High entropy oxide catalysts with SO2 resistance in RWGS reaction

被引:4
|
作者
Zhang, Mengyuan [1 ,2 ]
Lu, Xiaoyan [1 ]
Luo, Kongliang [1 ]
Ye, Jian [1 ]
Dong, Jia li [1 ]
Lu, Nana [1 ]
Wang, Xiaopeng [1 ]
Niu, Qiang [3 ]
Zhang, Pengfei [1 ,2 ]
Dai, Sheng [4 ]
机构
[1] Ningxia Univ, Coll Chem & Chem Engn, State Key Lab High Efficiency Utilizat Coal & Gree, Yinchuan 750021, Peoples R China
[2] Shanghai Jiao Tong Univ, Sch Chem & Chem Engn, Shanghai 200240, Peoples R China
[3] Inner Mongolia Erdos Elect Power & Met Grp Co Ltd, Natl Enterprise Technol Ctr, Ordos 016064, Inner Mongolia, Peoples R China
[4] Oak Ridge Natl Lab, Chem Sci Div, Oak Ridge, TN 37830 USA
关键词
High entropy oxide; SO; 2; resistance; Entropy engineering; In situ FTIR; In situ XPS; RWGS reaction; REDUCTION; MECHANISM; NOX;
D O I
10.1016/j.apcatb.2024.123845
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Ubiquitous presence of SO2 usually shows adverse effects on industrial catalysis. Herein, a concept of engineering entropy to design SO2 resistance oxide catalysts is proposed. (Ni0.2Mg0.2Cu0.2Zn0.2Co0.2)Fe2O4 showed excellent performance (the CO2 conv. = 41.4%, CO selec. = 99.6% at 400 degrees C) compared to the control samples in the reverse water-gas shift (RWGS). In addition, (Ni0.2Mg0.2Cu0.2Zn0.2Co0.2)Fe2O4 had the SO2-tolerant ability (the CO2 conv. = 38.5%, CO selec. = 99.2% at 400 degrees C) after being poisoned with 1000 ppm SO2 at 400 degrees C for 1 h. In sharp contrast, the control samples NiFe2O4, MgFe2O4, CuFe2O4 and CoFe2O4 lost their activity. O-1S XPS indicated that (Ni0.2Mg0.2Cu0.2Zn0.2Co0.2)Fe2O4 had higher oxygen vacancy concentrations. SO2 resistance mechanism was studied by infrared spectroscopy, SO2-TPD, in situ S 2p XPS and the DFT results, confirming that the low SO2 adsorption energy of (Ni0.2Mg0.2Cu0.2Zn0.2Co0.2)Fe2O4, which was attributed to the lower Gibbs free energy. This work may inspire the rational design of SO2-resistant catalysts.
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页数:12
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