氮掺杂多孔碳催化过硫酸盐方法及其水处理性能
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摘要
近年来,基于硫酸根自由基(SO4·-)的高级氧化技术因其氧化能力强(2.5-3.1 V),pH适应范围广(2-8)以及对有机污染物的高选择性而在水处理领域受到广泛关注[1]。已有研究采用紫外光、热或者过渡金属及其氧化物活化过硫酸盐产生硫酸根自由基,但是这些技术往往面临能耗较高、过程中产生毒性金属泄露的问题,限制了它们的应用。氮掺杂纳米碳材料因其独特的结构特性以及电子传递能力使其具有催化过硫酸盐的潜力,且其绿色非金属的特点使它相比于过渡金属更有优势[2]。本研究采用不同的含氮金属有机骨架材料(MOFs)为模板制备氮掺杂多孔碳材料,研究其催化过硫酸盐产生硫酸根自由基的性能,并探索了该材料的活性位点与催化机理。结果表明,掺氮多孔碳比不掺氮的多孔碳具有更好的过硫酸盐催化能力,甚至比传统的均相钴盐和非均相的四氧化三钴的催化活性更高。捕获实验证明该过程中存在羟基自由基和硫酸根自由基两种活性基团。
Recently,the sulfate radical(SO4·-) based AOPs has attracted increasing research interest for its use in wastewater treatment due to its strong oxidizing capability,independence of pH and high selectivity to organic matters.Generally,SO4·-can be generated from activating PMS by heating,UV irradiation and transitional metal ions or metallic oxidants.However,the high energy input and the inevitable toxic metal leaching limit their practical application.Owing to its unique structural feature,good electro-conductivity and metal-free nature,the nitrogen doped nanocarbon material holds great promise for PMS activation.In this study,different nitrogen doped porous carbons(NPCs) derived from MOFs were prepared and investigated for PMS activation.The results showed that the NPC performs better than that of porous carbon in PMS activation,even better than that of homogenous Co~(2+) or heterogeneous Co3O4.The quenching experiments proved that both ·OH and SO4·-were present in the catalytic process.
引文
[1]Yong F.;Deli W.;Yu D.;Tong Z.;Kaimin S.Environ.Sci.Technol.2016,50(6):3119.
    [2]Xiaoguang D.;Hongqi S.;Yuxian W.;Jian K.;Shaobin W.ACS Catal.2015,5:553.

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