氧化脱氢反应中六方氮化硼的低温氧化。

IF 3.9 2区 综合性期刊 Q1 MULTIDISCIPLINARY SCIENCES
Mehran Sajad, Kateřina Knotková, Roman Bulánek, Ota Bludský, Miroslav Rubeš
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引用次数: 0

摘要

采用实验技术和理论模拟相结合的方法研究了丙烷氧化脱氢过程中六方氮化硼(h-BN)的低温氧化反应。本研究探讨了气相自由基,如n-丙基和羟基自由基,在启动氧化过程中的作用,导致氧功能化h-BN边的形成。利用从头算分子动力学(AIMD)和密度泛函理论(DFT)计算,揭示了氢氮化硼的氧化机理,包括抽氢、分子氧吸附和氮氧化物脱附。实验结果证实,氧化只发生在氧气和丙烷同时存在的情况下,证明了气相自由基生成的关键依赖于反应器的几何形状。氧化过程导致氧掺入到h-BN中,形成影响催化活性的硼氢氧化物相。这些发现为氢氮化硼在ODHP条件下的行为提供了新的见解,并为优化硼基选择性烷烃脱氢催化剂提供了指导。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Low-temperature oxidation of hexagonal boron nitride during oxidative dehydrogenation reactions.

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.

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来源期刊
Scientific Reports
Scientific Reports Natural Science Disciplines-
CiteScore
7.50
自引率
4.30%
发文量
19567
审稿时长
3.9 months
期刊介绍: We publish original research from all areas of the natural sciences, psychology, medicine and engineering. You can learn more about what we publish by browsing our specific scientific subject areas below or explore Scientific Reports by browsing all articles and collections. Scientific Reports has a 2-year impact factor: 4.380 (2021), and is the 6th most-cited journal in the world, with more than 540,000 citations in 2020 (Clarivate Analytics, 2021). •Engineering Engineering covers all aspects of engineering, technology, and applied science. It plays a crucial role in the development of technologies to address some of the world''s biggest challenges, helping to save lives and improve the way we live. •Physical sciences Physical sciences are those academic disciplines that aim to uncover the underlying laws of nature — often written in the language of mathematics. It is a collective term for areas of study including astronomy, chemistry, materials science and physics. •Earth and environmental sciences Earth and environmental sciences cover all aspects of Earth and planetary science and broadly encompass solid Earth processes, surface and atmospheric dynamics, Earth system history, climate and climate change, marine and freshwater systems, and ecology. It also considers the interactions between humans and these systems. •Biological sciences Biological sciences encompass all the divisions of natural sciences examining various aspects of vital processes. The concept includes anatomy, physiology, cell biology, biochemistry and biophysics, and covers all organisms from microorganisms, animals to plants. •Health sciences The health sciences study health, disease and healthcare. This field of study aims to develop knowledge, interventions and technology for use in healthcare to improve the treatment of patients.
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