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バイオマスから化学品および冶金コークスを製造するための多段熱分解に関する研究

魏, 富 WEI, FU ウエイ, フー 九州大学

2022.09.22

概要

The world currently faces the challenge of reducing its reliance on fossil fuels and achieving a sustainable supply of renewable energy. The full development and utilization of lignocellulosic biomass, the only recyclable carbon source, is an important strategy for producing chemicals and liquid fuels to solve energy shortages and reduce CO2 emissions. Pyrolysis of lignocellulosic biomass, which can convert biomass into a series of high value-added products, especially pyrolytic volatiles containing a variety of condensable fine chemicals and non-condensable high calorific value gas products, is one of the most promising biomass utilization technologies. However, due to the influence of various factors such as the overlapping pyrolysis temperature of the components and the difference in reaction conditions, the products from direct pyrolysis have the defects of complex composition, low selectivity of valuable compounds, and poor stability, which make them unable to be directly utilized. Although certain kinds of high value-added compounds can be enriched by catalytic reforming volatiles by selecting suitable catalysts, most of the researches on this catalytic reforming focus on a single target product, and there are few reports on the co-production of multiple target products. This way of consuming the catalyst not only requires a large investment, but also causes the waste of the high value-added component resources of the bio-oil itself. Therefore, suitable pretreatment methods or the combination of different techniques to enrich high value-added compounds are necessary.

Considering the differences in decomposition temperatures and chemical structures of each component, in order to achieve efficient conversion of different biomass components, this thesis innovatively proposes the staged pyrolytic conversion strategy to obtain multi-target products. The brief summary of each chapter of this thesis is as follows:

Chapter 1 presents the background, motivation, objective and outline of this work.
Chapter 2 explores the chemical and thermal characteristics of torrefaction and in-situ pyrolytic reforming of the volatiles through torrefaction-in situ pyrolytic reforming. Also, in order to explore the influence of alkali and alkaline earth metallic species, the effects of water washing on the above described characteristics of the torrefaction and pyrolytic reforming is also reported. The results showed that torrefaction and in-situ pyrolytic reforming both successfully can conserve the chemical energy of biomass with relatively small heat requirements. in-situ pyrolytic reforming can convert the chemical energy of bio-oil to that of CO/H2-rich syngas with higher LHV of 17–18 MJ/Nm3 -dry, which was represented by those of CO and CH4, C2H4, and H2. The pyrolytic reforming can convert at most 90 wt% of the bio-oil from the torrefaction at 300 °C into gas, while selective removal of the heavier components was difficult only by the vapor-phase reforming.

Chapter 3 innovatively proposes and discusses in detail the staged pyrolysis of acid-loaded biomass for the co-production of chemicals and metallurgical coke. Wood biomass loaded with H2SO4 or H3PO4 was selected to produce levoglucosan and levoglucosenone during torrefaction. The obtained char after water washing was further pelletized and then carbonized to produce the coke. The product distribution of pellet carbonization was also analyzed. The results shows that loading acids, especially H2SO4, that are equal to or slightly less than the metals inherent in the biomass can produce more sugars at lower temperatures torrefaction. The maximum total yield of anhydrosugars from wood reached 12.1 wt% and 10.3 wt% after loading with suitable H2SO4 and H3PO4, respectively. The resulting char can be further prepared into high-strength metallurgical coke. In comparison with the direct carbonization of cedar, the staged conversion promoted strength enhancement of metallurgical coke. More importantly, unlike H3PO4 loading which increased the coke yield, H2SO4 loading further promoted the improvement of coke strength. The resulting coke had a much higher strength (24.2 MPa) than that of coke prepared directly from cedar (9.0 MPa). At the same time, the staged pyrolysis also promoted the formation of phenols because the obtained char was rich in lignin, although the yield was slightly low. Most notably was that the staged conversion loading of H2SO4 and H3PO4 achieved the valorization of cedar in total yields of 45.7 and 49.2 wt% for anhydrosugars, phenols, gas, and strong coke, respectively.

Chapter 4 develops a staged steam treatment progress to enrich the high value-added chemicals in the extracts such as terpenoids and coniferyl aldehyde. The results showed that the formation of coniferyl aldehyde was mainly produced from the binding sites of lignin and hemicellulose, not lignin. Steam treatment can promote the production of coniferyl aldehyde, especially at higher water-to-biomass ratio. The staged steam treatment can further improve the selectivity of coniferyl aldehyde in the extracts at 220 °C, and directly extract the natural component terpenoids below 160 °C.

Chapter 5 summarizes the findings described in previous chapters.

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参考文献

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