CN101913674B - Method for removing phosphorus in water by adopting aluminum salt modified eggshell - Google Patents
Method for removing phosphorus in water by adopting aluminum salt modified eggshell Download PDFInfo
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- CN101913674B CN101913674B CN2010102448160A CN201010244816A CN101913674B CN 101913674 B CN101913674 B CN 101913674B CN 2010102448160 A CN2010102448160 A CN 2010102448160A CN 201010244816 A CN201010244816 A CN 201010244816A CN 101913674 B CN101913674 B CN 101913674B
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- eggshell
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- aluminum salt
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- shell meal
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- 102000002322 Egg Proteins Human genes 0.000 title claims abstract description 89
- 108010000912 Egg Proteins Proteins 0.000 title claims abstract description 89
- 210000003278 egg shell Anatomy 0.000 title claims abstract description 86
- OAICVXFJPJFONN-UHFFFAOYSA-N Phosphorus Chemical compound [P] OAICVXFJPJFONN-UHFFFAOYSA-N 0.000 title claims abstract description 61
- 229910052698 phosphorus Inorganic materials 0.000 title claims abstract description 60
- 239000011574 phosphorus Substances 0.000 title claims abstract description 60
- 238000000034 method Methods 0.000 title claims abstract description 38
- AZDRQVAHHNSJOQ-UHFFFAOYSA-N alumane Chemical class [AlH3] AZDRQVAHHNSJOQ-UHFFFAOYSA-N 0.000 title claims abstract description 22
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 title claims abstract description 20
- 230000004048 modification Effects 0.000 claims abstract description 35
- 238000012986 modification Methods 0.000 claims abstract description 35
- 239000000243 solution Substances 0.000 claims abstract description 21
- 238000001179 sorption measurement Methods 0.000 claims abstract description 14
- 239000000843 powder Substances 0.000 claims abstract description 8
- 238000003756 stirring Methods 0.000 claims abstract description 8
- 238000001914 filtration Methods 0.000 claims abstract description 6
- 239000012528 membrane Substances 0.000 claims abstract description 6
- 239000012266 salt solution Substances 0.000 claims abstract description 5
- 239000000126 substance Substances 0.000 claims abstract description 5
- 235000012054 meals Nutrition 0.000 claims description 38
- 159000000013 aluminium salts Chemical class 0.000 claims description 15
- 229910000329 aluminium sulfate Inorganic materials 0.000 claims description 15
- 229910019142 PO4 Inorganic materials 0.000 claims description 9
- 239000010452 phosphate Substances 0.000 claims description 9
- NBIIXXVUZAFLBC-UHFFFAOYSA-K phosphate Chemical compound [O-]P([O-])([O-])=O NBIIXXVUZAFLBC-UHFFFAOYSA-K 0.000 claims description 9
- VSCWAEJMTAWNJL-UHFFFAOYSA-K aluminium trichloride Chemical compound Cl[Al](Cl)Cl VSCWAEJMTAWNJL-UHFFFAOYSA-K 0.000 claims description 4
- 241000287828 Gallus gallus Species 0.000 claims description 3
- 239000000203 mixture Substances 0.000 claims description 3
- 210000004681 ovum Anatomy 0.000 claims description 3
- 239000002245 particle Substances 0.000 claims description 3
- 230000003068 static effect Effects 0.000 claims description 3
- DIZPMCHEQGEION-UHFFFAOYSA-H aluminium sulfate (anhydrous) Chemical compound [Al+3].[Al+3].[O-]S([O-])(=O)=O.[O-]S([O-])(=O)=O.[O-]S([O-])(=O)=O DIZPMCHEQGEION-UHFFFAOYSA-H 0.000 claims description 2
- 238000007781 pre-processing Methods 0.000 claims description 2
- BHEPBYXIRTUNPN-UHFFFAOYSA-N hydridophosphorus(.) (triplet) Chemical compound [PH] BHEPBYXIRTUNPN-UHFFFAOYSA-N 0.000 claims 1
- 238000005259 measurement Methods 0.000 claims 1
- 239000010865 sewage Substances 0.000 abstract description 2
- 239000002699 waste material Substances 0.000 abstract description 2
- 238000001035 drying Methods 0.000 abstract 1
- 238000002156 mixing Methods 0.000 abstract 1
- 238000007873 sieving Methods 0.000 abstract 1
- 230000000274 adsorptive effect Effects 0.000 description 17
- 230000000694 effects Effects 0.000 description 13
- 238000010521 absorption reaction Methods 0.000 description 6
- 239000002351 wastewater Substances 0.000 description 5
- HEMHJVSKTPXQMS-UHFFFAOYSA-M Sodium hydroxide Chemical compound [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 description 3
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 3
- 229910052782 aluminium Inorganic materials 0.000 description 3
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 description 2
- 229910021536 Zeolite Inorganic materials 0.000 description 2
- 239000004411 aluminium Substances 0.000 description 2
- 239000002585 base Substances 0.000 description 2
- 230000015271 coagulation Effects 0.000 description 2
- 238000005345 coagulation Methods 0.000 description 2
- HNPSIPDUKPIQMN-UHFFFAOYSA-N dioxosilane;oxo(oxoalumanyloxy)alumane Chemical compound O=[Si]=O.O=[Al]O[Al]=O HNPSIPDUKPIQMN-UHFFFAOYSA-N 0.000 description 2
- 238000005516 engineering process Methods 0.000 description 2
- 238000012851 eutrophication Methods 0.000 description 2
- 239000000706 filtrate Substances 0.000 description 2
- 239000000463 material Substances 0.000 description 2
- 238000002203 pretreatment Methods 0.000 description 2
- 239000010457 zeolite Substances 0.000 description 2
- 241000195493 Cryptophyta Species 0.000 description 1
- WYWFMUBFNXLFJK-UHFFFAOYSA-N [Mo].[Sb] Chemical compound [Mo].[Sb] WYWFMUBFNXLFJK-UHFFFAOYSA-N 0.000 description 1
- 238000004458 analytical method Methods 0.000 description 1
- 230000001458 anti-acid effect Effects 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 238000010170 biological method Methods 0.000 description 1
- 230000037396 body weight Effects 0.000 description 1
- 239000000701 coagulant Substances 0.000 description 1
- 238000003795 desorption Methods 0.000 description 1
- 238000011026 diafiltration Methods 0.000 description 1
- 239000012153 distilled water Substances 0.000 description 1
- 238000002474 experimental method Methods 0.000 description 1
- 239000002440 industrial waste Substances 0.000 description 1
- 150000002500 ions Chemical class 0.000 description 1
- 229910052742 iron Inorganic materials 0.000 description 1
- 235000012204 lemonade/lime carbonate Nutrition 0.000 description 1
- 239000007788 liquid Substances 0.000 description 1
- 238000004519 manufacturing process Methods 0.000 description 1
- 239000002893 slag Substances 0.000 description 1
- 239000002594 sorbent Substances 0.000 description 1
- 238000002798 spectrophotometry method Methods 0.000 description 1
- 239000007858 starting material Substances 0.000 description 1
- 230000002195 synergetic effect Effects 0.000 description 1
Landscapes
- Water Treatment By Sorption (AREA)
- Solid-Sorbent Or Filter-Aiding Compositions (AREA)
Abstract
The invention discloses a method for removing phosphorus in water by adopting an aluminum salt modified eggshell, belonging to the field of phosphoric sewage treatment. The method comprises the following steps of: waste eggshell modification: mixing 0.1-0.4mol/L of aluminum salt solution with pretreated eggshell powder at the temperature of 20-60 DEG C to lead the ratio of the amount of substance of aluminum salt to the mass of the eggshell powder is 0.001-0.0015mol/g, and then carrying out continuous stirring; stirring for 24h and then filtering, and drying at the temperature of 100-105 DEG C, and sieving by 100 meshes to obtain modified eggshell powder; putting the modified eggshell powder in a dryer for later use; and modified eggshell adsorption: adding 0.1-1g of modified eggshell powder to 100mL phosphoric solution with the concentration of 0.2-50mg (P)/L and the pH of 3-10, carrying out constant temperature shaking at the temperature of 10-40 DEG C at the speed of 50-200r/min; and filtering with a 0.45mum filter membrane after 10min-6h.
Description
One, technical field
The present invention relates to a kind of method that adopts aluminum salt modified eggshell to remove phosphorus in the water, belong to the process field of phosphorus-containing wastewater.
Two, background technology
Frequent day by day mankind's activity the phosphor resource that can directly utilize is constantly reduced, and the phosphorus concentration in the water bodys such as rivers and lakes is in continuous increase.The phosphorus that water body weight increases is constantly grown organism such as algae, causes body eutrophication.Body eutrophication to Human's production life influence greatly, therefore produced the technology and method of various dephosphorization, but these methods all have shortcoming more or less, and this makes and seek efficiently, cleans, cheap phosphorus removal method becomes a focus of water treatment already.
The phosphorus treatment process is varied in the water, the biological method non-secondary pollution, but stable water outlet is relatively poor, and also responsive to outside atmosphere.Chemical dephosphorization mainly comprises Coagulation Method and absorption method.Coagulation Method has treatment effect preferably to phosphorus, but consequent refuse can't be recycled.Absorption method also has treatment effect preferably to phosphorus, and the waste residue that adsorption process produces can also be reused by desorption process.In absorption method, it is crucial selecting phosphorus to remove ability sorbent material strong, with low cost.Active aluminum, zeolite be because of having bigger specific surface area, obligate absorption, advantage such as porous and being widely used, but insufficient be that these prices of raw and semifnished materials are higher, and zeolite is difficult to resolve and analyses phosphorus.Scum as industrial waste is cheap, also demonstrates phosphorus treatment effect preferably in secular practice, but in the water treatment procedure, the use meeting of scrap iron slag stripping harmful ion in water forms secondary pollution.
Three, summary of the invention
In order to improve the removal ability of discarded eggshell to phosphorus in the waste water, the invention provides a kind of method that adopts aluminum salt modified eggshell to remove phosphorus in the water, eggshell after its modification has that phosphor-removing effect is good, cost is inexpensive, the source is abundant, advantages of simple operation, and this method has a good application prospect.
Technical scheme of the present invention is as follows:
A kind of method that adopts aluminum salt modified eggshell to remove phosphorus in the water, this method may further comprise the steps:
The modifying process of eggshell is as follows:
Under 20-60 ℃, mix the 0.1-0.4mol/L aluminum salt solution with through pretreated egg-shell meal, making the amount of substance of aluminium salt and the mass ratio of egg-shell meal is 0.001-0.0015mol/g, continues stirring subsequently; Stir the 24h after-filtration, dry under 100-105 ℃, cross 100 mesh sieves, get the modification egg-shell meal, it is standby to put into moisture eliminator.
The dephosphorization process of modification eggshell is as follows:
The above-mentioned modification egg-shell meal of 0.1-1g added in the 100mL solution containing phosphate that concentration is 0.2-50mg (P)/L carry out Static Adsorption, the pH of solution is 3-10, is to carry out the constant temperature vibration with the speed of 50-200r/min under 10-40 ℃ in temperature; Cross 0.45 μ m filter membrane behind the 10min-6h.
Used aluminum salt solution is chosen with Tai-Ace S 150 or liquor alumini chloridi.
The preprocessing process of eggshell is as follows: the discarded eggshell that will reclaim cleans, and removes inner membrance.Behind the dry eggshell, grind, cross 100 mesh sieves; Particle diameter is dried down at 102-105 ℃ less than 100 purpose Ovum crusta Gallus domesticus powder, and it is standby to put into moisture eliminator.
The main component of discarded eggshell is a lime carbonate, and its wide material sources the phosphorus in the water body is had certain removal ability, but its adsorptive capacity are relatively low.Aluminium salt pair phosphorus has better removal effect, and the source is abundant, cheap.Utilize aluminum salt modified eggshell, aluminium salt is coated in eggshell surface, can increase the aluminium base active sites of eggshell surface, improves the electrostatic force of eggshell surface to phosphorus.The present invention is in the hope of improving the dephosphorization ability of eggshell by be coupled discarded eggshell and aluminium salt.
Present method mainly is to utilize aluminium salt to come modified abandoned egg-shell meal, and aluminium salt is coated in eggshell surface, can increase the aluminium base active sites of eggshell surface, improves the electrostatic force of eggshell surface to phosphorus.Compare characteristics such as present method has the phosphorus removal effect significantly and stable, and the starting material source is abundant, and secondary pollution risk and running cost are low with the treatment process of phosphorus in the waste water that generally adopts at present.
Beneficial effect of the present invention:
(1) the present invention adopts aluminum salt modified discarded egg-shell meal to have good phosphorus and removes ability, its phosphorus adsorptive capacity is increased to 4.28mg (P)/g by 0.3064mg (the P)/g of original unmodified egg-shell meal, adsorptive capacity has improved more than ten times, and realizes the comprehensive utilization of discarded eggshell and the resource utilization of phosphorus.
(2) the present invention adopts aluminum salt modified egg-shell meal to be fit to apply to have stronger antiacid impact capacity in the environment that pH is 3-10.
Four, embodiment:
Embodiment 1
Adopt aluminum salt modified eggshell to remove the method for phosphorus in the water, this method may further comprise the steps:
1, discarded eggshell pre-treatment:
The discarded eggshell that reclaims is cleaned, remove inner membrance.Behind the dry eggshell, grind, cross 100 mesh sieves.Particle diameter is dried down at 105 ℃ less than 100 purpose Ovum crusta Gallus domesticus powder, and it is standby to put into moisture eliminator.
2, discarded eggshell modification:
In temperature is under 25 ℃, to the 0.25mol/L of 20mL AlCl
3Solution adds the good egg-shell meal of 4g pre-treatment and it is stirred.The 24h after-filtration, and use the distilled water diafiltration.Put into baking oven at last, dry under 105 ℃, cross 100 mesh sieves.
3, the dephosphorization of modification eggshell:
With the modification egg-shell meal adding concentration of 0.1g is in the 100mL solution containing phosphate of 15mg (P)/L, and the pH that regulates phosphorus liquid with NaOH solution is 7, is that the speed with 150r/min is carried out isothermal vibration under 25 ℃ in temperature.Cross 0.45 μ m filter membrane behind the 2h.With the phosphorus concentration in the molybdenum-antimony anti-spectrophotometric method survey filtrate, the phosphorus adsorptive capacity of modification egg-shell meal is 4.28mg (P)/g.
Embodiment 2
Substantially the same manner as Example 1, AlCl only
3Solution changes 60 ℃ into to the modification temperature of discarded eggshell, and the phosphorus adsorptive capacity of modification egg-shell meal is 4.20mg (P)/g.
Embodiment 3
Substantially the same manner as Example 1, the 0.4mol/L Al of employing 12.5mL
2(SO
4)
3Solution carries out modification to discarded eggshell, and the phosphorus adsorptive capacity of modification egg-shell meal is 4.23mg (P)/g.
Embodiment 4
In the solution containing phosphate of 100mL 15mg (P)/L, add aluminum chloride as coagulating agent (among consumption and the embodiment 1 during the eggshell modification aluminium salt 0.000125mol of the equivalent that consumes)).Record finally that phosphorus concentration drops to 14.89mg (P)/L from 15mg (P)/L in the 100mL phosphorus solution, show that aluminum salt under this condition is not clearly to the removal ability of phosphorus, effect far is inferior to aluminum salt modified eggshell.
Embodiment 5
The egg-shell meal of 1g is added 100mL, and to contain phosphorus concentration be that 15mg (P)/L, pH is in 7 the sewage, being 100 rev/mins with rotating speed under 25 ℃ temperature stirred 8 hours, carry out Static Adsorption, after absorption finishes, filter through 0.45 μ m filter membrane, recording egg-shell meal is 0.3064mg (P)/g to the adsorptive capacity of phosphorus.Even the concentration of phosphorus continues to increase in the solution in follow-up experiment, its adsorptive capacity does not have bigger variation yet.
By embodiment 1,2,3,5 as can be seen, the modification of aluminium salt has improved the adsorption effect of discarded egg-shell meal to phosphorus greatly, and its phosphorus adsorptive capacity has increased tens of times.
By embodiment 1,4,5 as can be seen, the modification egg-shell meal is removed the phosphorus removal effect sum of effect far above the modification aluminum salt and the natural egg-shell meal of equivalent to phosphorus in the water, so the removal effect to phosphorus in the waste water shows significant synergistic effect after the discarded eggshell modification of aluminium salt pair.
Embodiment 6
Among the embodiment 1, other conditions are constant, and the concentration of phosphorus changes 5mg (P)/L in the waste water, 10mg (P)/L, and the phosphorus adsorptive capacity of modification egg-shell meal is respectively 2.79,3.49mg (P)/g.
Embodiment 7
Among the embodiment 1, other conditions are constant, and the concentration of phosphorus changes 5mg (P)/L in the solution, and when adsorption time is 10min, the phosphorus adsorptive capacity of modification egg-shell meal is 1.90mg (P)/g; When adsorption time is 30min, the phosphorus adsorptive capacity of modification egg-shell meal is 2.25mg (P)/g.
Embodiment 8
Among the embodiment 1, other conditions are constant.When adsorption temp is 40 ℃.The phosphorus adsorptive capacity of modification egg-shell meal is 7.81mg (P)/g.When adsorption temp is 10 ℃.The phosphorus adsorptive capacity that records the modification egg-shell meal is 3.60mg (P)/g.
By embodiment 1 and 8 as can be seen, along with adsorption temp raises, the modification egg-shell meal is good more to the adsorption effect of phosphorus.
Embodiment 9
Among the embodiment 1, other conditions are constant, and the concentration of phosphorus is 5mg (P)/L in the solution, and when solution containing phosphate pH was 3, the phosphorus adsorptive capacity of modification egg-shell meal was 4.42mg (P)/g; When solution containing phosphate pH was 7, the phosphorus adsorptive capacity of modification egg-shell meal was 4.01mg (P)/g; When solution containing phosphate pH was 10, the phosphorus adsorptive capacity of modification egg-shell meal was 3.12mg (P)/g.
Embodiment 10
The present invention to the modification mode of natural egg-shell meal is: under 20-60 ℃, mix the 0.1-0.4mol/L aluminum salt solution with through pretreated egg-shell meal, making the amount of substance of aluminium salt and the mass ratio of egg-shell meal is 0.001-0.0015mol/g, continues stirring subsequently; Stir the 24h after-filtration, dry under 100-105 ℃, cross 100 mesh sieves, get the modification egg-shell meal, it is standby to put into moisture eliminator.
Utilize the method for modification egg-shell meal absorption phosphorus: with the modification egg-shell meal adding concentration of 0.1-1g is in the 100mL solution containing phosphate of 0.2-50mg (P)/L, and the pH of solution is 3-10, is to carry out the constant temperature vibration with the speed of 50-200r/min under 10-40 ℃ in temperature.Cross 0.45 μ m filter membrane behind the 10min-6h.Survey the phosphorus concentration in the filtrate at last.
Wherein, when 1. adopting the aluminium salt pair to discard the egg-shell meal modification, modification temperature is any numerical value in 20-60 ℃, for example 20 ℃, 25 ℃, 60 ℃ etc., the aluminium salt concn is any numerical value among the 0.1-0.4mol/L, for example 0.1,0.2,0.25,0.4 etc., and aluminium salt comprises Al
2(SO
4)
3, AlCl
3Deng.2. the starting point concentration of solution containing phosphate can be any numerical value among 0.2-50mg (P)/g, for example 0.2mg (P)/g, 0.6mg (P)/g, 3mg (P)/g, 15mg (P)/g, 30mg (P)/g, 50mg (P)/g etc.PH can make any numerical value among the 3-10, for example, and 3,7,9 etc.Adsorption temp can be 10 ℃, 20 ℃, 30 ℃, 40 ℃ etc., and adsorption time can be 10min, 30min, 1h, 2h, 6h etc.
Claims (3)
1. method that adopts aluminum salt modified eggshell to remove phosphorus in the water, it is characterized in that: this method may further comprise the steps:
Modifying process:
Under 20-60 ℃, mix the 0.1-0.4mol/L aluminum salt solution with through pretreated egg-shell meal, making the amount of substance of aluminium salt and the mass ratio of egg-shell meal is 0.001-0.0015mol/g, continues stirring subsequently; Stir the 24h after-filtration, dry under 100-105 ℃, cross 100 mesh sieves, get the modification egg-shell meal, it is standby to put into moisture eliminator;
The dephosphorization process:
The above-mentioned modification egg-shell meal of 0.1-1g added in the 100mL solution containing phosphate that concentration is 0.2-50mg/L carry out Static Adsorption, this concentration is with phosphorous concentration measurement, the pH of solution is 3-10, is to carry out the constant temperature vibration with the speed of 50-200r/min under 10-40 ℃ in temperature; Cross 0.45 μ m filter membrane behind the 10min-6h.
2. remove the method for phosphorus in the water according to the aluminum salt modified eggshell of the described employing of claim 1, it is characterized in that: described aluminium salt is chosen with Tai-Ace S 150 or aluminum chloride.
3. according to the method for phosphorus in claim 1 or the aluminum salt modified eggshell removal of the 2 described employings water, it is characterized in that: the preprocessing process of described eggshell is as follows: the discarded eggshell that will reclaim cleans, and removes inner membrance; Behind the dry eggshell, grind, cross 100 mesh sieves; Particle diameter is dried down at 102-105 ℃ less than 100 purpose Ovum crusta Gallus domesticus powder, and it is standby to put into moisture eliminator.
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Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN103288164A (en) * | 2013-06-25 | 2013-09-11 | 南京信息工程大学 | A method for synchronous nitrogen and phosphorus removal in sewage by combining modified zeolite and modified eggshell |
Families Citing this family (5)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN102432083B (en) * | 2011-10-28 | 2013-06-05 | 上海海洋大学 | Method for removing and recovering phosphate in waste water |
| CN105056872A (en) * | 2015-05-14 | 2015-11-18 | 苏州科技学院 | Novel calcium aluminum carbonate water purification agent preparation method and phosphorus removal process |
| CN104986837B (en) * | 2015-06-30 | 2017-03-22 | 南京工业大学 | Preparation method of polyaluminium sludge formed phosphorus removal material |
| CN108554372A (en) * | 2018-05-04 | 2018-09-21 | 南京信息工程大学 | The method that phosphorus in water removal is gone using aluminum salt modified clay |
| CN108892197A (en) * | 2018-07-23 | 2018-11-27 | 南京信息工程大学 | A kind of method that aluminum salt modified waste water clod removes phosphorus in water |
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|---|---|---|---|---|
| CN1475520A (en) * | 2002-08-15 | 2004-02-18 | 孙建宁 | Shell micro powder filler and its use |
| CN101058459A (en) * | 2006-04-21 | 2007-10-24 | 韩国科学技术研究院 | Substance for treatment of sewage and waste water, carrier containing the substance and method for preparing the same |
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| NO310716B1 (en) * | 1999-11-26 | 2001-08-20 | Health By Nature As | Means for improving drinking water |
| JP2008545549A (en) * | 2005-05-16 | 2008-12-18 | ジョン、ヨン−キル | Method for partially coating using hologram transfer film, method for producing coating composition, and apparatus used therefor |
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Patent Citations (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN1475520A (en) * | 2002-08-15 | 2004-02-18 | 孙建宁 | Shell micro powder filler and its use |
| CN101058459A (en) * | 2006-04-21 | 2007-10-24 | 韩国科学技术研究院 | Substance for treatment of sewage and waste water, carrier containing the substance and method for preparing the same |
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| Title |
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| JP特表2003-514665A 2003.04.22 |
Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN103288164A (en) * | 2013-06-25 | 2013-09-11 | 南京信息工程大学 | A method for synchronous nitrogen and phosphorus removal in sewage by combining modified zeolite and modified eggshell |
| CN103288164B (en) * | 2013-06-25 | 2015-07-01 | 南京信息工程大学 | A method for synchronous nitrogen and phosphorus removal in sewage by combining modified zeolite and modified eggshell |
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