期刊
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
卷 46, 期 5, 页码 3539-3553出版社
PERGAMON-ELSEVIER SCIENCE LTD
DOI: 10.1016/j.ijhydene.2020.10.181
关键词
MCM-41; Hydrogen; Catalyst synthesis; Mesoporous silica; Methanol steam reforming
CuZn-based catalysts synthesized by different methods showed diverse physico-chemical properties. Catalysts prepared by one pot hydrothermal synthesis and coimpregnation exhibited the highest methanol conversion and H2 selectivity, indicating that catalytic activity is largely affected by the nature of Cu species within the catalyst matrix.
CuZn-based catalysts are active in production of hydrogen by methanol steam reforming. However, there is a need to have further insight on their physico-chemical properties to improve selectivity to hydrogen. Therefore, a series of CuZn/MCM-41 catalysts was synthesized by four different routes; one pot hydrothermal synthesis (OPMCM), coimpregnation (COMCM), serial impregnation (SRMCM) and copper impregnated on ZnMCM-41 (ZNMCM). Samples of catalysts were characterized by X-ray diffraction (XRD), transmission electron microscopy (TEM), scanning electron microscopy (SEM) coupled with energy dispersive X-ray spectroscopy (EDS), inductively coupled plasma (ICP) emission spectrometry, Fourier transform infrared (FTIR) spectroscopy, thermogravimetric analysis (TGA) and X-ray photoelectron spectroscopy (XPS). XRD revealed disruption in the ordered pore network typical in MCM-41 for all catalysts synthesized and also showed that the one pot synthesis catalyst had wide spread dispersion of Cu and Zn. SEM micrographs captured irregularly shaped particles of different sizes. While XPS showed that different Cu and Zn species were formed within the catalyst matrix. XPS also confirmed that there was wide spread dispersion and interaction of Cu and Zn with MCM-41 matrix in the OPMCM catalyst. COMCM and OPMCM demonstrated the highest activity with 88 and 65% methanol conversion with corresponding H2 selectivity of 91 and 86% respectively. They are better than SRMCM and ZNMCM which had average H-2 selectivity of 19% and 31% respectively. CO selectivity was less than 1.8% for the COMCM and OPMCM catalysts. While SRMCM and ZNMCM had CO selectivity's as high as 8.9% and 7.2% respectively. The data generated shows that catalytic activity is largely affected by the nature of Cu species within the catalyst matrix. (C) 2020 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.
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