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氧化脱氢反应过程中六方氮化硼的低温氧化

Low-temperature oxidation of hexagonal boron nitride during oxidative dehydrogenation reactions.

作者信息

Sajad Mehran, Knotková Kateřina, Bulánek Roman, Bludský Ota, Rubeš Miroslav

机构信息

Department of Physical Chemistry, Faculty of Chemical Technology, University of Pardubice, Studentská 573, Pardubice, 532 10, Czech Republic.

Institute of Organic Chemistry and Biochemistry, Academy of Sciences of the Czech Republic, Flemingovo nám. 2, Prague, 162 10, Czech Republic.

出版信息

Sci Rep. 2025 Jul 2;15(1):22879. doi: 10.1038/s41598-025-05681-y.

Abstract

The low-temperature oxidation of hexagonal boron nitride (h-BN) during oxidative dehydrogenation of propane (ODHP) is investigated using a combination of experimental techniques and theoretical modeling. This study explores the role of gas-phase radicals, such as n-propyl and hydroxyl radicals, in initiating the oxidation process, leading to the formation of oxygen-functionalized h-BN edges. Using ab initio molecular dynamics (AIMD) and density functional theory (DFT) calculations, we reveal the mechanism of h-BN oxidation, including hydrogen abstraction, molecular oxygen adsorption, and nitrogen oxide desorption. Experimental results confirm that oxidation occurs only in the presence of both oxygen and propane, demonstrating a critical dependence on reactor geometry on gas-phase radical generation. The oxidation process leads to the incorporation of oxygen into h-BN, forming boron oxyhydroxide phases that influence catalytic activity. These findings provide new insights into h-BN behavior under ODHP conditions and offer guidance for optimizing boron-based catalysts for selective alkane dehydrogenation.

摘要

采用实验技术和理论建模相结合的方法,研究了丙烷氧化脱氢(ODHP)过程中六方氮化硼(h-BN)的低温氧化。本研究探讨了气相自由基(如正丙基和羟基自由基)在引发氧化过程中的作用,该过程导致形成氧官能化的h-BN边缘。通过从头算分子动力学(AIMD)和密度泛函理论(DFT)计算,我们揭示了h-BN氧化的机理,包括氢提取、分子氧吸附和氮氧化物解吸。实验结果证实,氧化仅在氧气和丙烷同时存在的情况下发生,表明对反应器几何形状对气相自由基生成的关键依赖性。氧化过程导致氧掺入h-BN,形成影响催化活性的硼羟基氧化物相。这些发现为ODHP条件下h-BN的行为提供了新的见解,并为优化用于选择性烷烃脱氢的硼基催化剂提供了指导。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/66dd/12217080/7f3a75e6c002/41598_2025_5681_Fig1_HTML.jpg

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