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碱性前体中沉淀的赤铁矿：甲烷氧化的结构和织构性质比较。

Hematites Precipitated in Alkaline Precursors: Comparison of Structural and Textural Properties for Methane Oxidation.

机构信息

Institute of Environmental Technology, CEET, VSB-Technical University of Ostrava, 17. listopadu 15/2172, 708 00 Ostrava, Czech Republic.

Department of Chemistry and Physico-Chemical Processes, Faculty of Material Science and Technology, VSB-Technical University of Ostrava, 17. listopadu 15/2172, 708 00 Ostrava, Czech Republic.

出版信息

Int J Mol Sci. 2022 Jul 25;23(15):8163. doi: 10.3390/ijms23158163.

DOI:10.3390/ijms23158163
PMID:35897740
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC9332227/
Abstract

Hematite (α-FeO) catalysts prepared using the precipitation methods was found to be highly effective, and therefore, it was studied with methane (CH), showing an excellent stable performance below 500 °C. This study investigates hematite nanoparticles (NPs) obtained by precipitation in water from the precursor of ferric chloride hexahydrate using precipitating agents NaOH or NHOH at maintained pH 11 and calcined up to 500 °C for the catalytic oxidation of low concentrations of CH (5% by volume in air) at 500 °C to compare their structural state in a CH reducing environment. The conversion (%) of CH values decreasing with time was discussed according to the course of different transformation of goethite and hydrohematites NPs precursors to magnetite and the structural state of the calcined hydrohematites. The phase composition, the size and morphology of nanocrystallites, thermal transformation of precipitates and the specific surface area of the NPs were characterized in detail by X-ray powder diffraction, transmission electron microscopy, infrared spectroscopy, thermal TG/DTA analysis and nitrogen physisorption measurements. The results support the finding that after goethite dehydration, transformation to hydrohematite due to structurally incorporated water and vacancies is different from hydrohematite α-FeO. The surface area BET of FeO_NH-70 precipitate composed of protohematite was larger by about 53 m/g in comparison with FeO_Na-70 precipitate composed of goethite. The oxidation of methane was positively influenced by the hydrohematites of the smaller particle size and the largest lattice volume containing structurally incorporated water and vacancies.

摘要

采用沉淀法制备的赤铁矿（α-FeO）催化剂具有很高的活性，因此，本文选用甲烷（CH）作为反应气体对其进行了研究，结果表明在 500°C 以下，该催化剂具有优异的稳定性。本研究采用沉淀法，以六水合氯化铁为前驱体，在 pH 值为 11 的条件下分别使用 NaOH 和 NHOH 作为沉淀剂制备了赤铁矿纳米粒子（NPs），然后在 500°C 下煅烧，用于研究低浓度 CH（空气中体积分数为 5%）在 500°C 下的催化氧化反应，并对比其在 CH 还原环境中的结构状态。根据针铁矿和水赤铁矿 NPs 前驱体向磁铁矿的不同转化过程以及煅烧水赤铁矿的结构状态，讨论了 CH 转化率随时间的变化情况。采用 X 射线粉末衍射、透射电子显微镜、红外光谱、热重/差热分析和氮气物理吸附等手段对沉淀的物相组成、纳米晶的尺寸和形貌、热转变以及 NPs 的比表面积进行了详细的表征。结果表明，在针铁矿脱水后，由于结构内包含的水和空位的存在，向水赤铁矿的转化与α-FeO 不同。与由针铁矿组成的 FeO_Na-70 沉淀相比，由纤铁矿组成的 FeO_NH-70 沉淀具有更大的 BET 比表面积，约大 53 m/g。甲烷的氧化受到较小粒径和具有较大晶格体积的水赤铁矿的影响，其中包含结构内包含的水和空位。

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