Abdel-Mageed Ali M, Widmann Daniel, Eckle Stephan, Behm R Jürgen
Institute of Surface Chemistry and Catalysis, Ulm University, 89069, Ulm, Germany.
Department of Chemistry, Faculty of Science, Cairo University, Giza, 12613, Egypt.
ChemSusChem. 2015 Nov;8(22):3869-81. doi: 10.1002/cssc.201500883. Epub 2015 Oct 12.
To better understand the role of water in the selective methanation of CO in CO2-rich reformate gases on Ru/Al2O3 catalysts, the influence of exposing these catalysts to H2O-rich reformate gases on their reaction characteristics in transient experiments was investigated by employing kinetic and in situ spectroscopic measurements as well as ex situ catalyst characterization. Transient exposure of the ruthenium catalyst to wet reaction gas (5 or 15% H2O) results in significantly enhanced activity and selectivity for CO methanation in subsequent reactions in dry reformate compared with activation and reaction in dry reformate directly. Operando X-ray absorption spectroscopy results reveal that this is in accordance with a significant decrease in ruthenium particle size, which is stable during subsequent reaction in dry reformate. The implications of these data and additional results from in situ IR spectroscopy on the role and influence of H2O on the reaction, also in technical applications, are discussed.
为了更好地理解水在富CO₂重整产物气中CO在Ru/Al₂O₃催化剂上的选择性甲烷化反应中的作用,通过动力学和原位光谱测量以及非原位催化剂表征,研究了在瞬态实验中将这些催化剂暴露于富水重整产物气对其反应特性的影响。与直接在干重整产物气中活化和反应相比,将钌催化剂瞬态暴露于湿反应气(5%或15% H₂O)会导致在随后的干重整产物气反应中CO甲烷化的活性和选择性显著提高。原位X射线吸收光谱结果表明,这与钌颗粒尺寸的显著减小一致,该尺寸在随后的干重整产物气反应中保持稳定。讨论了这些数据以及原位红外光谱的其他结果对H₂O在反应中的作用和影响的意义,以及在技术应用中的情况。