Spatial and Temporal Self-organization During CO Oxidation Over Ni

被引:0
作者
Alexei G. Makeev
Nickolai V. Peskov
Marina M. Slinko
Victor Yu. Bychkov
Vladimir N. Korchak
机构
[1] Lomonosov Moscow State University,Faculty of Computational Mathematics and Cybernetics
[2] Semenov Institute of Chemical Physics,undefined
来源
Topics in Catalysis | 2020年 / 63卷
关键词
CO oxidation; Ni catalyst; Mathematical modeling; Oscillations;
D O I
暂无
中图分类号
学科分类号
摘要
Oscillatory behavior during CO oxidation over a Ni foil in a continuous-flow catalytic reactor has been discovered in the reaction mixture containing CO excess at atmospheric pressure in the temperature range of 500–630 °C. The oscillations are accompanied by propagation of the oxidation and reduction fronts which were recorded by a photo–video camera. Dark fronts of the oxidized state appear periodically in the upstream part of the catalyst and propagate to the downstream region in the direction of the gas flow. Reduction fronts move in the opposite direction. A mathematical model has been developed to simulate the oscillatory dynamics. The developed model simulates experimental data almost quantitatively. The origin of oscillations is connected with periodic oxidation and reduction of the nickel surface. It is shown that a precursor-mediated adsorption of CO on Ni surface is required to simulate the oscillations under reducing conditions.
引用
收藏
页码:49 / 57
页数:8
相关论文
共 118 条
  • [1] Engel T(1979)Elementary steps in the catalytic oxidation of carbon monoxide on platinum metals Adv Catal 28 1-78
  • [2] Ertl G(2011)CO oxidation as a prototypical reaction for heterogeneous processes Angew Chem Int Ed 50 10064-10094
  • [3] Freund H-J(1995)Oscillatory kinetics in heterogeneous catalysis Chem Rev 95 697-733
  • [4] Meijer G(2005)Spatiotemporal patterns in catalytic systems Catal Today 105 254-274
  • [5] Scheffler M(2018)New oscillating system: CO oxidation over Ni Catal Lett 148 653-659
  • [6] Schlögl R(1980)Surface state and kinetic oscillations in the oxidation of hydrogen on nickel J Catal 66 11-27
  • [7] Wolf M(2006)Study of nickel catalyst in oscillating regime of methane oxidation by means of gravimetry and mass-spectrometry Appl Catal A 3042 21-29
  • [8] Imbihl R(2009)Nonlinear behavior during methane and ethane oxidation over Ni, Co and Pd catalysts Surf Sci 603 1680-1689
  • [9] Ertl G(2017)Reversible bulk oxidation of Ni foil during oscillatory catalytic oxidation of propane: a novel type of spatiotemporal self-organization Phys Rev Lett 119 026001-6533
  • [10] Luss D(1989)Spatial temperature oscillations during hydrogen oxidation on a nickel foil J Phys Chem 93 6530-6876