| MoO2@氮掺杂碳复合物的制备及其降解有机污染物 | |
| Preparation of MoO2@nitrogen doped carbon composites for degradation of organic pollutants | |
| 摘要: 以多巴胺、钼酸铵、碳酸氢铵为原料，通过一步煅烧法合成一种MoO2@氮掺杂碳复合物(MoO2@CN)，并利用扫描电子显微镜(SEM)、透射电子显微镜(TEM)、X射线光电子能谱(XPS)、拉曼光谱(Raman)等对其进行表征。以卡马西平(CBZ)为目标污染物，以过一硫酸氢钾(PMS)为氧化剂，在温度为25℃、pH为6.5的条件下，MoO2@CN/PMS在12 min内对CBZ的去除率达99.2%，与商用MoO2相比，其表观速率常数kobs(0.393 min-1)是商用MoO2(0.016 4 min-1)的24.0倍，这主要是由于制备的MoO2@CN比商用MoO2具有更好的电子传输能力以及更大的比表面积。MoO2@CN在pH为2.5~10.5时均能有效降解CBZ，而且对大多数染料、酚类化合物、抗生素等多种污染物均具有良好的降解性能。此外，MoO2@CN/PMS在60 min内对CBZ的总有机碳(TOC)去除率高达74.0%。电子顺磁共振波谱(EPR)和自由基猝灭实验显示MoO2@CN/PMS体系中主要起作用是硫酸根自由基(SO4·-)和羟基自由基(·OH)。更有意思的是，在Fe2+/PMS体系加入MoO2@CN后，其催化降解CBZ的性能显著增强，kobs(1.25 min-1)是单独Fe2+/PMS体系(0.079 7 min-1)的15.7倍，这主要归因于MoO2@CN的引入加快了Fe3+到Fe2+的转变，导致更多·OH的生成。 | |
| 关键词: 二氧化钼 多巴胺 过一硫酸盐 有机物降解 | |
| 基金项目: 国家自然科学基金(No.51772274)资助。 | |
| Abstract: The MoO2@nitrogen doped carbon composite (MoO2@CN) was designed via one-step calcination from dopamine, ammonium molybdate, and ammonium bicarbonate. Besides, MoO2@CN was characterized by scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), Raman spectroscopy, etc. The MoO2@CN/PMS system could reach 99.2% degradation rate for carbamazepine (CBZ) in 12 min under pH of 6.5 and temperature at 25 ℃. Moreover, the apparent rate constant (kobs) of MoO2@CN was calculated to be 0.393 min-1, about 24.0 times higher than that of the commercial MoO2 (0.016 4 min-1), which is attributed that MoO2@CN possessed better conductivity and larger specific surface area. MoO2@CN was capable to degrade CBZ effectively in the pH range of 2.5-10.5, and also exhibited effective degradation performance for most dyes, phenolic compounds, antibiotics, and other pollutants. In addition, the total organic carbon (TOC) degradation rate of CBZ was as high as 74.0% within 60 min in the MoO2@CN/PMS system. Electron paramagnetic resonance (EPR) spectroscopy and quenching tests were applied to verify that SO4·- and ·OH played a major role in the MoO2@CN/PMS system. Interestingly, the degradation performance of CBZ was significantly enhanced with high kobs value of 1.25 min-1 when MoO2@CN was introduced into the Fe2+/PMS system, which was about 15.7 times proceeding that of the Fe2+/PMS system (0.079 7 min-1). The phenomenon is mainly ascribed that MoO2@CN significantly accelerates the transition from Fe3+ to Fe2+, resulting in more ·OH production. | |
| Keywords: molybdenum dioxide dopamine peroxymonosulfate organics degradation | |
| 投稿时间：2022-06-29 修订日期：2022-10-17 | |
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| 曹诗雨,陈斌杰,郁非繁,徐象威,姚玉元.MoO2@氮掺杂碳复合物的制备及其降解有机污染物[J].无机化学学报,2023,39(1):80-90. | |
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