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CN115445565B - Copper-doped graphene aerogel for adsorbing VOCs and preparation method thereof - Google Patents

Copper-doped graphene aerogel for adsorbing VOCs and preparation method thereof Download PDF

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CN115445565B
CN115445565B CN202210975066.7A CN202210975066A CN115445565B CN 115445565 B CN115445565 B CN 115445565B CN 202210975066 A CN202210975066 A CN 202210975066A CN 115445565 B CN115445565 B CN 115445565B
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copper
graphene aerogel
roasting
doped graphene
atmosphere
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CN115445565A (en
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王敬楠
李程
于珊珊
蒋兴家
申明周
崔新安
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China Petroleum and Chemical Corp
Sinopec Engineering Group Co Ltd
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    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01JCHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J20/00Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof
    • B01J20/02Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising inorganic material
    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01DSEPARATION
    • B01D53/00Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
    • B01D53/02Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols by adsorption, e.g. preparative gas chromatography
    • B01D53/04Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols by adsorption, e.g. preparative gas chromatography with stationary adsorbents
    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01JCHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J20/00Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof
    • B01J20/02Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising inorganic material
    • B01J20/0203Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising inorganic material comprising compounds of metals not provided for in B01J20/04
    • B01J20/0233Compounds of Cu, Ag, Au
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    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01JCHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J20/00Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof
    • B01J20/30Processes for preparing, regenerating, or reactivating
    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01DSEPARATION
    • B01D2257/00Components to be removed
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    • B01D2257/708Volatile organic compounds V.O.C.'s
    • YGENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02ATECHNOLOGIES FOR ADAPTATION TO CLIMATE CHANGE
    • Y02A50/00TECHNOLOGIES FOR ADAPTATION TO CLIMATE CHANGE in human health protection, e.g. against extreme weather
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Abstract

The invention discloses copper-doped graphene aerogel for adsorbing VOCs and a preparation method thereof, and relates to the field of volatile organic compound adsorption materials.

Description

Copper-doped graphene aerogel for adsorbing VOCs and preparation method thereof
Technical Field
The invention relates to the field of volatile organic compound adsorption materials, in particular to copper-doped graphene aerogel for adsorbing VOCs and a preparation method thereof.
Background
Volatile Organic Compounds (VOCs) are a generic term for volatile organic compounds having a melting point below room temperature and a boiling point between 50 and 260℃and are commonly known as benzene, toluene, xylene, styrene, trichloroethylene, etc. VOCs are mainly derived from industrial production and social life. The most amount of VOCs produced by industry, such as pharmaceutical industry, petrochemical industry, printing industry, electronic industry, manufacturing industry and the like, is accompanied by a large amount of VOCs. VOCs are toxic, harmful, inflammable and explosive volatile organic matters, are harmful to animals, plants and human beings, and bring certain potential safety hazards to enterprise production due to the inflammable and explosive nature.
Hydrocarbon and nitrogen oxides in VOCs can generate a series of complex photochemical chain reactions under the action of sunlight and ultraviolet rays, and secondary pollution such as ozone, peroxyacetyl nitrate, high-activity free radicals, aldehydes, ketones, organic acids and the like can be generated in the reaction process. In addition, the high-activity free radicals and other intermediate products react with toluene, xylene and the like to generate organic aerosol and haze, so that the ecological environment is further destroyed, and the human health is influenced. Therefore, the efficient treatment of VOCs is particularly important, and among a plurality of VOCs treatment methods, the adsorption method has the advantages of low cost, wide application range, simple and convenient use, no secondary pollution, recycling of the adsorbent and the like, and is widely applied to the field of gas purification. As the core of the adsorption technology, the development of high-performance gas adsorption materials has been a research hotspot in this field.
Although the traditional adsorbents such as activated carbon, silica gel and the like have larger adsorption capacity for VOCs, the adsorption capacity of the materials can be obviously reduced in a humid environment, and the competitive adsorption of water molecules is caused by poor hydrophobicity of the materials. The graphene aerogel has surface functional groups which are easy to adjust, namely, the surface wettability of the graphene aerogel is easy to adjust and control, so that the graphene aerogel can efficiently adsorb VOCs in a humid environment. However, the graphene aerogel has a small specific surface area, a large pore diameter and a small adsorption capacity to VOCs because the graphene aerogel is purely physically adsorbed.
Disclosure of Invention
The invention aims to provide copper-doped graphene aerogel for adsorbing VOCs and a preparation method thereof, so as to solve the problem that the graphene aerogel has weaker adsorption force on VOCs.
In order to solve the technical problems, the invention adopts the following specific scheme: a copper doped graphene aerogel for adsorbing VOCs comprises graphene aerogel and nano copper loaded on the graphene aerogel.
The preparation method of the copper-doped graphene aerogel comprises the following steps: and cleaning and impregnating the graphene hydrogel with a copper salt ethanol aqueous solution, freeze-drying after impregnation, performing pyrolysis roasting on the gel subjected to freeze drying in an inert atmosphere, and finally performing activation roasting in an activation atmosphere containing carbon dioxide to obtain the copper-doped graphene aerogel.
As a further optimization of the above technical scheme, the inert atmosphere is a nitrogen atmosphere or an argon atmosphere.
As a further optimization of the above technical scheme, the activating atmosphere is a pure carbon dioxide atmosphere.
As a further optimization of the technical scheme, the activating atmosphere is a mixed atmosphere of carbon dioxide and inert gas, wherein the volume fraction of the carbon dioxide is more than 20%.
As a further optimization of the above technical scheme, the inert gas is nitrogen or argon.
As the technical proposal is further optimized, the pyrolysis roasting temperature is 150-450 ℃ and the roasting time is 1-10 h; the activating roasting temperature is 600-900 ℃ and the roasting time is 1-5 h.
As a further optimization of the above technical scheme, the copper salt in the copper salt ethanol aqueous solution is one of copper nitrate, copper acetate or copper sulfate.
As a further optimization of the technical scheme, the mass fraction of copper salt in the copper salt ethanol aqueous solution is 0.5% -5%, and the volume fraction of ethanol in the copper salt ethanol aqueous solution is 10% -20%.
As a further optimization of the technical scheme, the graphene hydrogel is washed 5-15 times by copper salt ethanol aqueous solution, is immersed for 12-36 hours, and is subjected to freeze drying for 24-72 hours after the immersion is completed.
As a further optimization of the above technical scheme, the graphene hydrogel is prepared by the following method: and ultrasonically dispersing graphene oxide in an aqueous solution to prepare graphene oxide dispersion liquid, adding a reducing agent, stirring, and performing a heating reaction to obtain the graphene hydrogel.
As a further optimization of the technical scheme, the reducing agent is one of ethylenediamine, ascorbic acid or hydrazine hydrate.
As further optimization of the technical scheme, the mass ratio of the reducing agent to the graphene oxide is 0.5-2:1.
As a further optimization of the technical scheme, the concentration of the graphene oxide dispersion liquid is 0.5-10g/L, and the ultrasonic treatment time is 10-90 min.
Compared with the prior art, the invention has the following beneficial effects: the invention provides a modification method of graphene aerogel, which comprises the steps of impregnating copper salt with the graphene aerogel, preparing copper-doped graphene aerogel through two-stage roasting, and carrying out copper salt pyrolysis and CO 2 The activation process acts together to greatly increase the micropore structure of the graphene aerogel, and copper is introduced as a chemical adsorption active center to greatly increase the saturated adsorption quantity of the graphene aerogel.
The copper-doped graphene aerogel prepared by the method disclosed by the invention has the advantages of small density, large specific surface area, high porosity, multiple micropore structures and the like as a three-dimensional porous aerogel material, and the graphene aerogel has surface functional groups which are easy to adjust, namely, the surface wettability of the graphene aerogel is easy to adjust and control, so that the graphene aerogel can efficiently adsorb VOCs in a humid environment.
Detailed Description
Example 1
A copper-doped graphene aerogel for adsorbing VOCs and a preparation method thereof specifically comprise the following steps:
(1) 0.04g of graphene oxide is dispersed in 40mL of aqueous solution, and ultrasonic treatment is carried out for 30min to obtain 1g/L graphene oxide dispersion liquid.
(2) Adding 0.04g of ascorbic acid into the graphene oxide dispersion liquid, stirring for 20min, taking 10mL, placing into a sample bottle, and placing the sample bottle into a 70 ℃ oven for heating reaction for 5h to obtain the graphene hydrogel.
(3) And (3) washing the graphene hydrogel for 10 times by using a copper acetate ethanol water solution with the mass fraction of copper acetate being 1% and the volume fraction of ethanol being 20%, wherein each washing step is carried out for 10 minutes, then a new solution is replaced, and the solution is used for soaking for 24 hours after washing. The impregnated hydrogel was freeze-dried for 72 hours and placed in a tube furnace for calcination. The first stage roasting is pyrolysis roasting, the temperature is 350 ℃, the heating rate is 5 ℃/min, the roasting time is 4 hours, and the pyrolysis roasting atmosphere is nitrogen; the second stage of roasting is activation roasting, the temperature is 800 ℃, the heating rate is 5 ℃/min, the roasting time is 2 hours, the activation roasting atmosphere is a mixed gas of carbon dioxide and nitrogen, and the volume fraction of the carbon dioxide is 30%. And cooling to room temperature after roasting to obtain the copper-doped graphene aerogel (Cu/AGA-1).
The specific surface area and the pore diameter of Cu/AGA-1 are analyzed to obtain the Cu/AGA-1 with the specific surface area of 524.9m 2 And/g, average pore diameter of 2.1nm.
Example 2
A copper-doped graphene aerogel for adsorbing VOCs and a preparation method thereof specifically comprise the following steps:
(1) 0.04g of graphene oxide is dispersed in 40mL of aqueous solution, and ultrasonic treatment is carried out for 30min to obtain 1g/L graphene oxide dispersion liquid.
(2) Adding 0.04g of ascorbic acid into the graphene oxide dispersion liquid, stirring for 20min, taking 10mL, placing into a sample bottle, and placing the sample bottle into a 70 ℃ oven for heating reaction for 5h to obtain the graphene hydrogel.
(3) And (3) washing the graphene hydrogel with a copper nitrate aqueous solution with the mass fraction of copper nitrate being 1% and the volume fraction of ethanol being 20% for 10 times, wherein each washing step is carried out for 10 minutes, then a new solution is replaced, and after washing, the solution is used for soaking for 24 hours. The impregnated hydrogel was freeze-dried for 72 hours and placed in a tube furnace for calcination. The first stage roasting is pyrolysis roasting, the temperature is 350 ℃, the heating rate is 5 ℃/min, the roasting time is 4 hours, and the pyrolysis roasting atmosphere is nitrogen; the second stage of roasting is activation roasting, the temperature is 800 ℃, the heating rate is 5 ℃/min, the roasting time is 2 hours, the activation roasting atmosphere is a mixed gas of carbon dioxide and nitrogen, and the volume fraction of the carbon dioxide is 30%. And cooling to room temperature after roasting to obtain the copper-doped graphene aerogel (Cu/AGA-2).
The specific surface area and the pore diameter of Cu/AGA-2 are analyzed to obtain the Cu/AGA-2 with the specific surface area of 450.8m 2 And/g, average pore diameter of 3.2nm.
Example 3
A copper-doped graphene aerogel for adsorbing VOCs and a preparation method thereof specifically comprise the following steps:
(1) 0.04g of graphene oxide is dispersed in 40mL of aqueous solution, and ultrasonic treatment is carried out for 30min to obtain 1g/L graphene oxide dispersion liquid.
(2) Adding 0.04g of ascorbic acid into the graphene oxide dispersion liquid, stirring for 20min, taking 10mL, placing into a sample bottle, and placing the sample bottle into a 70 ℃ oven for heating reaction for 5h to obtain the graphene hydrogel.
(3) And (3) washing the graphene hydrogel for 10 times by using a copper sulfate ethanol water solution with the mass fraction of copper sulfate being 1% and the volume fraction of ethanol being 20%, wherein each washing step is carried out for 10 minutes, then a new solution is replaced, and the solution is used for soaking for 24 hours after the washing is finished. The impregnated hydrogel was freeze-dried for 72 hours and placed in a tube furnace for calcination. The first stage roasting is pyrolysis roasting, the temperature is 350 ℃, the heating rate is 5 ℃/min, the roasting time is 4 hours, and the pyrolysis roasting atmosphere is nitrogen; the second stage of roasting is activation roasting, the temperature is 800 ℃, the heating rate is 5 ℃/min, the roasting time is 2 hours, the activation roasting atmosphere is a mixed gas of carbon dioxide and nitrogen, and the volume fraction of the carbon dioxide is 30%. And cooling to room temperature after roasting to obtain the copper-doped graphene aerogel (Cu/AGA-3).
The specific surface area and the pore diameter of Cu/AGA-3 are analyzed to obtain the specific surface area of 413.2m 2 And/g, average pore diameter of 3.4nm.
Example 4
A copper-doped graphene aerogel for adsorbing VOCs and a preparation method thereof specifically comprise the following steps:
(1) 0.04g of graphene oxide is dispersed in 40mL of aqueous solution, and ultrasonic treatment is carried out for 30min to obtain 1g/L graphene oxide dispersion liquid.
(2) Adding 0.04g of ascorbic acid into the graphene oxide dispersion liquid, stirring for 20min, taking 10mL, placing into a sample bottle, and placing the sample bottle into a 70 ℃ oven for heating reaction for 5h to obtain the graphene hydrogel.
(3) And (3) washing the graphene hydrogel for 10 times by using a copper acetate ethanol water solution with the mass fraction of copper acetate being 1% and the volume fraction of ethanol being 20%, wherein each washing step is carried out for 10 minutes, then a new solution is replaced, and the solution is used for soaking for 24 hours after washing. The impregnated hydrogel was freeze-dried for 72 hours and placed in a tube furnace for calcination. The first stage roasting is pyrolysis roasting, the temperature is 350 ℃, the heating rate is 5 ℃/min, the roasting time is 4 hours, and the pyrolysis roasting atmosphere is nitrogen; the second stage of roasting is activation roasting, the temperature is 800 ℃, the heating rate is 5 ℃/min, the roasting time is 2h, and the activation roasting atmosphere is carbon dioxide atmosphere. And cooling to room temperature after roasting to obtain the copper-doped graphene aerogel (Cu/AGA-4).
The specific surface area and the pore diameter of Cu/AGA-4 are analyzed to obtain the Cu/AGA-4 with the specific surface area of 518.9m 2 And/g, average pore diameter of 2.5nm.
Example 5
A copper-doped graphene aerogel for adsorbing VOCs and a preparation method thereof specifically comprise the following steps:
(1) 0.02g of graphene oxide is dispersed in 40mL of aqueous solution, and ultrasonic treatment is carried out for 10min to obtain 0.5g/L graphene oxide dispersion liquid.
(2) Adding 0.04g of ethylenediamine into the graphene oxide dispersion liquid, stirring for 20min, taking 10mL, placing into a sample bottle, and placing the sample bottle into a 70 ℃ oven for heating reaction for 5h to obtain the graphene hydrogel.
(3) And (3) washing the graphene hydrogel with a copper acetate aqueous solution with the mass fraction of copper acetate being 0.5% and the volume fraction of ethanol being 10% for 15 times, wherein each washing step is carried out for 10 minutes, then a new solution is replaced, and after washing, the solution is used for soaking for 12 hours. The impregnated hydrogel was freeze-dried for 36h and placed in a tube furnace for calcination. The first stage roasting is pyrolysis roasting, the temperature is 350 ℃, the heating rate is 5 ℃/min, the roasting time is 4 hours, and the pyrolysis roasting atmosphere is nitrogen; the second stage of roasting is activation roasting, the temperature is 800 ℃, the heating rate is 5 ℃/min, the roasting time is 2 hours, the activation roasting atmosphere is a mixed gas of carbon dioxide and nitrogen, and the volume fraction of the carbon dioxide is 30%. And cooling to room temperature after roasting is finished to obtain the Cu/AGA of the copper-doped graphene aerogel.
Example 6
A copper-doped graphene aerogel for adsorbing VOCs and a preparation method thereof specifically comprise the following steps:
(1) 0.4g of graphene oxide is dispersed in 40mL of aqueous solution, and ultrasonic treatment is carried out for 90min to obtain 10g/L graphene oxide dispersion liquid.
(2) Adding 0.2g of hydrazine hydrate into the graphene oxide dispersion liquid, stirring for 20min, taking 10mL of the mixture, placing the 10mL of the mixture into a sample bottle, and placing the sample bottle into a 70 ℃ oven for heating reaction for 5h to obtain the graphene hydrogel.
(3) And (3) washing the graphene hydrogel with a copper acetate ethanol water solution with the mass fraction of copper acetate being 5% and the volume fraction of ethanol being 15% for 5 times, wherein each washing step is carried out for 10 minutes, then a new solution is replaced, and the solution is used for soaking for 36 hours after washing. Freeze-drying the impregnated hydrogel for 24 hours, and placing the hydrogel into a tube furnace for roasting. The first stage roasting is pyrolysis roasting, the temperature is 450 ℃, the heating rate is 10 ℃/min, the roasting time is 1h, and the pyrolysis roasting atmosphere is nitrogen; the second stage of roasting is activation roasting, the temperature is 900 ℃, the heating rate is 10 ℃/min, the roasting time is 1h, the activation roasting atmosphere is a mixed gas of carbon dioxide and nitrogen, and the volume fraction of the carbon dioxide is 20%. And cooling to room temperature after roasting is finished to obtain the Cu/AGA of the copper-doped graphene aerogel.
Example 7
A copper-doped graphene aerogel for adsorbing VOCs and a preparation method thereof specifically comprise the following steps:
(1) 0.04g of graphene oxide is dispersed in 40mL of aqueous solution, and ultrasonic treatment is carried out for 30min to obtain 1g/L graphene oxide dispersion liquid.
(2) Adding 0.04g of ascorbic acid into the graphene oxide dispersion liquid, stirring for 20min, taking 10mL, placing into a sample bottle, and placing the sample bottle into a 70 ℃ oven for heating reaction for 5h to obtain the graphene hydrogel.
(3) And (3) washing the graphene hydrogel for 10 times by using a copper acetate ethanol water solution with the mass fraction of copper acetate being 1% and the volume fraction of ethanol being 20%, wherein each washing step is carried out for 10 minutes, then a new solution is replaced, and the solution is used for soaking for 24 hours after washing. The impregnated hydrogel was freeze-dried for 72 hours and placed in a tube furnace for calcination. The first stage roasting is pyrolysis roasting, the temperature is 150 ℃, the heating rate is 5 ℃/min, the roasting time is 10h, and the pyrolysis roasting atmosphere is argon; the second stage of roasting is activation roasting, the temperature is 600 ℃, the heating rate is 5 ℃/min, the roasting time is 5h, the activation roasting atmosphere is a mixed gas of carbon dioxide and argon, and the volume fraction of the carbon dioxide is 20%. And cooling to room temperature after roasting is finished to obtain the Cu/AGA of the copper-doped graphene aerogel.
Comparative example 1
The copper-doped graphene aerogel (Cu/GA-1) without second stage firing was taken as comparative example 1, and the specific steps were as follows:
(1) 0.04g of graphene oxide is dispersed in 40mL of aqueous solution, and ultrasonic treatment is carried out for 30min to obtain 1g/L graphene oxide dispersion liquid.
(2) Adding 0.04g of ascorbic acid into the graphene oxide dispersion liquid, stirring for 20min, taking 10mL, placing into a sample bottle, and placing the sample bottle into a 70 ℃ oven for heating reaction for 5h to obtain the graphene hydrogel.
(3) And (3) washing the graphene hydrogel for 10 times by using a copper acetate ethanol water solution with the mass fraction of copper acetate being 1% and the volume fraction of ethanol being 20%, wherein each washing step is carried out for 10 minutes, then a new solution is replaced, and the solution is used for soaking for 24 hours after washing. The impregnated hydrogel was freeze-dried for 72 hours and placed in a tube furnace for calcination. The roasting temperature is 350 ℃, the heating rate is 5 ℃/min, the roasting time is 4 hours, and the roasting atmosphere is nitrogen. And cooling to room temperature after roasting to obtain the Cu/GA of the copper-doped graphene aerogel.
The specific surface area and pore size of Cu/GA-1 were analyzed to obtain 362.1m2/g of specific surface area and 3.6nm of average pore size.
Comparative example 2
Copper-doped graphene aerogel (Cu/GA-2) without first stage firing was taken as comparative example 2, and the specific steps were as follows:
(1) 0.4g of graphene oxide is dispersed in 40mL of aqueous solution, and ultrasonic treatment is carried out for 30min to obtain 1g/L graphene oxide dispersion liquid.
(2) Adding 0.4g of ascorbic acid into the graphene oxide dispersion liquid, stirring for 20min, taking 10mL, placing into a sample bottle, and placing the sample bottle into a 70 ℃ oven for heating reaction for 5h to obtain the graphene hydrogel.
(3) And (3) washing the graphene hydrogel for 10 times by using a copper acetate ethanol water solution with the mass fraction of copper acetate being 1% and the volume fraction of ethanol being 20%, wherein each washing step is carried out for 10 minutes, then a new solution is replaced, and the solution is used for soaking for 24 hours after washing. The impregnated hydrogel was freeze-dried for 72 hours and placed in a tube furnace for calcination. The roasting temperature is 800 ℃, the heating rate is 5 ℃/min, the roasting time is 2h, the roasting atmosphere is a mixed gas of carbon dioxide and nitrogen, and the volume fraction of the carbon dioxide is 30%. And cooling to room temperature after roasting to obtain the copper-doped graphene aerogel Cu/GA-2'.
The Cu/GA-2 weight loss is serious compared with Cu/AGA-1, namely the process has high burning loss rate.
The specific surface area and pore size of Cu/GA-2 were analyzed to obtain a specific surface area of 389.1m2/g and an average pore size of 6.5nm.
Comparative example 3
Graphene Aerogel (GA) was used as comparative example 3, and the specific steps were as follows:
(1) 0.04g of graphene oxide is dispersed in 40mL of aqueous solution, and ultrasonic treatment is carried out for 30min to obtain 1g/L graphene oxide dispersion liquid.
(2) Adding 0.04g of ascorbic acid into the graphene oxide dispersion liquid, stirring for 20min, taking 10mL, placing into a sample bottle, and placing the sample bottle into a 70 ℃ oven for heating reaction for 5h to obtain the graphene hydrogel.
(3) And washing the graphene hydrogel with an ethanol aqueous solution with the volume fraction of 20% for 10 times, wherein the graphene hydrogel is soaked for 10 minutes in each washing, then is replaced with a new solution, and is dialyzed for 24 hours after washing. And freeze-drying the dialyzed hydrogel for 72 hours to obtain Graphene Aerogel (GA).
The GA was analyzed for specific surface area and pore size to give a specific surface area of 233.1m 2 And/g, average pore diameter of 4.4nm.
< evaluation of adsorption Performance of VOCs >
The test was performed using an adsorption evaluation device. By N 2 As carrier gas, N 2 Introducing into VOCs generator, adding toluene into gasification chamber of VOCs generator by injection pump for rapid gasification, and introducing into gasification chamber by N 2 The generator is carried out into the adsorber. The constant temperature adsorber is a glass tube with a jacket, and the adsorption temperature is controlled by adopting a super constant temperature tank. The inside diameter of the adsorber was 10mm, the length was 10cm, and the adsorbent loading was 0.1g. The toluene concentration before and after adsorption was measured by gas chromatography.
Test conditions:
the original concentration of toluene was 500ppm, the total gas flow rate was 100mL/min, and the adsorption temperature was 30 ℃.
Test results:
sample of Saturated adsorption quantity (mg/g)
Example 1 33.5
Example 2 22.4
Example 3 20.8
Comparative example 1 18.6
Comparative example 2 13.9
Comparative example 3 6.8
Studies have shown that the adsorption of VOCs on the aerogel is largely dependent on the micropores of the adsorbent, since the kinetic diameters of VOCs are within the micropore size range.
< analysis of specific surface area and pore Structure >
Comparing the data of example 1, comparative example 1 and comparative example 2, it can be obtained that the specific surface area of Cu/AGA-1 in example 1 is the largest and the average pore diameter is the smallest. The specific mechanism is as follows: the first stage roasting is a copper acetate pyrolysis process, and the GA impregnated copper acetate is decomposed by impurities on the surface and in larger pores of the copper acetate during the pyrolysis process to open a part of closed pores, and in addition, the GA skeleton is contracted to reduce the original pore size, so that the pyrolysis process increases the microporous structure of the graphene aerogel. The second stage roasting is CO 2 Activation process, CO in high temperature environment 2 Has certain oxidability of CO 2 As a gas, compared with Cu, it can enter into the graphene aerogel microporous structure to react more deeply with disordered carbon atoms and heteroatoms therein, further opening the closed pore structure, forming a new microporous pore structure. Copper acetate pyrolysis and CO 2 The activation process works together so that the microporous structure of the aerogel is greatly increased. Comparative example 1 is copper-doped graphene aerogel (Cu/GA-1) without second stage firing, without CO 2 The specific surface area of the activation process is far smaller than that of Cu/AGA-1, and the average pore diameter is also larger. Comparative example 2 is a copper-doped graphene aerogel (Cu/GA-2) without first stage firing, which can be found in CO 2 /N 2 Under a mixed atmosphere (high temperature)The copper acetate has certain oxidizing property), the copper acetate decomposition process is more severe, and the CO is added 2 In the activation process, excessive carbon burning in the aerogel is caused, so that the original pores of the aerogel are increased, and part of micropore structures are converted into mesoporous structures, so that the average pore diameter is larger than that of Cu/AGA-1, and the specific surface area is small.
The atmosphere of pyrolysis roasting is nitrogen atmosphere, the atmosphere of activation roasting is a mixed atmosphere of carbon dioxide and nitrogen, and CO 2 The activation needs to be carried out at very high temperatures (generally greater than 600 ℃), and therefore CO cannot be carried out in this temperature range from 150 to 450 ℃ 2 Activating.
< analysis of copper as principle of chemisorption Activity center >
The product generated by the pyrolysis of copper acetate at 150-300 ℃ is Cu 2 O, then Cu in the process of heating to 400 DEG C 2 O is continuously decomposed into Cu, and the product generated at the temperature of 400-450 ℃ is nano Cu. Toluene has pi bond, cu can absorb pi electron in toluene to form sigma bond, and pi complexing adsorption is formed, wherein pi complexing belongs to weak chemical bond category.

Claims (12)

1. The preparation method of the copper-doped graphene aerogel for adsorbing VOCs is characterized by comprising the steps of cleaning and impregnating graphene hydrogel with copper salt ethanol aqueous solution, freeze-drying after impregnation, performing pyrolysis roasting on the gel after freeze-drying in inert atmosphere, and finally performing activation roasting in activating atmosphere containing carbon dioxide to obtain the copper-doped graphene aerogel;
the activating atmosphere is a mixed atmosphere of carbon dioxide and inert gas, wherein the volume fraction of the carbon dioxide is more than 20%;
the pyrolysis roasting temperature is 150-450 ℃, and the roasting time is 1-10 h; the activation roasting temperature is 600-900 ℃ and the roasting time is 1-5 h;
the mass fraction of copper salt in the copper salt ethanol water solution is 0.5% -5%.
2. The method for preparing copper-doped graphene aerogel for adsorbing VOCs according to claim 1, wherein the inert atmosphere is a nitrogen atmosphere or an argon atmosphere.
3. The method for preparing copper-doped graphene aerogel for adsorbing VOCs according to claim 1, wherein the activating atmosphere is a pure carbon dioxide atmosphere.
4. The method for preparing copper-doped graphene aerogel for adsorbing VOCs according to claim 1, wherein the inert gas is nitrogen or argon.
5. The method for preparing copper-doped graphene aerogel for adsorbing VOCs according to claim 1, wherein the copper salt in the copper salt ethanol aqueous solution is one of copper nitrate, copper acetate or copper sulfate.
6. The method for preparing copper-doped graphene aerogel for adsorbing VOCs according to claim 1, wherein the volume fraction of ethanol in the copper salt ethanol aqueous solution is 10% -20%.
7. The method for preparing copper-doped graphene aerogel for adsorbing VOCs according to claim 1, wherein the graphene hydrogel is washed with copper salt ethanol aqueous solution for 5-15 times, impregnated for 12-36 hours, and freeze-dried for 24-72 hours after the impregnation is completed.
8. The method for preparing copper-doped graphene aerogel for adsorbing VOCs according to claim 1, wherein the graphene hydrogel is prepared by the following method: and ultrasonically dispersing graphene oxide in an aqueous solution to prepare graphene oxide dispersion liquid, adding a reducing agent, stirring, and performing a heating reaction to obtain the graphene hydrogel.
9. The method for preparing copper-doped graphene aerogel for adsorbing VOCs according to claim 8, wherein the reducing agent is one of ethylenediamine, ascorbic acid or hydrazine hydrate.
10. The method for preparing copper-doped graphene aerogel for adsorbing VOCs according to claim 8, wherein the mass ratio of the reducing agent to graphene oxide is 0.5-2:1.
11. The method for preparing copper-doped graphene aerogel for adsorbing VOCs according to claim 8, wherein the concentration of the graphene oxide dispersion liquid is 0.5-10g/L, and the ultrasonic treatment time is 10-90 min.
12. A copper-doped graphene aerogel for adsorbing VOCs, prepared by the method of any one of claims 1 to 11, characterized in that the copper-doped graphene aerogel comprises graphene aerogel and nano-copper supported on the graphene aerogel.
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