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Surface properties enhanced MnxAlO oxide catalysts derived from MnxAl layered double hydroxides for acetone catalytic oxidation at low temperature
Sun, Yonggang; Zhang, Xin; Li, Na; Xing, Xin; Yang, Hongling; Zhang, Fenglian; Cheng, Jie; Zhang, Zhongshen; Hao, Zhengping
2019-08-15
Source PublicationAPPLIED CATALYSIS B-ENVIRONMENTAL
ISSN0926-3373
Volume251Pages:295-304
AbstractMnxAlO mixed oxide catalysts derived from MnxAl-LDHs were prepared and tested for acetone catalytic oxidation. Detailed results indicated that the surface intrinsic and formed oxygen vacancies can induce the Mn-O bond of structural unit [MnO6] weakened. Subsequently, it can improve the redox properties of catalysts, and enhance the capacity of gaseous oxygen species dissociation and adsorption. Among them, Mn3AlO catalyst displayed the best catalytic performance for acetone oxidation (T-90 = 164 degrees C) with the production of low amount of byproduct (< 5 ppm) and high CO2 yield (> 99%) producted. Additionally, the Mn3AlO catalyst can proceed consecutively for 12 h reaction without notable deactivation. Furthermore, in situ DRIFT and theoretical calculations methods was adopted to explore the reaction mechanism. And eta 1(O)((ads)) (adsorption mode of acetone), CH2=C(CH3)=O-(ads), O*, CH3CHO*, CH2O* and COO(ads) were considered as the main intermediate species and/or transient state during the reaction process. It was revealed that the acetone and oxygen molecules were activated by the dehydrogenation (alpha-H abstraction) and dissociation process over Mn3AlO catalyst, respectively, and then the intermediate specie, CH2C(CH3)O and O*, were produced, which was followed by the breaking of -C-C- bonds to produce the CH3CHO* and CH2O* species. Finally, these species were attacked by dissociated oxygen (O*) and therefore further dehydrogenation occurred, form H2O and CO2 via the COO- adsorbed species. Particularly, -C-C- bond breaking was the main rate determining step for acetone oxidation.
Department环境纳米技术与健康效应重点实验室
KeywordSurface properties Acetone Layered double hydroxides Catalytic activity Reaction mechanism
Document Type期刊论文
Identifierhttps://ir.rcees.ac.cn/handle/311016/43213
Collection环境纳米技术与健康效应重点实验室
Affiliation1.Univ Chinese Acad Sci, Natl Engn Lab VOCs Pollut Control Mat & Technol, Beijing 101408, Peoples R China
2.Chinese Acad Sci, Res Ctr Ecoenvironm Sci, Beijing 100085, Peoples R China
Recommended Citation
GB/T 7714
Sun, Yonggang,Zhang, Xin,Li, Na,et al. Surface properties enhanced MnxAlO oxide catalysts derived from MnxAl layered double hydroxides for acetone catalytic oxidation at low temperature[J]. APPLIED CATALYSIS B-ENVIRONMENTAL,2019,251:295-304.
APA Sun, Yonggang.,Zhang, Xin.,Li, Na.,Xing, Xin.,Yang, Hongling.,...&Hao, Zhengping.(2019).Surface properties enhanced MnxAlO oxide catalysts derived from MnxAl layered double hydroxides for acetone catalytic oxidation at low temperature.APPLIED CATALYSIS B-ENVIRONMENTAL,251,295-304.
MLA Sun, Yonggang,et al."Surface properties enhanced MnxAlO oxide catalysts derived from MnxAl layered double hydroxides for acetone catalytic oxidation at low temperature".APPLIED CATALYSIS B-ENVIRONMENTAL 251(2019):295-304.
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