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

活化碳氢键的过渡金属对烷烃的催化选择性部分氧化

• 批准号: 9310198
• 负责人: William Armstrong
• 金额: $ 24.2万
• 依托单位: Boston College
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 1993
• 资助国家: 美国
• 起止时间: 1993-08-01 至 1997-01-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=9310198&HistoricalAwards=false
• 关键词: Catalytic; Selective; Partial; Oxidation; Alkanes

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.

这是一种利用铂催化剂和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的尝试。该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/水铁体系的关键评估，包括实验变量，高转化率下的选择性，以及机制的阐明，这被认为涉及烷基铂氢化中间体；催化剂支撑效应；钯取代铂的研究各种水性过渡金属氧化剂的使用；以及可模拟铂表面碳氢键解理的可溶性有机铂配合物的设计、合成和评价。轻烷烃（甲烷、丙烷、天然气等）的直接部分氧化是催化技术的重要目标；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、乙酸等，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进现有的燃料。尽管朝着这个目标还有很多工作要做，但这项工作的方法与传统的努力是完全不同的。这是与俄罗斯切尔诺戈洛夫卡化学物理研究所的a·e·希洛夫合作的成果。