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WO2014005227A1 - Stabilisation de laitier à l'aide de dioxyde de carbone capturé - Google Patents

Stabilisation de laitier à l'aide de dioxyde de carbone capturé Download PDF

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Publication number
WO2014005227A1
WO2014005227A1 PCT/CA2013/050514 CA2013050514W WO2014005227A1 WO 2014005227 A1 WO2014005227 A1 WO 2014005227A1 CA 2013050514 W CA2013050514 W CA 2013050514W WO 2014005227 A1 WO2014005227 A1 WO 2014005227A1
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WIPO (PCT)
Prior art keywords
slag
biocatalyst
solution
stream
contacting
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PCT/CA2013/050514
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English (en)
Inventor
Jonathan Andrew CARLEY
Jingui HUANG
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Co2 Solutions Inc.
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Publication of WO2014005227A1 publication Critical patent/WO2014005227A1/fr

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    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
    • B01D53/34—Chemical or biological purification of waste gases
    • B01D53/46—Removing components of defined structure
    • B01D53/62—Carbon oxides
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
    • B01D53/14—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols by absorption
    • B01D53/1456—Removing acid components
    • B01D53/1475—Removing carbon dioxide
    • C—CHEMISTRY; METALLURGY
    • C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B18/00—Use of agglomerated or waste materials or refuse as fillers for mortars, concrete or artificial stone; Treatment of agglomerated or waste materials or refuse, specially adapted to enhance their filling properties in mortars, concrete or artificial stone
    • C04B18/04—Waste materials; Refuse
    • C04B18/14—Waste materials; Refuse from metallurgical processes
    • C04B18/141—Slags
    • C04B18/142—Steelmaking slags, converter slags
    • C—CHEMISTRY; METALLURGY
    • C12—BIOCHEMISTRY; BEER; SPIRITS; WINE; VINEGAR; MICROBIOLOGY; ENZYMOLOGY; MUTATION OR GENETIC ENGINEERING
    • C12N—MICROORGANISMS OR ENZYMES; COMPOSITIONS THEREOF; PROPAGATING, PRESERVING, OR MAINTAINING MICROORGANISMS; MUTATION OR GENETIC ENGINEERING; CULTURE MEDIA
    • C12N9/00—Enzymes; Proenzymes; Compositions thereof; Processes for preparing, activating, inhibiting, separating or purifying enzymes
    • C12N9/88—Lyases (4.)
    • 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
    • C12P3/00—Preparation of elements or inorganic compounds except carbon dioxide
    • C—CHEMISTRY; METALLURGY
    • C12—BIOCHEMISTRY; BEER; SPIRITS; WINE; VINEGAR; MICROBIOLOGY; ENZYMOLOGY; MUTATION OR GENETIC ENGINEERING
    • C12Y—ENZYMES
    • C12Y402/00—Carbon-oxygen lyases (4.2)
    • C12Y402/01—Hydro-lyases (4.2.1)
    • C12Y402/01001—Carbonate dehydratase (4.2.1.1), i.e. carbonic anhydrase
    • C—CHEMISTRY; METALLURGY
    • C21—METALLURGY OF IRON
    • C21B—MANUFACTURE OF IRON OR STEEL
    • C21B3/00—General features in the manufacture of pig-iron
    • C21B3/04—Recovery of by-products, e.g. slag
    • C—CHEMISTRY; METALLURGY
    • C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22B—PRODUCTION AND REFINING OF METALS; PRETREATMENT OF RAW MATERIALS
    • C22B7/00—Working up raw materials other than ores, e.g. scrap, to produce non-ferrous metals and compounds thereof; Methods of a general interest or applied to the winning of more than two metals
    • C22B7/04—Working-up slag
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2251/00—Reactants
    • B01D2251/60—Inorganic bases or salts
    • B01D2251/606—Carbonates
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2255/00—Catalysts
    • B01D2255/80—Type of catalytic reaction
    • B01D2255/804—Enzymatic
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2258/00—Sources of waste gases
    • B01D2258/02—Other waste gases
    • B01D2258/025—Other waste gases from metallurgy plants
    • C—CHEMISTRY; METALLURGY
    • C21—METALLURGY OF IRON
    • C21B—MANUFACTURE OF IRON OR STEEL
    • C21B2100/00—Handling of exhaust gases produced during the manufacture of iron or steel
    • C21B2100/20—Increasing the gas reduction potential of recycled exhaust gases
    • C21B2100/28—Increasing the gas reduction potential of recycled exhaust gases by separation
    • C21B2100/282—Increasing the gas reduction potential of recycled exhaust gases by separation of carbon dioxide
    • 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
    • Y02C—CAPTURE, STORAGE, SEQUESTRATION OR DISPOSAL OF GREENHOUSE GASES [GHG]
    • Y02C20/00—Capture or disposal of greenhouse gases
    • Y02C20/40—Capture or disposal of greenhouse gases of CO2
    • 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
    • Y02P10/00—Technologies related to metal processing
    • Y02P10/10—Reduction of greenhouse gas [GHG] emissions
    • Y02P10/122—Reduction of greenhouse gas [GHG] emissions by capturing or storing CO2
    • 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
    • Y02P10/00—Technologies related to metal processing
    • Y02P10/20—Recycling
    • 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
    • Y02P20/151—Reduction of greenhouse gas [GHG] emissions, e.g. CO2
    • 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
    • Y02P20/50—Improvements relating to the production of bulk chemicals
    • Y02P20/59—Biological synthesis; Biological purification
    • 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
    • Y02W—CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO WASTEWATER TREATMENT OR WASTE MANAGEMENT
    • Y02W30/00—Technologies for solid waste management
    • Y02W30/50—Reuse, recycling or recovery technologies
    • 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
    • Y02W—CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO WASTEWATER TREATMENT OR WASTE MANAGEMENT
    • Y02W30/00—Technologies for solid waste management
    • Y02W30/50—Reuse, recycling or recovery technologies
    • Y02W30/91—Use of waste materials as fillers for mortars or concrete

Definitions

  • the present invention generally relates to the field of steelmaking and gaseous CO2 capture. More particularly, the present invention concerns processes for capturing CO2 from steelmaking operations using carbonate/bicarbonate based absorption in combination with biocatalysts.
  • CO2 emissions from a steelmaking process are about twice the amount of the steel produced.
  • global steel industry with a production of 1 147 Mt emitted 2200 to 2500 Mt C0 2 , including emissions from coke manufacture and indirect emissions due to power consumption.
  • the worldwide steel production was increased to 1414 Mt (www.worldsteel.org).
  • the CO2 emitted from the iron and steel industry was around 2830 Mt, which is about 7% of global C0 2 emissions.
  • Slag is a byproduct from iron and steel making processes. It includes calcium silicates and ferrites combined with oxides of iron, aluminum, manganese, calcium, and magnesium, as shown in Table 1 .
  • Table 1 Main chemical components and physical properties of steelmaking slags
  • BOF Basic Oxygen Furnace
  • EAF Electric Arc Furnace
  • LMF Ladle Metallurgy Furnace Process
  • Iron and steel slags are formed through the addition of fluxing agents such as limestone or dolomite to blast furnaces and steel furnaces to strip the impurities from iron ore, steel scrap, and other ferrous feeds.
  • fluxing agents such as limestone or dolomite
  • the slags are processed similar to bulk aggregate through sizing, separation and transport. Slag processing typically consists of crushing, screening, and magnetic separation.
  • the magnetically recovered slag may be returned to the blast and steel furnaces as ferrous and flux feed. Up to 50% of the slag volume is recovered as magnetic for return to the furnace.
  • the nonmagnetic materials of the slags are graded by size, and stockpiled for sale.
  • Slags are a mix of iron and other steelmaking wastes (see table 1 ). Magnetic separation is used to recover the Fe containing components of the slag. The amount of remaining nonmagnetic slags is massive and its storage causes land space occupation when landfilling is chosen. Otherwise, slags can be mainly used in building and road constructions.
  • iron and steel slags as high quality mineral aggregates (asphaltic concrete, road base and surfaces) accounts for 63% of the steel slag sold. The next largest use is unconfined construction (fill), accounting for approximately 12- 13%.
  • Slags contain a large amount of basic components inside the nonmagnetic slag materials such as CaO and MgO. When these basic components are in contact with moisture from surrounding air and/or water, alkaline chemicals can be leached out, causing environmental concerns related to land, in the underground water and ecosystems. As aforesaid, slags have many applications in the constructions field. However, slag main active components, CaO and MgO, may cause material swelling, expansion and construction damages. To avoid this problem, slag can be aged or the active components can be pretreated before use. Slags then often go through an ageing period to reach stabilization.
  • CaO/MgO phases in the slag react with water and carbon dioxide from the air to form hydroxides and carbonates. Formation of these compounds will result in a volume change and expansion (swelling) of the slag as evidenced by the following chemical reactions and volume changes.
  • Carbonation of steel slag offers an opportunity to reduce C0 2 emissions and at the same time recycle an industrial waste.
  • the C0 2 capture capacity of iron and steel slag could be around 400 kg C0 2 (109 kg carbon equiv.)/ton slag, depending on the metal being processed, the type of the furnace and the post-processing treatment, which can affect not only the chemical composition, but the crystallinity, phase development, and surface morphology.
  • the blast furnace slag shows a C0 2 capture capacity in a range of 170- 450 kg C0 2 /ton slag.
  • the total sequestration potential of steelmaking slag is about 6-1 1 % of the carbon dioxide emitted from integrated mills, and 35-45% from scrap-based steelmakers.
  • Huijgen et al (W. J. J. Huijgen, G. Witkamp, and R. N. J. Comans. Mineral CO 2 Sequestration by Slag Carbonation, Envirn. Sci. Techn. 2005, 39, 9676-9682) investigated the possibility of capture and sequestration of CO 2 by using steel slags at high temperature and pressure (e.g. @150°C, 20 bars). They found that fresh steel slags contain three major phases of calcium as portlandite Ca(OH) 2 , Ca-(Fe)-silicate, and Ca-Fe-O, as well as several mineral phases including Mg- Fe-O, FeO, and trace of calcite (CaC0 3 ).
  • US Pat. No. 7,906,086 proposes a method of mixing water with two other industrial wastes to prepare a slurry suspension as the scrubbing material for C0 2 capture and sequestration.
  • One of the wastes was selected from cement kiln dust, lime kiln dust, clinker dust, or slaked lime, and another was the iron and steel slag.
  • Such industrial wastes contain plenty of alkaline earth metal oxides such as CaO and MgO, which could be used for CO 2 sequestration.
  • 7,919,064 discloses an approach for CO2 capture by using diluted carbonate salt solutions such as Na 2 C0 3 or K 2 C0 3 or carbonate salts with metal ions from minerals of cement plants or the slag wastes. No detailed descriptions regarding the slag uses and mineral leaching, reaction and sequestration with the leached minerals are given. Further the absorption rate of C0 2 in the diluted carbonate salt solution would be low due to the intrinsic slow mass transfer behavior of the gaseous C0 2 into the carbonate salt system, thus the efficiency of C0 2 capture in the system would be limited.
  • diluted carbonate salt solutions such as Na 2 C0 3 or K 2 C0 3 or carbonate salts with metal ions from minerals of cement plants or the slag wastes.
  • carbonate solutions may exhibit numerous advantages over broadly used amine based absorption solutions such as good stability to oxygen and high temperatures, and lower energy requirements for desorption, they are characterized by a relatively low rate of C0 2 absorption which results in large capture equipment and corresponding capital costs.
  • calcium carbonate forms and accumulates on the surface of the slag particles, which could block some active sites and pathways for diffusion of the calcium ions from inside of the slag particles to the surface or the (bi)carbonate ions to access and react with the Ca ++ of the slag.
  • a slag sequestration system should be relatively simple, efficient and robust to allow for minimal cost impact on slag handling.
  • Bonieri et al (D. Bonieri, L. Kharoune, S. Sauve, R. Hausler, P. Niquette, M. Mimeault, M. Kharoune. Ind. Eng. Chem. Res. 2008, 47, 7610-7616) have showed that the main mineral component of calcium in the steel slags can be leached out at ambient pressure and temperature, and the leached minerals are readily reactive for the C0 2 sequestration. Similar behaviors have been observed by Stolaroff et al (Joshuah K. Stolaroof, Gregory V. Lowry, David W.
  • Biocatalysts have been used for CO 2 absorption applications because of their high efficiency and catalyzation.
  • CO 2 capture and transformation enhanced by biocatalysts such as carbonic anhydrase (CA) enzyme or analogues
  • CA carbonic anhydrase
  • the catalyzed turnover rate may reach 1 ⁇ 10 6 molecules/s, which means that one molecule of the biocatalyst, such as carbonic anhydrase or analogues, can hydrate one million molecules of carbon dioxide in a period of one second.
  • the present invention responds to the above need by providing processes and methods for capturing carbon dioxide, preferably from steelmaking processes, using enzymes.
  • an enzymatically enhanced method for stabilizing a ground slag produced from a steelmaking operation comprising contacting the slag with an ion loaded solution comprising bicarbonate and hydrogen ions produced from enzymatically enhanced absorption of CO 2 .
  • the ground slag and C0 2 may be both by-products of the steelmaking operation.
  • a process for conjointly stabilizing a ground slag containing CaO and MgO and absorbing C0 2 from a C0 2 -containing gas comprising the steps of: a) contacting the C0 2 -containing gas with an aqueous absorption solution in presence of a biocatalyst, in a reactor, for enzymatically catalyzing a hydration reaction of dissolved CO 2 into bicarbonate HCO 3 and hydrogen ions to produce an ion loaded solution and a C0 2 lean gas; b) contacting the ground slag with water to leach CaO and MgO and produce a slurry containing Ca(OH) 2 and Mg(OH) 2 , and c) contacting the slurry produced in step b) with the ion loaded solution produced in step a) to produce CaCO 3 and MgCO 3 and a slag depleted in CaO and MgO.
  • a process for stabilizing a ground slag containing CaO and MgO comprising the steps of: a) contacting a CO 2 -containing gas with an aqueous absorption solution in presence of a biocatalyst, in a reactor, for enzymatically catalyzing a hydration reaction of dissolved CO 2 into bicarbonate HCO 3 and hydrogen ions to produce an ion loaded solution and a CO 2 lean gas; b) desorbing CO 2 from the ion loaded solution; and c) contacting the ground slag containing CaO and MgO with water and the CO 2 produced in step b) to produce CaCO 3 , MgCO 3 and a stabilized slag depleted in CaO and MgO.
  • a process for conjointly stabilizing a ground slag containing CaO and MgO and absorbing CO 2 from a CO 2 -containing gas comprising the steps of: a) contacting the CO 2 -containing gas with an aqueous absorption solution in presence of a biocatalyst, in a reactor, for enzymatically catalyzing a hydration reaction of dissolved CO 2 into bicarbonate HCO 3 and hydrogen ions to produce an ion loaded solution and a CO2 lean gas; and b) contacting the ion loaded solution with the ground slag to produce CaC0 3 , MgC0 3 , a stabilized slag depleted in CaO and MgO, and an alkaline liquor comprising carbonate ions CO3 2" .
  • the process may further comprise the step of: c) recycling at least a part of carbonate ions C0 3 2" of the alkaline liquor produced in step b) as at least a portion of the aqueous absorption solution in the reactor of step a).
  • the process may further comprise mixing the ion loaded solution with water before step b) of contacting the ion loaded solution with the ground slag.
  • the process may further comprise mixing the ground slag with water before step b) of contacting the ion loaded solution with the ground slag.
  • the biocatalyst used may be free or immobilized biocatalyst.
  • the immobilized biocatalyst may be immobilized on or in particles or as aggregates.
  • the particles may be micro or nano particles.
  • the biocatalyst may remain or may be fixed inside the reactor.
  • the biocatalyst may flow through the reactor and may form part of the ion loaded solution.
  • the process may further comprise recovering the biocatalyst from the ion loaded solution before step b), and recycling at least a portion of the biocatalyst as at least a portion of the aqueous absorption solution in the reactor of step a).
  • the biocatalyst may be recovered from the suspension by sedimentation, filtration and/or hydro-cyclonic separation.
  • the process may further comprise: introducing the ion loaded solution containing the biocatalyst into a sedimentation separator to form a first stream rich in biocatalyst and a second stream rich in ion loaded solution having a remaining portion of biocatalyst; recovering the first stream at a bottom portion of the sedimentation separator and using at least a portion of the first stream as at least a portion of the aqueous absorption solution in the reactor of step a); recovering the second stream at a top portion of the sedimentation separator; filtering the second stream to form a third stream of biocatalyst and a fourth stream of ion loaded solution substantially free of biocatalyst; recycling at least a portion of the third stream as at least a portion of the aqueous absorption solution in the reactor of step a); and contacting the fourth stream with the ground slag.
  • the step of filtering may be performed using a membrane filter allowing ultra- or micro-filtration.
  • the process may further comprise: prior to step b), introducing the ion loaded solution into a sedimentation separator for separating the biocatalyst from the ion loaded solution; recovering the biocatalyst at a bottom portion of the sedimentation separator and using at least a portion of the recovered biocatalyst as at least a portion of the aqueous absorption solution in the reactor of step a); and recovering a primary stream comprising the ion loaded solution free of biocatalyst at a top portion of the sedimentation separator and contacting the ion loaded solution with the ground slag.
  • the process may further comprise: recovering a secondary stream comprising remaining biocatalyst and bicarbonate ions at a mid-portion of the sedimentation separator; introducing the secondary stream into a hydrocyclone separator for separating the remaining biocatalyst from the secondary stream; recovering the remaining biocatalyst from the hydrocyclone separator and using at least a portion of the remaining biocatalyst as at least a portion of the aqueous absorption solution in the reactor of step a) ; and recovering a tertiary stream of ion loaded solution free of biocatalyst from the hydrocyclone separator and contacting the tertiary stream with the ground slag.
  • the hydrocyclone separator may comprise a plurality of hydrocyclone separators that are configured in parallel and/or in series.
  • the process may further comprise: continuously conveying the slag on a conveyor; distributing the ion loaded solution in step b) over the ground slag to produce the alkaline liquor and the stabilized slag while the ground slag is continuously conveyed on the conveyor; separating the alkaline liquor from the stabilized slag; and recycling at least a portion of the alkaline liquor as at least a portion of the aqueous absorption solution in the reactor of step a).
  • the process may further comprise: contacting the slag with water to form a slurry comprising Ca(OH) 2 and Mg(OH) 2 , and a stabilized slag depleted in CaO and MgO; contacting the slurry comprising Ca(OH) 2 and Mg(OH) 2 with the ion loaded solution of step a) to produce a stream of CaCO 3 and MgCO 3 , and a stream of alkaline liquor comprising carbonate ions CO 3 2" ; and recycling at least a portion of the stream of alkaline liquor as at least a portion of the aqueous absorption solution in the reactor of step a).
  • the step of contacting the slag with water may further comprise: continuously conveying the slag on a conveyor; distributing water over the slag to form the slurry loaded in Ca(OH) 2 and Mg(OH) 2 and the stabilized slag depleted in CaO and MgO , while the slag is continuously transported on the conveyor; and introducing the slurry loaded in Ca(OH) 2 and Mg(OH) 2 into a tank where the step of contacting the slurry comprising Ca(OH) 2 and Mg(OH) 2 with the ion loaded solution of step a) is performed.
  • the ion loaded solution may comprise NaHCO 3 .
  • biocatalyst may be carbonic anhydrase and/or analogues thereof.
  • the ground slag and the C0 2 -containing gas may be both by-products of a steelmaking operation.
  • the carbonic anhydrase may be provided free in the water; dissolved in the aqueous absorption solution; immobilized on the surface of supports that are mixed in the water and flow therewith; immobilized on the surface of supports that are fixed within the reactor; entrapped or immobilized by or in porous supports that are mixed in the water; entrapped or immobilized by or in porous supports that are fixed within the reactor; as cross-linked enzyme aggregates (CLEA); and/or as cross linked enzyme crystals (CLEC); or a combination thereof.
  • CLSA cross-linked enzyme aggregates
  • CLEC cross linked enzyme crystals
  • the present invention is an improvement in the field of C0 2 capture and sequestration.
  • the invention involves minimal cost impact on the industrial iron and steel slag handling, and also provides opportunities to recycle such wastes for value-added applications.
  • Figure 1 a is a process block flow diagram illustrating one embodiment of the present invention, using biocatalysts of immobilized enzymes and/or crosslinked enzyme (CLEA) microparticles and alkaline carbonate salt solutions recycled from the slag stabilization system.
  • CLA crosslinked enzyme
  • Fig. 1 b is a process block flow diagram illustrating another embodiment of the present invention wherein biocatalyst particles are recovered for reuse through an integrated separation process combining sedimentation and hydrocyclone separators in parallel or in series.
  • Fig. 2 is a process block flow diagram illustrating another embodiment of the present invention wherein biocatalysts are separated by a membrane filter system before sending the ion loaded solution to the slag stabilization process and the recovered free enzymes or the immobilized biocatalysts are recirculated into the CO2 capture system.
  • Fig. 3 is a process block flow diagram illustrating another embodiment of the present invention wherein leached active components (mainly calcium hydroxide) may react with bicarbonate ions from the biocatalyst enhanced CO2 capture process to form an industrial applicable product which can be separated from the system.
  • leached active components mainly calcium hydroxide
  • Fig. 4 is a process block flow diagram illustrating another embodiment of the present invention wherein finely ground slag is continuously transported to a conveyor system where proper containers are provided to collect the ground slag particles.
  • Fig. 5 is a process block flow diagram illustrating another embodiment of the present invention wherein the ground slag is continuously stabilized and recycled of the leached minerals as precipitates which can be then separated and utilized for some specific applications.
  • the invention relates to processes for CO2 capture and sequestration from an iron and steel production process by using steelmaking wastes (such as slag) and biocatalysts.
  • Biocatalysts may be carbonic anhydrase or analogues thereof.
  • carbonic anhydrase or analogues thereof includes naturally occurring, modified, recombinant and/or synthetic enzymes including chemically modified enzymes, enzyme aggregates, cross-linked enzymes, enzyme particles, enzyme-polymer complexes, polypeptide fragments, enzymelike chemicals such as small molecules mimicking the active site of carbonic anhydrase enzymes and any other functional analogue of the enzyme carbonic anhydrase.
  • carbonic anhydrase is not just a single enzyme form, but a broad group of metalloproteins that exists in three genetically unrelated families of isoforms, ⁇ , ⁇ and ⁇ .
  • Carbonic anhydrase (CA) is present in and may be derived from animals, plants, algae, bacteria, etc.
  • the human variant CA II, located in red blood cells, is the most studied and has a high catalytic turnover number.
  • the carbonic anhydrase includes any analogue, fraction and variant thereof and may be alpha, gamma or beta type from human, bacterial, fungal or other organism origins, having thermostable or other stability properties, as long as the carbonic anhydrase can be provided to function in the CO2 capture or desorption processes to enzymatically catalyse the reaction.
  • the enzyme is provided directly as part of a formulation or solution.
  • the carbonic anhydrase may be in a free or soluble state in the formulation or immobilised on or in particles or as aggregates, chemically modified or stabilized, within the formulation.
  • enzyme used in a free state may be in a pure form or may be in a mixture including impurities or additives such as other proteins, salts and other molecules coming from the enzyme production process.
  • Immobilized enzyme free flowing in the solutions could be entrapped inside or fixed to a porous coating material that is provided around a support that is porous or non-porous.
  • the enzymes may be immobilised directly onto the surface of a support (porous or non porous) or may be present as cross linked enzyme aggregates (CLEAs) or cross linked enzyme crystals (CLECs).
  • CLEA comprise precipitated enzyme molecules forming aggregates that are then cross- linked using chemical agents.
  • the CLEA may or may not have a 'support' or 'core' made of another material which may or may not be magnetic.
  • CLEC comprise enzyme crystals and cross linking agent and may also be associated with a 'support' or 'core' made of another material.
  • a support it may be made of polymer, ceramic, metal(s), silica, solgel, chitosan, nylon, alumina, cellulose, alginate, polyacrylamide, magnetic particles, titanium oxide, zirconium oxide and/or other materials known in the art to be suitable for immobilization or enzyme support.
  • the enzymes are immobilised or provided on particles, such as micro-particles, the particles are preferably sized and provided in a particle concentration such that they are pumpable with the solution throughout the process.
  • CaO / MgO from steel slag waste can be dissolved in water and reacted with CO2. They can also react with bicarbonate and such reaction could be much faster in a solution environment, especially when the gaseous C0 2 is already dissolved and converted into an aqueous form, such as the bicarbonate from the biocatalyst enhanced C0 2 capture process.
  • Fig. 1 a presents a process flow diagram for an iron and steel slag stabilization and C0 2 capture system using biocatalysts of immobilized enzymes and/or crosslinked enzyme (CLEA) microparticles and alkaline carbonate salt solution recycled from the slag stabilization system as an aqueous absorption solution.
  • the aqueous absorption solution may be a carbonate- based solution, such as sodium carbonate solution, potassium carbonate solution, ammonium carbonate solution, promoted sodium carbonate solutions, promoted potassium carbonate solutions, or promoted ammonium carbonate; or any combination thereof. These carbonate-based solutions may be promoted with one or more of the above-mentioned biocatalysts.
  • the ion rich solution may contain from about 0.1 M to 10 M of bicarbonate ions.
  • the carbonate loading of the solution will depend on the operating conditions, reactor design and the chemical compounds that are added. For instance, when potassium or sodium bicarbonate compounds are used in the absorption solution, the ion rich solution may contain from about 0.2 M to 1.5 M of bicarbonate ions. When the ion rich solution is highly loaded with carbonate/bicarbonate ions, it may become much more viscous which can have a detrimental effect on mass transport within the solution.
  • the presence of carbonic anhydrase flowing with the solution further enhances the mass transport along with the enzymatic reaction, thus improving the overall C0 2 capture, for instance by supersaturating the solution with bubbles of gaseous C0 2 .
  • Various types of reactors may be used for the absorber, such as a packed column, a bubble column, a fluidized bed, a spray reactor, a flow wire reactor, or another type or design, preferably for gas-liquid contact.
  • the less settled suspension is pumped to a hydrocyclone separator 3 which separates the remaining particles as underflow 36 and the clear part (overflow) 34 from the system.
  • the clear aqueous solution 24 from the sedimentation separator 2, along with the overflow part 34 from the hydrocyclone separator 3, which are rich in bicarbonate ions (HC0 3 " ) are directed to the slag stabilization reactor or system 4.
  • HC0 3 " bicarbonate ions
  • water 42 may be supplied into the stabilization system 4, for instance during the very beginning to help the leaching of the active components from the ground slag, or to adjust the concentration of the bicarbonate solution when needed.
  • the stabilized slags 48 are released from the system, which may be further drained with additional processing or dewatered to recover the alkaline aqueous liquors if needed.
  • the stabilized slags could directly be used as construction materials.
  • the liquid phase (rich of sodium carbonate) 46 formed from the stabilization system 4 is collected in a reservoir tank 5. Some precipitates may be formed in the tank 5, due to settling of possible leached CaCO 3 , and MgCO 3 and slag particles from the system, which could be removed as discharge 56 from the system.
  • the present invention provides a number of advantages. It not only takes advantages of the high efficiency of the bio-enhanced CO2 capture technologies and advances, but provides an industrially applicable and efficient method to treat industrial iron and steel slags. Indeed, the slag stabilization and the C0 2 capture via a bio-enhanced process can be performed at ambient or low temperature and under atmospheric pressure. The present process also enables recycling of the aqueous absorption solution and biocatalysts from the suspension back to the absorber, adding efficiency to the system. Further, it comprises relatively simple apparatuses, which are relatively inexpensive to construct and maintain.
  • Fig. 1 b shows a process diagram for an iron and steel slag stabilization system by using a bio-enhanced C0 2 capture technique with an aqueous absorption solution recycled from the slag stabilization system, and the biocatalyst particles could be recovered for reuse through an integrated separation process combining sedimentation and hydrocyclone separators in parallel and series form.
  • the C0 2 rich flue gas is fed into the gas inlet port 12 near the bottom of the absorber 1.
  • the C0 2 from the flue gas is absorbed and converted into bicarbonate ions and collected at the bottom of the tower 16.
  • the C0 2 absorbed suspension is pumped into a sedimentation separator 2, where the heavier solid particles such as the immobilized biocatalyst particles and/or aggregates are precipitated and separated from the system and collected at the bottom 28.
  • the less settled suspension is pumped to a hydrocyclone separator system 3 of parallel and series hydrocyclones.
  • the feed 32 taken from the middle layer of the sedimentation separator 2 is fed into a hydrocyclone, which separates the remaining particles as underflow 36 and the clear part (overflow) 34 from the system.
  • a hydrocyclone which separates the remaining particles as underflow 36 and the clear part (overflow) 34 from the system.
  • the overflow from the first hydrocyclone is guided to a second hydrocyclone, and the underflow of the second hydrocyclone with rich of fine particles is recycled back to the first hydrycyclone as feed for further separation.
  • the underflow from the first hydrocyclone is fed into another hydrocyclone to give a dense particle suspension in the underflow 36.
  • the overflow from the third hydrocyclone is also recycled back to the first hydrocyclone, combined with the suspension 32 from the sedimentation separator 2 as feed to further concentrate.
  • the clear aqueous solution 24 from the sedimentation separator 2, along with the overflow part 34 from the second hydrocyclone separator 3, which are rich in bicarbonate ions (HC0 3 " ) are directed to the slag stabilization reactor or system 4. After contacting and reacting with the ground slag particles 44 rich in active CaO and MgO, stable solids of CaC0 3 and MgC0 3 are formed and the formed solids are mixed with the slag particles.
  • the stabilized slags 48 are released from the system which could be directly used as construction materials.
  • the collected suspension 28 from the sedimentation separator 2 could be partially removed from the system, which could be further regenerated for reuse.
  • the main part of the collected suspension 28, and the underflow 36 from the hydrocyclone system 3 rich in enzyme particles could be recirculated into the absorption system. They are pumped back to the absorption solution makeup system 7.
  • Some advantages of this process are improving recovery of biocatalyst particles and providing separation apparatuses that are quite simple and easy in maintenance as compared to other separation technologies such as centrifuges and membranes.
  • Fig. 2 is a process flow diagram for an iron and steel slag stabilization and C0 2 capture using biocatalysts of free enzymes and/or immobilized enzymes on particles and alkaline carbonate salt solutions recycled from the slag stabilization system.
  • the biocatalysts are separated by a membrane filter system before sending the ion loaded solution to the slag stabilization process, and the recovered free enzymes or the immobilized biocatalysts are recirculated into the C0 2 capture system.
  • Fig. 2 is a process flow diagram for an iron and steel slag stabilization and C0 2 capture using biocatalysts of free enzymes and/or immobilized enzymes on particles and alkaline carbonate salt solutions recycled from the slag stabilization system.
  • the biocatalysts are separated by a membrane filter system before sending the ion loaded solution to the slag stabilization process, and the recovered free enzymes or the immobilized biocatalysts are
  • a membrane filter 8 which may be part of an ultrafiltration or microfiltration system, preferably ultrafiltration for the free enzymes and ultra- or microfiltration that are capable of removing fine particles from the system for the immobilized particles.
  • the permeate 84 rich in sodium bicarbonate is sent to the slag stabilization system 4. After contacting and reacting with the ground slag particles 44 rich in active CaO and MgO, stable solids of CaC0 3 and MgC0 3 are formed and the formed solids are mixed with the stabilized slag particles 48.
  • the liquid phase rich in sodium carbonate formed from the stabilization system 4 is collected in the reservoir tank 5. Some precipitates may be formed in the tank 5, due to settling of possible leached CaC0 3 , MgC0 3 and slag particles from the system, which could be removed as discharge 56 from the system.
  • a stream of carbonate and water 54 is pumped to the absorption solution makeup system 7, where after being mixed with the clear aqueous solution, they are added as aqueous absorption solution 18 into the absorber 1.
  • Some aggregates and heavier particles from the absorption system 1 are precipitated and collected at the bottom of the sedimentation separator 2, which can be partially removed from the system 28.
  • the main part of the collected suspension 28, and the retentate 86 from the membrane filtration system are combined and pumped back to the absorption solution makeup system 7, via stream 74.
  • Fig. 3 is a process diagram as system for stabilization of an iron and steel slag through leaching of the active components from the slag and CO2 capture and sequestration using biocatalysts in the C0 2 capture system.
  • the leached active components mainly calcium hydroxide
  • the leached active components may react with the bicarbonate ions from the biocatalyst enhanced CO2 capture process to form an industrial applicable product 66, which can be separated from the system.
  • Fig. 3 there is shown an implementation using water 42 to leach the active components from the slag 44 in a slag stabilization system 4. Due to much lower (e.g. more than hundred times lower) solubility of the Mg(OH) 2 formed in the slag stabilization system 4 during the water leaching process, calcium hydroxide (Ca(OH) 2 ) would be the main component in the stream 47, which is then collected in a reservoir tank 5. Ca(OH) 2 / Mg(OH) 2 stream 64 can be pumped from the tank 5 into a reactor 6 to react with the solution 62 rich in bicarbonate ions to form calcium carbonate (and some magnesium carbonate) 66 that can be separated and collected as a product for some specific industrial applications.
  • Ca(OH) 2 / Mg(OH) 2 stream 64 can be pumped from the tank 5 into a reactor 6 to react with the solution 62 rich in bicarbonate ions to form calcium carbonate (and some magnesium carbonate) 66 that can be separated and collected as a product for some specific industrial
  • the alkaline liquor stream 68 rich in Na 2 C0 3 is pumped from the reactor 6 back to an absorption solution makeup tank 7, and used as the C0 2 capture aqueous absorption solution after mixing with an absorbent solution 72 and the recycled stream of the collected suspension 28 from the sedimentation separator 2 and the underflow 36 from the hydrocyclone system 3.
  • FIG.4 A continuous operation is illustrated on Fig.4 showing a process diagram with a roller conveyor 11 for the ground slag 44 continuous transportation while a spray system 25 for water and absorption solution spraying to stabilize the slag, collect and recycle the leached alkaline liquors 46 for C0 2 offgas capture use.
  • the proposed system could be used either for the slag stabilization and C0 2 capture and sequestration purpose (Fig.4) and/or to recycle the precipitated CaC0 3 solids as a product (Fig.5) for some specific industrial applications.
  • the finely ground slag 44 is continuously transported to a conveyor system 11 where proper containers are provided to collect the ground slag particles.
  • water 42 and the bicarbonate solution (HCO37H2O) 62 is sprayed through a spray injector 25 to leach active minerals from the fine ground slag and do the reaction between the minerals and bicarbonate ions.
  • the chain rolling speed could be adjusted to allow for a proper leaching time and the best stabilization of the slag.
  • the stabilized slag particles and the leached liquors are dropped into a collection system 4, where a Na 2 CO3/H 2 O stream 46 is separated and collected in the bottom, which could be used for CO 2 capture use 74.
  • the stabilized slag 48 could be directly used as construction materials or other purposes.
  • Fig. 5 shows another implementation process of continuously stabilizing the ground slag and recycling the leached minerals as precipitates which can be separated and utilized for some specific applications.
  • H 2 O 42 is sprayed on the fine ground slag through a spray injector 27.
  • a stream 47 of Ca(OH) 2 / Mg(OH) 2 is separated from the stabilized slag collection system 4 and pumped into a reactor 6 to react with stream 62 rich of bicarbonate ions formed from the CO 2 biocatalyst enhanced capture process.
  • precipitates of calcium carbonate (and magnesium carbonate) are produced 66, which can be separated and collected at the bottom of the reactor 6 as a product.
  • the liquid phase 68 from the reactor 6 with rich of Na 2 CO 3 is pumped back to the absorption solution makeup tank 7, and used as the CO 2 capture aqueous absorption solution after being mixed with the absorbent solution 72 and the recycled stream of the collected suspension 28 from the sedimentation separator 2 and the underflow 36 from the hydrocyclone system 3.
  • All the processes can be operated in ambient temperature and the captured CO2 from steelmaking off gas and/or other industrial flue gases could safely and permanently be stored in the form of stable carbonate minerals (CaC0 3 or MgCOs).
  • the present invention may relate to a process for stabilizing slags by injecting a C0 2 gas stream and water into a ground slag stabilization system.
  • the C0 2 gas stream may be produced from desorption of an ion-rich solution including bicarbonate ions.
  • the desorption may be performed in presence of an enzyme, such as carbonic anhydrase or analogues thereof.
  • the ion-rich solution may be derived from an enzymatic CO 2 capture system.
  • the stabilized slag product can be used directly as building and construction materials, and may have better sustainable properties. This will reduce or eliminate slag storage time and space requirements.

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Abstract

L'invention concerne des procédés et des modes de réalisation pour stabiliser un laitier granulé produit à partir d'une opération d'élaboration de l'acier. Éventuellement, un gaz contenant du CO2peut être mis en contact avec une solution d'absorption aqueuse en présence d'un biocatalyseur, dans un réacteur, afin de déclencher une catalyse enzymatique d'une réaction d'hydratation de CO2 dissous dans des ions bicarbonates et dans des ions hydrogènes pour produire une solution chargées en ions et un gaz pauvre en CO2. La solution chargée en ions est ensuite mise en contact avec le laitier granulé pour produire du CaCO3, du MgCO3, un laitier stabilisé appauvri en CaO et en MgO, et une liqueur alcaline comprenant des ions carbonates CO3 2-. En variante, le laitier granulé peut être mis en contact avec de l'eau pour lixivier le CaO et le MgO, et produire une boue contenant du Ca(OH)2 et du Mg(OH)2, laquelle est mise en contact avec la solution chargée en ions afin de produire du CaCO3 et du MgCO3 et le laitier stabilisé appauvri en CaO et MgO.
PCT/CA2013/050514 2012-07-03 2013-07-03 Stabilisation de laitier à l'aide de dioxyde de carbone capturé WO2014005227A1 (fr)

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CN106999842A (zh) * 2014-08-27 2017-08-01 二氧化碳处理公司 使用加氨热弧菌碳酸酐酶的co2捕获方法
WO2018081308A1 (fr) * 2016-10-26 2018-05-03 The Regents Of The University Of California Produit en béton recyclé co2-négatif destiné à être utilisé dans la construction
WO2018081310A1 (fr) * 2016-10-26 2018-05-03 The Regents Of The University Of California Intégration efficace de la fabrication d'un produit à base de béton de recyclage valorisé dans des centrales électriques
US10287652B2 (en) * 2015-03-23 2019-05-14 Nisshin Steel Co., Ltd. Method for recovering calcium-containing solid component from steelmaking slag and recovered solid component
TWI660051B (zh) * 2017-09-01 2019-05-21 經濟部水利署國立成功大學水工試驗所 轉爐石碳酸化裝置
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US11820710B2 (en) 2017-08-14 2023-11-21 The Regents Of The University Of California Mitigation of alkali-silica reaction in concrete using readily-soluble chemical additives
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US11919775B2 (en) 2017-06-30 2024-03-05 The Regents Of The University Of California CO 2 mineralization in produced and industrial effluent water by pH-swing carbonation
US12157709B2 (en) 2022-04-12 2024-12-03 Carbonbuilt, Inc. Process for production of hydraulic-carbonating binder systems through mechanochemical activation of minerals
US12203184B2 (en) 2022-07-18 2025-01-21 The Regents Of The University Of California Multi-chambered electrochemical cell for carbon dioxide removal
US12247303B2 (en) 2023-01-31 2025-03-11 The Regents Of The University Of California Oxygen-selective anodes
US12246993B2 (en) 2022-02-21 2025-03-11 Carbonbuilt Methods and systems for biomass-derived CO2 sequestration in concretes and aggregates
WO2025127739A1 (fr) * 2023-12-15 2025-06-19 포스코홀딩스 주식회사 Appareil de carbonatation minérale continue à base de carbonatation directe et procédé de carbonatation minérale continue l'utilisant
US12351527B2 (en) 2021-10-18 2025-07-08 The Regents Of The University Of California Integration of direct air capture system into CO2 mineralization process of concretes and aggregates

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US10287652B2 (en) * 2015-03-23 2019-05-14 Nisshin Steel Co., Ltd. Method for recovering calcium-containing solid component from steelmaking slag and recovered solid component
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WO2018081310A1 (fr) * 2016-10-26 2018-05-03 The Regents Of The University Of California Intégration efficace de la fabrication d'un produit à base de béton de recyclage valorisé dans des centrales électriques
EP3532445A4 (fr) * 2016-10-26 2020-06-17 The Regents of The University of California Intégration efficace de la fabrication d'un produit à base de béton de recyclage valorisé dans des centrales électriques
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US12351527B2 (en) 2021-10-18 2025-07-08 The Regents Of The University Of California Integration of direct air capture system into CO2 mineralization process of concretes and aggregates
US12246993B2 (en) 2022-02-21 2025-03-11 Carbonbuilt Methods and systems for biomass-derived CO2 sequestration in concretes and aggregates
CN114835465A (zh) * 2022-04-07 2022-08-02 太原理工大学 一种利用循环流化床粉煤灰改善生物水泥胶结砂土的方法
US12157709B2 (en) 2022-04-12 2024-12-03 Carbonbuilt, Inc. Process for production of hydraulic-carbonating binder systems through mechanochemical activation of minerals
US12203184B2 (en) 2022-07-18 2025-01-21 The Regents Of The University Of California Multi-chambered electrochemical cell for carbon dioxide removal
US12247303B2 (en) 2023-01-31 2025-03-11 The Regents Of The University Of California Oxygen-selective anodes
CN116283141A (zh) * 2023-03-03 2023-06-23 湖北工业大学 一种多固废协同高效吸附二氧化碳的透水混凝土及制备方法
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