Conversion of CO2(g) to CO(g) via reverse water-gas shift cycle on mixed cerium/praseodymium oxides at 500 °C

被引:1
|
作者
Pomiro, Federico J. [1 ,2 ]
Fouga, Gaston G. [2 ,3 ]
Tamietti, Agustin E. [2 ]
Bohe, Ana E. [2 ,3 ,4 ]
De Micco, Georgina [2 ,3 ]
机构
[1] Univ Nacl San Martin, Inst Tecnol Jorge A Sabato, Comis Nacl Energia Atom, Buenos Aires, Argentina
[2] Ctr Atom Bariloche, Dept Fisicoquim & Control Cal, Complejo Tecnol Pilcaniyeu, Comis Nacl Energia Atom, San Carlos De Bariloche, Rio Negro, Argentina
[3] Consejo Nacl Invest Cient & Tecn CONICET, Buenos Aires, Argentina
[4] Univ Nacl Comahue, Ctr Reg Univ Bariloche, RA-8400 San Carlos De Bariloche, Rio Negro, Argentina
关键词
Ce/Pr oxides; RWGS; CO; 2; conversion; CO generation; X-RAY-DIFFRACTION; CATALYTIC APPLICATIONS; THERMAL-DECOMPOSITION; DOPED CERIA; OXIDATION;
D O I
10.1016/j.cej.2024.155222
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Reactions of cerium/praseodymium oxides under hydrogen atmospheres, and subsequently, carbon dioxide, involved in chemical looping reverse water-gas shift cycles (RWGS) at 500 degrees C were investigated by in-situ hightemperature X-ray powder diffraction, FTIR and thermogravimetry. The RWGS cycle is a critical chemical process for converting carbon dioxide into useful products, such as carbon monoxide, which can be used to synthesize fuels and chemicals. The mixed oxides exploit the redox properties of Ce and Pr, which can switch between oxidation states, making them suitable for oxygen incorporation and release during the RWGS process allowing them to react with H2(g), and subsequently with CO2(g), promoting their interaction and conversion into H2O(g) and CO(g). Pure cerium and praseodymium oxides showed poor CO2(g) conversion efficiency. However, we found that nanometric Ce/Pr mixed oxides exhibit enhanced oxyreduction performance suitable for this application, particularly with a composition of 75 mol% Ce and 25 mol% Pr, significantly improved performance, achieving an average CO(g) yield of 0.6 mmol/(goxide.cycle) and a maximum rate of 0.26 mmol/ (goxide.min). Pr enhances oxygen mobility in CeO2, which improves the dissociation of C & boxH;O bonds in CO2(g). This is because the remaining oxygen atoms are delivered more quickly to the support sink, thereby cleaning up the vacant sites generated during the reduction step. These findings suggest that Ce/Pr mixed oxides are highly effective for CO2(g) conversion to CO(g) via RWGS cycle, offering a potentially viable option for industrial application.
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页数:13
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