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Exsolution-based Co/Ni bimetallic Catalysts for Dry Reforming of Methane
Dong Hyun Kim(김동현),Ahmed Al-Shahat Eissa(아흐메드 알사하트 이사),Kyubock Lee(이규복) 한국에너지기후변화학회 2021 한국에너지기후변화학회 학술대회 Vol.2021 No.11
Ni-based catalysts are widely used for dry reforming of methane (DRM), due to their high catalytic activity and low-cost. However, Ni-based catalysts suffer from deactivation, especially under long-term operating conditions, because of carbon deposition and catalyst sintering. As a result, the design of efficient noble-metal-free catalysts for the DRM still a great challenge. Incorporating another element with Ni has been reported to promote the catalytic activity and coke resistance of catalyst. In this study, we report a facile strategy for fabricating CoNi/MgAl₂O₄ catalyst by one-pot evaporation induced self-assembly combine with exsolution method. During the reduction process, the active metals were successfully exsolved on the catalyst surface, and it was confirmed that CoNi alloy was formed. Our results demonstrate that the formation of a stable exsolved CoNi alloy is an important factor for maintaining the catalyst durability under long-term DRM reaction conditions, and the catalytic activity varies greatly depending on the nickel content. At Co:Ni ratio of 1:4, the catalyst showed a surface area of 175 ㎡/g, and particles size of 12 - 14 nm. When applied for the DRM reaction at 800 ℃ and gas hourly space velocity of 36,000 h<SUP>-1</SUP>, it exhibited CO₂ and CH₄ conversions of 98 and 92%, respectively. After serving for the DRM reaction for 100 h, the catalyst displayed CO₂ and CH₄ conversions of 94 and 85%, respectively, indicating the excellent durability of the herein synthesized catalyst. In addition, a small amount of carbon (3.1%) was deposited on the catalyst’s surface after the long-term reaction test. The insights obtained from this study may have broad applications in developing highly stable CoNi bimetallic catalysts for methane reforming reactions.