Low-temperature abatement of toluene over Mn-Ce oxides catalysts synthesized by a modified hydrothermal approach

• Published in: Applied surface science 2018-03, Vol.433, p.1025-1035
• Main Authors: Du, Jinpeng, Qu, Zhenping, Dong, Cui, Song, Lixin, Qin, Yuan, Huang, Na
• Format: Article
• Language: English
• Subjects: Mn-Ce solid solution; Modified hydrothermal approach; Reaction path; Toluene oxidation
• ISSN: 0169-4332; 1873-5584
• DOI: 10.1016/j.apsusc.2017.10.116

[Display omitted] •Mn-Ce solid solution forms by combining redox-precipitation and hydrothermal method.•Mn0.6Ce0.4O2 shows the highest activity with toluene complete conversion at 210°C.•Abundant Ce3+ and Mn3+ in catalyst facilitate the formation of oxygen vacancies.•Benzyl alcohol, carbonate and formate species are the crucial intermediates. Mn-Ce oxides catalysts were synthesized by a novel method combining redox-precipitation and hydrothermal approach. The results indicate that the ratio between manganese and cerium plays a crucial role in the formation of catalysts, and the textual properties as well as catalytic activity are remarked affected. Mn0.6Ce0.4O2 possesses a predominant catalytic activity in the oxidation of toluene, over 70% of toluene is converted at 200°C, and the complete conversion temperature is 210°C. The formation of Mn-Ce solid solution markedly improves the surface area as well as pore volume of Mn-Ce oxide catalyst, and Mn0.6Ce0.4O2 possesses the largest surface area of 298.5m2/g. The abundant Ce3+ and Mn3+ on Mn0.6Ce0.4O2 catalyst facilitate the formation of oxygen vacancies, and improve the transfer of oxygen in the catalysts. Meanwhile, it is found that cerium in Mn-Ce oxide plays a key role in the adsorption of toluene, while manganese is proved to be crucial in the oxidation of toluene, the cooperation between manganese and cerium improves the catalytic reaction process. In addition, the reaction process is investigated by in situ DRIFT measurement, and it is found that the adsorbed toluene could be oxidized to benzyl alcohol as temperature rises around 80–120°C that can be further be oxidized to benzoic acid. Then benzoic acid could be decomposed to formate and/or carbonate species as temperature rises to form CO2 and H2O. In addition, the formed by-product phenol could be further oxidized into CO2 and H2O when the temperature is high enough.