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Research is being actively conducted to improve the carbon deposition and sintering resistance of Ni-based catalysts. Among them, the Al2O3-supported Ni catalyst has been broadly studied for the dry reforming reaction due to its high CH4 activity at the beginning of the reaction. However, there is a problem of deactivation due to carbon deposition of Ni/Al2O3 catalyst and sintering of Ni, which is a catalytically active material. Supplementing MgO in Ni/Al2O3 catalyst can result in an improved MgAl2O4 spinel structure and basicity, which can be helpful for the activation of methane and carbon dioxide molecules. In order to confirm the optimal supports’ ratio in Ni/MgO-Al2O3 catalysts, the catalysts were prepared by supporting Ni after controlling the MgO:Al2O3 ratio stepwise, and the prepared catalysts were used for CO2 reforming of CH4 (CDR) using coke oven gas (COG). The catalytic reaction was conducted at 800 °C and at a high gas hourly space velocity (GHSV = 1,500,000 h−1) to screen the catalytic performance. The Ni/MgO-Al2O3 (MgO:Al2O3 = 3:7) catalyst showed the best catalytic performance between prepared catalysts. From this study, the ratio of MgO:Al2O3 was confirmed to affect not only the basicity of the catalyst but also the dispersion of the catalyst and the reducing property of the catalyst surface.

CO2 Reforming of CH4 Using Coke Oven Gas over Ni/MgO-Al2O3 Catalysts: Effect of the MgO:Al2O3 Ratio