CN115925054B - Preparation method and application of membrane bubble phase synthetic carbon electrode composite material - Google Patents
Preparation method and application of membrane bubble phase synthetic carbon electrode composite material Download PDFInfo
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- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 title claims abstract description 69
- 229910052799 carbon Inorganic materials 0.000 title claims abstract description 65
- 239000012528 membrane Substances 0.000 title claims abstract description 63
- 239000002131 composite material Substances 0.000 title claims abstract description 45
- 238000002360 preparation method Methods 0.000 title claims abstract description 14
- 239000002243 precursor Substances 0.000 claims abstract description 35
- LZZYPRNAOMGNLH-UHFFFAOYSA-M Cetrimonium bromide Chemical compound [Br-].CCCCCCCCCCCCCCCC[N+](C)(C)C LZZYPRNAOMGNLH-UHFFFAOYSA-M 0.000 claims abstract description 31
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims abstract description 28
- 229910021645 metal ion Inorganic materials 0.000 claims abstract description 22
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims abstract description 22
- 229940051841 polyoxyethylene ether Drugs 0.000 claims abstract description 21
- 229920000056 polyoxyethylene ether Polymers 0.000 claims abstract description 21
- 239000002957 persistent organic pollutant Substances 0.000 claims abstract description 16
- 241000208822 Lactuca Species 0.000 claims abstract description 15
- 235000003228 Lactuca sativa Nutrition 0.000 claims abstract description 15
- 239000002994 raw material Substances 0.000 claims abstract description 14
- 239000002904 solvent Substances 0.000 claims abstract description 14
- PMZURENOXWZQFD-UHFFFAOYSA-L Sodium Sulfate Chemical compound [Na+].[Na+].[O-]S([O-])(=O)=O PMZURENOXWZQFD-UHFFFAOYSA-L 0.000 claims abstract description 12
- 229910052938 sodium sulfate Inorganic materials 0.000 claims abstract description 12
- 235000011152 sodium sulphate Nutrition 0.000 claims abstract description 12
- 238000001179 sorption measurement Methods 0.000 claims abstract description 12
- 150000002191 fatty alcohols Chemical class 0.000 claims abstract description 11
- 235000011389 fruit/vegetable juice Nutrition 0.000 claims abstract description 11
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims abstract description 10
- 229910052760 oxygen Inorganic materials 0.000 claims abstract description 10
- 239000001301 oxygen Substances 0.000 claims abstract description 10
- 230000032683 aging Effects 0.000 claims abstract description 8
- 238000001035 drying Methods 0.000 claims abstract description 8
- 238000000227 grinding Methods 0.000 claims abstract description 8
- 230000010355 oscillation Effects 0.000 claims abstract description 8
- 238000003756 stirring Methods 0.000 claims abstract description 6
- 238000013329 compounding Methods 0.000 claims abstract description 5
- 239000003610 charcoal Substances 0.000 claims abstract description 3
- 238000003487 electrochemical reaction Methods 0.000 claims abstract description 3
- 238000000034 method Methods 0.000 claims description 11
- UFMZWBIQTDUYBN-UHFFFAOYSA-N cobalt dinitrate Chemical compound [Co+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O UFMZWBIQTDUYBN-UHFFFAOYSA-N 0.000 claims description 7
- 229910001981 cobalt nitrate Inorganic materials 0.000 claims description 7
- XTVVROIMIGLXTD-UHFFFAOYSA-N copper(II) nitrate Chemical compound [Cu+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O XTVVROIMIGLXTD-UHFFFAOYSA-N 0.000 claims description 7
- 239000012153 distilled water Substances 0.000 claims description 7
- 230000008569 process Effects 0.000 claims description 3
- 239000010865 sewage Substances 0.000 claims description 3
- QGUAJWGNOXCYJF-UHFFFAOYSA-N cobalt dinitrate hexahydrate Chemical compound O.O.O.O.O.O.[Co+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O QGUAJWGNOXCYJF-UHFFFAOYSA-N 0.000 claims description 2
- SXTLQDJHRPXDSB-UHFFFAOYSA-N copper;dinitrate;trihydrate Chemical compound O.O.O.[Cu+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O SXTLQDJHRPXDSB-UHFFFAOYSA-N 0.000 claims description 2
- 238000005520 cutting process Methods 0.000 claims description 2
- 238000000746 purification Methods 0.000 claims description 2
- 238000002791 soaking Methods 0.000 claims description 2
- 238000005406 washing Methods 0.000 claims description 2
- 230000003197 catalytic effect Effects 0.000 abstract description 21
- 229960005404 sulfamethoxazole Drugs 0.000 description 23
- JLKIGFTWXXRPMT-UHFFFAOYSA-N sulphamethoxazole Chemical compound O1C(C)=CC(NS(=O)(=O)C=2C=CC(N)=CC=2)=N1 JLKIGFTWXXRPMT-UHFFFAOYSA-N 0.000 description 23
- 239000000463 material Substances 0.000 description 20
- 230000000813 microbial effect Effects 0.000 description 19
- 239000000446 fuel Substances 0.000 description 18
- 230000015556 catabolic process Effects 0.000 description 15
- 238000006731 degradation reaction Methods 0.000 description 15
- QAOWNCQODCNURD-UHFFFAOYSA-L Sulfate Chemical compound [O-]S([O-])(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-L 0.000 description 9
- 229910052708 sodium Inorganic materials 0.000 description 9
- 239000011734 sodium Substances 0.000 description 9
- 239000011148 porous material Substances 0.000 description 8
- 239000003575 carbonaceous material Substances 0.000 description 6
- 230000000694 effects Effects 0.000 description 5
- 239000000706 filtrate Substances 0.000 description 5
- -1 sodium fatty alcohol Chemical class 0.000 description 5
- DGAQECJNVWCQMB-PUAWFVPOSA-M Ilexoside XXIX Chemical compound C[C@@H]1CC[C@@]2(CC[C@@]3(C(=CC[C@H]4[C@]3(CC[C@@H]5[C@@]4(CC[C@@H](C5(C)C)OS(=O)(=O)[O-])C)C)[C@@H]2[C@]1(C)O)C)C(=O)O[C@H]6[C@@H]([C@H]([C@@H]([C@H](O6)CO)O)O)O.[Na+] DGAQECJNVWCQMB-PUAWFVPOSA-M 0.000 description 4
- 150000001875 compounds Chemical class 0.000 description 4
- 239000007772 electrode material Substances 0.000 description 4
- 230000005540 biological transmission Effects 0.000 description 3
- 230000002209 hydrophobic effect Effects 0.000 description 3
- 239000003054 catalyst Substances 0.000 description 2
- 229910002804 graphite Inorganic materials 0.000 description 2
- 239000010439 graphite Substances 0.000 description 2
- 244000005700 microbiome Species 0.000 description 2
- 238000012986 modification Methods 0.000 description 2
- 230000004048 modification Effects 0.000 description 2
- 238000001878 scanning electron micrograph Methods 0.000 description 2
- 239000000126 substance Substances 0.000 description 2
- 239000004094 surface-active agent Substances 0.000 description 2
- 239000002351 wastewater Substances 0.000 description 2
- 239000002028 Biomass Substances 0.000 description 1
- 125000000129 anionic group Chemical group 0.000 description 1
- 239000003945 anionic surfactant Substances 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 230000015572 biosynthetic process Effects 0.000 description 1
- 238000006555 catalytic reaction Methods 0.000 description 1
- 239000010406 cathode material Substances 0.000 description 1
- 239000003093 cationic surfactant Substances 0.000 description 1
- 238000006243 chemical reaction Methods 0.000 description 1
- 230000000593 degrading effect Effects 0.000 description 1
- 230000018109 developmental process Effects 0.000 description 1
- 238000009826 distribution Methods 0.000 description 1
- 230000005611 electricity Effects 0.000 description 1
- 230000007613 environmental effect Effects 0.000 description 1
- 239000003344 environmental pollutant Substances 0.000 description 1
- 239000004744 fabric Substances 0.000 description 1
- 239000006260 foam Substances 0.000 description 1
- 238000009472 formulation Methods 0.000 description 1
- 238000003837 high-temperature calcination Methods 0.000 description 1
- 238000011065 in-situ storage Methods 0.000 description 1
- 230000000670 limiting effect Effects 0.000 description 1
- 150000002632 lipids Chemical class 0.000 description 1
- 238000004519 manufacturing process Methods 0.000 description 1
- 239000002184 metal Substances 0.000 description 1
- 229910052751 metal Inorganic materials 0.000 description 1
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 1
- 238000002156 mixing Methods 0.000 description 1
- 239000000203 mixture Substances 0.000 description 1
- 235000015097 nutrients Nutrition 0.000 description 1
- 125000000913 palmityl group Chemical group [H]C([*])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])[H] 0.000 description 1
- 239000012466 permeate Substances 0.000 description 1
- 231100000719 pollutant Toxicity 0.000 description 1
- 230000009467 reduction Effects 0.000 description 1
- 239000010902 straw Substances 0.000 description 1
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Abstract
The invention discloses a preparation method and application of a membrane bubble phase synthetic carbon electrode composite material, and the specific preparation steps comprise: s1, stirring and juicing lettuce leaves, performing membrane treatment, stirring 100ml of lettuce leaf juice and 15ml of metal ion raw materials for 1h at room temperature, and setting the rotating speed to 800r/min to obtain a precursor solution of charcoal; s2, oscillating and shaking cetyl trimethyl ammonium bromide and fatty alcohol polyoxyethylene ether sodium sulfate according to the volume ratio of 1.0-1.5:1.0-2.0 under the condition of an ethanol solvent of 25-40%, standing after constant-temperature water bath, and compounding to form a membrane bubble phase solution; s3, adding the precursor solution of the carbon into the membrane bubble phase solution according to the volume ratio, aging for 10-12 hours at room temperature after ultrasonic oscillation, drying at 80-100 ℃, roasting under the condition of isolating oxygen, and grinding to obtain the membrane bubble phase synthetic carbon electrode composite material. The invention not only realizes high catalytic activity, but also can efficiently adsorb low-concentration organic pollutants, and has better application in various electrochemical reactions, low-concentration organic pollutant adsorption, electrodes and the like.
Description
Technical Field
The invention relates to the technical field of sewage treatment, in particular to a preparation method and application of a membrane bubble phase synthetic carbon electrode composite material.
Background
The microbial fuel cell is a novel energy conversion device and has the advantages of environmental friendliness, low price, cleanness, no secondary pollution and the like. The method is a process for degrading organic pollutants by utilizing microbial activity, and microorganisms near the anode can oxidize and degrade the organic pollutants in the wastewater, and finally a large amount of organic pollutants in the wastewater are degraded into small molecular substances which are converted into nutrient substances required by the survival of the microorganisms so as to reduce the concentration of the pollutants in the water. The electrode catalytic material of the microbial fuel cell is a key factor for determining the performance and cost of the cell, so that the development of the electrode material with low price and high catalytic activity has very important significance.
The anode of the microbial fuel cell is mainly made of carbon as a base material and comprises carbon paper, carbon cloth, graphite sheets (bars), carbon felt and foam graphite. The catalyst has limited catalytic activity, limited adsorption effect on organic pollutants, uneven mesoporous structure height, small specific surface area, no large number of active sites, no adsorption treatment on low-concentration organic pollutants, and no large pore volume, so that the transmission efficiency of the microbial fuel cell is limited.
Disclosure of Invention
Therefore, the invention provides a preparation method and application of a membrane bubble phase synthetic carbon electrode composite material, which utilizes metal ions, biomass juice, cetyltrimethylammonium bromide and fatty alcohol-polyoxyethylene ether sodium sulfate to prepare a novel composite electrode material, so that the catalytic activity is high, and meanwhile, the prepared composite material can efficiently adsorb low-concentration organic pollutants to solve the problems in the background technology.
In order to achieve the above object, the present invention provides the following technical solutions: the preparation method of the membrane bubble phase synthetic carbon electrode composite material comprises the following specific preparation steps:
s1, stirring and juicing lettuce leaves, performing membrane treatment, taking 100ml of lettuce leaf juice obtained and 15ml of metal ion raw materials, stirring for 1h at room temperature, and setting the rotating speed to 800r/min to obtain a precursor solution of charcoal.
S2, mixing cetyl trimethyl ammonium bromide and fatty alcohol polyoxyethylene ether sodium sulfate according to a volume ratio of 1.0-1.5:1.0-2.0 is vibrated and shaken evenly under the condition of 25-40 percent ethanol solvent, and the membrane bubble phase solution is formed by standing and compounding after constant temperature water bath.
S3, adding a precursor solution of carbon into the membrane bubble phase solution according to the volume ratio, performing ultrasonic oscillation for 20min at 100Hz, aging for 10-12 h at room temperature, drying at 80-100 ℃, roasting and grinding under the condition of isolating oxygen to obtain the membrane bubble phase synthesized carbon electrode composite material.
As a preferred technical scheme of the application, in the step S1, the specific preparation method of the lettuce leaf juice comprises the following steps: selecting fresh lettuce leaves, cutting into strips of 2cm-3cm, washing with distilled water, soaking for 20min-30min, taking out, naturally airing, squeezing, and passing the juice through 0.45 μm water-based film.
In the preferred technical scheme of the application, in the step S1, the metal ion raw material in the precursor solution is copper nitrate and/or cobalt nitrate. The metal ion raw material in the precursor solution is cobalt nitrate hexahydrate and/or copper nitrate trihydrate
As a preferable technical scheme of the application, the mass fraction of the metal ions in the metal ion raw material is 0.5% -2%.
As a preferable technical scheme of the application, the mass fraction of the metal ions in the metal ion raw material is 0.6% -1.5%.
As a preferable technical scheme of the application, the mass fraction of the metal ions in the metal ion raw material is 0.5%.
As a preferable technical scheme, the mass fraction of the metal ions in the metal ion raw material is 1%.
As a preferable technical scheme, the mass fraction of the metal ions in the metal ion raw material is 1.5%.
As a preferable technical scheme of the application, the mass fraction of the metal ions in the metal ion raw material is 2%.
As a preferable technical scheme of the application, in the step S2, the temperature of the constant-temperature water bath is 25-30 ℃, and the standing time is 24-26 hours.
As a preferred technical scheme of the present application, in the step S2, the volume ratio of cetyltrimethylammonium bromide (CTAB) to sodium fatty alcohol polyoxyethylene ether sulfate (AES) is 1.0:1.5, the concentration of ethanol solvent was 40%.
As a preferred technical scheme of the present application, in the step S2, the volume ratio of cetyltrimethylammonium bromide (CTAB) to sodium fatty alcohol polyoxyethylene ether sulfate (AES) is 1.0:1.6, the concentration of ethanol solvent was 40%.
As a preferred technical scheme of the present application, in the step S2, the volume ratio of cetyltrimethylammonium bromide (CTAB) to sodium fatty alcohol polyoxyethylene ether sulfate (AES) is 1.0:1.7, the concentration of ethanol solvent was 40%.
As a preferred technical scheme of the present application, in the step S2, the volume ratio of cetyltrimethylammonium bromide (CTAB) to sodium fatty alcohol polyoxyethylene ether sulfate (AES) is 1.0:1.8, the concentration of ethanol solvent was 40%.
As a preferred technical scheme of the present application, in the step S2, the volume ratio of cetyltrimethylammonium bromide (CTAB) to sodium fatty alcohol polyoxyethylene ether sulfate (AES) is 1.0:2.0, the concentration of ethanol solvent was 40%.
As a preferable technical scheme of the application, in the step S2, the concentration of the cetyltrimethylammonium bromide and the concentration of the fatty alcohol polyoxyethylene ether sodium sulfate are both 0.0012mol/L-0.025mol/L.
As a preferable technical scheme of the application, in the step S2, the concentration of the cetyl trimethyl ammonium bromide and the concentration of the fatty alcohol polyoxyethylene ether sodium sulfate are both 0.0018mol/L-0.020mol/L.
As a preferable technical scheme, in the step S2, the concentration of the cetyltrimethylammonium bromide and the concentration of the sodium fatty alcohol-polyoxyethylene ether sulfate are both 0.0012mol/L.
As a preferable technical scheme, in the step S2, the concentration of the cetyltrimethylammonium bromide and the concentration of the sodium fatty alcohol-polyoxyethylene ether sulfate are both 0.0016mol/L.
As a preferable technical scheme of the application, in the step S2, the concentration of the cetyltrimethylammonium bromide and the concentration of the sodium fatty alcohol-polyoxyethylene ether sulfate are both 0.0019mol/L.
As a preferable technical scheme, in the step S2, the concentration of the cetyltrimethylammonium bromide and the concentration of the sodium fatty alcohol-polyoxyethylene ether sulfate are both 0.025mol/L.
As a preferred technical scheme of the application, the volume ratio of the precursor solution of the carbon and the bubble phase solution in the step S3 is 1:30-1:70.
as a preferred technical scheme of the application, the volume ratio of the precursor solution of the carbon and the bubble phase solution in the step S3 is 1:40-1:60.
as a preferred technical scheme of the application, the volume ratio of the precursor solution of the carbon and the bubble phase solution in the step S3 is 1:30.
as a preferred technical scheme of the application, the volume ratio of the precursor solution of the carbon and the bubble phase solution in the step S3 is 1:40.
as a preferred technical scheme of the application, the volume ratio of the precursor solution of the carbon and the bubble phase solution in the step S3 is 1:50.
as a preferred technical scheme of the application, the volume ratio of the precursor solution of the carbon and the bubble phase solution in the step S3 is 1:70.
as a preferable technical scheme, the roasting temperature in the step S3 is 350-500 ℃ and the roasting time is 3-6 h.
As a preferable technical scheme of the application, the roasting temperature in the step S3 is 360-450 ℃ and the roasting time is 3-6 h.
As a preferable technical scheme, the roasting temperature in the step S3 is 350 ℃ and the roasting time is 3h.
As a preferable technical scheme, the roasting temperature in the step S3 is 400 ℃ and the roasting time is 3h.
As a preferable technical scheme, the roasting temperature in the step S3 is 400 ℃ and the roasting time is 4 hours.
As a preferable technical scheme, the roasting temperature in the step S3 is 450 ℃ and the roasting time is 5h.
As a preferable technical scheme, the roasting temperature in the step S3 is 500 ℃ and the roasting time is 6h.
As a preferred technical scheme of the application, the membrane bubble phase synthetic carbon electrode composite material is obtained according to any one of the preparation methods.
As the preferable technical scheme of the application, the membrane bubble phase synthetic carbon electrode composite material is applied to various electrochemical reactions, low-concentration organic pollutant adsorption, sewage purification treatment and electrodes.
Advantageous effects
1. The size of the membrane bubble is 30-1000 nm, as shown in figure 3, the size is easy to control, and the size is easy to adjust by changing the chain length or the proportion of the two surfactants, so that the morphology of the mesoporous carbon material prepared by taking the membrane bubble as a reactor can be changed. The carbon material prepared by the template method has a regular and ordered pore canal structure, a highly uniform mesoporous structure, a great specific surface area and a large pore volume, a large number of active sites exist, as shown in fig. 4, the application prospect in catalysis and adsorption is very high, the micro-element membrane bubbles (vesicles) formed spontaneously by compounding the anionic and cationic surfactants are used as precursors of the template dispersed carbon, the formed composite material has a large specific surface area, the large specific surface area can provide more adsorption sites, the increase of the adsorption amount of low-concentration organic pollutants is facilitated, the prepared material has good morphology, the porosity and the specific surface area by using the membrane bubbles as templates, and the aperture and the specific surface area of the composite material can be adjusted by changing the proportion of the carbon material to the membrane bubbles.
2. The metal element can generate high-efficiency multi-electron transfer oxygen reduction active sites and increase oxygen adsorption sites, so that the catalyst has high catalytic activity.
3. As shown in FIG. 5, a part of CTAB is also reserved at the roasting temperature of 350-500 ℃, the CTAB has a hydrophobic hexadecyl group, has strong affinity to organic matters, has excellent permeation flexibility, and is modified by CTAB, a certain amount of CTAB is inserted into a carbon internal structure, so that the adsorption effect of carbon materials on organic pollutants is improved, the distribution of pore diameters is more concentrated due to the addition of CTAB, the mechanical strength of the structure is ensured, and the excellent cycle stability, pore volume and specific surface area are obviously increased. The increase of the specific surface area means that the contact area of the material with the organic pollutants can be increased, and the increase of the pore volume can improve the transmission efficiency of the microbial fuel cell, and finally the electricity generation performance is improved.
Drawings
FIG. 1 is a flow chart of a process for preparing a membrane bubble phase synthetic carbon electrode composite material according to the invention;
fig. 2 is a schematic view of removal effects of sulfamethoxazole SMX and sulfamethoxazole PTA in a microbial fuel cell by using the membrane vesicle phase synthetic carbon electrode composite material prepared in examples 1-5;
FIG. 3 is an SEM image of a bubble;
FIG. 4 is an SEM image of the carbon material;
fig. 5 is a graph of power density versus current density for activated carbon and a bubble phase synthetic carbon electrode composite material prepared herein as a cathode catalytic material for a microbial fuel cell.
Detailed Description
Other advantages and advantages of the present invention will become apparent to those skilled in the art from the following detailed description, which, by way of illustration, is to be read in connection with certain specific embodiments, but not all embodiments. All other embodiments, which can be made by those skilled in the art based on the embodiments of the invention without making any inventive effort, are intended to be within the scope of the invention.
The surfactant bubble formation in the examples below was at 40℃and the concentration of the formulation was 25X 10 -3 mol/L, ph=5, with 40% ethanol as solvent.
The membrane bubble phase synthesized carbon electrode composite materials prepared in different embodiments are manufactured into cathode materials which are placed in a microbial fuel cell reactor to treat low-concentration organic pollutants.
Example 1
Fresh lettuce leaves were taken, cut into 2cm strips, washed with distilled water, soaked for 30 minutes, taken out, naturally dried, squeezed to juice, and the juice was passed through a 0.45 μm aqueous membrane. 100ml of the obtained filtrate and 15ml of copper nitrate/cobalt nitrate with mass fraction of 0.5% are taken and stirred for 1h at a rotating speed of 800r/min under the condition of room temperature to obtain a precursor solution of the carbon. 0.025mol/L hexadecyl trimethyl ammonium bromide and fatty alcohol polyoxyethylene ether sodium sulfate are taken according to the volume ratio of 1.0:1.5 shake and shake evenly under the condition of 40% ethanol solvent, stand for 24 hours after constant temperature water bath at 25 ℃, and compound to form a membrane bubble phase solution. Precursor solution of carbon according to volume ratio: bubble phase solution = 1:30 adding the precursor solution of the carbon into the membrane bubble phase solution, aging for 20min at room temperature after 100Hz ultrasonic oscillation for 12h, drying at 100 ℃, roasting for 3h at 350 ℃ under the condition of isolating oxygen, and grinding to obtain the membrane bubble phase synthesized carbon electrode composite material. The electrode composite material is manufactured into a cathode catalytic material, and the cathode catalytic material is applied to a microbial fuel cell to treat 10mg/L of Sulfamethoxazole (SMX) +10mg/L of PTA, wherein the measured sulfamethoxazole degradation rate is 86% after 48 hours, and the PTA degradation rate is 85%.
Example 2
Fresh lettuce leaves were taken, cut into two cm strips, washed with distilled water, soaked for 30 minutes, taken out, naturally dried, and then juiced, and the juice was passed through a 0.45 μm aqueous membrane. 100ml of the obtained filtrate and 15ml of copper nitrate/cobalt nitrate with the mass fraction of 1.0% are taken and stirred for 1h at the rotating speed of 800r/min under the room temperature condition to obtain a precursor solution of the carbon. 0.025mol/L hexadecyl trimethyl ammonium bromide and fatty alcohol polyoxyethylene ether sodium sulfate are taken according to the volume ratio of 1.0:1.6 shake and shake evenly under the condition of 40% ethanol solvent, stand for 25h after constant temperature water bath at 26 ℃, and compound to form a membrane bubble phase solution. Precursor solution of carbon according to volume ratio: bubble phase solution = 1:40, adding the precursor solution of the carbon into the membrane bubble phase solution, aging for 12 hours at room temperature after ultrasonic oscillation for 20 minutes at 100Hz, drying at 100 ℃, roasting for 3 hours at 400 ℃ under the condition of isolating oxygen, and grinding to obtain the membrane bubble phase synthesized carbon electrode composite material. The electrode composite material is manufactured into a cathode catalytic material, and the cathode catalytic material is applied to a microbial fuel cell to treat 10mg/L of Sulfamethoxazole (SMX) +10mg/L of PTA, wherein the measured sulfamethoxazole degradation rate is 92% after 48 hours, and the PTA degradation rate is 90%.
Example 3
Fresh lettuce leaves were taken, cut into two cm strips, washed with distilled water, soaked for 30 minutes, taken out, naturally dried, squeezed and passed through a 0.45 μm aqueous membrane. 100ml of the obtained filtrate and 15ml of copper nitrate/cobalt nitrate with the mass fraction of 1.5% are taken and stirred for 1h at the rotating speed of 800r/min under the condition of room temperature to obtain a precursor solution of the carbon. 0.025mol/L hexadecyl trimethyl ammonium bromide and fatty alcohol polyoxyethylene ether sodium sulfate are taken according to the volume ratio of 1.0:1.7 shake and shake evenly under the condition of 40% ethanol solvent, stand for 25h after constant temperature water bath at 27 ℃, and compound to form a membrane bubble phase solution. Precursor solution of carbon according to volume ratio: bubble phase solution = 1:50, adding the precursor solution of the carbon into the membrane bubble phase solution, aging for 12 hours at room temperature after ultrasonic oscillation for 20 minutes at 100Hz, drying at 100 ℃, roasting for 4 hours at 400 ℃ under the condition of isolating oxygen, and grinding to obtain the membrane bubble phase synthesized carbon electrode composite material. The electrode composite material is manufactured into a cathode catalytic material, and the cathode catalytic material is applied to a microbial fuel cell to treat 10mg/L of Sulfamethoxazole (SMX) +10mg/L of PTA, wherein the measured sulfamethoxazole degradation rate is 85% after 48 hours, and the PTA degradation rate is 82%.
Example 4
Fresh lettuce leaves were taken, cut into two cm strips, washed with distilled water, soaked for 30 minutes, taken out, naturally dried, squeezed and passed through a 0.45 μm aqueous membrane. 100ml of the obtained filtrate and 15ml of copper nitrate/cobalt nitrate with the mass fraction of 1.5% are taken and stirred for 1h at the rotating speed of 800r/min under the condition of room temperature to obtain a precursor solution of the carbon. 0.025mol/L hexadecyl trimethyl ammonium bromide and fatty alcohol polyoxyethylene ether sodium sulfate are taken according to the volume ratio of 1.0:1.8 shaking and shaking evenly under the condition of 40% ethanol solvent, standing for 25h after constant-temperature water bath at 28 ℃, and compounding to form a membrane bubble phase solution. Precursor solution of carbon according to volume ratio: bubble phase solution = 1:50, adding the precursor solution of the carbon into the membrane bubble phase solution, aging for 12 hours at room temperature after ultrasonic oscillation for 20 minutes at 100Hz, drying at 100 ℃, roasting for 5 hours at 450 ℃ under the condition of isolating oxygen, and grinding to obtain the membrane bubble phase synthesized carbon electrode composite material. The electrode composite material is manufactured into a cathode catalytic material, and the cathode catalytic material is applied to a microbial fuel cell to treat 10mg/L of Sulfamethoxazole (SMX) +10mg/L of PTA, wherein the measured sulfamethoxazole degradation rate is 82% after 48 hours, and the PTA degradation rate is 81%.
Example 5
Fresh lettuce leaves were taken, cut into two cm strips, washed with distilled water, soaked for 30 minutes, taken out, naturally dried, squeezed and passed through a 0.45 μm aqueous membrane. 100ml of the obtained filtrate and 15ml of copper nitrate/cobalt nitrate with mass fraction of 2.0% are taken and stirred for 1h at a rotating speed of 800r/min under the condition of room temperature to obtain a precursor solution of the carbon. 0.025mol/L hexadecyl trimethyl ammonium bromide and fatty alcohol polyoxyethylene ether sodium sulfate are taken according to the volume ratio of 1.0:2.0 shake and shake evenly under the condition of 40% ethanol solvent, stand for 26 hours after constant temperature water bath at 30 ℃, and compound to form a membrane bubble phase solution. Precursor solution of carbon according to volume ratio: bubble phase solution = 1:70, adding the precursor solution of the carbon into the membrane bubble phase solution, aging for 12 hours at room temperature after 100Hz ultrasonic oscillation for 20 minutes, drying at 100 ℃, roasting for 6 hours at 500 ℃ under the condition of isolating oxygen, and grinding to obtain the membrane bubble phase synthesized carbon electrode composite material. The electrode composite material is manufactured into a cathode catalytic material, and the cathode catalytic material is applied to a microbial fuel cell to treat 10mg/L of Sulfamethoxazole (SMX) +10mg/L of PTA, and the measured sulfamethoxazole degradation rate is 80% after 48 hours, and the PTA degradation rate is 80%.
The comparison of the degradation rates of the sulfamethoxazole SMX and the sulfamethoxazole PTA in the microbial fuel cell by the membrane bubble phase synthesized carbon electrode composite material prepared in the 5 embodiments can be seen in fig. 2, and as can be seen from fig. 2, the degradation rate of the sulfamethoxazole measured after 48 hours is 63% and the degradation rate of the PTA is 65% when the active carbon is prepared into the cathode catalytic material for the microbial fuel cell under the same conditions; under the same conditions, the straw biochar is manufactured into a cathode catalytic material which is applied to a microbial fuel cell, the degradation rate of sulfamethoxazole measured after 48 hours is 55%, the PTA degradation rate is 59%, and the cathode catalytic material has a good removal effect.
As shown in FIG. 5, compared with the existing active carbon electrode materials, the power density of the composite material is continuously increased along with the increase of the current density of the composite material, and the composite material of the membrane bubble phase synthetic carbon electrode prepared by the method is used as a cathode catalytic material of a microbial fuel cell, and the power density of the composite material is suddenly increased near 0.8A/m , so that the output electric energy of the composite material in unit time is superior to that of the existing electrode material, the transmission efficiency of the microbial fuel cell can be improved, the pore volume is increased, the removal efficiency of organic pollutants is better, and the prepared material has good morphology, the porosity and the specific surface area by using the membrane bubble as a template, and the large specific surface area can provide more adsorption sites which are beneficial to the increase of the adsorption quantity of the low-concentration organic pollutants.
On one hand, 3 large areas (the outer surface, the inner surface and the cavity of the double-layer membrane) of the membrane bubble can provide different microenvironments, serve as a soft template to assemble a precursor of carbon, and induce the growth process and the growth direction of the pore diameter of the carbon material by utilizing the special structure of the membrane bubble to obtain a microscopic ordered composite material;
on the other hand, the precursor of the carbon is limited in the hydrophobic gap of the membrane bubble bilayer by utilizing the internal limiting effect, water molecules at a lipid/water interface permeate, then the precursor is condensed in situ on the hydrophobic thin layer of the membrane bubble bilayer, and finally the membrane bubble phase carbon composite material is obtained by high-temperature calcination.
While the invention has been described in detail in the foregoing general description and specific examples, it will be apparent to those skilled in the art that modifications and improvements can be made thereto. Accordingly, such modifications or improvements may be made without departing from the spirit of the invention and are intended to be within the scope of the invention as claimed.
Claims (8)
1. A preparation method of a membrane bubble phase synthetic carbon electrode composite material is characterized by comprising the following steps: the preparation method comprises the following specific preparation steps:
s1, stirring and juicing lettuce leaves, performing membrane treatment, stirring 100ml of lettuce leaf juice and 15ml of metal ion raw materials for 1h at room temperature, and setting the rotating speed to 800r/min to obtain a precursor solution of charcoal;
s2, oscillating and shaking cetyl trimethyl ammonium bromide and fatty alcohol polyoxyethylene ether sodium sulfate according to the volume ratio of 1.0-1.5:1.0-2.0 under the condition of an ethanol solvent of 25-40%, standing for 24-26 hours after constant-temperature water bath, and compounding to form a film bubble phase solution; wherein, the concentration of the cetyl trimethyl ammonium bromide and the fatty alcohol polyoxyethylene ether sodium sulfate is 0.0012mol/L-0.025mol/L;
s3, a precursor solution of carbon and a bubble phase solution are mixed according to the volume ratio of 1:30-1:70, 100Hz ultrasonic oscillation for 20min, room temperature aging for 10-12 h, drying at 80-100 ℃, roasting at 350-500 ℃ under the condition of isolating oxygen, roasting for 3-6 h, and grinding to obtain the membrane bubble phase synthetic carbon electrode composite material.
2. The method for preparing the membrane bubble phase synthetic carbon electrode composite material according to claim 1, which is characterized in that: in the step S1, the specific preparation method of the lettuce leaf juice comprises the following steps: selecting clean fresh lettuce leaves, cutting into strips of 2cm-3cm, washing with distilled water, soaking for 20min-30min, taking out, naturally airing, squeezing, and passing the juice through 0.45 water-based film.
3. The method for preparing the membrane bubble phase synthetic carbon electrode composite material according to claim 1, which is characterized in that: in the step S1, the metal ion raw material in the precursor solution is copper nitrate and/or cobalt nitrate.
4. The method for preparing the membrane bubble phase synthetic carbon electrode composite material according to claim 3, which is characterized in that: in the step S1, the metal ion raw material in the precursor solution is cobalt nitrate hexahydrate and/or copper nitrate trihydrate.
5. The method for preparing the membrane bubble phase synthetic carbon electrode composite material, which is characterized in that: the mass fraction of metal ions in the metal ion raw material is 0.5% -2%.
6. The method for preparing the membrane bubble phase synthetic carbon electrode composite material according to claim 1, which is characterized in that: in the step S2, the constant-temperature water bath temperature is 25-30 ℃.
7. A membrane bubble phase synthetic carbon electrode composite material is characterized in that: the process according to any one of claims 1 to 6.
8. The use of the membrane bubble phase synthetic carbon electrode composite material according to claim 7 in various electrochemical reactions, low concentration organic pollutant adsorption, sewage purification treatment and electrodes.
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