Methanol and Hydrocarbon Catalysis of Palladium Particles and Palladium Carbonyl Clusters in Sodium Zeolite-Y

最近，利用“瓶中船”技术在钠沸石- y笼中成功制备了钯羰基配合物，这可能为利用沸石的几何和电子特性提供新的催化过程。本文在沸石- y上制备了钯催化剂，包括一些高度分散的催化剂和一些含有钯团簇的催化剂。在其他技术中，使用扩展x射线吸收精细结构，傅里叶变换红外光谱，程序升温反应和程序升温脱附来表征这些材料。一氧化碳在气态，吸附和配体形式的互换性是用红外光谱和温度程序化同位素交换确定的。测定了甲醇合成、新极性转化和相关反应的催化活性。在这项工作中研究的新型催化剂具有潜在的革命性。它应该提供目前在许多工业过程中使用的催化剂无法提供的选择性类型。目前，很难预测这些新系统的活性与旧催化剂的活性相比如何，但这项努力应该在回答这个问题方面有很长的路要走。

Recent success in preparing carbonyl complexes of palladium in the cages of sodium zeolite-Y using a "ship-in-a-bottle" technique potentially offers new catalytic processes exploiting both geometric and electronic properties of the zeolite. In this work, palladium catalysts on zeolite-Y are prepared, including some that are highly dispersed and some containing palladium clusters. These are characterized using, among other techniques, extend X-ray absorption fine structure, Fourier-transform infrared spectroscopy, temperature-programmed reaction, and temperature-programmed desorption. The exchangeability of carbon monoxide in gaseous, adsorbed, and ligand forms is determined using infrared spectroscopy and temperature-programmed isotope exchange. Catalytic activity for methanol synthesis, neopentance conversion, and related reactions are measured. The new class of catalysts investigated in this work is potentially revolutionary. It should offer types of selectivity not available with catalysts presently in use for a number of industrial processes. At present, it is difficult to predict how the activities of these new systems compare to those of older catalysts, but this effort should go a long way toward answering that.