首页|基于Langmuir-Hinshelwood机理的Ni/CeO2在甲烷干重整反应中的动力学研究

基于Langmuir-Hinshelwood机理的Ni/CeO2在甲烷干重整反应中的动力学研究

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以CH4 和CO2 为原料,通过甲烷干重整反应生成H2 和CO合成气,经Fischer-Tropsch反应进一步合成高附加值的甲醇、汽油和柴油等.以Ni/CeO2 为催化剂,基于Langmuir-Hinshel-wood机理对实验数据进行拟合并确定总反应速率常数、CH4 吸附平衡常数和CO2 吸附平衡常数等相关的动力学参数,并将实验测定CH4 转化速率与模型计算值进行对比和方差分析,动力学模型的均方根差(0.045 9)和残差平方和(0.082 2)最小,R2(0.984 4)最大,表明该模型的动力学方程最适用于甲烷干重整反应.Ni/CeO2 催化剂在甲烷干重整参与反应路径为双活性位点的缔合吸附、双分子的表面反应和双活性位点的脱附.
Kinetic investigation into Ni/CeO2 in dry reforming of methane based on Langmuir-Hinshelwood mechanism
Dry reforming of methane could transfer CH4 and CO2 into valuable syngas(H2 and CO),which is employed to synthesize high-value-added methanol,diesel and gasoline through Fis-cher-Tropsch reaction.According to the experimental date of Ni/CeO2 catalyst,the kinetic corre-lated parameters of each model based on Langmuir-Hinshelwood mechanism,such as the total rate constant,the adsorption equilibrium constant of CH4 and the adsorption equilibrium constant of CO2,are fitted and determined.Moreover the experimentally determined CH4 conversion rates were compared with the modeled values and analyzed by ANOVA.The kinetic model exhibits the smallest root mean square error(0.045 9)and the residual sum of squares(0.082 2),and the highest R2(0.984 4),which indicate that this model is the most applicable to Ni/CeO2 for dry re-forming of methane.The reaction pathway of Ni/CeO2 for dry reforming of methane contains the following several steps,such as dual-site associative adsorption of both CH4 and CO2,bimolecular surface reaction and dual-site desorption.

dry reforming of methanereaction kineticsNi/CeO2catalysisLangmuir-Hinshel-wood mechanismkinetic model

李亚楠、乔亦冰、刘朋、徐昊进、吴乐、王玉琪

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西安工程大学 环境与化学工程学院,陕西 西安 710048

西北大学 化工学院,陕西 西安 710069

陕西未来能源化工有限公司,陕西 榆林 719000

甲烷干重整 反应动力学 Ni/CeO2催化 Langmuir-Hinshelwood机理 动力学模型

2024

西安工程大学学报
西安工程大学

西安工程大学学报

CSTPCD
影响因子:0.473
ISSN:1674-649X
年,卷(期):2024.38(6)