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Effect of the Synthetic Method on the Properties of Ni-Based Hydrogen Oxidation Catalysts.

ABSTRACT: The latest progress in alkaline anion-exchange membranes has led to the expectation that less costly catalysts than those of the platinum-group metals may be used in anion-exchange membrane fuel cell devices. In this work, we compare structural properties and the catalytic activity for the hydrogen-oxidation reaction (HOR) for carbon-supported nanoparticles of Ni, Ni₃Co, Ni₃Cu, and Ni₃Fe, synthesized by chemical and solvothermal reduction of metal precursors. The catalysts are well dispersed on the carbon support, with particle diameter in the order of 10 nm, and covered by a layer of oxides and hydroxides. The activity for the HOR was assessed by voltammetry in hydrogen-saturated aqueous solutions of 0.1 mol dm^-1 KOH. A substantial activation by potential cycling of the pristine catalysts synthesized by solvothermal reduction is necessary before these become active for the HOR; in situ Raman spectroscopy shows that after activation the surface of the Ni/C, Ni₃Fe, and Ni₃Co catalysts is fully reduced at 0 V, whereas the surface of the Ni₃Cu catalyst is not. The activation procedure had a smaller but negative impact on the catalysts synthesized by chemical reduction. After activation, the exchange-current densities normalized with respect to the ECSA (electrochemically active surface area) were approximately independent of composition but relatively high compared to catalysts of larger particle diameter.

SUBMITTER: Davydova ES

PROVIDER: S-EPMC8153405 | biostudies-literature |

REPOSITORIES: biostudies-literature

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Project description:Deactivation of catalysts due to rapid blocking of active surfaces and pores is a major problem for methane cracking. The removal of the template using different calcination methods contributes to the different characteristics of catalyst support. Therefore, silica supports were prepared with the sol-gel method, where sodium silicate and chitosan are a silica source and a template, respectively. Calcination using a microwave muffle furnace (MWF) was preferred over the conventional electric muffle furnace at the heating rates of 2 and 17 °C/min (CEF2 and CEF17, respectively) in order to remove the chitosan template. A nickel nitrate precursor was loaded onto the obtained silica supports by the incipient wetness impregnation method. The properties of the silica support and the Ni/SiO2 catalysts were characterized by means of N2-sorption, X-ray diffraction, scanning electron microscopy-energy-dispersive X-ray, field emission transmission electron microscopy, and H2 temperature-programmed reduction. The catalytic activity was evaluated using a fixed-bed reactor at 550 °C with a CH4/N2 ratio of 1:4 in the feed. The amount and the allotropes of carbon deposited on the spent catalysts were investigated using thermogravimetric/differential thermal analysis. The results showed that the SiO2-MWF support had a higher surface area and a larger pore volume of a mesoporous structure with larger interparticle channels than that of the SiO2-CEF supports. This leads to the higher dispersion of Ni metal particles over and inside the interparticle channels of the SiO2-MWF support. This provided a higher metal-support interaction, resulting in lower rates of methane conversion and carbon deposition on the catalyst surface than those of Ni/SiO2-CEF catalysts. However, it displayed a lower bed pressure. It was found that the carbon fibers deposited on all the catalysts were multiwalled carbon nanotubes (MWCNTs). Additionally, the base-growth mechanism of MWCNTs was only exhibited by the Ni/SiO2-MWF catalyst.

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Effect of the Synthetic Method on the Properties of Ni-Based Hydrogen Oxidation Catalysts.

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