CN106809956A - Be applied to reparation pollution of nitrate nitrogen in underground water releases carbon material and preparation method thereof - Google Patents
Be applied to reparation pollution of nitrate nitrogen in underground water releases carbon material and preparation method thereof Download PDFInfo
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- CN106809956A CN106809956A CN201510867790.8A CN201510867790A CN106809956A CN 106809956 A CN106809956 A CN 106809956A CN 201510867790 A CN201510867790 A CN 201510867790A CN 106809956 A CN106809956 A CN 106809956A
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Abstract
The invention discloses it is a kind of be applied to repair pollution of nitrate nitrogen in underground water release carbon material and preparation method thereof, be related to groundwater remediation technical field.The present invention includes water, and carbon source material, the framework material and control carbon source material for wrapping up carbon source material releases the enzyme of carbon；The parts by weight of wherein each material are：3 parts of carbon source material, framework material 1-5 parts, enzyme:0-0.1 parts, 100 parts of water.The invention provides a kind of novel, efficiently, economically viable realizing controlled-release carbon material and preparation method, during for permeable reactive wall original position underground water repair process, act not only as carbon source material, it is also used as microorganism carrier, it releases carbon good stability simultaneously, compression strength is big, good biocompatibility, the technical advantage such as the prices of raw materials are cheap, suitable for the underground water by various contaminants, microorganism is coordinated to use the purpose for reaching continual and steady removal nitrate nitrogen in underground water, simultaneously also for the solution of straw from village problem provides an approach for sustainable development environmental protection.
Description
Technical field
The present invention relates to groundwater remediation technical field, and in particular to one kind is applied to repair underground
Water pollution of nitrate nitrogen releases carbon material and preparation method thereof
Background technology
Due to developing rapidly for modern industrialization technology, the pollution of nitrate in groundwater turns into works as
The environmental problem received much concern in modern society, nitrate can cause some cancers after being taken in by human body
The generation of disease, badly influences the healthy living of the mankind.
The method of removal pollution of nitrate nitrogen mainly has three below technology at present：
Peripheral doses technology：By infiltration, absorption and the mode such as exchange by the nitrate in water body
Retention, existing forms of the nitrogen in water body is not changed, mainly including the way of distillation, membrane separation process
With ion-exchange etc..Shortcoming：Can not be innocuous substance by nitrate transformation, thus require
Nitrate to concentrating is post-processed, and efficiency is low, poor selectivity, investment are high, operating cost
With height.
Chemical remediation technology：Reducing agent is mainly used to reduce nitrate nitrogen, according to reducing agent
Difference can be divided into active metal reducing process, catalytic reduction method.Shortcoming：The problem of presence is
While being nitrogen molecule by reducing nitrate radical, a part of nitrate anion is reduced to ammonium ion,
Product is difficult to control to, and larger by such environmental effects, and operating cost is high.
Bioremediation technology：It is the denitrification using microorganism by the nitrate nitrogen in water body
It is converted into N2Method, adopt this method, in will not changing water body in processing procedure other
The concentration of ion.The product N of biological denitrificaion method generation2Stabilization, no murder by poisoning, processing cost ratio
Relatively low, high treating effect；But, heterotrophic denitrification process needs sufficient organic carbon source conduct
Electron donor could occur, and organic carbon source deficiency is puzzlement biochemical denitrification treatment always.For this
Problem, modern study person sets about being solved in terms of following two：One is in the few situation of organic carbon source
Under, using the autotrophic denitrification for not needing organic carbon source, using Electrode-biofilm membrane reactor negative electrode
Hydrogen is produced as electron donor, nitrate carries out autotrophic denitrification denitrogenation as electron acceptor in water,
This kind of method is very limited to the removal ability of nitrate nitrogen；Two is the natural carbon source of addition, is such as sawed
End, newspaper, stalk etc., but such carbon source is easily blocked, to release carbon speed uncontrollable and easily cause out
Water organic matter is exceeded, causes secondary pollution.These carbon sources can not be continual and steady supply carbon source
Have a strong impact on underground water and repair biological prosthetic effect.
The content of the invention
The technical problems to be solved by the invention are to provide one kind and are applied to repair underground water nitric acid
Salt polluted by nitrogen, possesses and releases carbon and certain compressive property, with low cost, novel, efficient,
Carbon material is released in economically feasible, environmental protection.
In order to solve the above technical problems, the technical solution used in the present invention is：One kind is applied to
That repairs pollution of nitrate nitrogen in underground water releases carbon material, it is characterised in that：Including water, carbon source material
Material, the framework material and control carbon source material for wrapping up carbon source material releases the enzyme of carbon；It is wherein each
The parts by weight of material are：3 parts of carbon source material, framework material 1-5 parts, enzyme:0-0.1 parts,
100 parts of water.
Further technical scheme is that described carbon source material is cornstarch, wheaten starch,
Newspaper, wheat stalk, maize straw, straw, deadwood and rotten leaf, sawdust, cotton, luffa,
One or more in bagasse, degradable cutlery box, wood chip.
Further technical scheme is that described framework material is insoluble framework material, wax
One or more in matter framework material, hydrophilic gel matrix material.
Further technical scheme is, described insoluble framework material is ethyl cellulose,
One kind in polyethylene, polypropylene, polysiloxanes and polyoxyethylene；
Further technical scheme is that described wax framework material has：Beeswax, hydrogenation are planted
Thing oil, synthetic wax, butyl stearate, stearic acid, Brazil wax, stearine,
One kind in propane diols-stearate and octadecanol；
Further technical scheme is that described hydrophilic gel matrix material is from 1. cellulose
Derivative, 2. non-cellulosic polysaccharide, 3. natural gum, 4. polyvinyl or acroleic acid polymerization
A class in the class of thing four；
Further technical scheme is that described cellulose derivative is methylcellulose, hydroxyl
Ethyl cellulose, HEMC, hydroxypropyl cellulose, hydroxypropyl methyl cellulose,
One or more in hydroxymethyl cellulose, sodium cellulose glycolate；Described non-cellulose is more
Sugar is glucose, chitin, chitosan, one or more of galactomannan；
Described natural gum is glue, the locust trees such as pectin, sodium alginate, potassium alginate, agar, angle fork
Bean gum, pawl ear natural gum, one or more of tragacanth；Described polyvinyl or propylene
Acid polymer is one or more of polyvinyl alcohol and poly- hydroxyalkyl vinyl 934.
Further technical scheme is, described enzyme elect as AMS, beta amylase,
One kind in gamma amylase, cellulase, zytase.
Further technical scheme be applied to repair pollution of nitrate nitrogen in underground water release carbon
The preparation method of material, it is characterised in that：Comprise the following steps：
A, the carbon source material pulverizer of above-mentioned parts by weight is ground into smalls, dried to perseverance
Weight, sealing preserve.
B, by the framework material of above-mentioned parts by weight in more than 80 DEG C of temperature, and continue stirring until
Dissolving.
C, the enzyme of the product of step A and above-mentioned parts by weight, water are added to and are provided with stirring
Stirred with rotating speed 800-1500r/min under temperature 50 C in the reactor of device and temperature regulating device
Mix 2h.
D, the product of step C is added in the product of step B, at 80 DEG C of temperature, with
Rotating speed 1500-2000r/min stirs 1h.
E, by the product of step D be injected into according to technological requirement design mould in be cooled to room
Temperature, is subsequently placed into freeze forming in refrigerator.
F, the product of step E is cut into pieces, dries to constant weight and be made finished product.
Further technical scheme is also resided in, and described mould is the 5ml injections for removing syringe needle
Device.
It is using the beneficial effect produced by above-mentioned technical proposal：The invention provides a kind of new
Clever, efficient, economically viable realizing controlled-release carbon material and preparation method, the material are used to permeate anti-
When answering wall (PRB) original position underground water repair process, act not only as carbon source material, may be used also
As microorganism carrier, while it is released, carbon good stability, compression strength is big, bio-compatible
The technical advantage such as the good, prices of raw materials of property are cheap, it is adaptable to by the underground of various contaminants
Water, coordinates microorganism using the purpose for reaching continual and steady removal nitrate nitrogen in underground water, while
Also for the solution of straw from village problem provides an approach for sustainable development environmental protection.
Brief description of the drawings
The present invention is further detailed explanation with reference to the accompanying drawings and detailed description.
Fig. 1 be in the present invention material products made thereby of group number 1 SEM figures；
Fig. 2 be in the present invention material products made thereby of group number 2 SEM figures；
Fig. 3 be in the present invention material products made thereby of group number 3 SEM figures；
Fig. 4 be in the present invention material products made thereby of group number 4 SEM figures；
Fig. 5 be in the present invention material products made thereby of group number 5 SEM figures；
It in the present invention is that the material products made thereby of group number 4 releases the SEM figure groups after carbon that Fig. 6 is；
It in the present invention is the material products made thereby COD in reactor of group number 1 that Fig. 7 isGrWith when
Between change curve；
It in the present invention is the material products made thereby COD in reactor of group number 2 that Fig. 8 isGrWith when
Between change curve；
It in the present invention is the material products made thereby COD in reactor of group number 3 that Fig. 9 isGrWith when
Between change curve；
It in the present invention is the material products made thereby COD in reactor of group number 4 that Figure 10 isGrWith when
Between change curve；
It in the present invention is the material products made thereby COD in reactor of group number 5 that Figure 11 isGrWith when
Between change curve；
It in the present invention is prepared according to the situation of this city nitrate nitrogen in underground water content that Figure 12 is
Sustained release carbon material insert effect curve figure in denitrification reactor.
Specific embodiment
The technical scheme in the embodiment of the present invention is clearly and completely described below, it is clear that
Described embodiment is only a part of embodiment of the invention, rather than whole implementation
Example.Based on the embodiment in the present invention, those of ordinary skill in the art are not making creativeness
The every other embodiment obtained under the premise of work, belongs to the scope of protection of the invention.
Many details are elaborated in the following description in order to fully understand the present invention, but
It is that the present invention can also be different from other manner described here to implement using other, this area
Technical staff can be similar popularization, therefore the present invention in the case of without prejudice to intension of the present invention
Do not limited by following public specific embodiment.
Preparation technology of the invention comprises the following steps：
A, 3 parts of parts by weight carbon source material pulverizers are ground into smalls, dried to constant weight,
Sealing preserve.
Wherein, carbon source material is cornstarch, wheaten starch, newspaper, wheat stalk, corn
Stalk, straw, deadwood and rotten leaf, sawdust, cotton, luffa, bagasse, degradable cutlery box,
One or more in wood chip.
B, by the 1-5 parts of framework material of parts by weight in more than 80 DEG C of temperature, and continue stirring
To dissolving.
Wherein, framework material is insoluble framework material, wax framework material, hydrophilic gel bone
One or more in frame material.
Preferably, conventional insoluble framework material has：Ethyl cellulose, polyethylene, poly- third
Alkene, polysiloxanes and polyoxyethylene etc.；
Conventional wax framework material has：Beeswax, hydrogenated vegetable oil, synthetic wax, stearic acid fourth
Ester, stearic acid, Brazil wax, stearine, propane diols-stearate and 18
Alkanol etc.；
Hydrophilic gel matrix material can divide four classes：1. cellulose derivative, such as methylcellulose,
Hydroxyethyl cellulose, HEMC, hydroxypropyl cellulose, hydroxypropyl methyl fiber
Element, hydroxymethyl cellulose and sodium cellulose glycolate etc.；2. non-cellulosic polysaccharide, such as glucose,
Chitin, chitosan and galactomannan etc.；3. natural gum, such as pectin, sea
The glue such as mosanom, potassium alginate, agar, angle fork, locust bean gum, pawl ear natural gum and west Huang alpine yarrow
Glue etc.；4. polyvinyl or acrylate copolymer etc., such as polyvinyl alcohol and poly- hydroxyalkyl vinyl
934 etc..
C, product and enzyme by step A:0-0.04 parts, 100 parts of parts by weight water are added to and set
Have in the reactor of agitating device and temperature regulating device under temperature 50 C with rotating speed
800-1500r/min stirs 2h.
D, the product of step C is added in the product of step B, at 80 DEG C of temperature, with
Rotating speed 1500-2000r/min stirs 1h.
E, by the product of step D be injected into according to technological requirement design mould in be cooled to room
Temperature, is subsequently placed into freeze forming in refrigerator.
Wherein, mould is the 5ml syringes for removing syringe needle.
F, the product of step E is cut into pieces, dries to constant weight and be made finished product.
Embodiment
Release that carbon compositional selecting is with low cost, be readily available maize straw in this experiment；Framework material
It is the mechanical property for improving slow-release material, using polyvinyl alcohol (PVA)；In the system of material
During standby, it is added thereto to a certain amount of amylase and can significantly change it to release carbon speed, this
Research is using AMS, beta amylase, gamma amylase, cellulase, zytase
Five kinds of amylase are tested for additive, and each group experimental products are carried out again respectively after experiment
Mechanical characteristic, architectural characteristic, release carbon characteristic, nitrogen removal performance experimental analysis with research.
It is different from the addition of the proportion, the amylase of addition and amylase of PVA according to stalk
The sustained release carbon material that will be prepared is divided into No. 25 materials, wherein according to stalk and the ratio of PVA
Difference is divided into five groups, and specific material mixture ratio situation is as follows：
The material composition ratio of group number 1 is shown in Table 1：
Table 1
The material composition ratio of group number 2 is shown in Table 2：
Table 2
The material composition ratio of group number 3 is shown in Table 3：
Table 3
The material composition ratio of group number 4 is shown in Table 4：
Table 4
The material composition ratio of group number 5 is shown in Table 5：
Table 5
Above-mentioned material is carried out into application and preparation in reparation groundwater azotate according to preparation technology respectively
Polluted by nitrogen releases carbon material.
A pre-treatment of raw material
Stalk：The stalk length of results than larger needs stalk to be cut into section before experiment, use powder
Broken machine is ground into smalls, dries to constant weight, sealing preserve.
The dissolving of PVA：In order to strengthen uniformity when PVA mixes with starch, so needing
It is completely dissolved PVA during blending.The PVA of HMW is to be difficult dissolving under conditions of room temperature
, being completely dissolved it needs for the temperature of system to be increased to more than 80 DEG C, and continues stirring
Dissolving.
The hydrolysis of enzyme：First, by stalk drying to constant weight；Then, experiment is weighed the desired amount of
Starch and distilled water are added in the reactor of agitating device and temperature regulating device；Then, maintain
Reactor temperature is 50 DEG C and adds a certain amount of amylase, and constant temperature is with rotating speed 1000r/min
Stirring 2h.
B solution blendings
The straw solution that will be handled well is added in the PVA solution being completely dissolved, and keeps system
Temperature is 80 DEG C, in the presence of mixer, with rotating speed 2000r/min stirring 1h (because
Now the viscosity of blend solution is greatly increased, so when mixer rotating speed need increase) 1h.
C castings
After the completion of waiting to be blended, by well mixed idiosome injection preprepared mould.This
In research, the mould that carbon material is released in the preparation for being used is 5ml syringes (removing syringe needle),
Its material is plastics.
Material in injection mould is cooled to room temperature, freeze forming in refrigerator is then placed in.
Section is subsequently cut into, is dried to constant weight and is made finished product.
Carrying out experimental analysis and studying to above-mentioned 5 group number products, it is as a result as follows：
1 mechanical characteristic
In this experiment, using microcomputer controlled electro minor universal testing machine to releasing the crushing resistance of carbon material
Can be tested, the results are shown in Table 2.
The mechanical characteristics of the material of table 2
It can be seen from table 2, load is with PVA needed for the unit deformation for releasing carbon material being prepared into
Content increase and increase.This is because, when PVA contents are high, PVA is continuous phase,
Stalk is dispersed phase, and PVA is surrounded stalk, releases carbon material and shows the flexible of PVA
Property, its crushing resistance is stronger；And when straw content is high, stalk is continuous phase, PVA is point
Dephasing, stalk is surrounded PVA, releases the hard fragility that carbon material then shows stalk, its
Crushing resistance declines.So, the mechanical characteristic and the proportioning of starch and PVA for releasing carbon material have very
Big relation, is affected by it than larger.
2 architectural characteristics
Material surface is analyzed, pair with No. 3, No. 8, No. 13, No. 18, No. 23 materials
Material is analyzed, and can not only seek its internal architectural feature, and can be by material
The contrast of biological denitrificaion front and rear surfaces structure, obtains material structure and releases carbon process, biological denitrificaion
Relation, the material to preparing is scanned result such as Fig. 1-6 of Electronic Speculum.
In Fig. 1-6, Fig. 5 shows that the skeleton structure of PVA in group number 5 is obvious, and shape
Webbed structure, supporting construction of its crosslinking winding escalator into material；Fig. 1 is shown in group number 1
Stalk and PVA amalgamations be not high, and stalk structure is obvious；And work as the straw content of material between
When between group number 1 and group number 4, the characteristic of material surface then show it is a kind of gradually change become
Gesture.Causing the main cause of this phenomenon is：Release carbon material what blending was formed, stalk with
PVA form interleaved discs around structure, when straw content than it is relatively low when, stalk is dispersed phase,
PVA is continuous phase, and stalk is fully wrapped around by PVA, and then plays control stalk release
Effect；And when PVA comparision contents are low, PVA is dispersed phase, stalk is continuous phase,
PVA plays a part of to increase material the filled media of intensity.Thus illustrate, PVA contents
Higher, the mutual amalgamation of material is better.
By comparison diagram 4 and Fig. 6, it can be seen that before material releases carbon, stalk and PVA are compatible
Property is good；After releasing carbon, stalk and PVA fusions become apparent, and hole integrally occurs in material.
3 release carbon characteristic
In this research, with CODGr(COD) releases the mark of carbon performance as material is judged
It is accurate.As illustrated in figures 7-11, it is respectively the material of group number 1,2,3,4,5 as releasing carbon material
When, COD in its reactorGrWith the change curve of time.
By Fig. 7-11 it can be seen that, five groups of materials by after the static test of 20 days, group number
The average carbon amounts of releasing of 1 section bar material up to 150mg/L, release carbon amounts and exist by the average of the material of group number 2
120mg/L or so, the average carbon amounts of releasing of the material of group number 3 in 105mg/L or so, and group number 4,
The average of the material of group number 5 releases carbon amounts but not 100mg/L, it can be seen that as stalk is in material
Expect the reduction of proportion, the carbon amounts of releasing of material is gradually reduced, conversely, when stalk proportion is raised,
Material integrally releases carbon amounts increase；In addition, in figure each group material release carbon amounts highest be No. 4,9
Number, No. 14, No. 19, No. 24, and the additive this which material is added is cellulose
Enzyme, thus illustrates that stalk produces cellulose through decomposing, and addition cellulase can reach preferably to be released
Carbon effect.
4 nitrogen removal performances
The sustained release carbon material prepared according to the situation of this city nitrate nitrogen in underground water content is filled out
In entering denitrification reactor, through after a while, as a result as shown in figure 12.
As seen from the figure, dose and change the denitrification reactor for releasing carbon material and can just be reached within one week
Stabilization, effluent nitrate-nitrogen drops to 5mg/L or so from the 30mg/L of water inlet, and denitrification percent reaches 80%
More than, denitrification effect is good, and accumulation of the water outlet without nitrite nitrogen, reaches drinking water safety mark
It is accurate.
Carbon characteristic, mechanics anti-compression property, structure spy are released by material prepared by above-mentioned analysis
Property and chemical characteristic obtain optimal material mixture ratio.And by using prepared by optimum proportioning
Material is added in PRB bioreactors, studies the material to simulated groundwater nitric efficiency,
Prove that denitrification percent reaches more than 96%, meet the requirement of biological removal nitrate nitrogen in underground water.
Claims (10)
1. it is a kind of be applied to repair pollution of nitrate nitrogen in underground water release carbon material, it is characterised in that：Including water, carbon source material, the framework material and control carbon source material for wrapping up carbon source material release the enzyme of carbon；The parts by weight of wherein each material are：3 parts of carbon source material, framework material 1-5 parts, enzyme:0-0.1 parts, 100 parts of water.
2. it is according to claim 1 be applied to repair pollution of nitrate nitrogen in underground water release carbon material, it is characterised in that：Described carbon source material is one or more in cornstarch, wheaten starch, newspaper, wheat stalk, maize straw, straw, deadwood and rotten leaf, sawdust, cotton, luffa, bagasse, degradable cutlery box, wood chip.
3. it is according to claim 1 be applied to repair pollution of nitrate nitrogen in underground water release carbon material, it is characterised in that：Described framework material is one or more in insoluble framework material, wax framework material, hydrophilic gel matrix material.
4. it is according to claim 3 be applied to repair pollution of nitrate nitrogen in underground water release carbon material, it is characterised in that：Described insoluble framework material is the one kind in ethyl cellulose, polyethylene, polypropylene, polysiloxanes and polyoxyethylene.
5. it is according to claim 3 be applied to repair pollution of nitrate nitrogen in underground water release carbon material, it is characterised in that：Described wax framework material has：One kind in beeswax, hydrogenated vegetable oil, synthetic wax, butyl stearate, stearic acid, Brazil wax, stearine, propane diols-stearate and octadecanol.
6. it is according to claim 5 be applied to repair pollution of nitrate nitrogen in underground water release carbon material, it is characterised in that：Described hydrophilic gel matrix material from 1. cellulose derivative, 2. non-cellulosic polysaccharide, 3. natural gum, the 4. class in polyvinyl or the class of acrylate copolymer four.
7. it is according to claim 6 be applied to repair pollution of nitrate nitrogen in underground water release carbon material, it is characterised in that：Described cellulose derivative is one or more in methylcellulose, hydroxyethyl cellulose, HEMC, hydroxypropyl cellulose, hydroxypropyl methyl cellulose, hydroxymethyl cellulose, sodium cellulose glycolate；Described non-cellulosic polysaccharide is glucose, chitin, chitosan, one or more of galactomannan；Described natural gum is the glue such as pectin, sodium alginate, potassium alginate, agar, angle fork, locust bean gum, pawl ear natural gum, one or more of tragacanth；Described polyvinyl or acrylate copolymer are one or more of polyvinyl alcohol and poly- hydroxyalkyl vinyl 934.
8. it is according to claim 1 be applied to repair pollution of nitrate nitrogen in underground water release carbon material, it is characterised in that：Described enzyme elects the one kind in AMS, beta amylase, gamma amylase, cellulase, zytase as.
9. being applied to according to claim 1-4 any one claims repairs the preparation method for releasing carbon material of pollution of nitrate nitrogen in underground water, it is characterised in that：Comprise the following steps：
A, the carbon source material pulverizer of above-mentioned parts by weight is ground into smalls, dried to constant weight, sealing preserve；
B, by the framework material of above-mentioned parts by weight in more than 80 DEG C of temperature, and continue stirring until dissolving；
C, the enzyme of the product of step A and above-mentioned parts by weight, water are added to be provided with the reactor of agitating device and temperature regulating device 2h is stirred with rotating speed 800-1500r/min under temperature 50 C；
D, the product of step C is added in the product of step B, at 80 DEG C of temperature, 1h is stirred with rotating speed 1500-2000r/min；
E, by the product of step D be injected into according to technological requirement design mould in be cooled to room temperature, be subsequently placed into freeze forming in refrigerator.
F, the product of step E is cut into pieces, dries to constant weight and be made finished product.
10. it is according to claim 9 be applied to repair pollution of nitrate nitrogen in underground water the preparation method for releasing carbon material, it is characterised in that：Described mould is the 5ml syringes for removing syringe needle.
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| CN110937693A (en) * | 2019-12-09 | 2020-03-31 | 苏亮星 | Preparation method and application of bacterium-fixing sustained-release granules capable of efficiently removing nitrogen |
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| CN112678949A (en) * | 2020-12-09 | 2021-04-20 | 夏存忠 | Carbon source with controllable carbon release rate and preparation method thereof |
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Application publication date: 20170609 |