燃烧中汞与N_2O、O_3的反应机理  

Reaction Mechanism of Mercury and N_2O, O_3 During Coal Combustion

作　　者：刘晶[1] 郑楚光[1] 徐明厚[1] 张军营[1] 

机构地区：[1]华中科技大学煤燃烧国家重点实验室,武汉430074

出　　处：《燃烧科学与技术》2005年第2期155-158,共4页Journal of Combustion Science and Technology

基　　金：国家重点基础研究专项经费资助项目(2002CB211600;G1999022212);国家自然科学基金重点资助项目(20277014).

摘　　要：采用量子化学从头计算MP2/SDD方法研究了燃烧过程中汞与N2O、O3的反应机理,优化得到反应途径上的反应物、过渡态、中间体和产物的几何构型.用QCISD(T)方法计算能量,同时进行零点能校正,并以此能量计算活化能,同时计算指前因子、反应热效应及熵变,采用经典过渡态理论计算反应速率常数.研究结果表明,量子化学是研究汞等痕量元素、气体反应的机理、动力学参数和热力学参数的一种有效手段.The microcosmic mechanism of reaction between mercury and N2O, O3 was studied by ab initio calculations of quantum chemistry, and the geometry optimizations of reactant, transition state, intermediate and product were made at MP2/SDD level. All molecule energies were calculated at QCISD (T) level and corrected with zero point energy. The activation energies, pre-exponential factor, heat of reactions and change of entropy were calculated. The reaction rate constants were calculated directly from transition state theory (TST). The results show that quantum chemistry is an effective means for investigating kinetic mechanism of trace elements interaction with combustion-generated flue gas.

关 键 词：燃烧 汞 反应机理 量子化学 

分 类 号：TK16[动力工程及工程热物理—热能工程]