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WO2011145080A1 - Procédé pour la production d'hydrogène, la séquestration de dioxyde de carbone et la production de matériaux de construction à partir de laitiers et/ou de cendres industrielles - Google Patents

Procédé pour la production d'hydrogène, la séquestration de dioxyde de carbone et la production de matériaux de construction à partir de laitiers et/ou de cendres industrielles Download PDF

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Publication number
WO2011145080A1
WO2011145080A1 PCT/IB2011/052217 IB2011052217W WO2011145080A1 WO 2011145080 A1 WO2011145080 A1 WO 2011145080A1 IB 2011052217 W IB2011052217 W IB 2011052217W WO 2011145080 A1 WO2011145080 A1 WO 2011145080A1
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Prior art keywords
phase
slags
ashes
acid
process according
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Ceased
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PCT/IB2011/052217
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English (en)
Inventor
Paolo Plescia
Enrico Barbarese
Maurizio Pinna
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Asiu SpA
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Asiu SpA
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Priority to EP11729711A priority Critical patent/EP2571805A1/fr
Publication of WO2011145080A1 publication Critical patent/WO2011145080A1/fr
Anticipated expiration legal-status Critical
Ceased legal-status Critical Current

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    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B3/00—Hydrogen; Gaseous mixtures containing hydrogen; Separation of hydrogen from mixtures containing it; Purification of hydrogen
    • C01B3/02—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen
    • C01B3/06—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of inorganic compounds containing electro-positively bound hydrogen, e.g. water, acids, bases, ammonia, with inorganic reducing agents
    • 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
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B3/00—Hydrogen; Gaseous mixtures containing hydrogen; Separation of hydrogen from mixtures containing it; Purification of hydrogen
    • C01B3/02—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen
    • C01B3/04—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by decomposition of inorganic compounds, e.g. ammonia
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B3/00—Hydrogen; Gaseous mixtures containing hydrogen; Separation of hydrogen from mixtures containing it; Purification of hydrogen
    • C01B3/02—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen
    • C01B3/06—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of inorganic compounds containing electro-positively bound hydrogen, e.g. water, acids, bases, ammonia, with inorganic reducing agents
    • C01B3/061—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of inorganic compounds containing electro-positively bound hydrogen, e.g. water, acids, bases, ammonia, with inorganic reducing agents by reaction of metal oxides with water
    • 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
    • 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
    • C04B28/00—Compositions of mortars, concrete or artificial stone, containing inorganic binders or the reaction product of an inorganic and an organic binder, e.g. polycarboxylate cements
    • C04B28/02—Compositions of mortars, concrete or artificial stone, containing inorganic binders or the reaction product of an inorganic and an organic binder, e.g. polycarboxylate cements containing hydraulic cements other than calcium sulfates
    • 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
    • C04B7/00—Hydraulic cements
    • C04B7/14—Cements containing slag
    • C04B7/147—Metallurgical slag
    • C04B7/153—Mixtures thereof with other inorganic cementitious materials or other activators
    • C04B7/17—Mixtures thereof with other inorganic cementitious materials or other activators with calcium oxide containing activators
    • 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
    • C22B7/02—Working-up flue dust
    • 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
    • B01D2251/30—Alkali metal compounds
    • B01D2251/304—Alkali metal compounds of sodium
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2251/00—Reactants
    • B01D2251/30—Alkali metal compounds
    • B01D2251/306—Alkali metal compounds of potassium
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2251/00—Reactants
    • B01D2251/40—Alkaline earth metal or magnesium compounds
    • B01D2251/402—Alkaline earth metal or magnesium compounds of magnesium
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2251/00—Reactants
    • B01D2251/40—Alkaline earth metal or magnesium compounds
    • B01D2251/404—Alkaline earth metal or magnesium compounds of calcium
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2251/00—Reactants
    • B01D2251/60—Inorganic bases or salts
    • B01D2251/602—Oxides
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2251/00—Reactants
    • B01D2251/60—Inorganic bases or salts
    • B01D2251/604—Hydroxides
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2257/00—Components to be removed
    • B01D2257/50—Carbon oxides
    • B01D2257/504—Carbon dioxide
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2258/00—Sources of waste gases
    • B01D2258/06—Polluted air
    • 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
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/30—Hydrogen technology
    • Y02E60/36—Hydrogen production from non-carbon containing sources, e.g. by water electrolysis
    • 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
    • Y02P30/00—Technologies relating to oil refining and petrochemical industry
    • 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
    • Y02P40/00—Technologies relating to the processing of minerals
    • Y02P40/10—Production of cement, e.g. improving or optimising the production methods; Cement grinding
    • 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
    • Y02P40/00—Technologies relating to the processing of minerals
    • Y02P40/10—Production of cement, e.g. improving or optimising the production methods; Cement grinding
    • Y02P40/18—Carbon capture and storage [CCS]
    • 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 refers to a process for the production of hydrogen and the sequestration of carbon dioxide starting from slags and/or industrial ashes (such as steelworks waste, incineration waste, energy production processes waste), in which said slags and/or ashes result, preferably, from blast furnace iron metallurgy, from oxygen converters and/or electric furnaces, from incineration (for example, from grill furnaces, fluidized bed furnaces, plasma furnaces) , from pyrolysis and gasification plants, from energy production facilities, from fossil fuels and from biomasses, as also from all the dusts (from now on called “light dusts”) and the light ashes (from now on called “fly ashes”) that are generated in said processes.
  • slags and/or industrial ashes such as steelworks waste, incineration waste, energy production processes waste
  • slags and/or ashes result, preferably, from blast furnace iron metallurgy, from oxygen converters and/or electric furnaces, from incineration (for example, from grill furnace
  • the process of the invention allows to produce a gas substantially composed of hydrogen and, at the same time, allows to prepare materials having the characteristics of being avid sequestrants of carbon dioxide (C0 2 ) and of being advantageously usable as inert materials for preparing hydraulic mixtures with lime and/or cement.
  • the present invention refers to a process for the production of hydrogen (and therefore, of energy) and the sequestration of carbon dioxide (of any origin and/or provenance) , and also for the eventual preparation and/or recovery of inert materials of any type to be employed in the production of hydraulic mortars and/or concretes, using iron metallurgy slags and/or ashes, thermodestruction slags and/or ashes and any other type of industrial solid slag having a composition similar to the mentioned ones.
  • the slags resulting from the metallurgy industry are one of the most popular waste matters in the industrialized countries and they have been used/recycled in the building industry for over a hundred years. Just as a way of example, for each cast iron and steel ton produced, 200 to 400 kg of slag are produced. These materials have substantially a silicon calcium or ferro calcium composition, but there exist also materials that are richer in magnesium or in other elements and/or in highly toxic metallic waste. Due to the rigid European and national regulations, the slags are now subjected to rigid controls and to specific rules about their recovery/recycle, mainly created for the preparation of inert materials for road foundations, cement mixtures and other products with cement.
  • a further Italian patent application, IT2008CO0003 extends such a concept of recovery of the slags to their use as road inerts, but does not introduce any material change with respect to the technology already described in the preceding documents.
  • the authors of the present invention know that neither the patents mentioned above nor the other documents of the background art related to the use of slags for the production of inert or mixed materials or of catalyzed hydraulic mortars, are contemporaneously aimed also at the production of energy, preferably, at the production of hydrogen, and at the contemporaneous sequestration of carbon dioxide, of any origin and/or provenance .
  • patent US2009220410 Al uses the slags only at high temperature, that is at temperatures higher than 1500 °C, at which the water molecule turns into hydrogen and oxygen and the presence of reducing agents like carbon and/or metallic iron does not permit the recombination of such gases.
  • thermodestruction slags since they are formed at too low temperatures (on average comprised between 900 °C and 1200 °C) to be able to resolve the water molecule.
  • the carbon dioxide sequestered can derive from any source, for example from air and/or from any industrial process that produces it, including the extraction of gas and/or of liquids from the subsurface. Nevertheless, in these cases the documents of the background art just limit themselves to describe possible uses of the slags just as sequestering materials, without mentioning or much less making reference to other possible uses of them that are concurrent and/or combined.
  • the applicant has now unexpectedly found that, by appropriately treating in an appropriate acidic environment and then in an appropriate basic environment and at non-high temperatures slags and/or industrial ashes, it is possible to give an adequate answer to the problem generated by the above-mentioned technical need. It is therefore the aim of the present invention to provide a process for the production of hydrogen and the sequestration of carbon dioxide by means of at least one treatment in an acidic environment of slags and/or industrial ashes and/or a mixture thereof, followed by at least one treatment in a basic environment of the activated products resulting from the preceding acid treatment mentioned above, as per the attached independent claim.
  • Attached Figure 1 illustrates, by means of a scheme, a particularly preferred embodiment (and omni comprehensive) of the process according to the present invention, as well as of the possible type of plant preferably usable for carrying out said process.
  • the container (s) for example, silos
  • the leaching reactor/tank of waste with acid pH block (B) of the scheme) , where hydrogen gas is substantially generated
  • the leaching reactor/tank of waste at basic pH and in the presence of C0 2 block (C) of the scheme) , where hydrogen gas is generated and C0 2 is sequestered
  • the carbonation site/tank (block (D) of the scheme) where the carbonation of the exhausted scoriaceous waste is completed after the basic treatment
  • the mixing site/tank of all the different inert materials with cement and/or lime and/or additives and/or a mixture thereof block (E) of the scheme) , where
  • the present invention refers to a process for the production of hydrogen - and the sequestration, contemporaneous and/or combined, of carbon dioxide starting from slags and/or industrial ashes, comprising: at least one phase b) , preceding the following phase c) , of acidic leaching/maturation, in which said slags and/or industrial ashes and/or a mixture thereof are subjected, in a sealed reaction environment, to a treatment in an acid solution having a pH ⁇ 3,5, during which a gas substantially composed of hydrogen is produced and from the slags and/or ashes the hazardous metals are extracted under the form of soluble salts of nitrogen and/or sulphur, and/or chlorine and/or phosphorus and/or fluorine and/or acetic acid; and
  • phase c) following the above phase b) , of alkaline leaching/maturation, in which the slags and/or industrial ashes and/or preferably, a mixture thereof previously treated in above phase b) are subjected, in an appropriate sealed reaction environment and in the presence of C0 2 , to a treatment in an alkaline solution having a pH > 8, during which a gas substantially composed of hydrogen is produced and the CO 2 present/added in the environment is sequestered.
  • Said slags and/or industrial ashes comprise, preferably: steelworks slags, both from blast furnaces and electric furnaces, and/.or slags from oxygen converters, and/or light dusts and/or ashes from iron metallurgy and/or other slags and/or solid waste from iron, aluminum and non-ferrous metals iron metallurgy and/or bottom ashes and/or filter ashes from thermal plants, from incineration of special and/or urban waste and/or from thermal and/or pyrolysis plants and/or from gasification and/or from energy production facilities and/or fossil fuels and/or from biomasses.
  • said slags/industrial ashes are preferably, but anyway not exclusively, selected from the group comprising:
  • heavy and/or light slags from carbon and/or liquid fuels (or both) thermal or electric power plants comprised ashes from biomasses ;
  • the acid solution in said phase b) , has preferably a pH ⁇ 3, more preferably ⁇ 2,5, even more preferably ⁇ 2, even more preferably ⁇ 1,5. Further, in said phase b) , the acid solution contains an effective amount of at least one acid, preferably selected from: nitric acid and/or sulphuric acid and/or acetic acid and/or hydrochloric acid and/or phosphoric acid and/or hydrofluoric acid and/or aqua regia or a mixture thereof.
  • the reaction environment comprises at least one closed container/tank equipped with at least feeding means of said slags and/or ashes and/or, preferably, of a mixture thereof, agitation and control means, feeding means of the acid solution, extraction means of the generated gas, extraction means of the treated/exhausted material, extraction means of the resulting acid solution at the end of the treatment.
  • the C0 2 is added to the reaction environment by bubbling it, under the form of gas (for example, as such or as industrial gaseous waste that contains it) , in said alkaline solution or by bubbling air into said solution.
  • the alkaline solution has preferably a pH ⁇ 9, more preferably ⁇ 9,5, even more preferably ⁇ 10,5, even more preferably ⁇ 11,5.
  • the alkaline solution contains an effective amount of a least one alkali metal or alkaline earth metal oxide or hydroxide, preferably selected from the group comprising: NaO, K 2 0, CaO, MgO, NaOH, KOH, Mg (OH) 2 , Ca (OH) 2 ⁇
  • the reaction environment comprises at least one closed container/tank equipped with at least feeding means of said slags and/or ashes and/or, preferably, a mixture thereof, agitation and control means, CO 2 and/or air feeding means, feeding means of the alkaline solution, extraction means of the generated gas, extraction means of the treated/exhausted material, extraction means of the resulting alkaline solution at the end of the treatment.
  • the process of the invention further comprising:
  • phase d) following the phase c) above, in which the exhausted material resulting from said phase c) , is subjected to exhaustive carbonation, preferably in a sealed environment containing C0 2 , or also by exposing it to open air; said phase d) is followed by a phase e) , in which said exhaustively carbonated material resulting from said phase d) is mixed with an effective amount of inert materials and/or aggregates and with an effective amount of cement and/or lime and/or additives and/or a mixture thereof to give a final inert and non-toxic mixture advantageously usable for producing the inert, neutral and environmentally compatible products usable in the building industry.
  • the C0 2 can, for example, be taken from the atmosphere or from industrial gaseous wastes that contain it, for example, those originated from thermal plants, as well as the C0 2 /CO recovered from the mixture of the gases emitted from the basic leaching tank during the phase c) above.
  • the inert materials and/or aggregates are preferably selected from the group comprising: inerts from quarry and/or demolition and/or building debris and/or plastic inerts, such as PVC (polyvinyl chloride) and/or HOPE (high density polyethylene) granules and/or other plastics, for example, high density ones, including, among them, pellets resulting from the recovery of tires for cars, inerts obtained by crushing the discharged and classified as non-hazardous railway ballast, inerts from the process of scarification of road asphalts and inerts from the pelletizing of light dusts from the abatement of non- hazardous smokes and sludges.
  • PVC polyvinyl chloride
  • HOPE high density polyethylene
  • said inert non-toxic mixture usable for advantageously producing building products can be packaged and appropriately stored, in stand-by to be used, also for long periods of time, or is transported as such directly to the application site and added with the necessary amount of water, preferably at the time of use, to give the desired product for the building industry.
  • the process of the invention comprises, in sequence, the following phases :
  • the process of the invention comprises also one first phase a) in which the slags and/or ashes, previously treated, purified, grinded, selected by type and granulometry, are measured out and mixed together before being subjected to the subsequent treatments. Therefore, in this case, the process of the invention comprises, in sequence, the following phases: one first phase a) , according to what has been described before and further exemplified in what follows of the description;
  • the mixtures of scoriaceous materials can be constituted by slags of different origin (as already described above) and/or composition and/or property.
  • said slags contain, among others: silicon, calcium, magnesium, iron oxides and oxides of other metals, transition metals to the zero-valence or combined status and/or alkali and/or alkaline earth metals.
  • said slags show reactivity from pH 4,5 upwards, granulometric values comprised between 0 and 80 mm, preferably between 0 and 60 mm, more preferably between 0 and 40 mm, even more preferably between 0 and 30 mm.
  • the flying ashes can be constituted by calcium, magnesium, sodium, potassium silicates, metal oxides; further, they can contain metals in combined or zero-valence form, unburnt fractions and chlorine / sulphur, fluorine, nitrate salts and complex salts.
  • the different raw materials used in the process of the invention are substantially selected from the group comprising :
  • alkali and/or alkaline earth metal oxides or hydroxides in concentrations between 0,1 and 5 M, preferably between 0,1 and 3,5 , more preferably between 0,2 and 2 M; and/or
  • inert materials and/or aggregates which can derive from quarries (natural ones) or from demolition and building.
  • inert materials include the PVC (polyvinyl chloride) , HDPE (high density polyethylene) granules or other plastics, preferably high density ones, including the granules resulting from the recovery of tires for cars. Description on a particularly preferred embodiment of the process of the invention
  • the various materials are pre-treated, grinded, purified from useless or toxic waste, riddled and selected/subdivided by type and granulometry and stored in silos or tanks or deposits ad hoc or in another suitable protected environment to avoid, for example, the dispersion of the light dusts in the atmosphere and undesired reactivity (block (A) of the scheme of Figure 1) .
  • Slags and ashes are therefore measured out, with appropriate measurement systems known in the background art, on transporter tapes towards a first mixing apparatus.
  • Said mixing apparatus mixes the various components and feeds them in the acidic leaching/maturation tank ( s ) /reactor ( s ) (block (B) of the scheme of Figure 1) containing an acid solution, preferably with pH ⁇ 2.
  • Such tank(s) constitute ( s) the first reaction environment where the water reduction reaction takes place with relative emission of hydrogen and where the heavy metals present in the slags are contemporaneously solubilized and/or inertized.
  • the tank(s) is (are) provided with an hermetic closure to capture the gas produced, substantially hydrogen-based, avoiding its dispersion in a hazardous way in the atmosphere.
  • Such a gas is directed towards a cleaning and filtering circuit to be then stored and/or optimized in an ordinary energy recovery plant.
  • the scoriaceous material treated is directed towards one (or also more) basic maturation/leaching tank/reactor (a so-called “still pool”; schematized in block (C) of the scheme of Figure 1) where it is treated under agitation with high pH solutions, preferably ⁇ 11,5.
  • high pH solutions preferably ⁇ 11,5.
  • the residue soluble metallic phases inside the slags are first neutralized and then become insoluble hydroxides. Also in this phase significant emissions of hydrogen are generated, which are also directed towards the purification circuit and to the storage/use.
  • carbon dioxide (C0 2 ) is also let in/pumped/bubbled in the basic solution (for example, taken from the atmosphere or from industrial gaseous wastes, as those generated from thermal plants) , which is captured by the complex alkaline hydroxides of the slags, and fixed as carbonates.
  • the basic leaching liquid is then directed to a recovery circuit, where the insoluble sludges are separated, and the alkaline hydroxides are regenerated.
  • the leaching/maturation tanks are closed so that the hydrogen is not dispersed in the external environment, are preferably provided with a rotor that carries out the mixture and the agitation of the solid material and are also provided with appropriate control means, for example of the temperature and of the pH of the solutions employed.
  • the gases generated by the chemical actions that are carried outside the reaction tanks are analysed continuously to verify the rate of hydrogen and in other eventual fuel gases and in residue carbon dioxide.
  • the gas flow contains from 5 ppm to 40% in volume, preferably, from 10 ppm to 30% in volume, more preferably, from 20 ppm to 25% in volume, of hydrogen and other fuel gases and, after appropriate purification with methods and devices known in the background art, is directed to an idoneous collection and use system, while the CO 2 /CO in excess is separated from the hydrogen and from the other gases usable and recycled into the stilling pool (block (C) of the scheme of Figure 1) or, preferably, recycled in the carbonation tank (block (D) of the scheme of Figure 1) as described below.
  • a traditional screw system carries away the washed and exhausted material, now inert and non-toxic, from the basic maturation tank(s) towards an appropriate storage site where said material will wait to become, for example, part of a concrete or of an hydraulic mortar.
  • Said storage of said exhausted, inert and non-toxic material takes place preferably in an appropriate carbonation tank (block (D) of the scheme of Figure 1) or also into open air, for an appropriate period of time sufficient to complete the carbonation process.
  • the verification of the exhaustion of the carbonation process is carried out by means of the use of the calcimetry or in XR diffratometry (that is, X-ray) or by means of another known idoneous measurement system of the crystalline phases.
  • the- material when it has to be used, it is for example measured out and loaded on a tape that transports it towards a second mixer (block (E) of the scheme of Figure 1), in which the necessary raw materials, appropriately measured out in the desired percentages on the basis of the type of mixture to produce, are merged: inerts, slags, cement and/or hydrate lime and/or additives in specific amounts.
  • the material thus mixed is downloaded and, if necessary, immediately taken to the application site, where, last, the necessary water will be added, preferably at the time of use.
  • the formation of the carbonates in the mixture does not limit but, on the contrary, enhance the inert function of the slags and also determines a reduction of the risk of swelling of the manufacture due to the subsequent formation of the carbonates, above all of the magnesium ones, at the same time giving the residue lime the possibility of activating the silicates.
  • the acid and basic treatments, preferably combined among them, in the maturation tanks according to the process of the present invention allow to obtain different significant advantages with respect to the technologies already known and commonly in use, such as, for example :
  • the treatment of the slags and/or ashes eliminates the chlorine salts and the other soluble salts, in particular, of the heavy metals, and the organic materials in suspension;
  • the maturation tanks are made of non- reactive materials, such as polypropylene, Teflon, polyethylene, carbon fibre, plastic reinforced by fiber glass.
  • the temperature of the process is maintained at a value not lower than 40°C, preferably, without the use of external energetic sources, due to the exothermicity of the hydration reaction.
  • control systems will be inserted, such as pH and measurement systems, and inlet means of the reagents and of the initial or recycles gases and of extraction of the gases generated and of the materials treated and of the exhausted solutions.
  • the hydration water, including washing salts, will be recovered and treated in an appropriate water treatment plant.
  • silos (A) for piling up the slags and the light dusts (block (A) of the scheme of Figure 1) preferably provided with weights and with extraction systems, preferably remote controlled for measuring out the components; transporter tape(s) that carry the measured components towards a hopper;
  • a closed acid leaching tank (B) (block (B) of the scheme of Figure 1), with water having an acid pH, as described before, where the product reacts with the acid solution, produces hydrogen and dissolves into the solution most of the metals soluble and available from the scoriaceous product; from the tank itself (B) the reaction gases rich in hydrogen are extracted and directed towards filtering, storage and/or immediate use systems to produce energy; moreover, from the same tank (B) the exhausted leaching liquid is then pumped and taken to a water treatment plant, where the metal salts are extracted and the liquid is regenerated at the right acidity, and is afterwards re-fed in the tank (B) ;
  • a closed alkaline leaching tank (C) (block (C) of the scheme of Figure 1), with water having an alkaline pH, as described before, where the slag resulting from (B) undergoes a second chemical attack that causes the activation thereof; in fact, from the same tank (C) the reaction gases rich in hydrogen are extracted, while the slag sequestrates the C0 2 fed into the reaction environment; then, from the tank (C) the material is extracted with screws or countercurrent tapes and downloaded in a third closed tank (D) (block (D) of the scheme of Figure 1) , into which a gas enriched in carbon dioxide, or atmospheric air (with carbon dioxide) , or industrial gaseous wastes, are fed, including, preferably, the portion of CO 2 /CO recovered from the mixture of gases emitted from tank (C) during the basic treatment, and in which the carbonation process of the exhausted slags is appropriately completed (it is reminded that, as described before, in another embodiment of the invention, said exhausted carbonation process can also be carried out by
  • thermodestruction slag mobile grill furnace
  • quarted and sorted under the 3 mm An amount of about 100 g of thermodestruction slag (mobile grill furnace) , quarted and sorted under the 3 mm, has been put in contact with a solution of Ca(OH) 2 0,5 , in an amount of 250 cc.
  • the boiling effect results evident and is vividly manifested, providing an amount of hydrogen superior to 10% in volume, determined through the analysis of the evolved gases, by means of gas chromatography.
  • the carbon dioxide is sequestered quickly in the lime solution, with a yield of 0,16 kg/kg of slag.
  • LD blast furnace slag oxygen converter
  • nitric acid nitric acid
  • the relation between LD slag and acid solution is of 500 g/litre.
  • hydrogen gas is observed, in an amount comprised between 15% and 25% of the volume of the gases emitted, together with carbon dioxide and traces of carbon monoxide.
  • the analysis performed in XR fluorescence of the final content of metals in the LD slag treated shows a consistent reduction of chrome, nickel and vanadium that have been solubilized.
  • the residue of slag obtained after the treatment described in the preceding Example 5 is recovered, again placed in another calibrated flask and added of a solution 1M of NaOH in a ratio of 100 cc/g of slag waste.
  • the subsequent elaboration is the same as the one described in the preceding Example 1.
  • the system has produced a total flow of about 0,04 litres of hydrogen (0,4 1/kg of slag) determined through the gas chromatographic analysis of the evolved gases, with an average yield of around 120 ppm of 3 ⁇ 4.
  • the carbon dioxide has been sequestered with a yield of about 0,29 kg/kg of slag .
  • the leached/exhausted slag obtained after the treatment described in the preceding Example 6 is recovered, washed in water having a neutral pH and riddled so as to select the fraction comprised between 2 and 30 mm.
  • the product of the riddling is mixed with inerts from quarry, in turn riddled so as to provide an overall granulometric curve compliant to the prescriptions of Rule UNI8520.
  • the mixture is weighed and mixed with cement 325.
  • the mixture is poured into the moulds, subjected to vibration to eliminate the air bubbles and therefore placed in maturation for 24 hours into open air, and, immediately afterwards, in a maturation tank.
  • Such a mixture has given a Ck resistance equal to 230 Mpa after four days of maturation and has resulted perfectly suitable for the production of high resistance cement mixtures for road uses.

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Abstract

La présente invention porte sur un procédé pour la production d'hydrogène et la séquestration simultanée de dioxyde de carbone à partir de laitiers et/ou de cendres industrielles. En particulier, ledit procédé permet de produire un gaz essentiellement composé d'hydrogène et, en même temps, il permet de préparer des matériaux ayant les caractéristiques d'être des agents de séquestration de dioxyde de carbone avides et d'être avantageusement utilisables comme matériaux inertes pour la préparation de mélanges hydrauliques avec de la chaux et/ou du ciment.
PCT/IB2011/052217 2010-05-20 2011-05-20 Procédé pour la production d'hydrogène, la séquestration de dioxyde de carbone et la production de matériaux de construction à partir de laitiers et/ou de cendres industrielles Ceased WO2011145080A1 (fr)

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EP11729711A EP2571805A1 (fr) 2010-05-20 2011-05-20 Procédé pour la production d'hydrogène, la séquestration de dioxyde de carbone et la production de matériaux de construction à partir de laitiers et/ou de cendres industrielles

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ITPI2010A000058A IT1400139B1 (it) 2010-05-20 2010-05-20 Un procedimento per la produzione di idrogeno, per il sequestro di anidride carbonica e per la produzione di materiali da costruzione a partire da scorie e/o ceneri industriali.
ITPI2010A000058 2010-05-20

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ES2577078A1 (es) * 2015-01-12 2016-07-12 Raúl HERNANDO GARCÍA Tratamiento ácido de cenizas volantes de la incineración de RSU con recuperación de óxido de cal
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US10843935B2 (en) 2016-06-06 2020-11-24 Centre National De La Recherche Scientifique Method for producing nanomagnetite
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GB2613875A (en) * 2021-12-17 2023-06-21 Plastic Energy Ltd A method for the production of concrete
CN116768536A (zh) * 2022-03-16 2023-09-19 地聚合物解决方案有限责任公司 由金属采矿和生产废物制备冷熔混凝土和水泥组合物的方法
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US20170217770A1 (en) * 2013-03-29 2017-08-03 Centre National De La Recherche Scientifique Method for Producing High-Purity Hydrogen Gas and/or Nanomagnetite
US10899610B2 (en) * 2013-03-29 2021-01-26 Centre National De La Recherche Scientifique Method for producing high-purity hydrogen gas and/or nanomagnetite
RU2587165C1 (ru) * 2014-11-25 2016-06-20 Общество с ограниченной ответственностью "Комплексное обслуживание заводов" Способ утилизации пыли отходящих газов металлургического производства
ES2577078A1 (es) * 2015-01-12 2016-07-12 Raúl HERNANDO GARCÍA Tratamiento ácido de cenizas volantes de la incineración de RSU con recuperación de óxido de cal
US10843935B2 (en) 2016-06-06 2020-11-24 Centre National De La Recherche Scientifique Method for producing nanomagnetite
JP2023546286A (ja) * 2020-10-20 2023-11-01 ティケ テック プライベート リミティド 水素の生成のための方法
GB2613875A (en) * 2021-12-17 2023-06-21 Plastic Energy Ltd A method for the production of concrete
WO2023111135A1 (fr) 2021-12-17 2023-06-22 Plastic Energy Limited Procédé de production de béton
GB2613875B (en) * 2021-12-17 2023-12-06 Plastic Energy Ltd A method for the production of concrete
CN116768536A (zh) * 2022-03-16 2023-09-19 地聚合物解决方案有限责任公司 由金属采矿和生产废物制备冷熔混凝土和水泥组合物的方法
CN116768536B (zh) * 2022-03-16 2024-08-27 地聚合物解决方案有限责任公司 由金属采矿和生产废物制备冷熔混凝土和水泥组合物的方法
CN114920245B (zh) * 2022-07-04 2023-10-03 重庆大学 一种用于二氧化碳封存的矿化物及其应用
CN114920245A (zh) * 2022-07-04 2022-08-19 重庆大学 一种用于二氧化碳封存的矿化物及其应用

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