Wang Hui, Cui Guoqing, Lu Hao, Li Zeyang, Wang Lei, Meng Hao, Li Jiong, Yan Hong, Yang Yusen, Wei Min
State Key Laboratory of Chemical Resource Engineering, Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, 100029, Beijing, P. R. China.
State Key Laboratory of Heavy Oil Processing, China University of Petroleum (Beijing), 102249, Beijing, P. R. China.
Nat Commun. 2024 May 4;15(1):3765. doi: 10.1038/s41467-024-48122-6.
The dry reforming of methane provides an attractive route to convert greenhouse gases (CH and CO) into valuable syngas, so as to resolve the carbon cycle and environmental issues. However, the development of high-performance catalysts remains a huge challenge. Herein, we report a 0.6% Ir/CeO catalyst with a metal-support interface structure which exhibits high CH (72%) and CO (82%) conversion and a CH reaction rate of ~973 μmol g s which is stable over 100 h at 700 °C. The performance of the catalyst is close to the state-of-the-art in this area of research. A combination of in situ spectroscopic characterization and theoretical calculations highlight the importance of the interfacial structure as an intrinsic active center to facilitate the CH dissociation (the rate-determining step) and the CH* oxidation to CHO* without coke formation, which accounts for the long-term stability. The catalyst in this work has a potential application prospect in the field of high-value utilization of carbon resources.
甲烷干重整为将温室气体（CH₄和CO₂）转化为有价值的合成气提供了一条有吸引力的途径，从而解决碳循环和环境问题。然而，开发高性能催化剂仍然是一个巨大的挑战。在此，我们报道了一种具有金属-载体界面结构的0.6% Ir/CeO₂催化剂，该催化剂表现出高的CH₄转化率（72%）和CO₂转化率（82%），CH₄反应速率约为973 μmol g⁻¹ s⁻¹，在700℃下100小时内保持稳定。该催化剂的性能接近该研究领域的最先进水平。原位光谱表征和理论计算相结合突出了界面结构作为促进CH₄解离（速率决定步骤）和CH₄氧化为CHO而不形成焦炭的本征活性中心的重要性，这解释了其长期稳定性。这项工作中的催化剂在碳资源高值利用领域具有潜在的应用前景。
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