New insights into the removal of nitric oxide using UiO-66-NH2: Synergistic photooxidation and subsequent adsorption
发布时间：2023-01-30点击次数：
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DOI码：10.1016/j.jece.2022.108294
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发表刊物：Journal of Environmental Chemical Engineering
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关键字：Photooxidation；Adsorption；In-situ DRIFTS；DFT calculation；GCMC simulation
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摘要：UiO-66 variants are widely used for photocatalysis and adsorption, but few studies reported their combined effects in one process. This paper reports that the mechanism behind NO removal using UiO-66-NH2 includes photocatalytic oxidation and subsequent adsorption. First, the UiO-66-NH2 was selected out of UiO-66-X variants (X = H, NH2, NO2, OH, Br, Br2) because of its high NO removal efficiency (i.e., 80.54%), which is 8.55–64.95 times higher than those of other UiO-66 variants. Then, the NO reaction pathway and degradation mechanisms are proposed based on the experimental results and theoretical calculations. In an anhydrous environment, the NO removal efficiency increases from 80.54% at 40–60% of humidity to 96.23%. Moreover, NO2 emissions and catalyst deactivate are not observed. These findings indicate that the photocatalytic NO degradation includes the photocatalytic oxidation of NO into NO2 on the surface of UiO-66-NH2 and subsequent NO2 adsorption in micropores. The reason is that the formation of NOx- ions without H2O is theoretically impossible according to the principle of electroneutrality. In-situ DRIFTS also confirms the mechanism. Furthermore, density functional theory (DFT) and grand canonical Monte Carlo (GCMC) simulations were carried out to understand the improved NO removal caused by synergistic photocatalysis and adsorption. In summary, this work proposes a new mechanism for NO removal that combines the photocatalytic oxidation and adsorption capability of UiO-66-NH2, the new mechanism provides a new strategy to further improve the NO removal efficiency of UiO-66-NH2 and a new way of inhibiting the deactivation.
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论文类型：期刊论文
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论文编号：108294
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卷号：10
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期号：5
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是否译文：否
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发表时间：2022-10-01
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收录刊物：SCI、EI
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发布期刊链接：https://www.sciencedirect.com/science/article/pii/S2213343722011678
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俞和胜
职务：Professor
主要任职：
个人信息
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博士生导师
硕士生导师 - 教师拼音名称：yuhesheng
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- 所在单位：化工学院
- 职务：Professor
- 办公地点：中国矿业大学文昌校区综合楼203
- 性别：男
- 学位：博士
- 职称：教授
- 毕业院校：加拿大滑铁卢大学
学术荣誉：
- 2020当选：江苏特聘教授
曾获荣誉：
- 2020-08-01江苏特聘教授
- 2014-10-15加拿大国家自然科学基金工业博士后奖学金
- 2020-08-01中国矿业大学“高端人才计划”攀登学者
- 2019-06-01江苏省“六大人才高峰”高层次人才
- 2018-06-28江苏省“双创博士”
- 2016-08-01AIChE Journal Editor’s Choice Paper
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