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  • 1.
    Bach Oller, Albert
    Luleå University of Technology, Department of Engineering Sciences and Mathematics.
    Co-gasification of black liquor and pyrolysis oil: Fuel conversion and activity of alkali compounds2016Licentiate thesis, comprehensive summary (Other academic)
    Abstract [en]

    Gasification using entrained flow reactors generates syngas that can be upgraded tochemicals with little gas cleaning. Black liquor (BL) is a by-product from pulping industrythat consists of residual wood constituents and spent pulping chemicals. Currently, it iscombusted to recycle the pulping chemicals and at the same time generate steam and power.Alternatively, BL is one of the most attractive fuels for entrained flow gasification due to thecatalytic activity of alkali compounds inherent in BL, possibility for pressurized feeding andthe shared logistics with the pulping plant. However, the high content of ash in BL is also anenergy penalty. Therefore the efficiency of BL gasification can be improved by co-gasifyingit with more energy rich fuels.The current work investigates the gasification characteristics of BL and pyrolysis oil(PO) blends by means of laboratory experiments. Experiments with varying BL/PO blendingratios were conducted using three different devices. An isothermal thermogravimetric reactorwas used to measure the reactivity of char under varying temperature and gas compositions. Asingle particle reactor was used to investigate the conversion of single droplets when exposedto high temperature reactive gas flow using lean, stoichiometric and rich CH4-air flames.Finally, a drop tube furnace was used to study the effect of temperature, gas composition andparticle size on gas, tar, and gasification residues at high temperature (800-1400 °C).Char reactivity of mixture samples was more than 30 times that of PO and comparableto that of pure BL, thereby indicating that catalytic activity was still very high after theaddition of PO. High temperatures enhanced alkali release in the gas phase; however, theconcentration of alkali left in the particles remained high at any temperature and for anymixing ratio. Additionally the blends showed better carbon conversion than pure BL. Theconversion rate of large particles (500-630μm) was controlled by mass diffusion and completecarbon conversion was never reached even at T =1400 °C. In comparison with pine-wood thatwas used as a reference, BL-based samples showed much lower tar concentrations in thesyngas. The difference was attributed to alkali elements. Remarkably, the addition of PO toBL further promoted tar reforming in the presence of CO2. The addition of PO alsosignificantly increased the yields of CH4 and CO.

  • 2.
    Bach Oller, Albert
    et al.
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science.
    Kirtania, Kawnish
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science.
    Furusjö, Erik
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science.
    Umeki, Kentaro
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science.
    Co-gasification of black liquor and pyrolysis oil at high temperature: Part 1. Fate of alkali elements2017In: Fuel, ISSN 0016-2361, E-ISSN 1873-7153, Vol. 202, p. 46-55Article in journal (Refereed)
    Abstract [en]

    The catalytic activity of alkali compounds in black liquor (BL) enables gasification at low temperatures with high carbon conversion and low tar and soot formation. The efficiency and flexibility of the BL gasification process may be improved by mixing BL with fuels with higher energy content such as pyrolysis oil (PO). The fate of alkali elements in blends of BL and PO was investigated, paying special attention to the amount of alkali remaining in the particles after experiments at high temperatures. Experiments were conducted in a drop tube furnace under different environments (5% and 0% vol. CO2 balanced with N2), varying temperature (800–1400 °C), particle size (90–200 µm, 500–630 µm) and blending ratio (0%, 20% and 40% of pyrolysis oil in black liquor). Thermodynamic analysis of the experimental cases was also performed.

    The thermodynamic results qualitatively agreed with experimental measurements but in absolute values equilibrium under predicted alkali release. Alkali release to the gas phase was more severe under inert conditions than in the presence of CO2, but also in 5% CO2 most of the alkali was found in the gas phase at T = 1200 °C and above. However, the concentration of alkali in the gasification residue remained above 30% wt. and was insensitive to temperature variations and the amount of PO in the blend. Thermodynamic analysis and experimental mass balances indicated that elemental alkali strongly interacted with the reactor’s walls (Al2O3) by forming alkali aluminates. The experience indicated that adding PO into BL does not lead to alkali depletion during high temperature gasification.

  • 3.
    Bach Oller, Albert
    et al.
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science.
    Kirtania, Kawnish
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science.
    Furusjö, Erik
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science.
    Umeki, Kentaro
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science.
    Co-gasification of black liquor and pyrolysis oil at high temperature: Part 2. Fuel conversion2017In: Fuel, ISSN 0016-2361, E-ISSN 1873-7153, Vol. 197, p. 240-247Article in journal (Refereed)
    Abstract [en]

    The efficiency and flexibility of the BL gasification process may improve by mixing BL with more energy-rich fuels such as pyrolysis oil (PO). To improve understanding of the fuel conversion process, blends of BL and PO were studied in an atmospheric drop tube furnace. Experiments were performed in varying atmosphere (5% and 0% CO2, balanced by N2), temperature (800–1400 °C), particle size (90–200 μm and 500–630 μm) and blending ratio (0%, 20% and 40% of PO in BL on weight basis). Additionally, pine wood was used as a reference fuel containing little alkali. The addition of PO to BL significantly increased the combined yield of CO and H2 and that of CH4. BL/based fuels showed much lower concentration of tar in syngas than pine wood. Remarkably, the addition of PO in BL further promoted tar reforming in presence of CO2. Unconverted carbon in the gasification residue decreased with increasing fractions of PO. Small fuel particles showed complete conversion at 1000 °C but larger particles did not reach complete conversion even at T = 1400 °C.

  • 4.
    Bach-Oller, Albert
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science.
    Alkali-enhanced gasification of biomass: laboratory-scale experimental studies2018Doctoral thesis, comprehensive summary (Other academic)
    Abstract [en]

    Gasification seeks to break carbonaceous materials into synthetic gas (CO+H2) which can be subsequently upgraded into valuable products. Thus gasification can be utilized to convert low grade biomass stocks into carbon-neutral chemicals heat and power. Nonetheless, gasification produces tar and soot as a by-product, impurities which deposit on cold surfaces thereby risking operation downstream of the gasifier. Cleaning the syngas after the gasifier is a conventional way to attenuate the problem, yet a complex and expensive one. Thus, tar and soot should preferably be addressed already in the gasifier. Given that these impurities are non-equilibrium species they could be targeted by using some sort of catalytic material. Alkali elements have precisely shown to possess catalytic activity on char gasification, besides they have also been associated with a decrease in tar and soot. Yet, to design a functional alkali-catalysed gasification process we need to investigate in more detail on what exact products does alkali show an activity on, on what stage, under what circumstances and, on the measure that it is possible, the mechanism. This was investigated on the basis of experimental work that approached the topic from two opposite sides. On the one hand, we studied the effects of diluting the alkali content of a Na-rich black liquor (BL) by blending it with pyrolysis oil (PO), and on the other hand, we investigated adding various amounts of alkali on more conventional types of biomass fuels. Most of the experiments were conducted on a laminar drop tube furnace but the reactivity of BL chars was also studied through thermogravimetric analysis.

    Alkali was found to catalyse heterogeneous gasification reactions (e.g. char) and to lead to much lower yields of C2 hydrocarbons, heavy tars and soot, favouring the presence of lighter species over large aromatic clusters. Alkali was hypothesized to reduce the quantity of soot by inhibiting the formation and growth of PAH, key intermediates on the road to soot. Besides, it was found that the initial contact between the alkali and the organic matrix was not critical, neither for gas impurities nor regarding char conversion, suggesting that the activity of alkali was a gas-induced phenomenon. The latter implied the existence of a vaporization-condensation cycle that could supply alkali into the char. Nonetheless, the beneficial effects by alkali were impaired by the affinity of Si to capture K and form potassium silicates which are inert. This interaction effect was particularly noticeable on char conversion as the silicates are not only inert but also liquid and viscous and prompt to encapsulate the char particles, thereby limiting mass transfer.

    The experiments with blends of BL and PO showed that the concentration of alkali in BL could be decreased by 30% without any sign of a decrease in the catalytic activity on char gasification, thus indicating the existence a saturation threshold. Furthermore, adding PO into BL lead to a further reduction on the quantities of tar and soot, this finding was attributed to changes in the fuel composition unrelated to alkali. In any case the experiments with BL-based fuels showed lower amounts of tar and soot than those from alkali-impregnated biomass powder. The difference was partially attributed to the content of S in BL. The subsequent investigation targeting the role of S confirmed that S possessed a soot inhibiting role similar to that of alkali, yet unlike K, it did not show a catalytic effect on char gasification.

     

  • 5.
    Bach-Oller, Albert
    et al.
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science.
    Fursujo, Erik
    RISE Bioeconomy, Drottning Kristinas väg 61, Stockholm, Sweden.
    Umeki, Kentaro
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science.
    Effect of potassium impregnation on the emission of tar and soot from biomass gasification2019In: Energy Procedia, ISSN 1876-6102, E-ISSN 1876-6102, Vol. 158, p. 619-624Article in journal (Refereed)
    Abstract [en]

    Entrained flow gasification of biomass has the potential to generate synthesis gas as a source of renewable chemicals, electricity, and heat. Nonetheless, formation of tar and soot is a major challenge for continuous operation due to the problems they cause at downstream of the gasifier. Our previous studies showed the addition of alkali in the fuel can bring significant suppression of such undesirable products.

    The present work investigated, in a drop tube furnace, the effect of potassium on tar and soot formation (as well as on its intermediates) for three different types of fuels: an ash lean stemwood, a calcium rich bark and a silicon rich straw. The study focused on an optimal method for impregnating the biomass with potassium. Experiments were conducted for different impregnation methods; wet impregnation, spray impregnation, and solid mixing to investigate different levels of contact between the fuel and the potassium.

    Potassium was shown to catalyze both homogenous and heterogeneous reactions. Wet and spray impregnation had similar effects on heterogeneous reactions (in char conversion) indicating that there was an efficient molecular contact between the potassium and the organic matrix even if potassium was in the form of precipitated salts at a micrometer scale. On the other hand, potassium in the gas phase led to much lower yields of C2 hydrocarbons, heavy tars and soot. These results revealed that potassium shifted the pathways related to tar and soot formation, reducing the likelihood of carbon to end up as soot and heavy tars by favouring the formation of lighter compounds such as benzene. A moderate interaction between the added potassium and the inherent ash forming elements were also observed: Potassium had a smaller effect when the fuel was naturally rich in silicon.

    The combined results open the door to a gasification process that incorporates recirculation of naturally occurring potassium to improve entrained flow gasification of biomass.

  • 6.
    Bach-Oller, Albert
    et al.
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science.
    Furusjö, Erik
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science. RISE Bioeconomy, Stockholm, Sweden.
    Umeki, Kentaro
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science.
    On the role of potassium as a tar and soot inhibitor in biomass gasification2019In: Applied Energy, ISSN 0306-2619, E-ISSN 1872-9118, Vol. 254, article id 113488Article in journal (Refereed)
    Abstract [en]

    The work investigates in a drop tube furnace the effect of potassium on carbon conversion for three different types of fuels: an ash lean stemwood, a calcium-rich bark and a silicon-rich straw. The study focuses on an optimal method for impregnating the biomass with potassium. The experiments are conducted for 3 different impregnation methods; wet impregnation, spray impregnation, and dry mixing to investigate different levels of contact between the fuel and the potassium. Potassium is found to catalyse both homogenous and heterogeneous reactions. All the impregnation methods showed a significant effect of potassium on heterogeneous reactions (char conversion). The fact that dry mixing of potassium in the biomass shows an effect reveals the existence of a gas-induced mechanism that supply and distributes potassium on the char particles. Concerning the effect of potassium on homogenous reactions, it is found that potassium in the gas phase leads to much lower yields of C2 hydrocarbons, heavy tars and soot. The results indicate that potassium reduces the likelihood of light aromatic to progress toward heavier polyaromatic hydrocarbons clusters, thereby inhibiting the formation of soot-like material. A moderate interaction between the added potassium and the inherent ash forming elements is also observed: Potassium has a smaller effect when the fuel is naturally rich in silicon. The combined results are of interest for the design of a gasification process that incorporates recirculation of naturally occurring potassium to improve entrained flow gasification of biomass.

  • 7.
    Bach-Oller, Albert
    et al.
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science.
    Furusjö, Erik
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science. RISE Bioeconomy,.
    Umeki, Kentaro
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science.
    Reduction of tar and soot in biomass gasification with potassium: Effect of impregnation method and inherent inorganic speciesManuscript (preprint) (Other academic)
  • 8.
    Furusjö, Erik
    et al.
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science.
    Kirtania, Kawnish
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science.
    Jafri, Yawer
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science.
    Oller, Albert Bach
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science.
    Umeki, Kentaro
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science.
    Lundgren, Joakim
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science.
    Wetterlund, Elisabeth
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science.
    Landälv, Ingvar
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science.
    Gebart, Rikard
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science.
    Pettersson, Esbjörn
    SP ETC.
    Co-gasification of pyrolysis oil and black liquor - a new track for production of chemicals and transportation fuels from biomass2015Conference paper (Refereed)
    Abstract [en]

    Pressurized oxygen-blown entrained flow black liquor (BL) gasification, the Chemrec technology, has been demonstrated in a 3 MWth pilot plant in Piteå, Sweden for more than 25,000 h. The plant is owned and operated by Luleå University of Technology since 2013. It is well known that catalytic activity of alkali metals is important for the high reactivity of black liquor, which leads to a highly efficient BL gasification process. The globally available volume of BL is however limited and strongly connected to pulp production. By co-gasifying pyrolysis oil (PO) with BL it is possible to utilize the catalytic activity also for PO conversion to syngas. Adding PO leads to larger feedstock flexibility with the possibility of building larger biofuels plants based on BL gasification technology. This presentation summarizes new results from research activities aimed at developing and assessing the PO/BL co-gasification process. Results from laboratory experiments with PO/BL mixtures show that pyrolysis behavior and char gasification reactivity are similar to pure BL. This means that the decrease in the alkali metal concentration due to the addition of PO in the mixture does not decrease the reactivity. Pure PO is much less reactive. Mixing tests show that the fraction of PO that can be mixed into BL is limited by lignin precipitation as a consequence of PO acidity. Pilot scale PO/BL co-gasification experiments have been executed following design and construction of a new feeding system to allow co-feeding of PO with BL. The results confirm the conclusions from the lab scale study and prove that the co-gasification concept is practically applicable. Process performance of the pilot scale co-gasification process is similar to gasification of BL only with high carbon conversion and clean syngas generation. This indicates that the established BL gasification technology can be used for co-gasification of PO and BL without major modifications.

  • 9.
    Oller, Albert Bach
    et al.
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science.
    Furusjö, Erik
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science.
    Umeki, Kentaro
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science.
    Fuel conversion characteristics of black liquor and pyrolysis oil mixture for efficient gasification with inherent catalyst2014In: European biomass conference and exhibition proceedings, 2014Conference paper (Refereed)
    Abstract [en]

    This paper describes the technical feasibility of a catalytic co-gasification process using a mixture of black liquor (BL) and pyrolysis oil (PO). A technical concern is if gasifiers can be operated at low temperature (~1000 ºC) without problems of tar, soot or char, as is the case for pure BL due to the catalytic effect of fuel alkali. Hence, we investigated fuel conversion characteristics of BL/PO mixture: conversion of single droplet in flame, and char gasification reactivity. 20wt.% (BP20) and 30wt.% (BP30) were selected for weight fraction of PO because of lignin precipitation in BP30. Single droplet was devolatilized and gasified in a methane flame with a flat flame burner at various droplet sizes. Conversion time and swelling ratio were investigated with imaging. They were more sensitive to initial droplet size and reaction atmosphere than the mixing of BL and PO. Char gasification reactivity was measured in an isothermal thermogravimeter (iTG) at T=880–940 ºC and PCO2=1 bar. Both BP20 and BP30 showed complete char conversion and there was no statistically significant difference in char reactivity among BP20, BP30 and BL. These results show that PO can be co-gasified in BL gasification process without major changes in the operation.

  • 10.
    Oller, Albert Bach
    et al.
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science.
    Furusjö, Erik
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science.
    Umeki, Kentaro
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science.
    Fuel conversion characteristics of black liquor and pyrolysis oil mixtures: Efficient gasification with inherent catalyst2015In: Biomass and Bioenergy, ISSN 0961-9534, E-ISSN 1873-2909, Vol. 79, p. 155-165Article in journal (Refereed)
    Abstract [en]

    Alkali metals inherent in black liquor (BL) have strong catalytic activity during gasification. A catalytic co-gasification process based on BL with pyrolysis oil (PO) has the potential to be a part of efficient and fuel-flexible biofuel production systems. The objective of the paper is to investigate how adding PO into BL alters fuel conversion under gasification conditions. First, the conversion times of single fuel droplet were observed in a flat flame burner under different conditions. Fuel conversion times of PO/BL mixtures were significantly lower than PO and comparable to BL. Initial droplet size (300–1500 μm) was the main variable affecting devolatilization, indicating control by external heat transfer. Char oxidation was affected by droplet size and the surrounding gas composition. Then, the intrinsic reactivity of char gasification was measured in an isothermal thermogravimetric analyser at T = 993–1133 K under the flow of CO2–N2 mixtures. All the BL-based samples (100% BL, 20% PO/80% BL, and 30% PO/70% BL on mass basis) showed very high char conversion. Conversion rate of char gasification for PO/BL mixtures was comparable to that of pure BL although the fraction of alkali metal in char decreased because of mixing. The reactivities of BL and BL/PO chars were higher than the literature values for solid biomass and coal chars by several orders of magnitude. The combined results suggest that fuel mixtures containing up to 30% of PO on mass basis may be feasible in existing BL gasification technology.

  • 11.
    Oller, Albert Bach
    et al.
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science.
    Kirtania, Kawnish
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science.
    Furusjö, Erik
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science.
    Umeki, Kentaro
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science.
    Characterization of tar and soot formation for an improved co-gasification of black liquor and pyrolysis oil2015Conference paper (Other (popular science, discussion, etc.))
    Abstract [en]

    Black liquor (BL) gasification is a proven process with very low tar generation at lower temperature than other entrained-flow biomass gasification processes. Recently, BL gasification technology was further expanded to increase feedstock flexibility by co-gasifying pyrolysis oil (PO) with BL. Economic advantage was shown by a techno-economic study. Our previous lab-scale studies using a thermo-gravimetric analyzer and a flat flame burner showed high char reactivity of sample mixture (30wt.% blend of PO into BL) as alkali content in BL kept high catalytic activity despite being diluted by the addition of PO. However, tar and soot formation from this new feedstock remained unknown. In this study, we investigated how the reaction conditions affect the formation of tar and soot to understand their formation mechanism and to suggest suitable operation conditions for the industrial processes. Experiments were carried out with fuel blends containing between 0 and 40wt.% of PO in BL using a laminar entrained flow reactor under the flow of N2/CO2. The effects of operating parameters were evaluated by varying temperature (1073-1673 K), partial pressure of CO2 (0-20 kPa), particle size (90-200 μm and 500-630 μm) and residence time. High temperature (i.e. 1673 K), high heating rate and short residence time experiments were performed to mimic industrial-scale conditions. Soot yield was under detection limit while low amounts of tar (mainly benzene) were formed at low temperature and decreased as the temperature increased. Addition of PO maintained the yields of tar and soot very low while it increased the syngas yield. Overall, this study demonstrated the feasibility of co-gasification of PO and BL and provided valuable information about tar formation under different operating conditions.

  • 12.
    Umeki, Kentaro
    et al.
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science.
    Häggström, Gustav
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science.
    Bach-Oller, Albert
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science.
    Kirtania, Kawnish
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science.
    Furusjö, Erik
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science.
    Reduction of tar and soot formation from entrained-flow gasification of woody biomass by alkali impregnation2017In: Energy & Fuels, ISSN 0887-0624, E-ISSN 1520-5029, Vol. 31, no 5, p. 5104-5110Article in journal (Refereed)
    Abstract [en]

    Tar and soot in product gas have been a major technical challenge toward the large-scale industrial installation of biomass gasification. This study aims at demonstrating that the formation of tar and soot can be reduced simultaneously using the catalytic activity of alkali metal species. Pine sawdust was impregnated with aqueous K2CO3 solution by wet impregnation methods prior to the gasification experiments. Raw and alkali-impregnated sawdust were gasified in a laminar drop-tube furnace at 900–1400 °C in a N2–CO2 mixture, because that creates conditions representative for an entrained-flow gasification process. At 900–1100 °C, char, soot and tar decreased with the temperature rise for both raw and alkali-impregnated sawdust. The change in tar and soot yields indicated that potassium inhibited the growth of polycyclic aromatic hydrocarbons and promoted the decomposition of light tar (with 1–2 aromatic rings). The results also indicated that the catalytic activity of potassium on tar decomposition exists in both solid and gas phases. Because alkali salts can be recovered from product gas as an aqueous solution, alkali-catalyzed gasification of woody biomass can be a promising process to produce clean product gas from the entrained-flow gasification process at a relatively low temperature.

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