CN105621609B - A kind of autotrophic microbe denitrification method removes nitrate material in water removal - Google Patents
A kind of autotrophic microbe denitrification method removes nitrate material in water removal Download PDFInfo
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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
- C02F3/00—Biological treatment of water, waste water, or sewage
- C02F3/28—Anaerobic digestion processes
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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
- C02F3/00—Biological treatment of water, waste water, or sewage
- C02F3/34—Biological treatment of water, waste water, or sewage characterised by the microorganisms used
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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
- C02F2305/00—Use of specific compounds during water treatment
- C02F2305/06—Nutrients for stimulating the growth of microorganisms
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Abstract
The present invention relates to microbial method water-treatment technology fields, specifically disclose a kind of autotrophic microbe denitrification method and remove nitrate material and preparation method thereof in water removal.The material is graininess；Contain elemental sulfur and calcium carbonate in the material, the mass ratio of the elemental sulfur and calcium carbonate is 1.25：1~3.0：1.The material is by elemental sulfur and calcium carbonate composite molding in granular materials, rough surface, conducive to the attachment of microorganism, disposable addition provides electron donor sulphur, inorganic carbon source and the buffer for adjusting basicity using while for microorganism, make reaction continue efficiently to carry out, the nitrate in water is made all to be converted into harmless nitrogen, the removal efficiency of nitrate is high, it is easy to use it is not necessary that additive is additionally added；Nitrate and NH are practically free of using the underground water after material processing of the present invention4 +- N reaches national drinking water standard.Preparation method of the present invention, easy to operate, easily controllable, finished product stablizes easily transport, is suitable for industrial application.
Description
Technical field
The present invention relates to microbial method water-treatment technology fields, and in particular to a kind of microorganism denitrification removes nitric acid in water removal
Salt material and preparation method thereof.
Background technology
Underground water is a kind of freshwater resources being of great rarity, and is used as drinking water source, is widely used in countries in the world.
In the U.S., there are about 50% city dweller with 90% rural resident using underground water as drinking water source.In China, many north
The drinking water source in city is underground water.However, along with the gradually expansion of the rapid industrial development in our country and Process of Urbanization Construction,
The pollution problem getting worse of underground water.Groundwater monitoring that national 200 cities in 2011 carry out the result shows that, 55% city
City's underground water receives different degrees of pollution, and many of which Urban Underground water pollution has the tendency that aggravating year by year.Rural area
Generally make drinking water using phreatic water, and the pollution of area source of the formation such as fertilizer and pesticide, sewage irrigation is excessively used, causes very
The underground water in more areas is by different degrees of azotate pollution.The pollution problem of nitrate causes the extensive concern of society,
And have the tendency that deteriorating year by year, the groundwater azotate in some areas is at concentrations up to 100mg NO3 --N/L.Drink high nitrate
The underground water of content can cause damages to human health, and nitrate is to the harm of human body mainly since it is reduced in human body
Caused by nitrite, the saliva that this reduction is happened at any age bracket human body neutralizes and is less than three months babies'
In alimentary canal.Nitrite can lead to methemoglobinemia and induce kinds cancer, in larger dose also to human vas
There are harmful effects with cardiovascular system for nerve.Harm in view of nitrate to human body, countries in the world are to the nitric acid in drinking water
Salinity has formulated standard value, and water standard is 50mg NO as defined in the World Health Organization3 -- N/L, China is from July, 2007
The standards for drinking water quality (GB 5749-2006) implemented is acted also by the highest limit value of nitrate from original 20mg NO3 --
N/L is down to 10mg NO3 --N/L。
Currently, conventional nitrate removal technology includes physical processing techniques, chemical treatment method and biologic treating technique.
Physical includes ion-exchange, reverse osmosis membrane and electrodialysis embrane method etc..The cardinal principle of ion-exchange processing is to utilize
Chloride or carbonate in anion exchange resin carry out ion exchange with nitrate, to remove the nitrate in water removal.Its
Advantage is easy to operate, efficient, and resin can regenerate, but there are the process problems of regeneration liquid waste, and be unsuitable for scale
Larger azotate pollution problem.Reverse osmosis membrane forces other ion rejections such as nitrate outside film using impressed pressure, water
Molecule reaches the removal of nitrate by reverse osmosis membrane.Reverse osmosis membrane technical maturity, high treating effect, but can not select
Selecting property leaves the ion beneficial to human body.Electroosmose process is intake using selective ion exchange membrane as medium in the work of DC electric field
Under, nitrate is separated from water by film, and into high concentration brine side, light, dense two Room ion concentration difference is increased to reach
The purpose of separation.The removal efficiency of electroosmose process is high, but concentrate need to be further processed, cause this method in application by
Certain limitation.Chemical treatment method mainly utilizes active metal or nonmetallic grade reducing agents by nitrate reduction.It is common living
Bold and vigorous metal includes iron, aluminum and zinc etc., and processing cost is higher, and using being subject to certain restrictions, nonmetal catalyzed reduction method is generally logical
Overweight metallic reducing agent catalysis reduction nitrate, to improve reaction rate and reduce the generation of by-product.Chemical reduction method is anti-
Answer speed fast, it is adaptable, but have a large amount of nitrate transformations be ammonia nitrogen, therefore in drinking water nitrate treatment by
Certain limitation.
Biologic treating technique refers to the denitrification using microorganism, and the nitrate in water is finally reduced to nitrogen
Process.Biological treatment has the characteristics that efficient low-consume, has obtained the extensive concern of scholar at present.It is different according to carbon source needed for bacterium,
Biological denitrification is divided into as heterotrophic denitrification and autotrophic denitrification, and wherein autotrophic denitrification only needs inorganic carbon source, has biological production
Measure that low, sludge quantity is few, the secondary pollution problems without organic carbon source, application prospect is extensive.After autotrophic denitrification is handled, water outlet
Have many advantages, such as that the low water quality of bacterial content is good.In recent years, sulphur autotrophic denitrification technology receives the extensive concern of researchers.So
And as the progress that sulphur autotrophic denitrification reacts, system basicity constantly decline, microbial metabolism is suppressed, and treatment effect is not
It is good.Conventional buffer substance, such as NaHCO3And other effects significantly, but economy is not good enough.Therefore, research and develop it is a kind of it is at low cost,
The highly practical buffer that nitrate water removal is removed suitable for microorganism autotrophic denitrification, to improving microorganism autotrophic denitrification
Method is of crucial importance nitrate treatment effect in water.
Invention content
In order to overcome the deficiencies of existing technologies, the object of the present invention is to provide a kind of autotrophic microbe denitrification methods to go to remove water
Middle nitrate material, the material provide electron donor sulphur and basicity adjusting buffering in autotrophic microbe denitrification process simultaneously
Agent, it is at low cost, it is easy to use, it realizes economical and efficient and safely goes the purpose of nitrate in water removal.
Meanwhile removing nitrate material in water removal the present invention also aims to provide a kind of autotrophic microbe denitrification method
Preparation method.
In order to achieve the goal above, the technical solution adopted in the present invention is：
It is graininess that a kind of autotrophic microbe denitrification method, which removes nitrate material in water removal, the material,；The material
In contain elemental sulfur and calcium carbonate, the mass ratio of the elemental sulfur and calcium carbonate is 1.25：1~3.0：1.
The grain size of the material is 1~5mm.
With in lime stone, egg shell, scallop shell one kind or be arbitrarily combined as raw material, form the carbonic acid in the material
Calcium.It is hard that the elements such as nonmetallic silicon, magnesium metal, potassium, aluminium, the iron contained in lime stone, egg shell, scallop shell simultaneously increase material
While spending, indispensable trace element is also provided for microorganism, is conducive to the progress of microorganism anti-nitration reaction.
Above-mentioned autotrophic microbe denitrification method goes the preparation method of nitrate material in water removal, including following operation step
Suddenly：
1) it takes elemental sulfur to be heated to 105-115 DEG C of melting, obtains liquid sulfur；
2) it takes lime stone, egg shell or scallop shell to be added in liquid sulfur prepared by step 1), obtains mixture, mixture is held
The continuous elemental sulfur being warming up in 120-130 DEG C to mixture melts completely, is uniformly mixed, obtains mixture；
3) mixture prepared by step 2) is cooled to and is solidified as solid material, be crushed to get the autotrophic microbe
Denitrification method removes nitrate material in water removal.
Above-mentioned steps 2) in the mixture fusing point liter obtained after lime stone, egg shell or scallop shell is added in liquid sulfur
Height, is likely to result in liquid sulfur solidification phenomenon, thus it is persistently overheating to 120-130 DEG C to mixture in elemental sulfur it is completely molten again
Melt, and elemental sulfur can be effectively reduced and generate sulphur steam in melting process.
In order to avoid elemental sulfur aoxidizes and volatilizes at high temperature sulphur steam, step 1) and 2) middle useTemperature-gradient methodSide
Formula heats, and specific method is：In step 1) 105-115 DEG C is to slowly warm up to the rate of 5-10 DEG C/min；With 5- in step 2)
The rate of 10 DEG C/min is persistently overheating to 120-130 DEG C.
The lime stone, egg shell or scallop shell are using being preceding broken for 100~200 mesh powder shapes.
Sulphur steam is aoxidized and is volatilized too long in order to avoid elemental sulfur is heated, lime stone described in step 2), egg shell
Or the concrete mode that scallop shell is added in liquid sulfur prepared by step 1) is：By lime stone, egg shell or scallop shell, uniformly paving is spilt
On liquid sulfur surface, and liquid sulfur surface is completely covered.
It is broken for for solid material being broken for the graininess of 1~5mm described in step 3).
Above-mentioned autotrophic microbe denitrification method removes nitrate material in water removal, controls its addition when in use so that
While meeting the theoretical usage amount of sulphur, the pH value of the aqueous solution of the material is added in 7.0 to 8.5 ranges.
Autotrophic microbe denitrification method of the present invention goes in water removal nitrate to go the principle of nitrate in water removal to be with material：
Vulcanize denitrifying microorganism using the elemental sulfur in material, so that nitrate is obtained electronics and be reduced generation nitrogen, Asia
Nitrate or ammonia；Meanwhile hydrogen ion reduction solution basicity is generated with reacting into guild, hinder reaction to carry out afterwards to a certain extent,
And calcium carbonate can be slowly released in material and adjust basicity, make reaction continue efficiently to carry out, the nitrate in water is all converted
For harmless nitrogen, to achieve the purpose that nitrate all removes.Reaction equation during it is as follows：
Autotrophic microbe denitrification method of the present invention removes nitrate material in water removal, is granular material, wherein containing single
Matter sulphur and calcium carbonate, have the following advantages：
1) by elemental sulfur and calcium carbonate composite molding in granular materials, disposable addition uses while being autotrophic microbe
Denitrification method goes the reaction process of nitrate in water removal to provide electron donor sulphur, inorganic carbon source and the buffer for adjusting basicity, nothing
Additive need to additionally be added, it is easy to use；
2) granular material rough surface of the present invention is conducive to the attachment of microorganism, is conducive to the removal of nitrate；
3) since material of the present invention slowly releases elemental sulfur in water electron donor is provided for microorganism anti-nitration reaction
Sulphur, while calcium carbonate is slowly released, while providing inorganic carbon source for microorganism, the basicity of solution is adjusted, reaction is made to continue
It is efficient to carry out, so that the nitrate in water is all converted into harmless nitrogen, the removal efficiency of nitrate is high；
4) it is not necessarily to improved device using material of the present invention, it is easy to operate, it is stable, it is cost-effective；
5) using the water body after material processing of the present invention, inorganic salts isoconcentration reduces, and effluent quality is good；
6) material of the present invention can be used for the various water bodys by azotate pollution, such as underground water.
In short, autotrophic microbe denitrification method of the present invention removes nitrate material in water removal, it is anti-to improve autotrophic microbe
The efficiency of nitrification removal nitrate, is reduced the cost for being removed nitrate using microorganism, realizes and gone completely using bioanalysis
The purpose of nitrate in water removal.
Further, the present invention uses lime stone, egg shell or scallop shell for the calcium carbonate in raw material forming material, lime
While the elements such as the nonmetallic silicon, magnesium metal, potassium, aluminium, the iron that contain in stone, egg shell, scallop shell increase material hardness, also
Indispensable trace element is provided for microorganism, is conducive to the progress of microorganism anti-nitration reaction.
Autotrophic microbe denitrification method of the present invention goes the preparation method of nitrate material in water removal, easy to operate, is easy to
Control is suitable for industrial application.
Specific implementation mode
The technical scheme of the invention is described in detail through specific implementation examples.
Embodiment 1
The present embodiment autotrophic microbe denitrification method removes nitrate material in water removal, and the material is that grain size is 3mm
It is granular；Contain elemental sulfur and calcium carbonate in the material, the mass ratio of the elemental sulfur and calcium carbonate is 2.5：1；With 20~100
Purpose limestone powder is raw material, forms the calcium carbonate in the material.
The present embodiment autotrophic microbe denitrification method removes the preparation method of nitrate material in water removal, concrete operation step
For：
1) it uses masking foil to weigh 25.0g simple substance sulfur powders, four edges of masking foil is turned up in carton shape, simple substance is placed
It flows out, then masking foil and simple substance sulfur powder is collectively disposed on thermostatic electrothermal plate, with the heating rate of 5 DEG C/min after sulphur liquefaction
105 DEG C are warming up to, elemental sulfur is made to melt completely, obtains liquid sulfur；
2) 10.0g limestone powders are weighed, is added in liquid sulfur prepared by step 1), limestone powder is made to be completely covered on
Liquid sulfur surface, it is persistently overheating to 120 DEG C with the heating rate of 5 DEG C/min later, and be stirred continuously and make liquid sulfur and lime stone
It is in pureed that powder, which is uniformly mixed, obtains mixture；
3) mixture prepared by step 2) is placed in air at room temperature to be cooled to and is solidified as solid material, by solid material
It is broken for the particle of grain size 3mm, and crosses 3mm sieves and removes nitrate material in water removal to get the autotrophic microbe denitrification method
Material.
Embodiment 2
The present embodiment autotrophic microbe denitrification method removes nitrate material in water removal, and the material is that grain size is 1mm
It is granular；Contain elemental sulfur and calcium carbonate in the material, the mass ratio of the elemental sulfur and calcium carbonate is 3.0：1；With 20~100
Purpose egg shell powder is raw material, forms the calcium carbonate in the material.
The present embodiment autotrophic microbe denitrification method removes the preparation method of nitrate material in water removal, concrete operation step
For：
1) it uses masking foil to weigh 30.0g simple substance sulfur powders, four edges of masking foil is turned up in carton shape, simple substance is placed
It flows out, then masking foil and simple substance sulfur powder is collectively disposed on thermostatic electrothermal plate, with the heating rate of 7 DEG C/min after sulphur liquefaction
110 DEG C are warming up to, elemental sulfur is made to melt completely, obtains liquid sulfur；
2) 10.0g egg shell powder is weighed, is added in liquid sulfur prepared by step 1), limestone powder is made to be completely covered on
Liquid sulfur surface, it is persistently overheating to 125 DEG C with the heating rate of 7 DEG C/min later, and be stirred continuously and make liquid sulfur and lime stone
It is in pureed that powder, which is uniformly mixed, obtains mixture；
3) mixture prepared by step 2) is placed in air at room temperature to be cooled to and is solidified as solid material, by solid material
It is broken for the particle of grain size 1mm, and crosses 1mm sieves and removes nitrate material in water removal to get the autotrophic microbe denitrification method
Material.
Embodiment 3
The present embodiment autotrophic microbe denitrification method removes nitrate material in water removal, and the material is that grain size is 5mm
It is granular；Contain elemental sulfur and calcium carbonate in the material, the mass ratio of the elemental sulfur and calcium carbonate is 1.25：1；With 20~
The scallop shell powder of 100 mesh is raw material, forms the calcium carbonate in the material.
The present embodiment autotrophic microbe denitrification method removes the preparation method of nitrate material in water removal, concrete operation step
For：
1) it uses masking foil to weigh 25.0g simple substance sulfur powders, four edges of masking foil is turned up in carton shape, simple substance is placed
It flows out after sulphur liquefaction, then masking foil and simple substance sulfur powder is collectively disposed on thermostatic electrothermal plate, with the heating speed of 10 DEG C/min
Rate is warming up to 115 DEG C, and elemental sulfur is made to melt completely, obtains liquid sulfur；
2) 20.0g scallop shell powder is weighed, is added in liquid sulfur prepared by step 1), limestone powder is made to be completely covered on
Liquid sulfur surface, it is persistently overheating to 130 DEG C with the heating rate of 10 DEG C/min later, and be stirred continuously and make liquid sulfur and lime stone
It is in pureed that powder, which is uniformly mixed, obtains mixture；
3) mixture prepared by step 2) is placed in air at room temperature to be cooled to and is solidified as solid material, by solid material
It is broken for the particle of grain size 5mm, and crosses 5mm sieves and removes nitrate material in water removal to get the autotrophic microbe denitrification method
Material.
Test example
The sulphur autotrophic denitrification microorganism used in following test examples is derived from anaerobic fermentation sludge, is with thiobacillus denitrificans
It is main.
Test method：
It is separately added into the nitrate nitrogen aqueous solution of 400mL 60mg/L in three 500mL sterilize conical flask, weighs respectively
Material prepared by 7g Examples 1 to 3, is separately added into three conical flasks, and be separately added into 10ml in three conical flasks simultaneously
Anaerobic sludge, sealing, reacts 6 days under the conditions of 30 DEG C, 120rpm in gas bath constant temperature oscillator, and supernatant is taken to measure nitrate
The content of nitrogen is as a result as follows：
The material prepared using embodiment 1 reaches 95% or more to the removal rate of nitrate after second day；Using implementation
Material prepared by example 2 reaches 95% or more to the removal rate of nitrate after the 4th day；The material prepared using embodiment 3 is to nitre
The removal rate of hydrochlorate reaches 97% or more behind third day.
Claims (5)
1. a kind of autotrophic microbe denitrification method goes the preparation method of nitrate material in water removal, which is characterized in that the material
Material is graininess；Contain elemental sulfur and calcium carbonate in the material, the mass ratio of the elemental sulfur and calcium carbonate is 1.25：1~
3.0：1；With in lime stone, egg shell, scallop shell one kind or be arbitrarily combined as raw material, form the calcium carbonate in the material；
The preparation method of the material includes following operating procedure：
1) it takes elemental sulfur to be heated to 105-115 DEG C of melting, obtains liquid sulfur；
2) it takes lime stone, egg shell or scallop shell to be added in liquid sulfur prepared by step 1), obtains mixture, mixture is continued to rise
Temperature to 120-130 DEG C to mixture in elemental sulfur melt completely, be uniformly mixed, obtain mixture；
3) mixture prepared by step 2) is cooled to and is solidified as solid material, be crushed to get the anti-nitre of autotrophic microbe
Change method removes nitrate material in water removal；
The specific method of heating is in step 1)：It is warming up to 105-115 DEG C with the rate of 5-10 DEG C/min；
The persistently overheating heating rate of step 2) is 5-10 DEG C/min；Lime stone described in step 2), egg shell or scallop shell add
Enter step 1) preparation liquid sulfur in concrete mode be：By lime stone, egg shell or scallop shell, uniformly paving is sprinkled upon liquid sulfur table
Face, and liquid sulfur surface is completely covered.
2. autotrophic microbe denitrification method as described in claim 1 goes the preparation method of nitrate material in water removal, special
Sign is, the lime stone, egg shell or scallop shell are using being preceding broken for 100~200 mesh powder shapes.
3. autotrophic microbe denitrification method as described in claim 1 goes the preparation method of nitrate material in water removal, special
Sign is, is broken for for solid material being broken for the graininess of 1~5mm described in step 3).
4. as claims 1 to 3 any one of them autotrophic microbe denitrification method goes the preparation of nitrate material in water removal
Method, which is characterized in that the grain size of the material is 1~5mm.
5. as claims 1 to 3 any one of them autotrophic microbe denitrification method goes the preparation of nitrate material in water removal
Method, which is characterized in that the lime stone, egg shell, scallop shell are 100~200 mesh powder shapes.
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| CN108083452B (en) * | 2017-12-15 | 2021-01-05 | 浙江海洋大学 | Heterotrophic and sulfur autotrophic integrated solid-phase denitrification system for treating high-nitrate water body |
| CN110117124A (en) * | 2018-02-07 | 2019-08-13 | 深圳市深水生态环境技术有限公司 | The landfill leachate full dose further treatment technique technique up to standard and method and system of concentrate are not produced |
| CN109019877B (en) * | 2018-09-21 | 2020-04-17 | 中国科学院生态环境研究中心 | Nitrogen and phosphorus removal active biological carrier, and preparation method and application thereof |
| CN109734197A (en) * | 2019-01-24 | 2019-05-10 | 天津友爱环保科技有限公司 | A kind of processing material of nitrogenous acid waste water and its application |
| CN109607778A (en) * | 2019-01-31 | 2019-04-12 | 北京潮白环保科技股份有限公司 | The processing method of the carrier of nitrate in a kind of removal water body |
| CN109650539A (en) * | 2019-02-21 | 2019-04-19 | 天津友爱环保科技有限公司 | Biologic packing material and its preparation method and application for removing groundwater azotate |
| CN111252890B (en) * | 2019-12-30 | 2022-07-05 | 无锡映川环境技术有限公司 | Carbon source-sulfur composite material for autotrophic denitrification and denitrification, preparation method and application |
| CN111252896A (en) * | 2020-03-12 | 2020-06-09 | 安庆创益环保有限公司 | Sulfur autotrophic material for removing nitrate from underground water and preparation method thereof |
| CN111285462B (en) * | 2020-05-13 | 2020-11-17 | 北京涞澈科技发展有限公司 | Synergistic denitrification composite suspended filler, preparation method and application thereof |
| CN111977787A (en) * | 2020-08-10 | 2020-11-24 | 深圳市播绿者生态科技股份有限公司 | Self-activated denitrification carrier material and preparation method and application thereof |
| CN112897689B (en) * | 2021-01-26 | 2022-09-23 | 东北大学 | Composite biological filler and preparation method and application thereof |
| CN113104976B (en) * | 2021-05-08 | 2023-06-06 | 无锡映川环境技术有限公司 | Flocculent autotrophic denitrification composite material and preparation method thereof |
| CN114634247A (en) * | 2022-04-15 | 2022-06-17 | 合肥工业大学 | Sulfur autotrophic nitrogen removal material prepared from sulfur paste or sulfur slag and preparation and application methods thereof |
| CN114620832B (en) * | 2022-04-15 | 2023-05-02 | 合肥工业大学 | Sulfur-based autotrophic microorganism denitrification material and preparation and application methods thereof |
| CN115321680A (en) * | 2022-10-18 | 2022-11-11 | 北京涞澈科技发展有限公司 | Medical stone-doped carbon-sulfur integrated material and preparation method thereof |
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| US7109022B1 (en) * | 1998-09-25 | 2006-09-19 | Nitchitsu Co., Ltd | Composition containing calcium carbonate particles dispersed in sulfur for removing nitrate nitrogen |
| KR100336483B1 (en) * | 1999-02-27 | 2002-05-15 | 조양호 | Method for removing nitrogen from waste water through sulfur-utilizing denitrification |
| WO2001025157A1 (en) * | 1999-10-01 | 2001-04-12 | Nitchitsu Co., Ltd. | Material for use in denitrification for the purpose of removing nitrate nitrogen and method for preparing the same |
| KR20020038322A (en) * | 2000-11-17 | 2002-05-23 | 김효근 | Simultaneous removal process of N, P for the wastewater |
| JP2006015310A (en) * | 2004-07-05 | 2006-01-19 | Nippon Steel Chem Co Ltd | Nitrate nitrogen treatment material and production method therefor |
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