摘要
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。
The mechanism of methane reforming with supercritical CO2 on Nickel had been investigated by DFT,ab initio and perturbation methods.The results showed that the reforming reaction was divided into five steps under the supercritical state,the enthalpy of each step was：-86.889,47.453,75.812,54.658 and-209.460kJ/mol,respectively.Among them the second step was the rate determining step with activation energy of 287.081kJ/mol,this illustrated that the reforming reaction can proceed under the supercritical state.
出处
《化学通报》
CAS
CSCD
北大核心
2011年第8期732-736,共5页
Chemistry
基金
国家自然科学基金项目(30760137)
江西省自然科学基金项目(2008GQ0060)资助
关键词
CH4/CO2重整
反应机理
超临界
理论计算
Methane reforming with CO2
Mechanism
Supercritical
Theoretical calculation
