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Catalytic ozonation of NH4+-N in wastewater over composite metal oxide catalyst
Journal of Rare Earths ( IF 4.9 ) Pub Date : 2020-11-11 , DOI: 10.1016/j.jre.2020.11.003
Caiqing He , Yunnen Chen , Lin Guo , Ruoyu Yin , Tingsheng Qiu

Large amounts of water containing-ammonium nitrogen (NH4+-N) have attracted increasing attention. Catalytic ozonation technology, involving the generation of hydroxyl radical (·OH) with strong oxidation ability, was originally utilized to degrade organic-containing wastewater. In this paper, Ce/MnOx composite metal oxide catalysts prepared with different preparation conditions were used to degrade wastewater containing inorganic pollutant (NH4+-N). The as-prepared catalyst features were characterized using X-ray diffraction (XRD), Brunauer–Emmett–Teller method (BET), scanning electron microscopy (SEM), energy dispersive X-ray spectroscopy (EDS), Fourier transform infrared spectroscopy (FT-IR), X-ray photoelectron spectroscopy (XPS) and H2-temperature programmed reduction (H2-TPR) techniques. The results show that the catalyst, prepared by conditions with precipitant Na2CO3 and Ce/Mn molar ratio 1:2 calcined at 400 °C for 3 h in pH 11.0, displays the optimal performance, with the removal rate of NH4+-N and selectivity to gaseous nitrogen, 88.14 wt% and 53.67 wt%, respectively. The effects of several operating factors including solution pH, initial NH4+-N concentrations and scavengers were evaluated. In addition, XRD patterns of catalyst with the best performance and the comparative study on decontamination of NH4+-N by various processes (O3, catalyst and catalyst/O3) show that the primary metal oxides are CeO2 and MnO2 in Ce/MnOx composite metal oxide catalysts, which have a synergistic effect on the catalytic ozonation of NH4+-N, and the new phase MnO2 plays a great role. After 5 consecutive use cycles, the degradation efficiency is declined slightly, and can still achieve better than 70 wt% over 1 h reaction. Additionally, the application of catalytic ozonation for actual wastewater on the removal rate of NH4+-N was investigated. Possible mechanism and degradation pathway of NH4+-N were also proposed. In a word, the application of CeO2–MnO2 composite metal oxide catalysts in catalytic ozonation can be regarded as an effective, feasible and promising method for the treatment of NH4+-N.



中文翻译:

复合金属氧化物催化剂催化臭氧化废水中NH4+-N

大量含有铵态氮(NH 4 + -N)的水引起了越来越多的关注。催化臭氧化技术涉及产生具有强氧化能力的羟基自由基(·OH),最初用于降解含有机废水。本文采用不同制备条件制备的Ce/MnO x复合金属氧化物催化剂对含无机污染物(NH 4 +-N)。使用 X 射线衍射 (XRD)、Brunauer-Emmett-Teller 方法 (BET)、扫描电子显微镜 (SEM)、能量色散 X 射线光谱 (EDS)、傅里叶变换红外光谱 (FT -IR)、X 射线光电子能谱 (XPS) 和 H 2 -程序升温还原 (H 2 -TPR ) 技术。结果表明,在沉淀剂 Na 2 CO 3和 Ce/Mn 摩尔比 1:2条件下制备的催化剂在 400 °C、pH 11.0 条件下煅烧 3 h,表现出最佳性能,NH 4 +去除率较高。-N 和对气态氮的选择性,分别为 88.14 wt% 和 53.67 wt%。评估了几个操作因素的影响,包括溶液 pH 值、初始 NH 4 + -N 浓度和清除剂。此外,性能最好的催化剂的XRD图谱和不同工艺(O 3、催化剂和催化剂/O 3)去除NH 4 + -N的对比研究表明,主要金属氧化物为CeO 2和MnO 2。 Ce/MnO x复合金属氧化物催化剂,对NH 4 + -N的催化臭氧化具有协同作用,新相MnO 2起着很大的作用。连续使用 5 次循环后,降解效率略有下降,1 h 反应仍能达到 70 wt% 以上。此外,还研究了催化臭氧化处理实际废水对NH 4 + -N去除率的影响。还提出了NH 4 + -N 的可能机理和降解途径。总之,CeO 2 -MnO 2复合金属氧化物催化剂在催化臭氧化反应中的应用是一种有效、可行、有前景的NH 4 + -N处理方法。

更新日期:2020-11-11
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