Catalytic Functionalization of Hexagonal Boron Nitride for Oxidation and Epoxidation Reactions by Molecular Oxygen
Catalytic Functionalization of Hexagonal Boron Nitride for Oxidation and Epoxidation Reactions by Molecular Oxygen
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DOI：
10.1021/acs.jpcc.1c04661
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发表时间：
2021-08
期刊：
影响因子：
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通讯作者：
Min Gao;Ben Wang;T. Tsuneda;A. Lyalin;T. Taketsugu
中科院分区：
文献类型：
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作者：
Min Gao;Ben Wang;T. Tsuneda;A. Lyalin;T. Taketsugu
从理论上研究了碳掺杂六方氮化硼(h-BN)表面吸附的分子氧催化一氧化碳氧化和乙烯环氧化反应的机理。分析了能级分布和活化势垒随掺杂碳原子间距的变化规律。结果表明，所考虑的氧化和环氧化反应不仅发生在靠近C掺杂的B原子位置上，而且发生在距C掺杂较远的位置。因此，C-B/h-BN具有较多的活性中心，在较低的C浓度下，催化剂具有较宽的活化区(~5.0ä)。计算结果表明，随着与掺杂C原子距离的增加，这些反应途径上的反应中间体略有不稳定，但反应势垒基本保持不变。因此，碳掺杂h-BN是惰性h-BN材料催化功能化的一种很有前途的方法，可用于分子氧氧化和环氧化反应。
The mechanism of catalytic oxidation of carbon monoxide and epoxidation of ethylene by molecular oxygen adsorbed on the carbon-doped hexagonal boron nitride (h-BN) is investigated theoretically. The energy profiles and the dependence of the activation barriers on the distance between the doped carbon atom are analyzed. It is shown that the considered oxidation and epoxidation reactions can occur not only on the B atom sites in the close vicinity to the C dopant but also at relatively large distances from the C dopant. Therefore, C B /h-BN possesses many active sites and it is possible to achieve a wide activation area (~5.0 Å from the doped C) of the catalyst at the small concentration of C. The results of calculations demonstrate that the reaction intermediates along these reaction pathways are slightly destabilized with an increase in the distance from the doped C atom; however, the reaction barriers remain mainly intact. Therefore, C doping of h-BN is a highly promising way for catalytic functionalization of the inert h-BN based materials for oxidation and epoxidation reactions by molecular oxygen.