Department of Chemistry, University of California , Berkeley, California 94720, United States.
J Am Chem Soc. 2014 Jul 16;136(28):9898-901. doi: 10.1021/ja505286j. Epub 2014 Jul 7.
The mechanistic role of platinum and precious metals in promoting cobalt hydrogenation catalysts of the type used in reactions such as Fischer-Tropsch synthesis is highly debated. Here we use well-defined monometallic Pt and Co nanoparticles (NPs) and CO2 methanation as a probe reaction to show that Pt NPs deposited near Co NPs can enhance the CO2 methanation rate by up to a factor of 6 per Co surface atom. In situ NEXAFS spectroscopy of these same Pt NP plus Co NP systems in hydrogen shows that the presence of nearby Pt NPs is able to significantly enhance reduction of the Co at temperatures relevant to Fischer-Tropsch synthesis and CO2 methanation. The mechanistic role of Pt in these reactions is discussed in light of these findings.
铂和贵金属在促进费托合成等反应中所使用的钴氢化催化剂方面的作用机制存在很大争议。在这里,我们使用了明确的单金属 Pt 和 Co 纳米颗粒(NPs)以及 CO2 甲烷化作为探针反应,表明沉积在 Co NPs 附近的 Pt NPs 可以使 CO2 甲烷化的速率提高至每个 Co 表面原子的 6 倍。在原位氢条件下对这些相同的 Pt NP 加 Co NP 体系进行近边 X 射线吸收精细结构(NEXAFS)光谱研究表明,在与费托合成和 CO2 甲烷化相关的温度下,附近 Pt NPs 的存在能够显著增强 Co 的还原。根据这些发现,讨论了 Pt 在这些反应中的作用机制。