Selectivity of Catalytic Partial Oxidation Reactions and Reactors

摘要-施密特-962992在单步整体反应器中以极短的接触时间部分氧化烷烃生成化学品有望开辟化学合成的新途径。PI计划对这些过程进行系统检查，努力通过直接氧化小链烷烃来产生含氧有机分子，以形成醛、酮、醇和酸等产品。这将包括在高温反应器配置的低面积整体载体上的氧化物催化剂，具有快速点火、完全反应和快速猝灭，以最大限度地减少不必要的均质反应和中间体的分解。两个项目将涉及(1)在短接触时间内使用氧化物催化剂，高温部分氧化反应次数不超过20毫秒，温度高于6000摄氏度；(2)微秒级反应器，其中利用快速加热和快速淬火来优化多相-均相部分氧化过程，时间远不到1毫秒。特别要探讨的主题是：(1)高级烷烃、其他氧化剂和氨氧化的使用；(2)反应物喷射和级间冷却或加热的分层整体的使用；(3)超高和超音速流动效应的开发；以及(4)流态化反应器的进一步研究。PI将寻找新的催化剂体系和反应器几何结构，在这些条件下可以稳定运行，从而在高转化率下对特定产品产生非平衡选择性。这些过程的机理和优化也将通过对反应、传质、热传递和流体流动效应的广泛模拟来探索。

Abstract - Schmidt - 962992 Partial oxidation of alkanes to produce chemicals in single step monolith reactors at very short contact times promises to open new routes to chemical synthesis. The PI plans a systematic examination of these processes in an effort to produce oxygen-containing organic molecules by direct oxidation of small alkanes to form products such as aldehydes, ketones, alcohols, and acids. This will involve oxide catalysts on low area monolith supports in high temperature reactor configurations with rapid ignition, complete reaction, and rapid quenching to minimize unwanted homogeneous reactions and decomposition of intermediates. Two projects will involve (1) the use of oxide catalysts in short contact time, high temperature partial oxidation reactions for times less than 20 milliseconds and temperatures above 6000C and (2) microsecond reactors in which rapid heating and rapid quenching are exploited to optimize heterogeneous-homogeneous partial oxidation processes in times much less than one millisecond. Particular topics to be explored are (1) use of higher alkanes, other oxidants, and ammoxidation, (2) use of stratified monoliths with reactant injection and interstage cooling or heating, (3) exploitation of very high and sonic flow effects, and (4) further investigation of fluidized bed reactors. The PI will search for new catalyst systems and reactor geometries which can be operated in a stable state under these conditions and thus produce nonequilibrium selectivities to particular products at high conversions. The mechanisms and optimization of these processes will also be explored through extensive simulations of reactions, mass transfer, heat transfer, and fluid flow effects.