The Catalytic, Selective Partial Oxidation of Alkanes by Transition Metals that Activate Carbon-Hydrigen Bonds

劳伦斯·库尔9310198这是一种尝试开发一种使用铂催化剂和含水过渡金属氧化剂将烷烃直接转化为部分氧化产物的方法。这种方法不同于目前可用的方法，因为它不需要分子氧。这项工作包括对铂/铁水体系的关键评价，包括实验变量，高转化率下的选择性，以及阐明机理，被认为涉及烷基铂氢化合物；催化剂载体效应；钯替代铂；各种过渡金属水氧化剂的使用；以及可模拟铂表面碳氢键断裂的可溶性有机铂配合物的设计、合成和评价。低碳烷(甲烷、丙烷、天然气等)的直接部分氧化是催化技术的一个重要目标；目前的方法要么范围非常有限，要么是繁琐的多步骤过程。这些过程的产物，如甲醇、乙醇、甲醛、醋酸等，作为化学原料、燃料或单体有许多用途，或者它们可以进一步加工以改善现有燃料。尽管为实现这一目标做了很多工作，但这项工作的方法与常规努力截然不同。这是与俄罗斯切尔诺戈洛夫卡化学物理研究所的A·E·希洛夫的合作。

Lawrence Kool 9310198 This is an attempt to develop a method to convert alkanes directly to partially oxidized products using a platinum catalyst and an aqueous transition-metal oxidant. The approach differs from currently available methods in that it does not require molecular oxygen. This effort includes a critical evaluation of the platinum/aqueous ferric system covering experimental variables, selectivity at high conversion, and elucidation of the mechanism, which is thought to involve an alkylplatinum hydride intermediate; catalyst support effects; substitution of palladium for platinum; the use of various aqueous transition-metal oxidants; and the design, synthesis, and evaluation of soluble organoplatinum complexes that may model the carbon-hydrogen bond cleavage on the platinum surface. Direct partial oxidation of light alkanes (methane, propane, natural gas, etc.) is an important objective of catalytic technology; current methods are either very limited in scope or are cumbersome multistep processes. The products of such processes, such as methanol, ethanol, formaldehyde, acetic acid, etc., have many uses as chemical feedstocks, fuels, or monomers, or they can be further processed to improve existing fuels. Although there is much work toward this objective, the approach in this work is a radical departure from conventional efforts. This is a collaboration with A. E. Shilov at the Institute of Chemical Physics in Chernogolovka, Russia.