Atomically dispersed SrOx species on exposed {222} facets of pyrochlore La2Zr2O7 nanocrystals for boosting low-temperature oxidative coupling of methane

被引:14
|
作者
Wu, Tongtong [1 ]
Wei, Yuechang [1 ,2 ]
Xiong, Jing [1 ,2 ]
Yang, Yitao [1 ]
Han, Dawei [1 ]
Zhao, Zhen [1 ]
Liu, Jian [1 ]
机构
[1] China Univ Petr, State Key Lab Heavy Oil Proc, Beijing 102249, Peoples R China
[2] China Univ Petr, Key Lab Opt Detect Technol Oil & Gas, Beijing 102249, Peoples R China
基金
中国国家自然科学基金; 北京市自然科学基金;
关键词
Strontium oxide; Pyrochlore La2Zr2O7; {222} facet; Low-temperature oxidative coupling of methane; O-2(-) species; Alkaline sites; METAL-OXIDE ADDITIVES; IN-SITU IR; RARE-EARTH; VIBRATIONAL-SPECTRA; GLYCEROL CARBONATE; CATALYSTS; SURFACE; OXYGEN; CO2; ZR;
D O I
10.1016/j.fuel.2022.126479
中图分类号
TE [石油、天然气工业]; TK [能源与动力工程];
学科分类号
0807 ; 0820 ;
摘要
The efficient catalysts of strontium oxide (SrOx) supported on exposed {222} facets of pyrochlore La2Zr2O7 nanocrystals (SrOx/LZO-Y) were elaborately synthesized by incipient wetness impregnation method. The introduction of atomically dispersed SrOx species on La2Zr2O7 surface can increase the amount of surface oxygen vacancies induced by Sr2+ substitution of La3+ cations, and the increasing of moderate surface alkaline sites are beneficial to enhance catalytic performance for oxidative coupling of methane (OCM). The SrOx/LZO-Y catalysts have super catalytic performance during low-temperature OCM reaction. SrOx/LZO-12 catalyst with the highest concentrations of O-2(-) species exhibits the highest activity and the lowest apparent activation energy (84 kJ mol(-1)) during low-temperature OCM into C2H4 and C2H6 (C-2) products, i.e., its CH4 conversion, selectivity and yield of C-2 products at 600 degrees C are 30.5 %, 47.4 % and 14.5 %, respectively, and its ratio of C2H4/C2H6 products is 0.77. Based on the results of multiple experimental characterizations, the mechanism of SrOx/LZO-Y catalysts for OCM reaction is proposed: the surface alkaline active centers (O-2(-)) induced by doping of Sr ions can promote the critical step of CH4 activation significantly during low-temperature OCM reaction. It is a new strategy to develop the low-temperature and high-activity catalysts for OCM in practical application.
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页数:14
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