CN115090237B - Method for converting zero-valent iron into high-added-value fuel and environment restoration material by photo-thermal conversion of waste plastics - Google Patents
Method for converting zero-valent iron into high-added-value fuel and environment restoration material by photo-thermal conversion of waste plastics Download PDFInfo
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- CN115090237B CN115090237B CN202210551688.7A CN202210551688A CN115090237B CN 115090237 B CN115090237 B CN 115090237B CN 202210551688 A CN202210551688 A CN 202210551688A CN 115090237 B CN115090237 B CN 115090237B
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- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 title claims abstract description 84
- 239000004033 plastic Substances 0.000 title claims abstract description 70
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- 239000000463 material Substances 0.000 title claims abstract description 62
- 238000006243 chemical reaction Methods 0.000 title claims abstract description 43
- 238000000034 method Methods 0.000 title claims abstract description 30
- 239000000446 fuel Substances 0.000 title claims abstract description 27
- 229910052760 oxygen Inorganic materials 0.000 claims abstract description 49
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims abstract description 48
- 239000001301 oxygen Substances 0.000 claims abstract description 48
- 239000002253 acid Substances 0.000 claims abstract description 42
- -1 radical modified zero-valent iron Chemical class 0.000 claims abstract description 29
- 239000003054 catalyst Substances 0.000 claims abstract description 18
- 239000007789 gas Substances 0.000 claims abstract description 16
- KGBXLFKZBHKPEV-UHFFFAOYSA-N boric acid Chemical compound OB(O)O KGBXLFKZBHKPEV-UHFFFAOYSA-N 0.000 claims abstract description 14
- 239000004327 boric acid Substances 0.000 claims abstract description 14
- 229910019142 PO4 Inorganic materials 0.000 claims abstract description 13
- 239000010452 phosphate Substances 0.000 claims abstract description 13
- 239000007787 solid Substances 0.000 claims abstract description 6
- QMQXDJATSGGYDR-UHFFFAOYSA-N methylidyneiron Chemical compound [C].[Fe] QMQXDJATSGGYDR-UHFFFAOYSA-N 0.000 claims abstract description 5
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- 238000000498 ball milling Methods 0.000 claims description 27
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- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims description 17
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- 238000001816 cooling Methods 0.000 claims description 2
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- FHNFHKCVQCLJFQ-UHFFFAOYSA-N xenon atom Chemical compound [Xe] FHNFHKCVQCLJFQ-UHFFFAOYSA-N 0.000 claims description 2
- 229930195733 hydrocarbon Natural products 0.000 abstract description 21
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- HGUFODBRKLSHSI-UHFFFAOYSA-N 2,3,7,8-tetrachloro-dibenzo-p-dioxin Chemical compound O1C2=CC(Cl)=C(Cl)C=C2OC2=C1C=C(Cl)C(Cl)=C2 HGUFODBRKLSHSI-UHFFFAOYSA-N 0.000 description 1
- 229910018072 Al 2 O 3 Inorganic materials 0.000 description 1
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 description 1
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- 229920000915 polyvinyl chloride Polymers 0.000 description 1
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- 239000010865 sewage Substances 0.000 description 1
- 229910052709 silver Inorganic materials 0.000 description 1
- 239000001488 sodium phosphate Substances 0.000 description 1
- 229910000162 sodium phosphate Inorganic materials 0.000 description 1
- 239000012265 solid product Substances 0.000 description 1
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- 229910052723 transition metal Inorganic materials 0.000 description 1
- 150000003624 transition metals Chemical class 0.000 description 1
- RYFMWSXOAZQYPI-UHFFFAOYSA-K trisodium phosphate Chemical compound [Na+].[Na+].[Na+].[O-]P([O-])([O-])=O RYFMWSXOAZQYPI-UHFFFAOYSA-K 0.000 description 1
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- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10L—FUELS NOT OTHERWISE PROVIDED FOR; NATURAL GAS; SYNTHETIC NATURAL GAS OBTAINED BY PROCESSES NOT COVERED BY SUBCLASSES C10G, C10K; LIQUEFIED PETROLEUM GAS; ADDING MATERIALS TO FUELS OR FIRES TO REDUCE SMOKE OR UNDESIRABLE DEPOSITS OR TO FACILITATE SOOT REMOVAL; FIRELIGHTERS
- C10L3/00—Gaseous fuels; Natural gas; Synthetic natural gas obtained by processes not covered by subclass C10G, C10K; Liquefied petroleum gas
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- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
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- B01J19/08—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor
- B01J19/12—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor employing electromagnetic waves
- B01J19/122—Incoherent waves
- B01J19/127—Sunlight; Visible light
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
- B01J23/70—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper
- B01J23/74—Iron group metals
- B01J23/745—Iron
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J27/00—Catalysts comprising the elements or compounds of halogens, sulfur, selenium, tellurium, phosphorus or nitrogen; Catalysts comprising carbon compounds
- B01J27/02—Sulfur, selenium or tellurium; Compounds thereof
- B01J27/053—Sulfates
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J27/00—Catalysts comprising the elements or compounds of halogens, sulfur, selenium, tellurium, phosphorus or nitrogen; Catalysts comprising carbon compounds
- B01J27/14—Phosphorus; Compounds thereof
- B01J27/185—Phosphorus; Compounds thereof with iron group metals or platinum group metals
- B01J27/1853—Phosphorus; Compounds thereof with iron group metals or platinum group metals with iron, cobalt or nickel
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- B01J27/00—Catalysts comprising the elements or compounds of halogens, sulfur, selenium, tellurium, phosphorus or nitrogen; Catalysts comprising carbon compounds
- B01J27/20—Carbon compounds
- B01J27/232—Carbonates
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- B01J35/00—Catalysts, in general, characterised by their form or physical properties
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- B01J35/39—Photocatalytic properties
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- B01J35/391—Physical properties of the active metal ingredient
- B01J35/393—Metal or metal oxide crystallite size
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B09—DISPOSAL OF SOLID WASTE; RECLAMATION OF CONTAMINATED SOIL
- B09C—RECLAMATION OF CONTAMINATED SOIL
- B09C1/00—Reclamation of contaminated soil
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- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F1/00—Treatment of water, waste water, or sewage
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- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
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- C02F2101/10—Inorganic compounds
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- C—CHEMISTRY; METALLURGY
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- C02F2101/30—Organic compounds
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- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2103/00—Nature of the water, waste water, sewage or sludge to be treated
- C02F2103/06—Contaminated groundwater or leachate
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- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02W—CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO WASTEWATER TREATMENT OR WASTE MANAGEMENT
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Abstract
The invention relates to a method for photo-thermal conversion of waste plastics by using zero-valent iron as a high-added-value fuel and environment restoration material, which uses an oxygen-containing acid radical modified zero-valent iron material as a catalyst for photo-thermal conversion of waste plastics, wherein the oxygen-containing acid radical modified zero-valent iron material has an irregular granular microstructure with micron-scale and/or nano-scale dimensions, and surface species comprise boric acid and phosphate radicals. Compared with the prior art, the invention is used for converting waste plastics into high value-added fuel and environment restoration materials by photo-thermal catalysis, the conversion rate of gas hydrocarbon products can reach more than 53 percent, and the stability is better. Meanwhile, the residual iron-carbon solid can be used as an environment restoration material, so that organic pollutants and heavy metals in underground water and soil can be removed efficiently, and high efficiency can be maintained for a long time.
Description
Technical Field
The invention relates to the technical field of environmental catalysis, in particular to a method for converting zero-valent iron into high-added-value fuel and environmental repair materials by photo-thermal conversion of waste plastics.
Background
In recent years, the widespread accumulation of waste plastic blocks and particulates in landfill sites and the natural environment has received increasing worldwide attention, such as soil, rivers, oceans, mountains, polar regions, and the atmosphere. Waste plastics are stable in the environment for centuries due to their difficulty in biodegradation, presenting an immeasurable potential threat to wild/marine organisms and humans. The current plastic crisis comes from the plastic production and consumption speed far exceeding the recovery speed of waste plastic. The lack of recycling of waste plastics not only causes the loss of the value chain of the petrochemical industry, but also brings serious threat to energy, environment and climate safety. Therefore, development of a revolutionary new method integrating high efficiency, environmental protection and low carbon into a whole is needed to realize large-scale recycling of waste plastics. The chemical method can gasify and convert waste plastics into high-quality monomers and carbon materials, such as pyrolysis of the waste plastics into naphtha and carbon under the condition of anaerobic condition, partial oxidation gasification of the waste plastics into industrial synthesis gas, and depolymerization of the waste plastics into the monomers under the assistance of a solvent. The chemical method has the greatest advantages that the chain of the long-chain plastic can be broken in one pot directly without fine pre-classification, the product quality is high, and the method has a large-scale application basis. Therefore, the large-scale chemical recycling process is considered as the most promising plastic recycling way, and is expected to become a secondary engine for economic growth and carbon emission reduction in the background of sustainable development. However, the extremely strong C-H, C-O, C-S and C-Cl bonds exist in the molecular structure of plastics and can be broken effectively only when the reaction temperature is close to 800 ℃. This results in the current chemical recycling process of waste plastics consuming a lot of fossil energy, failing to meet the target requirement of "double carbon", and possibly leading to financial subsidy and refund before "double carbon", making the pyrolysis, gasification and depolymerization processes unavailable. In addition, conventional chemical processes require high pressure, additional solvents or chemical feedstocks, and product selectivity presents a serious challenge. These problems limit the scale-up of chemical processes, making the current worldwide recovery of waste plastics by chemical routes less than three million tons each year. Therefore, catalytic chemistry meeting new environmental and carbon emission requirements is still in the start-up phase. Specifically, catalytic chemistry involves two core components, a catalyst and a catalytic driving force. The existing catalytic method uses micro/nano material as catalyst, the catalyst has the advantages of high activity and controllable and adjustable product, and compared with the catalytic thermal cracking at 800 ℃, the catalytic reaction temperature is reduced to about 500 ℃, but a great amount of fossil energy is still required to be consumed to provide driving force.
The photo-thermal catalysis is an efficient solar-driven zero-carbon or negative-carbon catalysis mode, and is mainly applied to the carbon conversion and utilization process after carbon capture. The photo-thermal catalysis is to further introduce low energy barrier photochemistry and non-equilibrium thermochemical based on the thermal catalysis so as to optimize the reaction kinetics and the non-equilibrium thermochemicalThermodynamics to promote the selectivity and yield of the reaction product. More importantly, the photocatalytic driving force of the photo-thermal catalysis is clean and renewable solar energy, so that the problems of energy consumption and carbon footprint of fossil energy are fundamentally solved. Meanwhile, the photo-thermal catalysis does not involve any water or organic solvent, the catalysis process is anaerobic catalysis, sewage and highly toxic dioxin are not generated, secondary environmental pollution is avoided, and a new low-cost, efficient and environment-friendly way is provided for carbon neutralization and waste plastic recycling. The photo-thermal catalyst is typically a metal and support composite. The metal composition is mostly Ag, cu, al and conventional transition metals with plasmon resonance effect, while the source of the carrier material is extremely wide, including light-inert white materials (SiO 2 And Al 2 O 3 ) Conventional semiconductor photocatalysts (e.g. TiO 2 、ZnO、In 2 O 3 、NiO x And layered double hydroxide LDHs), conventional thermocatalytically active supports (such as metal hydrides, nitrides, carbides, phosphides, oxides, hydroxides and composites thereof). However, most advanced catalysts inevitably form serious carbon deposition-carbon materials or metal-carbon composites after long-term operation, resulting in rapid deterioration of catalytic performance. The development of inexpensive high-efficiency photo-thermal catalysts to convert waste plastics into gaseous hydrocarbons with high added value is a difficult challenge.
Disclosure of Invention
The invention aims to provide a method for converting zero-valent iron into high-added-value fuel and environment restoration materials by photo-thermal conversion of waste plastics.
The aim of the invention can be achieved by the following technical scheme: a method for photo-thermal conversion of waste plastics by using zero-valent iron into high-added-value fuel and environment restoration materials utilizes an oxygen-containing acid radical modified zero-valent iron material as a catalyst for photo-thermal conversion of waste plastics, wherein the oxygen-containing acid radical modified zero-valent iron material has an irregular granular microstructure with micron-scale and/or nano-scale dimensions, and surface species comprise boric acid and phosphate radicals.
Preferably, the boric acid mass content of the surface of the oxygen acid radical modified zero-valent iron material is 0.05-6.18%.
Further preferably, the boric acid mass content of the surface of the oxygen acid radical modified zero-valent iron material is 0.5-3.65%.
Preferably, the mass content of phosphate on the surface of the oxygen acid modified zero-valent iron material is 0.01-3.53%.
Further preferably, the mass content of phosphate on the surface of the oxygen acid modified zero-valent iron material is 0.2-2.18%.
Preferably, the particle diameters of the micrometer scale are all between 0.5 and 10 mu m, and the particle diameters of the nanometer scale are all between 80 and 800 nm.
Further preferably, the particles of the micron scale have a diameter of between 0.5 and 4 μm and the particles of the nanometer scale have a diameter of between 80 and 300 nm.
Preferably, the preparation method of the oxo-acid radical modified zero-valent iron material comprises the following steps:
1) Mixing an oxygen-containing acid radical precursor with zero-valent iron to obtain solid powder;
2) And mechanically ball milling the solid powder in an inert atmosphere, naturally cooling to room temperature, and collecting to obtain the oxygen acid modified zero-valent iron material.
Further preferably, the oxyacid radical precursor in step 1) is boric acid and a phosphate radical.
Further preferably, the zero-valent iron is commercial iron powder, and the mechanical ball milling is to perform surface modification treatment on the commercial iron powder in a co-ball milling mode with boric acid and phosphate.
Further preferably, the mechanical ball milling rotation speed in the step 2) is 100-500 rpm, and the ball milling time is 1-6 hours.
Further preferably, the inert atmosphere in step 2) is nitrogen or argon.
Preferably, the method for converting the zero-valent iron photo-thermal into the high-added-value fuel and the environment restoration material comprises the following steps: in a sapphire window high-pressure photo-thermal reactor, oxygen-containing boric acid and phosphate modified micron-scale and/or nanoscale zero-valent iron materials are used as photo-thermal catalysts, the photo-thermal catalysts are uniformly mixed with waste plastic precursors, nitrogen or argon is introduced into the photo-thermal reactor until an oxygen signal peak cannot be detected in gas chromatography, a xenon lamp light source is used for simulating sunlight, and the obtained products are high-added-value fuel and environment repair materials.
Further preferably, the high value fuel and environmental remediation material comprises H 2 High added value C1-C7 gas, C8-C30 medium carbon oil, high carbon wax and iron carbon environment restoration materials.
Further preferably, the mass ratio of the addition amount of the oxygen acid modified zero-valent iron material to the waste plastic to be treated is 5:1-1:10.
Further preferably, the photo-thermal reaction time is 1 to 8 hours.
Preferably, the waste plastics include, but are not limited to, polyethylene, polyvinyl chloride, polystyrene, polypropylene, polyurethane, polyethylene terephthalate.
In the invention, the photo-thermal catalysis can not only trigger the traditional photochemical (photo-catalytic) reaction by absorbing ultraviolet and visible light, but also utilize the residual solar energy by means of photo-thermal chemistry, including nano-scale local heat generated by the combination process of infrared photons and carriers, and the excited state photochemical and unbalanced state photo-thermal effects reduce the reaction energy barrier and increase the conversion rate, thereby optimizing the thermodynamics and dynamics of a plurality of challenging catalytic reactions. The method can maximally improve the conversion efficiency of solar energy to chemical energy, does not need water participation, and has incomparable advantages of traditional liquid phase photocatalysis in industrial amplification application.
Compared with the prior art, the invention has the following advantages:
1. the invention utilizes the oxygen-containing acid radical to modify the zero-valent iron material as a catalyst to perform photo-thermal catalytic conversion on waste plastics, realizes the simultaneous high-efficiency preparation of high-added-value fuel and environment restoration materials, ensures that the conversion rate of gas hydrocarbon products can reach more than 53 percent, has good stability, simultaneously ensures that the residual iron-carbon solid can be used as the environment restoration material, can efficiently remove organic pollutants and heavy metals in underground water and soil, and can maintain higher efficiency for a long time;
2. the invention successfully prepares the efficient photo-thermal conversion waste plastic catalyst by using oxygen-containing acid radical to modify zero-valent iron, and the catalyst can effectively photo-thermal convert waste plastic into high-added-value fuel and environment restoration material for a long time under the irradiation of sunlight;
3. the oxygen-containing acid radical modified on the surface of the zero-valent iron can change the pH value of the surface of the zero-valent iron while not affecting the sunlight response capability of the zero-valent iron, so that the C1-C7 hydrocarbon and the conversion rate and the selectivity in the conversion process of photo-thermal waste plastics are improved, and the oxygen-containing acid radical modified zero-valent iron photo-thermal catalyst with the full solar spectrum response capability is prepared by mechanical co-ball milling;
4. the invention skillfully provides a new way for recycling the next generation of waste plastics, which has the advantages of circular economy, environmental protection, controllable carbon emission and large scale, wherein the gas product can be used as high-added value fuel, and the solid product can be used as a high-efficiency environment restoration material, so that the synchronous combination of waste plastics recycling, pollution control and carbon emission is realized;
5. the oxygen acid modification in the oxygen acid modified zero-valent iron photo-thermal catalytic material is a surface substitution strategy, and the oxygen acid is less in dosage, so that the material cost is reduced, and the economic benefit of the material is improved;
6. the invention uses the iron-carbon material after carbon deposition as an environment restoration material, thereby realizing the secondary utilization of the material;
7. the material is environment-friendly, does not cause secondary pollution, and has certain circularity;
8. the catalyst has the advantages of low cost and easy acquisition of raw materials, easy realization of preparation conditions, no need of complex devices, simple operation, no danger and no need of using professional operators.
Drawings
FIG. 1 is an XRD pattern of the zero valent iron ball-milled and the zero valent iron ball-milled with oxyacid radical modification synthesized in example 1;
FIG. 2 is an SEM image of micrometer scale ball-milled zero valent iron and ball-milled oxoacid radical modified zero valent iron synthesized in example 1;
FIG. 3 is an SEM image of nanoscale ball-milled zero-valent iron and ball-milled oxoacid-modified zero-valent iron synthesized in example 1;
FIG. 4 is a TEM image of synthesized ball-milled zero-valent iron and ball-milled oxoacid-modified zero-valent iron;
FIG. 5 shows the detection of C1-C7 hydrocarbon content changes in gas chromatography mass spectrometry;
FIG. 6 shows the change in the content of gaseous products produced by photo-thermal conversion of waste plastics by ball milling of oxy-acid modified zero-valent iron;
FIG. 7 is a graph of C1-C7 hydrocarbon content of ball-milled zero-valent iron and ball-milled oxo-acid-modified zero-valent iron photo-thermal conversion waste plastic;
FIG. 8 is a graph showing the variation in C1-C7 hydrocarbon content of ball-milled zero-valent iron and non-ball-milled zero-valent iron photo-thermally converted waste plastics;
FIG. 9 is a graph showing the change in C1-C7 hydrocarbon content of air atmosphere ball-milled oxy-acid radical modified zero-valent iron and inert atmosphere ball-milled oxy-acid radical modified zero-valent iron photo-thermal conversion waste plastic;
FIG. 10 shows the variation of C1-C7 hydrocarbon content of ball milled boric acid/phosphate, carbonate, sulfate and silicate modified zero valent iron photo-thermal conversion waste plastics.
Detailed Description
The invention will now be described in detail with reference to the drawings and specific examples. The following examples are given by way of illustration of detailed embodiments and specific procedures based on the technical scheme of the present invention, but the scope of the present invention is not limited to the following examples.
Example 1
Ball milling preparation of oxygen acid modified zero-valent iron:
5.6g of commercial zero-valent iron powder (with the particle size of 80-150 mu m) is placed in an agate ball milling tank, then 0.62g of boric acid and 0.73g of sodium phosphate are added, inert gas is introduced into the ball milling tank, ball milling is carried out for 5 hours at the rotating speed of 500 revolutions per minute, and after the commercial zero-valent iron powder is naturally cooled to room temperature, the oxygen-containing acid modified zero-valent iron material is obtained after collection. Through IPC-OES test, the content of surface boric acid is 5.12%, and the content of surface phosphate is 3.43%.
FIG. 1 is an XRD pattern of ball-milled zero-valent iron and ball-milled oxoacid-modified zero-valent iron; as can be seen from the XRD pattern, the main component of the synthetic material is zero-valent iron.
Fig. 2 is an SEM image of micrometer scale ball milled zero valent iron and ball milled oxyacid radical modified zero valent iron: as can be seen from the SEM image, the particle size of the ball-milled, oxyacid radical-modified zero-valent iron (0.5 to 4 μm) was smaller than that of the ball-milled zero-valent iron (1 to 10 μm). (Panel a shows ball-milled zero-valent iron and panel b shows ball-milled oxygen acid modified zero-valent iron)
Fig. 3 is an SEM image of nanoscale ball-milled zero-valent iron and ball-milled oxyacid radical modified zero-valent iron: as can be seen from the SEM image, the particle size of the ball-milled, oxo-acid-modified zero-valent iron (80-300 nm) was smaller than that of the ball-milled, zero-valent iron (500-800 nm). (Panel a shows ball-milled zero-valent iron and panel b shows ball-milled oxygen acid modified zero-valent iron)
FIG. 4 is a TEM image of ball-milled zero-valent iron and ball-milled oxyacid radical modified zero-valent iron; from fig. 4 (a), it can be seen that the ball-milled zero-valent iron is irregular particles, the surface of the ball-milled zero-valent iron is not coated with a coating layer, and from fig. 4 (b), it can be seen that the ball-milled oxygen acid modified zero-valent iron mainly comprises an iron core and a carbon coating layer.
Preparation of control material ball milling zero-valent iron:
5.6g of commercial zero-valent iron powder is placed in an agate ball milling tank, inert gas is then introduced, ball milling is carried out for 5 hours at the rotation speed of 500 revolutions per minute, and after the commercial zero-valent iron powder is naturally cooled to room temperature, the commercial zero-valent iron powder is collected to obtain ball milling zero-valent iron.
Example 2
Realizing the preparation of high-added-value hydrocarbon fuel and environmental remediation materials by photo-thermal conversion of waste plastics:
waste plastics are mainly commercial low density polyethylene, which is washed, dried, sliced, and crushed to form smaller size precursors. Uniformly mixing 0.1g of waste plastic sample and 0.5g of catalyst (oxygen acid radical modified zero-valent iron obtained in example 1), introducing argon into a photo-thermal reactor, sampling and detecting the oxygen content in the gas in the reactor until the oxygen concentration is lower than a detection line. The simulated solar light source was turned on to photo-thermally convert waste plastic at lamp current 22A and the conversion of waste plastic to gas products was tested for different photo-thermal reaction times. The experimental results are shown in fig. 5: carbon dioxide, carbon monoxide and hydrocarbon (C1-C7) in the gas chromatograph, the photo-thermal reaction time is 8 hours, and the content of hydrocarbon products is the largest. FIG. 6 shows the detection of C1-C7 hydrocarbons in a gas chromatograph-mass spectrometer after 8 hours of photothermal reaction. FIG. 7 shows the change of the C1-C7 hydrocarbon content of the ball-milled zero-valent iron and the ball-milled oxygen acid radical modified zero-valent iron in different photo-thermal reaction time, and the ball-milled oxygen acid radical modified zero-valent iron has higher photo-thermal waste plastic conversion activity to produce C1-C7 hydrocarbon.
Comparative example 1
Non-ball-milling zero-valent iron photo-thermal conversion waste plastic to prepare high-added-value hydrocarbon fuel and environment restoration material:
uniformly mixing 0.1g of waste plastic sample and 0.5g of unground zero-valent iron, introducing argon into the photo-thermal reactor, sampling and detecting the oxygen content in the gas in the reactor until the oxygen concentration is lower than the detection line. The simulated solar light source was turned on to photo-thermally convert waste plastic at lamp current 22A and the conversion of waste plastic to gas products was tested for different photo-thermal reaction times. The experimental results are shown in fig. 8: compared with ball-milled zero-valent iron, non-ball-milled zero-valent iron cannot convert waste plastics through photo-thermal reaction to generate C1-C7 hydrocarbon.
Comparative example 2
Ball milling zero-valent iron photo-thermal conversion waste plastics in an air atmosphere and an inert atmosphere to prepare high-added-value hydrocarbon fuel and environment repairing materials:
uniformly mixing 0.1g of waste plastic sample and 0.5g of ball-milling oxyacid radical modified zero-valent iron (samples prepared in an air atmosphere and an inert atmosphere respectively), introducing argon into a photo-thermal reactor, sampling and detecting the oxygen content in the gas in the reactor until the oxygen concentration is lower than a detection line. The simulated solar light source was turned on to photo-thermally convert waste plastic at lamp current 22A and the conversion of waste plastic to gas products was tested for different photo-thermal reaction times. The experimental results are shown in fig. 9: compared with inert atmosphere ball milling oxy acid radical modified zero-valent iron, air atmosphere ball milling oxy acid radical modified zero-valent iron can not convert waste plastics through photo-thermal reaction to generate C1-C7 hydrocarbon.
Comparative example 3
Other oxygen-containing acid radical modified ball-milling zero-valent iron photo-thermal conversion waste plastics to prepare high-added value hydrocarbon fuel and environment repairing materials:
uniformly mixing 0.1g of waste plastic sample and 0.5g of ball-milling oxyacid radical modified zero-valent iron (respectively carbonate, sulfate and silicate), introducing argon into a photo-thermal reactor, sampling and detecting the oxygen content in the gas in the reactor until the oxygen concentration is lower than a detection line. The simulated solar light source was turned on to photo-thermally convert waste plastic at lamp current 22A and the conversion of waste plastic to gas products was tested for different photo-thermal reaction times. The experimental results are shown in fig. 10: compared with boric acid and phosphate modified ball-milling zero-valent iron, other oxo acid (carbonate, sulfate and silicate) modified ball-milling zero-valent iron cannot convert waste plastics through photo-thermal reaction to generate C1-C7 hydrocarbon.
The previous description of the embodiments is provided to facilitate a person of ordinary skill in the art in order to make and use the present invention. It will be apparent to those skilled in the art that various modifications can be readily made to these embodiments and the generic principles described herein may be applied to other embodiments without the use of the inventive faculty. Therefore, the present invention is not limited to the above-described embodiments, and those skilled in the art, based on the present disclosure, should make improvements and modifications without departing from the scope of the present invention.
Claims (8)
1. A method for photo-thermal conversion of zero-valent iron waste plastics into high-added-value fuel and environment restoration materials is characterized in that an oxygen-containing acid radical modified zero-valent iron material is used as a catalyst for photo-thermal conversion of waste plastics, the oxygen-containing acid radical modified zero-valent iron material has an irregular granular microstructure with micron-scale and/or nano-scale dimensions, and surface species comprise boric acid and phosphate radicals;
the diameter of the particles with the micron-scale size is between 0.5 and 10 mu m, and the diameter of the particles with the nanometer-scale size is between 80 and 800 nm;
the high value added fuel and environmental remediation material comprises H 2 High added value C1-C7 gas, C8-C30 medium carbon oil, high carbon wax and iron carbon environment restoration materials;
the preparation method of the oxygen acid modified zero-valent iron material comprises the following steps:
1) Mixing an oxygen-containing acid radical precursor with zero-valent iron to obtain solid powder;
2) And mechanically ball milling the solid powder in an inert atmosphere, naturally cooling to room temperature, and collecting to obtain the oxygen acid modified zero-valent iron material.
2. The method for converting zero-valent iron into high-value-added fuel and environment-repairing material by photo-thermal conversion waste plastics according to claim 1, wherein the boric acid mass content of the surface of the zero-valent iron material modified by the oxygen acid radical is 0.05-6.18%.
3. The method for converting zero-valent iron into high-value-added fuel and environmental remediation material by using waste plastics according to claim 1, wherein the mass content of phosphate on the surface of the zero-valent iron material modified by the oxygen acid radical is 0.01% -3.53%.
4. The method for converting zero-valent iron into high-value-added fuel and environmental remediation materials according to claim 1, wherein the oxygen-containing acid radical precursors in step 1) are boric acid and phosphate radicals.
5. The method for converting zero-valent iron into high-value-added fuel and environmental remediation materials by photo-thermal conversion waste plastics according to claim 1, wherein the mechanical ball milling rotational speed in step 2) is 100-500 rpm, and the ball milling time is 1-6 hours.
6. The method for converting zero-valent iron into high-value-added fuel and environment-repairing materials by photo-thermal conversion waste plastics according to claim 1, which is characterized in that the specific method comprises the following steps: the oxygen-containing acid radical modified zero-valent iron material is used as a photo-thermal catalyst, the oxygen-containing acid radical modified zero-valent iron material is uniformly mixed with waste plastics, inert gas is introduced into a photo-thermal reactor, a xenon lamp light source is used for simulating sunlight, and the obtained product is high-added-value fuel and an environment restoration material.
7. The method for converting zero-valent iron into high-value-added fuel and environmental remediation materials according to claim 6, wherein the mass ratio of the addition amount of the oxygen-containing acid-modified zero-valent iron material to the waste plastic to be treated is 5:1-1:10.
8. The method for photo-thermal converting zero-valent iron into high value-added fuel and environmental remediation material according to claim 6, wherein the photo-thermal reaction time is 1 to 8 hours.
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