Process for preparing asphalt mix composition

Abstract

To provide an improved process for obtaining an asphalt composition displaying advantageous physical properties in a highly effective manner, said advantages require increased efforts in both time and energy, in particular with regard to time- and energy-efficiency.SOLUTION: The present invention relates to a process for preparing an asphalt mix composition, the process comprising: (1) providing an asphalt composition and heating the composition to a temperature in the range of from 110 to 200°C; (2) providing a granular material and heating the material to a temperature in the range of from 110 to 240°C; (3) providing one or more thermosetting reactive compounds; (4) adding the one or more thermosetting reactive compounds provided in (3) to the asphalt composition obtained in (1) and homogenizing the mixture for a duration in the range of from 2 to 180 seconds; (5) adding the mixture obtained in (4) to the granular material obtained in (2) and homogenizing the slurry for a duration in the range of from 5 to 180 seconds. Further, the present invention relates to an asphalt mix composition obtained or obtainable by the process and its use.SELECTED DRAWING: None

Description

Technical Field

[0001] The present invention relates to a method for preparing an asphalt mixture composition, an asphalt mixture composition obtained or obtainable by said method, and its use.

Background Art

[0002] Introduction Generally, asphalt is a colloidal substance containing various molecular species classified as asphaltenes and maltenes. Since asphalt has viscoelasticity and thermoplasticity, its properties change at various temperatures from extreme cold to extreme heat. Asphalt becomes soft in hot climates and tends to crack in extremely cold weather. At low temperatures, asphalt becomes brittle and is prone to cracking, but at high temperatures, it becomes soft and loses its physical properties.

[0003] By adding a thermosetting reactive component as a binder or, more generally, a modifier, the physical properties of asphalt can be kept more constant at various temperatures and / or the physical properties can be improved over the temperature range to which the asphalt is exposed.

[0004] Such asphalt modified by the added binder or modifier has been known in the art for many years. However, there is still a need for improved asphalt in the asphalt industry. This is partly because currently known polymer-modified asphalts have a number of deficiencies. These deficiencies include, for example, permanent deformation (rutting), bending fatigue, susceptibility to moisture, and a decrease in elasticity during low-temperature operation.

[0005] In WO 01 / 30911 A1, an asphalt composition containing about 1 to 8% by mass of polymeric MDI based on the total mass of the composition, wherein the functionality of the polymeric MDI is at least 2.5, is disclosed. The document also relates to a method for preparing said asphalt composition using a reaction time of less than 2 hours. The formation of the product, MDI-asphalt, is measured by an increase in the viscosity of the product or, more preferably, by dynamic mechanical analysis (DMA).

[0006] In WO 01 / 30912 A1, an aqueous asphalt emulsion containing an emulsifiable polyisocyanate in addition to asphalt and water is disclosed. The document also relates to an aggregate composition containing said emulsion and a method for preparing said composition.

[0007] In WO 01 / 30913 A1, an asphalt composition containing about 1 to 5% by mass of a prepolymer based on polymeric MDI based on the total mass of the composition, wherein the functionality of the polymeric MDI is at least 2.5, is disclosed. The document also relates to a method for preparing said asphalt composition.

[0008] https: / / eapa.org / wp-content / uploads / 2018 / 07 / EAPA-paper-Warm-MixAsphalt-version-2014-1.pdf "The use of Warm Mix Asphalt", EAPA Position Paper, January 1, 2014, pages 1 - 23, discloses warm mix asphalt (WMA) technology for producing asphalt having properties or performance equivalent to conventional HMA at temperatures slightly above 100°C.

[0009] https: / / www.faa.gov / documentlibrary / media / advisory_circular / 150-5370-14A / 150_5370_14a_app 1 _part_I I_a. pdf: "Hot Mix Asphalt Paving Handbook, AC 150 / 5370-14A, Appendix 1, Part II-a", January 1, 2001, pages 1 - 11 disclose the operation of hot mix asphalt plants in several types of asphalt plant environments, namely batch plants, parallel flow drum mix plants, and counterflow drum mix plants.

[0010] http: / / web.archive.org / web / 20071223141536 / http: / / www.in.gov / indot / files / chapter_03(5).pdf: "HOT MIX ASPHALT PLANT OPERATIONS, Chapter 3", December 23, 2007, pages 1 - 78 disclose the influence of plant types on the operation of hot mix asphalt plants in batch and drum plant environments, the properties of HMA, aggregate mixing, plant inspection and scale checks, plant calibration, and plant troubleshooting.

[0011] http: / / www.astecinc.com / images / file / literature / Nomad_with_Baghouse.pdf: "NOMAD(TM) Hot Mix Asphalt Plant", January 1, 2008, pages 1 - 5 disclose the Nomad(TM) hot mix asphalt plant equipped with a cold feed bin, scalping screen, drying drum, liquid asphalt tank, twin shaft coater, baghouse, surge bin, and operating room.

[0012] https: / / store.asphaltpavement.org / pdfs / ec-101.pdf: "Best Management Practices To Minimize Emissions During HMA Construction; EC-101 4 / 00", April 1, 2000, pages 1 - 12, discloses best management practices to minimize emissions during HMA construction. In this regard, it is disclosed that hot mix asphalt (HMA) manufacturers need to recognize that using proper storage, mixing, and compaction temperatures for HMA is the key to minimizing emissions. Further, it is disclosed that the primary goal is to minimize temperature while meeting the specified density.

[0013] Malcolm D Graham et al., "Reduced Mixing Time for Asphalt Concrete Mixes", Paper presented at the 47 th Annual Meeting, January 1, 1968, pages 1 - 17, mentions in the context that individual plant designs and conditions affect the proper distribution of aggregate particles and the time requirements for asphalt coating, so plant - specific tests are required for mixing time reduction in asphalt concrete mixers to be considered reduced, and the reduction of mixing time in asphalt concrete mixers is disclosed.

[0014] Y Becker et al., "Polymer Modified Asphalt", VISION TECNOLOGICA, INTEVEP, LOS TEQUES, VE, vol. 9, no. 1, January 1, 2001, pp. 39-50, disclose that polymer modification of asphalt is considered to be the best option for improving the properties of asphalt. Furthermore, it is disclosed that the useful temperature range of the binder is significantly increased by the polymer. Furthermore, the limitations considered for modified bitumen are: (i) increased cost, (ii) possible compatibility and stability problems, (iii) some problems that may occur in the storage of bitumen, (iv) mixing temperature, and (v) the length of time the material is held at high temperature before laying.

[0015] Bjarne Bo Jensen et al., "15 YEARS EXPERIENCE ADDING POLYMER POWDER DIRECLY INTO THE ASPHALT MIXER", 5 th Eurasphalt & Eurobitume Congress, 13-15 th June 2012, Istanbul, June 15, 2012, pp. 1-8, disclose that an attempt was made to increase the addition of a special polymer powder to obtain better asphalt properties (better rutting resistance and better fatigue resistance). Laboratory results have shown an improvement in binder properties, and field tests on various types of roads have shown an improvement in the function of asphalt pavement (less crack propagation and better rutting resistance). Furthermore, it is disclosed that when the polymer is added directly to the asphalt mixer, it is possible to modify even small amounts of asphalt with different bitumen hardnesses and no special bitumen storage facilities are required.

[0016] HESAMI Ebrahim et al., "Study of the amine-based liquid anti-stripping agents by simulating hot mix asphalt plant production process", CONSTRUCTION AND BUILDING MATERIALS, vol. 157, 2017, pp. 1011-1017, disclose simulating the production conditions of HMA and then investigating the effects of two amine-based liquid anti-stripping agents on the performance of HMA using the tensile strength ratio (TSR) and semi-circular bend (SCB) tests. It is also disclosed that the results of this study showed a significant decrease in the effectiveness of these additives after long-term heating for HMA production.

[0017] LUO Sang et al., "Performance evaluation of epoxy modified open graded porous asphalt concrete", CONSTRUCTION AND BUILDING MATERIALS, ELSEVIER, NETHERLANDS, vol. 76, December 12, 2014, pp. 97-102, disclose a novel open-graded porous asphalt mixture using epoxy asphalt as a binder to improve the durability of the mixture. In this study, one type of epoxy asphalt normally applied to dense-graded asphalt concrete for bridge deck paving was selected. Furthermore, it is disclosed that a series of laboratory tests were conducted, including the Cantabro loss, permeability, sound absorption, flexural tensile, friction, shear stiffness, shear strength, and wheel rutting tests, to compact the mixture into slab specimens and evaluate the performance of the novel mixture. Furthermore, as a result, it is disclosed that the epoxy-modified open-graded porous asphalt mixture showed overall excellent performance compared to the conventional open-graded porous asphalt mixture.

[0018] Fang Changqing et al., "Preparation and properties of isocyanate and nano particles composite modified asphalt", CONSTRUCTION AND BUILDING MATERIALS, ELSEVIER, NETHERLANDS, vol. 119, May 13, 2016, pp. 113 - 118, disclose that samples of isocyanate - modified asphalt were obtained by adding a quantitative isocyanate to base asphalt. The composite - modified asphalt samples of isocyanate and nanoparticles were prepared by adding a quantitative isocyanate and three kinds of inorganic nanoparticles (silicon dioxide, titanium dioxide, zinc oxide) to base asphalt respectively. The isocyanate - modified asphalt, the isocyanate and nanoparticles composite - modified asphalt were characterized by physical tests, SEM, fluorescence microscopy, TG and FTIR tests, and it was demonstrated that the high - temperature and low - temperature performance of the isocyanate and nanoparticles composite - modified asphalt was effectively improved. Further, from a microscopic perspective, it is disclosed that the modification of base asphalt is very important, and as a result, the temperature sensitivity of the composite - modified asphalt was also shown to have decreased. Further, it is disclosed that the thermal stability was also improved simultaneously when compared with base asphalt and isocyanate - modified asphalt.

[0019] In EP 3 006 525 A1, a component (A) obtained by adding an MDI prepolymer produced by reacting a polyolefin polyol having two or more hydroxyl groups, a short - chain polyhydric alcohol, an MDI monomer, an MDI monomer, and a solvent a, and at least a component (B) containing asphalt, a catalyst, and a solvent b are disclosed for an asphalt - urethane composition.

[0020] In WO 2017 / 125421 A1, there is a step of mixing asphalt, a polyester resin, and an aggregate at a temperature of 130°C or higher and 200°C or lower for 30 seconds or longer. The polyester resin is a polyester having a constituent component derived from an alcohol component containing 65 mol% or more of an alkylene oxide adduct of bisphenol A and a constituent component derived from a carboxylic acid component containing 50 mol% or more of at least one selected from the group consisting of terephthalic acid and isophthalic acid. The polyester has a softening point of 95°C or higher and 130°C or lower, and a hydroxyl value of 20 mgKOH / g or higher and 50 mgKOH / g or lower. The polyester resin is mixed at a ratio of 5 parts by mass or more and 50 parts by mass or less with respect to 100 parts by mass of the asphalt. A method for producing an asphalt composition for road paving including this step is disclosed.

[0021] In EP 0 537 638 B1, there is a polymer-modified bitumen composition containing 0.5 to 10 parts by mass of a functionalized polyoctenamer and optionally a crosslinking agent with respect to 100 parts by mass of bitumen. The polyoctenamer is mainly a trans-polyoctenamer and is characterized by containing a carboxyl group and groups derived therefrom, such as maleic acid. The polymer-modified bitumen composition is disclosed.

[0022] On the other hand, in WO 2018 / 228840 A1, there is an improved asphalt composition showing improved physical properties in terms of being more constant at various temperatures. The asphalt composition is obtained by a method including mixing asphalt and a thermosetting reactive compound and stirring the mixture for at least 2.5 hours. The asphalt composition is disclosed.

Prior Art Documents

Patent Documents

[0023]

Patent Document 1

Patent Document 2

Patent Document 3

[0024] [Non-Patent Document 1] https: / / eapa.org / wp-content / uploads / 2018 / 07 / EAPA-paper-Warm-MixAsphalt-version-2014-1.pdf "The use of Warm Mix Asphalt", EAPA Position Paper, January 1, 2014, pp. 1 - 23 [Non-Patent Document 2] https: / / www.faa.gov / documentlibrary / media / advisory_circular / 150-5370-14A / 150_5370_14a_app 1 _part_I I_a. pdf: "Hot Mix Asphalt Paving Handbook, AC 150 / 5370-14A, Appendix 1, Part II-a", January 1, 2001, pp. 1 - 11 [Non-Patent Document 3] http: / / web.archive.org / web / 20071223141536 / http: / / www.in.gov / indot / files / chapter_03(5).pdf: "HOT MIX ASPHALT PLANT OPERATIONS, Chapter 3", December 23, 2007, pp. 1 - 78 [Non-Patent Document 4] http: / / www.astecinc.com / images / file / literature / Nomad_with_Baghouse.pdf: "NOMAD(TM) Hot Mix Asphalt Plant", January 1, 2008, pages 1 - 5

Non - Patent Document 5

Non - Patent Document 6

Non - Patent Document 7

Non - Patent Document 8

Non - Patent Document 9

Non-Patent Document 10

Non-Patent Document 11

Summary of the Invention

Problems to be Solved by the Invention

[0025] Regarding the physical properties of the asphalt composition, significant improvements have been achieved, but for the above advantages, greater efforts in both time and energy are required. Considering the above, there is still a need to provide an improved method for obtaining the material in a very effective manner, especially regarding time and energy efficiency.

Means for Solving the Problems

[0026] Accordingly, an object of the present invention was to provide an improved method for preparing an asphalt mixture composition exhibiting advantageous physical properties.

[0027] According to the present invention, the terms "reclaimed asphalt pavement" (also abbreviated as RAP), "recycled asphalt", "reclaimed asphalt", "reclaimed asphalt pavement material", and "reclaimed asphalt mixture" are used interchangeably to describe materials that may also be described as "reprocessed pavement materials containing asphalt and aggregates".

[0028] According to the present invention, the term "granular material" is used interchangeably to describe components that may also be described as "aggregate" or "aggregates". Further, according to the present invention, the granular material or aggregate may include one or more of gravel, sand, filler, and fine aggregate. Additional specific and / or preferred embodiments are disclosed herein with respect to this point.

[0029] Thus, surprisingly, in contrast to the teachings of the prior art, it has been found that the mixing time of the thermosetting reactive compound and asphalt before adding the resulting mixture to a granular material such as sand or gravel has little effect on the degree of modification of the asphalt. Rather, quite unexpectedly, it has been found that the physical properties of the asphalt can be substantially improved in terms of being more constant at various temperatures depending on the conditions and time when the obtained mixture is mixed with the granular material (i.e., the asphalt contained in such an asphalt mixing composition exhibits an increase in the useful temperature interval (UTI), a decrease in the non-recoverable creep compliance (Jnr), an increase in the elastic response, an increase in the softening point, and a decrease in the penetration, and thus, for example, in terms of rutting resistance, fatigue resistance, low-temperature resistance, and improvement in road durability over a wider temperature range, it results in better performance of the corresponding asphalt mixing composition). This can be achieved even after a relatively short mixing stage. Thus, quite surprisingly, an asphalt mixing composition having advantageous properties can be obtained using a specific continuous relatively short mixing process, which not only results in a significant saving of time and energy, but also makes it possible to in-line mix the starting components immediately before using the product in paving applications.

[0030] Accordingly, the present invention relates to a method for preparing an asphalt mixing composition, comprising: (1) preparing an asphalt composition and heating the composition to a temperature in the range of 110 to 200 °C; (2) preparing a granular material and heating the material to a temperature in the range of 110 to 240 °C; (3) preparing one or more thermosetting reactive compounds; (4) adding the one or more thermosetting reactive compounds prepared in (3) to the asphalt composition obtained in (1) and homogenizing the mixture for a time in the range of 2 to 180 seconds; and (5) adding the mixture obtained in (4) to the granular material obtained in (2) and homogenizing the slurry for a time in the range of 5 to 180 seconds.

[0031] The temperature of the homogenized slurry obtained in (5) is preferably in the range of 110 to 200 °C, more preferably 130 to 197 °C, more preferably 150 to 195 °C, more preferably 170 to 192 °C, more preferably 175 to 190 °C, and more preferably 180 to 185 °C.

[0032] Starting from the addition of the thermosetting reactive compound in (4), the total time until the homogenized slurry in (5) is obtained is preferably in the range of 10 seconds to 7 days, more preferably 10 seconds to 3 days, more preferably 15 seconds to 1 day, more preferably 15 seconds to 12 hours, more preferably 20 seconds to 6 hours, more preferably 20 seconds to 1 hour, more preferably 25 seconds to 30 minutes, more preferably 25 seconds to 15 minutes, more preferably 30 seconds to 6 minutes, more preferably 30 seconds to 3 minutes, more preferably 35 seconds to 2 minutes, more preferably 35 seconds to 90 seconds, more preferably 40 seconds to 85 seconds, more preferably 45 seconds to 70 seconds, and more preferably 50 seconds to 60 seconds.

[0033] Before (5) and after (4), the mixture obtained in (4) is preferably stored at a temperature in the range of 60 to 190 °C, more preferably 70 to 185 °C, more preferably 80 to 180 °C, more preferably 90 to 175 °C, more preferably 110 to 170 °C, more preferably 130 to 165 °C, and more preferably 150 to 160 °C.

[0034] Before (5) and after (4), the mixture obtained in (4) is preferably stored for a time in the range of 0 seconds to 7 days, more preferably 5 seconds to 3 days, more preferably 10 seconds to 1 day, more preferably 15 seconds to 12 hours, more preferably 20 seconds to 6 hours, more preferably 25 seconds to 1 hour, more preferably 30 seconds to 30 minutes, more preferably 35 seconds to 15 minutes, more preferably 40 seconds to 6 minutes, more preferably 45 seconds to 3 minutes, more preferably 50 seconds to 2 minutes, more preferably 55 seconds to 90 seconds, and more preferably 60 seconds to 70 seconds.

[0035] After (4) and before (5), the mixture obtained in (4) is preferably mixed at a mixing speed of 100 rpm or less, more preferably 50 rpm or less, more preferably 25 rpm or less, more preferably 20 rpm or less, more preferably 15 rpm or less, more preferably 10 rpm or less, more preferably 5 rpm or less, more preferably 3 rpm or less.

[0036] It is preferable that the mixture obtained in (4) is not mixed after (4) and before (5), and more preferably, the mixture obtained in (4) is not homogenized after (4) and before (5).

[0037] Alternatively, the mixture obtained in (4) is preferably directly treated in (5).

[0038] In (1), the asphalt composition is preferably heated to a temperature in the range of 130 to 197 °C, more preferably 150 to 195 °C, more preferably 170 to 192 °C, more preferably 175 to 190 °C, more preferably 180 to 185 °C.

[0039] In (2), the granular material is preferably heated to a temperature in the range of 130 to 220 °C, more preferably 150 to 200 °C, more preferably 170 to 195 °C, more preferably 175 to 190 °C, more preferably 180 to 185 °C.

[0040] The homogenization in (5) is preferably carried out at a temperature in the range of 110 to 200 °C, more preferably 130 to 195 °C, more preferably 150 to 190 °C, more preferably 170 to 185 °C, more preferably 175 to 180 °C.

[0041] Generally, the asphalt composition used in the present invention can be any known asphalt and generally includes any bitumen compound. The asphalt composition can be either a material called bitumen or asphalt. In particular, in the context of the present invention, the term "asphalt" or "asphalt composition" as used herein preferably refers to the definition described in ASTM D8-02 (asphalt is defined as a dark brown to black cementitious material whose main component is bitumen existing in nature or obtained by petroleum processing).

[0042] (1) The asphalt composition prepared in (1) has a penetration of 20 to 30, 30 to 45, 35 to 50, 40 to 60, 50 to 70, 70 to 100, 100 to 150, 160 to 220, and 250 to 330, or a performance grade of 52 to 16, 52 to 22, 52 to 28, 52 to 34, 52 to 40, 58 to 16, 58 to 22, 58 to 28, 58 to 34, 58 to 40, 64 to 16, 64 to 22, 64 to 28, 64 to 34, 64 to 40, 70 to 16, 70 to 22, 70 to 28, 70 to 34, 70 to 40, 76 to 16, 76 to 22, 76 to 28, 76 to 34, 76 to 40. More preferably, the asphalt composition prepared in (1) has a penetration of 30 to 45, 35 to 50, 40 to 60, 50 to 70, 70 to 100, 100 to 150, and 160 to 220, or a performance grade of 52 to 16, 52 to 22, 52 to 28, 52 to 34, 52 to 40, 58 to 16, 58 to 22, 58 to 28, 58 to 34, 58 to 40, 64 to 16, 64 to 22, 64 to 28, 64 to 34, 70 to 16, 70 to 22, 70 to 28, 76 to 16, 76 to 22. More preferably, the asphalt composition prepared in (1) has a penetration of 40 to 60, 50 to 70, 70 to 100, and 100 to 150, or a performance grade of 52 to 16, 52 to 22, 52 to 28, 52 to 34, 52 to 40, 58 to 16, 58 to 22, 58 to 28, 58 to 34, 64 to 16, 64 to 22, 64 to 28, 70 to 16, 70 to 22, 76 to 16, 76 to 22. More preferably, the asphalt composition prepared in (1) preferably has a penetration of 50 to 70 or 70 to 100, and the penetration is determined in accordance with DIN EN 1426.

[0043] (1) The asphalt composition prepared in (1) preferably contains modified bitumen, preferably polymer-modified bitumen. More preferably, the asphalt composition prepared in (1) consists of modified bitumen, more preferably polymer-modified bitumen.

[0044] When the asphalt composition prepared in (1) contains modified bitumen, the bitumen is preferably modified with one or more compounds selected from the group consisting of thermoplastic elastomers, latexes, thermoplastic polymers, thermosetting polymers, and mixtures of two or more of them.

[0045] When the bitumen is modified with a thermoplastic elastomer, the thermoplastic elastomer is preferably selected from the group consisting of styrene-butadiene elastomer (SBE), styrene-butadiene-styrene (SBS), styrene-butadiene rubber (SBR), styrene-isoprene-styrene (SIS), styrene-ethylene-butadiene-styrene (SEBS), ethylene-propylene-diene terpolymer (EPDT), isobutene-isoprene copolymer (IIR), polyisobutene (PIB), polybutadiene (PBD), polyisoprene (PI), and mixtures of two or more of them.

[0046] When the bitumen is modified with a latex, the latex is preferably natural rubber.

[0047] When the bitumen is modified with a thermoplastic polymer, the thermoplastic polymer is preferably selected from the group consisting of ethylene-vinyl acetate (EVA), ethylene-methyl acrylate (EMA), ethylene-butyl acrylate (EBA), atactic polypropylene (APP), polyethylene (PE), polypropylene (PP), polyvinyl chloride (PVC), polystyrene (PS), and mixtures of two or more of them.

[0048] When the bitumen is modified with a thermosetting polymer, the thermosetting polymer is preferably selected from the group consisting of epoxy resins, polyurethane resins, acrylic resins, phenolic resins, and mixtures of two or more of them.

[0049] When the asphalt composition prepared in (1) contains modified bitumen, the bitumen is a chemical modifier (e.g., organometallic compound, sulfur, phosphoric acid (PA), polyphosphoric acid (PPA), sulfonic acid, sulfuric acid, carboxylic anhydride, acid ester, dibenzoyl peroxide, silane, organic and inorganic urea sulfides), recycled material (e.g., crumb rubber, plastic), fiber (e.g., lignin, cellulose, glass fiber, magnesium aluminosilicate, polyester, polypropylene), adhesion enhancer (e.g., organic amine, amide), natural asphalt (e.g., Trinidad Lake Asphalt (TLA), gilsonite, rock asphalt), antioxidant (e.g., phenols, organic zinc compound, organic lead compound), filler (e.g., carbon black, slaked lime, lime, fly ash), viscosity modifier (e.g., flux oil, wax), reactive polymer (e.g., random terpolymer of ethylene, acrylate ester and glycidyl methacrylate, maleic anhydride grafted styrene-butadiene-styrene copolymer), and one or more compounds selected from the group consisting of a mixture of two or more of them. It is preferably modified using one or more compounds selected from the group consisting of:

[0050] The one or more thermosetting reactive compounds preferably include one or more compounds selected from the group consisting of polyisocyanate, epoxy resin, melamine formaldehyde resin, and a mixture of two or more of them, more preferably from the group consisting of fatty acid polyisocyanate, araliphatic polyisocyanate, aromatic polyisocyanate, and a mixture of two or more of them, and even more preferably from the group consisting of aromatic diisocyanate, oligomeric aromatic polyisocyanate, and a mixture of two or more of them. Even more preferably, the one or more thermosetting reactive compounds include a mixture of one or more aromatic diisocyanates and one or more oligomeric aromatic polyisocyanates, and even more preferably, the one or more thermosetting reactive compounds consist of a mixture of one or more aromatic diisocyanates and one or more oligomeric aromatic polyisocyanates.

[0051] According to the present invention, the polyisocyanate is preferably aliphatic, alicyclic, or araliphatic, more preferably an aromatic polyisocyanate known in the art. Such polyfunctional isocyanates are known and can be produced by methods known per se. The polyfunctional isocyanate can also be used especially as a mixture, and in this case the polyisocyanate contains various polyfunctional isocyanates. According to the present invention, the polyisocyanate is a polyfunctional isocyanate having two (hereinafter referred to as diisocyanate) or three or more isocyanate groups per molecule. Further, according to the present invention, the term "oligomeric polyisocyanate", more specifically "oligomeric aromatic polyisocyanate", refers to a polyfunctional isocyanate having three or four or more isocyanate groups per molecule.

[0052] In particular, according to the present invention, the polyisocyanate is preferably selected from the group consisting of alkylene diisocyanates having an alkyl group with 4 to 12 carbon atoms, such as 1,12-dodecane diisocyanate, 2-ethyltetramethylene diisocyanate-1,4, 2-methylpentamethylene diisocyanate-1,5, tetramethylene diisocyanate-1,4, preferably hexamethylene diisocyanate-1,6; alicyclic diisocyanates such as cyclohexane-1,3- and 1,4-diisocyanate, and any mixture thereof with isomers; 1-isocyanato-3,3,5-trimethyl-5-isocyanatomethylcyclohexane (IPDI), 2,4- and 2,6-hexahydrotoluene diisocyanate, and corresponding isomer mixtures; 4,4'-, 2,2'- and 2,4'-dicyclohexylmethane diisocyanate, and corresponding isomer mixtures; preferably aromatic polyisocyanates such as 2,4- and 2,6-toluene diisocyanate, and corresponding isomer mixtures; 4,4'-, 2,4'- and 2,2'-diphenylmethane diisocyanate, and corresponding isomer mixtures; mixtures of 4,4'- and 2,4'-diphenylmethane diisocyanate; polyphenyl polymethylene polyisocyanate; mixtures of 4,4'-, 2,4'- and 2,2'-diphenylmethane diisocyanate with polyphenyl polyethylene polyisocyanate; and mixtures of MDI and toluene diisocyanate.

[0053] Particularly preferred are 2,2'-, 2,4'- and / or 4,4'-diphenylmethane diisocyanate, 1,5-naphthylene diisocyanate (NDI), 2,4- and / or 2,6-toluene diisocyanate (TDI), 3,3'-dimethyldiphenyl diisocyanate, 1,2-diphenylethane diisocyanate and / or p-phenylene diisocyanate (PPDI), tri-, tetra-, penta-, hexa-, hepta- and / or octamethyl diisocyanate, 2-methylpentamethylene-1,5-diisocyanate, 2-ethylbutylene-1,4-diisocyanate, pentamethylene-1,5-diisocyanate, butylene-1,4-diisocyanate, 1-isocyanato-3,3,5-trimethyl-5-isocyanatomethyl-cyclohexane (isophorone diisocyanate, IPDI), 1,4- and / or 1,3-bis(isocyanatomethyl)cyclohexane (HXDI), 1,4-cyclohexane diisocyanate, 1-methyl-2,4- and / or -2,6-cyclohexane diisocyanate, and 4,4'-, 2,4'- and / or 2,2'-dicyclohexylmethane diisocyanate.

[0054] Modified polyisocyanates, i.e. products obtained by chemical reaction of organic polyisocyanates and containing at least two reactive isocyanate groups per molecule, are also preferably used. Particular mention is made of polyisocyanates containing ester, urea, biuret, allophanate, carbodiimide, isocyanurate, uretdione, carbamate and / or urethane groups, which are often mentioned together with unreacted polyisocyanates.

[0055] According to the present invention, the polyisocyanate is particularly preferably 2,2'-MDI, 2,4'-MDI, 4,4'-MDI, or a mixture of at least two of these isocyanates (also called monomeric diphenylmethane or MMDI), or an oligomeric MDI composed of homologues of higher-core MDI having at least three aromatic nuclei and at least three functional groups, or a mixture of two or more of the above diphenylmethane diisocyanates, or crude MDI obtained in the preparation of MDI, or preferably a mixture of at least one homologue of higher-core MDI and at least one low molecular weight MDI derivative 2,2'-MDI, 2,4'-MDI or 4,4'-MDI (this mixture is also called polymeric MDI). The average functionality of the polyisocyanate containing polymeric MDI can vary in the range of about 2.2 to about 4, particularly 2.4 to 3.8, particularly 2.6 to 3.0.

[0056] Polyfunctional isocyanates, or mixtures of several polyfunctional isocyanates based on MDI, are known and are commercially available, for example, from BASF. According to the present invention, one or more thermosetting reactive compounds preferably contain one or more isocyanates selected from the group consisting of 2,2'-MDI, 2,4'-MDI, 4,4'-MDI and homologues of larger MDI, in an amount of at least 70% by mass, particularly preferably at least 90% by mass, particularly 100% by mass, based on the total mass of the one or more thermosetting reactive compounds. The content of larger homologues having more than three rings is preferably at least 20% by mass, particularly preferably more than 30% and less than 80% by mass, based on the total mass of the one or more thermosetting reactive compounds.

[0057] The viscosity of one or more thermosetting reactive compounds used in the method of the present invention can vary over a wide range. The one or more thermosetting reactive compounds preferably have a viscosity of 100 to 3,000 mPa·s, particularly preferably 100 to 1,000 mPa·s, particularly preferably 100 to 600 mPa·s, particularly 200 to 600 mPa·s, particularly 400 to 600 mPa·s at 25°C. The viscosity of one or more thermosetting reactive compounds can vary within a wide range.

[0058] When one or more thermosetting reactive compounds contain an aliphatic polyisocyanate, the aliphatic polyisocyanate is an alkylene diisocyanate having an alkylene group with 4 to 12 carbon atoms, and a mixture of two or more thereof, 1,12-dodecane diisocyanate, 2-ethyltetramethylene diisocyanate-1,4, 2-methylpentamethylene diisocyanate-1,5, tetramethylene diisocyanate-1,4, hexamethylene diisocyanate-1,6, trimethyldiisocyanate, tetramethyldiisocyanate, pentamethyldiisocyanate, hexamethyldiisocyanate, heptamethyldiisocyanate, octamethyldiisocyanate, 2-methylpentamethylene-1,5-diisocyanate, 2-ethylbutylene-1,4-diisocyanate, pentamethylene-1,5-diisocyanate, butylene-1,4-diisocyanate, preferably selected from the group consisting of trimethyldiisocyanate, tetramethyldiisocyanate, pentamethyldiisocyanate, hexamethyldiisocyanate, heptamethyldiisocyanate, octamethyldiisocyanate, 2-methylpentamethylene-1,5-diisocyanate, 2-ethylbutylene-1,4-diisocyanate, pentamethylene-1,5-diisocyanate, butylene-1,4-diisocyanate, and a mixture of two or more thereof, more preferably, the aliphatic polyisocyanate contains hexamethylene diisocyanate-1,6, and more preferably, the aliphatic polyisocyanate consists of hexamethylene diisocyanate-1,6.

[0059] When one or more thermosetting reactive compounds contain an alicyclic polyisocyanate, the aliphatic polyisocyanate is 1-isocyanato-3,3,5-trimethyl-5-isocyanatomethyl-cyclohexane (isophorone diisocyanate, IPDI), 1,4-bis(isocyanatomethyl)cyclohexane and / or 1,3-bis(isocyanatomethyl)cyclohexane (HXDI), 1,4-cyclohexane diisocyanate, 1-methyl-2,4- and / or -2,6-cyclohexane diisocyanate, 4,4'-dicyclohexylmethane diisocyanate, 2,2'-dicyclohexylmethane diisocyanate, 2,4'-dicyclohexylmethane diisocyanate, cyclohexane-1,3-diisocyanate, cyclohexane-1,4-diisocyanate, 2,4-hexahydrotoluene diisocyanate, 2,6-hexahydrotoluene diisocyanate, 4,4'-dicyclohexylmethane diisocyanate, 2,2'-dicyclohexylmethane diisocyanate, 2,4'-dicyclohexylmethane diisocyanate, and a group consisting of a mixture of two or more of them. Preferably, 1-isocyanato-3,3,5-trimethyl-5-isocyanatomethyl-cyclohexane (isophorone diisocyanate, IPDI), 1,4-bis(isocyanatomethyl)cyclohexane and / or 1,3-bis(isocyanatomethyl)cyclohexane (HXDI), 1,4-cyclohexane diisocyanate, 1-methyl-2,4- and / or -2,6-cyclohexane diisocyanate, and 4,4'-dicyclohexylmethane diisocyanate, 2,2'-dicyclohexylmethane diisocyanate, 2,4'-dicyclohexylmethane diisocyanate, and a group consisting of a mixture of two or more of them. It is preferred to contain one or more alicyclic compounds selected from the group.

[0060] When one or more thermosetting reactive compounds contain an aromatic polyisocyanate, the aromatic polyisocyanate, and preferably the aromatic diisocyanate, is selected from the group consisting of 2,4-toluene diisocyanate, 2,6-toluene diisocyanate, 4,4'-diphenylmethane diisocyanate, 2,4'-diphenylmethane diisocyanate, 2,2'-diphenylmethane diisocyanate, 1,5-naphthylene diisocyanate (NDI), 3,3'-dimethyl diphenyl diisocyanate, 1,2-diphenylethane diisocyanate, p-phenylene diisocyanate (PPDI), and mixtures of two or more thereof; preferably from the group consisting of 2,4-toluene diisocyanate (2,4-TDI), 2,6-toluene diisocyanate (2,6-TDI), 4,4'-diphenylmethane diisocyanate (4,4'-MDI), 2,4'-diphenylmethane diisocyanate (2,4'-MDI), 2,2'-diphenylmethane diisocyanate (2,2'-MDI), crude MDI obtained in MDI preparation, and mixtures of two or more thereof; more preferably from the group consisting of 4,4'-diphenylmethane diisocyanate, 2,4'-diphenylmethane diisocyanate, 2,2'-diphenylmethane diisocyanate, and mixtures of two or more thereof (a mixture of the isomers 4,4'-, 2,4'- and 2,2'-diphenylmethane diisocyanate is also called monomeric diphenylmethane or MMDI); more preferably, the aromatic polyisocyanate, and preferably the aromatic diisocyanate, contains a mixture of 4,4'-diphenylmethane diisocyanate, 2,4'-diphenylmethane diisocyanate, and 2,2'-diphenylmethane diisocyanate; even more preferably, the aromatic polyisocyanate, and preferably the aromatic diisocyanate, consists of a mixture of 4,4'-diphenylmethane diisocyanate, 2,4'-diphenylmethane diisocyanate, and 2,2'-diphenylmethane diisocyanate.

[0061] When one or more thermosetting reactive compounds contain a polyisocyanate, the polyisocyanate preferably contains a modified polyisocyanate containing one or more ester, urea, biuret, allophanate, carbodiimide, isocyanurate, uretdione, carbamate and / or urethane groups, preferably a modified organic polyisocyanate, more preferably a modified organic polyisocyanate.

[0062] When one or more thermosetting reactive compounds contain an oligomeric aromatic polyisocyanate, the oligomeric aromatic polyisocyanate preferably contains one or more compounds selected from the group consisting of polyphenylpolymethylene polyisocyanate, polyphenylpolyethylene polyisocyanate, and mixtures of two or more thereof, preferably one or more polymethylene polyphenyl isocyanates, polyethylene polyphenyl isocyanates, and mixtures of two or more thereof, more preferably the aromatic polyisocyanate contains one or more polymethylene polyphenyl isocyanates, and even more preferably the aromatic polyisocyanate consists of one or more polymethylene polyphenyl isocyanates.

[0063] When one or more thermosetting reactive compounds contain an oligomeric aromatic polyisocyanate, the oligomeric aromatic polyisocyanate contains one or more oligomers consisting of one or more of 4,4'-diphenylmethane diisocyanate, 2,4'-diphenylmethane diisocyanate, and 2,2'-diphenylmethane diisocyanate and homologues with larger cores, and the homologues with larger cores preferably have at least three aromatic nuclei and at least three functional groups.

[0064] When one or more thermosetting reactive compounds contain one or more compounds selected from the group consisting of polyisocyanates, epoxy resins, melamine formaldehyde resins, and mixtures of two or more of them, the one or more thermosetting reactive compounds are polymeric MDI, and the total amount of 4,4'-MDI in the polymeric MDI is in the range of 26 to 98% by mass, preferably in the range of 30 to 95% by mass, more preferably in the range of 35 to 92% by mass, based on 100% by mass of the one or more thermosetting reactive compounds.

[0065] When one or more thermosetting reactive compounds contain one or more compounds selected from the group consisting of polyisocyanates, epoxy resins, melamine formaldehyde resins, and mixtures of two or more of them, the one or more thermosetting reactive compounds are polymeric MDI, and the bicyclic content of the polymeric MDI is in the range of 20 to 62%, more preferably in the range of 26 to 48% by mass, most preferably in the range of 26 to 48% by mass, based on 100% by mass of the polymeric MDI. When one or more thermosetting reactive compounds contain one or more compounds selected from the group consisting of polyisocyanates, epoxy resins, melamine formaldehyde resins, and mixtures of two or more of them, the average functionality of isocyanate groups in the one or more thermosetting reactive compounds, and preferably in the entire polyisocyanate contained in the compound, is preferably in the range of 2.1 to 3.5, more preferably in the range of 2.3 to 3.2, still more preferably in the range of 2.4 to 3, still more preferably in the range of 2.5 to 2.9, and still more preferably in the range of 2.6 to 2.8.

[0066] The iron content of the one or more thermosetting reactive compounds is preferably in the range of 1 to 100 wppm, more preferably in the range of 1 to 80 wppm, still more preferably in the range of 1 to 60 wppm, still more preferably in the range of 1 to 40 wppm, still more preferably in the range of 1 to 20 wppm, still more preferably in the range of 1 to 10 wppm, and still more preferably in the range of 1 to 5 wppm.

[0067] One or more thermosetting reactive compounds preferably exhibit a viscosity in the range of 100 to 3,000 mPa·s, preferably 100 to 1,000 mPa·s, more preferably 100 to 600 mPa·s, more preferably 200 to 600 mPa·s, and more preferably 400 to 600 mPa·s. The viscosity is the viscosity measured at 25°C.

[0068] When one or more thermosetting reactive compounds contain one or more epoxy resins, the epoxy resin is one or more compounds selected from the group consisting of aromatic epoxy resins, alicyclic epoxy resins, and mixtures of two or more of them. More preferably, it is bisphenol A diglycidyl ether (DGEBA), bisphenol F diglycidyl ether, cycloaliphatic bisphenol A diglycidyl ether, cycloaliphatic bisphenol F diglycidyl ether, bisphenol S diglycidyl ether (DGEBS), tetraglycidyl methylene dianiline (TGMDA), epoxy novolac (reaction product from epichlorohydrin and phenol resin (novolac)), 3,4-epoxycyclohexylmethyl, 3,4-epoxycyclohexanecarboxylate, diglycidyl hexahydrophthalate, and mixtures of two or more of them. More preferably, the epoxy resin contains bisphenol A diglycidyl ether and / or bisphenol F diglycidyl ether. More preferably, the epoxy resin consists of bisphenol A diglycidyl ether and / or bisphenol F diglycidyl ether.

[0069] When one or more thermosetting reactive compounds contain one or more melamine formaldehyde resins, the melamine formaldehyde resin preferably contains an aqueous melamine resin mixture with a resin content in the range of 50 to 70% by mass based on 100% by mass of the aqueous melamine resin mixture, and melamine and formaldehyde are present in the resin in a molar ratio of 1:3 to 1:1, preferably 1:1.3 to 1:2.0, more preferably 1:1.5 to 1:1.7.

[0070] Furthermore, when one or more thermosetting reactive compounds contain one or more melamine formaldehyde resins, the melamine formaldehyde resin contains 1 to 10% by mass of a polyhydric alcohol, more preferably 3 to 6% by mass of a polyhydric alcohol, and more preferably C2 to C 12 3 to 6% by mass of a diol, more preferably 3 to 6% by mass of one or more compounds selected from the group consisting of diethylene glycol, propylene glycol, butylene glycol, pentanediol, hexanediol, and mixtures of two or more thereof, and more preferably 3 to 6% by mass of diethylene glycol.

[0071] Furthermore, when one or more thermosetting reactive compounds contain one or more melamine formaldehyde resins, the melamine formaldehyde resin preferably contains 0 to 8% by mass of caprolactam and 0.5 to 10% by mass of 2-(2-phenoxyethoxy)-ethanol and / or polyethylene glycol having an average molecular weight of 200 to 1,500, respectively, based on 100% by mass of the melamine formaldehyde resin.

[0072] In (4), the mixture is preferably homogenized for a time in the range of 3 to 120 seconds, more preferably 4 to 90 seconds, more preferably 6 to 60 seconds, more preferably 8 to 40 seconds, more preferably 10 to 30 seconds, more preferably 12 to 25 seconds, and more preferably 15 to 20 seconds.

[0073] In (5), the slurry is preferably homogenized for a time in the range of 10 to 120 seconds, more preferably 15 to 100 seconds, more preferably 20 to 80 seconds, more preferably 30 to 60 seconds, and more preferably 40 to 50 seconds.

[0074] The mass ratio of the total amount of one or more thermosetting reactive compounds to the asphalt composition is preferably in the range of 0.1:99.9 to 25:75, more preferably 0.3:99.7 to 15:85, more preferably 0.5:99.5 to 10:90, more preferably 0.8:99.2 to 7:93, more preferably 1:99 to 5:95, more preferably 1.3:98.7 to 4:96, more preferably 1.5:98.5 to 3.5:96.5, more preferably 1.8:98.2 to 3.2:96.8, more preferably 2:98 to 3:97, more preferably 2.2:97.8 to 2.8:97.2, more preferably 2.4:97.6 to 2.6:97.4.

[0075] (4) The mass ratio of the mixture obtained in (4) to the granular material obtained in (2) is preferably in the range of 0.5:99.5 to 25:75, more preferably 1:99 to 20:80, more preferably 1.5:98.5 to 15:85, more preferably 2:98 to 10:90, more preferably 2.5:97.5 to 7:93, more preferably 3:97 to 5:95, more preferably 3.5:96.5 to 4.5:95.5.

[0076] (2) The granular material prepared in (2) is selected from the group consisting of gravel, recycled asphalt pavement material, sand, one or more filler materials, and mixtures of two or more thereof, more preferably from the group consisting of limestone, basalt, diabase, recycled asphalt pavement material, and mixtures of two or more thereof, more preferably from the group consisting of limestone, basalt, diabase, recycled asphalt pavement material, and mixtures of two or more thereof, and preferably contains one or more granular materials selected therefrom.

[0077] (1) The asphalt composition prepared in (1) preferably contains one or more additives, more preferably one or more fiber materials and / or one or more recycling additives. The asphalt composition prepared in (1) particularly preferably contains cellulose fibers. According to the present invention, fiber materials, recycling additives, and cellulose fibers are considered additives.

[0078] When the asphalt composition prepared in (1) contains one or more additives, the asphalt composition prepared in (1) preferably contains one or more additives in an amount of 10% by mass or less, preferably 5% by mass or less, more preferably 3% by mass or less, more preferably 2% by mass or less, more preferably 1% by mass or less, more preferably 0.5% by mass or less, based on 100% by mass of the asphalt composition. More preferably, the asphalt composition contains one or more additives in an amount of 0.1% by mass or less based on 100% by mass of the asphalt composition.

[0079] The granular material prepared in (2) preferably contains 5 to 100% by mass, more preferably 10 to 90% by mass, more preferably 15 to 80% by mass, more preferably 20 to 70% by mass, more preferably 25 to 60% by mass, more preferably 30 to 50% by mass, more preferably 35 to 45% by mass of the recycled asphalt pavement material, based on 100% by mass of the granular material.

[0080] There is no specific limitation on the particle size of the granular material prepared in (2). The granular material prepared in (2) preferably has a particle size in the range of 0.1 to 70 mm, more preferably 0.3 to 50 mm, more preferably 0.5 to 40 mm, more preferably 1 to 30 mm, more preferably 3 to 25 mm, more preferably 5 to 20 mm, more preferably 7 to 15 mm, more preferably 8 to 11 mm.

[0081] The addition in (4) is preferably carried out by introducing at least a part of one or more thermosetting reactive compounds into at least a part of the asphalt composition. The introduction is particularly preferably carried out using an injection pump.

[0082] The addition in (4) is preferably carried out in a receiver tank, more preferably a weighted receiver tank.

[0083] When the addition in (4) is carried out in a receiver tank or a weighted receiver tank, it is preferable to add the asphalt composition obtained in (1) to the receiver tank or the weighted receiver tank before adding one or more thermosetting reactive compounds.

[0084] The homogenization in (4) is preferably carried out using one or more dynamic mixers, more preferably using one or more circulation pumps, and / or high-shear mixers, and / or one or more stirrers, and / or one or more screws, and more preferably using one or more stirrers.

[0085] The homogenization in (4) is preferably carried out using one or more static mixers, more preferably using one or more nozzles, and / or Sulzer mixers, and / or Kenics mixers.

[0086] The homogenization in (4) is preferably carried out at least partially within a mixing unit, more preferably within a weighted stirred vessel.

[0087] The homogenization in (4) is preferably carried out by mixing. When the homogenization in (4) is carried out by mixing, the mixing speed is preferably in the range of 30 to 12,000 rpm, more preferably 50 to 8,000 rpm, more preferably 100 to 5,000 rpm, more preferably 300 to 4,000 rpm, more preferably 500 to 3,000 rpm, more preferably 800 to 2,500 rpm, more preferably 1,000 to 2,000 rpm, more preferably 1,200 to 1,800 rpm, more preferably 1,400 to 1,600 rpm.

[0088] The addition in (5) is preferably carried out by introducing at least a part of the mixture obtained in (4) into at least a part of the granular material obtained in (2). The addition in (5) is particularly preferably carried out by introducing at least a part of the mixture obtained in (4) into at least a part of the granular material obtained in (2) using an injection pump.

[0089] The homogenization in (5) is preferably carried out using one or more dynamic mixers, more preferably using one or more agitators and / or one or more screws, and even more preferably using a twin - shaft compulsion mixer (twin - shaft pugmill).

[0090] The homogenization in (5) is preferably carried out in a mixing device. It is particularly preferred that the mixing device is part of an asphalt mixing plant.

[0091] When the homogenization in (5) is carried out in a mixing device, it is preferable to add the granular material obtained in (2) to the mixing device before adding the mixture obtained in (4).

[0092] In (4), it is preferable that the addition and homogenization are carried out simultaneously.

[0093] In (5), it is preferable that the addition and homogenization are carried out simultaneously.

[0094] (4) and / or (5), more preferably (4) and (5), are preferably carried out in an oxygen - containing atmosphere, more preferably in an atmosphere containing oxygen in an amount of 1 - 21% by volume, more preferably 5 - 21% by volume, and even more preferably 10 - 21% by volume. (4) and / or (5), more preferably (4) and (5), are particularly preferably carried out in air.

[0095] (4) and / or (5), more preferably (4) and (5), are preferably carried out as a batch process or a continuous process. (4) and / or (5), more preferably (4) and (5), are particularly preferably carried out as a continuous process.

[0096] Furthermore, the present invention relates to an asphalt mixture composition obtained or obtainable according to the method described in any one of the embodiments disclosed herein.

[0097] Furthermore, the present invention relates to the use of the asphalt mixture composition described in any one of the embodiments disclosed herein for paving applications.

[0098] The present invention is further illustrated by the following series of embodiments and combinations of embodiments resulting from the dependencies and cross-references shown. In particular, in each case where the scope of an embodiment is referred to, for example, in the context of terms such as "a method according to any one of Embodiments 1 to 4", it should be noted that all embodiments within this scope are intended to be explicitly disclosed to those skilled in the art. That is, this turn of phrase should be understood by those skilled in the art as being synonymous with "a method according to any one of Embodiments 1, 2, 3, and 4". Furthermore, it should be clearly noted that the following series of embodiments do not represent a claim set for determining the scope of protection, but rather a preferably structured part of the description of the general and preferred aspects of the present invention.

[0099] 1. A method for preparing an asphalt mixture composition, comprising: (1) preparing an asphalt composition and heating the composition to a temperature in the range of 110 to 200 °C; (2) preparing a granular material and heating the material to a temperature in the range of 110 to 240 °C; (3) preparing one or more thermosetting reactive compounds; (4) adding the one or more thermosetting reactive compounds prepared in (3) to the asphalt composition obtained in (1) and homogenizing the mixture for a time in the range of 2 to 180 seconds; (5) adding the mixture obtained in (4) to the granular material obtained in (2) and homogenizing the slurry for a time in the range of 5 to 180 seconds, wherein the temperature of the homogenized slurry obtained in (5) is preferably in the range of 110 to 200 °C, more preferably in the range of 130 to 197 °C, more preferably in the range of 150 to 195 °C, more preferably in the range of 170 to 192 °C, more preferably in the range of 175 to 190 °C, more preferably in the range of 180 to 185 °C.

[0100] 2. The method according to embodiment 1, wherein the total time starting from the addition of the thermosetting reactive compound in (4) until the homogenized slurry in (5) is obtained is in the range of 10 seconds to 7 days, preferably in the range of 10 seconds to 3 days, more preferably in the range of 15 seconds to 1 day, more preferably in the range of 15 seconds to 12 hours, more preferably in the range of 20 seconds to 6 hours, more preferably in the range of 20 seconds to 1 hour, more preferably in the range of 25 seconds to 30 minutes, more preferably in the range of 25 seconds to 15 minutes, more preferably in the range of 30 seconds to 6 minutes, more preferably in the range of 30 seconds to 3 minutes, more preferably in the range of 35 seconds to 2 minutes, more preferably in the range of 35 seconds to 90 seconds, more preferably in the range of 40 seconds to 85 seconds, more preferably in the range of 45 seconds to 70 seconds, more preferably in the range of 50 seconds to 60 seconds.

[0101] 3. The method according to embodiment 1 or 2, wherein after (4) and before (5), the mixture obtained in (4) is stored at a temperature in the range of 60 to 190 °C, preferably in the range of 70 to 185 °C, more preferably in the range of 80 to 180 °C, more preferably in the range of 90 to 175 °C, more preferably in the range of 110 to 170 °C, more preferably in the range of 130 to 165 °C, more preferably in the range of 150 to 160 °C.

[0102] 4. After (4) and before (5), the mixture obtained in (4) is stored for a time in the range of 0 seconds to 7 days, preferably 5 seconds to 3 days, more preferably 10 seconds to 1 day, more preferably 15 seconds to 12 hours, more preferably 20 seconds to 6 hours, more preferably 25 seconds to 1 hour, more preferably 30 seconds to 30 minutes, more preferably 35 seconds to 15 minutes, more preferably 40 seconds to 6 minutes, more preferably 45 seconds to 3 minutes, more preferably 50 seconds to 2 minutes, more preferably 55 seconds to 90 seconds, and most preferably 60 seconds to 70 seconds, according to the method according to any one of Embodiments 1 to 3.

[0103] 5. After (4) and before (5), the mixture obtained in (4) is mixed at a mixing speed of 100 rpm or less, preferably 50 rpm or less, more preferably 25 rpm or less, more preferably 20 rpm or less, more preferably 15 rpm or less, more preferably 10 rpm or less, more preferably 5 rpm or less, more preferably 3 rpm or less, according to the method according to any one of Embodiments 1 to 4.

[0104] 6. After (4) and before (5), the mixture obtained in (4) is not mixed, preferably the mixture obtained in (4) is not homogenized after (4) and before (5), according to the method according to any one of Embodiments 1 to 4.

[0105] 7. The mixture obtained in (4) is directly treated in (5), according to the method according to Embodiment 1.

[0106] 8. In (1), the asphalt composition is heated to a temperature in the range of 130 to 197 °C, preferably 150 to 195 °C, more preferably 170 to 192 °C, more preferably 175 to 190 °C, more preferably 180 to 185 °C, according to the method according to any one of Embodiments 1 to 7.

[0107] 9. In (2), the granular material is heated to a temperature in the range of 130 to 220 °C, preferably 150 to 200 °C, more preferably 170 to 195 °C, more preferably 175 to 190 °C, more preferably 180 to 185 °C, according to the method according to any one of Embodiments 1 to 8.

[0108] 10. The homogenization in (5) is carried out at a temperature in the range of 110 to 200 °C, preferably 130 to 195 °C, more preferably 150 to 190 °C, more preferably 170 to 185 °C, more preferably 175 to 180 °C, according to the method described in any one of Embodiments 1 to 9.

[0109] 11. The penetration of the asphalt composition prepared in (1) is selected from the group consisting of 20 to 30, 30 to 45, 35 to 50, 40 to 60, 50 to 70, 70 to 100, 100 to 150, 160 to 220, and 250 to 330, more preferably from the group consisting of 30 to 45, 35 to 50, 40 to 60, 50 to 70, 70 to 100, 100 to 150, and 160 to 220, more preferably from the group consisting of 40 to 60, 50 to 70, 70 to 100, and 100 to 150, more preferably, the penetration of the asphalt composition prepared in (1) is 50 to 70 or 70 to 100, and the penetration is determined in accordance with DIN EN 1426, according to the method described in any one of Embodiments 1 to 10.

[0110] 12. The asphalt composition prepared in (1) contains a modified bitumen, preferably a polymer-modified bitumen, more preferably, the asphalt composition prepared in (1) consists of a modified bitumen, more preferably a polymer-modified bitumen, according to the method described in any one of Embodiments 1 to 11.

[0111] 13. The bitumen is modified with one or more compounds selected from the group consisting of a thermoplastic elastomer, a latex, a thermoplastic polymer, a thermosetting polymer, and a mixture of two or more of them, according to the method described in Embodiment 12.

[0112] 14. The method according to embodiment 13, wherein the thermoplastic elastomer is selected from the group consisting of styrene-butadiene elastomer (SBE), styrene-butadiene-styrene (SBS), styrene-butadiene rubber (SBR), styrene-isoprene-styrene (SIS), styrene-ethylene-butadiene-styrene (SEBS), ethylene-propylene-diene terpolymer (EPDT), isobutene-isoprene copolymer (IIR), polyisobutene (PIB), polybutadiene (PBD), polyisoprene (PI), and mixtures of two or more thereof.

[0113] 15. The method according to embodiment 13 or 14, wherein the latex is natural rubber.

[0114] 16. The method according to any one of embodiments 13 to 15, wherein the thermoplastic polymer is selected from the group consisting of ethylene-vinyl acetate (EVA), ethylene-methyl acrylate (EMA), ethylene-butyl acrylate (EBA), atactic polypropylene (APP), polyethylene (PE), polypropylene (PP), polyvinyl chloride (PVC), polystyrene (PS), and mixtures of two or more thereof.

[0115] 17. The method according to any one of embodiments 13 to 16, wherein the thermosetting polymer is selected from the group consisting of epoxy resins, polyurethane resins, acrylic resins, phenolic resins, and mixtures of two or more thereof.

[0116] 18. The modified bitumen is modified using one or more compounds selected from the group consisting of chemical modifiers (e.g., organometallic compounds, sulfur, phosphoric acid (PA), polyphosphoric acid (PPA), sulfonic acid, sulfuric acid, carboxylic anhydride, acid ester, dibenzoyl peroxide, silane, organic and inorganic urea sulfides), recycled materials (e.g., crumb rubber, plastic), fibers (e.g., lignin, cellulose, glass fiber, magnesium aluminosilicate, polyester, polypropylene), adhesion enhancers (e.g., organic amines, amides), natural asphalt (e.g., Trinidad Lake Asphalt (TLA), gilsonite, rock asphalt), antioxidants (e.g., phenols, organic zinc compounds, organic lead compounds), fillers (e.g., carbon black, slaked lime, lime, fly ash), viscosity modifiers (e.g., flux oil, wax), reactive polymers (e.g., random terpolymers of ethylene, acrylate ester and glycidyl methacrylate, maleic anhydride grafted styrene-butadiene-styrene copolymer), and mixtures of two or more thereof), the method according to any one of embodiments 12 to 17.

[0117] 19. One or more thermosetting reactive compounds include one or more compounds selected from the group consisting of polyisocyanates, epoxy resins, melamine formaldehyde resins, and mixtures of two or more thereof, preferably from the group consisting of fatty acid polyisocyanates, araliphatic polyisocyanates, aromatic polyisocyanates, and mixtures of two or more thereof, more preferably from the group consisting of aromatic diisocyanates, oligomeric aromatic polyisocyanates, and mixtures of two or more thereof, more preferably, one or more thermosetting reactive compounds include a mixture of one or more aromatic diisocyanates and one or more oligomeric aromatic polyisocyanates, more preferably, one or more thermosetting reactive compounds consist of a mixture of one or more aromatic diisocyanates and one or more oligomeric aromatic polyisocyanates, the method according to any one of embodiments 1 to 18.

[0118] 20. The aliphatic polyisocyanate contains one or more compounds selected from the group consisting of alkylene diisocyanates having an alkylene group with 4 to 12 carbon atoms, and mixtures of two or more thereof, 1,12-dodecane diisocyanate, 2-ethyltetramethylene diisocyanate-1,4, 2-methylpentamethylene diisocyanate-1,5, tetramethylene diisocyanate-1,4, hexamethylene diisocyanate-1,6, trimethyldiisocyanate, tetramethyldiisocyanate, pentamethyldiisocyanate, hexamethyldiisocyanate, heptamethyldiisocyanate, octamethyldiisocyanate, 2-methylpentamethylene-1,5-diisocyanate, 2-ethylbutylene-1,4-diisocyanate, pentamethylene-1,5-diisocyanate, butylene-1,4-diisocyanate, and more preferably, the aliphatic polyisocyanate contains hexamethylene diisocyanate-1,6, and more preferably, the aliphatic polyisocyanate consists of hexamethylene diisocyanate-1,6, the method according to Embodiment 19.

[0119] 21. The aliphatic polyisocyanate is selected from the group consisting of 1-isocyanato-3,3,5-trimethyl-5-isocyanatomethyl-cyclohexane (isophorone diisocyanate, IPDI), 1,4-bis(isocyanatomethyl)cyclohexane and / or 1,3-bis(isocyanatomethyl)cyclohexane (HXDI), 1,4-cyclohexane diisocyanate, 1-methyl-2,4- and / or -2,6-cyclohexane diisocyanate, 4,4'-dicyclohexylmethane diisocyanate, 2,2'-dicyclohexylmethane diisocyanate, 2,4'-dicyclohexylmethane diisocyanate, cyclohexane-1,3-diisocyanate, cyclohexane-1,4-diisocyanate, 2,4-hexahydrotoluene diisocyanate, 2,6-hexahydrotoluene diisocyanate, 4,4'-dicyclohexylmethane diisocyanate, 2,2'-dicyclohexylmethane diisocyanate, 2,4'-dicyclohexylmethane diisocyanate, and mixtures of two or more thereof; preferably, one or more alicyclic compounds selected from the group consisting of 1-isocyanato-3,3,5-trimethyl-5-isocyanatomethyl-cyclohexane (isophorone diisocyanate, IPDI), 1,4-bis(isocyanatomethyl)cyclohexane and / or 1,3-bis(isocyanatomethyl)cyclohexane (HXDI), 1,4-cyclohexane diisocyanate, 1-methyl-2,4- and / or -2,6-cyclohexane diisocyanate, and 4,4'-dicyclohexylmethane diisocyanate, 2,2'-dicyclohexylmethane diisocyanate, 2,4'-dicyclohexylmethane diisocyanate, and mixtures of two or more thereof, in the method according to embodiment 19 or 20.

[0120] 22. The aromatic polyisocyanate, and preferably the aromatic diisocyanate, is selected from the group consisting of 2,4-toluene diisocyanate, 2,6-toluene diisocyanate, 4,4'-diphenylmethane diisocyanate, 2,4'-diphenylmethane diisocyanate, 2,2'-diphenylmethane diisocyanate, 1,5-naphthylene diisocyanate (NDI), 3,3'-dimethyl diphenyl diisocyanate, 1,2-diphenylethane diisocyanate, p-phenylene diisocyanate (PPDI), and mixtures of two or more thereof; preferably from the group consisting of 2,4-toluene diisocyanate (2,4-TDI), 2,6-toluene diisocyanate (2,6-TDI), 4,4'-diphenylmethane diisocyanate (4,4'-MDI), 2,4'-diphenylmethane diisocyanate (2,4'-MDI), 2,2'-diphenylmethane diisocyanate (2,2'-MDI), crude MDI obtained by MDI preparation, and mixtures of two or more thereof; more preferably from the group consisting of 4,4'-diphenylmethane diisocyanate, 2,4'-diphenylmethane diisocyanate, 2,2'-diphenylmethane diisocyanate, and mixtures of two or more thereof (a mixture of isomers 4,4'-, 2,4'- and 2,2'-diphenylmethane diisocyanate is also called monomeric diphenylmethane or MMDI); more preferably, the aromatic polyisocyanate, and preferably the aromatic diisocyanate, contains a mixture of 4,4'-diphenylmethane diisocyanate, 2,4'-diphenylmethane diisocyanate, and 2,2'-diphenylmethane diisocyanate; more preferably, the aromatic polyisocyanate, and preferably the aromatic diisocyanate, consists of a mixture of 4,4'-diphenylmethane diisocyanate, 2,4'-diphenylmethane diisocyanate, and 2,2'-diphenylmethane diisocyanate, and is the method according to any one of Embodiments 19 to 21.

[0121] 23. The method according to any one of embodiments 19 to 22, wherein the polyisocyanate is a modified polyisocyanate containing one or more ester, urea, biuret, allophanate, carbodiimide, isocyanurate, uretdione, carbamate and / or urethane groups, preferably a modified organic polyisocyanate, more preferably a modified organic polyisocyanate.

[0122] 24. The oligomeric aromatic polyisocyanate is selected from the group consisting of polyphenylpolymethylene polyisocyanate, polyphenylethylene polyisocyanate, and mixtures of two or more thereof, preferably one or more compounds selected from the group consisting of one or more polymethylene polyphenyl isocyanates, polyethylene polyphenyl isocyanates, and mixtures of two or more thereof, more preferably the aromatic polyisocyanate contains one or more polymethylene polyphenyl isocyanates, and even more preferably the aromatic polyisocyanate consists of one or more polymethylene polyphenyl isocyanates. The method according to any one of embodiments 19 to 23.

[0123] 25. The oligomeric aromatic polyisocyanate contains one or more oligomers composed of one or more of 4,4'-diphenylmethane diisocyanate, 2,4'-diphenylmethane diisocyanate, and 2,2'-diphenylmethane diisocyanate, and homologues with larger cores. The homologues with larger cores have at least three aromatic nuclei and at least three functional groups. The method according to any one of embodiments 19 to 24.

[0124] 26. One or more thermosetting reactive compounds are polymeric MDI, and the total amount of 4,4'-MDI in the polymeric MDI ranges from 26 to 98% by mass, preferably from 30 to 95% by mass, more preferably from 35 to 92% by mass, based on 100% by mass of one or more thermosetting reactive compounds. The method according to any one of embodiments 19 to 25.

[0125] 27. The method according to any one of Embodiments 19 to 26, wherein one or more thermosetting reactive compounds are polymeric MDI, and the bicyclic content of the polymeric MDI is in the range of 20 to 62%, more preferably in the range of 26 to 48%, and most preferably in the range of 26 to 48% based on 100% by mass of the polymeric MDI.

[0126] 28. The method according to any one of Embodiments 19 to 27, wherein the average functionality of the isocyanate groups in one or more thermosetting reactive compounds, and preferably in the total polyisocyanate contained in the compound, is 2.1 to 3.5, preferably 2.3 to 3.2, more preferably 2.4 to 3, more preferably 2.5 to 2.9, and more preferably 2.6 to 2.8.

[0127] 29. The method according to any one of Embodiments 1 to 28, wherein the iron content of one or more thermosetting reactive compounds is in the range of 1 to 100 wppm, preferably 1 to 80 wppm, more preferably 1 to 60 wppm, more preferably 1 to 40 wppm, more preferably 1 to 20 wppm, more preferably 1 to 10 wppm, and more preferably 1 to 5 wppm.

[0128] 30. The method according to any one of Embodiments 1 to 29, wherein one or more thermosetting reactive compounds exhibit a viscosity in the range of 100 to 3,000 mPa·s, preferably 100 to 1,000 mPa·s, more preferably 100 to 600 mPa·s, more preferably 200 to 600 mPa·s, and more preferably 400 to 600 mPa·s, and the viscosity is the viscosity measured at 25°C.

[0129] 31. The epoxy resin is one or more compounds selected from the group consisting of aromatic epoxy resins, alicyclic epoxy resins, and mixtures of two or more of them, preferably bisphenol A diglycidyl ether (DGEBA), bisphenol F diglycidyl ether, cyclo-hydrogenated bisphenol A diglycidyl ether, cyclo-hydrogenated bisphenol F diglycidyl ether, bisphenol S diglycidyl ether (DGEBS), tetraglycidyl methylene dianiline (TGMDA), epoxy novolac (reaction product from epichlorohydrin and phenol resin (novolac)), 3,4-epoxycyclohexylmethyl, 3,4-epoxycyclohexanecarboxylate, diglycidyl hexahydrophthalate, and mixtures of two or more of them, more preferably the epoxy resin contains bisphenol A diglycidyl ether and / or bisphenol F diglycidyl ether, and more preferably the epoxy resin consists of bisphenol A diglycidyl ether and / or bisphenol F diglycidyl ether, the method according to any one of embodiments 19 to 30.

[0130] 32. The melamine formaldehyde resin contains an aqueous melamine resin mixture in which the resin content ranges from 50 to 70% by mass based on 100% by mass of the aqueous melamine resin mixture, and melamine and formaldehyde are present in the resin in a molar ratio of 1:3 to 1:1, preferably 1:1.3 to 1:2.0, more preferably 1:1.5 to 1:1.7, the method according to any one of embodiments 19 to 31.

[0131] 33. The melamine formaldehyde resin contains 1 to 10% by mass of a polyhydric alcohol, preferably 3 to 6% by mass of a polyhydric alcohol, more preferably C2 to C 12The method according to any one of Embodiments 19 to 32, containing 3 to 6% by mass of a diol, more preferably one or more compounds selected from the group consisting of diethylene glycol, propylene glycol, butylene glycol, pentanediol, hexanediol, and mixtures of two or more thereof in an amount of 3 to 6% by mass, and more preferably 3 to 6% by mass of diethylene glycol.

[0132] 34. The method according to any one of Embodiments 19 to 33, wherein the melamine formaldehyde resin contains 0 to 8% by mass of caprolactam and 0.5 to 10% by mass of 2-(2-phenoxyethoxy)-ethanol and / or polyethylene glycol having an average molecular weight of 200 to 1,500, respectively, based on 100% by mass of the melamine formaldehyde resin.

[0133] 35. In (4), the method according to any one of Embodiments 1 to 34, wherein the mixture is homogenized for a time in the range of 3 to 120 seconds, preferably 4 to 90 seconds, more preferably 6 to 60 seconds, more preferably 8 to 40 seconds, more preferably 10 to 30 seconds, more preferably 12 to 25 seconds, more preferably 15 to 20 seconds.

[0134] 36. In (5), the method according to any one of Embodiments 1 to 35, wherein the slurry is homogenized for a time in the range of 10 to 120 seconds, preferably 15 to 100 seconds, more preferably 20 to 80 seconds, more preferably 30 to 60 seconds, more preferably 40 to 50 seconds.

[0135] The method according to any one of Embodiments 1 to 36, wherein the mass ratio of the total amount of one or more thermosetting reactive compounds to the asphalt composition is in the range of 0.1:99.9 to 25:75, preferably 0.3:99.7 to 15:85, more preferably 0.5:99.5 to 10:90, more preferably 0.8:99.2 to 7:93, more preferably 1:99 to 5:95, more preferably 1.3:98.7 to 4:96, more preferably 1.5:98.5 to 3.5:96.5, more preferably 1.8:98.2 to 3.2:96.8, more preferably 2:98 to 3:97, more preferably 2.2:97.8 to 2.8:97.2, more preferably 2.4:97.6 to 2.6:97.4.

[0136] The method according to any one of Embodiments 1 to 37, wherein the mass ratio of the mixture obtained in (4) to the granular material obtained in (2) is in the range of 0.5:99.5 to 25:75, preferably 1:99 to 20:80, more preferably 1.5:98.5 to 15:85, more preferably 2:98 to 10:90, more preferably 2.5:97.5 to 7:93, more preferably 3:97 to 5:95, more preferably 3.5:96.5 to 4.5:95.5.

[0137] The method according to any one of Embodiments 1 to 38, wherein the granular material prepared in (2) comprises one or more granular materials selected from the group consisting of gravel, recycled asphalt pavement material, sand, one or more filler materials, and mixtures of two or more of them, preferably selected from the group consisting of limestone, basalt, diabase, recycled asphalt pavement material, and mixtures of two or more of them, more preferably selected from the group consisting of limestone, basalt, diabase, recycled asphalt pavement material, and mixtures of two or more of them.

[0138] The method according to any one of Embodiments 1 to 39, wherein the asphalt composition prepared in (1) contains one or more additives, preferably one or more fiber materials and / or one or more recycling additives, and more preferably the asphalt composition prepared in (1) contains cellulose fibers.

[0139] 41. The asphalt composition prepared in (1) contains 10% by mass or less, preferably 5% by mass or less, more preferably 3% by mass or less, more preferably 2% by mass or less, more preferably 1% by mass or less, more preferably 0.5% by mass or less, and more preferably 0.1% by mass or less of one or more additives with respect to 100% by mass of the asphalt composition. The method according to embodiment 40.

[0140] 42. The granular material prepared in (2) contains 5 to 100% by mass of recycled asphalt pavement material with respect to 100% by mass of the granular material, and more preferably, the granular material contains 10 to 90% by mass, more preferably 15 to 80% by mass, more preferably 20 to 70% by mass, more preferably 25 to 60% by mass, more preferably 30 to 50% by mass, and more preferably 35 to 45% by mass of recycled asphalt pavement material with respect to 100% by mass of the granular material. The method according to any one of embodiments 1 to 41.

[0141] 43. The granular material prepared in (2) exhibits a particle size in the range of 0.1 to 70 mm, preferably 0.3 to 50 mm, more preferably 0.5 to 40 mm, more preferably 1 to 30 mm, more preferably 3 to 25 mm, more preferably 5 to 20 mm, more preferably 7 to 15 mm, and more preferably 8 to 11 mm. The method according to any one of embodiments 1 to 42.

[0142] 44. The addition in (4) is carried out by introducing at least a part of one or more thermosetting reactive compounds into at least a part of the asphalt composition, and the introduction is preferably carried out using an injection pump. The method according to any one of embodiments 1 to 43.

[0143] 45. The addition in (4) is carried out in a receiver tank, preferably a weighted receiver tank. The method according to any one of embodiments 1 to 44.

[0144] The method according to embodiment 45, wherein the asphalt composition obtained in (1) is added to a receiver tank before the addition of one or more thermosetting reactive compounds.

[0145] 47. The method according to any one of embodiments 1 to 46, wherein the homogenization in (4) is carried out using one or more dynamic mixers, preferably using one or more circulation pumps, and / or high-shear mixers, and / or one or more stirrers, and / or one or more screws, preferably using one or more stirrers.

[0146] 48. The method according to any one of embodiments 1 to 47, wherein the homogenization in (4) is carried out using one or more static mixers, preferably using one or more nozzles, and / or Sulzer mixers, and / or Kenics mixers.

[0147] 49. The method according to any one of embodiments 1 to 48, wherein the homogenization in (4) is carried out at least partially inside a mixing unit, preferably inside a weighted stirring tank.

[0148] 50. The method according to any one of embodiments 1 to 49, wherein the homogenization in (4) is carried out by mixing, preferably with a mixing speed in the range of 30 to 12,000 rpm, preferably 50 to 8,000 rpm, more preferably 100 to 5,000 rpm, more preferably 300 to 4,000 rpm, more preferably 500 to 3,000 rpm, more preferably 800 to 2,500 rpm, more preferably 1,000 to 2,000 rpm, more preferably 1,200 to 1,800 rpm, more preferably 1,400 to 1,600 rpm.

[0149] 51. The method according to any one of embodiments 1 to 50, wherein the addition in (5) is carried out by introducing at least a part of the mixture obtained in (4) into at least a part of the granular material obtained in (2), and the introduction is preferably carried out using an injection pump.

[0150] The homogenization in (5) is carried out using one or more dynamic mixers, preferably using one or more stirrers and / or one or more screws, more preferably using a twin-shaft compulsion mixer (twin-shaft pugmill), according to any one of Embodiments 1 to 51.

[0151] The homogenization in (5) is carried out in a mixing device, preferably the mixing device is part of an asphalt mixing plant, according to any one of Embodiments 1 to 52.

[0152] Before adding the mixture obtained in (4), the granular material obtained in (2) is added to the mixing device, according to the method described in Embodiment 53.

[0153] In (4), the addition and homogenization are carried out simultaneously, according to any one of Embodiments 1 to 54.

[0154] In (5), the addition and homogenization are carried out simultaneously, according to any one of Embodiments 1 to 55.

[0155] In (4) and / or (5), preferably (4) and (5), are carried out in an oxygen-containing atmosphere, preferably an atmosphere containing oxygen in an amount of 1 to 21% by volume, more preferably 5 to 21% by volume, even more preferably 10 to 21% by volume, and more preferably (4) and / or (5), preferably (4) and (5) are carried out in air, according to any one of Embodiments 1 to 56.

[0156] In (4) and / or (5), preferably (4) and (5) are carried out as a batch process or a continuous process, preferably as a continuous process, according to any one of Embodiments 1 to 57.

[0157] An asphalt mixing composition obtained by the method according to any one of Embodiments 1 to 58.

[0158] Use of the asphalt mixture composition according to Embodiment 59 for paving applications.

[0159] The present invention is further illustrated by the following examples and reference examples.

[0160] Experimental section Characteristic evaluation method - Asphalt test Softening point DIN EN 1427 Two bitumen horizontal discs placed in a copper ring of seated type are heated in a liquid bath at a controlled rate while each supports a steel ball. The softening point is reported as the average of the temperatures at which the two discs soften such that each ball enclosed by the bitumen drops a distance of 25 ± 0.4 mm.

[0161] Rotary thin - film heating test (RTFOT) DIN EN 12607 - 1 The bitumen is heated in a bottle in an oven at 163 °C for 75 minutes. The bottle rotates at 15 rpm and heated air is blown in at 4,000 mL / min at the lowest point of travel of each bottle. The effects of heat and air are determined from the changes in physical test values measured before and after the oven treatment.

[0162] Pressure aging test (PAV) DIN EN 14769 The residue from RTFOT is placed in a standard stainless - steel pan and aged for 20 hours at a specified conditioning temperature (90 °C, 100 °C, or 110 °C) in a container pressurized with air to 2.10 MPa. The temperature is selected according to the grade (application) of the asphalt binder. Finally, the residue is vacuum - degassed.

[0163] Dynamic shear rheometer (DSR) DIN EN 14770 - ASTM D7175 The dynamic shear rheometer test system consists of parallel plates, means for controlling the specimen temperature, a loading device, and a control and data acquisition system.

[0164] Temperature sweep DIN EN 14770 This test aims to measure the complex shear modulus and phase angle of asphalt binders. The test consists of applying pressure to specimens with a diameter of 8 or 25 mm between parallel metal plates at specified frequencies and temperatures. One parallel plate vibrates with respect to the other parallel plate at 1.59 Hz and a deflection angle amplitude in this case. It is necessary to select the required amplitude so that the test falls within the region of linear behavior. The test is repeated at 30, 40, 50, 60, 70, 80, and 90 °C.

[0165] Repeated creep test (MSCRT) DIN EN 16659 - ASTM D7405 This test method is used to measure the elastic response and recovery of asphalt binders under shear creep at two stress levels (0.1 and 3.2 kPa) and a specified temperature (60 °C). In this test, a DSR is used to apply a load of 25 mm for 1 second at a constant stress and then recover for 9 seconds. 10 creep and recovery cycles are performed at a creep stress of 0.100 kPa, followed by 10 cycles at a creep stress of 3.200 kPa.

[0166] Bending beam rheometer (BBR) DIN EN 14771 - ASTM D6648 This test is used to measure the mid - point deflection of a simply - supported prismatic beam of asphalt binder with a constant load applied at the mid - point. The prismatic specimen is placed in a temperature - controlled fluid bath and a constant test load is applied for 240 seconds. A computer - controlled data acquisition system is used to observe the test load (980 ± 50 mN) and the mid - point deflection of the specimen over time. The maximum bending stress at the mid - point of the specimen is calculated from the dimensions of the specimen, the distance between the supports, and the load applied to the specimen at load times of 8.0, 15.0, 30.0, 60.0, 120.0, and 240.0 seconds. The stiffness of the specimen for a specific load time is calculated by dividing the maximum bending stress by the maximum bending strain.

[0167] Characteristic Evaluation Method - Asphalt Mixture Composition Test Repeated Compression Test (CCT) - TP Asphalt-StB Part 25 B1 DIN EN 12697-25:2016 The repeated uniaxial compression test is used to determine the deformation behavior of asphalt specimens. In this test, the specimens are tempered at 50 ± 0.3 °C for 150 ± 10 minutes. This is the same temperature at which the test is carried out. After the tempering period, the specimens are set on a universal testing machine and loaded periodically. Each cycle lasts for 1.7 seconds (loading time 0.2 seconds, pause 1.5 seconds). The upper load applied is 0.35 MPa and the lower load is 0.025 MPa. The number of cycles and the deformation are recorded. The test is terminated either when 10,000 load cycles are completed or when the deformation exceeds 40%.

[0168] Flexural Tensile Strength Test - TP Asphalt-StB Part 23 DIN EN 12697-23:2003 The flexural tensile strength test is used to determine the fatigue behavior of asphalt specimens. The asphalt mixture is processed by applying a load across the entire vertical diameter plane of cylindrical specimens at a specified deformation rate (in this case 50 ± 0.2 mm / min) and test temperature (in this case 20 ± 2 °C). The peak load at failure is recorded and used to calculate the flexural tensile strength of the specimens.

[0169] Uniaxial Tensile Stress Test and Thermal Stress Restrained Specimen Test - TP Asphalt-StB Part 46A (LTT = Low Temperature Tests) DIN EN 12697-46:2012 The uniaxial tensile stress test and the thermal stress restrained specimen test are used to determine the low-temperature behavior of asphalt specimens. Low-temperature cracking of asphalt mixtures is caused by thermal shrinkage during cooling, which induces tensile stress in the asphalt mixture. To simulate the situation of the pavement layer, the following asphalt specimen test methods compliant with European Standard EN 12697-46:2012 are used. (i) Thermal stress restrained specimen test (TSRST): The temperature is decreased at a pre-specified cooling rate while restraining the deformation of the specimen. (ii) Uniaxial tensile strength test (UTST): To evaluate the risk of low-temperature cracking, the stress induced by thermal shrinkage is compared with the respective tensile strength.

[0170] Wheel tracking test - TP Asphalt-StB Teil 22 DIN EN 12697-22:2003 The wheel tracking test is used to determine the rut depth of an asphalt mixture subjected to repeated passes of a loaded rubber wheel under certain controlled temperature conditions. It is usually carried out 10,000 times at 50 °C.

Example

[0171] (Example 1) Preparation of an asphalt mixing composition in an asphalt mixing plant - Short mixing time of asphalt and a thermosetting reactive compound 1,920 kg of coarse gravel with a particle size of 8 - 11 mm is heated to a temperature of 180°C and placed into a mixing unit. 80 kg of asphalt that has been preheated to a temperature of 160 - 170°C and shows a penetration (penetration degree 70 - 100) of 7 - 10 mm in accordance with DIN EN 1426 is weighed into a stirring container. Then, 2.075 kg of polymeric diphenylmethane diisocyanate (hereinafter referred to as "As20") with an average functionality of isocyanate groups of 2.7 is added to the asphalt under stirring (1,500 rpm). Next, the resulting mixture is stirred further. Here, the injection rate is set to 0.1 L / s - 2.0 L / s, and the stirring time is set to 20 seconds. Then, the obtained modified asphalt is added to the coarse gravel in the mixing unit while stirring, and then the mixture is stirred further. The total time of further stirring is 30 seconds. The temperature of the obtained asphalt mixture composition was 171.6°C. Subsequently, the modified asphalt was separated from the coarse gravel (by dripping) and further analyzed. The softening point was determined to be 52.4°C.

[0172] (Example 2) Preparation of Asphalt Mixture Composition in Asphalt Mixing Plant - Short Mixing Time of Asphalt and Thermosetting Reactive Compound Example 1 was repeated, and the temperature of the obtained asphalt mixture composition was 173.4°C. Subsequently, the modified asphalt was separated from the coarse gravel (by dripping) and further analyzed. The softening point was determined to be 52.4°C.

[0173] (Comparative Example 1) Preparation of Asphalt Mixture Composition in Asphalt Mixing Plant - Long Mixing Time of Asphalt and Thermosetting Reactive Compound Example 1 was repeated, but the step of adding As20 to the asphalt was changed such that the obtained mixture was stirred for a longer time, and the total duration of further stirring was 300 seconds. The temperature of the obtained asphalt mixture composition was 175.4°C. Subsequently, the modified asphalt was separated from the coarse gravel (by dripping) and further analyzed. The softening point was determined to be 53.9°C.

[0174] (Comparative Example 2) Preparation of Asphalt Mix Composition in Asphalt Mixing Plant - Long Mixing Time of Asphalt and Thermosetting Reactive Compound Example 1 was repeated, but the step of adding As20 to the asphalt was changed such that the obtained mixture was further stirred for a longer time, and the total stirring time was changed to 600 seconds. The temperature of the obtained asphalt mix composition was 172.8 °C. Subsequently, the modified asphalt was separated from the coarse gravel (by dropping) and further analyzed. The softening point was determined to be 53.8 °C.

[0175] (Example 3) Preparation of Asphalt Mix Composition in Asphalt Mixing Plant - Short Mixing Time of Asphalt and Thermosetting Reactive Compound, and Combination with Long Mixing Time of Granular Material and Mixture of Asphalt and Thermosetting Reactive Compound Example 1 was repeated, but the step of adding the modified asphalt to the coarse gravel was changed such that the obtained mixture was further stirred for a longer time, and the total stirring time was changed to 60 seconds. The temperature of the obtained asphalt mix composition was 172.8 °C. Subsequently, the modified asphalt was separated from the coarse gravel (by dropping) and further analyzed. The softening point was determined to be 56.7 °C.

[0176]

Table 1

[0177] (Example 4) Preparation of Asphalt Mix Composition without Mixing Asphalt and As20 Additive In an asphalt mixing plant, various asphalt mixing compositions are prepared. For all mixtures, the amounts of granular materials and asphalt are as follows (the selected particle size curve is SMA 11 S). Sand (particle size 0 - 2 mm) 519 kg, gravel (2 - 5 mm) 282 kg, gravel (5 - 8 mm) 372 kg, gravel (8 - 11 mm) 1,092 kg, gravel (11 - 16 mm) 300 kg, filler 60 kg, limestone 180 kg, cellulose fiber 9 kg, and 186 kg of asphalt showing a penetration of 5 - 7 mm ( = penetration 50 - 70) according to DIN EN 1426 and preheated to a temperature of 170 - 180°C. The granular materials are preheated to a temperature of 182°C.

[0178]

Table 2

[0179] In the comparative example, As20 is not added to the asphalt. When adding As20, 4.65 kg of As20 (2.5% by mass based on the amount of asphalt used) is added to the asphalt in two different ways: a) a method of simultaneously adding As20 and asphalt to the remainder, b) a method of first adding As20 and then adding asphalt. Regardless of the type of addition, stirring of the asphalt - As20 - mixture is not carried out. Then, the obtained mixture / asphalt without the As20 additive is added to the granular materials in the mixing unit while stirring, and then the mixture is stirred further. The total time of further stirring is 30 seconds. For each variant (see Table 2. (1) Without As20 additive, (2) Simultaneous addition of As20 and asphalt to the remainder, (3) First add As20, then add asphalt), two batches were prepared according to the above composition. The temperature of the obtained asphalt mixing composition was between 172°C and 175°C (see Table 2). Subsequently, three different asphalt mixing compositions were further analyzed. The corresponding results are shown in Table 2.

[0180] Surprisingly, it has been found that the mixing time of the thermosetting reactive compound and asphalt before adding to the granular material has substantially no effect on the softening point (i.e., degree of modification) of the resulting asphalt mixture composition. However, as shown in Example 4, mixing is necessary to effect the modification of asphalt. Highly unexpectedly, it has been found that the mixing time of the resulting modified asphalt mixture and coarse gravel substantially raises the softening point of the resulting asphalt mixture. As a result, very surprisingly, it has been found that a product with excellent properties can be obtained by a process of mixing the components of an asphalt mixture composition containing asphalt modified with a thermosetting reactive compound for a very short time. Therefore, the present invention provides a very efficient method for preparing an asphalt mixture composition which not only results in a significant saving of time and energy, but also enables in-line mixing of the components immediately before using the product for paving applications.

[0181] (Reference Example 5) Comparison of unmodified, batch and in-line modified asphalt samples prepared under laboratory conditions General procedure for preparing batch modified asphalt compositions according to the art (comparison) 2.5 kg of each grade of asphalt shown in Table 3 was heated to 140° C. with stirring at 400 rpm in an oil bath (temperature set at 150° C.) in air. When the internal temperature reached 100° C., 50 g of each thermosetting reactive compound shown in Table 3 (2% by mass of As20 based on the amount of asphalt used) was added to the molten asphalt. The reaction was carried out at 140° C. for 420 minutes and then cooled to room temperature. The samples were sent to cans for further testing and stored at room temperature.

[0182] Basic procedure for preparing in-line modified asphalt composition (invention) 350 g of asphalt of each grade shown in Table 3 was heated to 150°C in air inside an oven (temperature set to 150°C). 7 g of each thermosetting reactive compound shown in Table 3 (2 mass% of As2O3 based on the amount of asphalt used) was added to the molten asphalt. The mixture was stirred for a few seconds (<10 seconds) to achieve homogeneity. Next, the sample was divided into portions of 35 g + / - 0.5 g, and a Rolling Thin Film Oven Test (RTFOT, see the section "Characteristic Evaluation Method") for short-term deterioration was carried out. In this test, starting from the mixing process, the deterioration of the asphalt until the asphalt mixture is transported to the construction site and laid is simulated. After deterioration, the modified asphalt is stored at room temperature or used in further tests such as a long-term aging test (PAV, see the section "Characteristic Evaluation Method").

[0183] According to the procedures described for Comparative Example 5 and Example 5 of the present invention, surprisingly, it was found that inline modification of asphalt results in asphalt performance values that are essentially equivalent to those of the batch modification method described in WO 2018 / 228840 A1. Specifically, the values of MSCR and DSR indicate an increase in elasticity and rigidity under high-temperature conditions. At the same time, as can be seen from the BBR values, similar low-temperature performance is obtained. The useful temperature interval (UTI) increases from 80.1°C (unmodified (paving grade) asphalt) to 87.7°C (As2O3-modified asphalt, Example of the present invention). This is essentially the same increase as that achieved by the batch modification method within the error range. (87.9°C).

[0184] [Table 3]

[0185] In conclusion, as can be seen from the comparison of the results of the comparative examples and the examples of the present invention in Table 3, the examples of the present invention and the comparative examples show substantially the same values for the tests conducted. Therefore, and quite surprisingly, even after a very short mixing step of just a few seconds after the addition of the thermosetting reactive compound, the obtained asphalt was found to exhibit the same quality as the asphalt that had been mixed for 7 hours. Considering the large difference in time in the mixing stage between the examples of the present invention and the comparative examples, this is very unexpected.

[0186] (Example 6) Comparison between unmodified, batch, and in-line modified asphalt mixture composition samples prepared under laboratory conditions Preparation of asphalt mixture composition The selected gradation curve was SMA 8 S.

[0187] [Table 4]

[0188] The composition of the granular materials used in the asphalt mixture composition is as follows.

[0189] [Table 5]

[0190] The composition of the asphalt mixture consisting of granular materials, asphalt, and fibers is as follows.

[0191] [Table 6]

[0192] For the preparation of the asphalt mixture composition, the TP Asphalt-StB Part 35 standard was used. The following procedure was followed.

[0193] Mixing of components At a temperature of 150 ± 5 °C, mix the stone mastic asphalt in the following order: 1. Coarse aggregate, 2. Filler and fine aggregate, 3. Fibers, 4. Dry mix for 2 minutes, 5. Stir each unmodified (paving grade) asphalt or modified asphalt separately and then add it to the mixture obtained after performing steps 1 - 4. In the case of the in-line modification example, an additive (2.0% by mass of As20 based on the amount of asphalt used) is added to the unmodified (paving grade) asphalt and stirred for a short time (<60 seconds) to achieve homogeneity. The batch modification example is prepared as described in Example 5 (2.0% by mass of As20 based on the amount of asphalt used). 6. Mix in an asphalt test mixer (not sealed and exposed to air) at 30 rpm for 5 minutes.

[0194] Storage After mixing, store the mixture in air (the storage container is not closed) at a temperature 10 °C higher than the compaction temperature for 1 - 3 hours.

[0195] Manufacture and compaction of specimens For the manufacture and compaction of specimens, the TP Asphalt-StB Part 33 standard was used. This standard describes the procedure for manufacturing specimens in the laboratory using a roller (Walzsektor-Verdichtungsgerat).

[0196] To prepare the specimens, pour the hot mix asphalt mixture onto a plate and compact it using a roller. The plate is 320 mm long, 260 mm wide, and at least 40 mm high. The height of the plate varies depending on the dimensions of the specimens required for a specific test.

[0197] To compact the plate, heat the equipment (machine, mold, press) to 80 °C, and the temperature of the mixture during compaction must meet the following conditions (Table 5 (Table 7)).

[0198]

Table 7

[0199] Cutting of the specimen After plate manufacturing, it is necessary to cut to the required dimensions. The dimensions vary depending on the test.

[0200]

Table 8

[0201] As can be seen from the comparison of the results of the comparative examples and the examples of the present invention in Table 6 (Table 8), the examples of the present invention show substantially the same low-temperature behavior values as compared with the comparative examples. However, regarding the deformation behavior of the samples, the samples of the present invention show better results regarding inflection, and in particular, a lower deformation rate at the inflection point. Therefore, in order to bring about improved results as compared with the use of unmodified (paving grade) asphalt, even if it is not indispensable to bring about substantially improved results, a significantly longer mixing stage is expected. Very unexpectedly, following showing equivalent quality as compared with the materials according to the art, although the mixing step of the asphalt / thermosetting reactive compound mixture by the method of the present invention is very short, the material of the present invention has been found to show even better quality than the materials obtained by the art. Again, considering the large difference in time in the mixing stage between the examples of the present invention and the comparative examples, this is emphasized as being very unexpected.

[0202] (Example 7) Control of experimental results under actual conditions in an asphalt mixing plant equipped with an injection system customized for a thermosetting reactive compound Preparation of the asphalt mixing composition (the selected particle size curve was AC 22 BS) The asphalt mixing plant was equipped with a customized injection system (heatable injection line, injection pump) that enabled the injection of thermosetting reactive compounds into the remaining asphalt (mixing container) in the asphalt mixing plant. Furthermore, the remaining asphalt was equipped with i) a stirrer that was activated when the thermosetting reactive compound was injected and ii) a stirrer that operated when the minimum filling level of asphalt reached 20 kg. The injection amount and rate of the additive, as well as the mixing, were controlled via the process control system of the asphalt mixing plant.

[0203] The management of the experimental results focuses on the change in properties between unmodified (paving grade) asphalt pen70 / 100 (penetration of 7 - 10 mm in accordance with DIN EN 1426) and asphalt pen70 / 100 modified with 1.25% by mass of the thermosetting reactive compound As20 (penetration of 7 - 10 mm in accordance with DIN EN 1426). For each variant (unmodified and in-line modification), a batch size of 4 tons of asphalt mixture composition was selected. The particle size distribution shown in Table 7 (Table 9) was adjusted with 50% by mass of virgin granular material (using filler (particle size: 0 - 0.063 mm), fine aggregate (particle size: 0 - 2 mm), and coarse aggregate (particle size: 2 - 5 mm, 5 - 8 mm, 8 - 11 mm, 11 - 16 mm, 16 - 22 mm)), and 50% by mass of recycled asphalt paving material. The total asphalt content in the mixture of asphalt and granular material was 4.3% by mass, i.e., 172 kg of asphalt per 4t batch. Of the 172 kg of asphalt, 100 kg was derived from recycled asphalt paving material, and the remaining 72 kg was from the addition of unmodified (paving grade) asphalt pen70 / 100. In the case of the example of the present invention, the amount of the thermosetting reactive compound As20 used was 2.16 kg, i.e., 1.25% by mass based on the total amount of asphalt used (i.e., asphalt from recycled asphalt paving material + unmodified (paving grade) asphalt pen70 / 100). The virgin granular material and the recycled asphalt paving material were preheated separately, and then mixed together for 6 seconds so that the temperature of the corresponding mixture did not exceed 200°C. 72 kg of unmodified (paving grade) asphalt pen70 / 100 was preheated to a temperature of 175 - 180°C, weighed into a stirring container (= the remaining asphalt), and in the case of the comparative example, then 2.16 kg of As20 was added to the asphalt while stirring (1500 rpm), and the resulting mixture was further stirred. Here, the injection rate was set to 0.1 L / s - 2.0 L / s, and the stirring time was set to 20 seconds. The obtained modified asphalt was added to the granular material (a mixture of virgin granular material and recycled asphalt paving material with a temperature of 200°C or less) in a mixing unit (twin-shaft compulsory mixer), and the resulting mixture was further stirred. Here, the total time of further stirring was 30 seconds.The temperature of the asphalt mixture composition at this stage of the method was determined to be 175 - 180 °C. Subsequently, the asphalt mixture composition may be discharged into a silo, loaded onto a truck, or stored for several hours. All of the obtained asphalt mixture compositions were further analyzed. The results are shown in Table 8 (Table 10).

[0204]

Table 9

[0205]

Table 10

[0206] Comparing the results of the comparative examples and the examples of the present invention in Table 8 (Table 10), it is clear that the results obtained under laboratory conditions in the aforementioned examples are also obtained under actual conditions. Therefore, based on the results in Table 8 (Table 10), despite the fact that a very short mixing stage was used compared to the mixing procedure of asphalt and a thermosetting reactive compound taught in the prior art, for the experiment of the in-line test in the above examples, the surprising technical effects obtained under laboratory conditions are confirmed.

[0207] (References) TIFF2025108539000011.tif200152

Claims

1. A method for preparing an asphalt mixture composition, comprising: (1) preparing an asphalt composition and heating the composition to a temperature in the range of 110 to 200 °C; (2) preparing a granular material and heating the material to a temperature in the range of 110 to 240 °C; (3) preparing one or more thermosetting reactive compounds; (4) adding the one or more thermosetting reactive compounds prepared in (3) to the asphalt composition obtained in (1) and homogenizing the mixture for a time in the range of 2 to 180 seconds; (5) adding the mixture obtained in (4) to the granular material obtained in (2) and homogenizing the slurry for a time in the range of 5 to 180 seconds.

2. The method according to claim 1, wherein after (4) and before (5), the mixture obtained in (4) is stored at a temperature in the range of 60 to 190 °C.

3. The method according to claim 1 or 2, wherein after (4) and before (5), the mixture obtained in (4) is mixed at a mixing speed of 100 rpm or less.

4. The method according to claim 1, wherein the mixture obtained in (4) is directly processed in (5).

5. The method according to any one of claims 1 to 4, wherein the one or more thermosetting reactive compounds include one or more compounds selected from the group consisting of polyisocyanates, epoxy resins, melamine formaldehyde resins, and mixtures of two or more thereof.

6. The method according to any one of claims 1 to 5, wherein the mass ratio of the total amount of the one or more thermosetting reactive compounds to the asphalt composition is in the range of 0.1:99.9 to 25:

75.

7. The method according to any one of claims 1 to 6, wherein the mass ratio of the mixture obtained in (4) to the granular material obtained in (2) is in the range of 0.5:99.5 to 25:

75.

8. The method according to any one of claims 1 to 7, wherein the granular material prepared in (2) includes one or more granular materials selected from the group consisting of gravel, recycled asphalt pavement material, sand, one or more filler materials, and mixtures of two or more thereof.

9. The method according to any one of claims 1 to 8, wherein the asphalt composition prepared in (1) includes one or more additives.

10. The method according to any one of claims 1 to 9, wherein the granular material prepared in (2) includes 5 to 100% by mass of recycled asphalt pavement material.

11. The method according to any one of claims 1 to 10, wherein the granular material prepared in (2) exhibits a particle size in the range of 0.1 to 70 mm. **Claim 12** The method according to any one of claims 1 to 11, wherein (4) and / or (5) is carried out in an oxygen-containing atmosphere. **Claim 13** The method according to any one of claims 1 to 12, wherein (4) and / or (5) is carried out as a batch process or a continuous process. **Claim 14** An asphalt mixture composition obtained or obtainable according to the method according to any one of claims 1 to 13. **Claim 15** Use of the asphalt mixture composition according to claim 14 for paving applications.

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