水液相下依达拉奉与过氧化氢自由基反应的DFT研究  

The DFT Study on the Reaction of Edaravone with Hydrogen Peroxide Radical in Aqueous Solution

作　　者：孙伟 姜春旭 梁晴晴 杨应[2] 张勇 王佐成[2] 张雪娇[2] Sun Wei;Jiang Chunxu;Liang Qingqing;Yang Ying;Zhang Yong;Wang Zuocheng;Zhang Xuejiao(College of Nursing,Baicheng Medical College,Baicheng 137000,China;Theoretical Computing Center,Baicheng Normal University,Baicheng 137000,China;Laibin Senior High School,Physics Teaching Group,Laibin 546100,China)

机构地区：[1]白城医学高等专科学校护理学院,吉林白城137000 [2]白城师范学院理论计算中心,吉林白城137000 [3]广西来宾市来宾高级中学物理组,广西来宾546100

出　　处：《南开大学学报（自然科学版）》2023年第6期94-104,共11页Acta Scientiarum Naturalium Universitatis Nankaiensis

基　　金：吉林省教育厅重点项目(2022ZCZ012);吉林省自然科学基金(20160101308C)。

摘　　要：采用基于密度泛函理论的M06-2X和MN15杂化泛函方法,结合自洽反应场理论的极化连续介质模型(SMD模型),研究了水液相环境下依达拉奉(Eda)消除过氧化氢自由基(HO_(2))的反应机理.考察了HO_(2)抽H原子、HO_(2)加成到不饱和C和单电子从Eda向HO_(2)转移3个反应通道.势能面研究表明:HO_(2)抽H的自由能垒在0.0-153.9 kJ/mol之间;HO_(2)加成的自由能垒在68.9-90.3 kJ/mol之间;单电子从Eda向HO_(2)转移的自由能垒是143.7 kJ/mol.结果表明,水液相下Eda可通过抽H和加成反应消除HO_(2),依达拉奉可作为HO_(2)自由基的清除剂.The reaction mechanism of edaravone(Eda)scavenging hydrogen peroxide radical(HO_(2))in aqueous solution was studied by using M06-2X and MN15 hybrid functional methods based on density functional theory,combined with the polarized continuum model(SMD model)of self-consistent reaction field theory.Three reaction channels of HO_(2)extraction of H atom,HO_(2)addition to unsaturated C and single electron transfer from Eda to HO_(2)are investigated.The study of potential energy surface shows that the free energy barrier of HO_(2)extracting H is between 0.0 and 153.9 kJ/mol.The free energy barrier of HO_(2)addition reaction is between 68.9 and 90.3 kJ/mol.The free energy barrier of single electron transfer from Eda to HO_(2)is 143.7 kJ/mol.The results show that the Eda can scavenge HO_(2)by extracting H and addition reaction in aqueous solution,Eda can be used as HO_(2)free radical scavenger.

关 键 词：依达拉奉 过氧化氢自由基 密度泛函理论 过渡态 马库斯(Marcus)理论 电子转移 能垒 

分 类 号：O641.12[理学—物理化学]