A method and device for regenerating a VOC adsorbent based on sound-light cooperation
Patent Information
- Authority / Receiving Office
- CN · China
- Patent Type
- Applications(China)
- Current Assignee / Owner
- JIANGSU UNIV
- Filing Date
- 2026-03-23
- Publication Date
- 2026-05-29
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Figure CN122098533A_ABST
Abstract
Description
Technical Field
[0001] This invention belongs to the field of industrial waste gas purification, specifically relating to a method and apparatus for the regeneration and deactivation of VOCs adsorbents based on acoustic-optical synergistic regeneration. Background Technology
[0002] VOCs emitted from coal-fired boilers, waste incinerators, and industrial plants can cause serious harm to human health and the ecological environment, including carcinogenicity, teratogenicity, photochemical smog, and haze. To control the excessive emission of harmful VOCs, environmental scientists both domestically and internationally have developed numerous VOCs removal technologies, primarily including selective catalytic reduction (SCR) synergistic VOCs removal, catalytic combustion VOCs removal, adsorption VOCs removal, liquid-phase absorption VOCs removal, and free radical advanced oxidation VOCs removal. SCR technology can utilize existing equipment to synergistically remove VOCs, but it has limitations such as the susceptibility of SCR catalyst poisoning, and this technology is mainly limited to VOCs control in coal-fired flue gas. Catalytic combustion technology has advantages such as high treatment efficiency, wide applicability, and simple equipment, but it suffers from drawbacks such as high application costs and susceptibility to catalyst deactivation. Liquid-phase absorption VOCs removal technology has advantages such as mature processes and large processing capacity, but it is mainly suitable for organic compounds with high solubility, thus limiting its application scope. Free radical advanced oxidation VOCs removal technology is an emerging VOCs treatment technology in recent years, with advantages such as high pollutant degradation rate, wide range of pollutant applications, and environmentally friendly process. However, the maturity of related technologies is still relatively poor, requiring more research and development. Compared with other VOCs removal technologies, adsorption VOCs removal technology has comprehensive advantages such as high removal efficiency, mature and reliable technology, and environmentally friendly process. Its representative activated carbon and molecular sieve adsorption VOCs removal technologies have been widely used in various industries. However, the main challenge in the application of adsorption VOCs removal technology is its high operating cost. The main reason is that common adsorbents are susceptible to poisoning and deactivation caused by impurities such as sulfur, water, alkali metals, and heavy metals in the gas flow during operation, resulting in a short service life of the adsorbent and thus greatly increasing the operating cost of this technology. To reduce the operating costs of VOCs removal adsorbents, researching and developing efficient, environmentally friendly, and economical regeneration technologies for VOCs removal adsorbents is of significant scientific and engineering value. This can not only reduce the application costs of VOCs removal adsorption technology, but also effectively alleviate the solid waste post-treatment problems caused by deactivated VOCs removal adsorbents.
[0003] Domestic and international researchers have developed various regeneration technologies for VOCs adsorbents, including microwave regeneration, thermal regeneration, water washing regeneration, ultrasonic regeneration, acid washing regeneration, alkaline washing regeneration, traditional oxidant regeneration, and plasma regeneration. Acid washing and alkaline washing regeneration technologies can remove most harmful substances and have good regeneration effects, but strong acids and alkalis are highly corrosive to the adsorbent and easily damage its pore structure. Thermal and microwave regeneration technologies can achieve certain regeneration effects, but their operating energy consumption is very high, and they easily damage the pore structure of the adsorbent. Water washing regeneration technology can remove some loose harmful substances, but it is difficult to remove most stubborn harmful substances. Plasma regeneration has good regeneration effects, but plasma technology has drawbacks such as high energy consumption, low reliability of key devices, and poor safety; moreover, the extreme environment induced by plasma technology can easily damage the surface and pore structure of the adsorbent. Ultrasonic regeneration technology has low regeneration efficiency when used alone and is usually used as an auxiliary method in combination with other technologies. Traditional oxidants such as persulfate and hydrogen peroxide offer advantages like low cost and environmentally friendly processes for regenerating adsorbents. However, unactivated peroxides have very low oxidizing power, making it difficult to achieve good regeneration results. Traditional oxidants like sodium chlorite and potassium permanganate can achieve higher regeneration efficiency, but their high cost is a drawback. Furthermore, acid / alkali activation regeneration and regeneration with traditional oxidants (such as potassium permanganate and sodium chlorite) generate wastewater and waste liquid, leading to new secondary pollution problems. In summary, although numerous VOCs adsorbent regeneration technologies have been developed, these technologies generally suffer from low regeneration efficiency, high energy consumption, complex equipment, low reliability, high cost, or secondary pollution, hindering their widespread application. Therefore, it is necessary to actively develop a VOCs adsorbent regeneration method and device that is highly efficient, simple in equipment, low in cost, low in energy consumption, reliable, and environmentally friendly. Summary of the Invention
[0004] To address the aforementioned challenges, this invention provides a method and apparatus for the synergistic regeneration of deactivated VOCs adsorbents based on acoustic-optical regeneration. The principle involves using ultraviolet light and multi-frequency ultrasound in an acoustic-optical regeneration device to synergistically induce highly reactive free radicals and microjets carrying magnetic particles to activate and regenerate the deactivated VOCs adsorbent. The highly reactive free radicals can undergo vigorous chemical reactions with harmful substances covering the surface sites of the deactivated adsorbent, while the multi-gradient composite microjets generated by dual-frequency ultrasound, carrying magnetic nanoparticles, can efficiently impact the covering substances on the adsorbent surface and in the pores. The two synergistically regenerate the deactivated VOCs adsorbent from both chemical and physical perspectives. The method and apparatus for regenerating deactivated VOCs adsorbents provided by this invention have comprehensive advantages, including simple technology, high regeneration efficiency, high mass transfer and diffusion efficiency, energy saving and low carbon emissions, and green and environmentally friendly operation, making it of significant industrial value.
[0005] The present invention provides a device for regenerating deactivated VOCs adsorbent based on acoustic-optical synergistic regeneration, characterized in that it mainly includes an acoustic-optical regeneration device for regenerating deactivated VOCs adsorbent, a transverse low-frequency ultrasonic transmitter, an ultraviolet lamp tube, a longitudinal high-frequency ultrasonic transmitter, a magnetic nanoparticle trap, a membrane separator, as well as a material mixing tower, a waste heat drying and activation device, and a hot air circulation system.
[0006] The material mixing tower is connected to the main material inlet at the top of the acoustic-optical regeneration device and is used to mix the adsorbent, chemical reagents, and magnetic nanoparticles. Multiple transverse low-frequency ultrasonic transmitters, ultraviolet lamps, longitudinal high-frequency ultrasonic transmitters, and magnetic nanoparticle traps are evenly distributed within the acoustic-optical regeneration device. The transverse low-frequency ultrasonic transmitters emit transverse low-frequency ultrasonic waves, and the longitudinal high-frequency ultrasonic transmitters emit longitudinal high-frequency ultrasonic waves. A membrane separator is located at the bottom and is used to separate the residual liquid and adsorbent after regeneration.
[0007] The hot air circulation system is located at the waste heat drying and activation device, which is connected to the adsorbent outlet d of the acoustic-optical regeneration device, and uses process or flue gas waste heat to dry and activate the adsorbent.
[0008] Furthermore, the acoustic-optical regeneration device is a rectangular reactor with a cover plate on top, the material inlet c is the side of the top, the regenerated adsorbent outlet d is located on the lower side wall, and the bottom has a residual liquid outlet e; the material inlet c of the acoustic-optical regeneration device is connected to a material mixing tower, which has a reagent solution inlet a and a solid material inlet b.
[0009] Furthermore, in the aforementioned acoustic-optical regeneration device, the transverse low-frequency ultrasonic transmitter, the ultraviolet lamp, and the longitudinal high-frequency ultrasonic transmitter are all arranged in a sequential manner with equal spacing, and the effective length range of the spacing B is 10 cm to 40 cm.
[0010] Furthermore, multiple transverse low-frequency ultrasonic transmitters and magnetic nanoparticle traps are first suspended longitudinally at equal intervals on a vertically arranged hoisting shaft. Then, each row of transverse low-frequency ultrasonic transmitters and magnetic nanoparticle traps is arranged sequentially with ultraviolet lamps and longitudinal high-frequency ultrasonic transmitters at equal intervals. The effective length range of the spacing 2A between two adjacent transverse low-frequency ultrasonic transmitters in the same row is 10 cm to 40 cm. The effective range of the spacing A between the magnetic nanoparticle traps and the transverse low-frequency ultrasonic transmitters is 5 cm to 20 cm.
[0011] Furthermore, in the aforementioned sound-light regeneration device, the effective ultraviolet radiation intensity range of the ultraviolet lamp is 10 μW / cm². 2~ 220 μW / cm 2 The effective range of the emission wavelength is between 170 nm and 290 nm.
[0012] Furthermore, the transverse low-frequency ultrasound has a frequency range of 20-39 kHz and a power range of 20-200 W / L, while the longitudinal high-frequency ultrasound has a frequency range of 40-100 kHz and a power range of 30-250 W / L.
[0013] Furthermore, the chemical reagent is a mixture of potassium peroxymonosulfate and urea, wherein the concentration of potassium peroxymonosulfate is between 0.05 mol / L and 1.8 mol / L, the concentration of urea is between 0.01 mol / L and 1.2 mol / L, and the pH value is between 0.02 and 6.8.
[0014] Furthermore, the deactivated VOCs adsorbent mainly includes one or more of the following: biochar, porous carbon, molecular sieve, activated coke, petroleum coke, and activated carbon.
[0015] The method for regenerating and deactivating VOCs adsorbents based on the aforementioned acoustic-optical synergistic regeneration and deactivation device is characterized by comprising the following steps:
[0016] S1. Chemical reagents potassium persulfate and urea reagent are introduced into the material mixing tower through solution inlet a, and adsorbent and magnetic nanoparticles are introduced through solid material inlet b. Simultaneously, a transverse low-frequency ultrasonic transmitter, an ultraviolet lamp, and a longitudinal high-frequency ultrasonic transmitter are activated to synergistically induce strong oxidizing free radicals, including sulfate free radicals and hydroxyl free radicals, as well as strong reducing free radicals, including nitrogen atom free radicals and hydrogen atom free radicals. These highly active free radicals use their strong oxidizing and strong reducing properties to attack different types of harmful substances covering the active sites on the surface of the deactivated adsorbent. At the same time, a multi-gradient composite microjet induced by the combined transverse low-frequency ultrasound and longitudinal high-frequency ultrasound carries magnetic nanoparticles to impact the covering substances on the surface and pores of the adsorbent. The two work together to regenerate the deactivated VOCs adsorbent from both chemical and physical dimensions.
[0017] S2. After regeneration, magnetic nanoparticles in the solution are captured by magnetic separation using a magnetic nanoparticle trap. They are then released back into the solution during the next regeneration of the adsorbent for repeated use. The residual liquid and solid mixture after regeneration are rapidly separated by a membrane separator.
[0018] S3. The residual liquid after separation is discharged through residual liquid outlet e and then recycled and reused. The separated solid adsorbent enters the waste heat drying and activation device through regenerated adsorbent outlet d for drying and activation. The heat energy required for drying and activation is provided by process or flue gas waste heat. The dried and activated adsorbent is recycled and reused through dried and activated adsorbent outlet f.
[0019] Furthermore, the effective operating temperature of the acoustic-optical regeneration device is between 15°C and 68°C, while the effective operating temperature of the waste heat drying and activation device is between 60°C and 320°C.
[0020] The basic principle of the method and apparatus described in this invention is as follows: In the acoustic-optical regeneration device, ultraviolet light and multi-frequency ultrasound are used to synergistically induce highly active free radicals and microjets carrying magnetic particles to activate and regenerate the deactivated VOCs adsorbent. The regenerated adsorbent can be dried and activated using process or flue gas waste heat to obtain higher adsorption and VOCs removal performance. The above-mentioned adsorbent regeneration process can be represented by the following equations (1)-(3):
[0021] (1)
[0022] (2)
[0023] (3)
[0024] The principle behind this invention is to utilize ultraviolet light and multi-frequency ultrasound in a sound-optical regeneration device to synergistically induce highly reactive free radicals and microjets carrying magnetic particles to activate and regenerate deactivated VOCs adsorbents. The highly reactive free radicals can undergo vigorous chemical reactions with harmful substances covering the surface sites of the deactivated adsorbent, while the multi-gradient composite microjets generated by dual-frequency ultrasound, carrying magnetic nanoparticles, can efficiently impact the covering substances on the adsorbent surface and in the pores. The two work synergistically to regenerate the deactivated VOCs adsorbent from both chemical and physical perspectives. The method and apparatus for regenerating deactivated VOCs adsorbents provided by this invention have comprehensive advantages, including simple technology, high regeneration efficiency, high mass transfer and diffusion efficiency, energy saving and low carbon emissions, and green and environmentally friendly operation, making it highly valuable for industrial applications. The energy for the entire deactivated VOCs adsorbent regeneration process is mainly utilized from waste heat, and the residual liquid, residue, and byproducts during the regeneration process are all recovered and reused. Therefore, the entire regeneration process has multiple characteristics such as energy saving, low carbon emissions, and green environmental protection, demonstrating a sound approach to green and sustainable development.
[0025] This invention provides a method for regenerating deactivated VOCs adsorbents based on acoustic-optical synergistic regeneration. The physicochemical regeneration of deactivated VOCs adsorbents in a reaction solution is a multi-step heterogeneous physicochemical process involving diffusion, mass transfer, and chemical reactions. Mass transfer and diffusion are the dominant controlling steps in the VOCs adsorbent regeneration process. However, the most commonly used regeneration reactors in this field are currently heterogeneous reaction devices such as bubble beds, packed beds, and spray beds, which suffer from low diffusion and mass transfer rates and poor media mixing efficiency, hindering the industrial scale-up application of this technology. The acoustic-optical regeneration device provided by this invention utilizes multi-frequency ultrasound to synergistically induce multi-gradient composite microjets carrying magnetic particles to enhance the heterogeneous process of multiphase mass transfer-diffusion-reaction. This technology can form multi-gradient composite microjets, simultaneously carrying magnetic nanoparticles to impact or flush impurities on the adsorbent surface and in the pores from multiple dimensions. It exhibits strong multiphase and multi-dimensional mixing efficiency, and extremely high mass transfer and diffusion efficiency, demonstrating significant industrial application value.
[0026] In the field of regenerating deactivated VOCs adsorbents, most regeneration technologies generate waste liquids (such as alkalis, acids, potassium permanganate, and chlorine-containing oxidants), which can cause new secondary pollution problems and hinder the application of related technologies. The free radical oxidation technology provided by this invention mainly utilizes clean free radicals to activate and regenerate deactivated VOCs adsorbents. Compared with traditional adsorbent regeneration reagents, free radicals are a recognized clean oxidant, therefore their regeneration process has typical green and sustainable characteristics, making it a promising VOCs adsorbent regeneration reagent.
[0027] Existing VOCs adsorbent regeneration processes require high energy consumption, which hinders the large-scale application of related technologies. The VOCs regeneration method and apparatus provided by this invention mainly utilize waste heat from process or boiler flue gas to provide most of the heat energy required for several stages, including solution heating, adsorbent drying, and regeneration. Therefore, this technology has relatively low energy consumption, meets the current dual-carbon development strategy, and has good development and application prospects.
[0028] Therefore, compared with existing VOCs regeneration technologies, the method and apparatus for regenerating deactivated VOCs adsorbents by inducing free radical oxidation using free radicals in a clean and low-carbon manner, provided by this invention, has comprehensive technical and economic advantages, including simple apparatus, high regeneration efficiency, high mixing / mass transfer / diffusion efficiency, energy saving and low carbon emissions, and green and environmentally friendly operation. It is a novel VOCs adsorbent regeneration method and apparatus with broad development prospects. Attached Figure Description
[0029] Figure 1 This is a front view of the deactivated VOCs adsorbent regeneration device proposed in this invention.
[0030] Figure 2 This is a top view of the deactivated VOCs adsorbent regeneration device proposed in this invention.
[0031] Explanation of reference numerals in the attached diagram: 1. Acoustic-optical regeneration device; 2. Horizontal low-frequency ultrasonic transmitter; 3. Ultraviolet lamp; 4. Vertical high-frequency ultrasonic transmitter; 5. Magnetic nanoparticle trap; 6. Material mixing tower; 7. Cover plate; 8. Membrane separator; 9. Waste heat drying and activation device; 10. Hot air circulation system; 11. First control valve; 12. Second control valve; 13. Third control valve; a. Reagent solution inlet; b. Solid material inlet; c. Total material inlet; d. Regenerated adsorbent outlet; e. Residual liquid outlet; f. Dried and activated adsorbent outlet. Detailed Implementation
[0032] The present invention will be further described below with reference to the accompanying drawings and specific embodiments, but the scope of protection of the present invention is not limited to the following.
[0033] like Figure 1 and 2 As shown, this invention provides a method and apparatus for the synergistic regeneration and deactivation of VOCs adsorbents based on acoustic-optical regeneration. The principle is to utilize ultraviolet light and multi-frequency ultrasound in an acoustic-optical regeneration device to synergistically induce highly reactive free radicals and microjets carrying magnetic particles to activate and regenerate the deactivated VOCs adsorbent. The highly reactive free radicals can undergo vigorous chemical reactions with harmful substances covering the surface sites of the deactivated adsorbent, while the multi-gradient composite microjets generated by dual-frequency ultrasound, carrying magnetic nanoparticles, can efficiently impact the covering substances on the adsorbent surface and in the pores. The two work synergistically to regenerate the deactivated VOCs adsorbent from both chemical and physical perspectives. The method and apparatus for regenerating and deactivating VOCs adsorbents provided by this invention have comprehensive advantages such as simple technology, high regeneration efficiency, high mass transfer and diffusion efficiency, energy saving and low carbon emissions, and green and environmentally friendly operation, making it valuable for industrial applications.
[0034] The deactivated VOCs adsorbent regeneration device mainly includes an acoustic-optical regeneration device for regenerating deactivated VOCs adsorbents, a transverse low-frequency ultrasonic transmitter for emitting transverse low-frequency ultrasonic waves, an ultraviolet lamp for radiating ultraviolet light, a longitudinal high-frequency ultrasonic transmitter for emitting longitudinal high-frequency ultrasonic waves, a magnetic nanoparticle trap for capturing magnetic nanoparticles, a material mixing tower for mixing adsorbent / chemical reagents / magnetic nanoparticles and other materials, a membrane separator for separating the regenerated residual liquid and adsorbent, a waste heat drying and activation device for drying and activating the adsorbent using process or flue gas waste heat, a hot air circulation system for enhancing the drying and activation of the adsorbent, and various supporting pipelines and control valves.
[0035] The acoustic-optical regeneration device is a rectangular reactor with a cover plate 7 on top. Multiple horizontal low-frequency ultrasonic emitters, multiple ultraviolet lamps, multiple vertical high-frequency ultrasonic emitters, and a magnetic nanoparticle trap are located inside. A membrane separator is located at the bottom. The material inlet c is on the side of the top, and a first control valve 11 is located at the material inlet c. The regenerated adsorbent outlet d is located on the lower side wall, and a residual liquid outlet e is located at the bottom, with a third control valve 13 located at the residual liquid outlet e. The material inlet c of the acoustic-optical regeneration device is connected to a material mixing tower. The material mixing tower has a reagent solution inlet a and a solid material inlet b. The regenerated adsorbent outlet d of the acoustic-optical regeneration device is connected to a waste heat drying and activation device, with a second control valve 12 between them. The waste heat drying and activation device has a hot air circulation system and a dried and activated adsorbent outlet f.
[0036] The regeneration process of this method and apparatus is as follows: a chemical reagent composed of potassium persulfate and urea, along with the adsorbent and magnetic nanoparticles, are fed into a material mixing tower through the reagent solution inlet (a) and solid material inlet (b), respectively, and mixed uniformly. Inside the acoustic-optical regeneration device, a transverse low-frequency ultrasonic emitter, an ultraviolet lamp, and a longitudinal high-frequency ultrasonic emitter are simultaneously activated to synergistically activate and induce various highly reactive free radicals, such as strong oxidizing free radicals like sulfate radicals / hydroxyl radicals and strong reducing free radicals like nitrogen radicals / hydrogen radicals. These highly reactive free radicals attack different types of harmful substances covering the active sites on the surface of the deactivated adsorbent using both strong oxidizing and strong reducing properties. Simultaneously, a multi-gradient composite microjets induced by the combined transverse low-frequency and longitudinal high-frequency ultrasonic waves, carrying magnetic nanoparticles, efficiently impact the covering substances on the adsorbent surface and in the pores. The two processes synergistically regenerate the deactivated VOCs adsorbent from multiple dimensions, including chemical and physical processes. After regeneration, a magnetic nanoparticle trap is used to rapidly separate and capture the magnetic nanoparticles in the solution. These nanoparticles are then released back into the solution during the next adsorbent regeneration for repeated use, effectively solving the problem of rapid separation between magnetic nanoparticles and the adsorbent. The regenerated residual liquid and solid mixture undergo rapid liquid-solid separation via a membrane separator. The separated residual liquid is discharged through residual liquid outlet e and then recycled for reuse. For example, the generated ammonium sulfate and potassium sulfate can be evaporated and crystallized using process and flue gas waste heat to prepare agricultural fertilizers. The separated solid adsorbent enters a waste heat drying and activation device through regenerated adsorbent outlet d for further drying and activation. The heat energy required for drying and activation is provided by process or flue gas waste heat. The dried and activated adsorbent is recycled through dried and activated adsorbent outlet f, thus achieving the regeneration and reuse of deactivated VOCs adsorbents. The energy of the entire deactivated VOCs adsorbent regeneration process is mainly utilized from waste heat, and the residual liquid, residue, and by-products of the regeneration process are all recycled and reused. Therefore, the entire regeneration process has multiple characteristics such as energy saving, low carbon emissions, and green environmental protection, demonstrating a good green and sustainable development approach.
[0037] In the aforementioned sound-light regeneration device, as shown in the attached Figure 1 and 2As shown, the horizontal low-frequency ultrasonic transmitters, ultraviolet lamps, and vertical high-frequency ultrasonic transmitters are arranged in a sequentially arranged manner with equal spacing, and the effective length range of the spacing B is 10 cm to 40 cm. Specifically, multiple horizontal low-frequency ultrasonic transmitters and magnetic nanoparticle traps are first suspended on a vertically arranged hanging shaft in a longitudinally arranged manner with equal spacing. Then, each row of horizontal low-frequency ultrasonic transmitters and magnetic nanoparticle traps is arranged sequentially with equal spacing from the ultraviolet lamps and vertical high-frequency ultrasonic transmitters. The effective length range of the spacing 2A between two adjacent horizontal low-frequency ultrasonic transmitters in the same row is 10 cm to 40 cm; the effective range of the spacing A between the magnetic nanoparticle traps and the horizontal low-frequency ultrasonic transmitters is 5 cm to 20 cm.
[0038] In the aforementioned sound-light regeneration device, the effective ultraviolet radiation intensity range of the ultraviolet lamp is 10 μW / cm². 2 ~220 μW / cm 2 The effective range is between 170 nm and 290 nm. The frequency range of transverse low-frequency ultrasound is 20-39 kHz, and the power range is 20-200 W / L; the frequency range of longitudinal high-frequency ultrasound is 40-100 kHz, and the power range is 30-250 W / L.
[0039] The chemical reagent is a mixture of potassium peroxymonosulfate and urea. The concentration of potassium peroxymonosulfate ranges from 0.05 mol / L to 1.8 mol / L, the concentration of urea ranges from 0.01 mol / L to 1.2 mol / L, and the pH value ranges from 0.02 to 6.8. The effective operating temperature of the acoustic-optical regeneration device is between 15℃ and 68℃, while the effective operating temperature of the waste heat drying and activation device is between 60℃ and 320℃.
[0040] The deactivated VOCs adsorbents mainly include one or more of the following adsorbents: biochar, porous carbon, molecular sieve, activated coke, petroleum coke, and activated carbon.
[0041] The method for regenerating and deactivating VOCs adsorbents based on the aforementioned acoustic-optical synergistic regeneration and deactivation device is characterized by comprising the following steps:
[0042] S1. Chemical reagents potassium persulfate and urea reagent are introduced into the material mixing tower through solution inlet a, and adsorbent and magnetic nanoparticles are introduced through solid material inlet b. Simultaneously, a transverse low-frequency ultrasonic emitter, an ultraviolet lamp, and a longitudinal high-frequency ultrasonic emitter are activated to synergistically induce strong oxidizing free radicals, including sulfate free radicals and hydroxyl free radicals, as well as strong reducing free radicals, including nitrogen atom free radicals and hydrogen atom free radicals. These highly active free radicals use their strong oxidizing and strong reducing properties to attack different types of harmful substances covering the active sites on the surface of the deactivated adsorbent. At the same time, a multi-gradient composite microjets induced by the combined transverse low-frequency ultrasound and longitudinal high-frequency ultrasound carry magnetic nanoparticles to impact the covering substances on the surface and pores of the adsorbent. The two work together to regenerate the deactivated VOCs adsorbent from both chemical and physical dimensions.
[0043] S2. After regeneration, magnetic nanoparticles in the solution are captured by a magnetic nanoparticle trap. These nanoparticles are then released back into the solution during the next adsorbent regeneration for repeated use, effectively solving the problem of rapid separation between magnetic nanoparticles and the adsorbent. The residual liquid and solid mixture after regeneration undergoes rapid liquid-solid separation via a membrane separator.
[0044] S3. The residual liquid after separation is discharged through residual liquid outlet e and then recycled and reused. For example, the generated ammonium sulfate and potassium sulfate can be used to prepare agricultural fertilizers by evaporation and crystallization using process and flue gas waste heat. The separated solid adsorbent enters the waste heat drying and activation device through the regenerated adsorbent outlet d for drying and activation. The heat energy required for drying and activation is all heated by process or flue gas waste heat. The adsorbent after drying and activation is recycled and reused.
[0045] The following are implementation examples of the method and system's effect on adsorbent regeneration under different preliminary test conditions:
[0046] Example 1:
[0047] Taking self-made wheat straw biochar as an example (initial toluene removal efficiency of 93.2%), the concentration of potassium persulfate was 0.1 mol / L, the concentration of urea was 0.05 mol / L, the pH of the mixed reagent was 2.1, the operating temperature was 25℃, the drying and activation temperature was 160℃, and the ultraviolet radiation intensity was 41 μW / cm². 2 The wavelength of the ultraviolet light was 254 nm, the low-frequency ultrasound frequency was 28 kHz, and the high-frequency ultrasound frequency was 40 kHz. Preliminary results showed that the toluene removal efficiency after adsorbent regeneration was 40.1%.
[0048] Example 2:
[0049] Taking self-made wheat straw biochar as an example (initial toluene removal efficiency of 93.2%), the concentration of potassium persulfate was 0.2 mol / L, the concentration of urea was 0.05 mol / L, the pH of the mixed reagent was 2.1, the operating temperature was 25℃, the drying and activation temperature was 160℃, and the ultraviolet radiation intensity was 41 μW / cm². 2 The wavelength of the ultraviolet light was 254 nm, the low-frequency ultrasound frequency was 28 kHz, and the high-frequency ultrasound frequency was 40 kHz. Preliminary results showed that the toluene removal efficiency after adsorbent regeneration was 49.6%.
[0050] Example 3:
[0051] Taking self-made wheat straw biochar as an example (initial toluene removal efficiency of 93.2%), the concentration of potassium persulfate was 0.2 mol / L, the concentration of urea was 0.1 mol / L, the pH of the mixed reagent was 2.1, the operating temperature was 25℃, the drying and activation temperature was 160℃, and the ultraviolet radiation intensity was 41 μW / cm². 2 The wavelength of the ultraviolet light was 254 nm, the low-frequency ultrasound frequency was 28 kHz, and the high-frequency ultrasound frequency was 40 kHz. Preliminary results showed that the toluene removal efficiency after adsorbent regeneration was 58.0%.
[0052] Example 4:
[0053] Taking self-made wheat straw biochar as an example (initial toluene removal efficiency of 93.2%), the concentration of potassium persulfate was 0.2 mol / L, the concentration of urea was 0.1 mol / L, the pH of the mixed reagent was 2.1, the operating temperature was 25℃, the drying and activation temperature was 160℃, and the ultraviolet radiation intensity was 78 μW / cm². 2 The wavelength of the ultraviolet light was 254 nm, the low-frequency ultrasound frequency was 28 kHz, and the high-frequency ultrasound frequency was 40 kHz. Preliminary results showed that the toluene removal efficiency after adsorbent regeneration was 72.9%.
[0054] Example 5:
[0055] Taking self-made wheat straw biochar as an example (initial toluene removal efficiency of 93.2%), the concentration of potassium persulfate was 0.3 mol / L, the concentration of urea was 0.1 mol / L, the pH of the mixed reagent was 2.1, the operating temperature was 25℃, the drying and activation temperature was 160℃, and the ultraviolet radiation intensity was 78 μW / cm². 2 The wavelength of the ultraviolet light was 254 nm, the low-frequency ultrasound frequency was 28 kHz, and the high-frequency ultrasound frequency was 40 kHz. Preliminary results showed that the toluene removal efficiency after adsorbent regeneration was 80.7%.
[0056] Example 6:
[0057] Taking self-made wheat straw biochar as an example (initial toluene removal efficiency of 93.2%), the concentration of potassium persulfate was 0.4 mol / L, the concentration of urea was 0.1 mol / L, the pH of the mixed reagent was 2.1, the operating temperature was 25℃, the drying and activation temperature was 160℃, and the ultraviolet radiation intensity was 78 μW / cm². 2 The wavelength of the ultraviolet light was 254 nm, the low-frequency ultrasound frequency was 28 kHz, and the high-frequency ultrasound frequency was 40 kHz. Preliminary results showed that the toluene removal efficiency after adsorbent regeneration was 85.8%.
[0058] Example 7:
[0059] Taking self-made wheat straw biochar as an example (initial toluene removal efficiency of 93.2%), the concentration of potassium persulfate was 0.4 mol / L, the concentration of urea was 0.2 mol / L, the pH of the mixed reagent was 2.1, the operating temperature was 25℃, the drying and activation temperature was 160℃, and the ultraviolet radiation intensity was 78 μW / cm². 2 The wavelength of the ultraviolet light was 254 nm, the low-frequency ultrasound frequency was 28 kHz, and the high-frequency ultrasound frequency was 40 kHz. Preliminary results showed that the toluene removal efficiency after adsorbent regeneration was 88.9%.
[0060] Example 8:
[0061] Taking self-made wheat straw biochar as an example (initial toluene removal efficiency of 93.2%), the concentration of potassium persulfate was 0.5 mol / L, the concentration of urea was 0.2 mol / L, the pH of the mixed reagent was 2.1, the operating temperature was 25℃, the drying and activation temperature was 160℃, and the ultraviolet radiation intensity was 78 μW / cm². 2 The wavelength of the ultraviolet light was 254 nm, the low-frequency ultrasound frequency was 28 kHz, and the high-frequency ultrasound frequency was 40 kHz. Preliminary results showed that the toluene removal efficiency after adsorbent regeneration was 91.3%.
[0062] As demonstrated by the above embodiments, the regeneration method and system of the present invention can achieve high VOCs adsorbent regeneration efficiency and has advantages such as energy saving, low carbon emissions, simple equipment, and clean and environmentally friendly operation, exhibiting significant technical, economic, and market competitiveness. Furthermore, the embodiments described are preferred embodiments of the present invention, but the present invention is not limited to the embodiments mentioned above. Any obvious substitutions, improvements, or modifications that can be made by those skilled in the art without departing from the essence of the present invention are within the scope of protection of the present invention.
Claims
1. A device for the regeneration and deactivation of VOCs adsorbents based on acoustic-optical synergistic regeneration, characterized in that, It mainly includes an acoustic-optical regeneration device (1) for regenerating deactivated VOCs adsorbents, a transverse low-frequency ultrasonic transmitter (2) placed in the acoustic-optical regeneration device (1), an ultraviolet lamp (3), a longitudinal high-frequency ultrasonic transmitter (4), a magnetic nanoparticle trap (5), a membrane separator (8), a material mixing tower (6), a waste heat drying and activation device (9), and a hot air circulation system (10). The material mixing tower (6) is connected to the material inlet at the top of the acoustic-optical regeneration device (1) and is used to mix adsorbent, chemical reagents and magnetic nanoparticles. Multiple transverse low-frequency ultrasonic transmitters (2), ultraviolet lamps (3), longitudinal high-frequency ultrasonic transmitters (4) and magnetic nanoparticle traps (5) are evenly distributed in the acoustic-optical regeneration device (1). The transverse low-frequency ultrasonic transmitters (2) are used to emit transverse low-frequency ultrasonic waves, and the longitudinal high-frequency ultrasonic transmitters (4) are used to emit longitudinal high-frequency ultrasonic waves. The membrane separator (8) is located at the bottom and is used to separate the residual liquid and adsorbent after regeneration. The hot air circulation system (10) is located at the waste heat drying and activation device (9), which is connected to the adsorbent outlet d of the sound-light regeneration device (1) to dry and activate the adsorbent using process or flue gas waste heat.
2. The device for regenerating and deactivating VOCs adsorbent based on acoustic-optical synergistic regeneration according to claim 1, characterized in that, The sound-light regeneration device (1) is a rectangular reactor with a cover plate (7) on the top, the material inlet c is the side of the top, the regenerated adsorbent outlet d is located on the lower side wall, and the bottom has a residual liquid outlet e. The material inlet c of the sound-light regeneration device (1) is connected to the material mixing tower (6), and the material mixing tower (6) is provided with a reagent solution inlet a and a solid material inlet b.
3. The device for regenerating and deactivating VOCs adsorbent based on acoustic-optical synergistic regeneration according to claim 1, characterized in that, In the aforementioned acoustic-optical regeneration device (1), the transverse low-frequency ultrasonic transmitter (2), the ultraviolet lamp (3), and the longitudinal high-frequency ultrasonic transmitter (4) are arranged in a sequential manner with equal spacing, and the effective length range of their spacing B is 10 cm ~ 40 cm.
4. The device for regenerating and deactivating VOCs adsorbent based on acoustic-optical synergistic regeneration according to claim 1, characterized in that, Multiple transverse low-frequency ultrasonic transmitters (2) and magnetic nanoparticle traps (5) are first suspended longitudinally at equal intervals on a vertically arranged hoisting shaft. Then, each row of transverse low-frequency ultrasonic transmitters (2) and magnetic nanoparticle traps (5) is arranged sequentially with ultraviolet lamps (3) and longitudinal high-frequency ultrasonic transmitters (4) at equal intervals. The effective length range of the distance 2A between two adjacent transverse low-frequency ultrasonic transmitters (2) in the same row is 10 cm to 40 cm. The effective range of the distance A between the magnetic nanoparticle traps (5) and the transverse low-frequency ultrasonic transmitters (2) is 5 cm to 20 cm.
5. The device for regenerating and deactivating VOCs adsorbent based on acoustic-optical synergistic regeneration according to claim 1, characterized in that, In the aforementioned sound-light regeneration device (1), the effective ultraviolet radiation intensity range of the ultraviolet lamp tube (3) is within 10 μW / cm². 2 ~ 220μW / cm 2 The effective range of the emission wavelength is between 170 nm and 290 nm.
6. The device for regenerating and deactivating VOCs adsorbent based on acoustic-optical synergistic regeneration according to claim 1, characterized in that, The transverse low-frequency ultrasound has a frequency range of 20-39 kHz and a power range of 20-200 W / L, while the longitudinal high-frequency ultrasound has a frequency range of 40-100 kHz and a power range of 30-250 W / L.
7. The device for regenerating and deactivating VOCs adsorbent based on acoustic-optical synergistic regeneration according to claim 1, characterized in that, The chemical reagent is a mixture of potassium peroxymonosulfate and urea, wherein the concentration of potassium peroxymonosulfate is between 0.05 mol / L and 1.8 mol / L, the concentration of urea is between 0.01 mol / L and 1.2 mol / L, and the pH value is between 0.02 and 6.
8.
8. The device for regenerating and deactivating VOCs adsorbent based on acoustic-optical synergistic regeneration according to claim 1, characterized in that, The deactivated VOCs adsorbents mainly include one or more of the following: biochar, porous carbon, molecular sieve, activated coke, petroleum coke, and activated carbon.
9. A method for regenerating and deactivating a VOCs adsorbent based on the device for regenerating and deactivating a VOCs adsorbent based on the acoustic-optical synergistic method according to any one of claims 1-8, characterized in that, Includes the following steps: S1. Chemical reagents potassium persulfate and urea reagent are fed into the material mixing tower (6) through solution inlet a, and adsorbent and magnetic nanoparticles are fed into the material mixing tower (6) through solid material inlet b. Simultaneously, the transverse low-frequency ultrasonic transmitter (2), ultraviolet lamp (3) and longitudinal high-frequency ultrasonic transmitter (4) are activated to synergistically activate and induce strong oxidizing free radicals including sulfate free radicals and hydroxyl free radicals, as well as strong reducing free radicals including nitrogen atom free radicals / hydrogen atom free radicals. These highly active free radicals use strong oxidizing and strong reducing properties to attack different types of harmful substances covering the active sites on the surface of the deactivated adsorbent. At the same time, the multi-gradient composite microjets induced by the transverse low-frequency ultrasonic and longitudinal high-frequency ultrasonic carry magnetic nanoparticles to impact the covering substances on the surface and pores of the adsorbent. The two work together to regenerate the deactivated VOCs adsorbent from both chemical and physical dimensions. S2. After regeneration, magnetic nanoparticles in the solution are captured by magnetic separation using a magnetic nanoparticle trap (5). They are released back into the solution for repeated use during the next regeneration of the adsorbent. The residual liquid and solid mixture after regeneration are rapidly separated by a membrane separator (8). S3. The residual liquid after separation is discharged through the residual liquid outlet e and then recycled and reused. The solid adsorbent after separation enters the waste heat drying and activation device (9) through the regenerated adsorbent outlet d for drying and activation. The heat energy required for drying and activation is heated by the process or flue gas waste heat. The adsorbent after drying and activation is recovered through the dried and activated adsorbent outlet f.
10. The method for regenerating and deactivating VOCs adsorbent according to claim 9, characterized in that, The effective operating temperature of the sound-light regeneration device (1) is between 15°C and 68°C, while the effective operating temperature of the waste heat drying and activation device (9) is between 60°C and 320°C.