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用于甲烷干重整的Ni/LaO的溶液燃烧合成:调节碱金属和碱土金属氧化物促进剂的碱性

Solution combustion synthesis of Ni/LaO for dry reforming of methane: tuning the basicity alkali and alkaline earth metal oxide promoters.

作者信息

Ahmad Yahia H, Mohamed Assem T, Kumar A, Al-Qaradawi Siham Y

机构信息

Department of Chemistry and Earth Sciences, College of Arts and Sciences, Qatar University Doha 2713 Qatar

Department of Chemical Engineering, College of Engineering, Qatar University Doha 2713 Qatar.

出版信息

RSC Adv. 2021 Oct 15;11(53):33734-33743. doi: 10.1039/d1ra05511a. eCollection 2021 Oct 8.

Abstract

The production of syngas dry reforming of methane (DRM) has drawn tremendous research interest, ascribed to its remarkable economic and environmental impacts. Herein, we report the synthesis of K, Na, Cs, Li, and Mg-promoted Ni/LaO using solution combustion synthesis (SCS). The properties of the catalysts were determined by N physisorption experiments, scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray diffraction (XRD), X-ray photoelectron spectrometry (XPS), and H-TPR (temperature programmed reduction). In addition, their catalytic performance towards DRM was evaluated at 700 °C. The results demonstrated that all catalysts exhibited porous structures with high specific surface area, in particular, Mg-promoted Ni/LaO (Mg-Ni-LaO) which depicted the highest surface area and highest pore volume (54.2 m g, 0.36 cm g). Furthermore, Mg-Ni-LaO exhibited outstanding catalytic performance in terms of activity and chemical stability compared to its counterparts. For instance, at a gas hourly space velocity (GHSV) of 30 000 mL g h, it afforded 83.2% methane conversion and 90.8% CO conversion at 700 °C with no detectable carbon deposition over an operating period of 100 h. The superb DRM catalytic performance of Mg-Ni-LaO was attributed to the high specific surface area/porosity, strong metal-support interaction (MSI), and enhanced basicity, in particular the strong basic sites compared to other promoted catalysts. These factors remarkably enhance the catalytic performance and foster resistance to coke deposition.

摘要

合成气(甲烷干重整,DRM)的生产引起了极大的研究兴趣,这归因于其显著的经济和环境影响。在此,我们报告了使用溶液燃烧合成法(SCS)合成K、Na、Cs、Li和Mg促进的Ni/LaO。通过N物理吸附实验、扫描电子显微镜(SEM)、透射电子显微镜(TEM)、X射线衍射(XRD)、X射线光电子能谱(XPS)和H-程序升温还原(H-TPR)来确定催化剂的性能。此外,在700℃下评估了它们对DRM的催化性能。结果表明,所有催化剂均呈现出具有高比表面积的多孔结构,特别是Mg促进的Ni/LaO(Mg-Ni-LaO),其具有最高的表面积和最高的孔体积(54.2 m²/g,0.36 cm³/g)。此外,与其他催化剂相比,Mg-Ni-LaO在活性和化学稳定性方面表现出优异的催化性能。例如,在气体时空速(GHSV)为30000 mL g⁻¹ h⁻¹时,在700℃下它实现了83.2%的甲烷转化率和90.8%的CO转化率,并且在100小时的运行期间没有检测到碳沉积。Mg-Ni-LaO卓越的DRM催化性能归因于高比表面积/孔隙率、强金属-载体相互作用(MSI)和增强的碱性,特别是与其他促进型催化剂相比更强的碱性位点。这些因素显著提高了催化性能并增强了抗积炭能力。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/83af/9042257/897ea53f3034/d1ra05511a-f1.jpg

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