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Role of different coordinated Cu and reactive oxygen species on the highly active Cu-Ce-Zr mixed oxides in NH3-SCO: a combined in situ EPR and O-2-TPD approach

发表时间:2019-03-13
点击次数:
论文类型:
期刊论文
第一作者:
Qu, Zhenping
通讯作者:
Qu, ZP (reprint author), Dalian Univ Technol, Key Lab Ind Ecol & Environm Engn, Sch Environm Sci & Technol, Dalian 116024, Peoples R China.
合写作者:
Wang, Zhong,Zhang, Xiaoyu,Wang, Hui
发表时间:
2016-01-01
发表刊物:
CATALYSIS SCIENCE & TECHNOLOGY
收录刊物:
SCIE、EI
文献类型:
J
卷号:
6
期号:
12
页面范围:
4491-4502
ISSN号:
2044-4753
摘要:
Novel Cu-Ce-Zr mixed oxides were synthesized by a citric acid sol-gel method, and they exhibited an excellent NH3-SCO activity (180 degrees C, TOF = 1.33 h(-1)). The finely dispersed CuO, Cu-Ce-Zr solid solution and monomeric Cu2+ ions in octahedral sites were the main active sites. The finely dispersed CuO species were the NH3 adsorption sites, and their adsorption capacity could be improved by their good reducibility. The Cu-Ce-Zr solid solution was an important intermediate in oxygen transfer from bulk to surface. In situ EPR analysis indicated that the isolated Cu2+ located in the octahedral sites was more active compared with that located in the square-planar pyramidal sites, and it induced the formation of more Cu-Ce-Zr solid solution. Meanwhile, the in situ O-2-TPD results showed that both adsorbed oxygen and bulk lattice oxygen were the active oxygen adspecies, and the adsorbed oxygen molecules were more active than the bulk lattice oxygen in NH3 oxidation.
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