Transient studies of low-temperature dry reforming of methane over Ni-CaO/ZrO2-La2O3

被引:120
作者
Bachiller-Baeza, B. [1 ]
Mateos-Pedrero, C. [1 ]
Soria, M. A. [1 ]
Guerrero-Ruiz, A. [2 ]
Rodemerck, U. [3 ]
Rodriguez-Ramos, I. [1 ]
机构
[1] CSIC, Inst Catalisis & Petr Quim, Madrid 28049, Spain
[2] UNED, Dpto Quim Inorgan & Quim Tecn, Madrid 28040, Spain
[3] Univ Rostock, Leibniz Inst Katalyse eV, D-18059 Rostock, Germany
关键词
Dry reforming methane; TAP reactor; DRIFTS; Ni catalyst; Calcium oxide promoter; CARBON-DIOXIDE; SYNTHESIS GAS; MECHANISTIC FEATURES; PROBE MOLECULES; FT-IR; CATALYST; CO2; SURFACE; NICKEL; CH4;
D O I
10.1016/j.apcatb.2012.09.052
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 low temperature reforming of methane by carbon dioxide is studied over a calcium oxide promoted Ni catalyst supported on a tetragonal zirconia stabilized by lanthana, which presents an improved stability compared to the non-promoted catalyst. Steady-state catalytic activity measurements, diffuse reflectance infrared Fourier transform spectroscopic analysis and isotopic temporal analysis of products experiments reveal the occurrence of a bifunctional mechanism on the promoted catalyst: methane is activated on the Ni particles, carbon dioxide interacts with the calcium oxide to form carbonates which scavenge carbon from nickel at the Ni-O-Ca interphase, thus restoring Ni particles to the original state. This is assumed to hinder the formation of deactivating coke, which explains the improved catalytic stability of the promoted catalyst. The main route for the carbon deposit formation is found to be the methane cracking in spite of the low temperature reaction. (C) 2012 Elsevier B.V. All rights reserved.
引用
收藏
页码:450 / 459
页数:10
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