CN107900097A - Nitrogen and phosphorus sustained release agent and preparation method and the application in remedying oil-polluted intertidal zone - Google Patents
Nitrogen and phosphorus sustained release agent and preparation method and the application in remedying oil-polluted intertidal zone Download PDFInfo
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- CN107900097A CN107900097A CN201711121062.8A CN201711121062A CN107900097A CN 107900097 A CN107900097 A CN 107900097A CN 201711121062 A CN201711121062 A CN 201711121062A CN 107900097 A CN107900097 A CN 107900097A
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B09—DISPOSAL OF SOLID WASTE; RECLAMATION OF CONTAMINATED SOIL
- B09C—RECLAMATION OF CONTAMINATED SOIL
- B09C1/00—Reclamation of contaminated soil
- B09C1/10—Reclamation of contaminated soil microbiologically, biologically or by using enzymes
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- C—CHEMISTRY; METALLURGY
- C05—FERTILISERS; MANUFACTURE THEREOF
- C05C—NITROGENOUS FERTILISERS
- C05C9/00—Fertilisers containing urea or urea compounds
- C05C9/02—Fertilisers containing urea or urea compounds containing urea-formaldehyde condensates
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B09—DISPOSAL OF SOLID WASTE; RECLAMATION OF CONTAMINATED SOIL
- B09C—RECLAMATION OF CONTAMINATED SOIL
- B09C2101/00—In situ
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Abstract
The present invention provides a kind of nitrogen and phosphorus sustained release agent and preparation method and the application in remedying oil-polluted intertidal zone.The nitrogen and phosphorus sustained release agent includes guanite and isobutanediurea.Nitrogen and phosphorus sustained release agent provided by the invention prepares that simple, raw material is cheap and easy to get, non-secondary pollution, easy to implement, rushing for seawater in oil pollution intertidal organism repair process can not only be effective against for intertidal zone oil spill reparation to release, can also be under conditions of intertidal zone landscape not be influenced, persistently promote the growth metabolism of oil degradation microorganism, removal rate to oil pollution in its stimulation lower intertidal zone indigenous microorganism 104 days is 39.42%, is significantly higher than the 22.38% of Natural Attenuation.
Description
Technical field
The invention belongs to oil pollution recovery technique field, is related to a kind of nitrogen and phosphorus sustained release agent and preparation method and is repairing stone
Application in oily pollution intertidal zone.
Background technology
Intertidal zone is extra large land material, the intermediate zone of energy exchange, is the habitat of a large amount of extra large terrestrials.And with global stone
Oily demand is growing and Offshore Oil Industry, the fast development of sea transport industry, offshore oil exploration, exploitation and transport
Scale constantly increases, and coastal waters oil spill accident takes place frequently, and causes serious intertidal zone oil pollution.Since petroleum pollution is with higher
Viscosity, difficult water-soluble, chemical stability and bioaccumulation effect, devastating impact is produced to environment and human health, and
Under field conditions (factors), as long as its devastating impact may continue many decades even centuries in intertidal zone.Using microbial degradation as
The traditional biological recovery technique of dominant mechanism is considered as most future all the time because of its small, non-secondary pollution advantage of input
Petroleum pollution means.
After oil spill accident occurs, often lazy weight or activity are pressed down the oil degradation microorganism in the environment of intertidal zone
System, the process of self-purification are quite very long, it is therefore desirable to artificial to strengthen reclamation activities to improve going for coastline petroleum pollution
Except efficiency.The current situation of domestic and international bioremediation technology is analyzed, using biostimulation technology, i.e., by improving micro- life
Contaminant degradation environment (such as nutrition condition, O of thing2Condition, biological accessibility of pollutant etc.) improve rate of bioremediation
Significant effect.It is traditional and the hydrology due to intertidal zone environment, hydraulics and biological environment have particularity and complexity
Biostimulation preparation is often diluted by sea height under the effect such as wind, wave, tide and spreads and be lost in, and cannot not only effectively facilitate
The degraded of petroleum pollution, and the secondary pollutions such as local seawater eutrophication can be caused.For biostimulation preparation between tide
The limitation faced during with pollution environmental applications, particularly adds nitrogen and phosphorus preparation rapidly losing wait in marine environment and protrudes
Problem, it is most important to study a kind of nitrogen and phosphorus sustained release preparation that can be suitably used for intertidal zone environment.
Disclosed nitrogen and phosphorus sustained release preparation, is chiefly used in agricultural to promote the volume increase of crops, such as
CN106380284A, CN106278555A, CN106431785A, CN106396835A etc., and it is used for oil pollution reparation then
It is relatively fewer.
At present, it has been disclosed that the slow release fertilizer applied to oil pollution reparation only in CN101229983A and
Reported in CN101928188A, and be used to soil environment, the application in the environment of intertidal zone does not have been reported that also.
CN101229983A discloses a kind of lipophilic controlled release fertilizer for the environmental organism reparation of oily pollution field, it is included such as
Lower component：60~70% calcium dihydrogen phosphate of graininess nitrogenous fertilizer, 10%~20% trace element, 0.2%~0.5% polyvinyl alcohol 2%
5%~15% vegetable oil 3%~7% of~8% sealant.The preparation method of the lipophilic controlled release material is as follows：In proportion by particle
State nitrogenous fertilizer, is placed in rotary drum seed-coating machine, then by calcium dihydrogen phosphate, trace element and filler after mixing, is placed in coating
In the charging box of machine, then by polyvinyl alcohol, into the aqueous solution that concentration is 15%, pour into the head tank of seed-coating machine, according to setting
Rotating speed, temperature, start seed-coating machine and air compressor sprays to nitrogen manure particle surface；Meanwhile constantly it is spilled into biphosphate
The mixture of calcium, trace element and filler, heating rotate, and make its drying.Vegetable oil is gradually added dropwise, is rotated further, closes bag
Clothing machine and air compressor, are down to room temperature, that is, product is made.The fertilizer can be attached on oil and can slowly Releasing nutrient and maintain
The continued propagation of somatic cells, to significantly improve the biological prosthetic efficiency in oily pollution place.However, above-mentioned material preparation process answers
It is miscellaneous, manufacturing cost is high, it is difficult to be widely applied.In addition, due to the addition of filler, sealant and vegetable oil, it is easy to
Cause secondary pollution, (for example, intertidal zone) may cause secondary pollution in sensitive environment.
CN101928188A disclose it is a kind of be used to repairing the slow release fertilizer of polycyclic aromatic hydrocarbon pollution, the fertilizer mainly by
Polyhydroxyalkanoates, diatomite, chemical fertilizer raw material, humic acid, bioactivator, inorganic metal and other components composition.The sustained release
Fertilizer produces micropore by the biodegradable of polyhydroxyalkanoates, so that nutriment is slowly discharged from micropore.
However, with micropore generation and constantly become larger, the moisture in intertidal zone can be made constantly into the inside of slow-release fertilizer
Into internal nutrition composition with moisture outflow without breakdown lose, cause slow-release fertilizer failure it is too fast, the moisture content such as intertidal zone compared with
Repeatedly addition is not only needed to may also result in the eutrophication of marine environment in high environment.
Therefore, to tackle further serious intertidal zone oil pollution present situation, research and development are sought suitable for the nitrogen phosphorus of intertidal zone environment
It is most important to support sustained release preparation.
The content of the invention
It is an object of the invention to provide a kind of nitrogen and phosphorus sustained release agent and preparation method and in remedying oil-polluted intertidal zone
Application.The nitrogen and phosphorus sustained release agent prepares simple, cheap and easy to get, non-secondary pollution, easy to implement, dirty for intertidal zone oil spilling
Dye repair can effectively solve the problem that nutritional agents in oil spill intertidal organism repair process to add rear seawater dilution rate fast
Problem, and promote microorganism to remove the efficient of petroleum pollution.
The purpose of the present invention is achieved by the following technical programs：
On the one hand, the present invention provides a kind of nitrogen and phosphorus sustained release agent, which includes guanite and isobutyl
Pitch two ureas；Wherein, the mixed proportion of the guanite and the isobutanediurea is according to nitrogen phosphorus in the environment and environment applied
The concentration value of nutrition is set.
In above-mentioned nitrogen and phosphorus sustained release agent, it is preferable that the guanite and the mass ratio of the isobutanediurea are (1-
10)：(1-10).
In above-mentioned nitrogen and phosphorus sustained release agent, it is preferable that the guanite and the mass ratio of the isobutanediurea are 4:
1, at this time, the nitrogen and phosphorus that sustained release preparation is discharged is adapted to the growth metabolism of microorganism, the microorganism under this adding proportion the most
Oil degradation efficiency highest, be 37.86%.
In the present invention, guanite is product that magnesium ion, phosphate anion and ammonium ion are reacted, and molecular formula is
Mg(NH4)PO4·6H2O, it can be with the nitrogen and phosphorus needed for releasing microbe growth metabolism by chemical hydrolysis, and has longer
The sustained release cycle；Isobutanediurea (IBDU) is the product that isobutylaldehyde is obtained with urea reaction, and molecular formula is (CH3)2CHCH
(NHCONH2)2, it is shorter can be sustained the cycle with the nitrogen nutrition needed for releasing microbe growth metabolism by chemical hydrolysis.
Above-mentioned IBDU, which hydrolyzes discharged urea, can be converted into ammonium ion, can be not only the growth metabolism of microorganism
Nitrogen source needed for providing, can also suppress guanite Mg (NH4)PO4·6H2The hydrolysis of O.
Another method, the present invention also provides the preparation method of above-mentioned nitrogen and phosphorus sustained release agent, it is by guanite and isobutyl
Pitch two ureas and be uniformly mixed and be ground into solid granular, obtain the nitrogen and phosphorus sustained release agent.
In above-mentioned preparation method, it is preferable that the grain diameter of the nitrogen and phosphorus sustained release agent is according to the tide applied
Between corresponding particle diameter is ground into the particle size of gravel.On the one hand, it is contemplated that the ornamental value of intertidal zone environment, makes
It seems similar with sand；On the other hand, too big particle diameter makes it be not easy down to migrate in intertidalite, causes to sink
The growth metabolism of microorganism inside product thing is limited be subject to nutriment.
In above-mentioned preparation method, it is preferable that the grain diameter 0.05mm-1.2mm of the nitrogen and phosphorus sustained release agent.
Another further aspect, the present invention also provides above-mentioned nitrogen and phosphorus sustained release agent answering in remedying oil-polluted intertidal zone
With, but it is not limited only to the application of oil pollution intertidal zone.
In above application, since the hydrology of intertidal zone environment, hydraulics and biological environment have particularity and complexity
The problems such as property, traditional nutritive stimulus preparation is often too fast there are dilution rate when administering oil spill intertidal zone.Intertidal zone
Seawater can provide guanite synthesis needed for magnesium ion and phosphate anion, and using the ammonium root that IBDU is discharged from
Son, can be with microsynthesis guanite, and nitrogen, the phosphorus discharged with reducing slow release fertilizer is rushed by seawater and released, and increases the sustained release cycle, should
The density of nutrition slow-release preparation is more than seawater, will not be diluted by seawater, and under the washing away of seawater, can be gradually to deposit
Bottom migration is so as to can there are the longer time in the environment.
In above-mentioned application, it is preferable that the nitrogen and phosphorus sustained release agent is uniformly sowed in seashore during seawater low tide,
So that nutritional preparation can uniformly be distributed in intertidal zone, and reduce the input of human and material resources and material.
In above-mentioned application, it is preferable that the amount of sowing of the nitrogen and phosphorus sustained release agent is 0.1-2.0g/m2。
In above-mentioned application, it is preferable that the amount of sowing of the nitrogen and phosphorus sustained release agent is 0.5g/m2.This additive amount is root
The best proportion compounded according to the additive amount of microorganism, crude oil concentration, surfactant and nutrition slow-release preparation.
Nitrogen and phosphorus sustained release agent provided by the invention prepares that simple, raw material is cheap and easy to get, non-secondary pollution, easy to implement,
Rushing for seawater in oil pollution intertidal organism repair process can not only be effective against for intertidal zone oil spill reparation to release,
It under conditions of intertidal zone landscape is not influenced, can also persistently promote the growth metabolism of oil degradation microorganism, make in its stimulation
With being 39.42% to the removal rate of oil pollution in lower intertidal zone indigenous microorganism 104 days, it is significantly higher than Natural Attenuation
22.38%.
Brief description of the drawings
Fig. 1 be the nitrogen of guanite in the embodiment of the present invention 1, phosphorus nutrition with the time slow release effect figure；
The nitrogen nutrition that Fig. 2 is IBDU in the embodiment of the present invention 1 is with the slow release effect figure of time；
Fig. 3 is the slow-release nutrient material of guanite and IBDU in the embodiment of the present invention 2 to oil pollution microbial degradation
Facilitation figure；
Shadows of the Fig. 4 for the different proportion of guanite and IBDU in the embodiment of the present invention 3 to biodegradation of Petroleum-contaminated
Ring design sketch；
Fig. 5 is the change curve of 4 middle intertidal zone deposit petrochina concentration of the embodiment of the present invention.
Embodiment
In order to which technical characteristic, purpose and the beneficial effect of the present invention is more clearly understood, now to the skill of the present invention
Art scheme carry out it is described further below, but it is not intended that to the present invention can practical range restriction.
The nutrition slow-release performance evaluation of 1 guanite of embodiment and isobutanediurea (IBDU)
Weigh 2.5g guanites and IBDU is put into 50mL centrifuge tubes, add 40mL deionized waters, cover centrifugation tube cover.Will
Centrifuge tube traverse enters in shaking table, takes out all water samples in centrifuge tube after 24h is discharged under conditions of 30 DEG C, 150rpm, adds again
Enter 40mL pure water and shake 24h, repeat aforesaid operations daily until the sustained release performance of sample disappears.The water sample taken out daily exists
20min is centrifuged under the conditions of 3000rpm, then the sustained-release liquid after centrifugation is passed through into 0.45 μm of membrane filtration, survey its total nitrogen, total phosphorus contains
Amount.Above-mentioned result of implementation is as depicted in figs. 1 and 2.
As shown in Figure 1, after sustained release 2 days, the sustained release of guanite nitrogen basically reaches balance, and equilibrium concentration maintains 33mg/
L, with the progress of time, slightly floats up and down.Similarly, after sustained release 2 days, the nutrition slow-release of phosphorus reaches balance, and balance is dense
Degree maintains 36mg/L or so, with the progress of time, slightly floats up and down.After sustained release 85 days, nitrogen and phosphorus has been sustained
Finish.As shown in Figure 2, be sustained 2 days after, the sustained release of IBDU nitrogen basically reaches balance, and equilibrium concentration maintains 445mg/L, with when
Between progress, up and down slightly float.After sustained release 25 days, nitrogen concentration declines rapidly, and sustained release finishes after 28 days.
The result shows that indoors under stable environmental condition, sustained release cycle of guanite probably at 85 days, nitrogen, phosphorus nutrition
Sustained concentration about maintain 1:1, it is sustained the cycle and sustained release works well；Compared with guanite, IBDU has shorter delay
Release the cycle, but there is higher nitrogen nutrition sustained concentration, in sustained release 28 days, the sustained concentration of nitrogen maintains essentially in 4455mg/
L.The two is combined, and can meet a large amount of consumption of biological prosthetic nutriment at initial stage, and can ensure permanently effective nutrition supplying
Should.
2 guanite of embodiment and the nutrition slow-release liquid of isobutanediurea (IBDU) comment the effect of oil pollution shaking flask reparation
Valency
Using Venezuela's heavy oil as pollutant, guanite and IBDU nutrition slow-release liquid are investigated under simulated seawater salinity to stone
The influence of oil contaminants microbial degradation.Carry out as follows：2.5g laboratories self-control immobilized microbial inoculum is taken to be inoculated in 100mL
Simulate oil pollution sea water medium (inorganic salts, guanite and IBDU) in, heavy oil content 1g/L, 25 DEG C~30 DEG C,
Shaken cultivation 14d under the conditions of 180rpm, lucifuge, certain interval of time measure immobilized microbial inoculum counterweight in different sea water mediums
The degradation efficiency of oil contaminants.Each processing sets 3 repetitions, and to add the immobilized microbial inoculum of equivalent high-temperature inactivation as cloudy
Property control.Degrade after 14d, the content of zymotic fluid residual crude oil is carried out after carbon tetrachloride extraction, constant volume using Infrared Oil Determination Instrument
Measure, degradation rate (%)=(1- residual crude oils amount/original crude oil amount) × 100.Result of implementation is as shown in Figure 3.
Above-mentioned heavy oil is heavy crude oils of Venezuela, and 20 DEG C of density are 0.9593g/cm3, 50 DEG C of kinematic viscosity is 228.1mm2/
s。
The formula of above-mentioned inorganic salts sea water medium is：2g phosphate dihydrates disodium hydrogen, 3g potassium dihydrogen phosphates, 5g ammonium sulfate,
3g sodium chloride, 0.7g epsom salts, 1.0mL trace element solutions, are settled to 1L, and it is 7.4 to adjust pH.
The formula of above-mentioned guanite sea water medium is：3g sodium chloride, 0.7g epsom salts, 1.0mL trace elements are molten
Liquid, the guanite sustained-release liquid described in embodiment 1 are settled to 1L, and it is 7.4 to adjust pH.
The formula of above-mentioned IBDU sea water mediums is：2g phosphate dihydrates disodium hydrogen, 3g potassium dihydrogen phosphates, 3g sodium chloride,
0.7g epsom salts, 1.0mL trace element solutions, the IBDU sustained-release liquids described in embodiment 1 are settled to 1L, and it is 7.4 to adjust pH.
The formula of above-mentioned liquid microelement is：MnSO4·H2O 39.9mg/L, ZnSO4·H2O 42.8mg/L, (NH4)6Mo7O2·4H2O 34.7mg/L, be settled to 1L, adjust pH to be 7.0.
From the figure 3, it may be seen that the nitrogen and phosphorus that guanite and IBDU are discharged can be utilized by the microorganism, and since it can be with
Sustained release nutrition, the two facilitation to biodegradation of Petroleum-contaminated are above inorganic nutrient salt.In degraded 16 days
Afterwards, the immobilized microorganism using IBDU, guanite and inorganic salts as nitrogen and phosphorus source distinguishes the degradation efficiency of petroleum pollution
For 32%, 29% and 23%.
3 different proportion guanite of embodiment and IBDU are on the biodegradable influence of oil pollution
This implementation provides a kind of nitrogen and phosphorus sustained release agent, which includes guanite and isobutanediurea；
Investigate influence of the different compound proportions to crude oil microbial degradation.Take 2.5g laboratories self-control immobilized microbial inoculum inoculation
In 100mL real sea water culture mediums, the guanite and IBDU, 0.1g heavy oil of 0.1g different proportions are added in the medium,
25 DEG C~30 DEG C, 180rpm, shaken cultivation 14d under the conditions of lucifuge, measure oil degradation efficiency.Each processing sets 3 repetitions, and
Immobilized microbial inoculum to add equivalent high-temperature inactivation is used as negative control.Degrade after 14d, the content of zymotic fluid residual crude oil passes through
After carbon tetrachloride extraction, constant volume, it is measured using Infrared Oil Determination Instrument, degradation rate (%)=(1- residual crude oils amount/original crude oil
Amount) × 100.
The ratio of guanite and IBDU described above is respectively：1:1,2:1,3:Isosorbide-5-Nitrae:1,5:1 and 6:1.
Seawater described above is real sea water.
As shown in Figure 4, when guanite and the mass ratio of the isobutanediurea are 4:1, Microbes On Crude Oil has highest
Degradation efficiency, be 37.86%.When adding proportion is relatively low, phosphorus is probably the limiting factor of microorganism growth, works as adding proportion
When higher, nitrogen is probably limiting factor.
This implementation also provides the preparation method of the nitrogen and phosphorus sustained release agent, according to the mixed of above-mentioned guanite and isobutanediurea
Composition and division in a proportion example, guanite and isobutanediurea are uniformly mixed and are ground into solid granular, obtain the nitrogen and phosphorus sustained release agent, the nitrogen
The grain diameter of phosphorus nutrition sustained release agent is 0.05mm~1.2mm.
4 nutrition slow-release preparation of embodiment is in intertidal zone environment is simulated on the biodegradable influence of petroleum pollution
The present embodiment provides embodiment 3 nitrogen and phosphorus sustained release agent (wherein：The ratio of guanite and IBDU are 4:1) repairing
Application in multiple oil pollution intertidal zone.Specially：It is biological prosthetic that coastline oil pollution has been built by Mr. Yu's oil field mud and sand factory
Technology on-site verification system, tests continuous operation 3 months, periodic analysis sampling, investigates the nitrogen and phosphorus sustained release agent in actual rings
Application effect in border.
The long 5.2m of experiment pool × wide 1.7m × depth 1.5m, main analog grit matter coastline, is formed with fine sand place mat.Between tide
Band is minimum tide water level with underwater seashore line of demarcation.Inlet and outlet water uses different pipelines, and end of line sets granular membrane, to prevent
Only water inlet and water outlet obstruction.
After the completion of intertidalite is laid with, tide simulation is washed away 25 days or so.6kg crude oil is weighed respectively and adds 6L bavins
Oil, quickly stirred with electric mixer to crude oil it is dispersed after, crude oil mixed liquor is transferred in sprayer, it is equal in the declining time of tide
It is even to be sprayed on each test tank stromal surface, wash away 15 days, so that the physico-chemical property of seawater, deposit and heavy oil pollutant reaches steady
It is fixed.Oil spill is simulated after 15 days, uniformly adds nitrogen and phosphorus sustained release agent to intertidal zone surface in the declining time of tide, the ratio of adding is
0.5g/m2。
The results are shown in Figure 5 for above-described embodiment, after repairing 104 days, adds the crude oil of nitrogen and phosphorus sustained release agent test tank
Concentration drops to 5465mg/kg crude oil removals as 39.42% from 9473mg/kg, hence it is evident that higher than Natural Attenuation test tank
22.38%.
As it can be seen that the nitrogen and phosphorus sustained release agent of the present embodiment can be effective against the seawater diluting effect of intertidal zone environment, and
Efficiently stimulate the biodegradation of intertidal zone petroleum pollution.
In conclusion prepared by nitrogen and phosphorus sustained release agent provided by the invention, simple, raw material is cheap and easy to get, non-secondary pollution,
It is easy to implement, it can effectively solve the problem that nutritional agents in oil spill intertidal organism repair process for intertidal zone oil spill reparation
Add the problem of rear seawater dilution rate is fast, resist the seawater diluting effect of intertidal zone environment, and promote microorganism to oil
The efficient removal of pollutant, and the scenery external of intertidal zone is not influenced.
Claims (10)
- A kind of 1. nitrogen and phosphorus sustained release agent, it is characterised in that：The nitrogen and phosphorus sustained release agent includes guanite and isobutanediurea.
- 2. nitrogen and phosphorus sustained release agent according to claim 1, it is characterised in that：The guanite and the isobutanediurea Mass ratio be (1-10)：(1-10).
- 3. nitrogen and phosphorus sustained release agent according to claim 2, it is characterised in that：The guanite and the isobutanediurea Mass ratio be 4:1.
- 4. the preparation method of claim 1-3 any one of them nitrogen and phosphorus sustained release agents, it is by guanite and isobutyl fork two Urea, which is uniformly mixed, is ground into solid granular, obtains the nitrogen and phosphorus sustained release agent.
- 5. preparation method according to claim 4, it is characterised in that：The grain diameter of the nitrogen and phosphorus sustained release agent is root Corresponding particle diameter is ground into according to the particle size for the intertidal zone gravel applied.
- 6. preparation method according to claim 5, it is characterised in that：The grain diameter of the nitrogen and phosphorus sustained release agent exists Between 0.05mm-1mm.
- 7. application of the claim 1-3 any one of them nitrogen and phosphorus sustained release agents in remedying oil-polluted intertidal zone.
- 8. application according to claim 7, it is characterised in that：The nitrogen and phosphorus sustained release agent is equal during seawater low tide It is even to sow in seashore.
- 9. application according to claim 7, it is characterised in that：The amount of sowing of the nitrogen and phosphorus sustained release agent is 0.1- 2.0g/m2。
- 10. application according to claim 9, it is characterised in that：The amount of sowing of the nitrogen and phosphorus sustained release agent is 0.5g/m2。
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Cited By (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN110743907A (en) * | 2019-10-30 | 2020-02-04 | 东营金岛环境工程有限公司 | Microorganism and plant combined in-situ remediation process for petroleum-polluted soil |
| CN111434643A (en) * | 2019-01-14 | 2020-07-21 | 石河子大学 | Slow/controlled release fertilizer prepared based on natural protein and preparation method and application thereof |
| CN113044974A (en) * | 2021-03-18 | 2021-06-29 | 中交上海航道勘察设计研究院有限公司 | Denitrification material based on sulfur autotrophic denitrification, preparation method and application |
| CN115873838A (en) * | 2022-11-22 | 2023-03-31 | 天津科技大学 | Immobilized microorganism particles capable of slowly releasing nutrition and preparation method thereof |
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