Citation: MENG Hao, LIN Ming-gui, NIU Peng-yu, WANG Jun-gang, HOU Bo, LI De-bao. Effect of phase transformation of La₂Zr₂O₇ catalysts on catalytic performance for the oxidative coupling of methane[J]. Journal of Fuel Chemistry and Technology, ;2020, 48(8): 949-959. shu

Effect of phase transformation of La₂Zr₂O₇ catalysts on catalytic performance for the oxidative coupling of methane

MENG Hao ^1,2 ,
LIN Ming-gui ^1,, ,
NIU Peng-yu ¹ ,
WANG Jun-gang ¹ ,
HOU Bo ¹ ,
LI De-bao ^1,3,,

1.
State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001, China
2.
University of Chinese Academy of Sciences, Beijing 100049, China
3.
Dalian National Laboratory for Clean Energy, Dalian 116023, China

Corresponding author: LIN Ming-gui, linmg@sxicc.ac.cn LI De-bao, dbli@163.com
Received Date: 30 March 2020
Revised Date: 9 July 2020

Fund Project: The project was supported by Science and Technology Plan Unveiling Bidding Project of Shanxi (20191102006) and the Autonomous Research Project of State Key Laboratory of Coal Conversion (2020BWZ003)Autonomous Research Project of State Key Laboratory of Coal Conversion 2020BWZ003Science and Technology Plan Unveiling Bidding Project of Shanxi 20191102006

Figures(11)

La₂Zr₂O₇ catalyst was prepared using co-precipitation method and then calcined at different temperatures to obtain a series of catalysts with different phase structures. Their catalytic performances for oxidative coupling of methane were evaluated in a fixed bed micro-reactor. Meanwhile, the changes of phase structure, surface base sites and surface oxygen species upon these samples were characterized with XRD, Raman, CO₂-TPD, and XPS. With the increase of the calcination temperature from 700 to 1200℃, the crystallinity of La₂Zr₂O₇ catalysts increased continuously and the crystal phase changed obviously. The structure of the catalysts gradually changed from amorphous to disordered defective fluorite structure, and ultimately to phrochlore structure. Both the number of medium basic sites and the electrophilic oxygen species, such as O₂^2- and O₂^-, on the catalysts decreased with the phase transition caused by the temperature raising, resulting in the decrease of CH₄ conversion and C₂₊ selectivity. The amorphous LZO-CP-700 catalyst showed the best performance in methane oxidation coupling reaction.
- La₂Zr₂O₇,
- structural change,
- surface base,
- oxygen species,
- oxidative coupling of methane
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Effect of phase transformation of La₂Zr₂O₇ catalysts on catalytic performance for the oxidative coupling of methane