CN109574104A - A kind of bimetallic wind resistance wave type lock phosphate material and its preparation method and application - Google Patents
A kind of bimetallic wind resistance wave type lock phosphate material and its preparation method and application Download PDFInfo
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- CN109574104A CN109574104A CN201811492485.5A CN201811492485A CN109574104A CN 109574104 A CN109574104 A CN 109574104A CN 201811492485 A CN201811492485 A CN 201811492485A CN 109574104 A CN109574104 A CN 109574104A
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- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F1/00—Treatment of water, waste water, or sewage
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- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F11/00—Treatment of sludge; Devices therefor
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- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F11/00—Treatment of sludge; Devices therefor
- C02F11/008—Sludge treatment by fixation or solidification
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- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2101/00—Nature of the contaminant
- C02F2101/10—Inorganic compounds
- C02F2101/105—Phosphorus compounds
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- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2101/00—Nature of the contaminant
- C02F2101/30—Organic compounds
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- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2103/00—Nature of the water, waste water, sewage or sludge to be treated
- C02F2103/007—Contaminated open waterways, rivers, lakes or ponds
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- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2209/00—Controlling or monitoring parameters in water treatment
- C02F2209/06—Controlling or monitoring parameters in water treatment pH
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- Environmental & Geological Engineering (AREA)
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- Water Treatment By Sorption (AREA)
Abstract
The present invention discloses a kind of bimetallic wind resistance wave type lock phosphate material, be prepared by the following method: high-temperature heat treatment obtains semi-finished product after powdered dolomite attapulgite clay is granulated, then the semi-finished product are immersed in the mixed solution of lanthanum chloride and aluminium chloride and is loaded, stabilization processes are carried out in low temperature later, lock phosphate material after cleaning, drying up to the bimetallic wind resistance wave type.It is big that the material consolidates phosphate capacity, has significant capacity of anti-storm, and the lanthanum aluminium element being able to achieve in different water environment pH value variations consolidates phosphorus power and energy, to realize comprehensive phosphate fixation ability.The material draw materials extensive, cheap, Nantural non-toxic and ecological security it is higher, have broad application prospects.
Description
Technical field
The invention belongs to technical field of water pollution treatment, it is related to a kind of bimetallic wind resistance wave type lock phosphate material and its preparation side
Method and application.
Background technique
Lake eutrophication has become global water environmental problems.By being greater than 10km to 1382Lake survey
It was found that 85.4% lake is in eutrophic state, and there is 40.1% lake to be in serious rice-nutrient state.Therefore, urgently
The concentration that corresponding measure to be taken administers polluted water body and repaired, and control phosphorus in lake is considered as lake Fu Ying
The key that feedingization is administered.But correlative study shows after lake external source phosphorus is polluted and is effectively controlled, water body in lake eutrophy
Change still sustainable decades.Lay the blame on its reason, be there is " interior ghost " in lake, i.e., lake endogenous phosphorus release is to lead to lake Fu Ying
The main reason for feedingization is continued.Therefore, controlling lake endogenous phosphorus pollution is considered as that improvement lake eutrophication sample is simultaneous
Standby method.
Mainly there are Sediment Dredging, water plant to repair the traditional control method of lake endogenous phosphorus pollution, water body aeration
And in-situ chemical passivation based on molysite, aluminium salt and calcium salt etc..Comparatively, in-situ chemical passivation is in the world for lake
It moors Endogenous Phosphorus control and uses a kind of more mode.Its based on principle be to be thrown to the seriously polluted region of bed mud (deposit) phosphorus
Add the chemical substances such as aluminium salt (aluminum sulfate, aluminium chloride), molysite and calcium salt, sedimentary phosphate is by forming stabilization with aluminium, iron and calcium
Phosphorus reference state is to achieve the purpose that Internal phosphorus controls.Compared with molysite, aluminium salt due to not influenced by oxidation-reduction potential,
And it more applies in the control of bottom mud in lake phosphorus.Although however, aluminium salt lake endogenous phosphorus control achieve preferable effect,
But its there is also huge disputes.The reason is that the use of aluminium salt is to the requirement with higher of the pH value of water body.In the low lake of alkalinity
In pool (pH < 5.5), Al (OH)3Flocculate can be dissolved into Al3+, toxicity then is generated to water body fish and zoobenthos.In alkalinity
In lake (pH > 8), and the solid phosphorus efficiency of aluminium salt is also due to the competition of hydroxyl reduces.Further, since sediments re-suspension acts on
It can cause aluminium (Al3+) released from the bed mud of passivation, to endanger water body.
The in-situ passivation that lake endogenous phosphorus discharges is controlled to have obtained more and more passes based on lanthanum, aluminium, the modified clay of calcium
Note and application.However, natural clay generally all has, low to the adsorption capacity of phosphorus, effect is poor, influences (such as pH vulnerable to extraneous factor
Value) the shortcomings that.Therefore necessary modification must be carried out to it, but method of modifying must be simple and easy, not will increase material then in this way
The cost of material.Currently, occur it is numerous using clay as the lake endogenous phosphor passivation agent of modified material, such as lanthanum modified alta-mud
(English name Phoslock), ferroso-ferric oxide or magnesium-modified diatomite etc..Wherein with the sub- federal science in Australia and industrial organization
(Commonwealth Scientific and Industrial Research Organisation (CSIR O)) invention
Phoslock is most widely used, lake endogenous using showing that it can significantly be controlled in numerous lakes of the U.S. with Europe
The release of phosphorus, effectively control Lake Eutrophication.This is mainly due to lanthanum can be formed with the easily-activated state phosphorus of bed mud it is stable
Lanthanum orthophosphate precipitating, the type compound voluminosity is lower, not readily dissolves.However, under the organic interference of high concentration, then it can shadow
Ring the solid phosphorus efficiency of lanthanum.In addition, causing every square kilometre of lake treatment since its cost of manufacture is higher (1.5 ~ 20,000 yuan/ton)
Expense is up to more than millions of, this is greatly limited the product in developing country's popularization.Further, since
Phoslock can dissolve rapidly in aqueous solution and in suspended state, easily suspend, and it is frequent to be unsuitable for China's wave disturbance
Shallow water eutrophic lake in use.
The clay mineral of calcic, as dolomite concave convex rod has been found to have certain adsorption effect, Gao Wenre to phosphorus
Processing can be obviously improved its adsorption effectiveness to phosphorus, and material duct is abundant after heat treatment, be easy to utilize aluminium, iron isoreactivity gold
Belong to element to be loaded.After Overheating Treatment, quality is hard for particulate form or the rich calcium attapulgite clay of granulation, and it is insoluble to meet water
Solution has stronger capacity of anti-storm.But since solid phosphate capacity is still lower, endogenous seriously polluted sedimentary phosphate can not be carried out
Persistently control.
Summary of the invention
The present invention is seriously polluted for above-mentioned lake endogenous phosphorus, and sustained release causes serious water eutrophication problem,
It is proposed a kind of solution that the eutrophic lake based on Internal phosphorus passivation is administered.The lock being prepared by this method
Phosphate material is able to solve current sedimentary phosphate passivator generally existing easy suspension, wind and wave resistance disturbance, and is unable to satisfy in pH higher
Eutrophication alkalinity water body keep persistently control phosphorus effect the problem of.This method utilizes the dolomite attapulgite clay of Natural Rich Calcium
Particulate form crushing is carried out for raw material or is directly granulated, and heat treatment is carried out to semifinished material and prepares a kind of calcium aluminium with activity load
Compound sedimentary phosphate passivator, the preparation method is simple, low in cost, can be applied to control life or trade effluent, eutrophy
Change the release of phosphorus in water body and polluted bed mud, effectively control and alleviation water body eutrophication degree.
To achieve the above object, the technical solution adopted in the present invention is as follows:
A kind of bimetallic wind resistance wave type lock phosphate material, is prepared by the following method:
High-temperature heat treatment obtains semi-finished product after powdered dolomite attapulgite clay is granulated, then by the semi-finished product
It immerses in the mixed solution of lanthanum chloride and aluminium chloride and is loaded, carry out stabilization processes in low temperature later, after cleaning, drying i.e.
It obtains the bimetallic wind resistance wave type and locks phosphate material.
The present invention uses dolomite attapulgite clay for raw material, makes inertia therein by the method for high-temperature heat treatment first
Calcium is activated, and enhances it to phosphorus fixation ability, while expand material internal duct, then passes through lanthanum aluminium complex salt
Solution carries out load and forms calcium-aluminium-lanthanum compound material, to obtain high capacity phosphor-curing agent, the material is in water body and bed mud
Source phosphorus has preferable control effect.
Further, the method for the granulation are as follows: attapulgite is granulated with rotary drum granulator, adopts water as granulating agent,
Partial size is 1 ~ 2mm.
Further, the temperature of the high-temperature heat treatment is 600 ~ 800 DEG C, preferably 700 DEG C.
Further, the time of the high-temperature heat treatment is 2h.
Further, in the dolomite attapulgite clay, the mass content of concave convex rod is 30~50%, the matter of dolomite
Measuring content is 10~30%.
Further, the powdered dolomite attapulgite clay is glued by the dolomite concave convex rod of irregular particle state
What native or using powder preparation rounded bulbous dolomite attapulgite clay semi-finished product obtained after being mechanically pulverized, being sieved.
Further, in the mixed solution, the molar ratio of aluminium ion and lanthanum ion is 5 ~ 12.5:1, preferably 10:1.
Further, in the mixed solution, aluminum ions concentration is preferably 2 mol/L, and the concentration of lanthanum ion is preferably
0.2 mol/L。
Further, the mass ratio of the semi-finished product and the mixed solution is 1:2 ~ 3, preferably 1:2.5.
Further, the load is to stand later for 24 hours in 23 ~ 27 DEG C of sufficiently oscillation 1h.
Further, the condition of low temperature stabilization processing are as follows: be cooled to after placing 24 h in 50 ~ 90 DEG C of conditions
Room temperature.
Further, the cleaning detects to adopt to be washed with deionized to no chloride ion.
Above-mentioned bimetallic wind resistance wave type lock phosphate material can be applied to sanitary sewage, industrial wastewater and eutrophication water bottom
The control of mud Endogenous Phosphorus.
Bimetallic wind resistance wave type of the present invention locks phosphate material, is that can adsorb phosphorus and control sedimentary phosphate in overlying water
The passivator of release, can be also used for sanitary sewage, in industrial wastewater and eutrophication water phosphorus removal, and can make
For the filler of artificial Wetland Substrate.The material is the solid granule for being not dissolved in water, therefore has significant capacity of anti-storm,
And the lanthanum aluminium element being able to achieve in different water environment pH value variations consolidates phosphorus power and energy, to realize comprehensive phosphate fixation ability.It should
Bimetallic wind resistance wave type lock phosphate material can be used for the control of internal phosphorus release in shallow lake, alleviate water body eutrophication degree.
Due to the solid dirty performance not influence vulnerable to the variation of oxidation-reduction potential of aluminium, and lanthanide material to bed mud active phosphorus have compared with
Good control effect has significant advantage compared with iron and iron series substance modification material, not only can control in aerobic bed mud
Phosphorus, it can also be used to control the phosphorus in anaerobic bottom mud.Due to attapulgite material extensive, the cheap, Nantural non-toxic of materials and life
State safety is higher, therefore prepared material has broad application prospects.
Detailed description of the invention
Fig. 1 is that bimetallic obtained lock phosphate material removes water systems'phosphorus under different lanthanums, aluminium and lanthanum aluminium combination load concentration
Except effect contrast figure.
Fig. 2 is influence comparison diagram of the pH value to bimetallic lock phosphate material phosphor-removing effect.
Fig. 3 is removal effect of the bimetallic lock phosphate material to various concentration phosphorus-containing wastewater.
Fig. 4 is the control effect comparison diagram that bimetallic lock phosphate material discharges sedimentary phosphate.
Fig. 5 is control effect comparison diagram of the bimetallic lock phosphate material to bed mud active phosphorus.
Fig. 6 is bimetallic lock phosphate material wind and wave resistance performance comparison figure.
Specific embodiment
Technical solutions according to the invention are further described in detail below by specific embodiment, but it is necessary to
It points out that following embodiment is served only for the description to summary of the invention, does not constitute a limitation on the scope of protection of the present invention.In embodiment
Used dolomite concave convex rod is derived from the main place of production Xuyi Jiangsu of China's concave convex rod, but for the raw ore place of production and no requirement (NR), fits
When dolomite concave convex rod raw ore, composition in concave convex rod mass content be 30~50%, dolomite mass content be 10~
30%.
Embodiment 1
The dolomite attapulgite of pulverulence is used into drum granulating, uses water as granulating agent (partial size is 1 ~ 2mm), concave
The mass content of convex stick is 30%, and the mass content of dolomite is 10%.The dolomite attapulgite clay for being granulated and completing is taken, is passed through
High-temperature calcination stove is in 700 DEG C of 2 h of calcining.The Aluminium chloride hexahydrate for weighing certain mass is settled to 100 mL, is configured to 1mol/L
Liquor alumini chloridi, 2 mol/L liquor alumini chloridis, 0.1mol/L lanthanum chloride solution, 0.2mol/L lanthanum chloride solution, 0.3mol/L chlorine
Change lanthanum solution, 2 mol/L aluminium chloride and 0.1mol/L lanthanum chloride mixed solution, 2 mol/L aluminium chloride and 0.2mol/L lanthanum chloride
Mixed solution, 2 mol/L aluminium chloride and 0.3mol/L lanthanum chloride mixed solution and 2 mol/L aluminium chloride and 0.4mol/L chlorination
Lanthanum mixed solution.Material Jing Guo high-temperature calcination is added in above-mentioned each solution according to the ratio of water and soil mass ratio 1:2.5, is set
In shaking table, after sufficiently oscillation (160rpm) is reacted 1 hour in 23 DEG C, one day is stood at room temperature, discards supernatant liquid later, it will
Material 90 DEG C of 24 h of aging in an oven of lanthanum aluminium load, are cooled to room temperature, and material is finally washed to supernatant clarification, drying
Agent obtains the bimetallic lock phosphate material of different lanthanum aluminium load capacity afterwards.The material 0.5g for weighing above-mentioned preparation is in 50ml concentration
In the phosphorus solution of 100mgP/L and 400 mg/L, after sufficiently reaction 24 hours, the concentration of phosphorus is measured, the adsorbance of phosphorus is calculated and goes
Except efficiency, and then determine best lanthanum aluminium loading concentrations.Result of study is as shown in Figure 1, the bimetallic-modified dephosphorization of aluminium lanthanum combination is imitated
Fruit will be noticeably greater than the phosphor-removing effect of monometallic (aluminium or lanthanum).
It weighs and phosphate material is locked by the bimetallic loaded in 2 mol/L aluminium chloride and 0.2mol/L lanthanum chloride mixed solution
(the bimetallic lock phosphate material for calling best lanthanum aluminium load in the following text) 0.5 g passes through acid in the phosphorus solution of 10 mg/L and 100 mg/L
It is 4-11 that alkali, which adjusts phosphorus solution pH value range, and after reacting 24 hours in constant-temperature table (revolving speed 160rpm), centrifugal filtration is surveyed
Determine phosphorus content, calculates the phosphorus ligands efficiency under different pH condition, as a result as shown in Figure 2.
Weigh bimetallic lock 0.5 g of phosphate material of best lanthanum aluminium load in the phosphorus-containing wastewater of various concentration (pH=
7) after, reacting 24 hours in constant-temperature table (revolving speed 160rpm), centrifugal filtration measures phosphorus content, and the removal efficiency of phosphorus is such as
Shown in Fig. 3.
Using columnar sampler, acquires several no less than the column heavily contaminated bed mud (internal diameter 8cm) of 15cm, overlying waters and keep
10cm.The bed mud of 3 pillar surface layer 0-5cm is uniformly mixed, active phosphorus in part bed mud analysis bed mud is taken (to mention according to P form
The weakly stable state phosphorus that takes, iron phosphorus and the sum of organic phosphorus) content.Consolidate phosphate capacity according to material maximum and 0-5cm bed mud in surface layer is living
Property phosphorus content the material of certain mass is uniformly sent out in above-mentioned according to the theoretical dosages (2x) of theoretical dosage (1x) and 2 times
Column shaped deposit surface, while the space management of material is not added in setting.All column bed muds are placed in constant temperature water bath apparatus,
124 days (aerobic state 34 days, anaerobic state 90 days) is cultivated, and analyzes the content of titanium pigment in overlying water, bimetallic locks phosphorus
The control phosphorus efficiency of material is as shown in Figure 4.
It obtains phosphorus polluted bed mud to analyze bed mud P form using P form analysis method, by the title of certain mass
It takes the bimetallic lock phosphate material of best lanthanum aluminium load to be added in polluted bed mud and (adds maximal absorptive capacity and bottom of the dosage according to material
The ratio calculation of active phosphorus in mud), after 2 months, compare material processing with not plus material processing in active phosphorus (weakly stable state phosphorus,
Iron phosphorus and the sum of organic phosphorus) content, calculate and weigh the bimetallic lock phosphate material of best lanthanum aluminium load bed mud active phosphorus is cut
Decrement and percentage, as a result as shown in Figure 5.
Using columnar sampler, several no less than column heavily contaminated bed muds (internal diameter 8cm) of 15cm are acquired in Taihu Lake, are above covered
Water keeps 10cm.The bed mud of 3 pillar surface layer 0-5cm is uniformly mixed, take part bed mud analysis bed mud in active phosphorus (according to phosphorus
Weakly stable state phosphorus that form is extracted, iron phosphorus and the sum of organic phosphorus) content.Consolidate phosphate capacity and surface layer 0-5cm according to material maximum
The bimetallic lock phosphate material for weighing best lanthanum aluminium load of certain mass is uniformly sprinkling upon the table of bed mud by the content of bed mud active phosphorus
Face, while aluminium salt (aluminum sulfate) processing control is set, according to international standard, the amount for adding aluminium is 50 g/m2.According in the past too
Apoplexy and strong wind forcing frequency is arranged in the research experience in lake, and every kind of landscape disturb 3 times, and disturbance terminates each place of post analysis every time
The concentration of concentration of suspension, dissolved phosphorus acid group and total phosphorus in reason in overlying water.The result shows that bimetallic lock phosphate material tool
There is stronger wind and wave resistance disturbance ability, and can effectively cut down the concentration of dissolved phosphorus acid group and total phosphorus in water body.
Embodiment 2
The dolomite attapulgite of pulverulence is used into drum granulating, uses water as granulating agent (partial size is 1 ~ 2mm), concave
The mass content of convex stick is 40%, and the mass content of dolomite is 30%.The dolomite attapulgite clay for being granulated and completing is taken, is passed through
High-temperature calcination stove is in 800 DEG C of 2 h of calcining.The Aluminium chloride hexahydrate for weighing certain mass is settled to 100 mL, is configured to 2 mol/
L aluminium chloride and 0.16mol/L lanthanum chloride mixed solution.By the material Jing Guo high-temperature calcination according to the ratio of water and soil mass ratio 1:3
It is added in each above-mentioned mixed solution, is placed in shaking table, it is quiet at room temperature after in 27 DEG C, sufficiently oscillation (160rpm) is reacted 1 hour
It sets one day, discards supernatant liquid later, the material that lanthanum aluminium is loaded 70 DEG C of 24 h of aging in an oven are cooled to room temperature, finally
Material is washed to supernatant clarification, agent obtains bimetallic lock phosphate material after drying.
Embodiment 3
The dolomite attapulgite of pulverulence is used into drum granulating, uses water as granulating agent (partial size is 1 ~ 2mm), concave
The mass content of convex stick is 50%, and the mass content of dolomite is 20%.The dolomite attapulgite clay for being granulated and completing is taken, is passed through
High-temperature calcination stove is in 600 DEG C of 2 h of calcining.The Aluminium chloride hexahydrate for weighing certain mass is settled to 100 mL, is configured to 2 mol/
L aluminium chloride and 0.2mol/L lanthanum chloride mixed solution.Material Jing Guo high-temperature calcination is added according to the ratio of water and soil mass ratio 1:2
Enter into above-mentioned mixed solution, be placed in shaking table, after sufficiently oscillation (160rpm) is reacted 1 hour in 25 DEG C, stands one at room temperature
It, discards supernatant liquid later, and the material that lanthanum aluminium is loaded 50 DEG C of 24 h of aging in an oven are cooled to room temperature, finally by material
Material is washed to supernatant clarification, and agent obtains bimetallic lock phosphate material after drying.
Claims (10)
1. a kind of bimetallic wind resistance wave type locks phosphate material, which is characterized in that be prepared by the following method:
High-temperature heat treatment obtains semi-finished product after powdered dolomite attapulgite clay is granulated, then by the semi-finished product
It immerses in the mixed solution of lanthanum chloride and aluminium chloride and is loaded, carry out stabilization processes in low temperature later, after cleaning, drying i.e.
It obtains the bimetallic wind resistance wave type and locks phosphate material.
2. bimetallic wind resistance wave type according to claim 1 locks phosphate material, which is characterized in that the temperature of the high-temperature heat treatment
Degree is 600 ~ 800 DEG C, preferably 700 DEG C.
3. bimetallic wind resistance wave type according to claim 1 locks phosphate material, which is characterized in that the high-temperature heat treatment when
Between be 2h.
4. bimetallic wind resistance wave type according to claim 1 locks phosphate material, which is characterized in that the dolomite concave convex rod is viscous
In soil, the mass content of concave convex rod is 30~50%, and the mass content of dolomite is 10~30%.
5. bimetallic wind resistance wave type according to claim 1 locks phosphate material, which is characterized in that in the mixed solution, aluminium
The molar ratio of ion and lanthanum ion is 5 ~ 12.5:1, preferably 10:1.
6. bimetallic wind resistance wave type locks phosphate material according to claim 1 or 5, which is characterized in that the mixed solution
In, aluminum ions concentration is 2 mol/L, and the concentration of lanthanum ion is 0.2 mol/L.
7. bimetallic wind resistance wave type according to claim 1 locks phosphate material, which is characterized in that the semi-finished product are mixed with described
The mass ratio for closing solution is 1:2 ~ 3, preferably 1:2.5.
8. bimetallic wind resistance wave type according to claim 1 locks phosphate material, which is characterized in that the load be in 23 ~
27 DEG C of sufficiently oscillation 1h, stand for 24 hours later.
9. bimetallic wind resistance wave type according to claim 1 locks phosphate material, which is characterized in that the low temperature stabilization
The condition of processing are as follows: be cooled to room temperature after placing 24 h in 50 ~ 90 DEG C of conditions.
10. any bimetallic wind resistance wave type lock phosphate material of claim 1-9 is in the control of eutrophication Internal phosphorus
Application.
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| CN113426402A (en) * | 2021-07-01 | 2021-09-24 | 王彦达 | Preparation method and application of lanthanum-aluminum multi-element composite mineral phosphorus removal material |
| CN113426402B (en) * | 2021-07-01 | 2022-10-25 | 王彦达 | Preparation method and application of lanthanum-aluminum multi-element composite mineral phosphorus removal material |
| CN116371353A (en) * | 2023-04-06 | 2023-07-04 | 广东工业大学 | Lanthanum magnetic iron modified attapulgite phosphorus removal adsorbent and application thereof |
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