含锌纳米 MFI 沸石中羟基在甲烷光催化氧化中的作用

IF 7.5 2区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY
ChemSusChem Pub Date : 2024-09-12 DOI:10.1002/cssc.202401656
Diógenes Piva, Geqian Fang, Sajjad Ghojavand, Francesco Dalena, Nour AlHajjar, Vincent De Waele, Vitaly Ordomsky, Andrei Khodakov, Karima Ben Tayeb, Tiago Fernandes, Svetlana Mintova
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引用次数: 0

摘要

在温和条件下将甲烷有效转化为更有价值的碳氢化合物和氢气混合物是一项巨大的科学和实践挑战。在此,我们合成了含 Zn 的纳米 MFI 型沸石,用于在 H2O 和空气存在下直接氧化甲烷。红外傅立叶变换光谱(FTIR)证实了纳米 MFI 型沸石表面羟基的存在及其在含锌纳米 MFI 沸石中的显著减少。核磁共振、X 射线衍射和紫外可见分光光度法揭示了锌原子掺入纳米 MFI 沸石框架的情况。出乎意料的是,纯硅 MFI 沸石表现出最高的光催化性能。我们的研究结果表明,大量孤立的硅醇基团和硅醇巢可增加 -OH 的形成,提高含氧化合物和 C2H6 的生产率,而掺入沸石框架或附着在纳米沸石硅醇巢上的 Zn 则效率较低。提出了光催化甲烷氧化的机理。这些发现为开发表面羟基数量增加的活性纳米沸石光催化剂提供了启示,这种催化剂可在光催化甲烷转化中发挥关键作用。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Role of Hydroxyl Groups in Zn-containing Nanosized MFI Zeolite for the Photocatalytic Oxidation of Methane

Role of Hydroxyl Groups in Zn-containing Nanosized MFI Zeolite for the Photocatalytic Oxidation of Methane

The effective conversion of methane to a mixture of more valuable hydrocarbons and hydrogen under mild conditions is a significant scientific and practical challenge. Here, we synthesized Zn-containing nanosized MFI zeolite for direct oxidation of methane in the presence of H2O and air. The presence of the surface hydroxyl groups on nanosized MFI-type zeolite and their significant reduction in the Zn-containing nanosized MFI zeolite were confirmed with Infrared Fourier Transform (FTIR) spectroscopy. Incorporation of zinc atoms into the framework of nanosized MFI zeolite is revealed by Nuclear Magnetic Resonance, X-ray Diffraction and UV-Vis Spectroscopy. Unexpectedly, pure silica MFI zeolite exhibited the highest photocatalytic performance. Our findings demonstrated that large number of isolated silanol groups and silanol nests increase the formation of ⋅OH, and enhance the productivity of oxygenate compounds and C2H6, while the Zn incorporated into the zeolite framework or attached to the silanol nests of the nanosized zeolites are less efficient. A mechanism of photocatalytic methane oxidation is proposed. These findings provide insights into the development of active nanosized zeolite photocatalysts with an extended amount of surface hydroxyl groups that can play a key role in photocatalytic methane conversion.

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来源期刊
ChemSusChem
ChemSusChem 化学-化学综合
CiteScore
15.80
自引率
4.80%
发文量
555
审稿时长
1.8 months
期刊介绍: ChemSusChem Impact Factor (2016): 7.226 Scope: Interdisciplinary journal Focuses on research at the interface of chemistry and sustainability Features the best research on sustainability and energy Areas Covered: Chemistry Materials Science Chemical Engineering Biotechnology
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