CN114939396A - Inorganic silicon activated carbon for removing perfluorinated compounds, and preparation method and application thereof - Google Patents
Inorganic silicon activated carbon for removing perfluorinated compounds, and preparation method and application thereof Download PDFInfo
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Abstract
The present disclosure provides an inorganic silicon activated carbon for removing a perfluoro compound, and a preparation method and an application thereof, wherein the inorganic silicon activated carbon for removing a perfluoro compound comprises: the carbon layer is formed on the surface of the activated carbon, and the activated carbon and the poly-silicon dioxide layer are combined through a C-O-Si bond; wherein the mass ratio of silicon to carbon in the surface of the inorganic silicon activated carbon is 0.05-1.00.
Description
Technical Field
The disclosure belongs to the technical field of environment and chemistry, and particularly relates to inorganic silicon activated carbon for removing perfluorinated compounds, and a preparation method and application thereof.
Background
Perfluorinated compounds (PFASs) are a new class of pollutants with persistence, bioaccumulation and toxicity. Nowadays, PFASs are proved to be widely distributed in the earth water environment, the atmosphere and the soil, and surface water, underground water and sewage plants can detect the PFASs aiming at the water environment, and the PFASs as a refractory toxic organic pollutant have great threat to human health. The substance has strong polarity C-F bond and high bond energy, so the substance is difficult to be oxidized and biodegraded. The adsorption method attracts attention because of its advantages such as low cost, high operability, and high removal rate of PFASs. The activated carbon is the most commonly used adsorbent for adsorbing PFASs at present, but the activated carbon still has the problems of poor selectivity for adsorbing PFASs, particularly poor adsorption effect on short-chain PFAS and the like.
Disclosure of Invention
In view of the above technical problems, the present disclosure provides an inorganic silicon activated carbon for removing perfluorinated compounds, and a preparation method and an application thereof, so as to at least partially solve the above technical problems.
In order to solve the above technical problems, as one aspect of the present disclosure, there is provided an inorganic silicon activated carbon for removing a perfluoro compound, including:
an activated carbon and a polysilica layer formed on a surface of a carbon layer of the activated carbon, the activated carbon and the polysilica layer being bonded by a C-O-Si bond;
wherein the mass ratio of silicon to carbon in the surface of the inorganic silicon activated carbon is 0.05-1.00.
In one embodiment, the activated carbon comprises activated carbon powder or activated carbon particles;
sources of such activated carbon include: coal-based activated carbon or coconut shell activated carbon.
Also provided as another aspect of the present disclosure is a method for preparing an inorganic silicon activated carbon for removing a perfluoro compound, comprising:
adding inorganic polysilicic acid solution into active carbon to obtain active carbon impregnated with polysilicic acid;
carrying out hydrothermal reaction on the activated carbon impregnated with the polysilicic acid, and centrifuging, washing and drying to obtain a polymerized silicon activated carbon precursor;
and calcining the polymerized silicon activated carbon precursor to obtain the inorganic silicon activated carbon material.
In another embodiment, the inorganic polysilicic acid solution is prepared by the following steps:
adding the sodium silicate solution into dilute acid, adjusting the pH of the solution to be less than 2, and polymerizing and aging for 12-24h to obtain the inorganic polymeric silicic acid solution.
In another embodiment, the concentration of the inorganic polysilicic acid solution includes: 0.015-0.025 mol/L;
the mass ratio of silicon to carbon elements in the activated carbon added with the inorganic polysilicic acid solution comprises the following steps: 0.05-1.00.
In another embodiment, the mass ratio of silicon to carbon elements in the step of adding the inorganic polysilicic acid solution to the activated carbon further comprises: 0.1-0.8.
In another embodiment, the hydrothermal reaction conditions include:
the temperature of the hydrothermal reaction includes: 150 ℃ and 180 ℃;
the hydrothermal reaction time comprises: 24-48 h.
In another embodiment, the conditions of the calcination treatment include:
the temperatures of the calcination treatment include: 500 ℃ and 800 ℃;
the time of the calcination treatment includes: 1-3 h.
As another aspect of the disclosure, the application of the inorganic silicon activated carbon for removing the perfluorinated compounds is also provided, wherein the inorganic silicon activated carbon is used as a medicament for treating perfluorinated compound wastewater, and the addition amount of the inorganic silicon activated carbon is 5-15 mg/L.
In another embodiment, the above-mentioned perfluoro compound includes at least one of: perfluorooctanoic acid, perfluorooctane sulfonic acid, perfluorobutyl sulfonic acid.
Based on the technical scheme, the inorganic silicon activated carbon for removing the perfluorinated compounds, the preparation method and the application provided by the disclosure at least comprise the following beneficial effects:
(1) in the embodiment of the disclosure, the activated carbon is modified by using inorganic polysilicic acid, a polysilica layer is formed on the surface of the modified activated carbon, and the activated carbon and the polysilica are combined through Si-O-C bonds and are firmly combined. In the adsorption process of the inorganic silicon activated carbon and the perfluorinated compound, besides the hydrophobic effect of the activated carbon, the hydrophobic layer of the polysilica on the outer layer of the activated carbon can enhance the binding effect of the inorganic silicon modified activated carbon material and the perfluorinated compound through the hydrogen bonding effect with the carboxylic acid group or the sulfonic acid group in the perfluorinated compound.
(2) In the embodiment of the disclosure, inorganic silicon is used for replacing organic silicon to modify the activated carbon, and the activated carbon material with higher inorganic silicon load can be obtained under the condition of not using strong acid and strong base.
Drawings
FIG. 1 is a schematic illustration of the preparation of inorganic silicon activated carbon for removal of perfluorocompounds in an embodiment of the present disclosure;
FIG. 2 is an infrared spectrum of an inorganic silicon activated carbon prepared by a method in an embodiment of the disclosure and virgin carbon;
FIG. 3 is a graph of the effect of inorganic silicon activated carbon and virgin carbon on perfluorooctanoic acid wastewater removal in an example of the present disclosure;
FIG. 4 is a graph of the effect of inorganic silicon activated carbon and raw carbon on perfluorooctanesulfonic acid wastewater removal in examples of the present disclosure;
FIG. 5 is a graph of the effect of inorganic silicon activated carbon and virgin carbon on perfluorobutyl sulfonic acid wastewater removal in an example of the present disclosure;
FIGS. 6a and 6b are model calculations of raw carbon adsorption PFOA and PFOS and model calculations of example adsorption PFOA and PFOS, respectively.
Detailed Description
For the purpose of promoting a better understanding of the objects, aspects and advantages of the present disclosure, reference is made to the following detailed description taken in conjunction with the accompanying drawings.
Hydrophobic silica is effective in enhancing the ability to adsorb perfluorinated compounds (PFASs) by forming hydrogen bonds between the silica and the PFASs, and is effective in adsorbing PFASs even in the presence of competing organics. Therefore, the silica modified activated carbon hydrothermally generated by using inorganic polymeric silicic acid is expected to improve the performance of the activated carbon for adsorbing PFASs, especially for short-chain PFASs with weak hydrophobicity.
According to an embodiment of the present disclosure, an inorganic silicon activated carbon for removing a perfluoro compound includes:
the carbon layer is formed on the surface of the activated carbon, and the activated carbon and the poly-silicon dioxide layer are combined through a C-O-Si bond; wherein the mass ratio of silicon to carbon in the surface of the inorganic silicon activated carbon is 0.05 to 1.00, such as 0.10 to 1.00, 0.50 to 1.00, or 0.50 to 0.80.
According to an embodiment of the present disclosure, the activated carbon includes activated carbon powder or activated carbon particles; sources of activated carbon include: coal-made activated carbon or coconut shell activated carbon. The source and shape of the activated carbon can be selected as desired and is not more specifically limited herein.
FIG. 1 is a schematic illustration of the preparation of inorganic silicon activated carbon for removal of perfluorocompounds in an example of the present disclosure.
As shown in fig. 1, the preparation of inorganic silicon activated carbon for removing perfluoro compounds includes: adding inorganic polysilicic acid solution into active carbon to obtain active carbon impregnated with polysilicic acid; carrying out hydrothermal reaction on the activated carbon impregnated with the polysilicic acid, and centrifuging, washing and drying to obtain a polymerized silicon activated carbon precursor; and calcining the polymerized silicon activated carbon precursor to obtain the inorganic silicon activated carbon material.
According to the embodiment of the disclosure, the activated carbon is modified by using inorganic polysilicic acid, a polysilica dioxide layer is formed on the surface of the modified activated carbon material, and the activated carbon and the polysilica dioxide are combined firmly through Si-O-C bonds. In the adsorption process of the inorganic silicon activated carbon material and the perfluorinated compound, besides the hydrophobic effect of the activated carbon, the hydrophobic layer of the poly-silicon dioxide on the outer layer of the activated carbon can enhance the binding effect of the inorganic silicon activated carbon material and the perfluorinated compound through the hydrogen bonding effect with the carboxylic acid group or the sulfonic acid group in the perfluorinated compound.
According to an embodiment of the present disclosure, the inorganic polymeric silicic acid solution is obtained by the following steps: dropwise adding a sodium silicate solution with the concentration of 18-37 wt% into a dilute acid with the concentration of 0.5-1 mol/L, controlling the pH of the solution to be less than 2 in the whole reaction process, and adjusting the final pH of the solution to be about 1.5 to obtain a polymeric silicic acid solution, wherein the dilute acid comprises: any one of dilute hydrochloric acid, dilute nitric acid and dilute sulfuric acid.
According to an embodiment of the present disclosure, the inorganic polymeric silicic acid solution is formulated to have a concentration of 0.015 to 0.025mol/L, wherein 0.015, 0.020, 0.021, 0.022, 0.023, 0.024, 0.025, and the like may be selected.
In the embodiment of the disclosure, the concentration of the inorganic polysilicic acid solution is limited to 0.015-0.025mol/L, and when the polysilicic acid solution in the concentration range is mixed with the activated carbon, a certain mass ratio of silicon to carbon elements can be ensured, so that the modified activated carbon material loaded with high silicon dioxide is obtained.
According to the embodiment of the disclosure, the inorganic polysilicic acid solution is added into the activated carbon according to the predetermined silicon-carbon ratio, and the activated carbon impregnated with the polysilicic acid is obtained by stirring and impregnating for 2 to 12 hours at the speed of 100 to 300 r/min.
According to the embodiment of the disclosure, the mass ratio of silicon and carbon elements added into the activated carbon by the inorganic polymeric silicic acid solution comprises: 0.05 to 1.00, more preferably 0.1 to 0.8, wherein 0.05, 0.1, 0.2, 0.3, 0.4, 0.5, 0.6, 0.7, 0.8, 0.9, 1.0mol/L and the like can be selected.
In the examples of the present disclosure, there is a deterioration in the adsorption performance of the prepared activated carbon material if the concentration of the inorganic polymeric silicic acid is too high, and a deterioration in the effect of modifying the activated carbon if the content of the activated carbon is too high. The mass ratio of silicon to carbon is limited to 0.05-1, a layer of polysilicate silicon dioxide can be wrapped on the surface of the active carbon in the range, a modified active carbon material with higher loading of the polysilicate silicon dioxide is obtained, then the active carbon and the holes of the silicon dioxide can be effectively utilized to adsorb pollutants, the bonding force between the silicon dioxide on the outer surface of the active carbon and the pollutants is effectively enhanced by the hydrogen bonds formed by the perfluorinated compounds, and the adsorption capacity to the pollutants is improved.
According to the embodiment of the disclosure, the activated carbon impregnated with the polymeric silicic acid is added into a hydrothermal reaction kettle and reacts for 24-48h under the condition that the temperature of the hydrothermal reaction is 150-180 ℃. And then, centrifuging the powder after the hydrothermal reaction at the speed of 3000-8000 r/min, washing with ultrapure water until the pH value is recovered to be neutral, and drying in an oven at the temperature of 50-90 ℃ for 8-24 h.
In an embodiment of the present disclosure, a silica shell is formed on an outer surface of the activated carbon using a hydrothermal reaction.
According to the embodiment of the disclosure, the polymeric silicon activated carbon precursor is put into a tube furnace and subjected to calcination treatment in a nitrogen atmosphere to obtain the inorganic silicon activated carbon material.
According to an embodiment of the present disclosure, the ramp rate of the calcination includes: 5-15 deg.C/min, wherein 5, 10, 15 deg.C/min can be selected; the calcination temperature includes: 500 ℃ and 800 ℃, wherein 500 ℃, 600 ℃, 700 ℃, 800 ℃ and the like can be selected; the calcination treatment time comprises the following steps: 1. 2, 3h and the like.
The technical solution of the present disclosure is further illustrated by the following specific embodiments and the accompanying drawings. It should be noted that the following specific examples are given by way of illustration only, and the scope of the disclosure is not limited thereto. The chemicals and raw materials used in the following examples were either commercially available or self-prepared by a known preparation method.
Examples
10.0g of Na was weighed 2 SiO 3 ·9H 2 Dissolving O liquid in about 100mL of water, dropwise adding the O liquid into dilute hydrochloric acid with the concentration of 0.5-1 mol/L, adjusting the pH to be always less than 2 by using the dilute hydrochloric acid, controlling the final pH to be 1.5, and fixing the volume to 500mL to obtain 0.024mol/L (prepared by using SiO 2 Meter) of polymeric silicic acid solution. And then weighing 3g of wood powder activated carbon, adding a certain amount of polysilicic acid solution according to the silicon-carbon mass ratio of 0.1, and mixing and stirring at the speed of 100-300 r/min for 12 hours to obtain the polysilicic acid impregnated activated carbon. And then, putting the activated carbon impregnated with the polysilicic acid into a hydrothermal reaction kettle for hydrothermal reaction, reacting for 48 hours at 180 ℃, centrifuging the sample for many times at the speed of 5000r/min, washing with ultrapure water until the pH value is recovered to be neutral, and drying for 12 hours in an oven at 90 ℃ to obtain the polymeric silicon activated carbon precursor. Finally, the process is carried out in a batch,and (3) putting the dried polymerized silicon activated carbon precursor powder into a tubular furnace, heating to 600 ℃ at a speed of 10 ℃/min in a nitrogen atmosphere, keeping for 2h, and cooling to room temperature to obtain the inorganic silicon activated carbon material PAC-Si, wherein the inorganic silicon activated carbon material has a certain hydrophobic property.
Table 1 is a comparison of surface element mass ratios between inorganic silicon activated carbon prepared in example 1 of the present disclosure and virgin activated carbon (virgin carbon).
TABLE 1
| Examples | Virgin carbon | |
| C | 26.2 | 91.1 |
| O | 46.6 | 6.70 |
| N | 0.6 | 2.10 |
| Si | 26.5 | 0.20 |
As can be seen from table 1, the method in the example can obtain a highly inorganic silicon-supported activated carbon material, and the elemental ratio between silicon and carbon is high.
Fig. 2 is an infrared spectrum of inorganic silicon activated carbon prepared by the method in the examples of the present disclosure and virgin carbon.
As shown in fig. 2, Si — O — C bonds were formed in the inorganic silicon activated carbon prepared by the method in the example of the present disclosure, and also the successful loading of Si to the surface of the activated carbon was confirmed.
The inorganic silicon activated carbon prepared by the method in the example is used for simulating the removal of perfluorinated compound wastewater, and the specific experimental conditions and results are as follows:
perfluorinated compounds with varying chain lengths include: perfluorooctanoic acid (PFOA), perfluorooctane sulfonic acid (PFOS) and perfluorobutyl sulfonic acid (PFBS), PFOA, PFOS and PFBS were mixed with ultrapure water respectively to prepare wastewater solutions having a concentration of 200. mu.g/LPFOA, PFOS and PFBS, and the concentrations thereof were measured by a liquid chromatography-mass spectrometer, and the removal effect of the perfluorocompound was represented by removal rate (%).
The inorganic silicon activated carbon PAC-Si obtained in the example is applied to the removal of long-chain perfluorinated compound (PFBOA) wastewater, meanwhile, the original untreated activated carbon (original carbon, PAC) is used as a control to study the treatment effect of the inorganic silicon activated carbon PAC-Si on perfluorooctanoic acid (PFOA) wastewater, and the experimental result is shown in the following figure 3, wherein the adding amount of the inorganic silicon activated carbon and the original carbon is 10 mg/L.
Figure 3 is a graph of the effect of inorganic silicon activated carbon and virgin carbon on perfluorooctanoic acid (PFOA) wastewater removal in examples of the present disclosure.
As can be seen from FIG. 3, for the long-chain PFOA, the removal efficiency of the original carbon in about 30min can reach about 40%, the further time is increased to 180min, and the removal rate reaches about 65% and reaches the balance; the removal rate of PAC-Si is close to 50% in about 30min, and the highest removal rate can reach about 70% in the adsorption time of 180 min.
The inorganic silicon activated carbon PAC-Si obtained in the example is applied to removal of perfluorooctane sulfonate (PFOS) wastewater, and meanwhile, the original untreated activated carbon (original carbon, PAC) is used as a control to study the treatment effect of the inorganic silicon activated carbon PAC-Si on the perfluorooctane sulfonate (PFOS) wastewater, and the experimental result is shown in the following figure 4, wherein the adding amount of the inorganic silicon activated carbon and the original carbon is 10 mg/L.
Fig. 4 is a graph of the effect of inorganic silicon activated carbon and virgin carbon on perfluorooctanesulfonic acid wastewater removal in examples of the present disclosure.
As can be seen from FIG. 4, for sulfonic PFOS, the original carbon has better adsorption capacity, and about 60% of the original carbon can be removed in about 30 min; further increases to 180min with time, and the removal rate is balanced at about 90%. But the control effect of PAC-Si on the carbon is still better than that of the original carbon, the removal rate of the PAC-Si is close to 80% in about 30min, and the highest removal rate can reach about 95% in the adsorption time of 180 min.
The inorganic silicon activated carbon PAC-Si obtained in the examples was applied to removal of perfluorobutyl sulfonic acid (PFBS) wastewater, and the treatment effect of inorganic silicon activated carbon PAC-Si on perfluorobutyl sulfonic acid (PFBS) wastewater was studied by using the original untreated activated carbon (original carbon, PAC) as a control, and the experimental results are shown in fig. 5 below, in which the amounts of inorganic silicon activated carbon and original carbon added were both 10 mg/L.
FIG. 5 is a graph of the effect of inorganic silicon activated carbon and virgin carbon on perfluorobutyl sulfonic acid wastewater removal in examples of the present disclosure.
As can be seen from fig. 5, for the short chain sulfonate PFBS, the adsorption effect of the examples on PFBS is better than that of the original carbon for the removal effect of the comparative examples and the original carbon. Compared with PFBS, the adsorption removal rate of the original carbon is only less than 20% at about 30min, and PAC-Si reaches about 25%. When the adsorption time is further increased to 180min, the adsorption amount of the original carbon is still slightly lower than about 5 percent of PAC-Si.
The mechanism of removal efficiency is analyzed to discover that a layer of hydrophobic silica structure is formed on the surface of the inorganic silicon modified activated carbon, and an infrared spectrum can discover that the structure is combined through a C-O-Si bond, and through DFT and independent gradient model simulation calculation, the hydrophobic layer of the silica can enhance the combination effect of the modified activated carbon and the perfluorinated compound through the hydrogen bond effect with carboxylic acid groups or sulfonic acid groups except the hydrophobic acting force on the surface of the carbon layer in the adsorption process with the perfluorinated compound (fig. 6 a-b).
The above-mentioned embodiments are intended to illustrate the objects, aspects and advantages of the present disclosure in further detail, and it should be understood that the above-mentioned embodiments are only illustrative of the present disclosure and are not intended to limit the present disclosure, and any modifications, equivalents, improvements and the like made within the spirit and principle of the present disclosure should be included in the scope of the present disclosure.
Claims (10)
1. An inorganic silicon activated carbon for removal of perfluorinated compounds comprising:
the carbon layer is formed on the surface of the activated carbon, and the activated carbon and the silica layer are combined through a C-O-Si bond;
wherein the mass ratio of silicon to carbon in the surface of the inorganic silicon activated carbon is 0.05-1.00.
2. The inorganic silicon activated carbon of claim 1, wherein the activated carbon comprises activated carbon powder or activated carbon particles;
sources of the activated carbon include: coal-made activated carbon or coconut shell activated carbon.
3. A method for preparing the inorganic silicon activated carbon for removing a perfluoro compound according to claim 1 or 2, comprising:
adding inorganic polysilicic acid solution into active carbon to obtain active carbon impregnated with polysilicic acid;
carrying out hydrothermal reaction on the activated carbon impregnated with the polysilicic acid, and centrifuging, washing and drying to obtain a polymerized silicon activated carbon precursor;
and calcining the polymerized silicon activated carbon precursor to obtain the inorganic silicon activated carbon material.
4. The method of claim 3, wherein the solution of inorganic polymeric silicic acid is obtained by:
adding the sodium silicate solution into dilute acid, adjusting the pH of the solution to be less than 2, and polymerizing and aging for 12-24h to obtain the inorganic polymeric silicic acid solution.
5. The method of claim 4, wherein the concentration of the inorganic polymeric silicic acid solution comprises: 0.015-0.025 mol/L;
the mass ratio of silicon to carbon elements in the activated carbon added with the inorganic polysilicic acid solution comprises the following steps: 0.05-1.00.
6. The method of claim 5, wherein the adding of the inorganic polysilicic acid solution to the activated carbon further comprises: 0.1-0.8.
7. The method of claim 3, wherein the hydrothermal reaction conditions comprise:
the temperature of the hydrothermal reaction includes: 150 ℃ and 180 ℃;
the time of the hydrothermal reaction comprises: 24-48 h.
8. The method of claim 3, wherein the conditions of the calcination treatment comprise:
the temperatures of the calcination treatment include: 500 ℃ and 800 ℃;
the time of the calcination treatment includes: 1-3 h.
9. The use of the inorganic silicon activated carbon for removing perfluoro compounds as claimed in claim 1 or 2, wherein the inorganic silicon activated carbon is used as an agent for treating perfluoro compound wastewater, and the addition amount of the inorganic silicon activated carbon is 5-15 mg/L.
10. Use according to claim 9, wherein the perfluorinated compounds comprise at least one of: perfluorooctanoic acid, perfluorooctane sulfonic acid, perfluorobutyl sulfonic acid.
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