WO2011159352A2 - Production de gaz à faible teneur en goudrons dans un gazéificateur étagé - Google Patents

Production de gaz à faible teneur en goudrons dans un gazéificateur étagé Download PDF

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Publication number
WO2011159352A2
WO2011159352A2 PCT/US2011/001080 US2011001080W WO2011159352A2 WO 2011159352 A2 WO2011159352 A2 WO 2011159352A2 US 2011001080 W US2011001080 W US 2011001080W WO 2011159352 A2 WO2011159352 A2 WO 2011159352A2
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Prior art keywords
char
reactor
partial oxidation
gas
media
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PCT/US2011/001080
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English (en)
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WO2011159352A3 (fr
Inventor
Thomas J. Paskach
John P. Reardon
Paul Evans
Jerod Smeenk
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Frontline Bio Energy,Llc
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Publication of WO2011159352A2 publication Critical patent/WO2011159352A2/fr
Publication of WO2011159352A3 publication Critical patent/WO2011159352A3/fr

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    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
    • C10J3/00—Production of combustible gases containing carbon monoxide from solid carbonaceous fuels
    • C10J3/46—Gasification of granular or pulverulent flues in suspension
    • C10J3/48—Apparatus; Plants
    • C10J3/485—Entrained flow gasifiers
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
    • C10J3/00—Production of combustible gases containing carbon monoxide from solid carbonaceous fuels
    • C10J3/46—Gasification of granular or pulverulent flues in suspension
    • C10J3/463—Gasification of granular or pulverulent flues in suspension in stationary fluidised beds
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
    • C10J3/00—Production of combustible gases containing carbon monoxide from solid carbonaceous fuels
    • C10J3/46—Gasification of granular or pulverulent flues in suspension
    • C10J3/466—Entrained flow processes
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
    • C10J3/00—Production of combustible gases containing carbon monoxide from solid carbonaceous fuels
    • C10J3/46—Gasification of granular or pulverulent flues in suspension
    • C10J3/48—Apparatus; Plants
    • C10J3/482—Gasifiers with stationary fluidised bed
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
    • C10J3/00—Production of combustible gases containing carbon monoxide from solid carbonaceous fuels
    • C10J3/72—Other features
    • C10J3/721—Multistage gasification, e.g. plural parallel or serial gasification stages
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
    • C10J3/00—Production of combustible gases containing carbon monoxide from solid carbonaceous fuels
    • C10J3/72—Other features
    • C10J3/82—Gas withdrawal means
    • C10J3/84—Gas withdrawal means with means for removing dust or tar from the gas
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
    • C10J2300/00—Details of gasification processes
    • C10J2300/09—Details of the feed, e.g. feeding of spent catalyst, inert gas or halogens
    • C10J2300/0913—Carbonaceous raw material
    • C10J2300/0916—Biomass
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
    • C10J2300/00—Details of gasification processes
    • C10J2300/09—Details of the feed, e.g. feeding of spent catalyst, inert gas or halogens
    • C10J2300/0913—Carbonaceous raw material
    • C10J2300/0946—Waste, e.g. MSW, tires, glass, tar sand, peat, paper, lignite, oil shale
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
    • C10J2300/00—Details of gasification processes
    • C10J2300/09—Details of the feed, e.g. feeding of spent catalyst, inert gas or halogens
    • C10J2300/0953—Gasifying agents
    • C10J2300/0956—Air or oxygen enriched air
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
    • C10J2300/00—Details of gasification processes
    • C10J2300/09—Details of the feed, e.g. feeding of spent catalyst, inert gas or halogens
    • C10J2300/0953—Gasifying agents
    • C10J2300/0959—Oxygen
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
    • C10J2300/00—Details of gasification processes
    • C10J2300/09—Details of the feed, e.g. feeding of spent catalyst, inert gas or halogens
    • C10J2300/0983—Additives
    • C10J2300/0993—Inert particles, e.g. as heat exchange medium in a fluidized or moving bed, heat carriers, sand
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
    • C10J2300/00—Details of gasification processes
    • C10J2300/18—Details of the gasification process, e.g. loops, autothermal operation
    • C10J2300/1807—Recycle loops, e.g. gas, solids, heating medium, water
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E50/00—Technologies for the production of fuel of non-fossil origin
    • Y02E50/30—Fuel from waste, e.g. synthetic alcohol or diesel
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P20/00—Technologies relating to chemical industry
    • Y02P20/141—Feedstock
    • Y02P20/145—Feedstock the feedstock being materials of biological origin

Definitions

  • the present invention relates, in general, to gasifying materials such as biomass and waste to produce high quality gas.
  • secondary and tertiary reaction products of primary tars are termed “secondary tar” and “tertiary tar”.
  • Tertiary tars were sub-classified as tertiary-alkyl and tertiary- polynuclear aromatic hydrocarbons (PAH). It is hypothesized that once tertiary tars are formed these may require even higher temperatures and additional residence time for thermal destruction.
  • Partial Oxidation has been explored as an alternate method for achieving tar destruction.
  • This method includes blast containing oxygen subsequently added to raw generated gas.
  • the Energy Center of the Netherlands (ECN) performed experiments using an atmospheric circulating fluidized bed gasifier (operated at 850°C) where air was added subsequently to increase the product gas temperature to 1100° or more.
  • a temperature of 1150°C was required, resulting in a cold gas efficiency loss of 8%.
  • Naphthalene and tertiary PAH (3+ ring) were totally eliminated with an inlet hydrogen content greater than 30%vol, but single ring aromatics, e.g. toluene and benzene were retained. Therefore, gasifier operations that increase the fed hydrogen concentration should result in beneficial tar reduction for the same POX condition.
  • the natural minerals in biomass ash (MgO, CaO, 2 0, etc.) are believed to contribute to the catalytic effect, but the state of prior preparation (temperature history, surface area or oxidative exposure) is also thought to impact performance.
  • a partial oxidation zone that achieves higher temperatures (1150°C) can be used to help effectively convert tars with or without passing through a fixed bed of char.
  • the presence of hydrogen in the fed gas is an important feature to achieve maximum POX performance where opening aromatic rings can be favored over PAH growth. It is thought that the type of tars produced may also impact their ability to be subsequently reformed on a bed of char, and may impact the cracking performance in the POX stage; however, this has remained an unproven possibility.
  • the lowest tar performance occurs when the secondary air (45) added to the char bed (44) is at its maximum and thus primary air at its minimum. Setting the secondary air flow such that it is slightly below the level where "smoke" puffs out the open top describes the relativity desired of primary and secondary air. Peak temperatures over 1000°C were achieved in the char zone (46).
  • the first stage of the optimally operated two-stage downdraft gasifier functions as an indirectly heated devolatilization or pyrolysis stage (43) and is likely to produce simpler "primary" and “secondary” tar compounds. These primary and secondary tar compounds occur at relatively low temperatures (500 to 700°C) prior to encountering the hot char bed (47). The hot char bed is believed to provide high temperature thermal cracking opportunity as well as catalytic benefit from the biomass ash minerals.
  • An alternative downdraft gasifier having a separated POX zone is another possibility (See Fig. 4)._One of the challenges with the classical two-stage, fixed bed, downdraft gasifier is that injection of blast into a fixed bed of char can lead to difficult operational problems— slagging (temperatures well over the ash fusion point), clinkering (fused ash particles), chanelling ("rat holing"), fuel bridging and material degradation in the blast input tube.
  • the DTU gasifier incorporates a separate low temperature pyrolysis stage(52) (500 to 600°C) that is configured above a vortex flow partial oxidation section(55) operated to achieve peak temperatures ⁇ 1 150°C— this stage is the only zone of direct blast addition.
  • This partial oxidation zone (505) is situated above a downdraft, dense "fixed” bed of char (57) supported on a mechanical grate (58) comprised of pivoting angle iron.
  • the DTU design suffers from limited scale-up potential (due to the fixed bed of char (57) and indirectly heated feed auger (51)).
  • the DTU gasifier system proved to yield very low tars ( ⁇ 25 mg/Nm 3 ) and produced a rich gas with -25% hydrogen without steam addition, and -35% hydrogen with steam addition.
  • the gas quality was greatly enhanced by the recuperative indirect heat stage that can include indirect drying (52).
  • the main difficulty with the DTU system is that the gasifier system still relied on a fixed bed of char, which consists of low bulk density solids that are irregular in particle size and shape.
  • a relatively low superficial velocity is believed to be required for achieving a char pile without disruption on the mechanical grate (58) (previously described)— which indicates a costly scale- up for this reaction stage.
  • the low density bed of char exhibits chaotic solids flow properties that would be unmanageable in an industrial-scale system with commercial reliability requirements.
  • Moving granular beds have also been used in prior art to present char as a catalyst to produced gas but in a cross flow moving granular bed filter, see Fig. 1 (Van der Drift 2005).
  • the Van der Drift article describes a laboratory experiment for validating the theory that char can perform as a tar reduction catalyst and only employed a slip stream from a larger gasifier.
  • the cross-flow design was reported to achieve high filtration efficiency and about 75% reduction in tar at 900°C, being presented with gas from a fluid bed that was operated at 850°C.
  • the media retention screen (18) at the dust laden gas inlet (16) of the moving granular bed of char was reported to have dust fouling problems, and the system also suffered from media agglomeration within the gas media retention screens (18) which made media movement difficult.
  • FIG. 2 Another moving granular bed filter which is shown in Fig. 2 is disclosed in US
  • the present invention differs from the above referenced inventions and others similar in that these prior devices do not provide features that can be readily scaled up to industrial operational levels. What was needed was a gasifier system able to meet the low tar requirements while producing high quality gases, and which is feasible and operable in an industrial setting.
  • embodiments of the invention relate to a gasification system for converting feedstocks such as biomass and waste to combustible gases with low tar levels.
  • Embodiments of the invention include a gasifier wherein the char bed can be scaled up while managing the low bulk density solids and the irregularities in operation caused by variations in superficial velocity.
  • Some embodiments of the invention include a gasifier that provides a partial oxidation zone(s) to allow maximum advantage of the high temperatures required for lowest tar production. Additionally, embodiments of the invention provide a gasifier that fosters high quality gas production. Further embodiments of the invention include a gasifier constructed to provide disengagement screen scrubbing.
  • the utility of the present invention is to convert biomass and waste feedstock
  • solids into a combustible gas at elevated temperature and pressure with substantially reduced tar concentrations.
  • this invention may be applicability of this invention to gasification of other higher volatile matter solid fuels, including for example, various low rank coals, brown coal, peat, and lignite. Achieving low tar gas is the key to unlocking quantitative gas conditioning needed for. advanced high efficiency gas-to-power systems (engines, combustion turbines, solid oxide fuel cells, etc.) and advanced synthesis technology for biofuels (ethanol, mixed alcohols, and Fischer- Tropsch liquids) and chemicals such as hydrogen and ammonia.
  • Embodiments of the invention utilize an entrained flow reactor coupled downstream of a fluidized bed reactor.
  • An entrained flow reactor is a reactor in which the reactant feedstock and oxidant are fed into the top of the reactor so that the oxidant stream surrounds (e.g., "entrains") the feedstock and carries the feedstock through the reactor.
  • a fluidized bed reactor is one in which a fluid is forced upward through a granular bed at velocities sufficient to cause the granular material to behave, in many respects, as a fluid.
  • the entrained flow reactor incorporates a moving granular bed that captures and supports a catalytic char bed.
  • a first illustrative embodiment of the present invention relates to a multi-stage reaction system for producing low-tar combustible gas.
  • the system includes a fluidized bed reactor that includes a partial oxidation zone, in which a portion of the solid feedstock is partially oxidized, thereby creating a gas and a plurality of char particles.
  • the illustrative embodiment further includes an entrained flow partial oxidation reactor situated downstream from the fluidized bed reactor, and where the entrained flow partial oxidation reactor includes a moving granular bed.
  • a second illustrative embodiment of the present invention relates to a multi-stage reaction system for producing low-tar combustible gas.
  • the system includes a fluidized bed reactor that includes a partial oxidation zone, in which a portion of the feedstock is partially oxidized thereby creating a gas and a plurality of char particles.
  • the illustrative embodiment further includes an entrained flow partial oxidation reactor situated downstream from the fluidized bed reactor.
  • the entrained flow partial oxidation reactor includes a moving granular bed.
  • a media screening device screens media from the moving granular bed and a media recycle system returns the screened media to the entrained flow partial oxidation reactor.
  • a third illustrative embodiment of the present invention relates to a method for controlling an operating pressure of a two-stage gasification system.
  • the method includes performing a partial oxidation of a portion of the feedstock in a fluidized bed reactor; elutriating the resulting plurality of char particles and the gas from the fluidized bed reactor as a mixture of gas and char; receiving the mixture into an entrained flow reactor that includes a moving granular bed of filtering media; and allowing the mixture to flow through the moving granular bed of char and media.
  • embodiments of the method further include capturing a portion of the plurality of char particles in the filtering media; screening a portion of the filtering media to remove captured char particles; and returning the screened filtering media to the entrained flow reactor.
  • FIG. 1 is a schematic drawing of tar reduction by tar reduction equipment in accordance with the prior art
  • FIG. 2 is a schematic drawing of a counter-flow moving granular bed filter in accordance with the prior art
  • FIG. 3 is a schematic drawing of a classical two-stage downdraft gasifier in accordance with the prior art
  • FIG. 4 is a schematic drawing of a downdraft gasifier incorporating an indirect heat stage and separation of the partial oxidation zone and char fixed bed in accordance with the prior art
  • FIG. 5 is a schematic drawing of a gasifier system in accordance with a first embodiment of the invention described herein;
  • FIG. 6 is a schematic drawing of a gasifier system in accordance with a second embodiment of the invention described herein;
  • FIG. 7 is a schematic drawing of a gasifier system in accordance with a third embodiment of the invention described herein;
  • FIG. 8 is a schematic drawing of a gasifier system in accordance with a fourth embodiment of the invention described herein;
  • FIGS. 9 A and 9B are top-plan diagrammatic views of nozzle placement and air flow
  • FIG. 1 OA is a schematic drawing of a front view of a screen
  • FIG. 10B is a schematic drawing of an end view of a screen
  • FIG. 1 1 is a flow diagram depicting an illustrative method of the tar-reducing gasifier system in accordance with certain embodiments of the invention described herein;
  • the gasification system 100 includes a first reactor 101 and, situated downstream from the first reactor 101, a second reactor 102. As shown in FIG. 5, the gasification system 100 also includes a media screening device 103, a media recycle system 104, and a heat recovery device 105. It should be understood that the illustrative gasification system 100 is merely one example of a suitable gasification system and is not intended to express or suggest any particular limitations regarding implementations of aspects of embodiments of the invention.
  • the gasification system 100 can include any number of additional components such as, for example, those illustrated in FIGS. 6-8.
  • one or more of the components described herein can be integrated with one another and in other embodiments, one or more of the components described herein can be separated into any number of desired features, functions, and the like.
  • the first reactor 101 is a fluidized-bed reactor and the second reactor 102 is an entrained flow reactor.
  • the second reactor 102 can also include fluidized-bed technology, and in other embodiments, the first reactor 101 can include entrained flow technology. All of these various embodiments and implementation are considered to be within the ambit of the invention.
  • the first reactor 101 includes an upper portion
  • the upper portion 106 of the first reactor 101 includes a freeboard 110, which provides a partial oxidation zone 112.
  • the lower portion 108 of the first reactor 101 includes a fluidized bed 1 14 and a port 1 16 used for adding heat.
  • the first reactor 101 also includes, as illustrated in FIG. 5, a number of blast inlets 1 18, a solid fuel port 120, and a blast/steam inlet 122.
  • a fluidized-bed media discharge port 124 is situated at the bottom of the lower portion 108 of the first reactor 101.
  • the fluidized-bed media discharge port 124 discharges media into a media discharge system 125, which can carry the discharged media to any number of various destinations such as, for example, a waste receptacle, a storage tank, a recycling system, and the like.
  • the first reactor 101 creates a hydrogen-rich partial oxidation zone
  • the second reactor 102 is a two-stage entrained flow gasifier that is operated in a non-slagging mode.
  • the first stage is a partial oxidation stage and is accomplished in the partial oxidation zone 126 of the second reactor 102. As shown in FIG.
  • the partial oxidation zone 126 of the second reactor 102 is situated within an upper portion 128 of the second reactor 102.
  • the partial oxidation zone 126 includes a low-swirl partial oxidation burner 136.
  • a number of blast inlets 138 and 140 are located in the upper portion 128 of the second reactor 102 and will preferably include a multiple of blast nozzles 142 at each level, as needed to achieve localized "thermally intense zones," which will be described in more detail below, with reference to FIGS. 9 A and 9B.
  • the first reactor 101 can also include a partial oxidation burner such as the burner 136.
  • the second stage associated with the second reactor 102 is a "dense-bed" stage and is accomplished in a catalytic char-reduction zone 130 that is situated within a lower portion 132 of the second reactor 102.
  • the catalytic char-reduction zone 130 includes a moving granular bed 134 that facilitates operation of the second stage associated with the second reactor 102.
  • Embodiments of the invention can include a number of different options for configuring blast nozzles 142 around the periphery the first reactor 101 and/or the second reactor 102.
  • the configuration of the blast nozzles 142 facilitates forming localized regions of oxidative thermal intensity (by virtue of the mixing pattern), rather than achieving more uniform mixing patterns achieved by typical approaches to designing gas burners for lean fuel conditions.
  • FIGS. 9A and 9B top-view schematic drawings illustrate two different illustrative configuration options for placement of the blast nozzles 142, respectively.
  • a vessel (e.g., reactor) 145 includes a number of inlet ports 147 and 149 having blast nozzles 150 and 151, respectively.
  • the blast nozzles 150 and 151 are configured in an alternating pattern such that the blast nozzles 150 and 151 direct inputs toward tangent curves 152 and 154 associated with one or more target circles 1 3 and 156, the diameter of which can be varied according to various embodiments of the invention.
  • the blast nozzle 150 targets the tangent 152 of a first target circle 153, which has a first diameter 157a.
  • the blast nozzle 151 targets a tangent curve 154 of a second target circle 156, which has a second diameter 157b.
  • the first diameter 157a can be smaller in magnitude than the second diameter 157b.
  • the first diameter 157a can be larger in magnitude that the second diameter 157b.
  • the targeting direction of each of any additional blast nozzles is configured to alternate between tangent curves of the first and second target circle 153 and 156.
  • the blast nozzles 150 and 151 are oriented at the same elevation as one another, and therefore provide a coherent flow direction. Other flow patterns can be achieved, in other embodiments, by injection in a contrary flow direction at slightly different elevations.
  • FIG. 9B an alternative configuration option for configuring blast nozzles to achieve desirable flow patterns in a blast zone 162 situated within a reactor vessel 160 is depicted.
  • the vessel (e.g., reactor) 160 includes a number of inlet ports 163 and 165 having blast nozzles 166 and 168, respectively.
  • the blast nozzles 166 and 168 are configured in an alternating pattern such that the blast nozzles 166 and 168 direct inputs toward tangent curves of target circles that are defined at different elevations.
  • the blast nozzle 166 targets the tangent curve 171 of a first target circle 169, which has a first diameter 173a.
  • the blast nozzle 168 targets a tangent curve 174 of a second target circle 170, which has a second diameter 173b.
  • the first target circle 169 and the second target circle 170 are situated at different elevations with respect to one another. That is, in certain embodiments, the first target circle 169 can be situated at a lower elevation than the second target circle 170, while in other embodiments, the second target circle 170 can be situated at a lower elevation than the first target circle 169.
  • the first diameter 173a can be smaller in magnitude than the second diameter 173b. In other embodiments, the first diameter 173 a can be larger in magnitude that the second diameter 173b. In further embodiments, the first diameter 173a and the second diameter 173b can be substantially the same.
  • the targeting direction of each of any additional blast nozzles is configured to alternate between tangent curves of the first and second target circle 169 and 170.
  • one or more auxiliary blast zones will include multiple nozzles configured around the perimeter of the vessel so as to create at least two tangent target circles.
  • the nozzles can be configured such that the inputs are injected coherent at the same elevation, while in other embodiments, the nozzles can be configured such that the inputs are injected convergent at slightly different elevations.
  • mixing performance associated with the blast zones 146 and 162 can be optimized through computational fluid dynamics (CFD) calculations.
  • CFD software can be used to create 3-D patterns with thermally intense zones having various peak temperatures.
  • mixing performance can be optimized by varying relative diameters of the target circles, adjusting swirl number (e.g., utilizing a swirl number less than 0.4), and by optimizing the equivalence ratio of the total auxiliary blast addition.
  • the equivalence ratio, ⁇ is the blast to fuel ratio, relative to the stoichiometric blast to fuel required to just burn the fed gas and char.
  • the total auxiliary blast input is less than about 25% of the stoichiometric blast- to-fuel ratio calculated relative to the fed feedstock analysis. Additionally, in some embodiments, the total auxiliary blast can be about 50%, or more (and even up to 100%, particularly when indirect heat is supplied during the first stage), of the entire blast input to the reaction system.
  • the blast nozzle configuration is developed using CFD software to model at least one thermally intense zone having a peak temperature of ⁇ 1 150°C.
  • the total auxiliary blast addition is controlled such that it has an equivalence ratio, ⁇ , of approximately 0.2 (or less) in oxygen limited partial oxidation and incorporates a majority (>50%) of the total blast addition through auxiliary ports, configured to achieve localized zones of peak temperature of approximately 1 150°C. Configuring the blast nozzles accordingly can facilitate achieving desired performance objectives during operation.
  • a peak temperature of between about 1000°C and about 1200°C generally is sufficient for activating hydrogen molecules in the manner necessary for cracking aromatic ring compounds and providing the necessary termination to avoid ring polymerization. Too high a temperature in the bulk gas may cause melting of ash and slag formation that can interfere with operation. Accordingly, the partial oxidation zones are configured to include local thermally intense zones rather than high bulk gas temperatures. These localized thermally intense zones facilitate activation of hydrogen radicals that can subsequently initiate chemical reactions in the adjacent bulk gas. For example, hydrogen facilitates terminating the activated carbon atom in an aromatic ring that has been thermally cracked open, thereby providing for tar reduction rather than tar polymerization.
  • a gas containing elutriated char 199 escapes the first reactor 101 by an elutriation mechanism 200 and travels from the elutriation mechanism 200 through a gas conduit 202.
  • the elutriated char 199 is delivered, via the gas conduit 202, to the second reactor 102 through a main gas inlet 204.
  • the maximum size and delivery rate of the elutriated char 199 can be controlled, to a degree, by mamtaining the freeboard 1 10 superficial velocity through control of the operating pressure of the gasification system 100.
  • the elutriated char particles 199 pass into the second reactor 102, either in a dispersed manner, through the main gas inlet 204, as shown in FIG. 1, or in a separated and concentrated form, through an auxiliary blast port 140 (e.g., see FIG. 7).
  • the operating pressure of the gasification system 100 for a given gas production rate, it is possible to control (to a degree) the maximum particle size and the rate of release of char 199, and the maximum particle size of the char 199, through the elutriation mechanism 200 associated with the first reactor 101.
  • the particle size of the char 199 affects the catalytic performance of the char 199 for gas temperatures of less than 1000°C. In other words, a smaller particle size tends to produce more tar reduction for the same temperature, particularly if the temperature is less than 1000°C. For example, at 900° tar reduction in one study was 88% for one particle size range (1 to 2 mm) and 96% for another (0.1 to 0.15 mm).
  • certain embodiments of the invention incorporate a method of operating the gasification system to control the char 1 19 particle size and elutriation rate.
  • the method includes, at least in part, maintaining a target velocity in the freeboard 1 10 of the first reactor 101 by modulating the pressure set point.
  • pressure modulation can be accomplished in a number of ways such as, for example, modulating fuel and air inputs, modulating a downstream valve position (e.g., downstream from a particulate removal), and the like.
  • the gasification system 100 can include one or more modulating valves 210 that can be utilized to modulate downstream particulate removals, thereby providing some level of control over the operating pressure of the system 100.
  • pressure control can be achieved by controlling the flow of char 199 through the second reactor 102.
  • the gas 215 engaging the moving granular bed 134 in the second reactor 102 moves in co-flow direction with granular material 135.
  • the granular material is input via the main gas inlet 204 of the second reactor 102.
  • the moving granular bed 134 captures and dilutes char 199 in a matrix of granular solids 135 that has a higher specific gravity, thereby improving the solids' 135 flow properties.
  • a zone of gas-char 215 is created such that the gas-char 215 contacts, with sufficient residence time, the char 199 solids for catalytic tar-reduction-by-char.
  • the moving granular bed 134 captures and mixes the low density char 199 (usually ⁇ 190 kg/m ) with other media (usually >1900 kg/m 3 ), thereby improving the char 199 flow properties. In this manner, the flow of char 199 can be positively managed by its association with the co-flowing media matrix 134.
  • the concentration of char 199 in the granular bed 134 can be managed through a screening stage, accomplished by the media screening device 103.
  • a portion of char 199 and media 135 is removed, via a media discharge port 220 and provided to the media screening device 103.
  • the char 199 is separated from the media 135.
  • the media recycle system 104 is used to return the screened media 135 to the second reactor 102.
  • the char 199 screened from the media 135 is discharged via a residue discharge system 221.
  • the particle size of the moving granular bed 134 can be the same as the particle size of the fluidized bed 1 14 in the first reactor 101 (e.g., see FIG. 8). In other embodiments, particle size of the moving granular bed 134 can be much larger than the particle size of the fluidized bed 114 in the first reactor 101 (e.g., 10 times larger) to create a favorable pressure drop through the moving granular bed 134 in the second reactor 102.
  • a flow diagram depicts an illustrative method 300 of controlling an operating pressure of a two-stage gasification system.
  • the illustrative method includes performing a partial oxidation of solid feedstock in a fluidized bed reactor.
  • the fluidized bed reactor can be similar to, for example, the reactor 101 described above with reference to FIG. 5.
  • Performing the partial oxidation in the fluidized bed reactor generates, among other things, gas and char.
  • the char can be elutriated from the fluidized bed reactor as a gas/char mixture, as shown at step 312, using an elutriation device, or simply allowed to elutriate naturally without any additional device.
  • the mixture is received into an entrained flow reactor that has a moving granular bed.
  • the entrained flow reactor can be similar to the second reactor 102 described above with reference to FIG. 5.
  • the mixture is allowed to flow through the moving granular bed and, as the mixture moves through the moving granular bed, char particles are captured in the media of the moving granular bed, as indicated at step 318.
  • a portion of the media of the moving granular bed is screened to remove char particles, as shown at step 320.
  • the screened media is returned to the moving granular bed.
  • the illustrative method 300 can be used alone, or in conjunction with other methods, to affect control over the operating pressure of the gasification system by controlling the char flow rate in the entrained flow reactor.
  • embodiments of the moving granular bed 134 do not require an inlet screen for media retention at the gas engagement interface by virtue of the geometric down-flow design.
  • the media retention screen at the dust-laden gas inlet of the moving granular bed of the prior art illustrated in FIG. 1 was reported to have dust-fouling problems in the gas engagement.
  • embodiments of the present invention do not require any media retention screen at the gas engagement thereby providing an improved method of employing char as a catalyst.
  • conventional moving granular beds are tuned (e.g., adjusted and controlled) to provide optimum filtration
  • the moving granular bed 134 of the present invention is tuned to provide an optimal char contacting zone.
  • the moving granular bed 134 is operated to capture char 199 as a physical barrier.
  • the media residence time is correlated with the char residence time (the period of time that the average char particle spends in the reactor), and this char residence time can be modulated in a controlled manner with the media screening and recycle subsystem (103/104).
  • the moving granular bed 134 also can be configured to provide a zone of narrow gas residence time distribution through the char bed 134 in a conceptually plug flow reactor that allows for maximum tar cracking.
  • the gas residence time and char residence time can differ by several orders of magnitude; therefore, the differential velocity between the gas 215 and char 199 is very close to the local gas interstitial velocity through the bed 134.
  • the char in the char bed 134 is continuously refreshed by the char 199 supply from the first reactor 101 thereby reducing or eliminating the need for high performance filtration, even though some small particles of char 199 may slip through the bed with the gas 215.
  • the moving granular bed 134 includes a substantially vertical gas disengagement screen 222.
  • the disengagement screen 222 is comprised of a plurality of wires 224, oriented in a substantially parallel and vertical manner.
  • the wires 224 are situated between an upper frame edge 222a and a lower frame edge 222b.
  • the screen 222 can also include a pair of side frame edges 222c.
  • the disengagement screen 222 includes a number of gaps 225, each gap 225 being defined between two adjacent wires 224.
  • FIG. 10B depicts a bottom, partial view of the screen 222. As shown in FIG.
  • each wire 224 may be made of commercially available triangular profile wire, or includes a wedge or V-cross section defined by a first side 230 and a second side 232 that meet at a vertex 234.
  • the two sides 230 and 232 of the wire 224 converge (at the vertex 234) in the direction of gas flow.
  • the gaps 225 between the wires 224 are designed relative to the smaller cut size of the granular media.
  • the substantially vertical orientation (which, at a minimum, is steeper than the angle of repose of the char-media matrix 135 of FIG. 5) of the gas disengagement screen 222 provides for scrubbing action with the moving bed 134 to maintain the gas disengagement screen 222, without plugging.
  • Embodiments of the moving granular bed 134 of the present invention include features that are not known to the art and that have been described above. These features include, for example, a co-flow design that is preferred for its gas-char contacting zone for enhancing catalytic tar-reduction-by-char performance rather than for its filter performance; the lack of a need for a media retention screen for media retention at the gas engagement interface; and a substantially vertically oriented gas disengagement screen (e.g., which is steeper than the angle of repose of the blended char and media matrix to scrub the disengagement screen keeping it free of dust clogging).
  • Pat. No. 7,309,384 to Brown et al., and illustrated herein in FIG. 2, does not provide for disengagement screen scrubbing.
  • the counter filter 304, 307 disclosed in the Brown et al. patent also does not provide the opportunity for extended gas residence time in the presence of char. Instead, the gas residence time is shorter due to the rapid char and media disengagement in the counter flow design which, in turn, shortens the gas-char contact and reduces the catalytic reduction of tar by char.
  • embodiments of the present invention do not include, or require, the presence of a gas barrier for media retention whereas the Brown et al. invention will not work without such a barrier.
  • the residence time (increased internal age distribution) of the trapped char particles is controlled by modulating the media flow that captures the char through an external recycle loop.
  • a first embodiment employs a bubbling fluid bed reactor 101 , the transport disengagement height of the freeboard 1 10 design, and the target operating velocity to achieve a mixture of gas 215 and char 199 delivered to the second reactor 102.
  • the gasification system 100 of FIG. 5 includes an "external" active media recycle system 104 (which can be, for example, mechanical or pneumatic conveying).
  • the fluid bed reactor 101 can include processing of the discharge stream 125 to remove foreign "tramp" materials entering with the feedstock, and can optionally be recirculated and reheated in a direct or indirect heating loop and returned to the first reactor 101 via the port 116.
  • FIG. 6 another embodiment of a gasification system 240 is illustrated.
  • the gasification system 240 includes a first reactor 241, which is a fluidized bed reactor, a second reactor 242 having a moving granular bed 243, a media screening device 244, a media recycle system 246, and a heat recovery device 248.
  • This particular embodiment (illustrated in FIG. 6) is designed to enable a higher, more turbulent, velocity in the fluidized bed reactor 241 without excessive loss of fluid bed sand.
  • a sand recovery roughing cyclone 250 is an elutriation device included between the first reactor 241 and the second reactor 242.
  • the illustrative gasification system includes a first (fluidized bed) reactor 261, a second (entrained flow) reactor 262 having a moving granular bed 263, a media screening device 264, a media recycle system 265, and a heat recovery device 266.
  • the sand recovery cyclone 268 and turbulent fluid bed 263 are both included, but a char-concentrating cyclone 270 is also included to give an opportunity for separate, controlled char injection into the partial oxidation zone 276 of the second reactor 262.
  • FIG. 7 illustratesand recovery cyclone 268 and turbulent fluid bed 263
  • a char-concentrating cyclone 270 is also included to give an opportunity for separate, controlled char injection into the partial oxidation zone 276 of the second reactor 262.
  • the gasification system 260 can be optimized for char oxidation heat release by adding blast along with the char feed, therefore creating a hot zone through which the fed gas passes, in which case a lesser amount (or, in some implementations no amount) of blast gas is fed through an upper blast port 279.
  • FIG. 8 another embodiment of a gasification system 280 is illustrated.
  • FIG. 8 is a new form of a circulating fluidized bed reactor system
  • the illustrative gasification system 280 illustrated in FIG. 8 is quite different from the previously described embodiments herein in several respects.
  • this particular embodiment (shown in FIG. 8) requires no external media recycle system. Instead, the same media 283 is cycled between the first reactor 281 and the second reactor 282, and char concentration is modulated by adjusting the portion of discharged sand 290 that either returns to the first reactor 281 or that passes through the media screen 284 before recycling.
  • Circulated media 292 is the same particle size and same material used in the fluidized bed reactor
  • Bed material is circulated in a closed loop between the fluid bed reactor 281 and the second reactor 282.
  • the bed can have a ratio of superficial velocity relative to the minimum velocity required to fluidize (U Umf) of between 6 and 12 to cause increased sand elutriation.
  • Dust-laden media discharging flow (indicated as 290) is split by gravity assist and/or pneumatic push to return a portion into the fluid bed 281a and the balance is processed to remove fines and dust by the media screening device 284 as needed, to produce a cleaned media stream 296.
  • the media stream from the fluid bed 281a and the media screening device 284 combined 298 can optionally be used in a direct or indirect heating loop or cleaned of tramp materials and returned via the port 281b.
  • embodiments of the invention include a gasification system having a fluidized bed reactor situated upstream from an entrained flow reactor.
  • the entrained flow reactor includes a moving granular bed that holds up char and so presents catalytic properties of char to the gas for the purpose of tar cracking.
  • char concentration in the granular solids matrix is controlled with the media screening and recycle system (such as the media screening device 103 and the recycle system 104 illustrated in FIG. 5). Tests have shown that a gasification system having at least some of the features described herein performs as desired.
  • tests were performed under various operating conditions in a laboratory-scale entrained flow reactor, configured according to embodiments of the invention, using yellow seed cord as a model feedstock. Air or oxygen was used as blast as indicated in Table. 1. The stoichiometric air/fuel requirement is 5.45 kg air/kg biomass (dry), or 1.26 kg oxygen/kg biomass (dry). Air blown gasification tests used 3.7 kg/hr biomass, and oxygen blown tests used 6 kg hr biomass with ⁇ 0.45 kg steam/kg biomass. Inert rock material and low grade iron ore (taconite) were used as media in the entrained flow reactor, sized to approximately 1/8" x 1/4" granules.
  • the first stage (fluidized bed) gasifier was operated at various equivalence ratios, ⁇ , (Air/Fuel relative to the stoichiometric Air/Fuel requirement): 0.1 1 , 0.14, and 0.18, as indicated in Table 1 , and achieved fluid bed temperatures from 600 to 700°C.
  • the entrained flow reactor consisted of a small partial oxidation burner that injected blast laterally through 6 small holes (having an internal diameter of 1.4 mm) with slight swirling action, in the configuration illustrated in FIG. 9A, with a tangent circle that is 13 mm diameter, inside of a 40 mm inside diameter pipe, that subsequently expanded into an 100 mm (inside diameter) pipe.
  • Test results indicate that tars were converted with increasing blast (and increasing temperatures) up to a point, which correlated with delivering ⁇ 50% of the total blast into the secondary reactor.
  • the lowest tar condition was ⁇ 560 mg/Nm 3 dry gas.
  • the temperature in the partial oxidation zone was not measured, but the maximum measured temperature in the zone below was 980°C.
  • a reactor configured in accordance with embodiments of the invention, that combines a partial oxidation burner for tar reduction above a "pebble grate" (which is previously described as a bed of granular media supported by a vertical wire screen supporting the media at the gas disengagement) to support a bed of char has not heretofore been known to the art.
  • the integration of a first reactor that operates at lower temperatures in sequence with a higher temperature partial oxidation stage (sub-stoichiometric combustion) with a subsequent heat recuperative device that transports thermal energy back to the first reactor to drive pyrolysis reactions is also not previously known.
  • the co-flow design of the present invention is also not known because it does not impart ideal filtration conditions but rather it imparts ideal gas-char contact conditions for tar cracking.
  • Low density char that otherwise has chaotic solids flow properties—is dispersed into a granular bed material that has approximately ten (10) times the bulk density, which imparts improved solids flow properties. This is an improvement over prior art and contrasts with any reactor that includes a fixed bed of char in downdraft type gasifiers (integrated or separated from partial oxidation zones) that have been known to experience upsets associated with poor solids flow, "solids bridging", and "rat hole” formations due to the chaotic movement and anisotropic nature of low density char beds.

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Abstract

La présente invention concerne un système de gazéification de matières solides à plusieurs étages utilisé pour la production d'un gaz combustible à faible teneur en goudrons. Ledit système comprend un premier réacteur à lit fluidisé permettant la production d'un gaz contenant de l'hydrogène, des vapeurs de pyrolyse, des goudrons et des particules de résidu carboné à une température inférieure à la température de sortie du second réacteur et des zones de post-combustion à oxydation partielle présentant une température supérieure. Un second réacteur comprend une zone d'oxydation partielle présentant une température supérieure en vue de l'activation de l'hydrogène et du craquage de composés à noyau aromatique, un lit granulaire mobile à co-courant comportant un étage de gazéification des résidus carbonés en vue de la catalyse de la réduction des goudrons et de la régulation du temps de résidence des résidus carbonés et un support comprenant un tamis métallique parallèle orienté pratiquement à la verticale et supportant le milieu granulaire.
PCT/US2011/001080 2010-06-16 2011-06-16 Production de gaz à faible teneur en goudrons dans un gazéificateur étagé WO2011159352A2 (fr)

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US10315176B2 (en) 2014-06-09 2019-06-11 Hatch Ltd. Plug flow reactor with internal recirculation fluidized bed
CN108467750A (zh) * 2017-02-23 2018-08-31 中国石油化工股份有限公司 复合式分级气化反应装置及其方法
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