CN113588608B - Method for evaluating electron loss capability of micro plastic through oxidation rate of trivalent arsenic of micro plastic - Google Patents
Method for evaluating electron loss capability of micro plastic through oxidation rate of trivalent arsenic of micro plastic Download PDFInfo
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Abstract
The invention discloses a method for evaluating the electron losing capability of a micro plastic by the oxidation rate of trivalent arsenic of the micro plastic, which specifically comprises the following steps: uniformly mixing the micro plastic and a solution containing trivalent arsenic with the concentration of 0.25-1 mg/L according to the mass-volume ratio of 1-2 mg/ml, and then carrying out shake culture in an aerobic environment; sampling for 0, 1, 2, 4, 6 and 10 hours, filtering with a 0.22 micron filter membrane, storing the filtrate with 0.2M hydrochloric acid, then measuring the content of trivalent arsenic and total arsenic by an atomic fluorescence spectrophotometer, and calculating the oxidation rate of arsenic according to the change condition of the concentration of trivalent arsenic along with the reaction time for estimating the electron loss capability of the micro-plastic; the method has reasonable overall design, utilizes the functional group with electron losing ability in the micro plastic to react with oxygen to generate hydrogen peroxide which can further react with trivalent arsenic, and evaluates the electron losing ability of the micro plastic according to the oxidation speed of the trivalent arsenic; the method has simple process and is suitable for large-scale popularization.
Description
Technical Field
The invention relates to the technical field of micro-plastic electron capacity measurement, in particular to a method for evaluating the electron losing capacity of micro-plastic through the oxidation rate of trivalent arsenic of the micro-plastic.
Background
Plastic products are widely used in industrial and agricultural production and life, and over 55 percent of plastic products are released into the environment without being properly disposed after being used, so that micro plastic pollution generally exists in water body environment, land environment and atmospheric environment. When the micro plastic enters the environment, the micro plastic can undergo size reduction, specific surface area increase, hardness increase and generation of functional groups containing oxygen, sulfur and the like through physical, chemical and biological compound actions, and finally the migration, conversion and ecotoxicity effects in the micro plastic environment are changed.
In recent years, there has been a growing literature reporting that entry of micro-plastics into the environment can affect the biogeochemical cycle of carbon, nitrogen and oxygen. It has been suggested by researchers that it is possible that the redox-active functional groups in the microplastic have electron-accepting and electron-withdrawing capabilities and can mediate electron transfer during the redox conversion of a substance. The electron gaining capacity and electron losing capacity of microplastics are generally determined in the prior art by electrochemical methods or chemical reagent methods, wherein the electron losing capacity of microplastics increases with aging time. When the electron loss capacity of the micro-plastic is detected, the two analysis and detection methods need to be carried out in an anaerobic glove box, the reaction solution also needs to be aerated to remove oxygen, and the whole analysis process is extremely easy to be interfered by oxygen.
Therefore, there is a need to develop a method for estimating the electron-losing ability of micro-plastics in an aerobic environment.
Disclosure of Invention
The invention aims to solve the technical problems and provides a method for evaluating the electron losing capability of the micro plastic through the oxidation rate of trivalent arsenic of the micro plastic.
The technical scheme of the invention is as follows: a method for evaluating the electron loss capability of a micro plastic through the oxidation rate of trivalent arsenic of the micro plastic specifically comprises the following steps: uniformly mixing the micro plastic and a solution containing trivalent arsenic with the concentration of 1mg/L according to the mass-to-volume ratio of 1.5-2 mg/ml, and then carrying out shake culture in an aerobic environment; sampling for 0, 1, 2, 4, 6 and 10 hours, filtering with a 0.22 micron filter membrane, storing the filtrate with 0.2M hydrochloric acid, then measuring the content of trivalent arsenic and total arsenic with an atomic fluorescence photometer, and calculating the oxidation rate of arsenic according to the change condition of the concentration of trivalent arsenic along with the reaction time, wherein the oxidation rate is used for estimating the electron losing capability of the micro plastic; the principle of the method is as follows: in an aerobic environment, a functional group with electron losing capability in the micro plastic reacts with oxygen to generate hydrogen peroxide, the hydrogen peroxide reacts with trivalent arsenic in a solution, and the electron losing capability of the micro plastic is evaluated according to the speed of oxidation of the trivalent arsenic.
Further, the micro-plastic is an aged micro-plastic; the aged micro plastic is any one of aged phenolic resin micro plastic or aged polystyrene micro plastic; ozone aged phenolic resins and polystyrene microplastics were used to demonstrate the applicability of the process of the invention.
Further, the aged phenolic resin micro plastic adopts hydrogen peroxide aged phenolic resin micro plastic; the preparation method of the hydrogen peroxide aged phenolic resin micro plastic comprises the following steps: mixing phenolic resin micro plastic and hydrogen peroxide according to a mass volume ratio of 1-3: mixing the materials in a ratio of 20-80 g/ml, and performing shaking culture for 4-42 d to obtain the hydrogen peroxide aged phenolic resin micro plastic; as the aging time in hydrogen peroxide increases, C — OH content in the phenolic resin micro plastic gradually decreases, and C ═ O content gradually increases, and phenolic functional groups and semiquinone radicals on the surface generate hydrogen peroxide by reacting with oxygen, thereby oxidizing arsenic.
Further, the aged phenolic resin micro plastic is ozone aged phenolic resin micro plastic; the preparation method of the ozone aging phenolic resin micro plastic comprises the following steps: continuously aging the phenolic resin micro plastic for 20-22 h in an ozone environment to obtain ozone-aged phenolic resin micro plastic; ozone-aged phenolic resin microplastics also mediate arsenic oxidation by producing hydrogen peroxide.
Further, the aged polystyrene micro plastic is ozone aged polystyrene micro plastic; the preparation method of the ozone aging polystyrene micro plastic comprises the following steps: continuously aging the polystyrene micro plastic for 20-22 hours in an ozone environment to obtain ozone-aged polystyrene micro plastic; ozone-aged polystyrene microplastics also mediate arsenic oxidation by producing hydrogen peroxide.
On the other hand, the invention also provides application of the method for evaluating the electron losing capacity of the micro plastic through the oxidation rate of the trivalent arsenic of the micro plastic, and the method can be applied to treatment of arsenic polluted water bodies.
Furthermore, the method for treating the arsenic-polluted water body specifically comprises the following steps:
the method comprises the following steps: pretreatment of water body polluted by arsenic
Pretreating the water body polluted by arsenic;
the pretreatment method of the water body polluted by arsenic comprises the following specific steps: collecting water body polluted by arsenic, and filtering to remove large impurities;
step two: detection of arsenic content
Measuring the content of trivalent arsenic in the pretreated water body by using an atomic fluorescence spectrophotometer;
step three: treatment of
According to the content of trivalent arsenic in the water body, adding a restoration material into the water body to be treated according to the amount of 0.1-2 g/L added for treating 1mg/L of trivalent arsenic, and then restoring for 20-25 hours under the condition that the pH value is 5-9.
Still further, the restoration is any one of a micro plastic or an aged micro plastic.
Compared with the prior art, the invention has the following beneficial effects: the method has reasonable overall design, generates hydrogen peroxide by utilizing the phenolic functional groups and the semiquinone free radicals on the surface of the micro plastic through the reaction with oxygen so as to oxidize arsenic, and evaluates the electron losing capability of the micro plastic by utilizing the speed of the oxidation rate of the arsenic oxide; the method is not interfered by oxygen in actual use, and the method has simple process and is suitable for mass popularization.
Drawings
FIG. 1 is a graph of the hydrogen peroxide aged phenolic resin microplastic of the present invention's Experimental example 1 arsenic oxidation mediated in an aerobic environment;
FIG. 2 is a graph showing the correlation between electron-losing capacity and the mediated arsenic oxidation rate of the micro plastic of Experimental example 1 of the present invention;
FIG. 3 is a graph of the quenching effect of methanol and catalase addition on arsenic oxidation in Experimental example 1 of the present invention;
FIG. 4 is the concentration of hydrogen peroxide generated in the hydrogen peroxide aged phenolic resin microplastic solution of Experimental example 1 of the present invention;
FIG. 5 is a graph of ozone-aged phenolic resin microplastic in aerobic environment mediated arsenic oxidation according to Experimental example 1 of the present invention;
FIG. 6 shows the electron loss of the ozone-aged phenol resin micro plastic reacted with potassium ferricyanide in Experimental example 1 of the present invention;
FIG. 7 shows the arsenic oxidation mediated by ozone aged polystyrene microplastic in aerobic environment in Experimental example 1 of the present invention;
FIG. 8 shows the electron loss of the ozone-aged polystyrene microplastic reacted with potassium ferricyanide in Experimental example 1 of the present invention;
FIG. 9 shows the arsenic oxidation mediated by hydrogen peroxide aged phenolic resin microplastic in aerobic environment in Experimental example 2 of the invention;
FIG. 10 is a graph of the arsenic oxidation mediated by hydrogen peroxide aged phenolic resin microplastic of Experimental example 2 of the invention in an oxygen-free environment;
FIG. 11 is a graph of the quenching effect of alcohol and catalase addition on arsenic oxidation in Experimental example 2 of the present invention;
FIG. 12 is a graph showing the concentration of hydrogen peroxide generated in a hydrogen peroxide-aged phenol resin micro plastic solution according to Experimental example 2 of the present invention;
FIG. 13 is a graph of ozone-aged phenolic resin microplastic of Experimental example 2 of the present invention, in which arsenic oxidation was mediated in an aerobic environment;
FIG. 14 shows the concentration of hydrogen peroxide generated in ozone-aged phenolic resin microplastic solution of Experimental example 2 of the present invention;
FIG. 15 is a graph of ozone-aged polystyrene microplastic mediated arsenic oxidation in an aerobic environment according to Experimental example 2 of the present invention;
FIG. 16 is a graph showing the concentration of hydrogen peroxide generated in the ozone-aged polystyrene micro-plastic solution according to Experimental example 2 of the present invention;
Detailed Description
Example 1: a method for evaluating the electron loss capability of a micro plastic through the oxidation rate of trivalent arsenic of the micro plastic specifically comprises the following steps: uniformly mixing the micro plastic with a solution containing trivalent arsenic with the concentration of 0.25mg/L according to the mass-to-volume ratio of 1mg/ml, and then carrying out shake culture in an aerobic environment; and sampling at 0, 1, 2, 4, 6 and 10 hours, filtering with a 0.22 micron filter membrane, preserving the filtrate with 0.2M hydrochloric acid, then measuring the content of trivalent arsenic and total arsenic by an atomic fluorescence photometer, and calculating the oxidation rate of arsenic according to the change of the concentration of trivalent arsenic along with the reaction time, so as to estimate the electron loss capacity of the micro-plastic.
Example 2: a method for evaluating the electron loss capability of a micro plastic through the oxidation rate of trivalent arsenic of the micro plastic specifically comprises the following steps: uniformly mixing the micro plastic and a solution containing trivalent arsenic with the concentration of 0.5mg/L according to the mass-to-volume ratio of 1.5mg/ml, and then carrying out shake culture in an aerobic environment; and sampling for 0, 1, 2, 4, 6 and 10 hours, filtering with a 0.22 micron filter membrane, storing the filtrate with 0.2M hydrochloric acid, then measuring the content of trivalent arsenic and total arsenic by an atomic fluorescence photometer, and calculating the oxidation rate of arsenic according to the change of the concentration of trivalent arsenic along with the reaction time, so as to estimate the electron losing capacity of the micro-plastic.
Example 3: a method for evaluating the electron loss capability of a micro plastic through the oxidation rate of trivalent arsenic of the micro plastic specifically comprises the following steps: uniformly mixing the micro plastic and a solution containing trivalent arsenic with the concentration of 1mg/L according to the mass-to-volume ratio of 2mg/ml, and then carrying out shake culture in an aerobic environment; and sampling for 0, 1, 2, 4, 6 and 10 hours, filtering with a 0.22 micron filter membrane, storing the filtrate with 0.2M hydrochloric acid, then measuring the content of trivalent arsenic and total arsenic by an atomic fluorescence photometer, and calculating the oxidation rate of arsenic according to the change of the concentration of trivalent arsenic along with the reaction time, so as to estimate the electron losing capacity of the micro-plastic.
Example 4: the difference from example 1 is: the micro plastic is made of hydrogen peroxide aged phenolic resin; the preparation method of the hydrogen peroxide aged phenolic resin micro plastic comprises the following steps: mixing phenolic resin micro plastic and hydrogen peroxide according to a mass volume ratio of 1: after mixing at the ratio of 20g/ml, shaking and culturing for 4d to obtain the hydrogen peroxide aged phenolic resin micro plastic.
Example 5: the difference from example 1 is: the micro plastic is made of hydrogen peroxide aged phenolic resin; the preparation method of the hydrogen peroxide aged phenolic resin micro plastic comprises the following steps: mixing phenolic resin micro plastic and hydrogen peroxide according to a mass-volume ratio of 2: mixing at the ratio of 50g/ml, and performing shaking culture for 20 days to obtain the hydrogen peroxide aged phenolic resin micro plastic.
Example 6: the difference from example 1 is: the micro plastic is made of hydrogen peroxide aged phenolic resin; the preparation method of the hydrogen peroxide aged phenolic resin micro plastic comprises the following steps: mixing phenolic resin micro plastic and hydrogen peroxide according to a mass volume ratio of 3: mixing at a ratio of 80g/ml, and performing shaking culture for 42d to obtain the hydrogen peroxide aged phenolic resin micro plastic.
Example 7: the difference from example 1 is: the micro plastic is ozone aged phenolic resin micro plastic; the preparation method of the ozone aging phenolic resin micro plastic comprises the following steps: continuously aging the phenolic resin micro plastic for 20 hours in an ozone environment to obtain ozone-aged phenolic resin micro plastic; ozone-aged phenolic resin microplastics are also mediated by the production of hydrogen peroxide to oxidize arsenic.
Example 8: the difference from example 1 is: the micro plastic is ozone aged polystyrene micro plastic; the preparation method of the ozone-aged polystyrene micro plastic comprises the following steps: continuously aging the polystyrene micro plastic for 20 hours in an ozone environment to obtain ozone-aged polystyrene micro plastic; ozone-aged polystyrene microplastics also mediate arsenic oxidation by producing hydrogen peroxide.
Application example 1: the method for evaluating the electron losing capacity of the micro plastic by the oxidation rate of the trivalent arsenic of the micro plastic based on the embodiments 1-8 can be applied to treatment of arsenic polluted water bodies;
the method for treating the water body polluted by arsenic comprises the following steps:
the method comprises the following steps: pretreatment of water body polluted by arsenic
Collecting water body polluted by arsenic, and filtering to remove large impurities;
step two: detection of arsenic content
Measuring the content of trivalent arsenic in the pretreated water body by using an atomic fluorescence spectrophotometer;
step three: treatment of
According to the determination of the content of trivalent arsenic in the water body, phenolic resin micro plastic is added into the water body to be treated according to the amount of 0.1g/L of trivalent arsenic added for treating 1mg/L of trivalent arsenic, and then the water body is repaired for 20 hours under the condition that the pH value is 5.
Application example 2:
the method for treating the arsenic polluted water body specifically comprises the following steps:
the method comprises the following steps: pretreatment of water body polluted by arsenic
Collecting water bodies polluted by arsenic, and filtering to remove large impurities;
step two: detection of arsenic content
Measuring the content of trivalent arsenic in the pretreated water body by using an atomic fluorescence spectrophotometer;
step three: treatment of
According to the determination of the content of trivalent arsenic in the water body, phenolic resin micro plastic is added into the water body to be treated according to the amount of 1g/L of trivalent arsenic to be treated, and then the water body is repaired for 22 hours under the condition that the pH value is 7.
Application example 3:
the method for treating the arsenic polluted water body specifically comprises the following steps:
the method comprises the following steps: pretreatment of water body polluted by arsenic
Collecting water body polluted by arsenic, and filtering to remove large impurities;
step two: detection of arsenic content
Measuring the content of trivalent arsenic in the pretreated water body by using an atomic fluorescence spectrophotometer;
step three: treatment of
According to the content of the trivalent arsenic in the water body, phenolic resin micro-plastic is added into the water body to be treated according to the amount of 2g/L of the trivalent arsenic with the concentration of 1mg/L, and then the water body is repaired for 25 hours under the condition that the pH value is 9.
Application example 4:
the method for treating the water body polluted by arsenic comprises the following steps:
the method comprises the following steps: pretreatment of water body polluted by arsenic
h, collecting water bodies polluted by arsenic, and filtering to remove large impurities;
step two: detection of arsenic content
Measuring the content of trivalent arsenic in the pretreated water body by using an atomic fluorescence spectrophotometer;
step three: preparation of restorations
Mixing phenolic resin micro plastic and hydrogen peroxide according to a mass volume ratio of 1: after mixing at the ratio of 20g/ml, performing shaking culture for 4d to obtain hydrogen peroxide aged phenolic resin micro plastic, namely the restoration;
step four: treatment of
According to the determination of the content of trivalent arsenic in the water body, adding a restoration material into the water body to be treated according to the amount of 0.1g/L of trivalent arsenic added for treating 1mg/L of trivalent arsenic, and then restoring for 20 hours under the condition that the pH value is 5.
Application example 5:
the method for treating the water body polluted by arsenic comprises the following steps:
the method comprises the following steps: pretreatment of water body polluted by arsenic
h, collecting water bodies polluted by arsenic, and filtering to remove large impurities;
step two: detection of arsenic content
Measuring the content of trivalent arsenic in the pretreated water body by using an atomic fluorescence spectrophotometer;
step three: preparation of restorations
Mixing phenolic resin micro plastic and hydrogen peroxide according to a mass volume ratio of 1: after mixing at the ratio of 35g/ml, carrying out shaking culture for 10 days to obtain hydrogen peroxide aged phenolic resin micro plastic which is a restoration;
step four: treatment of
According to the determination of the content of trivalent arsenic in the water body, adding a repairing substance into the water body to be treated according to the amount of 1.2g/L of trivalent arsenic for treating 1mg/L, and then repairing for 22 hours under the condition that the pH value is 7.
Application example 6:
the method for treating the water body polluted by arsenic comprises the following steps:
the method comprises the following steps: pretreatment of water body polluted by arsenic
Collecting water body polluted by arsenic, and filtering to remove large impurities;
step two: detection of arsenic content
Measuring the content of trivalent arsenic in the pretreated water body by using an atomic fluorescence spectrophotometer;
step three: preparation of restorations
Mixing phenolic resin micro plastic and hydrogen peroxide according to a mass volume ratio of 3: mixing the materials in a ratio of 80g/ml, and performing shaking culture for 42d to obtain hydrogen peroxide aged phenolic resin micro plastic which is a restoration;
step four: treatment of
According to the determination of the content of trivalent arsenic in the water body, adding a restoration material into the water body to be treated according to the amount of adding 2g/L of trivalent arsenic for treating 1mg/L, and then restoring for 25 hours under the condition that the pH value is 9.
Application example 7:
the method for treating the arsenic polluted water body specifically comprises the following steps:
the method comprises the following steps: pretreatment of water body polluted by arsenic
Collecting water bodies polluted by arsenic, and filtering to remove large impurities;
step two: detection of arsenic content
Measuring the content of trivalent arsenic in the pretreated water body by using an atomic fluorescence spectrophotometer;
step three: preparation of restorations
Continuously aging the phenolic resin micro plastic for 20 hours in an ozone environment to obtain ozone aged phenolic resin micro plastic which is the restoration;
step four: treatment of
According to the determination of the content of trivalent arsenic in the water body, adding a repairing substance into the water body to be treated according to the amount of 1.5g/L of trivalent arsenic for treating 1mg/L, and then repairing for 22 hours under the condition that the pH value is 7.
Application example 8:
the method for treating the water body polluted by arsenic comprises the following steps:
the method comprises the following steps: pretreatment of water body polluted by arsenic
Collecting water bodies polluted by arsenic, and filtering to remove large impurities;
step two: detection of arsenic content
Measuring the content of trivalent arsenic in the pretreated water body by using an atomic fluorescence spectrophotometer;
step three: preparation of restorations
Continuously aging the polystyrene micro plastic for 20 hours in an ozone environment to obtain ozone-aged polystyrene micro plastic which is a restoration;
step four: treatment of
According to the content of the trivalent arsenic in the water body, adding a restoration material into the water body to be treated according to the amount of 1g/L of the trivalent arsenic to be treated, and then restoring for 20 hours under the condition that the pH value is 9.
Application example 9:
it should be noted that: in practical application, the content of arsenic in the water body can be detected, and whether the water body contains the micro plastic can also be detected, if the water body contains the micro plastic and the arsenic pollutants, the micro plastic can be repaired only by carrying out aging treatment on the micro plastic according to the method for carrying out aging treatment on the micro plastic in the embodiment of the invention.
Experimental example 1:
simulation experiments were performed based on the methods described in the examples. The specific test steps are as follows: 40mg of the microplastic powder was weighed into a 100mL Erlenmeyer flask, and 20mL of a solution containing 1mg/L of trivalent arsenic was added, the pH of the solution being controlled by the addition of 50mM phosphate buffer.
The following processing groups were set: trivalent arsenic; micro plastic + trivalent arsenic; micro plastic, trivalent arsenic and methanol; micro plastic, trivalent arsenic and catalase; placing the triangular flask into a shaking box for shaking culture; samples were taken at 0, 1, 2, 4, 6, 10h, filtered through a 0.22 micron filter, and the filtrate was stored with 0.2M hydrochloric acid, followed by determination of trivalent and total arsenic content in the solution using atomic fluorescence photometer. Wherein, the micro-plastics are respectively tested by adopting hydrogen peroxide aged phenolic resin micro-plastics, ozone aged phenolic resin micro-plastics and ozone aged polystyrene micro-plastics.
When the micro plastic adopts hydrogen peroxide aged phenolic resin micro plastic:
as shown in FIGS. 1 and 2, trivalent arsenic cannot be oxidized in the culture flask without the addition of the micro-plastic, but the addition of the micro-plastic of the phenolic resin can promote the rapid oxidation of the micro-plastic. And the longer the micro-plastic ages, the faster it mediates arsenic oxidation. When the reaction is carried out in an oxygen-free environment, the rate of the micro plastic arsenic oxide is very slow, indicating that oxygen is involved in the micro plastic arsenic oxide.
As shown in FIG. 3, after adding methanol to quench hydroxyl radicals in the reaction solution, arsenic oxidation was not affected, while arsenic oxidation was completely inhibited by adding catalase.
As shown in fig. 4, by detecting hydrogen peroxide in the solution, it was found that hydrogen peroxide could be continuously generated in the solution.
FIGS. 1-4 show that phenolic functional groups and semiquinone radicals on the surface of a micro-plastic react with oxygen to generate hydrogen peroxide, thereby oxidizing arsenic.
When the micro plastic adopts ozone aging phenolic resin micro plastic:
as shown in figures 5 and 6, after the phenolic resin micro plastic is aged by ozone, the mediation effect of the phenolic resin micro plastic on arsenic oxidation is obviously improved, and the arsenic oxidation rate is from 0.099h -1 Lifting to 0.460h -1 Corresponding electron loss capacity of from 0.292mmol e - g -1 Increase to 0.628mmol e - g -1 。
When the micro plastic is ozone-aged polystyrene micro plastic:
as shown in FIGS. 6 and 7, the original polystyrene micro-plastic PS can not obviously oxidize trivalent arsenic, and the ozone aged polystyrene micro-plastic PS-O after ozone aging 3 Can obviously mediate arsenic oxidation at the rate of 0.043h -1 The electron loss capacity of the corresponding ozone-aged polystyrene micro-plastic is 0.0572mmol e - g -1 。
Experimental example 2:
and carrying out a simulation experiment based on the method of the application example. The specific test steps are as follows: the method comprises the steps of directly selecting or preparing the restorations described in the embodiments 1-8, weighing 40mg of the restorations, putting the restorations into a 100mL triangular flask, adding 20mL of a solution containing 1mg/L of trivalent arsenic, controlling the pH of the solution by adding 50mM of phosphate buffer solution, and respectively setting a control group. Placing the triangular flask into a shaking box for shaking culture. Sampling at a given time, filtering the sample through a 0.22-micron filter membrane, preserving the filtrate by using 0.2M hydrochloric acid, and then measuring the trivalent and total arsenic content in the solution by using an atomic fluorescence spectrophotometer;
wherein, the preparation of the restoration specifically comprises the following steps:
1) hydrogen peroxide aged phenolic resin micro plastic: weighing 3g of phenolic resin micro plastic, filling the phenolic resin micro plastic into a glass bottle, adding 80mL of hydrogen peroxide, carrying out shaking culture at 150rpm, and reacting for 0, 4, 8, 12, 19, 26 and 42 days respectively to prepare micro plastic with different hydrogen peroxide aging degrees, wherein the micro plastic is named as PF-0, PF-4, PF-8, PF-12, PF-19, PF-26 and PF-42 respectively. It should be noted that: PF-0 is phenolic resin micro plastic.
2) Oxygen-aged phenolic resin micro plastic: 5g of phenolic resin micro plastic is weighed into a 250mL serum bottle for useThe butyl rubber plug seals the serum bottle, and two syringe needles are inserted into the rubber plug and respectively used as an air inlet and an air outlet; starting an ozone generator, connecting the generated ozone to an air inlet through a hose, ventilating for 20h to prepare the ozone-aged phenolic resin micro plastic named as PF-O 3 . It should be noted that: the ozone concentration was 25ppm and was fed in at 0.5L/min.
3) Ozone-aged polystyrene micro plastic: putting the purchased granular polystyrene plastic into a ball milling tank for ball milling for 10 hours to obtain powdery polystyrene micro plastic; weighing 5g of polystyrene micro plastic in a 250mL serum bottle, sealing the serum bottle by using a butyl rubber plug, and inserting two syringe needles on the rubber plug to respectively serve as an air inlet and an air outlet; turning on an ozone generator, connecting the generated ozone to an air inlet through a hose, and ventilating for 20h to prepare ozone-aged polystyrene micro plastic named PS-O 3 . It should be noted that: the ozone concentration was 25ppm and was fed in at 0.5L/min.
As shown in FIG. 9, trivalent arsenic cannot be oxidized in the culture flask without the addition of the micro-plastic, and the micro-plastic can be promoted to be rapidly oxidized after the addition of the phenolic resin micro-plastic and the hydrogen peroxide-aged phenolic resin micro-plastic; the longer the micro plastic is aged, the faster the micro plastic mediates arsenic oxidation; wherein CK is a control group, specifically a treatment group with arsenic only and no restoration.
As shown in fig. 10, when the reaction was carried out in an oxygen-free environment, the rate of arsenic oxidation was slower for the phenolic resin microplastics and the hydrogen peroxide aged phenolic resin microplastics; wherein CK is a control group, specifically a treatment group with only arsenic and no restoration.
As shown in fig. 11, after adding methanol to quench hydroxyl radicals in the reaction solution, arsenic oxidation was not affected, while arsenic oxidation was completely inhibited after adding catalase; wherein CK is a control group, specifically a treatment group with arsenic only and no restoration.
As shown in fig. 12, by detecting hydrogen peroxide in the solution, it can be seen that hydrogen peroxide can be continuously generated in the solution;
FIGS. 8 to 12 conclude that: phenol resin microplastic and hydrogen peroxide aged phenol resin microplastic surface phenolic functional groups and semiquinone radicals generate hydrogen peroxide by reaction with oxygen, thereby oxidizing arsenic.
As shown in fig. 13 and 14, the mediation effect of the ozone-aged phenolic resin micro-plastic on arsenic oxidation is significantly improved, and the results of the radical quenching reaction and the detection of hydrogen peroxide indicate that the ozone-aged phenolic resin micro-plastic mediates arsenic oxidation by generating hydrogen peroxide; wherein CK is a control group, specifically a treatment group with only arsenic and no restoration.
FIGS. 15 and 16 show that the original polystyrene micro-plastic PS can not oxidize the trivalent arsenic obviously, but PS-O is aged by ozone 3 The results of the free radical quenching reaction and the hydrogen peroxide detection show that the ozone-aged polystyrene micro plastic mediates arsenic oxidation by generating hydrogen peroxide; wherein CK is a control group, specifically a treatment group with arsenic only and no restoration.
Claims (4)
1. A method for evaluating the electron losing capability of a micro plastic through the oxidation rate of trivalent arsenic of the micro plastic is characterized by comprising the following steps: uniformly mixing the micro plastic and a solution containing trivalent arsenic with the concentration of 0.25-1 mg/L according to the mass-to-volume ratio of 1-2 mg/ml, and then carrying out shake culture in an aerobic environment; sampling for 0, 1, 2, 4, 6 and 10 hours, filtering with a 0.22 micron filter membrane, storing the filtrate with 0.2M hydrochloric acid, then measuring the content of trivalent arsenic and total arsenic by an atomic fluorescence spectrophotometer, and calculating the oxidation rate of arsenic according to the change condition of the concentration of trivalent arsenic along with the reaction time for estimating the electron loss capability of the micro-plastic;
the micro plastic is aged micro plastic; the aged micro plastic is any one of aged phenolic resin micro plastic or aged polystyrene micro plastic; the aged phenolic resin micro plastic is hydrogen peroxide aged phenolic resin micro plastic; the aged phenolic resin micro plastic is ozone aged phenolic resin micro plastic; the aged polystyrene micro plastic is ozone aged polystyrene micro plastic.
2. The method for evaluating the electron-losing capability of the micro-plastic according to the oxidation rate of trivalent arsenic of the micro-plastic, which is claimed in claim 1, wherein the hydrogen peroxide aged phenolic resin micro-plastic is prepared by the following steps: mixing phenolic resin micro plastic and hydrogen peroxide according to a mass volume ratio of 1-3: and mixing the materials in a ratio of 20-80 g/ml, and performing shaking culture for 4-42 d to obtain the hydrogen peroxide aged phenolic resin micro plastic.
3. The method for evaluating the electron losing capability of the micro plastic through the oxidation rate of trivalent arsenic by the micro plastic according to claim 1, wherein the ozone aged phenolic resin micro plastic is prepared by the following steps: and (3) continuously aging the phenolic resin micro plastic for 20-22 h in an ozone environment to obtain the ozone-aged phenolic resin micro plastic.
4. The method for evaluating the electron losing capability of the micro plastic through the oxidation rate of trivalent arsenic by the micro plastic according to claim 1, wherein the ozone aging polystyrene micro plastic is prepared by the following steps: and (3) continuously aging the polystyrene micro plastic for 20-22 h in an ozone environment to obtain the ozone-aged polystyrene micro plastic.
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| JP2007185604A (en) * | 2006-01-13 | 2007-07-26 | Japan Atomic Energy Agency | Synthesizing method of anionic adsorbent having zirconium residue and adsorbent obtained thereby |
| JP2009039666A (en) * | 2007-08-09 | 2009-02-26 | Dowa Metals & Mining Co Ltd | Method of treating arsenic by using resin, and method of transporting/storing arsenic-containing compound and arsenic |
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| CN109231484B (en) * | 2018-09-30 | 2021-05-07 | 中南大学 | Method for treating wastewater containing trivalent arsenic by organic matter and microorganism |
| CN110204030B (en) * | 2019-05-23 | 2020-11-24 | 华中科技大学 | Method for oxidizing trivalent arsenic in underground water by using biochar |
| CN110426444A (en) * | 2019-07-30 | 2019-11-08 | 浙江工业大学 | Micro- plastic degradation is detected in the process to the method for heavy metal adsorption and release characteristics based on ICP-MS |
| CN112577805B (en) * | 2019-09-27 | 2022-09-13 | 香港城市大学深圳研究院 | Method for separating micro plastic from sediment rich in organic matters |
| CN111398003A (en) * | 2020-04-30 | 2020-07-10 | 山东省科学院海洋仪器仪表研究所 | Digestion solution for digesting organic impurities in micro-plastic, preparation method thereof and digestion method based on digestion solution |
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| JP2009039666A (en) * | 2007-08-09 | 2009-02-26 | Dowa Metals & Mining Co Ltd | Method of treating arsenic by using resin, and method of transporting/storing arsenic-containing compound and arsenic |
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