(TSE03-C)Alkane production from renewable biomass by aqueous-phase catalytic reforming: A combined experimental and theoretical approach

该项目将利用新发现的低温水相重整工艺，从生物质衍生的含氧碳氢化合物催化生产烷烃。这一新工艺为利用可再生生物质资源生产烷烃提供了一条新途径。这项创新的核心是在低温（接近200摄氏度）下，通过含氧碳氢化合物与液态水的反应生产富含碳氢化合物的燃气。主要优点包括：(1)不需要挥发水就能生成烷烃，这是一项重大的节能措施；(2)在有利于水气转换反应的温度下运行，这使得在单个化学反应器中产生低含量CO的高质量燃气成为可能。这一过程为现代高效内燃机提供了一种生物可再生燃料。可再生烷烃与高效ICEs的结合提供了一种很有前途的方法，可以可持续地产生机械和电力能源，这是温室气体中性的，因为重整过程中排放的二氧化碳被下一年的生物质增长所消耗。这一新工艺对烷烃生产的潜在技术影响是巨大的，导致美国经济对进口化石燃料的依赖大大减少。目前确定的水相重整法生成烷烃的最佳催化剂是铂，铂是一种昂贵的金属。进一步的研究将用于开发新一代催化剂，以提供具有成本效益的方法，利用水相重整过程转化从生物质流中提取的反应物来生成烷烃。将研究添加剂以提高pt基催化剂的性能、成本和效率。反应条件（如温度、压力、进料浓度、溶液pH值）也将改变，以控制产品分布，并确定长时间在蒸汽上的催化性能。这些研究将依赖于：(1)高通量筛选候选催化剂，(2)对最有希望的候选催化剂进行详细的催化反应动力学研究，(3)对最有希望的催化材料进行光谱和表征研究，以及(4)对过渡金属上的C-C、C-O、C-H和O-H键活化进行系统的第一性原理研究。

This project will address the catalytic production of alkanes from biomass-derived oxygenated hydrocarbons utilizing a newly discovered low-temperature aqueous-phase reforming process. This new process provides a route for generation of alkanes from renewable biomass resources. The core of the innovation is the production of hydrocarbon-rich fuel-gas by reactions of oxygenated hydrocarbons with liquid water at low temperatures (near 200 C). The main advantages include: (1) generation of alkanes without the need to volatilize water, which represents a major energy saving, and (2) operation at temperatures where the water-gas shift reaction is favorable, making it possible to generate high-quality fuel-gas with low amounts of CO in a single chemical reactor. The process provides a strategy for delivering a biorenewable fuel for modern, highly efficient internal combustion engines (ICEs). The combination of renewable alkanes with efficient ICEs provides a promising method for sustainable generation of mechanical and electrical energy that is green house gas neutral, since the CO2 emitted from the reforming process is consumed by the next year's growth of biomass. The potential technological impact of this new process for the production of alkanes is substantial, leading to a considerable decrease in the dependence of the US economy on imported fossil fuels.The best catalysts identified at present for the generation of alkanes by the aqueous-phase reforming process are based on platinum, which is an expensive metal. Further research will be conducted to develop a new generation of catalysts to provide cost-effective methods to generate alkanes using the aqueous-phase reforming process to convert reactants extracted from biomass streams. Additives will be investigated to improve the performance, cost, and efficiency of Pt-based catalysts. The reaction conditions (such as temperature, pressure, feed concentrations, solution pH) will also be varied to control the product distribution, and catalytic performance with respect to long times on-steam will be determined. The investigations will rely on: (1) high throughput screening of catalyst candidates, (2) detailed catalytic reaction kinetics studies of the most promising catalyst candidates, (3) spectroscopic and characterization studies of the most promising catalytic materials, and (4) systematic first-principles studies for C-C, C-O, C-H, and O-H bond activation on transition metals.