CN116814086A - Plastic garbage recycling method - Google Patents
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Abstract
本发明属于塑料改性加工技术领域，涉及海洋塑料垃圾回收利用领域，公开了一种塑料垃圾回收利用方法，包括以下步骤：将待回收利用的塑料垃圾进行分选，获得重质塑料与轻质塑料；将重质塑料进行催化胺裂，得到重质塑料衍生添加剂；将全新沥青、回收沥青、沥青再生剂与重质塑料衍生添加剂按预设比例熔融密炼拌和，获得重质塑料衍生剂改性再生沥青；将轻质塑料催化热解，制备获得碳纳米管与富氢气体。本发明基于分选获得的重质塑料与轻质塑料分别制取改性沥青、以及碳纳米管与富氢气体；可解决塑料改性沥青的离析问题，同时能够实现塑料垃圾的高效回收与高附加值利用。
The invention belongs to the technical field of plastic modification processing and relates to the field of recycling and utilization of marine plastic waste. It discloses a plastic waste recycling method, which includes the following steps: sorting the plastic waste to be recycled to obtain heavy plastic and light plastic. Plastics; carry out catalytic amine cracking of heavy plastics to obtain heavy plastic derivative additives; melt and mix new asphalt, recycled asphalt, asphalt regenerant and heavy plastic derivative additives in preset proportions to obtain heavy plastic derivative additives Regeneration of asphalt; catalytic pyrolysis of lightweight plastics to prepare carbon nanotubes and hydrogen-rich gas. This invention produces modified asphalt, carbon nanotubes and hydrogen-rich gas respectively based on the heavy plastics and light plastics obtained by sorting; it can solve the problem of segregation of plastic modified asphalt, and at the same time achieve efficient recycling and high-efficiency plastic waste. Added value utilization.
Description
Technical Field
The invention belongs to the technical field of plastic modification processing, relates to the field of recycling of ocean plastic garbage, and particularly relates to a plastic garbage recycling method.
Background
Plastic, which is one of petrochemical products, is widely used in various fields due to its light weight, portability, low production cost, etc. Currently, the global production of more than 3 hundred million tons of plastic per year is achieved, and a large number of plastic products are discarded at will; wherein, more than 800 ten thousand tons of plastic garbage enter the ocean every year, accounting for 80 percent of all ocean garbage. The plastic has stable physical and chemical structures, can not be decomposed in natural environment for tens or hundreds of years, pollutes the ocean for a long time, threatens the survival of marine organisms, has serious influence on food safety, human health and coastal travel industry, and is one of the environmental problems in the ten world today.
In addition, asphalt is widely used in road construction in large quantities as cities rapidly develop; under the natural actions of sunlight, rainwater, oxidization and the like, a series of volatilization, oxidization and polymerization reactions can occur to the asphalt, so that the internal structure and performance of the asphalt are changed substantially, and the similar asphalt aging process leads the pavement to be dry and brittle, so that cracking and loosening occur, and the pavement performance is deteriorated. Illustratively, aging of asphalt is mainly represented by changes in the contained components, greatly reduced oil content, increased asphaltenes, changed colloid structure, increased viscosity of asphalt, and reduced rheological index, resulting in reduced asphalt performance.
Based on the above situation, the modified asphalt modified by waste plastics and garbage is an environment-friendly modified asphalt mode for recycling resources, and the current treatment mode is to mix the waste plastics into asphalt after physical treatment so as to improve asphalt performance. However, in the above-mentioned existing method, when the plastic garbage is mixed with the asphalt in a high-temperature molten state, the plastic is decomposed, the unstable factors of the components are many, the unstable influence is generated on the asphalt modification process, the storage stability of the modified asphalt at normal temperature is influenced, and the segregation problem of the plastic modified asphalt is difficult to be effectively solved.
Disclosure of Invention
The invention aims to provide a plastic garbage recycling method for solving one or more of the technical problems. In the technical scheme provided by the invention, plastic garbage is firstly subjected to sorting treatment, and modified asphalt, carbon nano tubes and hydrogen-rich gas are respectively prepared based on heavy plastic and light plastic obtained by sorting; can solve the segregation problem of the plastic modified asphalt and realize the efficient recovery and the high added value utilization of the plastic garbage.
In order to achieve the above purpose, the invention adopts the following technical scheme:
the plastic garbage recycling method provided by the first aspect of the invention comprises the following steps:
sorting the plastic garbage to be recycled to obtain heavy plastic and light plastic;
carrying out catalytic amine cracking on the heavy plastic to obtain a heavy plastic derivative additive; melting, mixing and stirring brand new asphalt, recycled asphalt, asphalt regenerant and the heavy plastic derivative additive according to a preset proportion to prepare heavy plastic derivative modified regenerated asphalt;
and carrying out catalytic pyrolysis on the light plastic to prepare the carbon nano tube and hydrogen-rich gas.
The method is further improved in that in the step of separating the plastic garbage to be recycled to obtain heavy plastic and light plastic,
the separation method is wind density separation method or buoyancy density separation method.
A further improvement of the process according to the invention consists in that, in the step of subjecting the heavy plastic to catalytic amine cleavage to obtain the heavy plastic-derived additive,
the amine cracking agent adopts triethylene diamine or ethylenediamine；
The catalyst adopts sodium acetate or sodium carbonate;
the reaction temperature for catalyzing amine cracking is 80-110 ℃.
The method is further improved in that in the step of preparing the modified regenerated asphalt of the heavy plastic derivative agent by carrying out melt-mixing and mixing on the brand new asphalt, the recycled asphalt, the asphalt regenerating agent and the heavy plastic derivative additive according to the preset proportion,
the preset proportion is that 40-80 parts of whole new asphalt, 60-120 parts of recycled asphalt, 10-20 parts of asphalt regenerant and the heavy marine plastic derived additive with the addition amount of 1-4wt% are calculated according to parts by weight.
The method is further improved in that in the step of preparing the modified regenerated asphalt of the heavy plastic derivative agent by carrying out melt-mixing and mixing on the brand new asphalt, the recycled asphalt, the asphalt regenerating agent and the heavy plastic derivative additive according to the preset proportion,
the melting and mixing steps include: stirring the recycled asphalt and the brand new asphalt at 210-240 ℃, blending, heating, melting the asphalt and fully mixing; then adding an asphalt regenerant, continuously stirring and adjusting the viscosity of the blend to be 1.8 Pa.s-2.3 Pa.s to prepare a regenerated asphalt sizing material; gradually cooling the regenerated asphalt sizing material, continuously stirring, adding heavy marine plastic derived additive particles when the temperature is reduced to 150-180 ℃, and stirring to obtain the heavy marine plastic derived additive modified regenerated asphalt.
The method is further improved in that in the step of preparing and obtaining the carbon nano tube and the hydrogen-rich gas by catalytic pyrolysis of the light plastic,
the light plastic is catalytically pyrolyzed by adopting a two-stage method.
The method of the invention is further improved in that the step of catalytically pyrolyzing the light plastic by a two-stage process specifically comprises the steps of:
fe (NO) 3 ) 3 ·9H 2 O is dissolved in ethanol solvent, and then gamma-Al is added 2 O 3 Forming suspension, drying, calcining, grinding to obtain Fe/gamma-Al 2 O 3 A cracking catalyst; wherein, in parts by mass, fe (NO 3 ) 3 ·9H 2 0.5 to 1.0 part of O, 2 to 4 parts of ethanol solvent and gamma-Al 2 O 3 0.5 to 1.0 part;
at N 2 Light plastic particles and Fe/gamma-Al under protective atmosphere 2 O 3 The cracking catalyst is catalytically pyrolyzed at the temperature of 500-600 ℃; wherein, the weight portions of the light plastic and the Fe/gamma-Al are calculated 2 O 3 The proportion relation of the cracking catalyst is (4-20): 1, a step of;
at N 2 Under the protective atmosphere, ni-Al is used 2 O 3 The metal catalyst carries out catalytic modification on pyrolysis gas obtained by catalytic pyrolysis at the temperature of 800-1000 ℃ to prepare the carbon nano tube and hydrogen-rich gas.
The second aspect of the invention provides a recycling method of ocean plastic garbage, which is based on the recycling method of plastic garbage in the first aspect of the invention;
wherein the plastic garbage to be recycled is marine plastic garbage.
The invention further improves that the step of separating the plastic garbage to be recycled to obtain heavy plastic and light plastic comprises the following steps:
sorting to obtain a density of more than 1.3g cm -3 The plastic of (2) is a heavy plastic with a density of less than 1.15 g.cm -3 The method comprises the steps of carrying out a first treatment on the surface of the The plastic of (2) is light plastic.
Compared with the prior art, the invention has the following beneficial effects:
in the technical scheme provided by the invention, plastic garbage is firstly subjected to sorting treatment, and modified asphalt, carbon nano tubes and hydrogen-rich gas are respectively prepared based on heavy plastic and light plastic obtained by sorting; can solve the segregation problem of the plastic modified asphalt and realize the efficient recovery and the high added value utilization of the plastic garbage. The invention replaces the raw material part of asphalt with aged recycled asphalt, and prepares and obtains regenerated modified asphalt by adding derivative additives obtained by amine cracking heavy plastic, wherein the recycling of plastic garbage is completed by greatly consuming plastic garbage, reducing new asphalt consumption, and realizing win-win of resource recycling and environmental protection; it is further emphasized that the regenerated modified asphalt prepared by the heavy plastic derived additive has the advantages of improved softening point, reduced penetration, improved high temperature performance and other technical performances, and prolonged service life.
The invention takes light plastic as raw material, and utilizes pyrolysis and catalytic reaction to prepare carbon nano tube and hydrogen-rich gas in a two-stage fixed bed, and the application of the method not only can solve the problem of a large amount of plastic garbage, but also can provide a cheap carbon source with unrestricted source and transportation for the preparation of the carbon nano tube, and simultaneously has the advantages of higher carbon conversion rate, high product quality, flexible operation, low running cost and the like.
The invention also provides a brand-new high-efficiency recycling method of the marine plastic garbage, and the method is based on the method, and the recycling of the marine plastic garbage is classified, so that the preparation of the heavy marine plastic derived additive regenerated modified asphalt, the carbon nano tube taking the light marine plastic as a carbon source and the hydrogen-rich gas of accessory products is completed.
Drawings
In order to more clearly illustrate the embodiments of the present invention or the technical solutions in the prior art, the following description of the embodiments or the drawings used in the description of the prior art will make a brief description; it will be apparent to those of ordinary skill in the art that the drawings in the following description are of some embodiments of the invention and that other drawings may be derived from them without undue effort.
FIG. 1 is a schematic flow chart of a plastic waste recycling method provided by an embodiment of the invention;
FIG. 2 is a schematic flow chart of a method for efficiently recycling marine plastic garbage, which is provided by the embodiment of the invention;
FIG. 3 is a schematic illustration of the process for preparing a heavy marine plastic derived additive and its reclaimed modified asphalt in accordance with an embodiment of the present invention;
FIG. 4 is a schematic flow chart of the process for preparing carbon nanotubes and hydrogen-rich gas products attached thereto by using light marine plastic as a carbon source in the embodiment of the invention.
Detailed Description
The invention is further illustrated below in connection with specific examples, which are to be understood as being illustrative of the invention and not limiting the scope of the invention.
Other advantages and effects of the present invention will become apparent to those skilled in the art from the following disclosure, which describes the embodiments of the present invention with reference to specific examples. The invention may be practiced or carried out in other embodiments that depart from the specific details, and the details of the present description may be modified or varied from the spirit and scope of the present invention.
It should be understood that the process equipment or devices not specifically identified in the examples below are all conventional in the art.
Furthermore, it is to be understood that the reference to one or more method steps in this disclosure does not exclude the presence of other method steps before or after the combination step or the insertion of other method steps between these explicitly mentioned steps, unless otherwise indicated; it should also be understood that the combined connection between one or more devices/means mentioned in the present invention does not exclude that other devices/means may also be present before and after the combined device/means or that other devices/means may also be interposed between these two explicitly mentioned devices/means, unless otherwise indicated. Moreover, unless otherwise indicated, the numbering of the method steps is merely a convenient tool for identifying the method steps and is not intended to limit the order of arrangement of the method steps or to limit the scope of the invention in which the invention may be practiced, as such changes or modifications in their relative relationships may be regarded as within the scope of the invention without substantial modification to the technical matter.
Referring to fig. 1, the plastic garbage recycling method disclosed by the embodiment of the invention comprises the following steps:
step 1, sorting plastic garbage to be recycled to obtain heavy plastic and light plastic;
step 2, carrying out catalytic amine cracking on the heavy plastic to obtain a heavy plastic derivative additive; melting, mixing and stirring brand new asphalt, recycled asphalt, asphalt regenerant and the heavy plastic derivative additive according to a preset proportion to prepare heavy plastic derivative modified regenerated asphalt;
and step 3, carrying out catalytic pyrolysis on the light plastic to prepare the carbon nano tube and the hydrogen-rich gas.
In the plastic garbage recycling method provided by the embodiment of the invention, plastic garbage is firstly subjected to sorting treatment, and modified asphalt, carbon nano tubes and hydrogen-rich gas are respectively prepared based on heavy plastic and light plastic obtained by sorting; can solve the segregation problem of the plastic modified asphalt and realize the efficient recovery and the high added value utilization of the plastic garbage.
Further exemplary embodiments of the present invention, step 1 may specifically include: the plastic garbage fragments are separated into heavy plastic and light plastic by a wind power density separation method or a buoyancy density separation method; wherein, the plastic with the density larger than or equal to the first preset density threshold value is selected as heavy plastic, and the plastic with the density smaller than or equal to the second preset density threshold value is selected as light plastic; further specifically exemplified, the first preset density threshold may be 1.3 g-cm -3 The second preset density threshold may be 1.15g cm -3 。
Further exemplary of embodiments of the present invention, in step 2, the new asphalt, the recycled asphalt, and the derived additive may be mixed in a melt-mixing manner in a certain ratio using melt-mechanical blending; wherein, the amine cracking agent adopts triethylene diamine or ethylenediamine，The catalyst adopts sodium acetate or sodium carbonate.
Further exemplary, in step 3, the light plastic may be catalytically pyrolyzed by a two-stage method to obtain the carbon nanotubes and the byproduct hydrogen-rich gas.
In the step 1, before plastic garbage to be recycled is separated, the recycled plastic garbage can be subjected to clear water washing, crushing and drying treatment to obtain plastic garbage fragments; and sorting based on the obtained plastic garbage fragments.
The embodiment of the invention is further exemplified by that in step 2, the heavy plastic is subjected to catalytic amine cracking by using an amine cracking agent and a catalyst, and in the step of obtaining the heavy plastic derivative additive, the weight portions are as follows: 5 to 10 parts of heavy plastic, 15 to 20 parts of ethylenediamine and 0.25 to 0.5 part of sodium acetate; wherein the reaction temperature of the amine cracking is 80-110 ℃ and the reaction is completed until the amine cracking is completed. Further specifically explaining, adding heavy plastic particles, an amine cracking agent and a catalyst into an amine cracking reaction device according to the proportion interval; wherein, the addition of the amine cracking agent is required to ensure complete dissolution of the catalyst and to avoid excessive infiltration of the heavy plastic particles. The device is gradually heated to the reaction temperature and is continuously stirred, and the amine cracking reaction temperature is 80-110 ℃; it is worth noting that higher temperatures promote the amine cleavage reaction, but too high temperatures will volatilize the amine cleavage agent in large amounts, thus limiting the reaction temperature window. And stopping heating after the reaction is uniform and the amine cracking is completed, cooling the reactor to room temperature, collecting solid products in the reactor, ventilating and drying, and crushing the dried solid to obtain the heavy marine plastic derivative additive particles.
In step 2, when the brand new asphalt, the aged recycled asphalt, the asphalt regenerant and the heavy plastic derivative additive are mixed in a melting and banburying way according to a certain proportion, the preparation raw materials of the heavy plastic derivative additive comprise the following components in parts by mass: 60-120 parts of aged asphalt, 40-80 parts of new asphalt, 10-20 parts of RA101 asphalt regenerant and heavy marine plastic derived additive particles with the addition amount of 1-4wt%. Further specifically explaining, adding aged asphalt and new asphalt into an internal mixer, mixing the aged asphalt and the new asphalt at the temperature of 210-240 ℃ at the stirring speed of 250-350 r/min, blending the heated asphalt to be molten and fully mixing, adding a regenerant into the internal mixer, continuously stirring for 20-30 min, and regulating the viscosity of the blend to be 1.8 Pa.s-2.3 Pa.s, thus preparing the regenerated asphalt sizing material. Cooling the regenerated asphalt sizing material, continuously stirring according to the original stirring speed, adding heavy marine plastic derived additive particles when the temperature is reduced to 150-180 ℃, improving the stirring speed to 600-650 r/min, and stirring for 10-20 min to obtain the heavy marine plastic derived additive modified regenerated asphalt. When heavy marine plastic derived additive particles are added, the temperature of the reclaimed asphalt sizing material has an upper limit to avoid the denaturation of the heavy marine plastic derived additive particles, and the stirring speed needs to be increased to ensure uniform mixing in a short time.
Further exemplary of embodiments of the present invention, in step 3, fe (NO 3 ) 3 ·9H 2 O is dissolved in ethanol solvent and thengamma-Al 2 O 3 Adding into the obtained solution to form suspension, drying, calcining and grinding to obtain Fe/gamma-Al 2 O 3 A cracking catalyst; wherein, in parts by mass, fe (NO 3 ) 3 ·9H 2 0.5 to 1.0 part of O, 2 to 4 parts of ethanol solvent and gamma-Al 2 O 3 0.5 to 1.0 part;
and then the light plastic particles and the cracking catalyst are mixed according to the following proportion of (4-20): 1 are added into a fixed bed cracking reactor together according to the proportion, the heating rate of the fixed bed reactor is set to be 5 ℃/min, the temperature is raised to 500 ℃ to 600 ℃, and protective atmosphere N is introduced into the reactor at the same time 2 Preserving heat for 1.5-2 hours, wherein the light plastic fragments are subjected to pyrolysis reaction along with the temperature rise inside the reactor to obtain pyrolysis reaction gas;
the gas outlet of the fixed bed reactor is connected with a catalytic modification reactor, and Ni-Al is placed in the catalytic modification reactor 2 O 3 The metal catalyst is prepared by setting the heating rate of a catalytic modification reactor to 10 ℃/min, heating to 800-1000 ℃, preserving heat for 1-1.5 hours, and simultaneously introducing protective atmosphere N 2 Catalytic reaction is carried out on pyrolysis gas production, and pyrolysis products are converted into carbon nano tubes and hydrogen-rich gas after the reaction is finished; wherein, the weight portion is 5-10 portions of light plastic and Ni-Al 2 O 3 0.5 to 1.0 part of metal catalyst.
Further explanation of the invention point of the embodiment of the present invention: heavy plastics in the plastic garbage are subjected to catalytic amine cracking to prepare a heavy plastic derivative additive, and the derivative additive is used for enhancing the stability, corrosion resistance, physical properties and the like of the regenerated asphalt, so that the segregation problem of the plastic modified asphalt is solved; the light plastic in the plastic garbage is prepared into the carbon nano tube and the hydrogen-rich gas by a two-stage catalytic pyrolysis method, so that a cheap carbon source with unlimited sources and transportation is provided for the preparation of the carbon nano tube, and the method has the advantages of higher carbon conversion rate, simple synthesis process and the like. In the embodiment of the invention, the high-efficiency recovery and high-added-value utilization of the plastic garbage are completed by sorting the plastic garbage by wind power density and recovering the plastic garbage by the two methods.
Referring to fig. 2 to 4, the method for efficiently recycling marine plastic garbage provided by the embodiment of the invention comprises the following steps:
firstly, washing, crushing and drying the recovered marine plastic garbage with clear water to obtain marine plastic garbage fragments;
secondly, separating the marine plastic garbage fragments into heavy marine plastic and light marine plastic by using a wind power density separation method; the heavy marine plastic is subjected to catalytic amine cracking by using an amine cracking agent and a catalyst to obtain a heavy marine plastic derivative additive, and new asphalt, recycled asphalt and the derivative additive are mixed in a melting and mixing way according to a certain proportion by adopting melting mechanical blending to obtain heavy marine plastic derivative agent modified recycled asphalt; the light marine plastic is catalytically pyrolyzed in two stages to prepare carbon nanotube and hydrogen-rich gas as side product. Illustratively, there are a wide variety of plastics in marine plastic waste, such as: low density polyethylene (LDPE, mainly used for manufacturing plastic bags and plastic films, widely used for food packaging, etc.), polystyrene (PPS, commonly used for manufacturing foam plastics), polypropylene (PP, very widely used for manufacturing various containers), polyethylene terephthalate (PET, mainly used for manufacturing polyester fibers, beverage bottles, etc.), and the like. In order to realize the efficient recycling of the marine plastic garbage, the marine plastic garbage needs to be classified and recycled. In addition, if the old asphalt mixture is recycled, the problem of asphalt performance regeneration should be considered.
The method is particularly explanatory, and has important engineering significance on reducing the marine white pollution and bringing resource saving benefits on how to realize the clean and high-value utilization of the marine waste plastics. The embodiment of the invention provides a high-efficiency recycling method of marine plastic garbage, which comprises the steps of firstly washing, crushing and drying the recycled marine plastic garbage by clear water to obtain dry marine plastic fragments, and then separating the fragments into heavy marine plastic and light marine plastic by a wind power density separation method; then modifying the recovered heavy marine plastic by a catalytic amine cracking technology, and drying and crushing the product to obtain a heavy marine plastic derivative additive; then mixing the heavy marine plastic derived additive with the molten regenerated asphalt to obtain regenerated modified asphalt; and then the light marine plastic is treated by a thermal cracking process to co-produce the carbon nano tube and the hydrogen-rich gas. The invention realizes the classified recovery and the efficient utilization of the marine plastic garbage and relieves the problem of marine environmental pollution.
Further illustratively, the embodiment of the invention combines the modification of waste plastics and the recycling of aged asphalt, thereby solving the problem of pollution of white garbage and the problem of performance degradation caused by asphalt aging. Wherein the heavy plastic component (with higher density, more than 1.3g cm) -3 And the main component is PET plastics) is subjected to catalytic amine cracking to prepare the derivative additive, the derivative additive is more stable in property, and can be mixed with the reclaimed asphalt, so that the high-temperature performance and storage stability of the reclaimed asphalt can be effectively improved, and the service life of the reclaimed asphalt can be prolonged. And the light plastic component (with lower density, less than 1.15 g.cm) -3 And the main components are PA, PP plastics and the like) are also required to be recycled with high efficiency, and the pyrolysis recycling can pyrolyze and gasify the light plastic components, so that the light plastic components are effectively converted into high added value products. In recent years, many researchers have tried to produce hydrogen gas from waste plastics as an ammonia source, and have found that waste plastics can also be used as a source of carbon materials under a suitable catalyst. Carbon nanotubes are an emerging material that can be synthesized using hydrocarbons, which has excellent mechanical, thermal and electrical properties, and are ideal materials for applications in fields where low density, low weight, high tensile strength or elastic modulus are required (e.g., transportation, structural materials, high-tech applications, etc.). The traditional synthesis of the carbon nano tube uses aromatic compounds (such as toluene, benzene and the like), ethylene and the like, the petroleum accompaniment is controlled, the source is limited, and the transportation is inconvenient. The light plastic component in the marine plastic garbage can prepare the carbon nano tube and the accessory products with high added value such as hydrogen thereof by catalytic pyrolysis, so that the carbon and hydrogen elements which are rich in the carbon nano tube are fully utilized, the problem of limited source of the synthetic raw materials of the carbon nano tube is solved, and the recovery of the residual marine plastic garbage is completed, thus having important application value.
Example 1
The embodiment of the invention is prepared from the modified asphalt regenerated by the heavy marine plastic derived additive, wherein the modified asphalt comprises the following raw materials in parts by mass;
80 parts of recycled asphalt (selecting asphalt reclaimed materials milled from a certain expressway of Shaanxi), 70 parts of brand new asphalt (the softening point is 48.5 ℃, the penetration at 25 ℃ is 63dmm, the ductility at 15 ℃ is greater than 100cm, the Brookfield rotational viscosity at 135 ℃ is 0.450 Pa.s), 10 parts of RA101 type asphalt regenerant, 5 parts of heavy marine plastic after wind power sorting of marine plastic garbage, 20 parts of ethylenediamine and 0.25 part of catalyst sodium acetate;
the preparation method for synthesizing the heavy marine plastic derivative additive modified recycled asphalt comprises the following steps of:
step 1: classifying the recycled marine plastic garbage, flushing with clear water and crushing into 16-25 mm 2 Drying the fragments with the size at 65-85 ℃ for 30 minutes to obtain completely dried marine plastic garbage fragments; separating the heavy marine plastic fragments and the light marine plastic fragments by a wind power density separation method;
step 2: adding heavy marine plastic fragments into a reaction kettle, adding excessive ethylenediamine and 0.5wt% of catalyst sodium acetate, stirring and heating at 105 ℃ until the solution is uniform and the amine cracking of the heavy marine plastic is completed, stopping heating, cooling the reactor to room temperature, collecting solid products therein, ventilating and drying, and crushing to obtain heavy marine plastic derivative additive particles;
step 3: adding aged asphalt and new asphalt into an internal mixer, heating to 230 ℃, regulating the stirring speed to 300r/min, heating and blending until the asphalt is molten, adding a regenerant into the internal mixer, continuously stirring for 30min, and regulating the viscosity of the blend to 2.0 Pa.s to prepare a regenerated asphalt sizing material;
step 4: stopping heating the regenerated asphalt mixture, stirring and maintaining a molten state, waiting for the regenerated asphalt to be cooled to 160 ℃, adding heavy marine plastic derived additive particles accounting for 1% of the asphalt mass, regulating the stirring speed to 600r/min, and continuously stirring for 10min to obtain the heavy marine plastic derived additive modified regenerated asphalt mixture.
In order to fully understand the performance of the heavy marine plastic derivative additive modified recycled asphalt, physical performance tests were performed on 1wt% of the heavy marine plastic derivative modified recycled asphalt according to the Highway engineering asphalt and asphalt mixture test procedure (JTJE 20-2011). The softening point of the 1wt% of the modified recycled asphalt of the marine plastic derived additive is 49.5 ℃, the penetration at 25 ℃ is 61dmm, the Brinell rotational viscosity at 135 ℃ is 0.50 Pa.s, and the modified recycled asphalt meets the related requirements of the Highway asphalt pavement construction technical specification.
Example 2
Embodiment 2 of the present invention is substantially the same as embodiment 1 except that: in the preparation process of the heavy marine plastic derivative additive modified recycled asphalt, the addition amount of the heavy marine plastic derivative additive particles is 2wt%.
The softening point of the 2wt% weight marine plastic derived additive modified recycled asphalt was 50.1 ℃, the penetration at 25 ℃ was 59dmm, and the brookfield rotational viscosity at 135 ℃ was 0.54pa·s, measured under the same test conditions.
Example 3
Embodiment 3 of the present invention is substantially the same as embodiment 1 except that: in the preparation process of the heavy marine plastic derivative additive modified recycled asphalt, the addition amount of the heavy marine plastic derivative additive particles is 3wt%.
The softening point of the 3wt% marine plastic derived additive modified recycled asphalt was 50.6 ℃, the penetration at 25 ℃ was 57dmm, and the brookfield rotational viscosity at 135 ℃ was 0.59pa·s, measured under the same test conditions.
Example 4
Embodiment 2 of the present invention is substantially the same as embodiment 1 except that: in the preparation process of the heavy marine plastic derivative additive modified recycled asphalt, the addition amount of the heavy marine plastic derivative additive particles is 4wt%.
The softening point of the 4wt% marine plastic derived additive modified recycled asphalt was 51.0 ℃, penetration at 25 ℃ was 56dmm, and brookfield rotational viscosity at 135 ℃ was 0.63pa·s, measured under the same test conditions.
Comparative example 1
Comparative example 1 is substantially the same as example 1 except that: the heavy marine plastic derived additive particles were added in an amount of 0wt% (i.e. no heavy marine plastic derived additive particles were added).
The softening point of the 0wt% marine plastic derived additive reclaimed asphalt was 48.9 ℃, the penetration at 25 ℃ was 65dmm, and the brookfield rotational viscosity at 135 ℃ was 0.47pa·s, as measured under the same test conditions.
Specifically explanatory, to further intuitively explain the comparison of the above examples 1 to 4 with comparative example 1, the test results of the different heavy marine plastic derived additive modified recycled asphalt are shown in table 1.
TABLE 1 test results of modified recycled asphalt with different heavy Marine Plastic derived additives
Based on the data in Table 1, the softening points of the heavy marine plastic derived additive modified recycled asphalt of comparative examples 1, 2, 3 and 4 are respectively increased by 0.4 ℃, 1.0 ℃, 1.6 ℃, 2.1 ℃ and 2.5 ℃ compared with that of the matrix asphalt, the penetration is respectively reduced by 2dmm, 6dmm, 8dmm, 10dmm and 11dmm compared with that of the matrix asphalt, the relevant requirements of the Highway asphalt pavement construction technical specification are met, the high-temperature performance of the asphalt can be obviously improved by the incorporation of the heavy marine plastic derived additive, and the viscosity of the modified recycled asphalt can be increased along with the increase of the dosage of the heavy marine plastic derived additive. In conclusion, the heavy marine plastic after amine cracking is used as a modifier, so that the heavy marine plastic can be effectively mixed at the mixing temperature of the reclaimed asphalt, and the comprehensive performance of the reclaimed asphalt can be further improved; in the embodiment of the invention, the optimal use level of the heavy marine plastic derived additive is also emphasized and protected by 3 weight percent by comprehensively considering other physical properties and the economic benefit of the modified recycled asphalt.
Example 5
Referring to fig. 4, in embodiment 5 of the present invention, a method for preparing a hydrogen-rich gas from a carbon nanotube and an accessory product using a marine plastic as a carbon source is provided, which comprises:
the preparation raw materials comprise the following components in parts by weight: 5 parts of light plastic after wind power sorting of marine plastic garbage and Ni-Al 2 O 3 0.5 part of metal catalyst, fe (NO 3 ) 3 ·9H 2 O0.5 part, ethanol solvent 2 parts, gamma-Al 2 O 3 0.5 parts;
step 1: classifying the recycled marine plastic garbage, flushing with clear water and crushing into 16-25 mm 2 Drying the fragments with the size at 65-85 ℃ for 30 minutes to obtain completely dried marine plastic garbage fragments; and the heavy marine plastic and the light marine plastic are separated by a wind power density separation method;
step 2: preparation of Fe/gamma-Al by impregnation 2 O 3 A catalyst; wherein Fe (NO) 3 ) 3 ·9H 2 O is dissolved in ethanol solvent, and then gamma-Al is added 2 O 3 Adding into the obtained solution to form suspension, drying, calcining and grinding to obtain Fe/gamma-Al 2 O 3 A cracking catalyst;
step 3: mixing the dried light plastic with a cracking catalyst according to a proportion of 20:1 are added into a fixed bed cracking reactor together according to the proportion, the heating rate of the fixed bed reactor is set to be 5 ℃/min, the temperature is raised to 600 ℃, and protective atmosphere N is introduced into the reactor at the same time 2 Preserving heat for 1.5 hours, wherein the light marine plastic fragments are subjected to pyrolysis reaction along with the temperature rise inside the reactor;
step 4: the gas outlet of the fixed bed reactor is connected with a catalytic modification reactor, and Ni-Al is placed in the catalytic modification reactor 2 O 3 The metal catalyst is prepared by setting the heating rate of a catalytic modification reactor to 10 ℃/min, heating to 800 ℃, preserving heat for 1 hour, and simultaneously introducing protective atmosphere N 2 And (3) carrying out catalytic reaction on the pyrolysis produced gas, and converting pyrolysis products into carbon nano tubes and hydrogen-rich gas after the reaction is finished.
Example 6
Example 6 of the present invention is substantially the same as example 5, except thatThe method comprises the following steps: in step 3, light plastic particles and Fe/gamma-Al 2 O 3 The addition ratio of the catalyst is 10:1.
example 7
Example 7 of the present invention is substantially the same as example 5 except that: in step 3, light plastic particles and Fe/gamma-Al 2 O 3 The addition ratio of the catalyst is 5:1.
example 8
Example 8 of the present invention is substantially the same as example 5, except that: in step 3, light plastic particles and Fe/gamma-Al 2 O 3 The addition ratio of the catalyst is 4:1.
example 9
Example 9 of the present invention is substantially the same as example 5 except that: in step 4, the temperature in the fixed bed cracking reactor was raised to 850 ℃.
Example 10
Embodiment 10 of the present invention is substantially the same as embodiment 5 except that: in step 4, the temperature in the fixed bed cracking reactor was raised to 900 ℃.
Example 11
Example 11 of the present invention is substantially the same as example 5, except that: in step 4, the temperature is raised to 1000 ℃ in the fixed bed cracking reactor.
Based on examples 5 to 11, the test results of carbon conversion of carbon nanotubes are shown in table 2 for further illustrative problems.
TABLE 2 test results of carbon conversion of carbon nanotubes
As can be seen from the carbon conversion shown in Table 2, the above examples gave good results, while Fe/gamma-Al in step 3 2 O 3 The amount of cracking catalyst used and the cracking temperature in step 3 are different, and the carbon conversion rate of the carbon nanotubes prepared by pyrolyzing the light marine plastics is different. It shows that the carbon conversion rate of the carbon nano tube increases and decreases with the increase of the using amount of the cracking catalyst, and increases and decreases with the increase of the cracking temperature, and the preferable using amount of the cracking catalyst and the cracking temperature of waste plastics exist in the preparation of the carbon nano tube.
Example 12
The plastic garbage recycling method provided by the embodiment of the invention comprises the following steps:
step 1, sorting plastic garbage to be recycled to obtain heavy plastic and light plastic; wherein, the method adopted for sorting is a wind power density sorting method;
step 2, carrying out catalytic amine cracking on the heavy plastic to obtain a heavy plastic derivative additive; melting, mixing and stirring brand new asphalt, recycled asphalt, asphalt regenerant and the heavy plastic derivative additive according to a preset proportion to prepare heavy plastic derivative modified regenerated asphalt; wherein, the amine cracking agent adopts triethylene diamine；The catalyst adopts sodium acetate; the reaction temperature for catalyzing amine cracking is 80 ℃; the preset proportion is that, in terms of parts by mass, 40 parts of brand new asphalt, 60 parts of recycled asphalt, 10 parts of asphalt regenerant and a heavy marine plastic derived additive with the addition amount of 1 wt%; the melting and mixing steps include: stirring the recycled asphalt and the brand new asphalt at 210 ℃, and blending, heating the asphalt to be molten and fully mixing; then adding an asphalt regenerant, continuously stirring and adjusting the viscosity of the blend to 1.8 Pa.s to prepare a regenerated asphalt sizing material; gradually cooling the regenerated asphalt sizing material, continuously stirring, adding heavy marine plastic derived additive particles when the temperature is reduced to 150 ℃, and stirring to obtain heavy marine plastic derived additive modified regenerated asphalt;
step 3, catalytically pyrolyzing the light plastic to prepare carbon nano tubes and hydrogen-rich gas; wherein, adopt two-stage method to carry out catalytic pyrolysis on light plastics, include: fe (NO) 3 ) 3 ·9H 2 O is dissolved in ethanol solvent, and then gamma-Al is added 2 O 3 Forming suspension, drying, calcining, grinding to obtain Fe/gamma-Al 2 O 3 A cracking catalyst; wherein, in parts by mass, fe (NO 3 ) 3 ·9H 2 0.5 part of O, 2 parts of ethanol solvent and gamma-Al 2 O 3 0.5 parts; at N 2 Light plastic particles and Fe/gamma-Al under protective atmosphere 2 O 3 The cracking catalyst is catalytically pyrolyzed at a temperature of 500 ℃; wherein, the weight portions of the light plastic and the Fe/gamma-Al are calculated 2 O 3 The ratio of the cracking catalyst is 4:1, a step of; at N 2 Under the protective atmosphere, ni-Al is used 2 O 3 The metal catalyst carries out catalytic modification on pyrolysis gas obtained by catalytic pyrolysis at the temperature of 800 ℃ to prepare the carbon nano tube and hydrogen-rich gas.
Example 13
The plastic garbage recycling method provided by the embodiment of the invention comprises the following steps:
step 1, sorting plastic garbage to be recycled to obtain heavy plastic and light plastic; wherein, the separation method is a buoyancy density separation method;
step 2, carrying out catalytic amine cracking on the heavy plastic to obtain a heavy plastic derivative additive; melting, mixing and stirring brand new asphalt, recycled asphalt, asphalt regenerant and the heavy plastic derivative additive according to a preset proportion to prepare heavy plastic derivative modified regenerated asphalt; wherein, the amine cracking agent adopts ethylenediamine；The catalyst adopts sodium carbonate; the reaction temperature for catalyzing amine cracking is 95 ℃; the preset proportion is that, in terms of parts by mass, 50 parts of brand new asphalt, 80 parts of recycled asphalt, 15 parts of asphalt regenerant and a heavy marine plastic derived additive with the addition amount of 3 wt%; the melting and mixing steps include: stirring the recycled asphalt and the brand new asphalt at 220 ℃, and blending, heating the asphalt to be molten and fully mixing; then adding an asphalt regenerant, continuously stirring and adjusting the viscosity of the blend to 2.0 Pa.s to prepare a regenerated asphalt sizing material; gradually cooling the regenerated asphalt sizing material, continuously stirring, adding heavy marine plastic derived additive particles when the temperature is reduced to 170 ℃, and stirring to obtain the modified regenerated heavy marine plastic derived additiveAsphalt;
step 3, catalytically pyrolyzing the light plastic to prepare carbon nano tubes and hydrogen-rich gas; wherein, adopt two-stage method to carry out catalytic pyrolysis on light plastics, include: fe (NO) 3 ) 3 ·9H 2 O is dissolved in ethanol solvent, and then gamma-Al is added 2 O 3 Forming suspension, drying, calcining, grinding to obtain Fe/gamma-Al 2 O 3 A cracking catalyst; wherein, in parts by mass, fe (NO 3 ) 3 ·9H 2 0.8 part of O, 34 parts of ethanol solvent and gamma-Al 2 O 3 0.8 parts; at N 2 Light plastic particles and Fe/gamma-Al under protective atmosphere 2 O 3 The cracking catalyst is catalytically pyrolyzed at 550 ℃; wherein, the weight portions of the light plastic and the Fe/gamma-Al are calculated 2 O 3 The ratio of the cracking catalyst is 10:1, a step of; at N 2 Under the protective atmosphere, ni-Al is used 2 O 3 The metal catalyst carries out catalytic modification on pyrolysis gas obtained by catalytic pyrolysis at the temperature of 900 ℃ to prepare the carbon nano tube and hydrogen-rich gas.
Example 14
The plastic garbage recycling method provided by the embodiment of the invention comprises the following steps:
step 1, sorting plastic garbage to be recycled to obtain heavy plastic and light plastic; wherein, the method adopted for sorting is a wind power density sorting method;
step 2, carrying out catalytic amine cracking on the heavy plastic to obtain a heavy plastic derivative additive; melting, mixing and stirring brand new asphalt, recycled asphalt, asphalt regenerant and the heavy plastic derivative additive according to a preset proportion to prepare heavy plastic derivative modified regenerated asphalt; wherein, the amine cracking agent adopts triethylene diamine；The catalyst adopts sodium carbonate; the reaction temperature for catalyzing amine cracking is 110 ℃; the preset proportion is 80 parts of brand new asphalt, 120 parts of recycled asphalt, 20 parts of asphalt regenerant and a heavy marine plastic derived additive with the addition amount of 4 wt%; the melting and mixing steps include: stirring the recycled asphalt and the brand new asphalt at 240 ℃ to obtain the asphalt mixtureThe mixed heating asphalt is in a molten state and is fully mixed; then adding an asphalt regenerant, continuously stirring and adjusting the viscosity of the blend to 2.3 Pa.s to prepare a regenerated asphalt sizing material; gradually cooling the regenerated asphalt sizing material, continuously stirring, adding heavy marine plastic derived additive particles when the temperature is reduced to 180 ℃, and stirring to obtain heavy marine plastic derived additive modified regenerated asphalt;
step 3, catalytically pyrolyzing the light plastic to prepare carbon nano tubes and hydrogen-rich gas; wherein, adopt two-stage method to carry out catalytic pyrolysis on light plastics, include: fe (NO) 3 ) 3 ·9H 2 O is dissolved in ethanol solvent, and then gamma-Al is added 2 O 3 Forming suspension, drying, calcining, grinding to obtain Fe/gamma-Al 2 O 3 A cracking catalyst; wherein, in parts by mass, fe (NO 3 ) 3 ·9H 2 O1.0 part, ethanol solvent 4 parts, gamma-Al 2 O 3 1.0 parts; at N 2 Light plastic particles and Fe/gamma-Al under protective atmosphere 2 O 3 The cracking catalyst is catalytically pyrolyzed at 600 ℃; wherein, the weight portions of the light plastic and the Fe/gamma-Al are calculated 2 O 3 The ratio of the cracking catalyst is 20:1, a step of; at N 2 Under the protective atmosphere, ni-Al is used 2 O 3 The metal catalyst carries out catalytic modification on pyrolysis gas obtained by catalytic pyrolysis at the temperature of 1000 ℃ to prepare the carbon nano tube and hydrogen-rich gas.
Finally, it should be noted that: the above embodiments are only for illustrating the technical aspects of the present invention and not for limiting the same, and although the present invention has been described in detail with reference to the above embodiments, it should be understood by those of ordinary skill in the art that: modifications and equivalents may be made to the specific embodiments of the invention without departing from the spirit and scope of the invention, which is intended to be covered by the claims.
Claims (9)
1. The plastic garbage recycling method is characterized by comprising the following steps of:
sorting the plastic garbage to be recycled to obtain heavy plastic and light plastic;
carrying out catalytic amine cracking on the heavy plastic to obtain a heavy plastic derivative additive; melting, mixing and stirring brand new asphalt, recycled asphalt, asphalt regenerant and the heavy plastic derivative additive according to a preset proportion to prepare heavy plastic derivative modified regenerated asphalt;
and carrying out catalytic pyrolysis on the light plastic to prepare the carbon nano tube and hydrogen-rich gas.
2. The method for recycling plastic waste according to claim 1, wherein in the step of sorting plastic waste to be recycled to obtain heavy plastic and light plastic,
the separation method is wind density separation method or buoyancy density separation method.
3. The method for recycling plastic waste according to claim 1, wherein in the step of subjecting the heavy plastic to catalytic amine cracking to obtain the heavy plastic derivative additive,
the amine cracking agent adopts triethylene diamine or ethylenediamine；
The catalyst adopts sodium acetate or sodium carbonate;
the reaction temperature for catalyzing amine cracking is 80-110 ℃.
4. The method for recycling plastic garbage according to claim 1, wherein in the step of preparing the heavy plastic derivative agent modified recycled asphalt by melting and mixing brand new asphalt, recycled asphalt, asphalt recycling agent and the heavy plastic derivative additive according to a preset proportion,
the preset proportion is that 40-80 parts of whole new asphalt, 60-120 parts of recycled asphalt, 10-20 parts of asphalt regenerant and the heavy marine plastic derived additive with the addition amount of 1-4wt% are calculated according to parts by weight.
5. The method for recycling plastic garbage according to claim 4, wherein in the step of preparing the heavy plastic derivative agent modified recycled asphalt by melting and mixing brand new asphalt, recycled asphalt, asphalt recycling agent and the heavy plastic derivative additive according to a preset proportion,
the melting and mixing steps include: stirring the recycled asphalt and the brand new asphalt at 210-240 ℃, blending, heating, melting the asphalt and fully mixing; then adding an asphalt regenerant, continuously stirring and adjusting the viscosity of the blend to be 1.8 Pa.s-2.3 Pa.s to prepare a regenerated asphalt sizing material; gradually cooling the regenerated asphalt sizing material, continuously stirring, adding heavy marine plastic derived additive particles when the temperature is reduced to 150-180 ℃, and stirring to obtain the heavy marine plastic derived additive modified regenerated asphalt.
6. The method for recycling plastic waste according to claim 1, wherein in the step of preparing and obtaining carbon nanotubes and hydrogen-rich gas by catalytic pyrolysis of the light plastic,
the light plastic is catalytically pyrolyzed by adopting a two-stage method.
7. The method for recycling plastic waste according to claim 6, wherein the step of catalytically pyrolyzing the light plastic by a two-stage method comprises:
fe (NO) 3 ) 3 ·9H 2 O is dissolved in ethanol solvent, and then gamma-Al is added 2 O 3 Forming suspension, drying, calcining, grinding to obtain Fe/gamma-Al 2 O 3 A cracking catalyst; wherein, in parts by mass, fe (NO 3 ) 3 ·9H 2 0.5 to 1.0 part of O, 2 to 4 parts of ethanol solvent and gamma-Al 2 O 3 0.5 to 1.0 part;
at N 2 Light plastic particles and Fe/gamma-Al under protective atmosphere 2 O 3 The cracking catalyst is catalytically pyrolyzed at the temperature of 500-600 ℃; wherein, the weight portions of the light plastic and the Fe/gamma-Al are calculated 2 O 3 The proportion relation of the cracking catalyst is that(4～20)：1；
At N 2 Under the protective atmosphere, ni-Al is used 2 O 3 The metal catalyst carries out catalytic modification on pyrolysis gas obtained by catalytic pyrolysis at the temperature of 800-1000 ℃ to prepare the carbon nano tube and hydrogen-rich gas.
8. A method for recycling ocean plastic waste, which is characterized by being based on the plastic waste recycling method in claim 1;
wherein the plastic garbage to be recycled is marine plastic garbage.
9. The method for recycling marine plastic waste according to claim 8, wherein the step of sorting the plastic waste to be recycled to obtain heavy plastic and light plastic comprises:
sorting to obtain a density of more than 1.3g cm -3 The plastic of (2) is a heavy plastic with a density of less than 1.15 g.cm -3 The method comprises the steps of carrying out a first treatment on the surface of the The plastic of (2) is light plastic.
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