AU2021105368A4 - Method for Preparing and Applying Long-life Friction-sensitive Graphdiyne-based Piezoelectric Material - Google Patents
Method for Preparing and Applying Long-life Friction-sensitive Graphdiyne-based Piezoelectric Material Download PDFInfo
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- 239000000463 material Substances 0.000 title claims abstract description 62
- 238000000034 method Methods 0.000 title claims abstract description 38
- 230000003197 catalytic effect Effects 0.000 claims abstract description 33
- 239000002131 composite material Substances 0.000 claims abstract description 30
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims abstract description 26
- 238000000498 ball milling Methods 0.000 claims abstract description 21
- 238000006555 catalytic reaction Methods 0.000 claims abstract description 16
- 238000002360 preparation method Methods 0.000 claims abstract description 5
- 239000000843 powder Substances 0.000 claims description 47
- MCMNRKCIXSYSNV-UHFFFAOYSA-N Zirconium dioxide Chemical compound O=[Zr]=O MCMNRKCIXSYSNV-UHFFFAOYSA-N 0.000 claims description 24
- 239000003054 catalyst Substances 0.000 claims description 20
- 239000002243 precursor Substances 0.000 claims description 19
- 239000008367 deionised water Substances 0.000 claims description 13
- 229910021641 deionized water Inorganic materials 0.000 claims description 13
- 229920001343 polytetrafluoroethylene Polymers 0.000 claims description 13
- 239000004810 polytetrafluoroethylene Substances 0.000 claims description 13
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims description 12
- -1 polytetrafluoroethylene Polymers 0.000 claims description 12
- 239000005997 Calcium carbide Substances 0.000 claims description 9
- CLZWAWBPWVRRGI-UHFFFAOYSA-N tert-butyl 2-[2-[2-[2-[bis[2-[(2-methylpropan-2-yl)oxy]-2-oxoethyl]amino]-5-bromophenoxy]ethoxy]-4-methyl-n-[2-[(2-methylpropan-2-yl)oxy]-2-oxoethyl]anilino]acetate Chemical compound CC1=CC=C(N(CC(=O)OC(C)(C)C)CC(=O)OC(C)(C)C)C(OCCOC=2C(=CC=C(Br)C=2)N(CC(=O)OC(C)(C)C)CC(=O)OC(C)(C)C)=C1 CLZWAWBPWVRRGI-UHFFFAOYSA-N 0.000 claims description 9
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- 230000008569 process Effects 0.000 claims description 5
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- 239000000919 ceramic Substances 0.000 claims description 4
- 229910052961 molybdenite Inorganic materials 0.000 claims description 4
- CWQXQMHSOZUFJS-UHFFFAOYSA-N molybdenum disulfide Chemical compound S=[Mo]=S CWQXQMHSOZUFJS-UHFFFAOYSA-N 0.000 claims description 4
- 229910052982 molybdenum disulfide Inorganic materials 0.000 claims description 4
- 239000012299 nitrogen atmosphere Substances 0.000 claims description 4
- 229910002113 barium titanate Inorganic materials 0.000 claims description 3
- 238000005119 centrifugation Methods 0.000 claims description 3
- 239000000835 fiber Substances 0.000 claims description 3
- CAYGQBVSOZLICD-UHFFFAOYSA-N hexabromobenzene Chemical compound BrC1=C(Br)C(Br)=C(Br)C(Br)=C1Br CAYGQBVSOZLICD-UHFFFAOYSA-N 0.000 claims description 3
- 239000000203 mixture Substances 0.000 claims description 3
- 239000002994 raw material Substances 0.000 claims description 3
- 229910003090 WSe2 Inorganic materials 0.000 claims description 2
- 239000004744 fabric Substances 0.000 claims description 2
- 239000012065 filter cake Substances 0.000 claims description 2
- CKAPSXZOOQJIBF-UHFFFAOYSA-N hexachlorobenzene Chemical compound ClC1=C(Cl)C(Cl)=C(Cl)C(Cl)=C1Cl CKAPSXZOOQJIBF-UHFFFAOYSA-N 0.000 claims description 2
- QNMKKFHJKJJOMZ-UHFFFAOYSA-N hexaiodobenzene Chemical compound IC1=C(I)C(I)=C(I)C(I)=C1I QNMKKFHJKJJOMZ-UHFFFAOYSA-N 0.000 claims description 2
- 230000000977 initiatory effect Effects 0.000 claims description 2
- 239000011812 mixed powder Substances 0.000 claims description 2
- 238000003756 stirring Methods 0.000 claims description 2
- 239000000376 reactant Substances 0.000 claims 1
- 230000000694 effects Effects 0.000 abstract description 11
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- 230000009977 dual effect Effects 0.000 abstract 1
- 239000002957 persistent organic pollutant Substances 0.000 abstract 1
- HEMHJVSKTPXQMS-UHFFFAOYSA-M Sodium hydroxide Chemical compound [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 description 6
- 238000005516 engineering process Methods 0.000 description 6
- ISWSIDIOOBJBQZ-UHFFFAOYSA-N Phenol Chemical compound OC1=CC=CC=C1 ISWSIDIOOBJBQZ-UHFFFAOYSA-N 0.000 description 5
- 239000004098 Tetracycline Substances 0.000 description 5
- 230000005540 biological transmission Effects 0.000 description 5
- PYWVYCXTNDRMGF-UHFFFAOYSA-N rhodamine B Chemical compound [Cl-].C=12C=CC(=[N+](CC)CC)C=C2OC2=CC(N(CC)CC)=CC=C2C=1C1=CC=CC=C1C(O)=O PYWVYCXTNDRMGF-UHFFFAOYSA-N 0.000 description 5
- 229960002180 tetracycline Drugs 0.000 description 5
- 229930101283 tetracycline Natural products 0.000 description 5
- 235000019364 tetracycline Nutrition 0.000 description 5
- 150000003522 tetracyclines Chemical class 0.000 description 5
- 230000009471 action Effects 0.000 description 4
- 230000015556 catabolic process Effects 0.000 description 4
- 238000006731 degradation reaction Methods 0.000 description 4
- 230000007613 environmental effect Effects 0.000 description 4
- UMGDCJDMYOKAJW-UHFFFAOYSA-N thiourea Chemical compound NC(N)=S UMGDCJDMYOKAJW-UHFFFAOYSA-N 0.000 description 4
- 238000005286 illumination Methods 0.000 description 3
- 238000003801 milling Methods 0.000 description 3
- 229940043267 rhodamine b Drugs 0.000 description 3
- 239000002351 wastewater Substances 0.000 description 3
- CDBYLPFSWZWCQE-UHFFFAOYSA-L Sodium Carbonate Chemical compound [Na+].[Na+].[O-]C([O-])=O CDBYLPFSWZWCQE-UHFFFAOYSA-L 0.000 description 2
- XSQUKJJJFZCRTK-UHFFFAOYSA-N Urea Natural products NC(N)=O XSQUKJJJFZCRTK-UHFFFAOYSA-N 0.000 description 2
- 230000015572 biosynthetic process Effects 0.000 description 2
- 230000008878 coupling Effects 0.000 description 2
- 238000010168 coupling process Methods 0.000 description 2
- 238000005859 coupling reaction Methods 0.000 description 2
- 238000010303 mechanochemical reaction Methods 0.000 description 2
- JRKICGRDRMAZLK-UHFFFAOYSA-L persulfate group Chemical class S(=O)(=O)([O-])OOS(=O)(=O)[O-] JRKICGRDRMAZLK-UHFFFAOYSA-L 0.000 description 2
- 230000001699 photocatalysis Effects 0.000 description 2
- 239000011941 photocatalyst Substances 0.000 description 2
- 238000003786 synthesis reaction Methods 0.000 description 2
- DZKDPOPGYFUOGI-UHFFFAOYSA-N tungsten(iv) oxide Chemical compound O=[W]=O DZKDPOPGYFUOGI-UHFFFAOYSA-N 0.000 description 2
- HEFNNWSXXWATRW-UHFFFAOYSA-N Ibuprofen Chemical compound CC(C)CC1=CC=C(C(C)C(O)=O)C=C1 HEFNNWSXXWATRW-UHFFFAOYSA-N 0.000 description 1
- 102000004310 Ion Channels Human genes 0.000 description 1
- 239000002033 PVDF binder Substances 0.000 description 1
- 229910011011 Ti(OH)4 Inorganic materials 0.000 description 1
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 description 1
- 230000004913 activation Effects 0.000 description 1
- APUPEJJSWDHEBO-UHFFFAOYSA-P ammonium molybdate Chemical compound [NH4+].[NH4+].[O-][Mo]([O-])(=O)=O APUPEJJSWDHEBO-UHFFFAOYSA-P 0.000 description 1
- 239000011609 ammonium molybdate Substances 0.000 description 1
- 235000018660 ammonium molybdate Nutrition 0.000 description 1
- 229940010552 ammonium molybdate Drugs 0.000 description 1
- 239000012298 atmosphere Substances 0.000 description 1
- JRPBQTZRNDNNOP-UHFFFAOYSA-N barium titanate Chemical compound [Ba+2].[Ba+2].[O-][Ti]([O-])([O-])[O-] JRPBQTZRNDNNOP-UHFFFAOYSA-N 0.000 description 1
- 238000010923 batch production Methods 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
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- 239000011248 coating agent Substances 0.000 description 1
- 238000000576 coating method Methods 0.000 description 1
- 230000000593 degrading effect Effects 0.000 description 1
- 238000010586 diagram Methods 0.000 description 1
- 238000001523 electrospinning Methods 0.000 description 1
- 239000012530 fluid Substances 0.000 description 1
- 238000001027 hydrothermal synthesis Methods 0.000 description 1
- 229960001680 ibuprofen Drugs 0.000 description 1
- 159000000014 iron salts Chemical class 0.000 description 1
- 229910052451 lead zirconate titanate Inorganic materials 0.000 description 1
- HFGPZNIAWCZYJU-UHFFFAOYSA-N lead zirconate titanate Chemical compound [O-2].[O-2].[O-2].[O-2].[O-2].[Ti+4].[Zr+4].[Pb+2] HFGPZNIAWCZYJU-UHFFFAOYSA-N 0.000 description 1
- 229910052808 lithium carbonate Inorganic materials 0.000 description 1
- XGZVUEUWXADBQD-UHFFFAOYSA-L lithium carbonate Chemical compound [Li+].[Li+].[O-]C([O-])=O XGZVUEUWXADBQD-UHFFFAOYSA-L 0.000 description 1
- 238000004137 mechanical activation Methods 0.000 description 1
- 238000001000 micrograph Methods 0.000 description 1
- 239000002105 nanoparticle Substances 0.000 description 1
- 230000003647 oxidation Effects 0.000 description 1
- 238000007254 oxidation reaction Methods 0.000 description 1
- 238000011056 performance test Methods 0.000 description 1
- 238000007146 photocatalysis Methods 0.000 description 1
- 238000013033 photocatalytic degradation reaction Methods 0.000 description 1
- 238000013032 photocatalytic reaction Methods 0.000 description 1
- 229920000642 polymer Polymers 0.000 description 1
- 229920002981 polyvinylidene fluoride Polymers 0.000 description 1
- BITYAPCSNKJESK-UHFFFAOYSA-N potassiosodium Chemical compound [Na].[K] BITYAPCSNKJESK-UHFFFAOYSA-N 0.000 description 1
- 230000035484 reaction time Effects 0.000 description 1
- 230000008439 repair process Effects 0.000 description 1
- 230000003252 repetitive effect Effects 0.000 description 1
- 239000010865 sewage Substances 0.000 description 1
- 229910000029 sodium carbonate Inorganic materials 0.000 description 1
- 235000017550 sodium carbonate Nutrition 0.000 description 1
- 238000001308 synthesis method Methods 0.000 description 1
- 238000009210 therapy by ultrasound Methods 0.000 description 1
- 239000010936 titanium Substances 0.000 description 1
- OGIDPMRJRNCKJF-UHFFFAOYSA-N titanium oxide Inorganic materials [Ti]=O OGIDPMRJRNCKJF-UHFFFAOYSA-N 0.000 description 1
- 238000002604 ultrasonography Methods 0.000 description 1
- 238000004065 wastewater treatment Methods 0.000 description 1
Classifications
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J27/00—Catalysts comprising the elements or compounds of halogens, sulfur, selenium, tellurium, phosphorus or nitrogen; Catalysts comprising carbon compounds
- B01J27/20—Carbon compounds
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J35/00—Catalysts, in general, characterised by their form or physical properties
- B01J35/30—Catalysts, in general, characterised by their form or physical properties characterised by their physical properties
- B01J35/33—Electric or magnetic properties
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B32/00—Carbon; Compounds thereof
- C01B32/15—Nano-sized carbon materials
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- Chemical & Material Sciences (AREA)
- Engineering & Computer Science (AREA)
- Materials Engineering (AREA)
- Organic Chemistry (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Organic Low-Molecular-Weight Compounds And Preparation Thereof (AREA)
- Catalysts (AREA)
Abstract
The invention relates to a method for preparing and applying a friction-sensitive graphdiyne
based piezoelectric material with long service life, in particular to the application of the
material in the fields of interface catalytic reaction and water purification, and belongs to the
technical field of preparation and application of novel functional materials. The material mainly
uses a new type of graphyne material with high-voltage electrical response as a structural
control agent to in situ induce the orientation growth of the piezoelectric material at its edge,
forming active defects, accelerating the separation of electrons and holes, and significantly
improving the piezoelectric catalytic performance of the composite material. At the same time,
materials are synthesized by mechanochemical method, and the size and layer thickness of
materials are adjusted to improve the friction sensitivity and mechanical stability of composite
piezoelectric catalytic materials, thus achieving the dual goals of high voltage electrical activity
and long life. Under the condition of mechanical force provided by in-situ ball milling, organic
pollutants in water can be oxidized and degraded efficiently and sustainably through
piezoelectric catalytic reaction.
Description
Method for Preparing and Applying Long-life Friction-sensitive Graphdiyne-based
Piezoelectric Material
The invention provides a method for preparing and applying a long-life friction-sensitive
graphdiyne-based piezoelectric material, relates to a preparation method of a long-life
friction-sensitive graphdiyne-based piezoelectric material, particularly relates to the
application in the fields of interface catalytic reaction and water purification, and belongs
to the technical field of preparation and application of novel functional materials.
Piezoelectric catalytic materials are one of the emerging excellent materials in recent
years. However, most of the materials are mainly used in the energy field, and the
applications in the environmental field need to be further expanded and studied. Recently,
CN109331882A discloses an organic piezoelectric-photocatalytic composite spiral fiber,
which can continuously generate self-repairing piezoelectric potential under the action of
water flow, effectively promote the separation of photo-generated electron-hole pairs of
photocatalyst, and greatly improve the efficiency of photocatalytic degradation of
pollutants. CN108772063A discloses an Ag20/Bi4Ti3012 piezoelectric photocatalyst and
a synthesis method thereof, which remarkably improves the capability of the catalytic
material for degrading organic matters under the condition of ultrasonic-assisted
illumination catalysis. CN109529807A obtains composite catalyst material by coating
lead zirconate titanate piezoelectric powder with titanium oxide nanoparticles generated
by in-situ light. When material is induced by fluid mechanical energy, piezoelectric field will be generated, which significantly improves the photocatalytic reaction effect. Liu
Lifen et al. of Dalian University of Technology invented a new type of piezoelectric
materials to build photocatalytic self-bias pollution control system (CN110165243A),
which can degrade pollutants through photocatalysis and piezoelectric effect under
illumination conditions, and realize electric energy output through piezoelectric effect
under no illumination conditions. Coupling advanced oxidation technology can improve
sewage treatment effect. It can be seen that most piezoelectric catalytic environmental
applications need to be coupled with other purification technologies, and relatively few
piezoelectric catalytic environmental applications alone.
The existing water treatment equipment in China is relatively simple and difficult to
improve, and most of them are carried out in dark environment. How to realize the
coupling of the original process to degrade pollutants in water in dark environment is a
difficult research point. Liu Zhiyong et al. of Nanchang Hangkong University used
K2C03, Na2CO3, Nb2CO5and Li2CO3 as raw materials to obtain potassium sodium
niobate-based piezoelectric ceramics by high temperature treatment, and the piezoelectric
catalytic reaction was initiated by ultrasound, which realized the efficient degradation of
dye wastewater (CN110092440A). He Chun et al. of Sun Yat-sen University disclosed
the application of piezoelectric material barium titanate in ultrasonic activated persulfate
treatment of wastewater (CN109607739A). In the piezoelectric activated persulfate
system, various free radicals can be generated, and the removal rate of ibuprofen and
other pharmaceutical wastewater can reach over 98%, and the application is not selective
and can be widely used in various wastewater treatment systems.
The catalytic activity and mechanical stability of piezoelectric catalytic materials are the
main factors that restrict its engineering application. How to improve the piezoelectric
catalytic activity of materials is also a research hotspot at present. Tang Yufei et al.
(CN108411406B) of Xi 'an University of Technology compounded piezoelectric ceramic
precursor with spinnable polymer by electrospinning technology, and reduced the
impedance between composite materials by calcination at high temperature, thus
improving the piezoelectric properties of materials. In addition, they also found that
piezoelectric materials with multi-stage structure can be constructed through multi-stage
hydrothermal reaction. Through piezoelectric performance test, it is found that multi
stage structure is beneficial to electron-hole separation and improves piezoelectric
catalytic activity (CN110540430A). However, under the action of mechanical force, the
active sites of piezoelectric catalytic materials will be gradually destroyed, and the
activity will gradually decrease. Studies show that fixing piezoelectric catalytic materials
on PVDF can improve the stability of materials, but after 10 cycles, the catalytic activity
only maintains 80%.
Therefore, aiming at the shortcomings of the prior art, the purpose of the present
invention is to provide a method for preparing and applying a long-life friction-sensitive
graphdiyne-based piezoelectric material. Graphdiyne-based composite piezoelectric
catalytic materials are obtained by introducing new graphdiyne materials as structural
regulators and fast channels for electron transmission. In the process of material
synthesis, ball milling is used to initiate mechanochemical reaction synthesis, adjust and
control the mesoscopic size of the material, and strengthen the friction sensitivity of the
material. Meanwhile, ball milling is used to provide mechanical force and initiate piezoelectric catalytic reaction in situ, thus realizing self-repair of active sites, significantly improving the stability of the material and expanding its engineering application field.
The purpose of the invention is to provide a method for preparing and applying a long
life friction-sensitive graphdiyne-based piezoelectric material aiming at the defects of the
existing piezoelectric catalytic material and application. The method initiates
mechanochemical reaction by ball milling method, and uses graphdiyne to induce the
orientation growth of the piezoelectric material in situ to obtain the friction-sensitive
composite piezoelectric catalytic material. In the process of ball milling, the mesoscopic
size and mechanical flexibility of the material are controlled, and the piezoelectric
catalytic reaction is initiated in situ by ball milling, so that the self-repair of active sites of
the material is realized, and the catalytic activity and service life are greatly improved,
and the applicability is improved.
In order to achieve this purpose, the invention adopts the following technical scheme.
The invention relates to a method for preparing and applying a long-life friction-sensitive
graphdiyne-based piezoelectric material, which comprises the following technical scheme
and steps.
1) Taking phenyl-hexahalide and calcium carbide as raw materials, accurately weigh the
phenyl-hexahalide and calcium carbide according to the molar ratio of phenyl-hexahalide
to calcium carbide of 1: (5-10), and place them in a vacuum polytetrafluoroethylene ball
milling reactor.
2) Weigh zirconia balls according to the mass ratio of materials to zirconia balls of 1:100
500, place them in a reactor, vacuumize the reactor, and ball mill for 6-20 h at the
rotating speed of 500-1000 rpm.
3) Collect the ball milled powder, wash it twice with deionized water and ethanol in
sequence, filter to obtain filter cake, and dry at 50-100°C for 2-10 h to obtain thin layer
graphdiyne powder.
4) Weigh 0.1-1 g graphdiyne powder, weigh piezoelectric material precursor according to
the mass ratio of graphdiyne to piezoelectric catalytic fabric precursor of 1:(50-1000),
add it into graphdiyne powder, and mix evenly.
) Add the mixed powder obtained in the step 4) into a polytetrafluoroethylene ball
milling kettle, add zirconia balls according to the mass ratio of materials to zirconia balls
of 1:100-500, and ball mill for 3-5 h under the condition that the rotating speed is 500
1500 rpm to obtain precursor powder of the graphdiyne-based composite piezoelectric
catalytic material.
6) Put the precursor powder into a tube furnace, activate it at 300-500°C for 2-5 h in N2
atmosphere, and naturally cool it to room temperature.
7) Collect the cooled powder, wash the powder with deionized water to neutrality, and
dry the powder at 120°C for 5-24 h to obtain the graphdiyne-based composite
piezoelectric catalyst product.
8) Weigh 0.01-0.5 g of graphdiyne-based composite piezoelectric catalyst powder, and
put it in a piezoelectric catalytic system to test its piezoelectric catalytic performance.
The specific operation is as follows. Weigh 0.01-0.5 g of graphdiyne-based composite piezoelectric catalyst powder, add it into a pollutant water sample with a volume of 20-80 mL, introduce mechanical force to stimulate piezoelectric catalytic reaction for 0.01-2 h, and centrifuge the sample to obtain the supernatant for determining the concentration of the target pollutants.
9) The catalyst powder obtained by centrifugation is washed with deionized water for 3-5
times, dried at 120°C for 5-24 h, added into the piezoelectric catalytic reaction system,
and the piezoelectric catalytic reaction process in steps 6-7 is repeated, and the
repeatability of the catalyst sample is measured.
The phenyl-hexahalide can be one or two or more iron salts of hexachlorobenzene,
hexabromobenzene and hexaiodobenzene.
The piezoelectric material precursor can be the precursor corresponding to the
preparation of MoS2, WS2, MoSe2, WSe2, ZnO, BiTiO3, CdS, BaTiO3, Pb(Zr 0.52 Ti 0.48
)03, piezoelectric fibers and piezoelectric ceramics.
The mechanical force initiation method applied by the piezoelectric catalytic reaction
system can be one or more composite methods of providing mechanical force, such as
ball milling method, ultrasonic method, stirring method, air flow method and water flow
method.
Graphdiyne is a new type of two-dimensional carbon material in recent years, which has
the advantages of fast electron transmission, multi-level channels and many ion channels.
It is an excellent structural regulator and has obvious piezoelectric response, but the
research on its piezoelectric properties is still relatively few. Compared with other
technologies, the invention has the advantages as follows. (1) The graphdiyne-based composite piezoelectric catalyst provided by the invention has simple operation flow, low cost and easy batch production. (2) The graphdiyne-based piezoelectric catalytic material synthesized by the invention has obvious friction response, and can realize in-situ piezoelectric catalysis and active site repair by an in-situ ball milling method. (3) The piezoelectric catalytic material prepared by the invention has both long service life and high catalytic activity, and can meet the requirements of environmental engineering application.
Figure 1 A transmission electron microscope photograph of graphdiyne-based WS2
composite material prepared by the present invention
Figure 2 The effect of different mechanical activation methods on piezoelectric properties
of graphdiyne-based WS2 composite material
Figure 3 A repetitive experimental result of the piezoelectric catalytic degradation of
phenol by the graphdiyne-based MoS2 material prepared by the invention
Figure 4 An effect diagram of rapid piezoelectric catalytic degradation of rhodamine by
the graphdiyne-based Bi4Ti3012 material prepared by the invention
Hereinafter, the specific embodiments of the present invention will be further explained
with reference to the drawings and technical solutions.
Embodiment 1
1) Weigh hexabromobenzene and calcium carbide according to the molar ratio of 1:6, put
them into a 100 mL vacuum polytetrafluoroethylene ball milling reactor, add 50 ml of
ethanol, add 100 g of zirconia balls with a diameter of 4mm as medium, vacuumize the
reactor, and ball mill for 8 h at the rotating speed of 800 rpm.
2) Take out the ball milled powder sample, wash it twice with deionized water and
ethanol in sequence, and dry it at 90°C for 10 h to obtain thin layer graphdiyne powder.
3) Weigh tungsten dioxide, thiourea and sodium hydroxide according to the molar ratio
of 1: 10: 0.1, and put them into a 100 mL polytetrafluoroethylene ball milling reactor.
4) Weigh 0.2 g of graphdiyne powder obtained in step 2), add it into the reactor in step 3),
and ball mill for 3 h under the condition of 800 rpm to obtain precursor powder of
graphdiyne-based composite piezoelectric catalytic material.
) Put the precursor powder obtained in step 4) into a tube furnace, activate it at 450°C
for 2 h in N2 atmosphere, and naturally cool it to room temperature.
6) Collect the cooled powder, wash it with deionized water to neutrality, and dry it at
120°C for 10 h to obtain the graphdiyne-based composite piezoelectric catalyst product.
The transmission electron microscope characterization results are shown in Figure 1.
7) Respectively measure three 50 mL water samples containing 100 mg/L tetracycline,
numbered 1, 2 and 3, and add 0.05 g of graphdiyne-based composite piezoelectric
catalyst powder into the three groups of samples, wherein the No.1 system is placed in a
polytetrafluoroethylene ball milling reactor, ball milled for 60 min under the condition of
rotating speed of 1000 r/min, and centrifuged to obtain the supernatant for determining
the tetracycline concentration. The No.2 system is placed in a beaker, and after ultrasonic treatment at 200 HZ for 60 min, it is centrifuged to obtain the supernatant for determining the concentration of tetracycline. The No.3 system is placed in a beaker, magnetically stirred for 60 min at 1000 rpm, and centrifuged to obtain the supernatant for determining the concentration of tetracycline. See Figure 2 for the comparison of the removal effects of the three groups of samples.
8) It can be proved from the transmission electron microscope image in Figure 1 that the
graphdiyne-based WS2 composite material has a thin layer structure, and WS2 grows
along the epitaxial orientation of graphdiyne segment, with about 3-10 layers. It can be
seen from Figure 2 that graphdiyne-based WS2 has different piezoelectric catalytic
activities under different activation modes, and is most sensitive under the action of ball
milling friction, and can remove more than 98% of tetracycline within 60 min.
Embodiment 2
1) Weigh phenyl-hexahalide and calcium carbide according to the molar ratio of 1:8, put
them into a 100 mL vacuum polytetrafluoroethylene ball milling reactor, add 200 g of
zirconia balls with a diameter of 4mm as medium, vacuumize the reactor, and ball mill
for 6 h at the rotating speed of 1000 rpm.
2) Take out the ball milled powder sample, wash it twice with deionized water and
ethanol in sequence, and dry it at 80°C for 6 h to obtain thin layer graphdiyne powder.
3) Weigh ammonium molybdate, thiourea and sodium hydroxide according to the molar
ratio of 1: 8: 0.5, and put them into a 100 mL polytetrafluoroethylene ball milling reactor.
4) Weigh 0.1 g of graphdiyne powder obtained in step 2), add it into the reactor in step 3),
and ball mill for 5 h under the condition of 800 rpm to obtain precursor powder of
graphdiyne-based composite piezoelectric catalytic material.
) Put the precursor powder obtained in step 4) into a tube furnace, activate it at 500°C
for 4 h in N2 atmosphere, and naturally cool it to room temperature.
6) Collect the cooled powder, wash it with deionized water to neutrality, and dry it at
120°C for 8 h to obtain the graphdiyne-based composite piezoelectric catalyst product.
7) Measure 50 mL of water sample containing 100 mg/L phenol, add 0.05 g of
graphdiyne-based composite piezoelectric catalyst powder, put the sample in a
polytetrafluoroethylene ball milling reactor, ball mill for 60 /min under the condition of
rotating speed of 1000 rpm, and centrifuge the sample to obtain the supernatant for
determining the concentration of phenol.
8) The catalyst powder obtained by centrifugation was washed with deionized water for 3
times, dried at 120°C for 5 hours, and the reaction process of piezoelectric catalytic
degradation of phenol in step 7) was repeated for 50 times to obtain the repeatability of
catalyst samples under 50 cycles (Figure 3).
9) It can be seen from Figure 3 that in 50 cycles, the removal rate of phenol by
graphdiyne-based MoS2 is maintained above 95%, which shows that it has high
repeatability and long service life.
Embodiment 3:
1) Weigh phenyl-hexahalide and calcium carbide according to the molar ratio of 1:4, put
them into a 100 mL vacuum polytetrafluoroethylene ball milling reactor, add 200 g of
zirconia balls with a diameter of 6mm as medium, vacuumize the reactor, and ball mill
for 6 h at the rotating speed of 1000 rpm.
2) Remove the ball milled sample, wash with deionized water and ethanol twice in
sequence, and dry to obtain thin layer graphdiyne powder.
3) Weigh Bi(OH)3 and Ti(OH)4 powders according to the molar ratio of 4: 3, and place
them in a 100 mL PTFE ball milling reactor.
4) Weigh 0.5 g of graphdiyne powder obtained in step 2), add it into the reactor in step 3),
and ball mill for 6 h under the condition of 1000 rpm to obtain precursor powder of
graphdiyne-based composite piezoelectric catalytic material.
) Put the precursor powder obtained in step 4) into a tube furnace, activate it at 250°C
for 4 h in N2 atmosphere, and naturally cool it to room temperature.
6) Collect the cooled powder, wash it with deionized water to neutrality, and dry it at
120°C for 10 h to obtain the graphdiyne-based Bi4Ti3 012 composite piezoelectric catalyst
product.
7) Measure 50 mL of water sample containing 100 mg/L rhodamine B, add 0.05 g of
graphdiyne-based composite piezoelectric catalyst powder, put the sample in a
polytetrafluoroethylene ball milling reactor, ball mill for 5 min at the rotating speed of
1000 rpm, centrifuge to take the supernatant to determine the concentration of rhodamine
B, and the removal effect is shown in Figure 4.
8) It can be seen from Figure 4 that the prepared graphdiyne-based Bi4Ti3 012 material
can rapidly degrade rhodamine B under the action of friction, and when the reaction time
is 2 min, the removal rate of rhodamine B is close to 100%.
Claims (1)
- THE CLAIMS DEFINING THE INVENTION ARE AS FOLLOWS:1. A method for preparing and applying a long-life friction-sensitive graphdiyne-basedpiezoelectric material, characterized by comprising the following specific steps:1) taking phenyl-hexahalide and calcium carbide as raw materials, accurately weigh thephenyl-hexahalide and calcium carbide according to the molar ratio of phenyl-hexahalideto calcium carbide of 1: (5-10), and place them in a vacuum polytetrafluoroethylene ballmilling reactor;2) weigh zirconia balls according to the mass ratio of materials to zirconia balls of 1:100500, place them in a reactor, vacuumize the reactor, and ball mill for 6-20 h at therotating speed of 500-1000 rpm;3) collect the ball milled powder, wash it twice with deionized water and ethanol insequence, filter to obtain filter cake, and dry at 50-100°C for 2-10 h to obtain thin layergraphdiyne powder;4) weigh 0.1-1 g graphdiyne powder, weigh piezoelectric material precursor according tothe mass ratio of graphdiyne to piezoelectric catalytic fabric precursor of 1:(50-1000),add it into graphdiyne powder, and mix evenly;) add the mixed powder obtained in the step 4) into a polytetrafluoroethylene ballmilling kettle, add zirconia balls according to the mass ratio of materials to zirconia ballsof 1:100-500, and ball mill for 3-5 h under the condition that the rotating speed is 5001500 rpm to obtain precursor powder of the graphdiyne-based composite piezoelectriccatalytic material;6) put the precursor powder into a tube furnace, activate it at 300-500 0 C for 2-5 h in N2atmosphere, and naturally cool it to room temperature;7) collect the cooled powder, wash the powder with deionized water to neutrality, and drythe powder at 1200 C for 5-24 h to obtain the graphdiyne-based composite piezoelectriccatalyst product;8) weigh 0.01-0.5 g of graphdiyne-based composite piezoelectric catalyst powder,determine the concentrationperformance; the specific operation is as follows: weigh 0.010.5 g of graphdiyne-based composite piezoelectric catalyst powder, add it into a pollutantwater sample with a volume of 20-80 mL, introduce mechanical force to stimulatepiezoelectric catalytic reaction for 0.01-2 h, and centrifuge the sample to obtain thesupernatant for determining the concentration of the target pollutants;9) the catalyst powder obtained by centrifugation is washed with deionized water for 3-5times, dried at 1200 C for 5-24 h, added into the piezoelectric catalytic reaction system,and the piezoelectric catalytic reaction process in steps 6-7 is repeated, and therepeatability of the catalyst sample is measured.2. The method according to claim 1, characterized in that the phenyl-hexahalide in step 1)can be one or a mixture of two or more of hexachlorobenzene, hexabromobenzene andhexaiodobenzene.3. The method according to claim 1, characterized in that the piezoelectric materialprecursor can be a reactant corresponding to the preparation of MoS2, WS2, MoSe2,WSe2, ZnO, BiTiO3, CdS, BaTiO3, Pb(Zr 0.52 Ti 0.48 )03, piezoelectric fibers andpiezoelectric ceramics.4. The method according to claim 1, characterized in that the mass ratio of the graphdiyneto the piezoelectric material precursor in step 4) is controlled to be 1:50-1:1000.5. The method according to claim 1, characterized in that the mass ratio of materials usedin the ball milling method in step 5) to zirconia balls is 1:100-1:500.6. The method according to claim 1, characterized in that the mechanical force initiationmethod applied by the piezoelectric catalytic reaction system in step 8) can be one ormore composite methods of providing mechanical force, such as ball milling method,ultrasonic method, stirring method, air flow method and water flow method.
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| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN114229828A (en) * | 2021-11-24 | 2022-03-25 | 上海工程技术大学 | Preparation method of gamma-graphite monoalkyne |
| CN114436244A (en) * | 2021-12-06 | 2022-05-06 | 中国地质大学（武汉） | Preparation method of graphite diyne |
| CN114751373A (en) * | 2022-04-15 | 2022-07-15 | 山东大学 | Mechanical catalysis method for preparing hydrogen and carbon by cracking methane |
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Cited By (5)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN114229828A (en) * | 2021-11-24 | 2022-03-25 | 上海工程技术大学 | Preparation method of gamma-graphite monoalkyne |
| CN114436244A (en) * | 2021-12-06 | 2022-05-06 | 中国地质大学（武汉） | Preparation method of graphite diyne |
| CN114436244B (en) * | 2021-12-06 | 2023-10-17 | 中国地质大学（武汉） | Preparation method of graphite diyne |
| CN114751373A (en) * | 2022-04-15 | 2022-07-15 | 山东大学 | Mechanical catalysis method for preparing hydrogen and carbon by cracking methane |
| CN114751373B (en) * | 2022-04-15 | 2023-10-27 | 山东大学 | Mechanocatalytic method for preparing hydrogen and carbon by methane pyrolysis |
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