摘要
为探究经MnO2改性后活性炭（C14H6）吸附汞的反应机理,应用量子化学从头计算的MP2方法,优化6-311＋g（d,p）/SDD基组得到反应物、中间体、过渡态和产物的几何构型,计算反应的动力学参数.采用经典过渡态理论分别计算了在298~1 500K和0.000 1~3 MPa条件下各反应的反应速率常数,并比较分析各反应速率常数的变化趋势.结果表明：在同时含有Hg、C14H6和MnO2的情况下,MnO2和C14H6的反应要比Hg和C14H6的反应快,且MnO2（C14H6）要比C14H6更易与Hg反应;反应速率常数随温度和压力的升高呈现增大趋势;经MnO2改性后的活性炭比未改性的活性炭吸附Hg的效果要好.
To study the reaction mechanism of Hg adsorption by MnO2-modified activated carbons （C14H6）, the quantum chemistry method MP2 ab initio calculation was used to optimize the 6-311＋g（d, p）/SDD basis set to obtain the geometric configuration of the reactants, intermediates, transition states and products, so as to calculate the reaction kinetics. The reaction rate constants at 298-1 500 K and 0. 000 1- 3 MPa were calculated via transition state theory, and their variation tendency with temperature and pressure was analyzed simultaneously. Results show that in the environment simultaneously containing Hg, C14H6 and MnO2, the reaction between MnO2 and C14 H6 is faster than between Hg and C14 H6, and MnO2 （C14 H6） is easier to react with Hg than C14 H6. The reaction rate constant increases with the rise of both temperature and pressure. The adsorption effect of MnO2-modified activated carbons for Hg is better than unmodified activated carbons.
出处
《动力工程学报》
CAS
CSCD
北大核心
2015年第11期923-928,933,共7页
Journal of Chinese Society of Power Engineering
基金
国家自然科学基金资助项目(51076045)
关键词
活性炭
MNO2
汞
量子化学计算
反应机理
activated carbon
MnO2
Hg
quantum chemistry calculation
reaction mechanism
