State Key Laboratory of Fine Chemicals, Liaoning Key Laboratory for Catalytic Conversion of Carbon Resources, School of Chemical Engineering, Dalian University of Technology, Dalian, 116024, Liaoning, China.
Nat Commun. 2023 Jan 5;14(1):73. doi: 10.1038/s41467-022-35776-3.
Oxidative dehydrogenation (ODH) of alkane over boron nitride (BN) catalyst exhibits high olefin selectivity as well as a small ecological carbon footprint. Here we report an unusual phenomenon that the in-situ formed olefins under reactions are in turn actively accelerating parent alkane conversion over BN by interacting with hydroperoxyl and alkoxyl radicals and generating reactive species which promote oxidation of alkane and olefin formation, through feeding a mixture of alkane and olefin and DFT calculations. The isotope tracer studies reveal the cleavage of C-C bond in propylene when co-existing with propane, directly evidencing the deep-oxidation of olefins occur in the ODH reaction over BN. Furthermore, enhancing the activation of ethane by the in-situ formed olefins from propane is successfully realized at lower temperature by co-feeding alkane mixture strategy. This work unveils the realistic ODH reaction pathway over BN and provides an insight into efficiently producing olefins.
在氮化硼（BN）催化剂上进行烷烃的氧化脱氢（ODH）反应具有高烯烃选择性和较小的生态碳足迹。在这里，我们报告了一个不寻常的现象，即在反应中原位形成的烯烃通过与过氧氢和烷氧自由基相互作用，并生成促进烷烃氧化和烯烃形成的活性物质，从而积极加速BN 上的母体烷烃转化，通过进料烷烃和烯烃的混合物和 DFT 计算。同位素示踪研究表明，当丙烯与丙烷共存时，丙烯中的 C-C 键被裂解，直接证明了 BN 上的 ODH 反应中烯烃的深度氧化。此外，通过共进料烷烃混合物策略，在较低温度下成功地实现了由丙烷原位生成的烯烃对乙烷的活化增强。这项工作揭示了 BN 上真实的 ODH 反应途径，并为高效生产烯烃提供了新的思路。
