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Investigating the differences of active oxygen species and carbonate species on the surface of Ce0.95M (M = Mn and Zr)0.05O2−δ catalysts prepared by the aerosol method during CO oxidation using operando TPR-DRIFTS-MS
Dalton Transactions ( IF 3.5 ) Pub Date : 2024-12-20 , DOI: 10.1039/d4dt02920h Jiacheng Xu, Yan Sun, Shuiliang Yao
Dalton Transactions ( IF 3.5 ) Pub Date : 2024-12-20 , DOI: 10.1039/d4dt02920h Jiacheng Xu, Yan Sun, Shuiliang Yao
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Surface oxygen species and carbonate species play an important role in CO oxidation. However, their essential relationsh with CO oxidation activity remains unclear. In this paper, Ce0.95M (M = Mn and Zr)0.05O2−δ catalysts are selected as the research target and operando TPR-DRIFTS-MS is used to investigate the changes of oxygen species and carbonate species on the catalyst surface. The Ce0.95Mn0.05O2−δ catalyst has the best CO conversion (145 °C) and CO2 selectivity (99%). Operando DRIFTS-MS results show that M![[double bond, length as m-dash]](https://www.rsc.org/images/entities/char_e001.gif)
O plays a key role on the catalyst surface and can react with CO at low temperatures. Importantly, the high content of MO is conducive to the formation of monodentate carbonate (M–O–CO2) (M–O–CO2 decomposes at 50 °C). As the temperature increases, CeO and M–O–Ce also react with CO and produce M–Ov–Ce (oxygen vacancies). CO can combine with O2 adsorbed on the M–Ov–Ce (M2+–O22−) to form bidentate carbonate (M–O2–CO). The decomposition temperature of M–O2–CO is much higher than that of M–O–CO2, and its existence is the decisive step of CO oxidation. The above results provide a new way to regulate the surface oxygen species and carbonate species of Ce based catalysts in the later stages.
更新日期：2024-12-20
O plays a key role on the catalyst surface and can react with CO at low temperatures. Importantly, the high content of MO is conducive to the formation of monodentate carbonate (M–O–CO2) (M–O–CO2 decomposes at 50 °C). As the temperature increases, CeO and M–O–Ce also react with CO and produce M–Ov–Ce (oxygen vacancies). CO can combine with O2 adsorbed on the M–Ov–Ce (M2+–O22−) to form bidentate carbonate (M–O2–CO). The decomposition temperature of M–O2–CO is much higher than that of M–O–CO2, and its existence is the decisive step of CO oxidation. The above results provide a new way to regulate the surface oxygen species and carbonate species of Ce based catalysts in the later stages.
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