirmed the formation of soluble Mn(III) in the presence of ligands, which would otherwise disproportionate spontaneously to yield solid MnO2. Also, these results suggested a catalytic role of Mn(II) in the oxidation of triclosan by potassium permanganate. |
Key words: potassium permanganate triclosan manganese intermediates ligands enhanced role |
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