Tang Xin, Song Chuqiao, Li Haibo, Liu Wenyu, Hu Xinyu, Chen Qiaoli, Lu Hanfeng, Yao Siyu, Li Xiao-Nian, Lin Lili
Institute of Industrial Catalysis, State Key Laboratory of Green Chemistry Synthesis Technology, College of Chemical Engineering, Zhejiang University of Technology, Hangzhou, Zhejiang, 310014, China.
Zhejiang Carbon Neutral Innovation Institute & Zhejiang International Cooperation Base for Science and Technology on Carbon Emission Reduction and Monitoring, Zhejiang University of Technology, Hangzhou, 310014, China.
Nat Commun. 2024 Apr 10;15(1):3115. doi: 10.1038/s41467-024-47403-4.
Nickel is the most widely used inexpensive active metal center of the heterogeneous catalysts for CO hydrogenation to methane. However, Ni-based catalysts suffer from severe deactivation in CO methanation reaction due to the irreversible sintering and coke deposition caused by the inevitable localized hotspots generated during the vigorously exothermic reaction. Herein, we demonstrate the inverse CeAlO/Ni composite constructed on the Ni-foam structure support realizes remarkable CO methanation catalytic activity and stability in a wide operation temperature range from 240 to 600 °C. Significantly, CeAlO/Ni/Ni-foam catalyst maintains its initial activity after seven drastic heating-cooling cycles from RT to 240 to 600 °C. Meanwhile, the structure catalyst also shows water resistance and long-term stability under reaction condition. The promising thermal stability and water-resistance of CeAlO/Ni/Ni-foam originate from the excellent heat and mass transport efficiency which eliminates local hotspots and the formation of Ni-foam stabilized CeAlO/Ni inverse composites which effectively anchored the active species and prevents carbon deposition from CH decomposition.
镍是用于将一氧化碳加氢制甲烷的多相催化剂中使用最广泛且价格低廉的活性金属中心。然而,由于在剧烈放热反应过程中不可避免地产生局部热点,导致不可逆烧结和积碳,镍基催化剂在一氧化碳甲烷化反应中会严重失活。在此,我们展示了在泡沫镍结构载体上构建的反相CeAlO/Ni复合材料在240至600 °C的宽操作温度范围内实现了显著的一氧化碳甲烷化催化活性和稳定性。值得注意的是,CeAlO/Ni/泡沫镍催化剂在从室温到240至600 °C的七个剧烈加热-冷却循环后仍保持其初始活性。同时,该结构催化剂在反应条件下还表现出耐水性和长期稳定性。CeAlO/Ni/泡沫镍具有良好的热稳定性和耐水性,这源于其优异的传热传质效率消除了局部热点,以及泡沫镍稳定的CeAlO/Ni反相复合材料的形成有效地固定了活性物种并防止了CH分解产生的碳沉积。