CN106512952A - Method for treating antibiotic and heavy metal combined pollution water by using modified graphene oxide - Google Patents
Method for treating antibiotic and heavy metal combined pollution water by using modified graphene oxide Download PDFInfo
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- CN106512952A CN106512952A CN201611044606.0A CN201611044606A CN106512952A CN 106512952 A CN106512952 A CN 106512952A CN 201611044606 A CN201611044606 A CN 201611044606A CN 106512952 A CN106512952 A CN 106512952A
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J20/00—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof
- B01J20/02—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising inorganic material
- B01J20/20—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising inorganic material comprising free carbon; comprising carbon obtained by carbonising processes
- B01J20/205—Carbon nanostructures, e.g. nanotubes, nanohorns, nanocones, nanoballs
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J20/00—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof
- B01J20/22—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising organic material
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J20/00—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof
- B01J20/28—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof characterised by their form or physical properties
- B01J20/28002—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof characterised by their form or physical properties characterised by their physical properties
- B01J20/28004—Sorbent size or size distribution, e.g. particle size
- B01J20/28007—Sorbent size or size distribution, e.g. particle size with size in the range 1-100 nanometers, e.g. nanosized particles, nanofibers, nanotubes, nanowires or the like
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J20/00—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof
- B01J20/28—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof characterised by their form or physical properties
- B01J20/28002—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof characterised by their form or physical properties characterised by their physical properties
- B01J20/28009—Magnetic properties
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F1/00—Treatment of water, waste water, or sewage
- C02F1/28—Treatment of water, waste water, or sewage by sorption
- C02F1/288—Treatment of water, waste water, or sewage by sorption using composite sorbents, e.g. coated, impregnated, multi-layered
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2101/00—Nature of the contaminant
- C02F2101/10—Inorganic compounds
- C02F2101/20—Heavy metals or heavy metal compounds
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2101/00—Nature of the contaminant
- C02F2101/30—Organic compounds
- C02F2101/34—Organic compounds containing oxygen
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2101/00—Nature of the contaminant
- C02F2101/30—Organic compounds
- C02F2101/36—Organic compounds containing halogen
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2101/00—Nature of the contaminant
- C02F2101/30—Organic compounds
- C02F2101/38—Organic compounds containing nitrogen
Abstract
The invention relates to a method for treating antibiotic and heavy metal combined pollution water by using modified graphene oxide. Specifically, nitrilotriacetic acid modified magnetic graphene oxide is taken as an adsorbent and then added to ciprofloxacin and heavy metal ion combined pollution water. An experiment result proves that each gram of the adsorbent contains almost hundreds of milligrams of exchanging ciprofloxacin by mass, the mass of exchanging copper ions reaches more than 60 milligrams, amination modified magnetic graphene oxide has a very good adsorption effect on ciprofloxacin and copper ions, and solids and liquids can be well separated after adsorption. Compared with the prior art, the treatment method is simple, the material preparation and operation cost is low, and antibiotics and heavy metals in the water can be effectively and simultaneously removed.
Description
Technical field
The invention belongs to environment functional material and water process new technical field, are related to while removing antibiotic and a huge sum of money in eliminating water
The processing method of category, and in particular to a kind of magnetic oxygenated Graphene of use amination removes Ciprofloxacin and copper in water body simultaneously
Method.
Background technology
Antibiotic is widely used in treating the bacterium infection of humans and animals, and is often added to animal feed
In, with its growth of prevention disease and promotion.In China, every year about 2.1 × 105Ton antibiotic produced, and 85% it
Be used for animal husbandry and medical industries.Most antibiotic is difficult to be removed by traditional sewage treatment plant, eventually with original shape
Or metabolite form enters environment, its pollution problem gradually causes extensive concern.However, in actual polluted-water, resisting
Raw element shows as the combined pollution with heavy metal more, and heavy metal can be reacted with antibiotic, and it is right that both may influence each other
The removal of side.Both pollutant are present in water body simultaneously, can cause serious threat to ecosystem and health.Therefore
Explore a kind of economical and efficient and can be while the treatment technology for removing antibiotic and heavy metal is imperative.
At present, absorption is proved to be a kind of simple to operate, economic, and the method that can effectively remove pollutant in water body,
In actual pollutant effluents is administered have been obtained for being widely applied.There are various adsorbents on the market usual
Costly, adsorption effect is poor for price, and is merely able to adsorb single heavy metal or antibiotic.And graphene oxide is used as suction
A kind of emerging adsorbing material in attached method, with wide material sources, dispersive property is good, stability is strong, specific surface area is big, oxygen-containing sense
The advantages of group is abundant and can produce in batches, can effectively adsorb the heavy metal ion of antibiotic, but graphene oxide adsorption potential
Put the limited and extremely difficult separation from aqueous solution.Therefore, research and develop it is new with graphene oxide as substrate, at a low price simultaneously
And efficient composite, have become graphene oxide and further develop and apply that absorption method processes antibiotic and heavy metal is given up
One key matter of science and technology of water.
Graphene oxide is product of the powdered graphite Jing after chemical oxidation and stripping, and it is a kind of New Type of Carbon of superior performance
Material, with than larger surface area and abundant surface functional group.Therefore, graphene oxide resists in having removal waste water simultaneously
The potentiality of raw element and heavy metal.However, graphene oxide is affected by its particle diameter and surface hydrophilic group, cause the material in water
In have superior dispersibility, be difficult to be separated from the water and recycle.In addition, the limited adsorption potential of graphene oxide
Point, limits which and applies in Practical Project.Magnetic nano-particle is loaded to into surface of graphene oxide, oxidation stone can be given
Black alkene magnetic so as to can separate from solid liquid phase well.But, the magnetic nanoparticle of load can occupy graphene oxide table
The adsorption site in face, graft modification prepare graphene oxide derived material and can improve which to antibiotic and heavy metal polluted waste water
Absorbability.Nitrilotriacetic acid is loaded to magnetic oxygenated graphenic surface by proper method by the present invention, improves its solid-liquid point
From ability, and it is to antibiotic in waste water and the removal ability of heavy-metal composite pollution thing.
The content of the invention
Present invention aims to above-mentioned existing adsorbent is relatively costly, adsorption effect is poor, and can not go simultaneously
The problem of removing heavy metals and antibiotic, there is provided a kind of magnetic oxygenated graphene composite material of amination modification is gone in eliminating water simultaneously
The method of Ciprofloxacin and copper, makes Ciprofloxacin and the concentration of copper substantially be reduced, while solid-liquid can be obtained very after absorption
Good separation.The purpose of the present invention is achieved through the following technical solutions:The present invention relates to a kind of magnetic of amination modification
Property the graphene oxide composite material method of simultaneously removing the third husky star of eliminating water medium ring and copper, first graphene oxide is carried out plus magnetic changes
Property, then which is modified with nitrilotriacetic acid again, finally applied to while in the water body containing Ciprofloxacin and copper, observing
Its removal effect to two kinds of pollutant, comprises the following steps that：
(1) graphene oxide in the present invention is prepared from by the Hummers oxidizing process for improveing by natural graphite powder.
6g graphite powders, 5gK is added in 1L conical flasks2S2O8, 5gP2O5With the 98% of 24mL H2SO4, stir in 80 DEG C of water-baths
Mix 4.5h.Room temperature is cooled to, 1L ultra-pure waters is subsequently adding and is diluted and stand overnight 12h.Mixture is filtered and deionized water punching
The acid of residual is washed off to neutrality.At 60 DEG C, oven drying obtains pre-oxidizing graphite；
(2) the pre-oxidation graphite for obtaining is added to into 240mL98%H2SO4In solution (0 DEG C).Add while stirring
5gNaNO3, 30gKMnO4(potassium permanganate is slowly added in mixed solution in batches) is reacted 4 hours below 0 DEG C.Then will rise
Temperature is reacted 2 hours at 35 DEG C, adds 500mL ultra-pure waters to react 1 hour at 98 DEG C, after mixed liquor is cooled to room temperature, uses 1L
Deionized water dilutes, and adds 40mL30%H2O2Continue reaction two hours.The mixture for obtaining is washed with 10% HCl, then
Washed to the neutral and constant volume that adds water with massive laundering, at 50 DEG C, ultrasonic disperse obtains graphene oxide aqueous suspensions in 2 hours；
(3) the ferrous sulfate mixed solution of the iron chloride and 0.05mol/L of 100mL 0.1mol/L is added to into 200mL
In 5mg/mL graphene oxides, heated and stirred 2 minutes in 85 DEG C of water-baths add ammonia, stir 45 minutes, and Magnetic Isolation is washed
Wash；
(4) addition 0.2g 1- (3- the dimethylamino-propyls) -3- ethyl carbodiimides in the aqueous solution of 0.4g nitrilotriacetic acids
Hydrochlorate (EDC) and 0.2g N-hydroxy-succinamides (NHS), persistently stir under room temperature two hours, are subsequently adding 20mL diethyls
Magnetic oxygenated Graphene obtained in alkene triamine and above-mentioned steps, mixed solution persistently stir 6h in 80 DEG C of water-bath.Obtain
Product be cooled to room temperature, be washed with deionized to neutrality and obtain described material modified.
(5) above-mentioned material is added in Ciprofloxacin and the simultaneous water body of copper, mixes solid-liquid point after reaction
From studying the mechanism of its removal ability and absorption to both.
In above-mentioned preparation method, the order of preparation is first to carry out adding magnetic to be modified by graphene oxide, is then activated with two kinds
The surface functional group of nitrilotriacetic acid is activated by agent NHS and EDC, then prepares the compound of nitrilotriacetic acid and magnetic oxygenated Graphene
Material.
In above-mentioned adsorption process, the time for mixing reaction is 14h.
In above-mentioned adsorption process, reaction temperature is 25 DEG C.
In above-mentioned adsorption process, quantity of sorbent is 0.0033g/mL.
In above-mentioned adsorption process, solid-liquid separation is carried out using Magnet.
The magnetic oxygenated graphene composite material adsorbed water body of the nitrilotriacetic acid modification prepared using the inventive method
In Ciprofloxacin and copper.
Compared with prior art, it is an advantage of the current invention that：
1. the adsorbing material preparation process used in the present invention is fairly simple, and nonhazardouss effect, raw material sources extensively, make
Chemical drugss FeCl3·6H2O and FeSO4·4H2O etc. is conventional chemical products.
2. using after absorption method adsorption treatment, it is possible to use Magnet carries out solid-liquid separation, easy to be recycled.
3. the present invention can make Ciprofloxacin and copper while being effectively addressed under relatively low processing cost, and by
It is different with the cutting mechanisms of Organic substance in the magnetic oxygenated Graphene heavy metal of nitrilotriacetic acid modification, therefore nitrilotriacetic acid modification
Magnetic oxygenated Graphene when the combined pollution of Organic substance and heavy metal is administered, the phenomenon of competitive Adsorption is weaker, is conducive to ammonia
A kind of popularization of the triacetic acid modified magnetic oxygenated Graphene as new adsorbent in combined pollution improvement.
Description of the drawings
Fig. 1 is the SEM schematic diagrams of the magnetic oxygenated graphene composite material of the nitrilotriacetic acid modification of the embodiment of the present invention 1；
Fig. 2 is the XRD schematic diagrams of the magnetic oxygenated graphene composite material of the nitrilotriacetic acid modification of the embodiment of the present invention 1；
Specific embodiment
The present invention is described in further details below with reference to Figure of description and specific embodiment.
Embodiment 1：
By 6g graphite powders, 5gK2S2O8, 5gP2O5It is added to the 98% of 24mL H2SO4In, 4.5h is aoxidized at 80 DEG C.Cooling
To room temperature, 1L ultra-pure waters are added to dilute and stand overnight 12h.Mixture filters simultaneously deionized water and rinses out the acid of residual into
Property.At 60 DEG C, oven drying obtains pre-oxidizing graphite；Pre-oxidation graphite is added to into 240mL98%H2SO4In solution (0 DEG C).Side
Stirring side adds 5gNaNO3, 30gKMnO4React 4 hours under condition of ice bath.Then it is warmed up at 35 DEG C and reacts 2 hours, adds
500mL ultra-pure waters are reacted at 98 DEG C 1 hour, then continue addition 1L ultra-pure waters and 40mL30%H at room temperature2O2, continue anti-
Answer two hours.The mixture for obtaining is washed with 10% HCl, is then washed to the neutral and constant volume that adds water, ultrasound with massive laundering
Dispersion obtains graphene oxide aqueous suspensions in 2 hours；The ferrous sulfate of the iron chloride and 0.05mol/L of 100mL 0.1mol/L is mixed
Close solution to be added in 200mL 5mg/mL graphene oxides, in 85 DEG C of water-baths, heated and stirred 2 minutes, add ammonia, stir
Mix 45 minutes, Magnetic Isolation washing；0.2g1- (3- dimethylamino-propyls) -3- second is added in the aqueous solution of 0.4g nitrilotriacetic acids
Base carbodiimide hydrochloride (EDC) and 0.2g N-hydroxy-succinamides (NHS), persistently stir under room temperature two hours, Ran Houjia
Enter magnetic oxygenated Graphene obtained in 20mL diethylenetriamines and above-mentioned steps, mixed solution is persistently stirred in 80 DEG C of water-bath
Mix 6h.The room temperature in the aqueous solution containing 0.4g nitrilotriacetic acids that 0.2gEDC and 0.2gNHS is added to persistently stirs two hours, then
Above-mentioned magnetic oxygenated graphene dispersing solution and 20mL diethylenetriamines, mixed solution is added persistently to stir the water-bath that 6h is at 80 DEG C
In.The product deionized water for obtaining is rinsed to neutrality and obtains the composite.Nitrilotriacetic acid modification obtained above
Magnetic oxygenated graphene composite material outward appearance be in black, be placed under scanning electron microscope observe, its surface texture such as Fig. 1 institutes
Show, it can be seen that a large amount of modified particles of surface of graphene oxide uniform load.Material is observed under X-ray diffractometer, such as
Shown in Fig. 2, it can be seen that significantly Fe3O4Diffraction maximum, it was demonstrated that the material is already provided with magnetic.
Under conditions of pH is 9 and temperature is 25 DEG C, the ring third that above-mentioned composite is added to single 50mg/L is husky
In the copper of star and 10mg/L, and the mixed solution of the copper of the Ciprofloxacin and 10mg/L of 50mg/L, after stirring reaction 14h, use
Magnet is separated, and its solid-liquid separation effect is very notable.
Embodiment 2：
In the mixed solution of the different Ciprofloxacin of pH value and copper, the magnetic oxygenated stone of above-mentioned nitrilotriacetic acid modification is added
Black alkene, comprises the following steps：
The magnetic oxygenated graphene composite material that 0.0033g nitrilotriacetic acids are modified is added into 25mL 50mg/L Ciprofloxacin
In the mixed solution of 10mg/L copper, it is 4.0～10.0 to adjust pH, carries out vibration absorption in 25 DEG C of water-bath constant temperature oscillators anti-
Should, the adsorbent is separated from waste water by Magnet after 14 hours, determined in waste water at 276nm with ultraviolet spectrophotometer
The content of Ciprofloxacin not to be adsorbed, with copper content not to be adsorbed in atomic absorption spectrometry waste water, the suction of calculating
Attached amount result is as shown in table 1：
Table 1：Adsorbance data of the adsorbent to Ciprofloxacin and copper under condition of different pH
As shown in Table 1, with the increase of pH, the adsorbent gradually strengthens to the absorbability of Ciprofloxacin and copper.
Embodiment 3：
The copper solution of variable concentrations is added in ciprofloxacin solution, adds the magnetic oxygenated of above-mentioned nitrilotriacetic acid modification
Graphene, comprises the following steps：
Initial concentration adds three second of 0.0033g ammonia for adding the copper ion of 0-4mg/L in the ciprofloxacin solution of 50mg/L
The magnetic oxygenated graphene composite material of acid modification, carries out vibration adsorption reaction in 25 DEG C of water-bath constant temperature oscillators, after 14 hours
The adsorbent is separated from waste water by Magnet, determine not to be adsorbed in waste water with ultraviolet spectrophotometer at 276nm
The content of Ciprofloxacin, the adsorbance result of calculating are as shown in table 2：
Table 2：Adsorbance data of the adsorbent to Ciprofloxacin under different copper concentrations
| Copper concentration (mg/L) | 0 | 0.01 | 0.1 | 0.5 | 1 | 2 | 4 |
| Ciprofloxacin adsorbance (mg/g) | 236.10 | 222.93 | 213.88 | 220.77 | 235.93 | 267.72 | 335.19 |
As shown in Table 2, with the increase of copper concentration, adsorbent is presented to Ciprofloxacin adsorbance and first reduces becoming of increasing afterwards
Gesture.This copper for being possibly due to low concentration can be with Ciprofloxacin competitive Adsorption site, and with the increase of copper concentration, the coupling of copper is made
With competitive Adsorption effect is greater than, so as to be conducive to the removal of Ciprofloxacin.
Embodiment 4：
Research external ions intensity adsorbs the impact of Ciprofloxacin and copper to adsorbent, comprises the following steps：
The sodium chloride solution of 0-1mol/L is added in the mixed solution of 25mL 50mg/L Ciprofloxacin and 10mg/L copper,
The magnetic oxygenated graphene composite material of 0.0033g nitrilotriacetic acids modification is added, is vibrated in 25 DEG C of water-bath constant temperature oscillators
The adsorbent is separated from waste water by adsorption reaction 14h by Magnet, determines waste water with ultraviolet spectrophotometer at 276nm
In Ciprofloxacin not to be adsorbed content, with copper content not to be adsorbed in atomic absorption spectrometry waste water, calculating
Adsorbance result is as shown in table 3：
Table 3：Adsorbance data of the adsorbent to Ciprofloxacin and copper under different ionic strength
As shown in Table 3, as sodium chloride concentration increases to 1mol/L from 0, in waste water, the adsorbance of Ciprofloxacin first increases
After reduce, and the adsorbance of copper is reduced always.
The above is only the preferred embodiment of the present invention, protection scope of the present invention is not limited merely to above-mentioned enforcement case
Example, the various process programs without substantial differences are in protection scope of the present invention with present inventive concept.
Claims (6)
1. a kind of method that use modified graphene oxide processes antibiotic and heavy-metal composite pollution water body, it is characterised in that
During the graphene oxide that nitrilotriacetic acid is modified adds antibiotic and heavy-metal composite pollution water, solid-liquid point after reaction is mixed
From, you can the antibiotic and heavy metal are removed from water.
2. a kind of use modified graphene oxide as claimed in claim 1 processes antibiotic and heavy-metal composite pollution water body
Method, described main method are absorption methods.
3. a kind of use modified graphene oxide as claimed in claim 1 processes antibiotic and heavy-metal composite pollution water body
Method, the antibiotic and heavy metal are Ciprofloxacin and copper respectively.
4. a kind of use modified graphene oxide as claimed in claim 1 processes antibiotic and heavy-metal composite pollution water body
Method, the time of the mixing reaction is 14h.
5. a kind of use modified graphene oxide as claimed in claim 1 processes antibiotic and heavy-metal composite pollution water body
Method, the solid-liquid separating method are magnetic separation techniques.
6. a kind of modified graphene oxide as claimed in claim 1 consumption in waste water is 0.0033g/mL.
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Cited By (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN107930607A (en) * | 2017-11-23 | 2018-04-20 | 湖南大学 | A kind of method that tetracycline and Ciprofloxacin single and binary-combined contamination water body are handled using modified graphene oxide |
| CN109395695A (en) * | 2018-09-03 | 2019-03-01 | 华南理工大学 | A kind of modified 3 D graphene composite material and the preparation method and application thereof |
| CN110255694A (en) * | 2019-07-05 | 2019-09-20 | 重庆大学 | A kind of method of artificial synthesized redox mediators activation potassium permanganate degradation organic pollutants |
| CN112723500A (en) * | 2019-10-28 | 2021-04-30 | 华东理工大学 | Environment-friendly efficient nano copper ion compound and preparation method and application thereof |
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| US20130314844A1 (en) * | 2012-05-23 | 2013-11-28 | Nanyang Technological University | Method of preparing reduced graphene oxide foam |
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Cited By (5)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN107930607A (en) * | 2017-11-23 | 2018-04-20 | 湖南大学 | A kind of method that tetracycline and Ciprofloxacin single and binary-combined contamination water body are handled using modified graphene oxide |
| CN109395695A (en) * | 2018-09-03 | 2019-03-01 | 华南理工大学 | A kind of modified 3 D graphene composite material and the preparation method and application thereof |
| CN110255694A (en) * | 2019-07-05 | 2019-09-20 | 重庆大学 | A kind of method of artificial synthesized redox mediators activation potassium permanganate degradation organic pollutants |
| CN112723500A (en) * | 2019-10-28 | 2021-04-30 | 华东理工大学 | Environment-friendly efficient nano copper ion compound and preparation method and application thereof |
| CN112723500B (en) * | 2019-10-28 | 2023-10-27 | 华东理工大学 | Environment-friendly high-efficiency nano copper ion compound and preparation method and application thereof |
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