CN107486231B - A kind of preparation method of graphite phase carbon nitride colloid photochemical catalyst - Google Patents
A kind of preparation method of graphite phase carbon nitride colloid photochemical catalyst Download PDFInfo
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- CN107486231B CN107486231B CN201710733743.3A CN201710733743A CN107486231B CN 107486231 B CN107486231 B CN 107486231B CN 201710733743 A CN201710733743 A CN 201710733743A CN 107486231 B CN107486231 B CN 107486231B
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- JMANVNJQNLATNU-UHFFFAOYSA-N oxalonitrile Chemical compound N#CC#N JMANVNJQNLATNU-UHFFFAOYSA-N 0.000 title claims abstract description 40
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 title claims abstract description 34
- 239000000084 colloidal system Substances 0.000 title claims abstract description 33
- 229910002804 graphite Inorganic materials 0.000 title claims abstract description 21
- 239000010439 graphite Substances 0.000 title claims abstract description 21
- 239000003054 catalyst Substances 0.000 title claims abstract description 19
- 238000002360 preparation method Methods 0.000 title claims abstract description 8
- WCUXLLCKKVVCTQ-UHFFFAOYSA-M Potassium chloride Chemical compound [Cl-].[K+] WCUXLLCKKVVCTQ-UHFFFAOYSA-M 0.000 claims abstract description 26
- 235000011164 potassium chloride Nutrition 0.000 claims abstract description 13
- 239000001103 potassium chloride Substances 0.000 claims abstract description 13
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims abstract description 12
- SOIFLUNRINLCBN-UHFFFAOYSA-N ammonium thiocyanate Chemical compound [NH4+].[S-]C#N SOIFLUNRINLCBN-UHFFFAOYSA-N 0.000 claims abstract description 9
- 238000012719 thermal polymerization Methods 0.000 claims abstract 2
- 239000000843 powder Substances 0.000 claims description 29
- 239000007787 solid Substances 0.000 claims description 26
- 238000000034 method Methods 0.000 claims description 9
- 230000001699 photocatalysis Effects 0.000 claims description 8
- 238000007146 photocatalysis Methods 0.000 claims description 7
- 239000012298 atmosphere Substances 0.000 claims description 4
- 238000000502 dialysis Methods 0.000 claims description 4
- 239000002243 precursor Substances 0.000 claims description 4
- 239000003795 chemical substances by application Substances 0.000 claims description 3
- 229910021383 artificial graphite Inorganic materials 0.000 claims 1
- VIKNJXKGJWUCNN-XGXHKTLJSA-N norethisterone Chemical compound O=C1CC[C@@H]2[C@H]3CC[C@](C)([C@](CC4)(O)C#C)[C@@H]4[C@@H]3CCC2=C1 VIKNJXKGJWUCNN-XGXHKTLJSA-N 0.000 claims 1
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 abstract description 9
- 239000001257 hydrogen Substances 0.000 abstract description 9
- 229910052739 hydrogen Inorganic materials 0.000 abstract description 9
- 239000000463 material Substances 0.000 abstract description 9
- 238000006555 catalytic reaction Methods 0.000 abstract description 5
- 238000004519 manufacturing process Methods 0.000 abstract description 5
- 238000003786 synthesis reaction Methods 0.000 abstract description 4
- 230000015572 biosynthetic process Effects 0.000 abstract description 3
- 238000005286 illumination Methods 0.000 abstract 1
- 230000003287 optical effect Effects 0.000 abstract 1
- 229910052799 carbon Inorganic materials 0.000 description 13
- 239000011941 photocatalyst Substances 0.000 description 11
- 238000001816 cooling Methods 0.000 description 6
- 238000000634 powder X-ray diffraction Methods 0.000 description 4
- 238000005033 Fourier transform infrared spectroscopy Methods 0.000 description 3
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 description 3
- 239000007864 aqueous solution Substances 0.000 description 3
- 238000006243 chemical reaction Methods 0.000 description 3
- 239000006185 dispersion Substances 0.000 description 3
- 230000000694 effects Effects 0.000 description 3
- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 description 2
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 description 2
- 239000012300 argon atmosphere Substances 0.000 description 2
- 230000005540 biological transmission Effects 0.000 description 2
- 238000001354 calcination Methods 0.000 description 2
- 238000000354 decomposition reaction Methods 0.000 description 2
- 239000000126 substance Substances 0.000 description 2
- 229910052719 titanium Inorganic materials 0.000 description 2
- 239000010936 titanium Substances 0.000 description 2
- -1 Cyano Chemical group 0.000 description 1
- 241000790917 Dioxys <bee> Species 0.000 description 1
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Natural products CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 description 1
- 229910002621 H2PtCl6 Inorganic materials 0.000 description 1
- ZLMJMSJWJFRBEC-UHFFFAOYSA-N Potassium Chemical compound [K] ZLMJMSJWJFRBEC-UHFFFAOYSA-N 0.000 description 1
- 150000001412 amines Chemical class 0.000 description 1
- 229910002092 carbon dioxide Inorganic materials 0.000 description 1
- 239000001569 carbon dioxide Substances 0.000 description 1
- 239000003153 chemical reaction reagent Substances 0.000 description 1
- 238000001246 colloidal dispersion Methods 0.000 description 1
- 239000013078 crystal Substances 0.000 description 1
- 230000008021 deposition Effects 0.000 description 1
- 238000010586 diagram Methods 0.000 description 1
- 238000005265 energy consumption Methods 0.000 description 1
- 235000019441 ethanol Nutrition 0.000 description 1
- PCHJSUWPFVWCPO-UHFFFAOYSA-N gold Chemical compound [Au] PCHJSUWPFVWCPO-UHFFFAOYSA-N 0.000 description 1
- 239000010931 gold Substances 0.000 description 1
- 229910052737 gold Inorganic materials 0.000 description 1
- 125000000623 heterocyclic group Chemical group 0.000 description 1
- 238000011065 in-situ storage Methods 0.000 description 1
- 230000004298 light response Effects 0.000 description 1
- 239000007788 liquid Substances 0.000 description 1
- 239000000203 mixture Substances 0.000 description 1
- 239000002105 nanoparticle Substances 0.000 description 1
- 238000006303 photolysis reaction Methods 0.000 description 1
- 230000015843 photosynthesis, light reaction Effects 0.000 description 1
- 125000004193 piperazinyl group Chemical group 0.000 description 1
- 239000002861 polymer material Substances 0.000 description 1
- 229910052700 potassium Inorganic materials 0.000 description 1
- 239000011591 potassium Substances 0.000 description 1
- 230000005855 radiation Effects 0.000 description 1
- 230000029058 respiratory gaseous exchange Effects 0.000 description 1
- 239000004575 stone Substances 0.000 description 1
- 239000010409 thin film Substances 0.000 description 1
- 229910052724 xenon Inorganic materials 0.000 description 1
- FHNFHKCVQCLJFQ-UHFFFAOYSA-N xenon atom Chemical compound [Xe] FHNFHKCVQCLJFQ-UHFFFAOYSA-N 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
- B01J27/24—Nitrogen 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
- B01J35/39—Photocatalytic properties
-
- 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
- B01J35/50—Catalysts, in general, characterised by their form or physical properties characterised by their shape or configuration
-
- 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
- B01J37/00—Processes, in general, for preparing catalysts; Processes, in general, for activation of catalysts
- B01J37/08—Heat treatment
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B3/00—Hydrogen; Gaseous mixtures containing hydrogen; Separation of hydrogen from mixtures containing it; Purification of hydrogen
- C01B3/02—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen
- C01B3/04—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by decomposition of inorganic compounds, e.g. ammonia
- C01B3/042—Decomposition of water
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
- C01B2203/10—Catalysts for performing the hydrogen forming reactions
- C01B2203/1041—Composition of the catalyst
- C01B2203/1088—Non-supported catalysts
-
- Y—GENERAL 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
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/30—Hydrogen technology
- Y02E60/36—Hydrogen production from non-carbon containing sources, e.g. by water electrolysis
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- Chemical & Material Sciences (AREA)
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- Engineering & Computer Science (AREA)
- Materials Engineering (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Physics & Mathematics (AREA)
- Thermal Sciences (AREA)
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- General Health & Medical Sciences (AREA)
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Abstract
The present invention relates to a kind of preparation methods of graphite phase carbon nitride colloid photochemical catalyst, belong to catalysis material technical field.The synthesis of the graphite phase carbon nitride is with ammonium thiocyanate, and potassium chloride is predecessor, is obtained by a step thermal polymerization.Graphite phase carbon nitride prepared by the present invention good can be dispersed in water, and form colloid, and keep stable, compared with traditional body phase carbon nitride, special chemistry and optical property are shown, there are stronger absorbing properties, show good Photocatalyzed Hydrogen Production performance under visible light illumination.The present invention has synthesized novel material and has improved preparation process, with important application prospects.
Description
Technical field
The invention belongs to catalysis material technical fields, and in particular to a kind of system of graphite phase carbon nitride colloid photochemical catalyst
Preparation Method and purposes.
Background technique
It is a kind of more uniform mixture that colloid, which is also known as colloidal dispersion system, containing there are two types of the objects of different conditions in colloid
Matter, a kind of dispersed phase, another continuous phase.Dispersion system of colloid is multiphase since degree of scatter is higher, is widely used
Material, catalysis, sensing, in terms of, therefore colloidal materials have great importance.In recent years, more and more
Colloid catalyst is used in photocatalysis field.It is wherein colloidal tio 2 material than more typical example.However dioxy
Changing titanium colloidal materials only has ultraviolet light response, and contains Titanium, is unfavorable for large-scale application.Therefore suitable non-gold is found
Belong to the key problem that colloid catalysis material is the development of colloid photochemical catalyst.
In recent years, graphite phase carbon nitride semiconductive polymer material is as a kind of metal-free photochemical catalyst, due to it
Visible light absorbing, and there is good physical and chemical stability, therefore the extensive concern (Nat. by researcher
Mater. 2009,8,76).Graphite phase carbon nitride material photolysis water hydrogen (ACS Catalysis. 2016,6,
3921), photocatalysis carbon dioxide conversion (Angew. Chem. Int. Ed. 2017,56,6627) and photocatalysis are organic
Synthesis (J. Am. Chem. Soc. 2010,132,16299) etc. has a wide range of applications.But since it is
Body phase substance disperses the problems such as uneven, constrains the raising of its photocatalysis performance there is not dissolving.Then it is desirable to
Synthesis nitridation carbon colloid improves its photocatalytic activity.In addition, nitridation carbon colloid has extensively in the manufacture of thin-film device etc.
General application prospect.Therefore, we use ammonium thiocyanate and potassium chloride to synthesize carbon nitride photocatalyst for presoma.Test table
Bright: the carbon nitride photocatalyst that this method prepares good can be dispersed in water, and form colloid, and keep stable, and
The carbon nitride photocatalyst shows good visible light and produces hydrogen activity.
Summary of the invention
The present invention relates to a kind of preparation methods of graphite phase carbon nitride colloid photochemical catalyst.Carbonitride light prepared by the present invention
Catalyst good can be dispersed in water to form colloid, and keep stable.It is insoluble to solve conventional bulk phase carbon nitride, dispersion
The problems such as uneven, can be realized efficient photocatalysis Decomposition aquatic products hydrogen reaction.
To achieve the above object, the present invention adopts the following technical scheme:
A kind of graphite phase carbon nitride colloid photochemical catalyst is dissolved in water and forms colloid, which has apparent elecrtonegativity, energy
Enough it is stabilized.
A method of preparing graphite phase carbon nitride colloid photochemical catalyst as described above, comprising the following steps:
(1) two kinds of precursors of potassium chloride, ammonium thiocyanate that mass ratio is 1:50 are uniformly mixed；
(2) solid sample is obtained after the solid powder that step (1) obtains being calcined 600 DEG C in air atmosphere；
(3) add water to remove remaining potassium chloride the solid powder that step (2) obtains, liquid is evaporated, solid powder is obtained
Last sample.；
(4) by step (3) obtains 20 milligrams of solid powder be dissolved in 100 milliliters of water, obtain nitridation carbon colloid.
Remarkable advantage of the invention is:
(1) the nitridation carbon colloid photochemical catalyst prepared by the present invention has good dispersion in aqueous solution, has simultaneously
Higher Photocatalyzed Hydrogen Production activity is a kind of novel photochemical catalyst.
(2) entire production process of the invention is simply easily with control, and low energy consumption, at low cost, and meeting actual production needs
It wants, is conducive to promote on a large scale.
Detailed description of the invention
Fig. 1 is X-ray powder diffraction (XRD) figure of the resulting graphite phase carbon nitride of embodiment 2.
Fig. 2 is Fourier transform infrared spectroscopy (FT-IR) figure of the resulting graphite phase carbon nitride of embodiment 2.
Fig. 3 is Zeta potential (Zeta potential) figure of the resulting nitridation carbon colloid of embodiment 3.
Fig. 4 is scanning electron microscope (SEM) figure of the resulting graphite phase carbon nitride photochemical catalyst of embodiment 2.
Fig. 5 is scanning electron microscope (SEM) figure of the resulting nitridation carbon colloid of embodiment 3.
Fig. 6 is transmission electron microscope (TEM) figure of the resulting carbonitride solid powder of embodiment 3.
Fig. 7 is the activity figure of the photocatalysis Decomposition aquatic products hydrogen of the resulting graphite phase carbon nitride photochemical catalyst of embodiment 2:
A indicates prepared graphite phase carbon nitride colloid；B indicates traditional body phase carbon nitride.
Specific embodiment
It is several embodiments of the present invention below, further illustrates the present invention, but the present invention is not limited only to this.
Embodiment 1
The potassium chloride and ammonium thiocyanate that mass ratio is 1:50 are weighed first, are uniformly mixed and are evaporated molten in aqueous solution
Agent.Uniformly mixed solid powder is placed into alumina crucible, calcines 12 under the conditions of argon atmosphere, temperature are 600 DEG C
Hour.Sample is taken out after natural cooling to be ground into powder.Sample is taken out after natural cooling to be ground into powder.Pass through dialysis
Method removes remaining potassium chloride, and dialysate is evaporated, carbon nitride photocatalyst solid powder is obtained.The solid powder is dissolved in
Water to get to nitridation carbon colloid.
Embodiment 2
The potassium chloride and ammonium thiocyanate that mass ratio is 1:50 are weighed first, and ground and mixed is uniform.Ground and mixed is uniform
Solid powder is placed into alumina crucible, is calcined 12 hours under the conditions of air atmosphere, temperature are 600 DEG C.After natural cooling
Sample is taken out to be ground into powder.Sample is taken out after natural cooling to be ground into powder.It is removed by the method for dialysis remaining
Dialysate is evaporated by potassium chloride, obtains carbon nitride photocatalyst solid powder.The solid powder is dissolved in water to get nitridation is arrived
Carbon colloid.
Embodiment 3
The potassium chloride and ammonium thiocyanate that mass ratio is 1:50 are weighed first, and ground and mixed is uniform.Ground and mixed is uniform
Solid powder is placed into alumina crucible, is calcined 12 hours under the conditions of argon atmosphere, temperature are 600 DEG C.After natural cooling
Sample is taken out to be ground into powder.Sample is taken out after natural cooling to be ground into powder.It is removed by the method for dialysis remaining
Dialysate is evaporated by potassium chloride, obtains carbon nitride photocatalyst solid powder.The solid powder is dissolved in water to get nitridation is arrived
Carbon colloid.
Fig. 1 is the XRD diagram of the resulting carbon nitride photocatalyst solid powder of embodiment 2.It can be found that carbonitride from figure
Solid powder is 8.1oWith 27.5oThere are two XRD for significantly belonging to graphite phase carbon nitride (100) and (002) crystal face in place
Diffraction maximum, it was demonstrated that the product of preparation is graphite phase carbon nitride.
Fig. 2 is that the FT-IR of the resulting carbon nitride photocatalyst solid powder of embodiment 2 schemes.The bright carbonitride light of the chart is urged
The successful synthesis of agent.800 cm in figure-1With 1200 ~ 1600 cm-1The signal in section corresponds respectively to the breathing vibration of piperazine ring
With armaticity CN heterocycle stretching vibration.In 2170 cm-1Cyano of the neighbouring signals assignment in sample, 980 cm-1Neighbouring
Signal is potassium and NC2The vibration of key.
Fig. 3 is the Zeta potential figure of the resulting nitridation carbon colloid of embodiment 3.As can be seen from the figure nitridation carbon colloid is band
There is apparent elecrtonegativity.
Fig. 4 is the scanning electron microscope (SEM) photograph of the resulting carbon nitride photocatalyst solid powder of embodiment 2.As can be seen from the figure stone
Black phase carbon nitride sample stacked in the form of sheets, and have part cavernous structure.
Fig. 5 is the scanning electron microscope (SEM) photograph of the resulting nitridation carbon colloid of embodiment 3.As can be seen from the figure nitridation carbon colloid is in water
In be separated into nano particle.
Fig. 6 is transmission electron microscope (TEM) figure of the resulting carbonitride solid powder of embodiment 2.As can be seen from the figure graphite
Phase carbon nitride sample stacked in the form of sheets, and apparent lattice fringe can be observed.
Fig. 7 is the property of the resulting carbon nitride photocatalyst of embodiment 2 and body phase carbon nitride photochemical catalyzing hydrogen making
Figure can be compared.50mg carbon nitride photocatalyst solid powder is dispersed in 100 mL reaction reagents (tri- ethyl alcohol containing 10 vol. %
The aqueous solution of amine, uses H2PtCl6Light deposition Pt in situ, i.e. 3 wt. % Pt), using being reacted in upper illuminated reactor.
From figure it can be found that using this method prepare photochemical catalyst under the conditions of radiation of visible light (xenon lamp 300W, cut out tab λ >
420 nm) hydrogen-producing speed reach 282 μm of ol/h, calcine and obtain at 600 DEG C as precursor with ammonium thiocyanate is used alone
Body phase carbon nitride photochemical catalyst (25 μm of ol/h) compare, hydrogen-producing speed improves 11 times.
The foregoing is merely presently preferred embodiments of the present invention, all precursor dosages done according to scope of the present invention patent
The variation of ratio, calcination temperature and time and calcination atmosphere, is all covered by the present invention.
Claims (1)
1. a kind of preparation method of graphite phase carbon nitride colloid photochemical catalyst, it is characterised in that: use ammonium thiocyanate and potassium chloride
As presoma, pass through a step thermal polymerization method synthetic graphite phase carbon nitride photochemical catalyst；The following steps are included:
(1) two kinds of precursors of potassium chloride, ammonium thiocyanate that mass ratio is 1:50 are uniformly mixed；
(2) solid sample is obtained after the solid powder that step (1) obtains being calcined 600 DEG C under the conditions of air atmosphere；
(3) solid powder for obtaining step (2) removes remaining potassium chloride by the method for dialysis, and dialysate is evaporated, is obtained
To solid powder sample；
(4) by 20 milligrams of obtained solid sample of step (3), add 100 milli liter of water, form the photocatalysis of graphite phase carbon nitride colloid
Agent.
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| CN109179349A (en) * | 2018-10-08 | 2019-01-11 | 深圳大学 | A kind of Carbon Nitride Crystal and preparation method thereof |
| CN109603876B (en) * | 2018-12-14 | 2022-07-19 | 深圳大学 | Carbon nitride material and preparation method and application thereof |
| CN109603875B (en) * | 2018-12-14 | 2022-05-17 | 深圳大学 | Carbon nitride material and preparation method and application thereof |
| CN109847785A (en) * | 2019-02-25 | 2019-06-07 | 牟富书 | A kind of preparation method nitrogenizing carbon colloid |
| CN109833895A (en) * | 2019-03-28 | 2019-06-04 | 南昌航空大学 | A kind of preparation method for the heterogeneous class Fenton photochemical catalyst of alkalization class graphite phase carbon nitride modified with visible light-responded manganese metal |
| CN114558606B (en) * | 2022-02-28 | 2023-07-25 | 中国科学院西北生态环境资源研究院 | Catalyst for extracting and separating uranium from uranium-containing wastewater or seawater and application of catalyst |
| CN115025803B (en) * | 2022-06-29 | 2024-01-09 | 安徽大学 | Cyano modified carbon nitride and preparation method and application thereof |
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