Probing the functionality of nanostructured MnCeOx catalysts in the carbon monoxide oxidation Part I. Influence of cerium addition on structure and CO oxidation activity

被引:53
作者
Arena, Francesco [1 ]
Di Chio, Roberto [1 ]
Fazio, Barbara [2 ]
Espro, Claudia [1 ]
Spiccia, Leone [3 ]
Palella, Alessandra [4 ]
Spadaro, Lorenzo [4 ]
机构
[1] Univ Messina, Dipartimento Ingn, Viale F Stagno DAlcontres 31, I-98166 Messina, Italy
[2] Inst CNR, Ist & Proc Chim Fis, Viale F Stagno DAlcontres 37, I-98158 Messina, Italy
[3] Monash Univ, Sch Chem, Melbourne, Vic 3800, Australia
[4] Inst CNR ITAE Nicola Giordano, Via Salita S Lucia 5, I-98126 Messina, Italy
关键词
Nanostructured MnCeOx catalysts; Structural and electronic effects; CO oxidation; Structure-activity relationships; Active sites; OXYGEN REDUCTION REACTION; PHASE SELECTIVE OXIDATION; MN-BASED CATALYSTS; WET OXIDATION; OXIDE CATALYSTS; MIXED OXIDES; MNOX-CEO2; CATALYSTS; RAMAN-SPECTROSCOPY; LOW-TEMPERATURES; BENZYL ALCOHOL;
D O I
10.1016/j.apcatb.2017.03.049
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
The effects of cerium addition on the physico-chemical properties and CO oxidation activity of nanostructared MnCeOx catalysts (0 <= C-Ce <= 1) have been assessed. Irrespective of the loading, cerium hinders any significant long-range crystalline order promoting surface exposure, oxide dispersion, and reducibility of composite catalysts. Noticeable structural effects and strong oxide interaction lead to different arrangement of the active MnOx phase, explaining the peculiar reactivity scale of the studied catalysts in the CO oxidation reaction. High activity, good stability, CO2 productivity values depending on the MnOx loading, and similar activation energy values in the range of 353-533K (37-47 kj/mol) uncover an unchanging reaction mechanism, irrespective of composition and temperature. Although some chemical effects at high Ce loading (chi(Ce) >= 0.5), structure-activity relationships indicate that surface Mn-IV centers are the active sites of bulk MnOx and composite MnCeOx catalysts. (C) 2017 Elsevier B.V. All rights reserved.
引用
收藏
页码:14 / 22
页数:9
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