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利用第一原理密度泛函理论,研究了CO在铜基MOF(CuBTC)上氧化的反应机理.研究显示CO和O2弱吸附在轮形Cu2构筑单元铜的顶位上,并且电子从O2和CO转移到Cu,通过两个机理(Eley-Rideal机理和Langmuir-Hinshelwood机理)的研究,揭示了CO在CuBTC的氧化是准Langmuir-Hinshelwood机理,先在铜上吸附的CO和氧气先越过1.8eV的能垒形成OOCO的中间体,然后分解成CO2,同时有活性氧吸附在Cu位,活性氧与第二个CO反应生成CO2.总的来说,研究有助于理解CO在铜基MOFs的氧化.
The first principle of density functional theory was used to study the reaction mechanism of CO oxidation on copper-based MOF (CuBTC) .The results show that CO and O 2 are weakly adsorbed on the top of the copper Cu 2 structure, It is revealed that the oxidation of CO in CuBTC is quasi-Langmuir-Hinshelwood mechanism. The first adsorption of CO and oxygen on copper first crosses 1.8eV The energy barrier forms the OOCO intermediate and then decomposes into CO2, with active oxygen adsorbed at the Cu site, and the reactive oxygen species reacts with the second CO to form CO2. Overall, the study is useful in understanding the oxidation of CO on copper-based MOFs .