Catalytic Combustion of Lean Methane Assisted by Electric Field over Pd/Co3O4 Catalysts at Low Temperature
Catalytic Combustion of Lean Methane Assisted by Electric Field over Pd/Co3O4 Catalysts at Low Temperature
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Pd/Co3O4 催化剂电场辅助贫甲烷低温催化燃烧
DOI：
10.1007/s12204-018-2017-7
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发表时间：
2018-12
期刊：
影响因子：
--
通讯作者：
Huang Zhen
中科院分区：
文献类型：
--
作者：
Liu Ke;Li Ke;Xu Dejun;Lin He;Guan Bin;Chen Ting;Huang Zhen
采用自蔓延高温合成（SHS）法制备了一系列Pd/Co 3 O 4催化剂，并在其上施加电场进行了低温贫甲烷催化燃烧的研究。施加电场后，Pd/Co 3 O 4催化剂的催化燃烧性能得到了很大的改善，电场的施加可以在一定程度上降低活性元素Pd的负载量，同时保持相同的效率。结合X射线衍射（XRD）、X射线光电子能谱（XPS）、氢程序升温还原（H2-TPR）和原位漫反射红外光谱（in-situ DRIFTS）分析结果，探讨了电场作用下Pd/Co 3 O 4催化剂催化氧化CH 4的机理。一般情况下，甲烷的催化燃烧只有在温度高于250 °C时才发生，而施加电场后，甲烷的整个氧化过程得到明显的促进，反应温度降低。电场能促进载体Co 3 O 4还原释放晶格氧，增加PdOx和表面化学吸附氧，为CH 4低温氧化提供更多活性位。此外，电场可以促进CoOOH的脱羟基反应，进一步提高催化剂的活性。
A series of Pd/Co3O4 catalysts were prepared by Self-Propagating High-Temperature Synthesis (SHS) method in this study, and electric field was applied for catalytic combustion of lean methane over Pd/Co3O4 catalysts at low temperature. When electric field was applied, the catalytic combustion performance of Pd/Co3O4 catalysts was greatly improved, and the application of electric field could reduce the load of active element Pd to some extent while maintaining the same efficiency. Based on experimental tests and the analysis results of X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), H2-temperature-programmed reduction (H2-TPR) and in-situ diffuse reflectance infrared Fourier transform spectroscopy (in-situ DRIFTS), the mechanism of catalytic oxidation of CH4 over Pd/Co3O4 catalysts in electric field was proposed. The catalytic combustion of CH4 occurs only when the temperature is higher than 250 °C normally, but when electric field was applied, the whole process of CH4 oxidation was promoted significantly and the reaction temperature was reduced. Electric field could promote the reduction of the support Co3O4 to release the lattice oxygen, resulting in the increase of PdOx and the surface chemisorbed oxygen, which could provide more active sites for the low-temperature oxidation of CH4. Furthermore, electric field could accelerate the dehydroxylation of CoOOH to further enhance the activity of the catalysts.
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