Acetone synthesis from ethanol and the Mars and Van Krevelen mechanism using CeO2 and AgCeO2 nanostructured catalysts

被引:13
作者
de Lim, Adriana F. F. [1 ,2 ]
Moreira, Carla R. [3 ]
Alves, Odivaldo C. [4 ]
de Avillez, Roberto R. [5 ]
Zotin, Fatima M. Z. [2 ]
Appel, Lucia G. [1 ]
机构
[1] Inst Nacl Tecnol, Div Catalise & Proc Quim, Av Venezuela 82,Sala 518, BR-20081312 Rio De Janeiro, RJ, Brazil
[2] Univ Estado Rio de Janeiro, Inst Quim, Programa Posgrad Engn Quim, Ave Sao Francisco Xavier 524, BR-20550900 Rio De Janeiro, RJ, Brazil
[3] Inst Nacl Tecnol, Ctr Caracterizacao Nanotecnol Mat & Catalise, Av Venezuela 82,Anexo 3, BR-20081312 Rio De Janeiro, RJ, Brazil
[4] Univ Fed Fluminense, Inst Quim, Outeiro Sao Joao Batista S-N,Campus Valonguinho, BR-24020007 Niteroi, RJ, Brazil
[5] Pontificia Univ Catolica Rio de Janeiro, Dept Engn Quim & Mat, PUC Rio, Rua Marques de Sao Vicente 225, BR-22451900 Rio De Janeiro, RJ, Brazil
关键词
Ethanol; Acetaldehyde; Mars and Van Krevelen mechanism; CeO2; Acetone;
D O I
10.1016/j.apcata.2020.117949
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Nanostructured CeO2 based catalysts were employed as tools to shed light on the mechanism of the acetone synthesis from ethanol. The oxides were characterized using HRTEM, EPR, and other techniques. Rates of ethanol consumption and products formation were measured at differential conditions. The catalysts prepared employing Ce(NO3)(3) generate nanocubes, whereas when (NH4)(2)Ce(NO3)(6) is used, nanopolyhedral particles are synthesised. The later forms O vacancies more easily. This property enhances when Ag is added to the nanopolyhedral catalyst. The correlation between the catalytic behaviour and the nanocatalysts's physicochemical properties showed that O vacancies participate as Brunsted basic sites in the acetaldehyde synthesis and that the easier the O vacancies generation, the higher the rate of the acetone synthesis is. The O abstraction from the CeO2 lattice by acetaldehyde (Mars and Van Krevelen mechanism) is the slowest step of the acetone synthesis from ethanol, showing that this synthesis exhibits a relevant redox characteristic.
引用
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页数:10
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