Nickel doping MnO2 with abundant surface pits as highly efficient catalysts for propane deep oxidation

被引:85
作者
Chen, Long [1 ]
Jia, Jingbo [2 ]
Ran, Rui [2 ]
Song, Xiping [1 ]
机构
[1] Univ Sci & Technol Beijing, State Key Lab Adv Met & Mat, Beijing 100083, Peoples R China
[2] Tsinghua Univ, Key Lab Adv Mat MOE, Sch Mat Sci & Engn, Beijing 100084, Peoples R China
基金
国家重点研发计划;
关键词
Nickel doping MnO2; Surface pit; Propane deep oxidation; Structural defects; In situ DRIFTS; REACTION-MECHANISM; PROMOTIONAL ROLE; OXIDE; COMBUSTION; PERFORMANCE; PT/AL2O3; ACID;
D O I
10.1016/j.cej.2019.03.142
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Series of nickel doping MnO2 with irregular surface pits were synthesized and employed for propane deep oxidation. The partial substitution of Ni for Mn resulted in the formation of structural defects, which could be observed by high-resolution transmission electron microscopy. The MnNi0.09 sample exhibited the best catalytic activity for propane oxidation with the conversion of 90% at 220 degrees C. The presence of pits on the MnNi0.09 sample could facilitate the dissociation of propane and mobility of oxygen along the conduction channels of surface pits, thus promoting the catalytic efficiency. Moreover, the in situ studies found that different intermediates were formed on the MnO2 and MnNi0.09 catalysts during the propane oxidation process. The propane was oxidized to propanoyl species on the surface of MnO2 catalyst, while it was oxidized to hydrogen carbonates and carbonates on the surface of MnNi(0.09 )sample, which were thermally less stable and converted into CO2 at lower temperature. The finding provides a new perspective on understanding the effect of cation doping.
引用
收藏
页码:1129 / 1137
页数:9
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