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原位傅里叶变换红外光谱研究:温度高达600°C时异丙醇在SnO上的氧化反应,以及与类似等离子体驱动过程的比较。

In situ FTIR studies on the oxidation of isopropyl alcohol over SnO as a function of temperature up to 600 °C and a comparison to the analogous plasma-driven process.

作者信息

Christensen P A, Mashhadani Z T A W, Md Ali Abd Halim Bin

机构信息

School of Engineering, Newcastle University, Bedson Building, Newcastle upon Tyne, NE1 7RU, UK.

出版信息

Phys Chem Chem Phys. 2018 Apr 4;20(14):9053-9062. doi: 10.1039/c7cp07829c.

DOI:10.1039/c7cp07829c
PMID:29384162
Abstract

This paper reports the application of in situ reflectance Fourier Transform InfraRed spectroscopy to the study of the thermal and plasma driven reaction of IsoPropyl Alcohol (IPA) at SnO2-coated Macor, the latter a ceramic material comprised of the oxides of Al, Mg and Si. The data so obtained were compared to those obtained using uncoated Macor. When uncoated Macor was employed, no reaction of the IPA was observed up to 600 °C in the thermal experiments, whereas a number of products were observed in the plasma-driven experiments. The results obtained using coated Macor were somewhat different, with no reaction taking place in the plasma-driven experiments, whilst significant reaction took place in the thermally-driven process. In the latter experiments, the chemistry was observed to show four distinct temperature regions, with electron injection into the conduction band of the SnO2 playing a significant role, culminating in the production of CO2. The data were interpreted in terms of a model in which physisorbed IPA was converted to two forms of isopropoxide: this was converted to acetone and acetaldehyde via adsorbed enolate. The data clearly support the catalytic activity of Macor in the plasma-driven conversion of IPA.

摘要

本文报道了原位反射傅里叶变换红外光谱在研究异丙醇(IPA)在涂有SnO₂的Macor(一种由铝、镁和硅的氧化物组成的陶瓷材料)上的热驱动和等离子体驱动反应中的应用。将由此获得的数据与使用未涂覆Macor获得的数据进行比较。当使用未涂覆的Macor时,在热实验中,高达600°C未观察到IPA的反应,而在等离子体驱动实验中观察到了许多产物。使用涂覆Macor获得的结果有所不同,在等离子体驱动实验中未发生反应,而在热驱动过程中发生了显著反应。在后一种实验中,观察到化学过程呈现四个不同的温度区域,电子注入到SnO₂的导带中起到了重要作用,最终产生了CO₂。数据根据一个模型进行解释,在该模型中,物理吸附的IPA转化为两种形式的异丙醇盐:通过吸附烯醇盐转化为丙酮和乙醛。数据清楚地支持了Macor在等离子体驱动的IPA转化中的催化活性。

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