CN114749149B - Carbon nanomaterial for purifying formaldehyde and preparation method thereof - Google Patents

Carbon nanomaterial for purifying formaldehyde and preparation method thereof Download PDF

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CN114749149B
CN114749149B CN202210414342.2A CN202210414342A CN114749149B CN 114749149 B CN114749149 B CN 114749149B CN 202210414342 A CN202210414342 A CN 202210414342A CN 114749149 B CN114749149 B CN 114749149B
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plant extract
gqds
plant
carbon material
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CN114749149A (en
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刘协
朱明山
林晓瑜
董浩杰
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Guangzhou Quangao Environmental Protection Technology Co ltd
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    • B01J20/00—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof
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    • B01J27/00—Catalysts comprising the elements or compounds of halogens, sulfur, selenium, tellurium, phosphorus or nitrogen; Catalysts comprising carbon compounds
    • B01J27/24—Nitrogen compounds
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Abstract

The invention belongs to the technical field of air purification, and particularly relates to a formaldehyde-purified carbon material and a preparation method thereof. The invention takes plant leaves as raw materials, and firstly adopts a physical method to obtain plant extract. Then, the plant extract, nitrogen source and dimethyl sulfoxide are used as raw materials, and the sulfur-nitrogen co-doped graphene quantum dot (S, N-GQDs) nanomaterial is synthesized in one step through a solvothermal method. The powder of S, N-GQDs is applied to formaldehyde adsorption experiments, and has high adsorption performance and high adsorption capacity on formaldehyde. The method has the advantages of low raw material cost, simple synthesis method and wide application prospect. The preparation method has the advantages of simple preparation process, mild reaction conditions and low cost, and is suitable for mass production.

Description

Carbon nanomaterial for purifying formaldehyde and preparation method thereof
Technical Field
The invention belongs to the technical field of air purification, and particularly relates to a formaldehyde-purified carbon material and a preparation method thereof.
Background
People live and work indoors most of the time, and indoor air quality is closely related to human health. The exceeding of the gaseous formaldehyde content caused by indoor decoration has become a social problem. The science proves that the formaldehyde and other polluted gases have great influence on human bodies, and the respiratory tract is easy to cause. Diseases, cancers, leukemias and neurological disorders are particularly detrimental to pregnant women, children and the elderly. Therefore, the problem of exceeding the standard of the indoor gaseous formaldehyde is solved.
Physical adsorption techniques are often used for the purification of low concentrations of harmful substances in air. The adsorbent generally requires a large specific surface area, has a large adsorption capacity, and has good adsorptivity to the target gas. The carbon nanomaterial is known to have the characteristics of large specific surface area, abundant surface functional groups, strong adsorption capacity and the like, and is an excellent physical adsorption material. Graphene Quantum Dots (GQDs) are a novel fluorescent carbon nanomaterial consisting of multiple layers of graphene with smaller lateral dimensions. GQDs are smaller than 10nm in size, have excellent large specific surface area and stability, and furthermore, heteroatom doping is one of the effective means to improve the intrinsic properties of nanomaterials due to similar atomic size and five valence electron bonds capable of binding to carbon atoms. The functional groups rich in the GQD surface can be further modified according to the requirement, so that the adsorption performance of the GQD on target gas molecules is effectively improved. Therefore, developing and applying S, N-GQDs carbon nanomaterials to formaldehyde purification is one of the hot spots of research.
Disclosure of Invention
The invention aims to provide a synthesis method of formaldehyde-removing nano carbon material with low cost and simple preparation process, which takes an organic matter containing nitrogen element as a carbon source and a nitrogen source, dimethyl sulfoxide as a reducing agent and a sulfur source, takes plant extract as a stabilizer and a supplementary carbon source, and adopts simple hydrothermal synthesis to obtain the S, N-GQDs carbon quantum dot with good water solubility, good stability and uniform dispersion.
The technical scheme adopted by the invention for solving the technical problems is as follows: the preparation method of the carbon material for formaldehyde purification specifically comprises the following steps:
(1) Mechanically treating plant leaves to obtain plant leaf extract, filtering the extract to obtain clear and transparent plant extract, and refrigerating for later use;
(2) Weighing plant extract and nitrogen source, dissolving in dimethyl sulfoxide, and stirring to obtain clear solution;
(3) Heating the clarified solution obtained in the step (2) to 160-200 ℃ and keeping the temperature for 8-15 hours, and naturally cooling to room temperature to obtain the sulfur-nitrogen co-doped graphene quantum dot carbon nanomaterial S, N-GQDs, namely the carbon material for formaldehyde purification.
The plant leaf in the step (1) is one or more of chlorophytum comosum leaf, aloe leaf and fleshy leaf.
In the step (1), the plant leaves are firstly ground into juice by adopting a grinding method, then soaked by using excessive ethanol/water solution, filtered by suction, and the ethanol in the clarified filtrate is removed by adopting a rotary evaporation mode and then dried. Preferably, the concentration of the ethanol/water solution is 60% ethanol; the rotary evaporation temperature is 60-80 ℃, the drying temperature is 40-60 ℃ and the time is 4-8 h.
The nitrogen source in the step (2) is at least one of triethanolamine, melamine, thiourea and urea.
The mass ratio of the plant extract to the ammonia source in the step (2) is 1:0.2 to 1, preferably 1:0.2 to 0.6;
The mass volume ratio of the plant extract to the dimethyl sulfoxide in the step (2) is 1g: 10-20 mL; preferably 1g: 12-18 mL.
Preferably, the temperature after the temperature rise in the step (3) is 170-190 ℃ and the holding time is 10-13 h.
Preferably, acetone is added after the reaction in the step (3) is completed, and then the sulfur-nitrogen co-doped graphene quantum dot carbon nanomaterial is obtained through centrifugal drying.
Preferably, the solvent reagents are all analytically pure.
The carbon material for purifying formaldehyde is prepared by the method.
The carbon material for formaldehyde purification is applied to adsorption and photocatalytic degradation of formaldehyde.
Compared with the prior art, the invention has the following advantages:
The invention uses plant extract as carbon source and stabilizer, and obtains S, N-GQDs nanometer material by solvothermal method. The preparation method has the advantages of abundant sources, low cost, simple and controllable operation and short time consumption; the prepared nano material has good water solubility and is beneficial to the coating of products; and has strong stability and large specific surface area.
Drawings
FIG. 1 is a schematic diagram showing the structure of S, N-GQDs obtained in example 1 of the present invention.
FIG. 2 shows a TEM image (b) of S, N-GQDs and a particle size distribution (c) thereof, obtained in example 1 of the present invention.
FIG. 3 is a FT-IR chart of S, N-GQDs nanomaterial made in example 1 of the present invention.
Detailed Description
The present invention is described in further detail below with reference to examples, but the technical solution of the present invention is not limited to the following specific embodiments, and any combination of the specific embodiments is also included.
Example 1
(1) Taking 50g of cleaned aloe leaves, drying, firstly cutting the aloe leaves into pieces with the size of 2cm 2 by using scissors, then placing the pieces into a mortar, grinding for 30min, transferring the pieces into 50mL of 60% ethanol/water solution, soaking for 30min, filtering, removing precipitates, removing ethanol by rotary evaporation at the temperature of 80 ℃, and then placing the pieces into a vacuum drying box for vacuum drying at the temperature of 40 ℃ to obtain transparent plant extract. And (3) putting the obtained plant extract into a refrigerator, and refrigerating at 0 ℃ for standby.
(2) 1.0G of the plant extract obtained in the step (1) and 3.0mmol (0.448 g) of triethanolamine are dissolved in 15mL of dimethyl sulfoxide, stirred for 30min to clarify the solution, then the solution is transferred into a 20mL high-pressure reaction kettle for reaction for 12 hours at 180 ℃, acetone is added to generate precipitate after the solution is cooled to room temperature, the precipitate is centrifugally separated, washed 3-5 times by absolute ethyl alcohol, and vacuum drying is carried out at 40 ℃ to obtain sulfur-nitrogen co-doped graphene quantum dots, abbreviated as S, N-GQDs.
Example 2
(1) Taking 100g of cleaned fleshy leaves, drying, firstly cutting the fleshy leaves into pieces with the size of 2cm 2 by using scissors, then placing the pieces into a mortar, grinding for 30min, transferring the pieces into 50mL of 60% ethanol/water solution, soaking for 30min, filtering, removing precipitates, removing ethanol by rotary evaporation at the temperature of 80 ℃, and then placing the pieces into a vacuum drying box for vacuum drying at the temperature of 40 ℃ to obtain transparent plant extract. And (3) putting the obtained plant extract into a refrigerator, and refrigerating at 0 ℃ for standby.
(2) 1.0G of the plant extract obtained in the step (1) and 2.0mmol of melamine are dissolved in 15mL of dimethyl sulfoxide, stirred for 30min to clarify the solution, then the solution is transferred into a 20mL high-pressure reaction kettle, reacted for 16 hours at 180 ℃, cooled to room temperature, added with acetone to generate precipitate, centrifugally separated and washed 3-5 times by absolute ethyl alcohol, and vacuum dried at 40 ℃ to obtain sulfur-nitrogen co-doped graphene quantum dots abbreviated as S, N-GQDs.
Example 3
(1) Taking 100g of cleaned fleshy leaves, drying, firstly cutting the fleshy leaves into pieces with the size of 2cm 2 by using scissors, then placing the pieces into a mortar, grinding for 30min, transferring the pieces into 50mL of 60% ethanol/water solution, soaking for 30min, filtering, removing precipitates, removing ethanol by rotary evaporation at the temperature of 80 ℃, and then placing the pieces into a vacuum drying box for vacuum drying at the temperature of 40 ℃ to obtain transparent plant extract. And (3) putting the obtained plant extract into a refrigerator, and refrigerating at 0 ℃ for standby.
(2) 1.0G of the plant extract obtained in the step (1) and 0.2g of thiourea are dissolved in 15mL of dimethyl sulfoxide, ultrasonic stirring is carried out for 30min to clarify the solution, then the solution is transferred into a 20mL high-pressure reaction kettle, the reaction is carried out for 16 hours at 180 ℃, acetone is added to generate precipitate after cooling to room temperature, the precipitate is centrifugally separated and washed for 3-5 times by absolute ethyl alcohol, and vacuum drying is carried out at 40 ℃ to obtain sulfur-nitrogen co-doped graphene quantum dots, which are abbreviated as S, N-GQDs.
FIG. 1 is a schematic structural diagram of S, N-GQDs, wherein part of S, N elements replace the position of C in graphene quantum dots. FIG. 2a is a photograph of a sol of S, N-GQDs, showing the resulting sol as a brown clear solution; FIG. 2b is a TEM of S, N-GQDs, showing that the prepared quantum dots are uniformly dispersed, and the particle size of the quantum dots is between 2 and 10nm (FIG. 2 c). Fig. 3 is an SEM image of the carbon material synthesized without the participation of the plant extract (comparative example 3), and it can be seen that the obtained carbon material is an aggregated bulk material, demonstrating the stabilizer effect of the plant extract. The functional groups on the surface of the prepared S, N-GQDs nano material are tested by Fourier infrared (FTIR), and FIG. 4 shows characteristic peaks of the functional groups on the surface of the S, N-GQDs nano material.
Formaldehyde adsorption test with the carbon nanomaterial made in example 1:
Formaldehyde gas (1 mg/m 3) with a certain concentration is selected as pollution source gas to carry out static formaldehyde adsorption experiments. The adsorption device is a self-made airtight gas experiment box (the total volume is 0.008m 3), a certain mass (0.2 g) of the S, N-GQDs nano material prepared in the example 1 (2) is put into the box, the experimental environment temperature is 25+/-1 ℃, the relative humidity is (30+/-5)%, and the illumination condition is in a dark state. The formaldehyde concentration is monitored in real time by a formaldehyde concentration tester, and the sampling frequency is 1 time/10 min. The experimental time was 2 hours. After the adsorption experiment is finished, the formaldehyde content in the experiment box is measured to be reduced by 35.08%, which shows that the S, N-GQDs nano material has better adsorption capacity on formaldehyde gas.
Test of photocatalytic degradation of formaldehyde with the carbon nanomaterial prepared in example 1:
0.2g of the S, N-GQDs powder sample prepared in the example 1 (2) is taken and uniformly placed in a culture dish, the culture dish is placed at the bottom of a self-made airtight gas experiment box, and quartz glass is used as a material above the experiment box and covered with black paper to avoid light. The formaldehyde concentration in the experimental box is monitored in real time by a formaldehyde concentration tester. Before the reaction starts, 2mg/m 3 of formaldehyde gas is injected into a gas experiment box, and when the concentration of formaldehyde in the gas experiment box is not changed any more, the adsorption-desorption process of the S, N-GQDs on formaldehyde is balanced. And taking off the black paper covered on the surface of the quartz glass, and adopting a 300W xenon lamp to carry out illumination and starting the photocatalytic reaction. The sampling frequency of the formaldehyde concentration tester to formaldehyde gas is 1 time/10 min, and the experimental time is 2 hours. After the adsorption experiment is finished, the formaldehyde content in the experiment box is measured to be reduced by 52.81%, which shows that the S, N-GQDs nano material has better photocatalytic removal capability on formaldehyde gas.
Example 4
The difference from example 1 as a comparison is that the amount of the plant extract added is changed in step (2), specifically as follows:
Dissolving 0.5g of the plant extract obtained in the step (1) and 3.0mmol (0.448 g) of triethanolamine in 15mL of dimethyl sulfoxide, stirring for 30min to clarify the solution, transferring the solution into a 20mL high-pressure reaction kettle, reacting for 12 hours at 180 ℃, cooling to room temperature, adding acetone to generate precipitate, centrifugally separating the precipitate, washing the precipitate for 3-5 times by absolute ethyl alcohol, and vacuum drying at 40 ℃ to obtain the sulfur-nitrogen co-doped graphene quantum dot.
And (3) testing the adsorption of formaldehyde by using the prepared carbon nanomaterial:
formaldehyde gas (1 mg/m 3) with a certain concentration is selected as pollution source gas to carry out static formaldehyde adsorption experiments. The adsorption device is a self-made airtight gas experiment box (the total volume is 0.008m 3), S, N-GQDs nano material prepared by a certain mass (0.2 g) is put into the box, the experimental environment temperature is 25+/-1 ℃, the relative humidity is (30+/-5)%, and the illumination condition is in a dark state. The formaldehyde concentration is monitored in real time by a formaldehyde concentration tester, and the sampling frequency is 1 time/10 min. The experimental time was 2 hours. After the adsorption experiment is finished, the formaldehyde content in the experiment box is measured to be reduced by 30.34%.
And taking 0.2g of prepared S, N-GQDs powder sample, uniformly placing the sample in a culture dish, placing the culture dish at the bottom of a self-made airtight gas experiment box, wherein quartz glass is used as a material above the experiment box, and covering the experiment box with black paper to avoid light. The formaldehyde concentration in the experimental box is monitored in real time by a formaldehyde concentration tester. Before the reaction starts, 2mg/m 3 of formaldehyde gas is injected into a gas experiment box, and when the concentration of formaldehyde in the gas experiment box is not changed any more, the adsorption-desorption process of the S, N-GQDs on formaldehyde is balanced. And taking off the black paper covered on the surface of the quartz glass, and adopting a 300W xenon lamp to carry out illumination and starting the photocatalytic reaction. The sampling frequency of the formaldehyde concentration tester to formaldehyde gas is 1 time/10 min, and the experimental time is 2 hours. After the adsorption experiment is finished, the formaldehyde content in the experiment box is measured to be reduced by 41.62 percent.
Comparative example 1
The difference from example 1 as a comparison is that no plant extract was added in step (2), the specific procedure is as follows: 0.448g of triethanolamine is dissolved in 15mL of dimethyl sulfoxide, stirred for 30min to clarify the solution, then the solution is transferred into a 20mL high-pressure reaction kettle for reaction for 12 hours at 180 ℃, acetone is added to generate precipitate after cooling to room temperature, the precipitate is centrifugally separated, the precipitate is washed 3-5 times by absolute ethyl alcohol, and vacuum drying is carried out at 40 ℃ to obtain a product.
And (3) testing the adsorption of formaldehyde by using the prepared carbon nanomaterial:
Formaldehyde gas (1 mg/m 3) with a certain concentration is selected as pollution source gas to carry out static formaldehyde adsorption experiments. The adsorption device is a self-made airtight gas experiment box (the total volume is 0.008m 3), the nano material prepared by a certain mass (0.2 g) is put into the box, the experiment environment temperature is 25+/-1 ℃, the relative humidity is (30+/-5)%, and the illumination condition is in a dark state. The formaldehyde concentration is monitored in real time by a formaldehyde concentration tester, and the sampling frequency is 1 time/10 min. The experimental time was 2 hours. After the adsorption experiment is finished, the formaldehyde content in the experiment box is reduced by 22.18 percent.
And (3) testing the photocatalytic degradation of formaldehyde by using the prepared carbon nanomaterial:
Taking 0.2g of the prepared powder sample, uniformly placing the powder sample into a culture dish, placing the culture dish into the bottom of a self-made airtight gas experiment box, wherein the upper part of the experiment box is made of quartz glass, and covering the experiment box with black paper to avoid light. The formaldehyde concentration in the experimental box is monitored in real time by a formaldehyde concentration tester. Before the reaction starts, 2mg/m 3 of formaldehyde gas is injected into a gas experiment box, and when the concentration of formaldehyde in the gas experiment box is not changed any more, the adsorption-desorption process of the formaldehyde of the sample obtained in the comparative example reaches equilibrium. And taking off the black paper covered on the surface of the quartz glass, and adopting a 300W xenon lamp to carry out illumination and starting the photocatalytic reaction. The sampling frequency of the formaldehyde concentration tester to formaldehyde gas is 1 time/10 min, and the experimental time is 2 hours. After the adsorption experiment is finished, the formaldehyde content in the experiment box is reduced by 33.04 percent.
Comparative example 2
The preparation method of the unmodified carbon quantum dot comprises the following specific steps: 1.05g of citric acid monohydrate solid and 335mL of ethylenediamine are dissolved in 15mL of deionized water, after mechanical stirring for 10 minutes, the solution is transferred into a 25mL high-pressure reaction kettle, reacted for 5 hours at 180 ℃, the obtained brown solution is dialyzed by a semipermeable membrane and then dried, and the carbon quantum dots, abbreviated as GQDs, are obtained.
And (3) testing the photocatalytic degradation of formaldehyde by using the prepared carbon nanomaterial:
And uniformly placing 0.2g of the prepared GQDs powder sample into a culture dish, placing the culture dish at the bottom of a self-made airtight gas experiment box, wherein quartz glass is used as a material above the experiment box, and black paper is used for covering the experiment box to avoid light. The formaldehyde concentration in the experimental box is monitored in real time by a formaldehyde concentration tester. Before the reaction starts, 2mg/m 3 of formaldehyde gas is injected into a gas experiment box, and when the concentration of formaldehyde in the gas experiment box is not changed any more, the adsorption-desorption process of GQDs on formaldehyde is balanced. And taking off the black paper covered on the surface of the quartz glass, and adopting a 300W xenon lamp to carry out illumination and starting the photocatalytic reaction. The sampling frequency of the formaldehyde concentration tester to formaldehyde gas is 1 time/10 min, and the experimental time is 2 hours. After the adsorption experiment is finished, the formaldehyde content in the experiment box is reduced by 18.04 percent.
And (3) testing the adsorption of formaldehyde by using the prepared carbon nanomaterial:
Formaldehyde gas (1 mg/m 3) with a certain concentration is selected as pollution source gas to carry out static formaldehyde adsorption experiments. The adsorption device is a self-made airtight gas experiment box (the total volume is 0.008m 3), the GQDs nano material prepared by a certain mass (0.2 g) is put into the box, the experimental environment temperature is 25+/-1 ℃, the relative humidity is (30+/-5)%, and the illumination condition is in a dark state. The formaldehyde concentration is monitored in real time by a formaldehyde concentration tester, and the sampling frequency is 1 time/10 min. The experimental time was 2 hours. After the adsorption experiment is finished, the formaldehyde content in the experiment box is measured to be reduced by 30.51 percent.

Claims (6)

1. The preparation method of the carbon material for purifying formaldehyde is characterized by comprising the following steps of:
(1) Mechanically treating plant leaves to obtain plant leaf extract, filtering the extract for multiple times to obtain clear and transparent plant extract, and refrigerating for later use; the mechanical treatment is that firstly, plant leaves are ground into juice by adopting a grinding method, then the juice is soaked by using excessive ethanol/water solution, suction filtration is carried out, and the ethanol in the clarified filtrate is removed by adopting a rotary evaporation mode, and then the juice is dried; the plant leaf is aloe leaf;
(2) Weighing plant extract and nitrogen source, dissolving in dimethyl sulfoxide, and stirring to obtain clear solution; the nitrogen source is at least one of triethanolamine, melamine, thiourea and urea; the mass ratio of the plant extract to the nitrogen source is 1: 0.2 to 1;
(3) And (3) heating the clarified solution obtained in the step (2) to 160-200 ℃ and keeping the temperature for 8-15 hours, and cooling to room temperature to obtain the sulfur-nitrogen co-doped graphene quantum dot carbon nanomaterial S, N-GQDs, namely the carbon material for formaldehyde purification.
2. The method of manufacturing according to claim 1, characterized in that: the mass volume ratio of the plant extract to the dimethyl sulfoxide in the step (2) is 1g: 10-20 mL.
3. The method of manufacturing according to claim 1, characterized in that: the mass ratio of the plant extract to the nitrogen source in the step (2) is 1: 0.2 to 0.6.
4. The method of manufacturing according to claim 1, characterized in that: the temperature after the temperature rise in the step (3) is 170-190 ℃ and the holding time is 10-13 h.
5. A carbon material for formaldehyde purification prepared by the method of any one of claims 1 to 4.
6. The use of the carbon material for formaldehyde purification according to claim 5 for adsorption and photocatalytic degradation of formaldehyde.
CN202210414342.2A 2022-04-20 2022-04-20 Carbon nanomaterial for purifying formaldehyde and preparation method thereof Active CN114749149B (en)

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