学位论文详细信息
Surface chemistry on interaction of biomass derived oxygenates with heterogeneous catalyst
Biomass;Surface chemistry;Heterogeneous catalyst;IR spectroscopy
So, Jungseob ; Sievers, Carsten Chemical and Biomolecular Engineering Meredith, Carson Deng, Yulin Liotta, Charles ; Sievers, Carsten
University:Georgia Institute of Technology
Department:Chemical and Biomolecular Engineering
关键词: Biomass;    Surface chemistry;    Heterogeneous catalyst;    IR spectroscopy;   
Others  :  https://smartech.gatech.edu/bitstream/1853/61113/1/SO-DISSERTATION-2018.pdf
美国|英语
来源: SMARTech Repository
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【 摘 要 】
The discovery of crude oils in the 19th century and processed inexpensive fuels has contributed to the industrialization of the word and heavily lifted standard of living. However, the alarming about the finite nature and limited availability of fossil fuels has directed government, academy, and industry to focus on finding more sustainable replacements feedstock for transportation fuels and chemicals. Biomass is one of the most promising alternatives for fossil fuels for the production transportation fuels and value-added chemicals. The combination of low vapor pressure and high polarity of most biomass-derived molecules due to its high degree of functionalities often requires processing in the condensed phase for biomass upgrading. The development of effective and efficient processes in petrochemical refining is due to the design of catalyst based on an understanding of the relevant surface chemistry involved. Similarly, the discovery of catalysts for biomass upgrading should depend on an in-depth knowledge of how biomass molecules interact with heterogeneous catalyst surfaces. Investigating the interaction of biomass-derived feedstocks with heterogeneous catalysts is challenging due to their chemical compositions since most traditional surface science techniques require dosing the molecule being investigated via gas phase and the use of ultra-high vacuum conditions. Therefore, there is still a lack of understanding in the reaction mechanisms and surface interactions between biomass-derived oxygenates and catalysts. In this study, we investigated the surface chemistry of the biomass-derived oxygenates IR spectroscopic techniques coupled with the probe molecules which has similar functionality to biomass-derived feedstocks to elucidate the reaction mechanisms and catalyst properties to be active for reactions. This work mainly consists of studies on i) the formation of surface species on 5 wt% Pt/Al2O3 in aqueous phase reforming (APR) reaction using in-situ ATR-IR spectroscopy. ii) the surface chemistry on the adsorption of simple C3 oxygenates on the heteroatom-doped beta zeolites and iii) the formation of oxygen vacancies of MoO3 by interaction with simple C2 oxygenates and their effect on the reaction pathway. These studies proves that a deep understanding of surface chemistry can help with understanding the reaction mechanism at microscopic level and provides a meaningful insights into the efficient design of the heterogeneous catalysts for the biomass upgrading.
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