CN105251441A - High-performance mesoporous-micro double hole controllable molecular sieve adsorbent and preparation and application thereof - Google Patents
High-performance mesoporous-micro double hole controllable molecular sieve adsorbent and preparation and application thereof Download PDFInfo
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Abstract
The invention belongs to the technical field of air pollution control and particularly relates to high-performance mesoporous-micro double hole controllable molecular sieve adsorbent and preparation and application thereof. The preparation method includes the following steps that a silicon source, an aluminium source, a microporous structure guide agent, a mesoporous template agent, organosilane and water serve as raw materials for synthesizing mother liquor, the mother liquor assists into a hydrothermal reaction through microwaves, a product obtained through the reaction is subjected to centrifugation, drying and calcinations, and the high-performance mesoporous-micro double hole controllable molecular sieve adsorbent is obtained. According to the high-performance mesoporous-micro double hole controllable molecular sieve adsorbent and preparation and application thereof, an efficient method is utilized for preparing a mesoporous type zeolite molecular sieve which is high in specific surface, high in pore volume and high in adsorptive property, the synthesis time is greatly shortened, and the synthesis process is simplified. The synthesized zeolite type molecular sieve adsorbent is of a hierarchical pore structure, the pore diameter is adjustable, the mass transfer resistance is small, high adsorptive property of VOCs is achieved, high hydrophobic property and hydrothermal stability are achieved, and the high-performance mesoporous-micro double hole controllable molecular sieve adsorbent has high application value in the field of VOCs processing technologies.
Description
Technical field
The invention belongs to technical field of air pollution control, be specifically related to a kind of high-performance and be situated between the controlled adsorbent of molecular sieve of micro-diplopore and Synthesis and applications thereof.
Background technology
Volatile organic matter (VolatileOrganicCompounds, VOCs) refers to that saturated vapour pressure is greater than the organic compound of boiling point within 260 DEG C under 70Pa, normal pressure at normal temperatures.VOCs is a kind of common atmosphere pollution, is mainly derived from the industries such as printing, application, pharmacy, Furniture manufacture and petrochemical industry.These organic exhaust gas majorities are inflammable and explosive, and often distribute in atmosphere with peculiar smell, stench, just can produce spread effect to the eye of people, nose, respiratory system, even can bring out human canceration, sudden change under lower solubility.
Along with the enhancing of people's environmental protection consciousness; atmosphere pollutants emission standards is subject to various countries and more and more payes attention to; " discharge standard of air pollutants " (GB16297-1996) that China comes into effect on January 1st, 1997 defines the 14 class VOCs discharge standards such as toluene, dimethylbenzene, vinyl chloride, and various places have also in succession been put into effect industry VOCs and discharged provincial standard.Conventional VOCs emission-reduction technology has adsorption condensing, direct oxidation, catalytic oxidation, photochemical catalytic oxidation and biological filter membrane etc.Wherein absorption method is one of most effective method, and it is with low cost, easy to operate, has higher clearance at low concentration.Active carbon is current most popular adsorbent, but inflammability limits active carbon absorption property under the high temperature conditions; Silica gel has higher adsorption capacity to VOCs in dry conditions, but due to its hydrophilic character, is declining to a great extent under complex industrial condition to VOCs adsorbance.Patent 201110006599.6 discloses a kind of organic resin organic matter to superpower absorption property, but the restriction of its matter property, and this adsorbent can only use at a lower temperature; Patent 01126842.5 utilizes the character of diatomite porous property high-ratio surface to synthesize a kind of fly ash-based adsorbent, although have certain adsorption capacity to VOCs, generated time is long, consumes energy high, is unfavorable for industrial applications.
Summary of the invention
For solving the shortcoming and defect part of prior art, primary and foremost purpose of the present invention is to provide a kind of high-performance to be situated between the preparation method of the controlled adsorbent of molecular sieve of micro-diplopore.
The high-performance that another object of the present invention is to provide above-mentioned preparation method to obtain is situated between the controlled adsorbent of molecular sieve of micro-diplopore.
Another object of the present invention is to provide above-mentioned high-performance to be situated between the application of the controlled adsorbent of molecular sieve of micro-diplopore.
The object of the invention is achieved through the following technical solutions:
A kind of high-performance is situated between the preparation method of the controlled adsorbent of molecular sieve of micro-diplopore, comprise the following steps: be Material synthesis mother liquor with silicon source, aluminium source, microcellular structure directed agents, mesoporous template, organosilan and water, mother liquor utilizes microwave radiation technology hydro-thermal reaction, by centrifugal, dry, the roasting of product of reaction gained, obtain described high-performance and to be situated between the controlled adsorbent of molecular sieve of micro-diplopore.
Described silicon source is with SiO
2meter, aluminium source is with Al
2o
3meter, reaction raw materials mol ratio is SiO
2: water=0.025, SiO
2: microcellular structure directed agents=5, SiO
2: Al
2o
3=50 ~ 400, SiO
2: organosilan=10 ~ 40, the addition of described mesoporous template can be selected at SiO
2: mesoporous template=5 ~ 20, the pore-size distribution that can regulate product with dosage is added by the kind changing mesoporous template.
Described mesoporous template is anion surfactant; Described silicon source is ethyl orthosilicate; Described aluminium source is aluminium isopropoxide; Described microcellular structure directed agents is at least one in TPAOH (TPAOH), tetraethyl ammonium hydroxide (TEAOH) and ethylenediamine.
Described anion surfactant is preferably at least one in n-hexadecyl sodium sulfonate, myristyl sodium sulfonate, neopelex and sodium laurate.
Described organosilan is preferably at least one in 3-aminopropyl triethoxysilane, (3-mercaptopropyi) trimethoxy silane and chloropropyl triethoxysilane.
Described preparation method's concrete steps are as follows:
(1) take microcellular structure directed agents soluble in water, add aluminium source, be stirred to the hydrolysis of aluminium source; Then add silicon source under agitation, obtain A liquid;
(2) take mesoporous template to be added to the water, add organosilan after stirring a period of time, obtain B liquid;
(3) joined by the B liquid that step (2) is obtained in the obtained A liquid of step (1), adjust ph, continues to stir a period of time, obtains mother liquor;
(4) mother liquor that step (3) is obtained is proceeded to reactor, microwave hydrothermal reacts; By centrifugal, dry, the roasting of product of reaction gained, obtain described high-performance and to be situated between the controlled adsorbent of molecular sieve of micro-diplopore.
The time of stirring described in step (2) is 10 ~ 60 minutes; PH value described in step (3) is for being adjusted to 8.8 ~ 10.2; The time of the stirring described in step (3) is 1 ~ 2 hour.
Microwave hydrothermal optimum condition described in step (4) is that temperature arranges 80 ~ 170 DEG C, hydro-thermal reaction 0.5 ~ 4 hour.
Temperature dry described in step (4) is 80 ~ 110 DEG C, and the dry time is 8 ~ 24h; The temperature of described roasting is preferably 450 ~ 750 DEG C, and the time of roasting is preferably 4 ~ 12 hours.Centrifugal described in step (4) refer to repeatedly centrifugal to supernatant in neutral.
Present invention also offers a kind of high-performance obtained by above-mentioned preparation method to be situated between the controlled adsorbent of molecular sieve of micro-diplopore.Mesoporous, the micropore ratio of this adsorbent can control, and high adsorption capacity is also applicable to multiple industrial condition, and has high hydrophobicity and hydrothermal stability.
The above-mentioned high-performance controlled adsorbent of molecular sieve of micro-diplopore that is situated between can be applicable to purifying organic, particularly volatile organic matter (VOCs).Use toluene to carry out adsorption experiment for analog gas in the present invention, adsorbance reaches 300 ~ 500mg/g.
Mechanism of the present invention is: construct mesoporous in traditional zeolite molecular sieve by adding mesoporous template, improves molecular sieve to while VOCs adsorption capacity, maintains the original high hydrophobicity of zeolite molecular sieve, high thermal stability and high hydrothermal stability energy.The method utilizes microwave radiation technology hydro-thermal reaction, obtain mesoporous in order, degree of crystallinity is high, aperture is adjustable hydrophobic type zeolite molecular sieve, and this molecular sieve is carried out to the adsorption experiment of low-concentration organic, result shows this molecular sieve and has high-adsorption-capacity to VOCs.Present invention process is simple, and generated time is short, and cost is low, and has good absorption property to volatile organic matter, has a good application prospect in adsorbing domain.
Prior art uses synthesized by surfactant is the molecular sieve of pure mesoporous type, and hole wall is unformed shape, and this makes their heat endurance, hydrothermal stability and hydrophobicity poor, limits the application in VOCs absorption.And innovative point of the present invention is, construct mesoporous in traditional zeolite type micro porous molecular sieve, the zeolite-type molecular sieves that the micro-diplopore of synthesis Jie is controlled, this molecular sieve maintains the intrinsic heat endurance of zeolite type micro porous molecular sieve and hydrothermal stability, expand aperture simultaneously and be conducive to organic mass transfer, the character of the micropore that is situated between in addition is conducive to the VOCs gas absorption of different molecular radius.
Another innovative point of the present invention in traditional zeolite type micro porous molecular sieve synthesis technique, adds surfactant and organosilan constructed mesoporous (comprise medicament and add kind, sequentially) by the acting in conjunction of electrostatic assembly principle, organosilan one end can be combined with silicon species, the other end combines with surfactant micella, thus in crystallization process, form intracrystalline mesoporous.
Use microwave radiation technology hydro-thermal can improve generated time by high degree, simplify synthesis technique, this technique has and is used in synthetic zeolite type micro porous molecular sieve, but yet there are no systematic research in synthesis Jie micro porous molecular sieve technique.The present invention uses using microwave assisted aqueous extraction heat to shorten generated time, is also conducive to the combination between silicon species and organosilan agent surfactant simultaneously, promotes to obtain degree of crystallinity product better.
Compared with prior art, the present invention has the following advantages and beneficial effect:
(1) the present invention uses a kind of efficient method to prepare the mesoporous type zeolite molecular sieve of high-ratio surface, high pore volume and high absorption property, significantly shortens generated time, simplifies synthesis technique.
(2) the zeolite-type molecular sieve adsorbant of the present invention's synthesis is hierarchical porous structure, and mesoporous, micropore ratio controllable, resistance to mass tranfer is little, is conducive to the adsorption desorption process of large molecule VOCs.
(3) adsorbent of molecular sieve of the present invention's synthesis has high absorption property to VOCs, can reach the adsorption capacity of 300 ~ 500mg/g to toluene; And there is high hydrophobicity and hydrothermal stability, the industrial condition that can be applicable to hot humid carries out absorption to VOCs and reduces discharging process; In VOCs processing technology field, there is higher using value.
(4) technology of preparing of the present invention is flexible, and zeolite molecular sieve that can be dissimilar according to the synthesis of structure directing agent difference, as Y type, X, beta molecular sieve and ZSM-5 molecular sieve etc.
Accompanying drawing explanation
The N of Fig. 1 controlled adsorbent of molecular sieve of the micro-diplopore of Jie of high absorption property synthesized by the embodiment of the present invention 3
2adsorption and desorption isotherms.
The N of Fig. 2 controlled adsorbent of molecular sieve of the micro-diplopore of Jie of high absorption property synthesized by the embodiment of the present invention 5
2adsorption and desorption isotherms.
The controlled adsorbent of molecular sieve of the micro-diplopore of Jie of Fig. 3 high absorption property synthesized by the embodiment of the present invention 3 is to the adsorption isotherm of toluene.
The controlled adsorbent of molecular sieve of the micro-diplopore of Jie of Fig. 4 high absorption property synthesized by the embodiment of the present invention 5 is to the adsorption isotherm of toluene.
Detailed description of the invention
Below in conjunction with embodiment and accompanying drawing, the present invention is described in further detail, but embodiments of the present invention are not limited thereto.
Microwave equipment used in the embodiment of the present invention is preferably the MARS6 high flux airtight microwave digestion system that U.S. CE M company produces.
Embodiment 1
Prepare high-performance according to following steps to be situated between the controlled adsorbent of molecular sieve of micro-diplopore:
(1) add in 20mL distilled water by 8.12g TPAOH (TPAOH, 25% aqueous solution), stirred at ambient temperature adds aluminium isopropoxide 0.102g after mixing, and is stirred to aluminium isopropoxide complete hydrolysis; Take ethyl orthosilicate 10.4g, under 750r/min rotating speed stirs, dropwise instill above-mentioned solution, obtain A liquid;
(2) 1.5g myristyl sodium sulfonate is dissolved in 16mL distilled water, 40 DEG C of stirring in water bath, after 1 hour, in solution, add 0.3g3-chloropropyl triethoxysilane, obtain B liquid;
(3) the B liquid that step (2) is obtained is joined in the obtained A liquid of step (1) fast, regulate pH=9.7, stir 2 hours, obtain mother liquor;
(4) mother liquor obtained for step (3) is proceeded in 100mL polytetrafluoroethylene (PTFE) reactor, 80 DEG C of hydro-thermal reactions 4 hours under microwave radiation technology; Centrifugal, dry, 450 DEG C of roastings 12 hours, remove template, obtain white powder samples, are described high-performance and are situated between the controlled adsorbent of molecular sieve of micro-diplopore, be labeled as A1.
Embodiment 2
Prepare high-performance according to following steps to be situated between the controlled adsorbent of molecular sieve of micro-diplopore:
(1) add in 20mL distilled water by 8.12g TPAOH (TPAOH, 25% aqueous solution), stirred at ambient temperature adds aluminium isopropoxide 0.204g after mixing, and is stirred to aluminium isopropoxide complete hydrolysis.Take ethyl orthosilicate 10.4g, under 750r/min rotating speed stirs, dropwise instill above-mentioned solution, obtain A liquid;
(2) 3.28g n-hexadecyl sodium sulfonate is dissolved in 16mL distilled water, 40 DEG C of stirring in water bath, after 1 hour, in solution, add 1.1g3-aminopropyl triethoxysilane, obtain B liquid;
(3) the B liquid that step (2) is obtained is joined in the obtained A liquid of step (1) fast, regulates pH=8.8, stir 2 hours,
(4) mixed liquor is proceeded in 100mL polytetrafluoroethylene (PTFE) reactor, 110 DEG C of hydro-thermal reactions 3 hours under microwave radiation technology; Centrifugal, dry, 550 DEG C of roastings 8 hours, remove template, obtain white powder samples, are described high-performance and are situated between the controlled adsorbent of molecular sieve of micro-diplopore, be labeled as A2.
Embodiment 3
Prepare high-performance according to following steps to be situated between the controlled adsorbent of molecular sieve of micro-diplopore:
(1) add in 20mL distilled water by 8.12g TPAOH (TPAOH, 25% aqueous solution), stirred at ambient temperature adds aluminium isopropoxide 0.408g after mixing, and is stirred to aluminium isopropoxide complete hydrolysis; Take ethyl orthosilicate 10.4g, under 750r/min rotating speed stirs, dropwise instill above-mentioned solution, obtain A liquid;
(2) 3.48g neopelex is dissolved in 16mL distilled water, 40 DEG C of stirring in water bath, after 1 hour, in solution, add 0.55g3-aminopropyl triethoxysilane, obtain B liquid;
(3) the B liquid that step (2) is obtained is joined in the obtained A liquid of step (1) fast, regulates pH=9.7, stir 2 hours,
(4) mixed liquor is proceeded in 100mL polytetrafluoroethylene (PTFE) reactor, 140 DEG C of hydro-thermal reactions 2 hours under microwave radiation technology; Centrifugal, dry, 650 DEG C of roastings 6 hours, remove template, obtain white powder samples, are described high-performance and are situated between the controlled adsorbent of molecular sieve of micro-diplopore, be labeled as A3.
Embodiment 4
Prepare high-performance according to following steps to be situated between the controlled adsorbent of molecular sieve of micro-diplopore:
(1) add in 20mL distilled water by 8.12g TPAOH (TPAOH, 25% aqueous solution), stirred at ambient temperature adds aluminium isopropoxide 0.051g after mixing, and is stirred to aluminium isopropoxide complete hydrolysis; Take ethyl orthosilicate 10.4g, under 750r/min rotating speed stirs, dropwise instill above-mentioned solution, obtain A liquid;
(2) dissolve in 16mL distilled water by 0.56g laurate acid sodium, 40 DEG C of stirring in water bath, after 1 hour, add 0.49g (3-mercaptopropyi) trimethoxy silane, obtain B liquid in solution;
(3) the B liquid that step (2) is obtained is joined in the obtained A liquid of step (1) fast, regulates pH=10.2, stir 2 hours,
(4) mixed liquor is proceeded in 100mL polytetrafluoroethylene (PTFE) reactor, 170 DEG C of hydro-thermal reactions 0.5 hour under microwave radiation technology; Centrifugal, dry, 750 DEG C of roastings 4 hours, remove template, obtain white powder samples, are described high-performance and are situated between the controlled adsorbent of molecular sieve of micro-diplopore, be labeled as A4.
Embodiment 5
Prepare high-performance according to following steps to be situated between the controlled adsorbent of molecular sieve of micro-diplopore:
(1) add in 20mL distilled water by 7.35g tetraethyl ammonium hydroxide (TEAOH, 20% aqueous solution), stirred at ambient temperature adds aluminium isopropoxide 0.408g after mixing, and is stirred to aluminium isopropoxide complete hydrolysis; Take ethyl orthosilicate 10.4g, under 750r/min rotating speed stirs, dropwise instill above-mentioned solution, obtain A liquid;
(2) 3.48g neopelex is dissolved in 16mL distilled water, 40 DEG C of stirring in water bath, after 1 hour, in solution, add 0.55g3-aminopropyl triethoxysilane, obtain B liquid;
(3) the B liquid that step (2) is obtained is joined in the obtained A liquid of step (1) fast, regulates pH=9.7, stir 2 hours,
(4) mixed liquor is proceeded in 100mL polytetrafluoroethylene (PTFE) reactor, 140 DEG C of hydro-thermal reactions 2 hours under microwave radiation technology; Centrifugal, dry, 650 DEG C of roastings 6 hours, remove template, obtain white powder samples, are described high-performance and are situated between the controlled adsorbent of molecular sieve of micro-diplopore, be labeled as A5.
Embodiment 6: pore passage structure analysis is carried out to the controlled adsorbent of molecular sieve of the micro-diplopore of Jie of high absorption property;
Get above-described embodiment 3 and the molecular sieve 0.1g prepared by embodiment 5,180 DEG C degassed 8 hours; The ASAP2020 physical adsorption appearance using Merck & Co., Inc of the U.S. to produce is N to molecular sieve
2adsorption and desorption isotherms, as shown in Figure 1 and Figure 2; Adopt BET method, t-plot method and BJH equation calculated specific surface area, pore volume and pore-size distribution.Specific surface is respectively 478m
2/ g and 444m
2/ g, total pore volume is 0.43cm
3/ g and 0.51cm
3/ g.
Embodiment 7: Adsorption of Toluene analysis is carried out to the controlled adsorbent of molecular sieve of the micro-diplopore of Jie of high absorption property;
Get above-described embodiment 3 and the molecular sieve 50mg prepared by embodiment 5, intelligent gravimetric method adsorption instrument IGA002 is adopted to measure 35 DEG C of Toluene adsorption isotherms, as shown in Figure 3, Figure 4, result shows that molecular sieve has high adsorption capacity to toluene, reaches 305mg/g and 502mg/g.
Embodiment 8: hydrophobic performance analysis is carried out to the controlled adsorbent of molecular sieve of the micro-diplopore of Jie of high absorption property;
Get above-described embodiment 3 and the molecular sieve prepared by embodiment 5, adopt Dataphysics, OCA20 type contact angle measurement measures molecular sieve Static water contact angles, when result shows room temperature, contact angle is 129 ° and 106 °, illustrate that molecular sieve has high hydrophobicity, this is conducive to molecular sieve in wet environment to organic absorption.
Embodiment 9: the analysis of hydrothermally stable performance is carried out to the controlled adsorbent of molecular sieve of the micro-diplopore of Jie of high absorption property
Get above-described embodiment 3 and the molecular sieve prepared by embodiment 5, put into boiling water process drying after 100 hours, do the analysis of nitrogen adsorption desorption, step is identical with embodiment 6.Found that after before and after boiling water treating, molecular sieve Adsorption and desorption isotherms is almost identical, specific surface drops to 422m respectively
2/ g and 399m
2/ g, total pore volume reduces to 0.39cm
3/ g and 0.47cm3/g, the range of decrease is less.Illustrate that molecular sieve has good hydrothermal stability.
Above-described embodiment is the present invention's preferably embodiment; but embodiments of the present invention are not restricted to the described embodiments; change, the modification done under other any does not deviate from Spirit Essence of the present invention and principle, substitute, combine, simplify; all should be the substitute mode of equivalence, be included within protection scope of the present invention.
Claims (10)
1. a high-performance is situated between the preparation method of the controlled adsorbent of molecular sieve of micro-diplopore, it is characterized in that, comprise the following steps: be Material synthesis mother liquor with silicon source, aluminium source, microcellular structure directed agents, mesoporous template, organosilan and water, mother liquor utilizes microwave radiation technology hydro-thermal reaction, by centrifugal, dry, the roasting of product of reaction gained, obtain described high-performance and to be situated between the controlled adsorbent of molecular sieve of micro-diplopore.
2. high-performance according to claim 1 is situated between the preparation method of the controlled adsorbent of molecular sieve of micro-diplopore, and it is characterized in that, described silicon source is with SiO
2meter, aluminium source is with Al
2o
3meter, reaction raw materials mol ratio is SiO
2: water=0.025, SiO
2: microcellular structure directed agents=5, SiO
2: Al
2o
3=50 ~ 400, SiO
2: organosilan=10 ~ 40, SiO
2: mesoporous template=5 ~ 20.
3. high-performance according to claim 1 is situated between the preparation method of the controlled adsorbent of molecular sieve of micro-diplopore, and it is characterized in that, described mesoporous template is anion surfactant; Described silicon source is ethyl orthosilicate; Described aluminium source is aluminium isopropoxide; Described microcellular structure directed agents is at least one in TPAOH, tetraethyl ammonium hydroxide and ethylenediamine.
4. high-performance according to claim 3 is situated between the preparation method of the controlled adsorbent of molecular sieve of micro-diplopore, it is characterized in that, described anion surfactant is at least one in n-hexadecyl sodium sulfonate, myristyl sodium sulfonate, neopelex and sodium laurate.
5. high-performance according to claim 1 is situated between the preparation method of the controlled adsorbent of molecular sieve of micro-diplopore, it is characterized in that, described organosilan is at least one in 3-aminopropyl triethoxysilane, (3-mercaptopropyi) trimethoxy silane and chloropropyl triethoxysilane.
6. high-performance according to claim 1 is situated between the preparation method of the controlled adsorbent of molecular sieve of micro-diplopore, and it is characterized in that, described preparation method's concrete steps are as follows:
(1) take microcellular structure directed agents soluble in water, add aluminium source, be stirred to the hydrolysis of aluminium source; Then add silicon source under agitation, obtain A liquid;
(2) take mesoporous template to be added to the water, add organosilan after stirring a period of time, obtain B liquid;
(3) joined by the B liquid that step (2) is obtained in the obtained A liquid of step (1), adjust ph, continues to stir a period of time, obtains mother liquor;
(4) mother liquor that step (3) is obtained is proceeded to reactor, microwave hydrothermal reacts; By centrifugal, dry, the roasting of product of reaction gained, obtain described high-performance and to be situated between the controlled adsorbent of molecular sieve of micro-diplopore.
7. high-performance according to claim 6 is situated between the preparation method of the controlled adsorbent of molecular sieve of micro-diplopore, it is characterized in that, the time of stirring described in step (2) is 10 ~ 60 minutes; PH value described in step (3) is for being adjusted to 8.8 ~ 10.2; The time of stirring described in step (3) is 1 ~ 2 hour.
8. high-performance according to claim 6 is situated between the preparation method of the controlled adsorbent of molecular sieve of micro-diplopore, it is characterized in that, the reaction of microwave hydrothermal described in step (4) is 80 ~ 170 DEG C of reactions 0.5 ~ 4 hour; The temperature of described drying is 80 ~ 110 DEG C, and the dry time is 8 ~ 24h; The temperature of described roasting is 450 ~ 750 DEG C, and the time of roasting is 4 ~ 12 hours.
9. the high-performance that the preparation method being situated between the controlled adsorbent of molecular sieve of micro-diplopore by high-performance described in any one of claim 1 to 8 obtains is situated between the controlled adsorbent of molecular sieve of micro-diplopore.
10. high-performance according to claim 9 is situated between the application of the controlled adsorbent of molecular sieve of micro-diplopore in purifying organic.
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| CN111229184A (en) * | 2020-01-19 | 2020-06-05 | 生态环境部华南环境科学研究所 | Silicon source-controllable modified mesoporous and microporous adsorbent and preparation method and application thereof |
| CN113198433A (en) * | 2021-03-30 | 2021-08-03 | 天津大学 | Molecular sieve and porous organic polymer core-shell structure composite adsorbent and preparation method thereof |
| CN114768748A (en) * | 2022-04-22 | 2022-07-22 | 山东亮剑环保新材料有限公司 | Preparation method of all-silicon micro-mesoporous composite molecular sieve VOCs adsorbent |
| CN116328739A (en) * | 2023-02-22 | 2023-06-27 | 东洋和光净化材料(江苏)有限公司 | Hydrophobic VOC adsorbent and production method thereof |
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