Ethanol Steam Reforming on Ni-Based Catalysts: Effect of Cu and Fe Addition on the Catalytic Activity and Resistance to Deactivation

Abstract

Ethanol steam reforming (ESR) on a group of multifunctional xFeyCu10Ni-Beta catalysts was studied using in X-ray diffraction (XRD), scanning electron microscopy coupled with energy-dispersive spectroscopy (SEM-EDS), temperature-programmed reduction in hydrogen (H2-TPR), temperature-programmed oxidation (TPO), and X-ray absorption fine structure (XAFS) techniques with a focus on the structural characterization of the active sites, the effect of different amounts of Cu and Fe phases and understanding the reaction pathway for the catalysts. The 1.5Fe1.5Cu10Ni-Beta catalyst exhibited very good catalytic performance for the ESR, including high activity, high H2 selectivity, and low undesired products, because of the synergistic catalysis of Ni, Cu, and Fe phases. The Cu site preferentially facilitates the dehydrogenation of ethanol at the initial reaction step, and with subsequent Ni metal catalyzes dissociation of the C–C bond in acetaldehyde to form CO and CH4. The Fe phase, which has a tendency to be enriched on the alloy particle surface, is suitable for acetaldehyde and CH4 reforming above 350 °C. Moreover, the effect of the Cu–Ni­(Fe) alloy could further to enhance the catalytic performance of the ESR reaction. The analyses of deactivated catalyst by means of several techniques suggest that the synergistic effect among Ni, Cu, and Fe phases on the spent catalysts proved to be highly resistant to coking, compared to the monometallic Ni catalysts, and the multifunctional catalyst exhibited very good antisintering ability.

First-principles study of a new structure and oxidation mechanism of Pt3Zr

“…are important parts of solid oxide fuel cells. [32][33][34][35] To estimate the catalytic activity of Pt 3 Zr, we compare the oxygen doped formation energy between Pt 3 Zr and many metals. As shown in Fig.…”

Selective steam reforming of n‐dodecane over stable subnanometric NiPt clusters encapsulated in Silicalite‐1 zeolite

“…Generally, hydrogen has been mainly produced by partial oxidation, steam reforming, and autothermal reforming of natural gas and petroleum oil fractions . Among these technologies, catalytic steam reforming of hydrocarbons is a dominant way for industrial‐scale hydrogen production on account of its mature technology and low cost . Long‐chain hydrocarbons are considered as the promising feedstock for on‐board hydrogen generation, owing to its good properties in relatively easy transport and high energy density …”

“…[4][5][6][7][8] Among these technologies, catalytic steam reforming of hydrocarbons is a dominant way for industrial-scale hydrogen production on account of its mature technology and low cost. 9,10 Long-chain hydrocarbons are considered as the promising feedstock for on-board hydrogen generation, owing to its good properties in relatively easy transport and high energy density. [11][12][13] For the steam reforming of hydrocarbons, nickel-based catalysts have been widely employed for its excellent activity in breaking C─C and C─H bonds.…”

Effects of dealumination on the performance of Ni-containing BEA catalysts in bioethanol steam reforming

“…In spite of vast literature devoted to the ESR reaction in the last years, zeolite supported catalysts have not been widely studied. The micro-mesoporous structure of zeolites may promote formation of the small metal nanoparticles [16][17][18][19][20][21]. On the other hand, high acidity of zeolites may drive to the extensive formation of carbon deposits in the ESR reaction.…”