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Removal of organics and ammonia in landfill leachate via catalytic oxypyrolysis over MOF-derived Fe2O3@SiO2-Al2O3
Separation and Purification Technology ( IF 8.1 ) Pub Date : 2022-10-28 , DOI: 10.1016/j.seppur.2022.122467
Tao Wei , Bochen Zhao , Zihan Zhou , Hongxiang Di , Tapiwanashe Shumba , Mifen Cui , Zhe Zhou , Xihua Xu , Min Qi , Jihai Tang , Patrick G. Ndungu , Xu Qiao , Zhuxiu Zhang

Landfill leachate has a severe impact on both human health and ecosystem. To address this matter, we report herein a systematic study of a new oxypyrolysis process composed of cracking-combustion coupled reactions over Fe2O3@SiO2-Al2O3 catalyst for the removal of organics and ammonia in landfill leachate. Fe2O3@SiO2-Al2O3, which contains Brönsted acidity and oxidative sites, is derived from calcination of iron-based MIL-101 nanocast with silica-alumina sol. Fluidized-bed experiments at 339 ℃ reveal the exceptional catalytic activity of Fe2O3@SiO2-Al2O3 as manifested by the high removal efficiency of COD (99.2 %) and NH3-N (95.2 %). The concentration of COD and ammonia nitrogen in the condensed effluent is as low as 18.1 mg/L and 78.9 mg/L respectively, the best performance yet seen in other chemical treatment approaches. The non-condensable gas from the oxypyrolysis reaction only contains CO2, N2 and a trace amount of nonmethane hydrocarbons. Insight into oxypyrolysis reaction is provided by thermogravimetric-gas chromatography/mass spectrometry and in-situ infrared spectroscopy. The amorphous SiO2-Al2O3 enables the catalytic cracking of heavy fractions in landfill leachate to small organic molecules, and the Fe2O3 nanoparticles realize the catalytic combustion of small organic molecules and ammonia to CO2, H2O and N2. A theoretical analysis of the operation cost estimate shows that the oxypyrolysis reaction is among the most cost-effective treatment methods. Taken together, these findings suggest that the oxypyrolysis is highly applicable for the leachate treatment.



中文翻译:

MOF衍生Fe2O3@SiO2-Al2O3催化氧解去除垃圾渗滤液中的有机物和氨

垃圾渗滤液对人类健康和生态系统都有严重影响。为了解决这个问题,我们在此报告了一种新的氧裂解过程的系统研究,该过程由 Fe 2 O 3 @SiO 2 -Al 2 O 3催化剂上的裂解-燃烧耦合反应组成,用于去除垃圾渗滤液中的有机物和氨。Fe 2 O 3 @SiO 2 -Al 2 O 3含有布朗斯台德酸度和氧化位点,源自铁基 MIL-101 纳米铸件与硅铝溶胶的煅烧。339 ℃流化床实验揭示了Fe 2 O 3的优异催化活性@SiO 2 -Al 2 O 3表现为对 COD (99.2 %) 和 NH 3 -N (95.2 %) 的高去除效率。冷凝出水的 COD 和氨氮浓度分别低至 18.1 mg/L 和 78.9 mg/L,是迄今为止其他化学处理方法中表现最好的。来自氧裂解反应的不凝气仅含有CO 2、N 2和微量的非甲烷烃。通过热重-气相色谱/质谱和原位红外光谱提供对氧解反应的深入了解。无定形SiO 2 -Al 2 O 3能够将垃圾渗滤液中的重质馏分催化裂解为有机小分子,Fe 2 O 3纳米颗粒实现有机小分子和氨催化燃烧生成CO 2、H 2 O和N 2。运行成本估算的理论分析表明,氧裂解反应是最具成本效益的处理方法之一。总之,这些发现表明,氧热解非常适用于渗滤液处理。

更新日期:2022-11-02
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