Theoretical study about adsorbed oxygen reduction over χ-Fe5C2: formation of H2O and CO2

被引：8
|
作者：
Bai, Ya [1 ,2 ,3 ]
Liu, Jinjia [2 ,3 ]
Wang, Tao [1 ]
Song, Yu-Fei [1 ]
Li, Yong-Wang [2 ,3 ]
Yang, Yong [2 ,3 ]
Wen, Xiaodong [2 ,3 ]
机构：
[1] Beijing Univ Chem Technol, Beijing Adv Innovat Ctr Soft Matter Sci & Engn, State Key Lab Chem Resource Engn, Beijing 100029, Peoples R China
[2] Chinese Acad Sci, Inst Coal Chem, State Key Lab Coal Convers, Taiyuan 030001, Peoples R China
[3] Synfuels China Co Ltd, Natl Energy Ctr Coal Clean Fuels, Beijing 101400, Peoples R China
来源：
MOLECULAR CATALYSIS | 2022年 / 524卷
基金：
中国国家自然科学基金;
关键词：
heterogeneous catalysis; oxidation; adsorbed oxygen; mechanism; Fe5C2; FISCHER-TROPSCH SYNTHESIS; FINDING SADDLE-POINTS; GENERALIZED GRADIENT APPROXIMATION; WATER DISSOCIATIVE ADSORPTION; DENSITY-FUNCTIONAL THEORY; ELASTIC BAND METHOD; IRON CARBIDE; TUNGSTEN CARBIDE; STRENGTH DEGRADATION; MAGNETIC-PROPERTIES;
D O I：
10.1016/j.mcat.2022.112236
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：
The removal of surface oxygen adsorbed on iron carbides is essential to protect the nanoparticle from oxidation in heterogeneous catalysis. Herein, we explored the removal of pre-adsorbed oxygen on seven facets of chi-Fe5C2, and four pathways including both direct and indirect routes for generating H2O and CO2 were investigated. The removal mechanism shows diversity over different facets. On (010), the formation of CO2 through the reaction between surface oxygen and adsorbed CO is more favorable. While on (510), (001), (110), (11-1) and (-411), the elimination in the form of H2O through OH disproportionation dominates. In particular, surface oxygen can be removed facilely either in H2O or CO2 on (111) surface. What's more, surface with more carbons exhibits higher barriers to direct CO2 formation, like (110) and (111). Our work provides knowledge about mechanism of O removal and CO2 formation, which may be helpful in protecting the nanoparticle from further oxidation.
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页数：7
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