摘要
本文用量子化学从头计算法研究了Cr/O_2/Ar气相体系所发生的两个反应的机理。在MP2/SDD水平上优化了反应物、过渡态、中间体和产物的几何构型。在同一水平上计算了能量,同时进行零点能校正,并且计算出反应的热效应、熵变、活化能和绝对速率常数,并与文献数据进行了比较。计算结果与文献数据比较吻合,表明量子化学计算是研究铬等痕量元素气相反应机理和计算热力学及动力学参数的一种有效手段。
Reaction mechanism of two reactions in Cr/O2/Ar system has been studied by ab ini-tio calculations of quantum chemistry. The geometry optimizations of reactant, transition state, in-term8ediate and product are made at MP2/SDD level. Then, the reaction potential barriers are calculated at the same level and the zero-point energies are also corrected. Finally, the reaction heat, reacion entropy, active energy and absolute rate constant are calculated and compared with reference data. The calculated results approach reference data, which shows that quantum chemical calculation is an effective method to study gas-phase reaction mechanism of trace elements (such as chromium), and to calculate therrnodynamical and kinetic parameters.
出处
《工程热物理学报》
EI
CAS
CSCD
北大核心
2003年第5期877-880,共4页
Journal of Engineering Thermophysics
基金
国家重点基础研究专项经费资助项目(No.G199902212)
关键词
铬
反应机理
从头计算法
量子化学
chromium
reaction mechanism
ab initio calculation
quantum chemistry
