How the interaction between In2O3-ZrO2 promotes the isobutene synthesis from ethanol?

被引:15
作者
Bronsato, Bruna J. da S. [1 ,2 ]
Zonetti, Priscila C. [2 ]
Moreira, Carla R. [3 ]
Mendoza, Cesar D. [4 ]
Maia da Costa, Marcelo E. H. [4 ]
Alves, Odivaldo C. [5 ]
de Avillez, Roberto R. [1 ]
Appel, Lucia G. [2 ]
机构
[1] 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
[2] Inst Nacl Tecnol, Div Catalise & Proc Quim, INT, Av Venezuela 82-518, BR-21081312 Rio De Janeiro, RJ, Brazil
[3] Ctr Caracterizacao Nanotecnol Mat & Catalise, Inst Nacl Tecnol, Av Venezuela 82, BR-20081312 Rio De Janeiro, RJ, Brazil
[4] Pontificia Univ Catolica Rio de Janeiro, Dept Fis, PUC Rio, Rua Marques de Sao Vicente 225, BR-22451900 Rio De Janeiro, RJ, Brazil
[5] Univ Fed Fluminense, Dept Fis Quim, Outeiro Sao Joao Batista S-N,Campus Valonguinho, BR-24020141 Niteroi, RJ, Brazil
关键词
India; Zirconia; Oxygen vacancies; EPR; Ethanol; Acetone; Isobutene; Acetaldehyde; cus; Ethanol-TPD; XPS; ZNXZRYOZ MIXED OXIDES; CO2; HYDROGENATION; INDIUM OXIDE; BIO-ETHANOL; METHANOL SYNTHESIS; DIRECT CONVERSION; ACID PROPERTIES; LOWER OLEFINS; LEWIS-ACID; SURFACE;
D O I
10.1016/j.cattod.2020.07.004
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
A physical mixture comprising In2O3 and ZrO2 and its components were employed as catalysts in the generation of isobutene from ethanol. These solids were characterized by means of several techniques such as EPR, HRTEM, XPS, XRD, N-2 physical adsorption, isopropanol-TPD, CO2-TPD, ethanol-TPD and pyridine adsorption. The addition of 7% of In2O3 to ZrO2 employing the physical mixture procedure generates a catalyst which shows physicochemical and catalytic properties which are not a linear combination of its components properties. This catalyst is not only much more active compared with In2O3 and ZrO2, but it also generates isobutene at high selectivity. The interaction between In2O3 and ZrO2 changes the quantity and strength of the acidic and basic sites. However, these modifications do not correlate with the catalytic behavior. The HRTEM data suggest that the epitaxy alignment occurs between these two oxides which might cause stresses in the In2O3 lattice. The XRD and XPS analysis have identified distortions in the In2O3 lattice provoked by ZrO2, which facilitate the generation of O vacancies and consequently increases the concentration of these species during the reaction. This phenomenon promotes the acetone and acetaldehyde syntheses which are very relevant intermediate of this cascade reaction. Thus, it can be suggested that the catalytic behavior of the modified physical mixture is associated with the In2O3 lattice distortions promoted by ZrO2.
引用
收藏
页码:224 / 233
页数:10
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