Phase Composition and Catalytic Properties of MnNaW/SiO2 Oxide System in Oxidative Conversion of Methane

IF 0.7 4区化学 Q4 CHEMISTRY, MULTIDISCIPLINARY

Theoretical and Experimental Chemistry Pub Date : 2022-06-02 DOI:10.1007/s11237-022-09723-8

E. H. Ismailov, D. B. Taghiyev, S. M. Zulfugarova, S. N. Osmanova, G. R. Azimova, J. W. Thybaut

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Abstract

MnNaW/SiO₂ oxide system based on a mesoporous silica matrix synthesized using tetraethoxysilane and cetyltrimethylammonium bromide as precursors were prepared and characterized by SEM/EDS, XRD, EPR, N₂ adsorption-desorption measurements and studied in the oxidative conversion of methane (OCM). It is shown that MnNaW/SiO₂ catalyst consists of MnO_x, Na₂WO₄, MnWO₄, and SiO₂ phases. At the reaction temperature of 750-850°C the molten Na₂WO₄ phase covers the surface of crystalline SiO₂, and the interaction of MnO_x, Na₂WO₄ and SiO₂ matrix forms “liquid glass”. It is assumed that Na_1–yMnO_x particles formed as a result of the interaction of the system components during catalyst formation and characterized by the presence of ion-radical lattice oxygen are catalytically active sites in the OCM process.

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MnNaW/SiO2氧化体系在甲烷氧化转化中的相组成及催化性能

以四乙氧基硅烷和十六烷基三甲基溴化铵为前驱体，制备了基于介孔二氧化硅基体的MnNaW/SiO2氧化物体系，采用SEM/EDS、XRD、EPR、N2吸附-脱附等手段对其进行了表征，并对甲烷(OCM)氧化转化进行了研究。结果表明，MnNaW/SiO2催化剂由MnOx、Na2WO4、MnWO4和SiO2相组成。在750 ~ 850℃的反应温度下，熔融的Na2WO4相覆盖在结晶SiO2表面，MnOx、Na2WO4和SiO2基体相互作用形成“液态玻璃”。假设Na1-yMnOx颗粒是催化剂形成过程中系统组分相互作用的结果，并以离子自由基晶格氧的存在为特征，是OCM过程中的催化活性位点。

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来源期刊

Theoretical and Experimental Chemistry CHEMISTRY, MULTIDISCIPLINARY-

CiteScore

1.60

自引率

10.00%

发文量

审稿时长

6-12 weeks

期刊介绍： Theoretical and Experimental Chemistry is a journal for the rapid publication of research communications and reviews on modern problems of physical chemistry such as: a) physicochemical bases, principles, and methods for creation of novel processes, compounds, and materials; b) physicochemical principles of chemical process control, influence of external physical forces on chemical reactions; c) physical nanochemistry, nanostructures and nanomaterials, functional nanomaterials, size-dependent properties of materials.