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采用密度泛函理论(B3LYP)、从头计算及微扰方法计算了超临界状态下镍基催化剂上甲烷逐步脱氢与超临界CO2重整制合成气的反应机理。计算结果表明,甲烷与CO2的重整反应分为5步进行,其超临界态下各反应的焓变分别为:-86.889、47.453、75.812、54.658和-209.460kJ/mol。各步反应的活化能数据表明重整的速控步是第二步,其正反应的活化能为287.081kJ/mol。
Density functional theory (B3LYP) was used to calculate the reaction mechanism of syngas with gradual dehydrogenation of methane and supercritical CO 2 reforming over Ni-based catalysts under supercritical conditions by ab initio calculations and perturbation methods. The calculation results show that the reforming reaction between methane and CO2 is divided into five steps. The enthalpy changes of each reaction in the supercritical state are -86.889, 47.453, 75.812, 54.658 and -209.460 kJ / mol, respectively. The activation energy data of each step reaction shows that the second step of the rate control step of reforming is that the activation energy of the positive reaction is 287.081 kJ / mol.