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高Ce/(Ce+Ce) 比例增强了n-十一烷在CeO/γ-AlO上的等离子体催化降解。

High ratio of Ce/(Ce+Ce) enhanced the plasma catalytic degradation of n-undecane on CeO/γ-AlO.

作者信息

Xia Tongtong, Yao Shuiliang, Wu Zuliang, Li Guojian, Li Jing

机构信息

School of Environmental and Safety Engineering, Advanced Plasma Catalysis Engineering Laboratory for China Petrochemical Industry, Changzhou University, Jiangsu 213164, China.

School of Environmental and Safety Engineering, Advanced Plasma Catalysis Engineering Laboratory for China Petrochemical Industry, Changzhou University, Jiangsu 213164, China.

出版信息

J Hazard Mater. 2022 Feb 15;424(Pt D):127700. doi: 10.1016/j.jhazmat.2021.127700. Epub 2021 Nov 5.

Abstract

n-Undecane (C11) is the main component of volatile organic compounds (VOCs) emitted from the printing industry, and its emission to the atmosphere should be controlled. In this study, a dielectric barrier discharge reactor coupled with CeO/γ-AlO catalysts was used to degrade C11. The effect of the chemical state of CeO on C11 degradation was evaluated by varying the CeO loading on γ-AlO. The C11 conversion and COx selectivity were as high as 92% and 80%, respectively, under mild reaction conditions of energy density 34 J/L and 423 K to degrade 134 mg/m C11 in a simulated air using 10 wt%CeO impregnated on γ-AlO. After analyses using in-situ plasma diffuse reflectance Fourier transform infrared spectroscopy and gas chromatography-mass spectrometry, it was found that most of C11 were degraded to CO, and the main by-products on catalyst surfaces were alcohols and ketones. It was concluded from X-ray photoemission spectroscopy that the good performance of the 10 wt%CeO/γ-AlO catalyst was due to its high Ce/(Ce+Ce) ratio as well as the oxygen vacancies. The Ce/(Ce+Ce) ratio of CeO on γ-AlO is crucial for the degradation of C11, providing a further roadmap for the plasma catalytic oxidation of alkanes.

摘要

正十一烷(C11)是印刷行业排放的挥发性有机化合物(VOCs)的主要成分,其向大气中的排放应受到控制。在本研究中,采用介质阻挡放电反应器与CeO/γ -Al₂O₃催化剂相结合来降解C11。通过改变γ -Al₂O₃上CeO的负载量,评估CeO化学状态对C11降解的影响。在能量密度为34 J/L和423 K的温和反应条件下,使用负载10 wt%CeO的γ -Al₂O₃在模拟空气中降解134 mg/m³的C11时,C11转化率和COx选择性分别高达92%和80%。通过原位等离子体漫反射傅里叶变换红外光谱和气相色谱 - 质谱分析发现,大部分C11被降解为CO,催化剂表面的主要副产物是醇类和酮类。通过X射线光电子能谱得出结论,10 wt%CeO/γ -Al₂O₃催化剂的良好性能归因于其高Ce³⁺/(Ce³⁺+Ce⁴⁺) 比率以及氧空位。γ -Al₂O₃上CeO的Ce³⁺/(Ce³⁺+Ce⁴⁺) 比率对于C11的降解至关重要,为烷烃的等离子体催化氧化提供了进一步的路线图。

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