Investigation of supported palladium catalysts for combustion of methane: The activation effect caused by SO2

被引:44
作者
Ding, Ya [1 ,2 ]
Wang, Sheng [1 ]
Zhang, Lei [1 ,2 ]
Lv, Lirong [1 ,2 ]
Xu, Dekang [1 ,2 ]
Liu, Wei [1 ]
Wang, Shudong [1 ]
机构
[1] Chinese Acad Sci, Dalian Inst Chem Phys, Dalian Natl Lab Clean Energy, Dalian 116023, Peoples R China
[2] Univ Chinese Acad Sci, Beijing 100049, Peoples R China
基金
中国国家自然科学基金;
关键词
Ceria-zirconia solid solution; Pd; Catalytic combustion; SO2; Activation; Acidity; PD-BASED CATALYSTS; LOW-TEMPERATURE; PROPANE OXIDATION; SULFUR-DIOXIDE; HIGH-STABILITY; CO OXIDATION; MIXED-OXIDE; REDUCTION; CERIA; DEACTIVATION;
D O I
10.1016/j.cej.2019.122969
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Catalytic combustion of methane was studied over Ce0.5Zr0.5O2 and CeO2 supported Pd (Pd/CZ and Pd/Ce) catalysts in the presence of SO2. The effect of sulfation (air including 100 ppm SO2 for 6 h at 500 degrees C) on the sulfur-tolerant performance of the catalysts was also investigated. Results indicated that there is a considerable promotion effect for CH4 complete oxidation on Pd/CZ catalyst, while the activity of Pd/Ce catalyst was inevitably inhibited. Further, the superior sulfur-tolerant behavior of Pd/CZ was verified through a 50 h time-on-stream stability test. Mechanistic insights into the synergistic effect between the support and Pd were unveiled by Raman, H-2-TPR, XPS, NH3-TPD, DRIFTS, HAADF-STEM, etc. It was deduced that the formation of sulfates at the Pd-support interface could promote the dissociative adsorption of methane on Pd/CZ catalyst. Meanwhile, the higher relative acid strength and the acid amount were also decisive factors for the high sulfur-resistant performance. The enhanced acid strength and acid amount prevented the further formation of bulk-like sulfate species for the SO2 treated Pd/CZ catalyst, thus enhancing the sulfur-tolerant ability of the catalyst.
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页数:12
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