共 44 条
Experimental and theoretical insights into the reaction mechanism of spinel CuMn2O4 with CO in chemical-looping combustion
被引:29
作者:

Fang, Ruixue
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Huazhong Univ Sci & Technol, State Key Lab Coal Combust, Sch Energy & Power Engn, Wuhan 430074, Peoples R China Huazhong Univ Sci & Technol, State Key Lab Coal Combust, Sch Energy & Power Engn, Wuhan 430074, Peoples R China

Liu, Feng
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Huazhong Univ Sci & Technol, State Key Lab Coal Combust, Sch Energy & Power Engn, Wuhan 430074, Peoples R China Huazhong Univ Sci & Technol, State Key Lab Coal Combust, Sch Energy & Power Engn, Wuhan 430074, Peoples R China

Liu, Jing
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Huazhong Univ Sci & Technol, State Key Lab Coal Combust, Sch Energy & Power Engn, Wuhan 430074, Peoples R China Huazhong Univ Sci & Technol, State Key Lab Coal Combust, Sch Energy & Power Engn, Wuhan 430074, Peoples R China

Li, Yu
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h-index: 0
机构:
Huazhong Univ Sci & Technol, State Key Lab Coal Combust, Sch Energy & Power Engn, Wuhan 430074, Peoples R China Huazhong Univ Sci & Technol, State Key Lab Coal Combust, Sch Energy & Power Engn, Wuhan 430074, Peoples R China
机构:
[1] Huazhong Univ Sci & Technol, State Key Lab Coal Combust, Sch Energy & Power Engn, Wuhan 430074, Peoples R China
基金:
中国国家自然科学基金;
关键词:
Chemical-looing combustion;
Oxygen carrier;
Spinel CuMn2O4;
Density functional theory;
Reaction mechanism;
OXYGEN CARRIERS;
COMPOSITE-MATERIALS;
METAL-OXIDE;
CU;
MN;
PERFORMANCE;
SURFACE;
GASIFICATION;
FE;
D O I:
10.1016/j.apsusc.2021.150065
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:
Chemical-looping combustion has been regarded as a promising technology to realize low-cost CO2 separation. CuMn2O4 homogeneously combining Cu and Mn into spinel matrix is a potential oxygen carrier owing to the synergistically improved performance. The involved reaction mechanism of spinel CuMn2O4 with CO was systematically studied by experiments and theoretical calculations. Thermo-gravimetric analysis results suggested that CuMn2O4 can be reduced into Cu and MnO. The reactivity of CuMn2O4 is superior than that of Mn2O3 due to the existence of Cu. To further understand the improved reactivity of CuMn2O4, the interaction between CO and spinel CuMn2O4 was studied by density functional theory calculations. The results indicated that CO prefers to chemisorb at Mn site. The oxidation of CO on CuMn2O4 surface is found to be a three-step reaction including CO adsorption, CO diffusion and CO2 desorption. CO oxidation on CuMn2O4 surface is an exothermic reaction mainly limited by the CO diffusion step. The activation energy for oxidizing CO upon Mn-terminated surface is 64.59 kJ/mol. However, the rate-limiting-step possesses a lower activation energy (58.83 kJ/mol) over Cu-terminated surface due to the high reactivity of Cu. The calculated results can well explain the improved reactivity of spinel CuMn2O4 observed in the experiments.
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