生物油/水蒸汽/CO2重整制氢体系中催化剂积碳机理和基本规律研究

Bio-oil is a kind of liquid fuel obtained by fast pyrolysis of biomass. The high oxygen content, low pH value, poor stability and corrosivity limit the scale application of bio-oil. In recent years, bio-oil and its water-phase catalytic reforming for hydrogen production are particularly noteworthy, but the catalyst deactivation is the biggest bottleneck to constraint the industrialization of the process. In order to prevent the catalyst deactivation of carbon deposition, this project puts forward the bio-oil/water/CO2 reforming system for hydrogen production. There are more key technical problems in the reforming system. The mainly problem is the carbon of the catalyst and it needs to study the key scientific problems of "mechanism of carbon deposition and carbon features of the catalyst" to solve. Around the key scientific problems, it needs to research the mass transfer and reaction characteristics of bio-oil/water/CO2 reforming process to explore the mechanism of reforming reaction and establish the carbon dynamics model. It needs to research the carbon formation mechanism of the process to reduce the amount of carbon deposition. To research the composition, structure and morphology of the carbon can provide theoretical support for preparation of anti-carbon deposition catalyst. To research the steam, CO2 regeneration mechanism and method of the deactivated catalyst can prolong the life of the catalyst. All research will be providing a certain theoretical guidance for the industrial application of bio-oil/flue gas reforming for hydrogen production.

生物油是生物质通过快速热裂解制备的一种液体燃料，生物油具有含氧量高、pH值低、不稳定性和腐蚀性等特点，限制了其规模化利用。近年来生物油及其水相催化重整制氢尤其引人注目，但催化剂容易积碳失活是制约该技术工业化的最大瓶颈。为了防止催化剂积碳失活，本项目提出了生物油/水蒸汽/CO2重整制氢反应体系，该体系中存在较多关键技术问题，其中主要是催化剂积碳问题，该问题需要通过研究"催化剂积碳机理及积碳特征"这一关键科学问题来解决。围绕关键科学问题，通过研究生物油/水蒸汽/CO2重整过程的传质及其反应特性，探索重整制氢反应机理，并建立积碳动力学模型；通过研究生物油重整过程中积碳形成机理，降低积碳反应的发生；通过研究积碳物种的组成、结构和形态，为制备抗积碳催化剂提供理论支持；通过研究失活催化剂的蒸汽、CO2再生机理及方法，延长催化剂的寿命。该项目的研发将为生物油/烟道气重整制氢工业化应用提供一定的理论指导。

生物油及其水相催化重整制氢是一种较好的利用生物油的方法，但重整过程中催化剂容易积碳失活。为了阐明催化剂积碳特征和积碳机理，本项目提出了生物油/水蒸汽/CO2重整制氢反应体系，开发了生物油/CO2干重整和生物油/水蒸汽/CO2联合重整技术，深入研究了生物油两段催化重整制氢技术，降低了金属催化剂的失活速率；阐明了重整制氢过程中催化剂积碳规律及积碳特征, 探究了积碳物种的组成、结构和形态，并制备了一种抗积碳催化剂Ni/MgO-La2O3-Al2O3；开发了失活催化剂的蒸汽、CO2再生机理及方法，为延长催化剂的寿命提供了理论基础。开发了微波裂解制备生物油技术。该项目的研究成果中生物油/水蒸汽/CO2联合重整技术，积碳机理，失活催化剂再生技术等为生物油重整制氢工业化应用提供一定的理论指导。