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用于甲烷催化分解的基质隔离镍-聚合物复合材料的催化设计

Catalytic Design of Matrix-Isolated Ni-Polymer Composites for Methane Catalytic Decomposition.

作者信息

Kulikova Mayya V, Ivantsov Mikhail I, Sotnikova Anastasia E, Samoilov Vadim O

机构信息

A.V. Topchiev Institute of Petrochemical Synthesis, Russian Academy of Sciences, Leninsky Prospect 29, 119991 Moscow, Russia.

出版信息

Polymers (Basel). 2023 May 31;15(11):2534. doi: 10.3390/polym15112534.

Abstract

Targeted synthesis of C/composite Ni-based material was carried out by the method of matrix isolation. The composite was formed with regard to the features of the reaction of catalytic decomposition of methane. The morphology and physicochemical properties of these materials have been characterized using a number of methods: elemental analysis, scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FTIR), Raman spectroscopy, temperature programmed reduction (TPR-H), specific surface areas (SSA), thermogravimetric analysis, and differential scanning calorimetry (TGA/DSC). It was shown by FTIR spectroscopy that nickel ions are immobilized on the polymer molecule of polyvinyl alcohol, and during heat treatment, polycondensation sites are formed on the surface of the polymer molecule. By the method of Raman spectroscopy, it was shown that already at a temperature of 250 °C, a developed conjugation system with sp2-hybridized carbon atoms begins to form. The SSA method shows that the formation of the composite material resulted in a matrix with a developed specific surface area of 20 to 214 m/g. The XRD method shows that nanoparticles are essentially characterized by Ni, NiO reflexes. The composite material was established by microscopy methods to be a layered structure with uniformly distributed nickel-containing particles 5-10 nm in size. The XPS method determined that metallic nickel was present on the surface of the material. A high specific activity was found in the process of catalytic decomposition of methane-from 0.9 to 1.4 g/g/h, X, from 33 to 45% at a reaction temperature of 750 °C without the stage of catalyst preliminary activation. During the reaction, the formation of multi-walled carbon nanotubes occurs.

摘要

采用基质隔离法进行了C/复合镍基材料的定向合成。根据甲烷催化分解反应的特点形成了复合材料。使用多种方法对这些材料的形态和物理化学性质进行了表征:元素分析、扫描电子显微镜(SEM)、透射电子显微镜(TEM)、X射线衍射(XRD)、傅里叶变换红外光谱(FTIR)、拉曼光谱、程序升温还原(TPR-H)、比表面积(SSA)、热重分析和差示扫描量热法(TGA/DSC)。FTIR光谱表明镍离子固定在聚乙烯醇的聚合物分子上,并且在热处理过程中,聚合物分子表面形成了缩聚位点。通过拉曼光谱法表明,在250℃的温度下,已经开始形成具有sp2杂化碳原子的发达共轭体系。SSA方法表明,复合材料的形成导致了一种比表面积为20至214m/g的发达基质。XRD方法表明,纳米颗粒的基本特征是Ni、NiO反射。通过显微镜方法确定复合材料是一种层状结构,其中尺寸为5-10nm的含镍颗粒均匀分布。XPS方法确定材料表面存在金属镍。在甲烷催化分解过程中发现了高比活性——在750℃的反应温度下,无需催化剂预活化阶段,X为0.9至1.4g/g/h,从33%至45%。在反应过程中,会形成多壁碳纳米管。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/3d72/10255178/e5b6273dc3ce/polymers-15-02534-g001.jpg

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