BMIMBF4中2-氨基-3-氯-1,4-萘醌电化学捕获CO2的机理

利用循环伏安法（CV）和现场红外光谱电化学技术研究了2-氨基-3-氯-1，4-萘醌（ACNQ）在1-丁基-3-甲基咪唑四氟硼酸盐（BMIMBF₄）中电化学捕获CO₂的机理.研究结果表明，当体系中不存在CO₂时，ACNQ在BMIMBF₄中经历可逆的两步一电子过程；当体系中引入CO₂时，电化学还原过程中形成的二价阴离子（ACNQ^2-）作为亲核试剂，可攻击CO₂的亲电子碳中心，形成稳定的CO₂加合物.对电化学捕获CO₂的化学计量进行了评估，结果表明，1摩尔的ACNQ^2-可捕获1摩尔的CO₂.结合B3LYP方法在6-311++G^**水平上计算分析了反应中CO₂加合物可能的结构.

Mechanism of Electrochemical Capture of CO2 via Redox Cycle of 2-Amino-3-chloro-1,4-naphthoquinone in BMIMBF4

The mechanism of electrochemical capture of CO₂ via redox cycle of 2-amino-3-chloro-1,4-naphthoquinone(ACNQ) in 1-butyl-3-methylimidazolium tetrafluoroborate(BMIMBF₄) was investigated by cyclic voltammetry(CV) and in-situ Fourier transform infrared(FTIR) spectroelectrochemistry techniques. In the absence of CO₂, ACNQ undergoes a reversible two-step one-electron process in BMIMBF₄. The dianion(ACNQ^2-) formed during electrochemical reduction can be used as nucleophiles to attack the eletrophilic carbon center of CO₂ and form a stable CO₂ adduct when CO₂ is introduced. Furthermore, the stoichiometry of CO₂ electrochemical capture was evaluated. The result indicates that 1 mol of ACNQ^2- can capture 1 mol of CO₂. Also, the possible structures of CO₂ adducts in the reaction were calculated by the B3LYP method at the 6-311++G^** level.