CN110127806A - Utilize the method for electron beam irradiation degradation anticancer drug capecitabine - Google Patents
Utilize the method for electron beam irradiation degradation anticancer drug capecitabine Download PDFInfo
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- CN110127806A CN110127806A CN201910414587.3A CN201910414587A CN110127806A CN 110127806 A CN110127806 A CN 110127806A CN 201910414587 A CN201910414587 A CN 201910414587A CN 110127806 A CN110127806 A CN 110127806A
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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
- C02F1/00—Treatment of water, waste water, or sewage
- C02F1/30—Treatment of water, waste water, or sewage by irradiation
- C02F1/305—Treatment of water, waste water, or sewage by irradiation with electrons
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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
- C02F1/00—Treatment of water, waste water, or sewage
- C02F1/72—Treatment of water, waste water, or sewage by oxidation
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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
- C02F2101/00—Nature of the contaminant
- C02F2101/30—Organic compounds
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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
- C02F2305/02—Specific form of oxidant
- C02F2305/023—Reactive oxygen species, singlet oxygen, OH radical
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Abstract
The invention discloses a kind of methods using electron beam irradiation degradation anticancer drug capecitabine, realize efficient degradation under low radiation parameter by addition persulfate.Electron beam irradiation meets quasi- first order kinetics R > 0.99 to the good degrading effect of capecitabine.Irradiation dose constant reduces with the increase of initial concentration, radiates more effective to low concentration pollution.G value is reduced with the reduction of initial concentration, and is reduced with the increase of dose of radiation.Acid medium is conducive to the degradation of capecitabine, and alkaline medium is unfavorable for reacting.Addition oxidant potassium peroxydisulfate is obviously promoted effect, K to electron beam irradiation2S2O8Addition enhance irradiation to the removal effect of capecitabine pollutant effluents.The method of the present invention has the characteristics that degradation time-consuming is short, remediation efficiency is high, strong operability, and has good environmental benefit, Social benefit and economic benefit, administers for anticancer drug difficult to degrade and provides a kind of new method.
Description
Technical field
The present invention relates to a kind of organic pollutant degradation method of water body, more particularly to a kind of anticancer drug of water body
Biodegrading process is applied to Organic Pollutants In Water degradation treatment and water ecology recovery technique field.
Background technique
Cancer (malignant tumour) is the main public health problem in China and the whole world.It is widely used anti-in cancer chemotherapy
Cancer drug bio-toxicity with higher does not follow any control after incomplete metabolic drug excretion after entering patient's body
It manages and enters waste water and environment, because of its highest attention of potential environmental risk by domestic and international scientific research person.Antineoplastic
Object is classified as possible human carcinogen by international cancer research institution (IARC), destroys or hinders by interference DNA synthesis
Only cell Proliferation, with cytotoxicity, genotoxicity, some there is secretion interference performance in vivo, mutagenesis is carcinogenic.And it may
Directly or indirectly influence human health and natural ecosystems.
Conventional sewage processing technique and common high-level oxidation technology can not effectively control the shadow of anticancer drug in the environment
A possibility that sound harm, most of anti-tumor drug have biological degradability low, direct photolysis very little at all cannot；
Degradation of the technical applications such as ozone oxidation, hydrogen peroxide, photochemical catalyst and ultraviolet irradiation in anticancer drug, it is difficult to permineralization this
Class hard-degraded substance, but the compound for having toxicity even also stronger than parent is generated, cause bigger environmental hazard.
Irradiation can generate oxyradical and reduction free radical to make various degradations difficult to degrade, extensively simultaneously
Applied to degrading pesticide, nitroaromatic, herbicide and medical compounds etc..But it yet there are no and irradiation is applied to drop
Solve the relevant report of anticancer drug in water body.
Summary of the invention
In order to solve prior art problem, it is an object of the present invention to overcome the deficiencies of the prior art, and to provide one kind
Using the method for electron beam irradiation degradation anticancer drug capecitabine, enhances irradiation effect using potassium peroxydisulfate, utilize electron beam
Irradiation carries out efficient degradation to capecitabine, and promotes irradiation-induced degradation efficiency using potassium peroxydisulfate, reduces spoke irradiation dose.This hair
It is bright that capecitabine in sewage is efficiently removed using electronic beam irradiation technology, realize that mineralization degree is high, product toxicity is low, tool
Standby stronger application prospect.
In order to achieve the above objectives, the present invention adopts the following technical scheme:
A method of using electron beam irradiation degrade anticancer drug capecitabine, using addition oxidant potassium peroxydisulfate,
And irradiated by auxiliary electron beam, it degrades, includes the following steps: to anticancer drug capecitabine in water body
(1) anticancer drug capecitabine concentration is taken no more than 150mg/L containing capecitabine solution, is placed in transparent modeling
Material packaging bag simultaneously seals, as to degradation treatment water body；It is preferred that taking anticancer drug capecitabine concentration is 50-150mg/L's
Containing capecitabine solution, as to degradation treatment water body；
(2) contain addition oxidant K in capecitabine solution to what is taken in the step (1)2S2O8, after making mixing
Be not higher than 20mM containing oxidant concentration in capecitabine solution, and adjust the mixed pH containing capecitabine solution and be
3~11；It is preferred that adjusting the mixed pH containing capecitabine solution is 3~5；It is preferred that regulating and controlling mixed containing capecitabine
Oxidant concentration is 1-20mM in solution；Further preferably regulate and control and mixed is containing oxidant concentration in capecitabine solution
5-20mM；
(3) electron beam irradiation is utilized, in the case where absorbing radiation parameter of the metering no more than 8.0kGy, in the step
(2) electron beam irradiation degradation treatment is carried out containing capecitabine solution in.It is preferred that electron beam irradiation dosage is 0.5~8.0kGy.
After the completion of degradation, preferably by liquid chromatography-mass spectrometry measurement by the capecitabine concentration in water body during degradation treatment.
The present invention carries out efficient degradation to capecitabine in solution using electron beam irradiation, and it includes: hydroxyl that irradiation, which generates living radical,
Free radical has strong oxidizing property；Hydroperoxyl radical and hydrated ion are generated, there is strong reducing property, these types of free radical and Ka Peita
The group and carbocyclic ring of shore react, and ultimately generate nontoxic carbon dioxide and hydrone.
The present invention compared with prior art, has following obvious prominent substantive distinguishing features and remarkable advantage:
1. the method for the present invention makes to carry out efficient degradation to capecitabine in solution using electron beam irradiation, in 3kGy condition
Under, capecitabine concentration is in 150mg/L and solution degradation rate below up to 100%；
2. the method for the present invention is by adjusting pH value of solution, discovery acidity is conducive to the degradation of capecitabine, and alkalinity inhibits；With
PH=7 compares, and under the conditions of pH=3 and 5,8.64% and 4.94% is respectively increased in degradation rate；PH=9 and 11 degradation rates respectively under
Drop 6.17% and 11.11%；The present invention can also improve the degradation of irradiation by addition oxidant potassium peroxydisulfate, make to add
Potassium sulfate can be compared under low irradiation dose, reaching higher removal effect；When potassium peroxydisulfate concentration increases to 20mM from 0mM
When, the removal rate of capecitabine is increased to 91% by 57%, and removal rate and blank improve 59.65%；
3. the method for the present invention can be by pollutant exhaustive oxidation at small molecule inorganic matter, therefore substantially increases and utilize electronics
Beam irradiation technique is removed rate to capecitabine in sewage, realizes that mineralization degree is high, product toxicity is low, before having stronger application
Scape.
Detailed description of the invention
Fig. 1 is that staying water has different anticancer drug capecitabine initial concentrations in one method of the embodiment of the present invention
With the different irradiation doses of use to anticancer drug capecitabine degradation influence curve comparison diagram.
Fig. 2 is the various concentration anticancer drug capecitabine aqueous solution in one method of the embodiment of the present invention under radiation parameter
G value curve comparison figure.
Fig. 3 is influence comparison of the pH different in two method of the embodiment of the present invention to anticancer drug capecitabine irradiation-induced degradation
Figure.
Fig. 4 is that sour potassium influences comparison diagram to anticancer drug capecitabine irradiation-induced degradation in three method of the embodiment of the present invention.
Specific embodiment
Above scheme is described further below in conjunction with specific implementation example, the preferred embodiment of the present invention is described in detail such as
Under:
Embodiment one:
In the present embodiment, a method of using electron beam irradiation degradation anticancer drug capecitabine, utilizing addition oxygen
Agent potassium peroxydisulfate, and irradiated by auxiliary electron beam, it degrades to anticancer drug capecitabine in water body, including walk as follows
It is rapid:
(1) at room temperature, anticancer drug capecitabine standard items are dissolved in ultrapure water, obtaining ultimate density is
The simulation water body sample of the capecitabine containing anticancer drug of 50mg/L, 75mg/L, 100mg/L, 150mg/L, is placed in transparent plastic
Packaging bag simultaneously seals, as to degradation treatment water body；And the phosphoric acid tune that the sodium hydroxide and concentration for concentration being 0.1M are 0.1M
The pH for saving the simulation water body sample solution of the capecitabine containing anticancer drug, makes pH value of solution 11；
(2) contain addition oxidant K in capecitabine solution to what is taken in the step (1)2S2O8, after making mixing
Be 20mM containing oxidant concentration in capecitabine solution, keep adjusting the mixed pH containing capecitabine solution being 9
~11；
(3) persulfate auxiliary electron beam irradiation method is used, using GJ-II type electron beam irradiation, is measured absorbing
Under the radiation parameter of 0.5kGy, 1kGy, 1.5kGy, 2kGy, 3kGy, 5kGy, 8kGy, block to containing in the step (2)
It trains his shore solution and carries out electron beam irradiation degradation treatment.
Experimental test and analysis
After the completion of degradation, trained preferably by liquid chromatography-mass spectrometry measurement by the card in water body during degradation treatment
His shore concentration, judging that initial concentration and irradiation dose degrade on capecitabine influences.Interpretation of result:
The influence of capecitabine initial concentration and irradiation dose to degradation is as shown in Figure 1.Under identical dose of radiation, card
Training his removal rate of the shore under different initial concentrations, there were significant differences.When absorbed dose is 0.5kGy, initial concentration 50mg/
The removal rate of capecitabine in the simulation water body of the capecitabine containing anticancer drug of L is up to 95%, and capecitabine is initially dense
Degree is the removal rate of the capecitabine in the simulation water body of the capecitabine containing anticancer drug of 75mg/L, 100mg/L and 150mg/L
Respectively 86%, 80% and 57%.Under identical initial concentration, the removal rate of capecitabine is rapid with the increase of irradiation dose
Increase.When initial concentration is 150mg/L, the absorbed dose of 0.5kGy can reach 57% removal rate, and exposure dose 1kGy,
The corresponding removal rate of 1.5kGy, 2kGy and 3kGy are respectively 84%, 93%, 98% and 100%.Laboratory sample is irradiated in 3kGy
Under, up to 100%, this shows that electron beam irradiation is high to capecitabine degradation efficiency for removal.
Illustration indicates that capecitabine irradiation dose constant relationship under various concentration, table 1 are that capecitabine is each initial dense in Fig. 1
Spend lower irradiation-induced degradation kinetic parameter.
Irradiation-induced degradation kinetic parameter under each initial concentration of 1. capecitabine of table
As known from Table 1, capecitabine degradation trend substantially conforms to first-order kinetics, maximum dose constant under 50mg/L
For 5.48kGy, when initial concentration 75mg/L, 100mg/L and 150mg/L, dose factor be respectively 3.57kGy, 2.93kGy and
2.19kGy shows that dose factor and reaction rate increase with concentration and reduced.
The variation of G value is as shown in Figure 2 under different initial concentrations and irradiation dose.When capecitabine initial concentration is 50mg/L
When, G value drops to 0.16 from 2.44, when capecitabine initial concentration is 150mg/L, as irradiation dose increases from 0.5kGy
To 8kGy, G value drops to 0.49 from 4.54.The result shows that the G value of irradiation-induced degradation increases with the increase of initial concentration, with spoke
According to dosage increase and reduce.
The method that the present embodiment utilizes electron beam irradiation degradation capecitabine, and low irradiation is realized by addition persulfate
Under the conditions of efficient degradation.Electron beam irradiation meets quasi- first order kinetics, R > 0.99 to the good degrading effect of capecitabine.?
Under the conditions of 3kGy, 150mg/L capecitabine removal rate is up to 100%.Dose constant reduces with the increase of initial concentration, radiation pair
Low concentration pollution is more effective.G value is reduced with the reduction of initial concentration, and is reduced with the increase of dose of radiation.It originally is this
Embodiment method has the characteristics that degradation time-consuming is short, remediation efficiency is high, strong operability, and has good environmental benefit, society
Meeting benefit and economic benefit administer for anticancer drug difficult to degrade and provide a kind of new method.
Embodiment two:
The present embodiment is basically the same as the first embodiment, and is particular in that:
In the present embodiment, a method of using electron beam irradiation degradation anticancer drug capecitabine, utilizing addition oxygen
Agent potassium peroxydisulfate, and irradiated by auxiliary electron beam, it degrades to anticancer drug capecitabine in water body, including walk as follows
It is rapid:
(1) at room temperature, anticancer drug capecitabine standard items are dissolved in ultrapure water, obtaining initial concentration is
The simulation water body sample of the capecitabine containing anticancer drug of 150mg/L, is placed in Transparent plastic pack bag and seals, as wait degrade
Handle water body；And the phosphoric acid that the sodium hydroxide and concentration for concentration being 0.1M are 0.1M adjusts the mould of the capecitabine containing anticancer drug
The pH of quasi- water body sample solution, making pH value of solution is respectively 3,5,7,9 and 11；
(2) contain addition oxidant K in capecitabine solution to what is taken in the step (1)2S2O8, after making mixing
Be 20mM containing oxidant concentration in capecitabine solution, keep adjusting the mixed pH containing capecitabine solution being 9
~11；
(3) persulfate auxiliary electron beam irradiation method is used, using GJ-II type electron beam irradiation, is measured absorbing
To carry out electron beam irradiation degradation treatment to capecitabine solution is contained in the step (2) under the radiation parameter of 1kGy.
Experimental test and analysis
After the completion of degradation, trained preferably by liquid chromatography-mass spectrometry measurement by the card in water body during degradation treatment
His shore concentration, judges influence of the pH to capecitabine irradiation-induced degradation.Interpretation of result: influence of the pH value to capecitabine degradation efficiency
As shown in Figure 3.When pH value is 3,5,7,9 and 11, initial concentration is the simulation water of the capecitabine containing anticancer drug of 150mg/L
Final degradation rate of the capecitabine molecule in water environment in body sample is respectively 88%, 85%, 81%, 76% and 72%.
From experimental result as can be seen that capecitabine removal rate is higher in acid condition, compared with pH=7, in pH=3 and 5 conditions
Under, 8.64% and 4.94% is respectively increased in degradation rate；And the removal rate reacted under alkaline condition is lower, pH=9 and 11 and pH=7
Compare, degradation rate declines 6.17% and 11.11% respectively.
The method that the present embodiment utilizes electron beam irradiation degradation capecitabine, and low irradiation is realized by addition persulfate
Under the conditions of efficient degradation.Acid medium is conducive to the degradation of capecitabine, and alkaline medium is unfavorable for reacting.It originally is the present embodiment
Method has the characteristics that degradation time-consuming is short, remediation efficiency is high, strong operability, and has good environmental benefit, social benefit
And economic benefit, it is administered for anticancer drug difficult to degrade and provides a kind of new method.
Embodiment three:
The present embodiment is substantially the same as in the previous example, and is particular in that:
In the present embodiment, a method of using electron beam irradiation degradation anticancer drug capecitabine, utilizing addition oxygen
Agent potassium peroxydisulfate, and irradiated by auxiliary electron beam, it degrades to anticancer drug capecitabine in water body, including walk as follows
It is rapid:
(1) at room temperature, anticancer drug capecitabine standard items are dissolved in ultrapure water, obtaining initial concentration is
The simulation water body sample of the capecitabine containing anticancer drug of 150mg/L, is placed in Transparent plastic pack bag and seals, as wait degrade
Handle water body；And the phosphoric acid that the sodium hydroxide and concentration for concentration being 0.1M are 0.1M adjusts the mould of the capecitabine containing anticancer drug
The pH of quasi- water body sample solution, making pH value of solution is respectively 11；
(2) contain addition oxidant K in capecitabine solution to what is taken in the step (1)2S2O8, after making mixing
Be 0mM, 1mM, 5mM, 10mM, 15mM and 20mM containing oxidant concentration in capecitabine solution, keep adjusting mixed
PH containing capecitabine solution is 9~11；
(3) persulfate auxiliary electron beam irradiation method is used, using GJ-II type electron beam irradiation, is measured absorbing
To carry out electron beam irradiation degradation treatment to capecitabine solution is contained in the step (2) under the radiation parameter of 0.5kGy.
Experimental test and analysis
After the completion of degradation, trained preferably by liquid chromatography-mass spectrometry measurement by the card in water body during degradation treatment
His shore concentration, judges influence of the potassium peroxydisulfate to capecitabine irradiation-induced degradation.Interpretation of result: Fig. 4 shows various concentration over cure
The influence that sour potassium degrades to capecitabine.As shown in figure 4, potassium peroxydisulfate is added in the concentration range of 0~20mM to Ka Peita
The removal of shore remarkably promotes effect.It is obvious to the facilitation of electron beam irradiation to add oxidant potassium peroxydisulfate, K2S2O8Add
Add and enhances irradiation to the removal effect of CPC pollutant effluents.It can be compared under low irradiation dose, reaching higher removal effect.
When potassium peroxydisulfate concentration increases to 20mM from 0mm, the removal rate of capecitabine is increased to 91% by 57%, removal rate and blank
Comparison improves 59.65%.As it can be seen that addition potassium peroxydisulfate is preferable to the treatment effect of capecitabine waste water.In our current research, water
Reproducibility the particle e-aq and H that RADIATION DECOMPOSITION generates generate SO4- free radical with S2O82-.What reaction system generated
SO4- amount increases, and the oxidation reaction enhancing in solution, the degradation rate of capecitabine in the solution improves, and promotes capecitabine
Further degradation.The method that the present embodiment utilizes electron beam irradiation degradation capecitabine, and realized by addition persulfate
Efficient degradation under low radiation parameter.Acid medium is conducive to the degradation of capecitabine, and alkaline medium is unfavorable for reacting.It originally is this
Embodiment method has the characteristics that degradation time-consuming is short, remediation efficiency is high, strong operability, and has good environmental benefit, society
Meeting benefit and economic benefit administer for anticancer drug difficult to degrade and provide a kind of new method.
In conclusion the above embodiment of the present invention has carried out efficient drop to capecitabine in solution using electron beam irradiation
Solution, it includes hydroxyl radical free radical that irradiation, which generates living radical, has strong oxidizing property；Hydroperoxyl radical and hydrated ion are generated, is had
Strong reducing property, these types of free radical are reacted with capecitabine group and carbocyclic ring, ultimately generate nontoxic carbon dioxide and hydrone.
Under the conditions of 3kGy, capecitabine concentration is in 150mg/L and solution degradation rate below up to 100%.The above embodiment of the present invention
By adjusting pH value of solution, discovery acidity is conducive to the degradation of capecitabine, and alkalinity inhibits.Compared with pH=7, in pH=3 and 5
Under the conditions of, 8.64% and 4.94% is respectively increased in degradation rate；PH=9 and 11 degradation rates decline 6.17% and 11.11% respectively.It is logical
Cross the degradation that addition oxidant potassium peroxydisulfate improves irradiation, discovery addition potassium peroxydisulfate can compared under low irradiation dose,
Reach higher removal effect.When potassium peroxydisulfate concentration increases to 20mM from 0mm, the removal rate of capecitabine is improved by 57%
To 91%, removal rate and blank improve 59.65%.The above embodiment of the present invention is using electron beam irradiation to blocking in solution
It trains his shore and carries out efficient degradation, it includes: hydroxyl radical free radical that irradiation, which generates living radical, has strong oxidizing property；It is free to generate hydrogen
Base and hydrated ion, have strong reducing property, and these types of free radical is reacted with the group of capecitabine and carbocyclic ring, ultimately generated nontoxic
Carbon dioxide and hydrone.
Combination attached drawing of the embodiment of the present invention is illustrated above, but the present invention is not limited to the above embodiments, it can be with
The purpose of innovation and creation according to the present invention makes a variety of variations, under the Spirit Essence and principle of all technical solutions according to the present invention
Change, modification, substitution, combination or the simplification made, should be equivalent substitute mode, as long as meeting goal of the invention of the invention,
The technical principle and inventive concept of the method for electron beam irradiation degradation anticancer drug capecitabine are utilized without departing from the present invention,
Belong to protection scope of the present invention.
Claims (7)
1. a kind of method using electron beam irradiation degradation anticancer drug capecitabine, which is characterized in that utilize addition oxidant
Potassium peroxydisulfate, and irradiated by auxiliary electron beam, it degrades, includes the following steps: to anticancer drug capecitabine in water body
(1) anticancer drug capecitabine concentration is taken no more than 150mg/L containing capecitabine solution, is placed in transparent plastic packet
It packs and seals, as to degradation treatment water body；
(2) contain addition oxidant K in capecitabine solution to what is taken in the step (1)2S2O8, make mixed contain
There is in capecitabine solution oxidant concentration be not higher than 20mM, and adjust the mixed pH containing capecitabine solution be 3~
11；
(3) electron beam irradiation is utilized, in the case where absorbing radiation parameter of the metering no more than 8.0kGy, in the step (2)
In containing capecitabine solution carry out electron beam irradiation degradation treatment.
2. utilizing the method for electron beam irradiation degradation anticancer drug capecitabine according to claim 1, it is characterised in that:
In the step (1), taking anticancer drug capecitabine concentration is 50-150mg/L containing capecitabine solution, as wait drop
Solution processing water body.
3. utilizing the method for electron beam irradiation degradation anticancer drug capecitabine according to claim 1, it is characterised in that:
In the step (2), adjusting the mixed pH containing capecitabine solution is 3~5.
4. utilizing the method for electron beam irradiation degradation anticancer drug capecitabine according to claim 1, it is characterised in that:
In the step (2), regulate and control it is mixed containing oxidant concentration in capecitabine solution be 1-20mM.
5. utilizing the method for electron beam irradiation degradation anticancer drug capecitabine according to claim 1, it is characterised in that:
In the step (2), regulate and control it is mixed containing oxidant concentration in capecitabine solution be 5-20mM.
6. utilizing the method for electron beam irradiation degradation anticancer drug capecitabine according to claim 1, it is characterised in that:
In the step (3), electron beam irradiation dosage is 0.5~8.0kGy.
7. utilizing the method for electron beam irradiation degradation anticancer drug capecitabine according to claim 1, it is characterised in that:
In the step (3), after the completion of degradation, using liquid chromatography-mass spectrometry measurement by the card in water body during degradation treatment
Train his shore concentration.
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Application publication date: 20190816 |