WO2023208307A1 - Procédés de production combinée de combustibles gazeux et liquides - Google Patents

Procédés de production combinée de combustibles gazeux et liquides Download PDF

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WO2023208307A1
WO2023208307A1 PCT/DK2023/050106 DK2023050106W WO2023208307A1 WO 2023208307 A1 WO2023208307 A1 WO 2023208307A1 DK 2023050106 W DK2023050106 W DK 2023050106W WO 2023208307 A1 WO2023208307 A1 WO 2023208307A1
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feed mixture
temperature
range
thermo
digestate
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PCT/DK2023/050106
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English (en)
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Lina Johanna Nåbo ANDERSEN
Martin Dan JEPPESEN
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Nature Energy Green Hydrogen A/S
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Publication of WO2023208307A1 publication Critical patent/WO2023208307A1/fr

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    • C—CHEMISTRY; METALLURGY
    • C12—BIOCHEMISTRY; BEER; SPIRITS; WINE; VINEGAR; MICROBIOLOGY; ENZYMOLOGY; MUTATION OR GENETIC ENGINEERING
    • C12P—FERMENTATION OR ENZYME-USING PROCESSES TO SYNTHESISE A DESIRED CHEMICAL COMPOUND OR COMPOSITION OR TO SEPARATE OPTICAL ISOMERS FROM A RACEMIC MIXTURE
    • C12P5/00—Preparation of hydrocarbons or halogenated hydrocarbons
    • C12P5/02—Preparation of hydrocarbons or halogenated hydrocarbons acyclic
    • C12P5/023—Methane
    • C—CHEMISTRY; METALLURGY
    • C12—BIOCHEMISTRY; BEER; SPIRITS; WINE; VINEGAR; MICROBIOLOGY; ENZYMOLOGY; MUTATION OR GENETIC ENGINEERING
    • C12M—APPARATUS FOR ENZYMOLOGY OR MICROBIOLOGY; APPARATUS FOR CULTURING MICROORGANISMS FOR PRODUCING BIOMASS, FOR GROWING CELLS OR FOR OBTAINING FERMENTATION OR METABOLIC PRODUCTS, i.e. BIOREACTORS OR FERMENTERS
    • C12M21/00—Bioreactors or fermenters specially adapted for specific uses
    • C12M21/04—Bioreactors or fermenters specially adapted for specific uses for producing gas, e.g. biogas
    • C—CHEMISTRY; METALLURGY
    • C12—BIOCHEMISTRY; BEER; SPIRITS; WINE; VINEGAR; MICROBIOLOGY; ENZYMOLOGY; MUTATION OR GENETIC ENGINEERING
    • C12M—APPARATUS FOR ENZYMOLOGY OR MICROBIOLOGY; APPARATUS FOR CULTURING MICROORGANISMS FOR PRODUCING BIOMASS, FOR GROWING CELLS OR FOR OBTAINING FERMENTATION OR METABOLIC PRODUCTS, i.e. BIOREACTORS OR FERMENTERS
    • C12M23/00—Constructional details, e.g. recesses, hinges
    • C12M23/58—Reaction vessels connected in series or in parallel
    • C—CHEMISTRY; METALLURGY
    • C12—BIOCHEMISTRY; BEER; SPIRITS; WINE; VINEGAR; MICROBIOLOGY; ENZYMOLOGY; MUTATION OR GENETIC ENGINEERING
    • C12P—FERMENTATION OR ENZYME-USING PROCESSES TO SYNTHESISE A DESIRED CHEMICAL COMPOUND OR COMPOSITION OR TO SEPARATE OPTICAL ISOMERS FROM A RACEMIC MIXTURE
    • C12P7/00—Preparation of oxygen-containing organic compounds
    • C12P7/64—Fats; Fatty oils; Ester-type waxes; Higher fatty acids, i.e. having at least seven carbon atoms in an unbroken chain bound to a carboxyl group; Oxidised oils or fats
    • C12P7/6436—Fatty acid esters
    • C—CHEMISTRY; METALLURGY
    • C12—BIOCHEMISTRY; BEER; SPIRITS; WINE; VINEGAR; MICROBIOLOGY; ENZYMOLOGY; MUTATION OR GENETIC ENGINEERING
    • C12P—FERMENTATION OR ENZYME-USING PROCESSES TO SYNTHESISE A DESIRED CHEMICAL COMPOUND OR COMPOSITION OR TO SEPARATE OPTICAL ISOMERS FROM A RACEMIC MIXTURE
    • C12P2201/00—Pretreatment of cellulosic or lignocellulosic material for subsequent enzymatic treatment or hydrolysis
    • C—CHEMISTRY; METALLURGY
    • C12—BIOCHEMISTRY; BEER; SPIRITS; WINE; VINEGAR; MICROBIOLOGY; ENZYMOLOGY; MUTATION OR GENETIC ENGINEERING
    • C12P—FERMENTATION OR ENZYME-USING PROCESSES TO SYNTHESISE A DESIRED CHEMICAL COMPOUND OR COMPOSITION OR TO SEPARATE OPTICAL ISOMERS FROM A RACEMIC MIXTURE
    • C12P2203/00—Fermentation products obtained from optionally pretreated or hydrolyzed cellulosic or lignocellulosic material as the carbon source

Definitions

  • the present invention relates to the area of biogas production using an anaerobic digester and more specifically handling of feedstock for the anaerobic digester to increase the biogas production.
  • Anaerobic digesters have been known for numerous years and the technology is constantly undergoing development in order to improve the production of the biogas. In the present transition towards a more sustainable energy supply to society the need for as well as the desire for the improvement of the technology has significantly increased.
  • As the anaerobic digester due to their inherent limitation in converting certain parts of a typical biomass feedstock, there is a need for moving the present limits to enhance the capabilities of the anaerobic digestion process.
  • the object of the present invention is therefore to provide for an improved method for production of biogas that will enhance the yields of biogas obtained, increase the speed of biogas production or both objectives at the same time.
  • the invention relates to a method for producing gaseous and liquid fuels, the method comprising: a. providing a feedstock, b. adding the feedstock to an anaerobic digester for producing a biogas and a digestate as a residual product, c. dewatering the digestate to a predetermined level, d.
  • thermo-chemical process for producing a biooil
  • upgrading at least partly the carbon dioxide in said biogas to methane in a biomethanation reactor may be that the combined anaerobic digestion process and thermo-chemical process will significantly increase the ability to take in abundant lignin-containing feedstock.
  • thermo-chemical process a combined increase of fuels in the form of biogas and biooil may be obtained.
  • the much more efficient utilization of the feedstock for fuel production may allow of a less intensive processing in the anaerobic digester due to the remaining energy potential of the feedstock being utilized for production of biooil.
  • a further advantage of the invention may be that a nutrient rich product, which is substantially free of pathogens, may be obtained from the process. By applying a combination of anaerobic digestion with application of thermo-chemical processing of the digestate a resulting nutrient rich product may be obtained that is substantially free of pathogens.
  • a further advantage of the invention may be that the nutrient rich product is substantially free of microplastics. By applying a combination of anaerobic digestion with application of thermo-chemical processing of the digestate a resulting nutrient rich product may be obtained that is substantially free of microplastics.
  • a further advantage of the invention may be that the nutrient rich product is substantially free of pharmaceutical traces.
  • thermo-chemical process may decrease the retention time of the feedstock in the anaerobic digestion. It should be understood within the present context that dewatering the digestate to a predetermined level results in a digestate with an increased dry matter content. The digestate with increased dry matter content may also be referred to as a concentrated digestate. In the present context it should be understood that the thermo-chemical process may also be referred to as a thermo-chemical step, a thermo reductive step, or a thermo reductive process.
  • the desired level of dewatering of the digestate correspond to a dry matter content of at least 15% by weight of the digestate, such as at least 20% by weight of the digestate, such as at least 30% by weight of the digestate, such as at least 40% by weight of the digestate.
  • the method comprises a pretreatment of the feedstock before the adding of the feedstock to the anaerobic digester.
  • the thermo-chemical step comprises a pyrolysis process, such as a slow pyrolysis process or a catalytic pyrolysis process.
  • the concentrated digestate is further dried to a dry matter content of at least 85 % by weight such as at least 90 % by weight prior to entering the pyrolysis process.
  • the heat required for drying the digestate is at least partly supplied by heat recovered from the pyrolysis process.
  • the process further comprises a step of drying the digestate using heat that is at least partly supplied by heat recovered from the pyrolysis process.
  • the drying step may also be referred to as the drying process.
  • evaporated moisture in the drying process is condensed, and wherein the recovered latent heat is used to heat the incoming feedstock to the anaerobic digestor.
  • the thermo-chemical step comprises a hydrothermal liquefaction process.
  • hydrothermal liquefaction may also be referred to as HTL.
  • the thermo-chemical step comprises a hydrothermal liquefaction process characterized by f. preparing a pumpable feed mixture from the concentrated digestate; g. pressurizing the feed mixture; h. heating the feed mixture to a conversion temperature thereby producing a converted feed mixture; i. cooling the converted feed mixture; j. depressurizing the converted feed mixture; k. separating the converted feed mixture into an oil phase, a gas phase, and aqueous phase, and a solid phase.
  • the step of pressurizing the feed mixture comprises pressurizing the feed mixture to a pressure in the range 100 to 400 bar.
  • the conversion temperature is in the range 250 to 410 °C.
  • the step of cooling the converted feed mixture comprises cooling the converted feed mixture to a temperature in the range 50 to 250 °C.
  • the step of depressurizing the converted feed mixture comprises depressurizing the converted feed mixture to a pressure in the range 1 to 70 bar.
  • the method comprises heating and converting the feed mixture at a temperature up to 410°C , such as up to 400 °C such as heating and converting the feed mixture at a temperature of up to 390 °C; preferably heating and converting the feed mixture at a temperature of up to 380 °C such as heating and converting the feed mixture at a temperature of up to 374 °C.
  • the hydrothermal liquefaction process comprises heating and converting the feed mixture to a temperature of above 250°C, such as above 280°C such as heating and converting the feed mixture at a temperature of above to 300 °C; preferably heating and converting the feed mixture at a temperature of above to 330 °C such as heating and converting the feed mixture at a temperature above 350 °C.
  • the hydrothermal liquefaction process comprises heating and converting the feed mixture to a temperature of 250 to 400°C, such as 280 to 400°C, such as 300 to 390°C, such as 330 to 380°C, such as 350 to 374°C.
  • the pumpable feed mixture is preheated to at least 80 °C prior to entering the pressurization step such as preheating the feed mixture to at least 100 °C prior to entering the preheating step; preferably the feed mixture is preheated to a temperature of at least 120 °C such as a temperature of at least 150 °C prior to entering the pressurization step; even more preferably the feed mixture is heated to at least 170 °C such as at least 200 °C prior to entering the pressurization step.
  • the pumpable feed mixture may be preheated to a temperature of 80 to 240°C prior to entering the pressurization step, such as 100 to 235°C, such as 120 to 230 °C, such as 150 to 225°C, such as 170 to 220°C, such as 200 to 220°C.
  • the method further includes that the feed mixture is pre-pressurized to a pressure of up to 50 bars prior to the preheating step such as a pre-pressurization of the feed mixture of up to 40 bars prior to the preheating step; preferably the feed mixture is pre-pressurized to a pressure of up to 30 bars prior to the preheating step such as pre-pressurizing the feed mixture to a pressure of up to 20 bars prior to the preheating step.
  • the method further includes that the feed mixture is pre-pressurized to a pressure of 2 to 50 bars prior to the preheating step, such as 3 to 40 bars, such as 5 to 30 bars, such as 10 to 20 bars.
  • the feed mixture is pressurized to at least 50 bars in the pressurization step prior to heating the feed mixture to the conversion temperature in the heating step (h) such as pressurizing the feed mixture to a pressure of at least 80 bars in the pressurization step; preferable the feed mixture is pressurized to a pressure of at least 150 bars prior to heating the feed mixture to the conversion temperature such as a pressurizing the feed mixture to a pressure of at least 180 bars prior to heating the feed mixture to the conversion temperature.
  • the feed mixture is pressurized to a pressure of 50 to 400 bars in the pressurization step prior to heating the feed mixture to the conversion temperature in the heating step (h), such as 80 to 380 bars, such as 150 to 350 bars such as 180 to 300 bars.
  • the thermo-chemical step comprises a hydrothermal liquefaction process characterized by f. preparing a pumpable feed mixture from the concentrated digestate; g. pressurizing the feed mixture to a pressure in the range 100 to 400 bar; h. heating the feed mixture to a conversion temperature in the range 250 to 410 °C thereby producing a converted feed mixture; i. cooling the converted feed mixture to a temperature in the range 50 to 250 °C; j.
  • the density of the feed mixture during the conversion at the conversion temperature is maintained in the range 100 to 800 kg/m 3 such as in the range 300 to 700 kg/m 3 ; preferably the density of the feed mixture at the conversion temperature is maintained in the range 350 to 650 kg/m 3 such as in the range 400 to 600 kg/m 3 .
  • pH of the conversion process is maintained so that the pH value of the aqueous phase separated from the converted feed mixture is alkaline.
  • the alkaline pH value may be at least 7.5, such as at least 8.0, such as at least 8.5.
  • the pH of the conversion process is controlled so that the pH value of the aqueous phase separated from the converted feed mixture is alkaline.
  • the alkaline pH value may be at least 7.5, such as at least 8.0, such as at least 8.5.
  • the temperature of biomethanation reactor is in the range 10 to 70 °C, such as a temperature in the range 25 to 65 °C, such as in the range 35 to 65 °C, such as in the range 50 to 60 °C.
  • the gas (CO 2) from the thermo-chemical process is processed in a biomethanation reactor and converted into methane.
  • the gas from the thermo-chemical process is processed by biomethanation.
  • this increases the total yield of methane.
  • CO2 gas from the thermo-chemical process it may preferably be in the form of a CO2-containing gas from the thermo-chemical process, e.g. as a raw CO2-containing gas from the thermo- chemical process or as a processed CO2-containing gas from the thermo-chemical process.
  • the gas (CO 2 ) from the thermo-chemical process is processed in the biomethanation reactor and converted into methane.
  • the gas (CO 2 ) from the thermo-chemical process is processed in the biomethanation reactor and converted into methane, thus increasing the methane yield of the total process.
  • the biomethanation of the gas (CO 2 ) from the thermo-chemical process is controlled between a state of joint biomethanation with the carbon dioxide of said biogas and separate biomethanation from the carbon dioxide of said biogas.
  • the gas (CO 2 ) from the thermo-chemical process is processed separately from the carbon dioxide of said biogas.
  • the gas (CO 2 ) from the thermo-chemical process is processed together with the carbon dioxide of said biogas.
  • the gas (CO 2 ) from the thermo-chemical process is added to the carbon dioxide of said biogas prior to biomethanation.
  • the gas from the thermo- chemical process subjected to a gas cleaning process prior to adding to the carbon dioxide of said biogas.
  • the retention time of the feedstock in the anaerobic digester is less than 100 days, such as less than 80 days, such as less than 60 days, such as less than 40 days, such as less than 30 days, such as less than 25 days, such as less than 20 days, such as less than 15 days.
  • the retention time of the feedstock in the anaerobic digester is at least 12 hours, such as at least 1 day, such as at least 5 days, such as at least 10 days.
  • the retention time in the anaerobic digestion step is 12 hours to 100 days, such as 12 hours to 80 days, such as 1 to 60 days, such as 5 to 40 days, such as 10 to 40 days.
  • the retention time of the feedstock in the anaerobic digester is 12 hours to 40 days, such as 12 hours to 30 days, such as 1 to 25 days, such as 5 to 20 days, such as 10 to 15 days.
  • the anaerobic digester is configured for performing continuous anaerobic digestion process.
  • the anaerobic digester is configured for performing a batch process.
  • the temperature of the anaerobic digester is 45 to 70 °C, such as 48 to 60 °C, such as 45 to 70 °C, such as 49 to 59 °C, such as 50 to 55 °C.
  • the pH value of the anaerobic digester is 6.0 to 9.0, such as 6.0 to 8.5, such as 6.5 to 8.5, such as 7.0 to 8.5.
  • the invention further relates to a system for producing gaseous and liquid fuels according to the method of the invention or any of its embodiments, the system comprising an anaerobic digester, a thermo-chemical reactor, and a biomethanation reactor.
  • the objective of the invention is achieved through a method for producing gaseous and liquid fuels, the method comprising: a. providing a feedstock, b. adding the feedstock to an anaerobic digester for producing a biogas and a digestate as a residual product, c.
  • the method comprises a pretreatment of the feedstock before the adding of the feedstock to the anaerobic digester.
  • the thermo reductive step may comprise a pyrolysis process such as a slow pyrolysis process or a catalytic pyrolysis process.
  • the concentrated digestate is further dried to a dry matter content of at least 85 % by weight such as at least 90 % by weight prior to entering the pyrolysis process.
  • the heat required for drying the digestate is at least partly supplied by heat recovered from the pyrolysis process.
  • evaporated moisture in the drying process is condensed, and wherein the recovered latent heat is used to heat the incoming feedstock to the anaerobic digestor.
  • the thermo reductive step comprises a hydrothermal liquefaction process characterized by f. preparing a pumpable feed mixture from the concentrated digestate; g. pressurizing the feed mixture to a pressure in the range 100 to 400 bar; h. heating the feed mixture to a conversion temperature in the range 250 to 410 °C thereby producing a converted feed mixture; i. cooling the converted feed mixture to a temperature in the range 50 to 250 °C; j.
  • the method comprises heating and converting the feed mixture at a temperature up to 400 °C such as heating and converting the feed mixture at a temperature of up to 390 °C; preferably heating and converting the feed mixture at a temperature of up to 380 °C such as heating and converting the feed mixture at a temperature of up to 374 °C.
  • the hydrothermal liquefaction process may comprise heating and converting the feed mixture to a temperature of above 280°C such as heating and converting the feed mixture at a temperature of above to 300 °C; preferably heating and converting the feed mixture at a temperature of above to 330 °C such as heating and converting the feed mixture at a temperature above 350 °C.
  • the pumpable feed mixture may be preheated to at least 80 °C prior to entering the pressurization step such as preheating the feed mixture to at least 100 °C prior to entering the preheating step; preferably the feed mixture is preheated to a temperature of at least 120 °C such as a temperature of at least 150 °C prior to entering the pressurization step; even more preferably the feed mixture is heated to at least 170 °C such as at least 200 °C prior to entering the pressurization step.
  • the method further includes that the feed mixture is pre-pressurized to a pressure of up to 50 bars prior to the preheating step such as a pre-pressurization of the feed mixture of up to 40 bars prior to the preheating step; preferably the feed mixture is pre-pressurized to a pressure of up to 30 bars prior to the preheating step such as pre-pressurizing the feed mixture to a pressure of up to 20 bars prior to the preheating step.
  • the feed mixture is pressurized to at least 50 bars in the pressurization step prior to heating the feed mixture to the conversion temperature in the heating step (h) such as pressurizing the feed mixture to a pressure of at least 80 bars in the pressurization step; preferable the feed mixture is pressurized to a pressure of at least 150 bars prior to heating the feed mixture to the conversion temperature such as a pressurizing the feed mixture to a pressure of at least 180 bars prior to heating the feed mixture to the conversion temperature.
  • the density of the feed mixture during the conversion at the conversion temperature is maintained in the range 100 to 800 kg/m 3 such as in the range 300 to 700 kg/m 3 ; preferably the density of the feed mixture at the conversion temperature is maintained in the range 350 to 650 kg/m 3 such as in the range 400 to 600 kg/m 3 .
  • pH of the conversion process is maintained so that the pH value of the aqueous phase separated from the converted feed mixture is alkaline.
  • the pH of the conversion process is controlled so that the pH value of the aqueous phase separated from the converted feed mixture is alkaline.
  • FIG. 1 shows a schematic overview of a combined biogas and biooil production facility.
  • FIG.2 shows a schematic overview of a further embodiment of a combined biogas and biooil production facility.
  • FIG.3 shows a schematic overview of a further embodiment of a combined biogas and biooil production facility.
  • FIG. 1 shows an embodiment of a process/method for producing gaseous and liquid fuels and/or other chemicals from organic matter such as biomass and/or waste comprising a.
  • a digestate concentration step concentrating the dry matter content of the digestate thereby producing an aqueous stream and a concentrated digestate stream enriched in dry matter content; d.
  • a thermo-chemical step converting the concentrated digestate stream to liquid fuels/bio-oil and/or other chemicals, where the thermo-chemical step is a hydrothermal liquefaction step or pyrolysis step.
  • An upgrading step for nutrient rich residuals The process may in the thermo-chemical step also comprise producing a nutrient rich product that can be utilized directly or after separation and/or mixing with other materials as a fertilizer product in agriculture.
  • the retention time in the anaerobic digestion step (b) is typically less than 40 days such as less than 30 days; preferably the retention time in the anaerobic digestion step (b) is less than 25 days; even more preferably the retention time in the anaerobic digestion step is less than 20 days such as less than 15 days.
  • the retention time of the anaerobic digestion step (b) is typically at least 12 hours such as a retention time of at least 1 day; preferably the retention time of the anaerobic digestion step is at least 5 days such as at least 10 days.
  • Preferred the anaerobic digestion step comprises a continuous anaerobic digestion process. However, the process may also be a batch process.
  • the anaerobic digestion step (b) comprises a thermophilic digestion step.
  • the temperature of the anaerobic digester is typically in the range 45 to 70 °C such as in the range 48 to 60 °C; preferably the temperature of the anaerobic digester is in the range 45 to 70 °C such as in the range 49 to 59 °C; even more preferably the temperature of the anaerobic digester is in the range 50 to 55 °C.
  • the pH value of the digester is typically in the range 6.0-9.0 such as a pH value in the range 6.0-8.5; preferably the pH value of the digester is in the range 6.5-8.5 such as a pH value in the range 6.5 -8.0.
  • the feedstock to the anaerobic digester typically comprises animal manures including animal beddings such as manure from dairy production such a manure from livestock production, cattle manure, pig manure, horse manure, deep litter or a combination thereof.
  • animal manures including animal beddings such as manure from dairy production such a manure from livestock production, cattle manure, pig manure, horse manure, deep litter or a combination thereof.
  • the feedstock to the anaerobic digester may also comprise food waste such as kitchen waste, restaurant wastes including oil and greases, separated organic fraction from municipal solid waste, industrial food and non-food waste such as slaughterhouse waste, fats, oils and grease from restaurants, organic household waste, glycerine or a combination thereof. These feedstocks may also be used alone.
  • the feedstock may further comprise one or more lignocellulosic feedstock such as agricultural residues like straw, grasses, husks, corn stover, green house waste, bagasse from sugar production, yard waste, woody biomass such as branches, demolition wood etc., seaweed, lake weed, energy crops, rice crop residue.
  • the lignin content of the feedstock to the anaerobic digester is typically in the range 0.1 to 50 % by weight such as a lignin content of 1 to 30 wt % by weight; preferably the lignin content of the feedstock to the anaerobic digester is in the range 5 to 20 % by weight such as a lignin content of 5 to 15 wt % by weight.
  • Lignin is normally not immediately digestible and therefore an indirect measure of feedstock flexibility i.e. feedstock that will normally not be converted and hence result in lower carbon efficiency for the anaerobic digestion process as such.
  • pretreatment may give some improvements in this the digestate typically will have a relatively high content of lignin, obviously dependent on the feedstock.
  • Typical wheat straw has 15-20% lignin content. The combined anaerobic digestion process and thermo-chemical process will significantly increase the ability to take in abundant lignin-containing feedstock.
  • the nitrogen content of the feedstock to the anaerobic digestion step (b) is typically in the range 0.1 to 10 % by weight such as a nitrogen content of the feedstock to the anaerobic digestion step (b) in the range to 1.0 to 5.0 % by weight; preferably the nitrogen content of the feedstock to the anaerobic digestion step (b) is in the range 1 to 3 % by weight.
  • Introduction of the feedstock to the anaerobic digester comprises preparing a pumpable/movable feedstock slurry prior to the anaerobic digestion step (b) wherein the dry matter content the feedstock slurry is of up to 25 % by weight such as up to 20 % by weight; preferably the feedstock slurry is of up to 15 % by weight such as up to 10 % by weight; even more preferably the dry matter content of the slurry is up to 5 % by weight such as up to 2.5 % by weight.
  • the feedstock slurry preparation step may include reducing the particle size of the feedstock to less than 50 mm such a size reduction of the feedstock to a particle size of less than 40 mm; preferably the particle size of the feedstock is reduced to less than 30 mm prior to the anaerobic digestion step (b) such as a particle size of less than 20 mm.
  • the feedstock dry matter content may be controlled by mixing with a recirculated stream of digestate from the anaerobic digestion or adding diluted one or more water streams from the digestate concentration step (c) and/or the thermo-reductive step.
  • the feedstock preparation may further comprise adding bio oil produced in the thermo- reductive step (d) to the slurry in the feedstock slurry preparation step.
  • bio oil produced in the thermo-reductive step (d) may be used to heat the feedstock slurry prior to entering the anaerobic digestion step (b).
  • the methane content in the biogas is at least 50 % by volume such as a methane content of the biogas of at least 60 % by volume; preferably at least the methane content in the biogas is at least 65 % by volume such as at least 70 % by volume.
  • the biogas from the anaerobic digestion stage is further upgraded by contact with hydrogen in a fixed bed biomethanation reactor comprising anaerobic microorganisms.
  • the biogas upgrading in the biomethanation reaction comprises biological conversion of the carbon dioxide (CO 2 ) and hydrogen into methane and water.
  • the biomethanation reactor is filled with granular support structures upon which a biofilm is developed through occasional sprinkling of the biomethanation reactor with liquid digestate comprising hydrogenotrophic methanogens from an anaerobic digester.
  • the hydrogenotrophic methanogens are multiplied as a result of feeding the reactor with CO 2 and hydrogen, rendering a biofilm suited for CO 2 upgrading.
  • the sprinkling of digestate over the biomethanation reactor ensures sufficient buffer capacity in the reactor to control the pH and provides the necessary macro- and micronutrients.
  • the use of digestate microbacterial cultures ensures resistance towards potential inhibitors such as for example hydrogen sulfide.
  • the temperature of the fixed bed bioreactor for biogas upgrading is in the range 10 to 70 °C such as a temperature in the range 25 to 65 °C; preferably the temperature of the fixed bed bioreactor for biogas upgrading is in the range 35 to 65 °C such as a temperature in the range 50 to 60 °C.
  • the hydrogen required for the biogas upgrading step is preferably produced by electrolysis using renewable electricity.
  • the stoichiometric relationship between CO 2 and hydrogen is 1:4 according to the reaction: ⁇ ⁇ ⁇ ⁇ ⁇ ⁇ ⁇ ⁇ ⁇ ⁇ ⁇ ⁇ ⁇ ⁇ ⁇ ⁇ ⁇
  • the CO 2 may preferably be added in small excess to ensure full utilization of the hydrogen.
  • the biogas from the anaerobic digestion step (b) may be heated by heat exchange with a stream from the thermo-chemical step (d).
  • - Pretreatment by leaching Gas production per dry matter content in feedstock averages 254 m3 methane per ton dry matter feedstock, which is a considered a high yield of production again significantly contributing to a circularity.
  • the scale is significant as gas production per day in a modern anaerobic digestion facility is around 20.000.000 m3 methane per year.
  • the anaerobic digestion takes place in three overall stages.
  • the first stage is hydrolysis, where large structures, i.e. polymers (proteins, carbohydrates and fats) are broken down to monomers (amino acids, sugars and fatty acids) by acidogenic hydrolytic bacteria.
  • the second stage is fermentation, where these monomers are degraded further into smaller molecules such as volatile fatty acids by acidogenic fermentative bacteria.
  • the third stage is methanogenesis, where acetogenic bacteria further degrade the molecules to acetate or hydrogen and CO 2 .
  • the acetate can then be converted into methane and CO 2 by aceticlastic methanogenic bacteria and the hydrogenotrophic methanogenic bacteria finally converts the hydrogen and CO 2 into methane and water.
  • the nutrient rich product produced in the thermo-chemical process comprises phosphorous in a concentration of at least 0.1 wt % such as at least 1.0 wt %; preferably in a concentration of at least 2.0 wt %; even more preferably the nutrient rich product comprises phosphorous in a concentration of at least 3.0 wt % such as a phosphorous content of at least 4.0 wt %.
  • the nutrient rich product produced by the process are substantially free of pathogens. By substantially free of pathogens is meant that the content is reduced below detection. Further, and again due to the process conditions in the thermo-chemical process, the nutrient rich product is substantially free of microplastics.
  • substantially free of microplastics is meant that the content is reduced to below 0.006 wt%.
  • the nutrient rich product is substantially free of pharmaceutical traces.
  • substantially free of pharmaceutical traces is meant that the content is reduced to below detection limits.
  • the nutrient rich solid product from the thermo-chemical step may be mixed with a part of the concentrated digestate from the concentration step (c) for use as a fertilizer product.
  • the nutrient rich solid product and/or a solid product from the thermo-chemical step may be dried using heat recovered from the thermo-chemical step. If the thermo-reductive step is a slow pyrolysis, the carbon content in the nutrient rich solid product may be above 50 wt%.
  • thermo-reductive step is fast pyrolysis
  • the carbon content in the nutrient rich solid product may be below 50 wt%.
  • the dry matter content of digestate from the anaerobic digestion step (b) is preferably concentrated to at least 25 % by weight in the digestate concentration step (c) prior to the thermo reductive step (d) such as at least 30 % by weight; preferably the dry matter content of the digestate from the anaerobic digestion step (b) is concentrated to at least 35 % by weight such as at least 40 % by weight prior to the thermo reductive step (d).
  • the digestate concentration step (c) comprises for example use of a filter press and/or a decanter centrifuge and/or a screw press and/or a double screw press.
  • the thermo reductive step (d) may comprise a pyrolysis process such as a slow pyrolysis process or a catalytic pyrolysis process.
  • the concentrated digestate is further dried to a dry matter content of at least 85 % by weight such as at least 90 % by weight prior to entering the pyrolysis process.
  • the heat required for drying the digestate is at least partly supplied by heat recovered from the pyrolysis process, for example the heat may be generated from combustion of the pyrolysis gas and/or oil.
  • the evaporated moisture in the drying process is condensed, and wherein the recovered latent heat is used to heat the incoming feedstock to the anaerobic digestor.
  • Temperature range for slow pyrolysis process above 350 °
  • Products from slow pyrolysis process biochar (around 50% of feedstock C), bio-oil (around 25% of feedstock C), pyrolysis gas (CO, CO2, H2, other; around 25% of feedstock C)
  • Catalytic pyrolysis process will typically be carried out at 450-600 °C, and the residence time will typically be between x and y seconds.
  • the process requires an inert atmosphere (no oxygen), for maximizing bio oil yield.
  • thermo reductive step (d) may comprise a hydrothermal liquefaction process characterized by f. Preparing a pumpable feed mixture from the concentrated digestate; g. pressurizing the feed mixture to a pressure in the range 100 to 400 bar; h. heating the feed mixture to a conversion temperature in the range 250 to 410 °C thereby producing a converted feed mixture; i. cooling the converted feed mixture to a temperature in the range 50 to 250 °C; j. depressurizing the converted feed mixture to a pressure in the range 1 to 70 bar; k. separating the converted feed mixture into an oil phase, a gas phase, and an aqueous phase, and a solid phase.
  • the hydrothermal liquefaction process may comprise heating and converting the feed mixture at a temperature up to 400 °C such as heating and converting the feed mixture at a temperature of up to 390 °C; preferably heating and converting the feed mixture at a temperature of up to 380 °C such as heating and converting the feed mixture at a temperature of up to 374 °C.
  • the hydrothermal liquefaction process may comprise heating and converting the feed mixture to a temperature of above 280°C such as heating and converting the feed mixture at a temperature of above to 300 °C; preferably heating and converting the feed mixture at a temperature of above to 330 °C such as heating and converting the feed mixture at a temperature above 350 °C.
  • the pumpable feed mixture may be preheated to at least 80 °C prior to entering the pressurization step such as preheating the feed mixture to at least 100 °C prior to entering the preheating step; preferably the feed mixture is preheated to a temperature of at least 120 °C such as a temperature of at least 150 °C prior to entering the pressurization step; even more preferably the feed mixture is heated to at least 170 °C, such as at least 200 °C prior to entering the pressurization step.
  • the hydrothermal liquefaction process may include that the feed mixture is pre- pressurized to a pressure of up to 50 bars prior to the preheating step such as a pre- pressurization of the feed mixture of up to 40 bars prior to the preheating step; preferably the feed mixture is pre-pressurized to a pressure of up to 30 bars prior to the preheating step such as pre-pressurizing the feed mixture to a pressure of up to 20 bars prior to the preheating step.
  • the feed mixture is pressurized to at least 50 bars in the pressurization step prior to heating the feed mixture to the conversion temperature in the heating step (h) such as pressurizing the feed mixture to a pressure of at least 80 bars in the pressurization step; preferable the feed mixture is pressurized to a pressure of at least 150 bars prior to heating the feed mixture to the conversion temperature such as a pressurizing the feed mixture to a pressure of at least 180 bar prior to heating the feed mixture to the conversion temperature.
  • the density of the feed mixture during the conversion at the conversion temperature is maintained in the range 100 to 800 kg/m 3 such as in the range 300 to 700 kg/m 3 ; preferably the density of the feed mixture at the conversion temperature is maintained in the range 350 to 650 kg/m 3 such as in the range 400 to 600 kg/m 3 .
  • the pH of the conversion process is maintained so that the pH value of the aqueous phase separated from the converted feed mixture is alkaline.
  • the pH of the conversion process is controlled so that the pH value of the aqueous phase separated from the converted feed mixture is alkaline.
  • the pH of the conversion process is maintained so that the pH value of the aqueous phase separated from the converted feed mixture is above 8 such as a pH value of aqueous phase separated from the converted feed mixture of at least 8.5; preferably the pH value of the aqueous phase separated from the converted feed mixture is in the range 8 to 10 such as a pH of the aqueous phase separated from the converted feed mixture in the range 8.5-9.5.
  • the pH of the aqueous phase separated from the converted feed mixture is controlled by adding a base to the feed mixture in the feed mixture preparation step.
  • the base is selected among potassium carbonate, potassium hydroxide, potassium formate, potassium acetate, sodium carbonate, sodium hydroxide, sodium formate and/or sodium acetate, ammonia or a combination thereof.
  • the control of the pH may at least partly be performed by at least partly recycling the separated aqueous phase from the separation to the feed mixture preparation step.
  • the bio-oil produced is at least partly recycled to the feed mixture preparation step (a).
  • a solid phase is separated from the converted feed mixture prior to cooling the converted feed mixture. To obtain individual parts of the solid phase residue as separate streams the solid phase is separated in a hydro cyclone and/or one or more filters.
  • the concentrated digestate fraction may advantageously be washed with water prior to the thermo-chemical step.
  • the water may preferably be a recycled, water stream from the thermo-chemical process step or the drying step in case of a hydrothermal liquefaction process or a pyrolysis process, respectively.
  • the wash water may be mixed with the liquid digestate fraction from the separation step b).
  • the recycling streams are shown including further options for reusing water and residual heat, hereby increasing the energy efficiency of the gas and bio-oil production further. The fact that some of the streams shown in Fig. 1 or 3 are left out does not exclude the combination of these.
  • the recycling streams are shown including further options for reusing water and residual heat, hereby increasing the energy efficiency of the gas and bio-oil production further. The fact that some of the streams shown in Fig. 1 or 2 are left out does not exclude the combination of these.

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Abstract

L'invention concerne un procédé de production de combustibles gazeux et liquides, le procédé comprenant les étapes suivantes : mise à disposition d'une matière première ; ajout de la matière première à un digesteur anaérobie pour produire un biogaz et un digestat comme produit résiduel ; déshydratation du digestat à un niveau prédéterminé ; ajout du digestat déshydraté à un processus thermochimique pour produire une biohuile ; et valorisation au moins partielle du dioxyde de carbone dans ledit biogaz en méthane dans un réacteur de biométhanisation.
PCT/DK2023/050106 2022-04-28 2023-04-28 Procédés de production combinée de combustibles gazeux et liquides WO2023208307A1 (fr)

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Non-Patent Citations (5)

* Cited by examiner, † Cited by third party
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