Crystal structure and surface species of CuFe2O4 spinel catalysts in steam reforming of dimethyl ether

被引:83
|
作者
Faungnawakij, Kajornsak [1 ]
Shimoda, Naohiro [2 ]
Fukunaga, Tetsuya [3 ]
Kikuchi, Ryuji [2 ]
Eguchi, Koichi [2 ]
机构
[1] Natl Sci & Technol Dev Agcy, Natl Nanotechnol Ctr, Pathum Thani 12120, Thailand
[2] Kyoto Univ, Grad Sch Engn, Dept Energy & Hydrocarbon Chem, Nishikyo Ku, Kyoto 6158510, Japan
[3] Idemitsu Kosan Co Ltd, Cent Res Labs, Chiba 2990293, Japan
基金
日本科学技术振兴机构;
关键词
Copper-iron spinel; X-ray photoelectron spectroscopy; Auger electron spectroscopy; Methanol; Hydrogen; Regeneration; GAS SHIFT REACTION; HYDROGEN-PRODUCTION; COMPOSITE CATALYSTS; METHANOL; WATER; MECHANISM; MN; HYDROLYSIS; PRECURSOR; CU/ZNO;
D O I
10.1016/j.apcatb.2009.08.013
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
Copper-iron spinel (CuFe2O4) in cubic phase was prepared via a simple citrate sol-gel method and was, transformed into tetragonal phase of high crystallinity by calcining in air at 900 degrees C. Composites of CuFe2O4 spinel and gamma-Al2O3 were investigated for catalytic production of hydrogen from dimethyl ether steam reforming (DME SR). X-ray photoelectron spectroscopy showed Cu1+-rich surface species (Cu1+/Cu-0 approximate to ca. 3/2 with negligible Cu2+) over the calcined CuFe2O4 subjected to in situ H-2 reduction. The spinel-oxides with lower content of reducible Cu species possessed higher amount of Cu1+ species under the reducing atmosphere, corresponding to higher DME SR activity. Copper clusters highly dispersed in the matrix of iron oxides were reduced from the spinel structure, and the strong interaction between them should result in the high activity and durability. The degraded catalysts after DME SR were regenerated by calcining in air in the temperature range of 350-800 degrees C. Slow deactivation of the composites observed during DME SR at 375 degrees C was mainly attributable to non-graphitic carbonaceous species deposited on the catalyst surface. (C) 2009 Elsevier B.V. All rights reserved.
引用
收藏
页码:341 / 350
页数:10
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