Abstract

<p class="Default">Nickel catalysts supported on different carriers (θ-Al<sub>2</sub>O<sub>3</sub>, γ-Al<sub>2</sub>O<sub>3</sub>, HZSM-5 with γ-Al<sub>2</sub>O<sub>3</sub>, HZSM-5, and NaX) have been investigated for the partial oxidation of methane. All the supported nickel catalysts showed a high activity for the formation of synthesis gas, and γ-Al<sub>2</sub>O<sub>3</sub> was the most effective among all the tested carriers. The effect of the heat-treatment temperature of the 3 wt.% Ni/γ-Al<sub>2</sub>O<sub>3</sub> catalyst on its catalytic activity was studied, and a considerable decrease in its activity was observed by the heat-treatment of the catalyst at 1000 °C compared with the catalysts prepared by the 300–800 °C – calcination. The XRD analysis suggested the formation of NiAl<sub>2</sub>O<sub>4</sub> that is a non-reducible compound at the high calcination temperature. The addition of a modifier (Co, Ce, or La) to the 3 wt.% Ni/γ-Al<sub>2</sub>O<sub>3</sub> catalyst increased the selectivity to H<sub>2</sub> and CO with the decreasing selectivity to CO<sub>2</sub>, and the highest selectivity to H<sub>2</sub> was obtained by the 5 wt.% NiLa/γ-Al<sub>2</sub>O<sub>3</sub>. The developed 5 wt.% NiLa/γ-Al<sub>2</sub>O<sub>3</sub> catalyst showed a high stability for 30 h for the partial oxidation of methane at 750 °C. The methane conversion reached 95%, selectivity to hydrogen 83% and 52% to carbon monoxide.</p>

Highlights

  • According to the International Energy Agency (IEA), the demand of natural gas for energy production will increase until 2020

  • The composition of synthesis gas obtained in the process is more preferable for the production of methanol and liquid products by the Fischer-Tropsch reaction, because the cost of synthesis-gas produced by the partial oxidation of methane is estimated to be almost 1.5 times lower than that produced by steam reforming [6, 7]

  • Carriers (θ-Al2O3, γ-Al2O3, HZSM-5 with Al2O3, HZSM-5, and NaX) with different properties have been investigated for the partial oxidation of methane

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Summary

Introduction

According to the International Energy Agency (IEA), the demand of natural gas for energy production will increase until 2020. Synthesis gas is produced by the steam-reforming of natural gas, the most promising one of all the known processes for synthesis–gas production is the oxidative conversion of methane. Various nickel-based catalysts, such as Ni-γAl2O3 [14, 15], Ni-M-γ-Al2O3 (M = La [16], Co [17], Rh [18] and Cu [19]), and Ni supported on La2O3, CeLaOx, and CeO2 [20], were investigated for the oxidative conversion of methane. In these reactions, most of the catalysts showed a high activity, and the methane conversion value were in the range of 67–95%. The effects of promoting additives (Co2O3, CeO2, La2O3) on the performance and the physicochemical characteristics of the nickel catalysts were investigated

Experimental
Results and Discussion
Conclusions
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