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New insights into structure-activity relationships for propane hydrogenolysis over Ni-Cu bimetallic catalysts

机译:Ni-Cu双金属催化剂上丙烷氢解的结构活性关系的新见解

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Propane hydrogenolysis has been investigated on Ni-Cu/SiO2 model catalysts under elevated pressure conditions. The surface Ni active sites on Ni-Cu/SiO2 were measured by selective hydrogen adsorption under ultrahigh vacuum (UHV) conditions. The specific activity of propane hydrogenolysis shows a slight increase and then decrease with increasing Cu coverages on Ni-Cu/SiO2 bimetallic catalysts, and varies within the 0.6 s(-1) to 2.0 s(-1) range. On the contrary, many previous studies show a three-to-five order decrease in the specific activity of ethane or propane hydrogenolysis over Ni-Cu bimetallic catalysts. The significant difference was explained by the possible over counting of active Ni sites in the selective hydrogen chemisorptions under atmospheric pressure conditions due to hydrogen spillover from Ni to Cu. New structure-activity relationships for Ni-Cu bimetallic catalysts in propane hydrogenolysis were established based on the present work. Furthermore, possible carbon deposits in this reaction were examined by post reaction Auger electron spectroscopy.
机译:已经在高压条件下在Ni-Cu / SiO2模型催化剂上研究了丙烷的氢解反应。通过在超高真空(UHV)条件下进行选择性氢吸附来测量Ni-Cu / SiO2上的表面Ni活性位。丙烷氢解的比活表现出轻微的增加,然后随着Ni-Cu / SiO2双金属催化剂上Cu覆盖率的增加而降低,并且在0.6 s(-1)到2.0 s(-1)范围内变化。相反,许多先前的研究表明,与Ni-Cu双金属催化剂相比,乙烷或丙烷的氢解比活性降低了三到五个数量级。显着性差异的解释是,由于氢气从Ni扩散到Cu,在大气压力条件下选择性氢气化学吸附中可能存在的活性Ni位置的计数过高。基于目前的工作,建立了Ni-Cu双金属催化剂在丙烷氢解中的新的结构-活性关系。此外,通过后反应俄歇电子能谱检查了该反应中可能的碳沉积。

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