EP4436728A1 - Matériaux adsorbants pour sols minéraux - Google Patents

Matériaux adsorbants pour sols minéraux

Info

Publication number
EP4436728A1
EP4436728A1 EP22822435.8A EP22822435A EP4436728A1 EP 4436728 A1 EP4436728 A1 EP 4436728A1 EP 22822435 A EP22822435 A EP 22822435A EP 4436728 A1 EP4436728 A1 EP 4436728A1
Authority
EP
European Patent Office
Prior art keywords
adsorbent
weight
topsoil
subsoil
soil
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Pending
Application number
EP22822435.8A
Other languages
German (de)
English (en)
Inventor
Jürgen KISCHKEWITZ
Andreas Schlegel
Jan Siemens
Anne Wagner
Martin Kaupenjohann
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Lanxess Deutschland GmbH
Original Assignee
Lanxess Deutschland GmbH
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by Lanxess Deutschland GmbH filed Critical Lanxess Deutschland GmbH
Publication of EP4436728A1 publication Critical patent/EP4436728A1/fr
Pending legal-status Critical Current

Links

Classifications

    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B09—DISPOSAL OF SOLID WASTE; RECLAMATION OF CONTAMINATED SOIL
    • B09C—RECLAMATION OF CONTAMINATED SOIL
    • B09C1/00—Reclamation of contaminated soil

Definitions

  • the present invention relates to adsorbent material containing at least subsoil and at least one adsorbent, mineral soils containing such adsorbent materials, methods for producing such adsorbent materials, methods for producing mineral soils containing such adsorbent materials, the use of adsorbents for producing adsorbent materials and the use of adsorbent materials for Production of mineral soils.
  • Soils are formed on the earth's surface in the overlapping area of atmosphere, lithosphere, hydrosphere and biosphere through the interaction of the soil-forming factors rock, climate, vegetation, flora/fauna, relief, water and man.
  • the expert understands soil as a three-phase system of solid mineral and organic substance and cavities, which are partly filled with water and partly with air.
  • Soils are divided into horizons. Soil horizons are areas within the soil that have uniformly similar characteristics and properties and differ from the areas above or below in one or more characteristics.
  • the top three mineral soil horizons are subdivided as follows: topsoil (A horizon), subsoil (B horizon) and bedrock (C horizon).
  • topsoil A horizon
  • subsoil B horizon
  • bedrock C horizon
  • the expert understands the topsoil as the soil horizon enriched with organic matter, which can usually be distinguished from the underlying subsoil by its dark color and is intensively rooted.
  • topsoil and subsoil of a soil sample can be recognized purely visually and can also be determined quantitatively using special color charts, such as the Munsell Soil Color Charts, based on hue, gray value (value) and color saturation (chroma).
  • color charts such as the Munsell Soil Color Charts, based on hue, gray value (value) and color saturation (chroma).
  • topsoil in contrast to lower-lying soil horizons, contains a high proportion of nutrients (especially nitrogen) and organic matter (humus) as well as a large amount of soil organisms. Aerobic bacteria usually live in the topsoil, while the subsoil contains little or no humus, only little root penetration and hardly any life. As a rule, only the Topsoil processed by arable farming.
  • Topsoil and subsoil are also called mineral soils due to their high proportion of inorganic substances of at least 70 percent by weight. They have a proportion of organic substances of at most 30% by weight. Above the topsoil, especially under forest use, there can be an organic soil horizon that contains more than 30 percent by weight (approx. 90 percent by volume) organic substances. All of the organic matter in the soil minus the roots and soil organisms is called humus. This includes all dead plant and animal matter in and on the ground as well as their organic transformation products. Humus does not represent a uniform soil fraction, but is the sum of different amounts of decomposed organic matter. The amount of organic matter in a soil is usually determined by determining the organic carbon content (Corg content) in the soil.
  • Corg content organic carbon content
  • the humus content ie the content of organic matter
  • the Corg content can be determined using various methods, for example elemental analysis (dry ashing, DIN ISO10964), wet ashing of the organic substance (Lichterfeld method, DIN ISO 19684 Part 2) or determining the loss on ignition (DIN ISO 19684 Part 3). take place.
  • the Corg levels are usually measured in soil that has been dried at over 100 °C.
  • the topsoils usually have a higher biological activity than the subsoils, which leads to a dynamic release of nutrients from the organic matter and the formation of aggregate structures.
  • the subsoils are characterized by a low content of humus and a segregated or coherent structure and can easily be distinguished visually from the topsoils on the basis of these characteristics.
  • the nutrient release occurs mainly in the topsoil through weathering from the minerals.
  • a and B horizons can be divided into further subclasses. According to the invention, the respective subclasses of these horizons are also always included in the A horizon and B horizon.
  • the C horizons of the soils can be solid to loose, calcareous to calcareous and sandy to clayey (texture).
  • Rock strength, lime content and texture are essential for the speed of soil formation and thus determine the thickness of the soil, the pedogenetic horizons and the associated soil properties, such as the soil structure.
  • a horizon, B horizon and C horizon of a specific soil or soil sample by core drilling in different soils by one or more characteristics. These characteristics are, for example, color, color distribution, color intensity, proportion of inorganic substances, proportion of organic substances, degree of root penetration, composition of the main mineral components, aggregation of primary particles, proportion of nutrients (e.g. nitrogen or phosphorus), or proportion and type of soil organisms.
  • characteristics are, for example, color, color distribution, color intensity, proportion of inorganic substances, proportion of organic substances, degree of root penetration, composition of the main mineral components, aggregation of primary particles, proportion of nutrients (e.g. nitrogen or phosphorus), or proportion and type of soil organisms.
  • Terrestrial and semi-terrestrial soils are exposed to external influences that can affect the natural composition and functions of the soil. These include, for example, pollutants that are or have been introduced into the soil through human activity. As pollutants, salts of z. B. heavy metals such. B. Pb, Hg, Cd, Cr, Ni, Cu cations, which are known to have high toxicity.
  • the groundwater has to be cleaned at great expense until it reaches the required level of purity.
  • the water has to be pumped out of the ground, for example, in order to clean it above ground before it can be used or to return it to the water cycle.
  • soil remediation Another method to reduce levels, availability and mobility of pollutants in soil is soil remediation.
  • Various methods for soil remediation are known from the prior art. For example, numerous phytoremediation methods are known which aim to achieve the highest possible absorption of the pollutants by the plant by sowing special fast-growing plants, even before the ions can be washed out into the groundwater. The plants are then harvested, thermally utilized and the pollutants remain fixed in the ash.
  • the mobility of the pollutants mentioned can be reduced by mixing various adsorptive substances into the soil close to the surface, which has been experimentally tested and described.
  • WO2005/014492 describes a method for soil or groundwater remediation using spherical, porous particles of zero-valent iron. However, no specific information is given here on the type of soil, the type of mixture with the soil and the adsorbing properties of these zero-valent iron particles.
  • EP1318103A2 describes iron particles, which have a metallic ⁇ -Fe phase and a proportion of magnetic FeC, for cleaning contaminated soil or groundwater. These iron particles are made from goethite (a-FeOOH) by partial reduction. However, no specific information on the type of soil, the type of mixture with the soil is described here. The production of these iron particles is very complex and therefore not economically feasible for the use of large quantities.
  • magnetites generated in situ in soils by chemical reaction of soluble iron salts with caustic soda are produced as reactive barriers, for example around tanks that are filled with pollutants and have leaks. Substances contained therein are thus bound. Due to the handling of aggressive chemicals, this method is only possible with great effort and with high safety precautions and is therefore prohibited in soils, for example arable land, on which plants grow.
  • CN107501012A1 describes a mixture of 20 to 30 parts attapulgite powder, 10 to 20 parts sodium pyrophosphate, 30 to 45 parts activated weathered carbon, 10 to 25 parts fungal residues, 1 to 5 parts iron powder, 10 to 20 parts struvite and 1 to 3 parts sucrose , which is placed under the soil in greenhouses as an adsorbent barrier. Nitrates and phosphates are retained in this barrier, preventing them from being washed out of the soil by watering. Disadvantages: complex production of the mixture, not economically feasible when using large quantities.
  • the incorporation of metal oxides close to the surface leads to a reduction in the substance concentrations of the substances necessary for plant growth (P, Zn, Cu, etc.) in the soil solution of the topsoil and can thus lead to an insufficient supply of the plants with these substances as a result of adsorptive binding.
  • reduced leaching of these substances is only achieved if their accumulation is limited to the near-surface area covered by the interference. If the substances have already penetrated into the subsoil, it is no longer possible to effectively reduce their leaching by working in oxides close to the surface.
  • the reduction in the availability of phosphorus and trace nutrient elements in the topsoil also prevents the remediation of these polluted soils by removing phosphorus and heavy metals by plants (phytoremediation or phytoremediation).
  • the present invention was therefore based on the object, on the one hand, of preventing the entry of harmful soil constituents into the groundwater, for example through leaching, so that subsequent groundwater treatment can be dispensed with.
  • the task was based certain ions, for example phosphate, not to be completely removed from the topsoil or to be fixed in the soil, since otherwise essential ions for the plant are immobilized and can no longer be absorbed by the plant.
  • the components of the adsorber material according to the invention are at least 0 to 10% by weight of topsoil, 1 to 99% by weight of subsoil, 1 to 99% by weight of adsorbent and optionally other components, the percentages by weight being measured in the dry matter and the contents of the individual components add up to 100% by weight.
  • the adsorber material according to the invention preferably has as components at least 0 to 10% by weight of topsoil, 80 to 99% by weight of subsoil, 1 to 20% by weight of adsorbent and optionally other components, the percentages by weight being measured in dry matter and the contents of the individual components add up to 100% by weight.
  • the adsorber material according to the invention particularly preferably has as components at least 0 to 10% by weight of topsoil, 90 to 99% by weight of subsoil, 1 to 10% by weight of adsorbent and optionally other components, the weight percentages in the dry matter are measured and the contents of the individual components add up to 100% by weight.
  • topsoil is defined as the A-horizon according to the terminology commonly used in Germany.
  • This A horizon and its border to the B horizon can be clearly identified by a person skilled in the art in a core drilling of the mineral soil to be examined.
  • the A horizon preferably has a high mineral content of 70 to 100% by weight.
  • underbody is defined as the B horizon, according to the terminology commonly used in Germany. This B horizon and its boundaries to the A horizon and the C horizon can be clearly identified by a person skilled in the art in a core drilling of the mineral soil to be examined.
  • the B horizon preferably has a mineral content of 70 to 100 percent by weight.
  • Topsoil and subsoil are firmly defined terms in soil science, which are also defined in legal regulations, for example in the ordinance for the introduction of a substitute building material ordinance for the revision of the Federal Soil Protection and Contaminated Sites Ordinance and for the amendment of the Landfill Ordinance and the Commercial Waste Ordinance of 9 July 2021, Federal Law Gazette 2021, Part I No. 43, issued in Bonn on July 16, 2021, page 2717: Article 2, Federal Soil Protection and Contaminated Sites Ordinance (BBodSchV), Section 1, Section 2 Definitions, Number 2: Top soil, Number 3 : underbody.
  • BBodSchV Federal Soil Protection and Contaminated Sites Ordinance
  • topsoil and subsoil in different soils are also presented in detail in standard works on soil science, for example in Bodenkuriume Kartierantechnisch, KA5, 2005, ed.: Wolf Eckelmann; E. Schweizerbart'sche Verlagsbuchmaschine, Chapter 5.6 Horizon-related data, sub-chapter 5.6.3.3.3 Mineral horizons, pages 92 to 98.
  • adsorbent z As activated carbon, ion exchangers, clay minerals, zeolites are used, which have a high binding capacity to substances. Some iron oxides, but particularly iron oxyhydroxides, have a very high adsorption capacity for arsenate, vanadate, antimonate, chromate or phosphate ions. In addition, numerous Heavy metal cations such as cadmium, lead, mercury, nickel or copper ions are effectively adsorbed on the iron oxyhydroxide surface.
  • the at least one adsorbent contained in the adsorbent material according to the invention is selected from the group consisting of activated carbon, ion exchangers, clay minerals, zeolites, iron oxides and iron oxyhydroxides, or any mixtures thereof. Iron oxides and iron oxyhydroxides are preferred as adsorbents. Iron oxyhydroxides are particularly preferred as adsorbents.
  • iron oxides and iron oxyhydroxides in particular iron oxyhydroxides, also have a high binding power for the ions mentioned when they are introduced in granular form into the horizon below the topsoil without significantly changing the soil permeability at the same time.
  • the pollutant ions are in the topsoil and do not get into the subsoil due to binding to the iron oxide surface in the adsorber material according to the invention and therefore cannot be washed out into the groundwater.
  • certain iron oxyhydroxides have a high mechanical granulate stability against abrasion and water flow. Maintaining the granular structure of the adsorbent in the soil is critical. On the one hand, the soil structure is retained after the granules have been introduced and there is no compaction and/or sticking together of the soil structure, which would be the case with powdery adsorbers. In addition, the granules are stable with regard to disintegration, so that they do not disintegrate into powder in the soil, which would lead to the iron oxyhydroxide powder contaminated with pollutants being unintentionally washed out into the groundwater. Granules can also be dosed well and largely dust-free, which is important for the production of the adsorber material.
  • Iron oxyhydroxides ie goethite, which has the modification a-FeOOH, in lumpy form, also called granulate form, are therefore very particularly preferred as adsorbents. These usually have a grain size of 0.2 to 40 mm, preferably from 0.2 to 20 mm.
  • the preparation of these lumpy iron oxyhydroxides is described, for example, in EP1582505B1 and EP1328476B1.
  • Also particularly preferred as adsorbents are therefore lumpy iron oxyhydroxides which have the ⁇ -FeOOH modification and specific BET surface areas of greater than 20 m 2 /g, in particular from 80 to 400 m 2 /g.
  • Examples of such lumpy iron oxyhydroxides or iron oxyhydroxide granules are the products Bayoxide® E 33 and Bayoxide® E 33 HC, which are produced by LANXESS GmbH.
  • the iron oxyhydroxides preferably have a high BET specific surface area, so that rapid adsorption kinetics of the pollutants on the granulate is ensured.
  • Also very particularly preferred as adsorbents are yellow pigments, generally needle-shaped goethite which has the modification a-FeOOH, in granular or compact form, as are produced, for example, by the LANXESS Group, for example from the Bayferrox or Bayoxide product line .
  • the adsorber material according to the invention is present in the soil preferably as a layer, particularly preferably as a horizontal layer, which has a layer thickness of 1 to 200 mm, preferably 2 to 100 mm.
  • Established measuring methods are available to the person skilled in the art for determining the content of adsorbents in dry solids mixtures.
  • the invention also includes the production of the adsorber material according to the invention using a method, characterized in that the adsorbent has a content of 1 to 99% by weight, preferably 1 to 10% by weight, particularly preferably 1 to 5% by weight. %, based on the sum of the total dry masses of the adsorbent used, the topsoil used and the subsoil used, is homogeneously mixed with subsoil and optionally with topsoil.
  • the adsorber material according to the invention is produced in that the adsorbent(s), for example activated carbon, ion exchangers, clay minerals, zeolites, iron oxides and iron oxyhydroxides or any mixtures thereof, preferably iron oxyhydroxides, particularly preferably iron oxyhydroxides in lumpy form, are introduced under the intensively rooted topsoil becomes.
  • the adsorbent as such can either be mixed into the subsoil with few roots or applied to the surface as a layer, preferably as a horizontal layer.
  • this can be done, for example with suitable technical devices, in that, for example on an arable area, the topsoil is removed at the border to the subsoil, then the adsorbent is applied to the subsoil as a layer, preferably as a horizontal layer, and as a last step, the topsoil is reapplied to this layer, for example turned 180 degrees.
  • this can be done, for example with suitable technical devices, in that, for example on an arable area, the topsoil is removed at the border to the subsoil, then a defined layer of subsoil is removed, then the adsorbent is mixed with the removed subsoil , and then this mixture is applied to the remaining subsoil as a layer, preferably as a horizontal layer, and as a last step the topsoil, for example turned 180 degrees, is applied again to the adsorber material present as a layer.
  • ploughshares can be used as technical means, for example, which lift, loosen and, if necessary, turn the topsoil from the subsoil in such a way that the adsorbent material and/or the adsorbent can be introduced before the topsoil is again over the adsorbent material and / or the adsorbent is applied.
  • this creates a permeable, reactive layer at the topsoil/subsoil boundary layer or in the subsoil itself, which effectively reduces the leaching of anions, for example phosphate and heavy metals, without impeding the uptake of these substances by the plant.
  • anions for example phosphate and heavy metals
  • An example is the cultivation of plants, e.g. to remove heavy metals as part of phytoremediation.
  • the method according to the invention also creates a new mineral soil that has a new structure.
  • the invention thus also includes a new mineral soil.
  • This soil according to the invention is characterized in that it has an upper layer of topsoil, and a layer of adsorber material according to the invention located underneath and a layer of subsoil underneath.
  • the soil according to the invention preferably has a layer of adsorbent material and/or adsorbent which has a layer thickness of 1 mm to 200 mm, preferably 2 mm to 100 mm.
  • the topsoil contained in the mineral soil according to the invention also preferably has a mineral content of 70 to 100 percent by weight.
  • the subsoil contained in the mineral soil according to the invention also preferably has a mineral content of 70 to 100 percent by weight.
  • topsoil and subsoil of a specific soil can also preferably be distinguished by further characteristics such as color, color distribution, color intensity, proportion of inorganic substances, proportion of organic substances, degree of root penetration, composition of the main mineral components, aggregation of primary particles, proportion of nutrients (e.g. nitrogen or phosphorus), or proportion and type of soil organisms are clearly distinguished from each other.
  • further characteristics such as color, color distribution, color intensity, proportion of inorganic substances, proportion of organic substances, degree of root penetration, composition of the main mineral components, aggregation of primary particles, proportion of nutrients (e.g. nitrogen or phosphorus), or proportion and type of soil organisms are clearly distinguished from each other.
  • the layer of adsorbent material contained in the mineral soil according to the invention also contains an adsorbent selected from the group consisting of activated carbon, ion exchangers, clay minerals, zeolites, iron oxides and iron oxyhydroxides, or mixtures thereof.
  • Iron oxyhydroxides ie goethite, which has the modification a-FeOOH, in lumpy form, also called granulate form, are very particularly preferred as adsorbents in the mineral soil according to the invention. These usually have a grain size of 0.2 to 40 mm, preferably 0.2 to 20 mm, on. Also very particularly preferred as adsorbents in the mineral soil according to the invention are lumpy iron oxyhydroxides which have the ⁇ -FeOOH modification and specific BET surface areas of greater than 20 m 2 /g, in particular from 80 to 400 m 2 /g.
  • Examples of such lumpy iron oxyhydroxides or iron oxyhydroxide granules are the products Bayoxide® E 33 and Bayoxide® E 33 HC, which are produced by LANXESS GmbH.
  • the iron oxyhydroxides also very particularly preferably have a high BET specific surface area, so that rapid adsorption kinetics of the pollutants on the granulate is ensured.
  • Also very particularly preferred as adsorbents are yellow pigments, generally needle-shaped goethite which has the modification a-FeOOH, in granular or compact form, as are produced, for example, by the LANXESS Group, for example from the Bayferrox or Bayoxide product line .
  • topsoil the layer of adsorber material and/or adsorbent and subsoil using a soil sample, for example in the form of core drillings, based on one or more features.
  • features are, for example, color, color distribution, color intensity, proportion of inorganic substances, proportion of organic substances, proportion of adsorbents, degree of root penetration, composition of the main mineral components, aggregation of primary particles, proportion of nutrients (e.g. nitrogen or phosphorus), or proportion and type of soil organisms.
  • the invention also relates to a method for producing the trays according to the invention, characterized in that the adsorber material according to the invention and/or the adsorbent is introduced between the topsoil and the subsoil.
  • adsorbent material and/or the adsorbent into the boundary layer between the topsoil and subsoil
  • technical devices can preferably be used which lift, loosen and, if necessary, turn the topsoil from the subsoil in such a way that the adsorbent material and/or the adsorbent can be introduced before the topsoil again over the created layer of the adsorber material according to the invention and/or the Adsorbent is applied.
  • a plow is particularly preferably used as the technical device, which has ploughshares that lift, loosen and, if necessary, turn the topsoil from the subsoil in such a way that the adsorber material and/or the adsorbent can be introduced before the topsoil again covers the layer produced according to the invention Adsorber material and / or the adsorbent is applied.
  • this can be done, for example with suitable technical devices, in that, for example on an arable area, the topsoil is removed at the border to the subsoil, then the adsorber material is applied as a layer to the subsoil and as a last step the topsoil, turned, for example, by 180 degrees, is applied again to the produced layer of the adsorber material and/or the adsorbent.
  • the adsorber material according to the invention and the soils according to the invention can be easily identified by core drillings in the relevant soil by taking samples of different layer thicknesses from the cores around the boundary layer between subsoil and topsoil. In these samples, the adsorbent content in relation to the topsoil and subsoil is then determined by suitable quantitative measuring methods in the relevant layer thickness of the sample.
  • the invention also relates to the use of adsorbents selected from the group consisting of activated carbon, ion exchangers, clay minerals, zeolites, iron oxides, iron oxyhydroxides, including their preferred and particularly preferred embodiments described above for producing the adsorbent material according to the invention.
  • adsorbents selected from the group consisting of activated carbon, ion exchangers, clay minerals, zeolites, iron oxides, iron oxyhydroxides, including their preferred and particularly preferred embodiments described above for producing the adsorbent material according to the invention.
  • the invention also relates to the use of the adsorber material described above, including its preferred and particularly preferred embodiments described above, for the production of the mineral soils according to the invention described above, including its preferred and particularly preferred embodiments described above.
  • the adsorber materials according to the invention and the mineral soils according to the invention newly formed from them surprisingly have the advantage that the availability of the target substances for the plant in the topsoil is retained, but the contamination of the subsoil and the groundwater thus is minimized.
  • Example I For this purpose, a mixture from Example I was transferred into a percolation column A as the bottom layer. For comparison, the same mass of the same subsoil without adsorbent was filled into a percolation column B. The same amount of topsoil was filled into both percolation columns as the upper layer.
  • the percolation columns A and B from Example II were sprinkled with water and the eluates from percolation column A (eluate A) and percolation column B (eluate B) were collected in different fractions of the same size.
  • the concentration of the eluates "c(Eluate A)” and “c(Eluate B)” of ortho-phosphate, phosphorus (total phosphorus), lead, copper, cadmium and zinc ions were measured.
  • the Cu, Zn, Pb and Cd contents of the eluate and the loaded iron oxyhydroxide or the solutions were determined using conventional methods, for example using atomic adsorption spectrometry or mass spectrometry (ICP-MS) in accordance with DIN 38406-29 (1999) or optical emission spectroscopy (ICP-OES) according to EN-ISO 11885 (1998) with inductively coupled plasma as the excitation unit.

Landscapes

  • Life Sciences & Earth Sciences (AREA)
  • Soil Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Environmental & Geological Engineering (AREA)
  • Processing Of Solid Wastes (AREA)
  • Soil Conditioners And Soil-Stabilizing Materials (AREA)
  • Solid-Sorbent Or Filter-Aiding Compositions (AREA)

Abstract

La présente invention concerne un matériau adsorbant qui contient au moins un sous-sol et au moins un adsorbant, des sols minéraux contenant lesdits matériaux adsorbants, un procédé de production des matériaux adsorbants, un procédé de production de sols minéraux qui contiennent lesdits matériaux adsorbants, l'utilisation d'adsorbants pour la production de matériaux adsorbants, et l'utilisation de matériaux adsorbants pour la production de sols minéraux.
EP22822435.8A 2021-11-25 2022-11-25 Matériaux adsorbants pour sols minéraux Pending EP4436728A1 (fr)

Applications Claiming Priority (2)

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EP21210540 2021-11-25
PCT/EP2022/083311 WO2023094608A1 (fr) 2021-11-25 2022-11-25 Matériaux adsorbants pour sols minéraux

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EP4436728A1 true EP4436728A1 (fr) 2024-10-02

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EP (1) EP4436728A1 (fr)
JP (1) JP2024542583A (fr)
CN (1) CN118302259A (fr)
AU (1) AU2022398118B2 (fr)
CA (1) CA3240028A1 (fr)
CL (1) CL2024001528A1 (fr)
MX (1) MX2024006236A (fr)
WO (1) WO2023094608A1 (fr)

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