Department of Chemical Engineering and Materials Science, University of Minnesota, 421 Washington Ave SE, Minneapolis, MN 55455, USA.
ChemSusChem. 2011 Aug 22;4(8):1151-6. doi: 10.1002/cssc.201100026. Epub 2011 Aug 10.
The concurrent decomposition and deoxygenation of ethanol was accomplished in a stratified reactor with 50-80 ms contact times. The stratified reactor comprised an upstream oxidation zone that contained Pt-coated Al(2)O(3) beads and a downstream dehydration zone consisting of H-ZSM-5 zeolite films deposited on Al(2)O(3) monoliths. Ethanol conversion, product selectivity, and reactor temperature profiles were measured for a range of fuel:oxygen ratios for two autothermal reactor configurations using two different sacrificial fuel mixtures: a parallel hydrogen-ethanol feed system and a series methane-ethanol feed system. Increasing the amount of oxygen relative to the fuel resulted in a monotonic increase in ethanol conversion in both reaction zones. The majority of the converted carbon was in the form of ethylene, where the ethanol carbon-carbon bonds stayed intact while the oxygen was removed. Over 90% yield of ethylene was achieved by using methane as a sacrificial fuel. These results demonstrate that noble metals can be successfully paired with zeolites to create a stratified autothermal reactor capable of removing oxygen from biomass model compounds in a compact, continuous flow system that can be configured to have multiple feed inputs, depending on process restrictions.
在具有 50-80ms 接触时间的分层反应器中完成了乙醇的同时分解和脱氧。分层反应器由上游氧化区组成,该氧化区包含涂有 Pt 的 Al(2)O(3)珠和下游脱水区组成,该脱水区由沉积在 Al(2)O(3)整体式上的 H-ZSM-5 沸石膜组成。对于两种自热式反应器构型,使用两种不同的牺牲燃料混合物:平行的氢-乙醇进料系统和串联的甲烷-乙醇进料系统,测量了一系列燃料:氧气比的乙醇转化率、产物选择性和反应器温度分布。与燃料相比,增加氧气的量会导致两个反应区中乙醇转化率的单调增加。转化的大部分碳以乙烯的形式存在,其中乙醇的碳-碳键保持完整,而氧被去除。使用甲烷作为牺牲燃料可实现超过 90%的乙烯收率。这些结果表明,贵金属可以与沸石成功配对,以创建分层自热式反应器,该反应器能够在紧凑的连续流动系统中从生物质模型化合物中去除氧,该系统可以根据工艺限制配置多个进料输入。