期刊
CATALYSIS TODAY
卷 383, 期 -, 页码 236-246出版社
ELSEVIER
DOI: 10.1016/j.cattod.2020.12.003
关键词
Graphene related materials; Graphene; Few layer graphene; Stainless steel foam; Catalytic methane decomposition; Carburization
资金
- MICINN (Madrid, Spain) FEDER [ENE2017-82451-C3]
- MICINN [BES-2014-069010]
This study explores the preparation of graphene-related materials (GRMs) grown on stainless steel foams via catalytic decomposition of methane (CDM). Fe nanoparticles segregated from the stainless steel after the activation stage of the foam were found to be the main active phases for the reaction. Factors affecting productivity, stability, and selectivity to GRMs include feed composition and reaction temperature.
This work explores the preparation of graphene-related materials (GRMs) grown on stainless steel foams via catalytic decomposition of methane (CDM). The main active phases for the reaction are the Fe nanoparticles segregated from the stainless-steel after the activation stage of the foam. The effect of the feed composition and reaction temperature has been studied in order to maximize the productivity, stability and selectivity to GRMs. The maximum productivity attained was 0.116 g(C)/g(foam) h operating at 950 degrees C with a feed ratio of CH4/H-2 = 3 (42.9 %CH4:14.3 %H-2). The carbonaceous nanomaterials (CNMs) obtained were characterized by X-Ray diffraction, Raman spectroscopy and by transmission and scanning electron microscopy. The parameters of the kinetic model developed are directly related to the relevant stages of the process, including carburization, diffusion-precipitation and deactivation-regeneration. The balance among these sequential stages determines the overall performance of the activated foam. In conditions of rapid carburization of the Fe NPs (p(CH4) > 14 %), the productivity to CNMs is favoured, avoiding an initial deactivation of the active sites by fouling with amorphous carbon. After a rapid carburization, the selectivity to the different CNMs is governed by the ratio CH4/H-2, and mainly by the temperature. Thus, the formation of GRMs, mainly Few Layer Graphene (FLG) and even graphene, is favoured at temperatures above 900 degrees C. At lower temperatures, carbon nanotubes are formed.
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