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煅烧温度对用于合成气甲烷化的Ni-La/AlO催化剂结构-活性关系的影响

Effects of calcination temperatures on the structure-activity relationship of Ni-La/AlO catalysts for syngas methanation.

作者信息

Wu Hongli, Zou Meng, Guo Lisheng, Ma Fengyun, Mo Wenlong, Yu Yuming, Mian Inamullah, Liu Jingmei, Yin Shuangjie, Tsubaki Noritatsu

机构信息

Key Laboratory of Coal Cleaning Conversion and Chemical Engineering Process Xinjiang Uyghur Autonomous Region, College of Chemistry and Chemical Engineering, Xinjiang University Urumqi Xinjiang 830046 China

Department of Applied Chemistry, School of Engineering, University of Toyama Gofuku 3190 Toyama 930-8555 Japan

出版信息

RSC Adv. 2020 Jan 27;10(7):4166-4174. doi: 10.1039/c9ra09674d. eCollection 2020 Jan 22.

Abstract

A series of Ni-La/AlO catalysts for the syngas methanation reaction were prepared by a mechanochemical method and characterized by thermogravimetric analysis (TG-DTA), X-ray fluorescence (XRF), X-ray diffraction (XRD), N adsorption-desorption, H temperature-programmed reduction (H-TPR), and X-ray photoelectron spectroscopy (XPS). The calcination temperatures (350-700 °C) had significant impacts on the crystallite sizes and interactions between NiO and AlO. The catalyst calcined at 400 °C (cat-400) showed a 12.1% Ni dispersion degree and the maximum bound state of NiO (54%) through the Gaussian fitting of H-TPR. Cat-400 also achieved the highest CO conversion, CH selectivity and yield. Cat-400 exhibited good stability and catalytic activity in a lifetime testing of 200 h. The deactivation of cat-400 was mainly caused by carbon deposition according to the data from XRD, TG-DTG and XPS.

摘要

通过机械化学方法制备了一系列用于合成气甲烷化反应的Ni-La/AlO催化剂,并采用热重分析(TG-DTA)、X射线荧光光谱(XRF)、X射线衍射(XRD)、N2吸附-脱附、H2程序升温还原(H-TPR)和X射线光电子能谱(XPS)对其进行了表征。煅烧温度(350-700℃)对微晶尺寸以及NiO与AlO之间的相互作用有显著影响。通过H-TPR的高斯拟合,在400℃煅烧的催化剂(cat-400)显示出12.1%的Ni分散度和最大的NiO结合态(54%)。Cat-400还实现了最高的CO转化率、CH4选择性和产率。在200小时的寿命测试中,Cat-400表现出良好的稳定性和催化活性。根据XRD、TG-DTG和XPS的数据,cat-400的失活主要是由积碳引起的。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/41c2/9048969/e4c2dfbefdd8/c9ra09674d-f1.jpg

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