Tian Jinshu, Tan Jiangqiao, Xu Mingliang, Zhang Zhaoxia, Wan Shaolong, Wang Shuai, Lin Jingdong, Wang Yong
Department of Chemistry, College of Chemistry and Chemical Engineering, National Engineering Laboratory for Green Chemical Productions of Alcohols-Ethers-Esters, State Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials, Xiamen University, Xiamen 361005, China.
Voiland School of Chemical Engineering and Bioengineering, Washington State University, Pullman, WA 99164, USA.
Sci Adv. 2019 Mar 15;5(3):eaav8063. doi: 10.1126/sciadv.aav8063. eCollection 2019 Mar.
Hexagonal boron nitride (-BN) catalyst has recently been reported to be highly selective in oxidative dehydrogenation of propane (ODHP) for olefin production. In addition to propene, ethylene also forms with much higher overall selectivities to C2-products than to C1-products. In this work, we report that the reaction pathways over the -BN catalyst are different from the V-based catalysts in ODHP. Oxidative coupling reaction of methyl, an intermediate from the cleavage of C─C bond of propane, contributes to the high selectivities to C2-products, leading to more C2-products than C1-products over the -BN catalyst. This work not only provides insight into the reaction mechanisms involved in ODHP over the boron-based catalysts but also sheds light on the selective oxidation of alkanes such as direct upgrading of methane via oxidative upgrading to ethylene or CH O on boron-based catalysts.
最近有报道称,六方氮化硼(-BN)催化剂在丙烷氧化脱氢(ODHP)制烯烃反应中具有高选择性。除了丙烯外,乙烯也会生成,且对C2产物的总选择性远高于对C1产物的选择性。在这项工作中,我们报道了- BN催化剂上的反应路径与ODHP中基于V的催化剂不同。丙烷C─C键断裂产生的中间体甲基发生氧化偶联反应,这导致了对C2产物的高选择性,使得在 - BN催化剂上生成的C2产物多于C1产物。这项工作不仅深入了解了硼基催化剂上ODHP所涉及的反应机理,还为烷烃的选择性氧化提供了思路,例如通过硼基催化剂上的氧化升级将甲烷直接转化为乙烯或CH₂O。