Yang Yuan, Li Ya-Ke, Zhao Yan-Xia, Wei Gong-Ping, Ren Yi, Asmis Knut R, He Sheng-Gui
State Key Laboratory for Structural Chemistry of Unstable and Stable Species, Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190, P.R. China.
University of Chinese Academy of Sciences, Beijing, 100049, P.R. China.
Angew Chem Int Ed Engl. 2021 Jun 14;60(25):13788-13792. doi: 10.1002/anie.202103808. Epub 2021 May 17.
Catalytic co-conversion of methane with carbon dioxide to produce syngas (2 H +2 CO) involves complicated elementary steps and almost all the elementary reactions are performed at the same high temperature conditions in practical thermocatalysis. Here, we demonstrate by mass spectrometric experiments that RhTiO promotes the co-conversion of CH and CO to free 2 H +CO and an adsorbed CO (CO ) at room temperature; the only elementary step that requires the input of external energy is desorption of CO from the RhTiO CO to reform RhTiO . This study not only identifies a promising active species for dry (CO ) reforming of methane to syngas, but also emphasizes the importance of temperature control over elementary steps in practical catalysis, which may significantly alleviate the carbon deposition originating from the pyrolysis of methane.
甲烷与二氧化碳催化共转化生成合成气（2H + 2CO）涉及复杂的基元步骤，并且在实际的热催化中几乎所有基元反应都在相同的高温条件下进行。在此，我们通过质谱实验证明，RhTiO在室温下促进CH和CO共转化为游离的2H + CO以及吸附的CO（CO ）；唯一需要输入外部能量的基元步骤是CO从RhTiO CO上脱附以重整RhTiO 。这项研究不仅确定了一种用于甲烷干（CO ）重整为合成气的有前景的活性物种，还强调了在实际催化中对基元步骤进行温度控制的重要性，这可能会显著减轻源自甲烷热解的积碳。
