CN105060455A - Natural pyrite based photocatalysis method for synergic removal of heavy metal-organic pollutants from water - Google Patents
Natural pyrite based photocatalysis method for synergic removal of heavy metal-organic pollutants from water Download PDFInfo
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Abstract
The invention discloses a natural pyrite based photocatalysis method for synergic removal of heavy metal-organic pollutants from water. The catalyst pyrite involved in the photocatalysis system is crushed, ground and sieved, and then composes a pyrite photocatalysis system together with ultraviolet. The pyrite photocatalysis technology involved in the invention can be applied to synergic removal of heavy metal Cr (VI) and organic matter malachite green from water. Under ultraviolet irradiation, the removal rates of malachite green and Cr (VI) can respectively reach 97% and 52%. The pyrite photocatalyst has good repeated use performance, can maintain good reaction activity after five times of repeated use, and is fully used. The catalytic reaction operation conditions involved in the reaction are simple, and the catalyst raw materials are cheap and easily available. Based on the pollution treatment concept of using waste to treat waste, the method provided by the invention has good application prospects.
Description
Technical field:
The present invention relates to the water treatment method containing heavy metal-organic contamination, be specifically related to a kind of photocatalytic method working in coordination with removal Heavy Metals in Waters-organic pollutant based on Natural pyrite.
Background technology:
At present, along with developing rapidly of industry, the quick raising of economic level, the material that the mankind ask for from nature and discharge also reaches unprecedented level, considerably beyond the capacity of environment itself, thus cause the havoc of Environment-Ecosystem, occur a series of problem of environmental pollution.In the face of environmental pollution situation severe at present, some are applied in current contaminated surrounding medium as traditional environment restoring methods such as chemical precipitation method, physisorphtion, chemical oxidization method, microorganism treatments, although these environment restoring methods all serve significant role to the current control of environmental pollution, these traditional environment remediation technology also exist all to some extent efficiency low, can not thoroughly environmental pollutant be removed or the new source of pollution of innoxious, easy generation; Or use operating restraint narrow, be only applicable to specific pollutent; Or energy consumption is too high, material cost is expensive, is not suitable for the limitation of the aspects such as large-scale promotion application.Thus, efficient, the less energy-consumption of exploitation, low cost, environment remediation Treatment process applied widely have become current scientific research environmental administration and have been badly in need of one of important topic solved.
But, a kind of extensive concern making light-catalysed technology more and more be subject to environmental worker, it is the emerging environment remediation Treatment process progressively grown up from 20 century 70s, it utilize semiconductor oxide materials under light illumination surface energy by the characteristic of activating signal activation, luminous energy is utilized to produce the free radical of strong oxidizing property, can oxygenolysis organism efficiently at short notice, or kill bacteria, elimination gas with foreign flavor, or produce the heavy metal ion of electron reduction high price, reduce the toxicity of heavy metal ion.Due to photocatalysis technology have simple to operate, reaction thoroughly, energy consumption cost is low, efficiency is high and the advantage of toxicological harmless, be considered to a kind of environment remediation Treatment process of most application prospect, be widely used in the repairing and treating field of various kinds environmental pollution medium.But the scavenging effect of photocatalysis technology is directly relevant to photocatalyst material, at present, TiO
2photocatalitic Technique of Semiconductor is considered to the most stable, the most ripe.Except TiO
2and material modified outside, other photocatalyst is as ZnO, Al
2o
3, SnO
2, Co
3o
4deng and various composite material photocatalyst be also widely used in environmental pollution repairing and treating field, and demonstrate good environment remediation effect.It is reported, pyrite (FeS
2) also can as a kind of photocatalytic semiconductor material, pyrite energy band structure determines it and has good photoelectric properties, existing relevant report pyrite being applied to catalyze and degrade organic pollutants.Moreover, pyrite particle also has good absorption property, pollutent absorption can be removed; in addition; pyrite also has stronger reductibility, heavy metal ion such as the Cr (VI) of high price can be reduced to Cr (III), reduce the toxicity of heavy metal ion.Therefore, have concurrently in oxidation and the environment remediation improvement in pollution medium of the pyrite of reduction characteristic and there is good application potential.
In fact, pyrite is metal sulfide ore the most common on the earth, and is prevalent in various ore and mine tailing, and the oxidation of this mineral discharges a large amount of iron ions and sulfuric acid, is the main cause that acid wastewater in mine is formed.And pyritous economic use value is cheap, be usually looked at as the waste minerals after mining ore dressing.But in recent years, a large amount of domestic and international investigators directly adopts or transforms waste material to thing of curbing environmental pollution, and obtain good effect by test.Environmental pollution improvement's theory of this " treatment of wastes with processes of wastes against one another " by refuse reclamation more and more gets more and more people's extensive concerning.As the pyrite of mine solid waste, the improvement aspect of environmental pollutant also should be applied in.
But current industrial pollution source mainly contains heavy metal and organism, heavy metal mainly contains chromium, lead and cadmium etc., and organism mainly contains phenol, chlorophenol and dyestuff etc.Pollution in actual environment is a kind of combined pollution of jointly existing of various heavy and organic contamination often, it is pollution type environment being produced to biggest threat that heavy metal-organic composite pollutes, under the situation of current rigorous, the environmental improvement of heavy metal-organic composite contamination characteristics is extremely urgent.Existing most of environment remediation technology is all by heavy metal or Organic pollutants water body for simple, therefore, strive to find a kind of efficient context restorative procedure simultaneously removing Heavy Metals in Waters-organic pollutant and become the most important subject under discussion of Environmental Science.Having photochemical catalytic oxidation and reduction characteristic concurrently based on pyrite semi-conductor, take pyrite as photocatalyst, collaborative removal Heavy Metals in Waters-organic pollutant under ultraviolet lighting, but up to the present, similar patented technology have not been reported.
Summary of the invention:
The object of this invention is to provide the Natural pyrite that utilizes that a kind of reaction conditions is simple, reaction is thorough, energy consumption cost is low, efficiency is high and can work in coordination with the photocatalysis method removing Heavy Metals in Waters-organic pollutant.The method can work in coordination with removal heavy metal Cr (VI) and organism malachite green effectively, and minimizing Cr (VI) and malachite green are to the harm of environment; And catalyzer pyrite has and reuses stability preferably, for the heavy metal-organic composite pollution law of complexity provides one " treatment of wastes with processes of wastes against one another " river harnessing ideas.
The photocatalytic method working in coordination with removal Heavy Metals in Waters-organic pollutant based on Natural pyrite of the present invention, it is characterized in that, concrete steps are as follows:
(1), first catalyzer pyrite is carried out fragmentation, grinds, sieved, make its particle radius within the scope of 20 ~ 40 μm;
(2) water pH value containing heavy metal Cr (VI) and organism malachite green, is regulated;
(3), under ultraviolet light conditions, to in the water body containing heavy metal Cr (VI) and organism malachite green, add the catalyzer pyrite that step (1) processed, react, redox is worked in coordination with and is removed Cr (VI) in water body and malachite green.
Preferably, the pH value of step (2) is 2 ~ 7.
Further preferably, the pH value of step (2) is 3.
The described water body containing heavy metal Cr (VI) and organism malachite green, preferably, the mass concentration of Cr (VI) is 2.5 ~ 30mg/L.
The described water body containing heavy metal Cr (VI) and organism malachite green, preferably, the mass concentration of malachite green is 30mg/L.
Ultraviolet light conditions described in step (3), preferably, ultraviolet ray intensity is 10 ~ 20W.
The catalyzer pyrite that adding described in step (3) processed, preferred dosage is 0.5 ~ 1.5g/L.
Carrying out described in step (3) reacts, and the reaction times is preferably 100 ~ 120min.
Concerted reaction principle of the present invention is: highly toxic Cr (VI) is converted into the low Cr of toxicity (III) by reductive action; Malachite green then destroys chromophore by oxygenizement and generates small organic molecule, and is finally converted into water and carbonic acid gas.Water pollution substrate concentration after associated treatment obtains and effectively reduces, and alleviates the pressure of subsequent disposal.
After being processed the water body containing heavy metal Cr (VI) and organism malachite green by method of the present invention, carry out centrifugal recovery to catalyzer pyrite, catalyzer pyrite reuses number of times can reach five times.
Compared with prior art, the present invention has the following advantages and beneficial effect:
1, reaction conditions is simple to operate: the present invention adds catalyzer pyrite in the water body containing Cr (VI) and malachite green, can remove under normal temperature and pressure effectively simultaneously;
2, processing cost is low: compared to other photocatalysts as TiO
2, the present invention's pyrite used is mine solid waste, and be cheaply easy to get, and treating processes is easy, the environmental improvement theory of the treatment of wastes with processes of wastes against one another, has a good application prospect;
3, reaction thoroughly: in 120min, malachite green achieves the degraded of more than 97%, and mineralising is carbonic acid gas and water effectively; Cr (VI) then has more than 52% to be converted into Cr (III), and toxicity obtains and effectively reduces;
4, be suitable for target compound scope wide: the present invention is not only applicable to the removal of the polluted-water containing Cr (VI) or malachite green, be also suitable for the removal of the polluted-water simultaneously containing Cr (VI) and malachite green.
Accompanying drawing illustrates:
Fig. 1 is different pH on the impact of Cr (VI) and malachite green removal effect;
Fig. 2 is different catalysts amount on the impact of Cr (VI) and malachite green removal effect;
Fig. 3 is the impact of different Pollutant levels comparison Cr (VI) and malachite green removal effect;
Fig. 4 be pyrite photochemical catalysis collaborative remove Cr (VI) and malachite green reuse effect;
Embodiment:
Following examples further illustrate of the present invention, instead of limitation of the present invention.
In the examples below, the concentration of Cr (VI) ion in water sample adopts diphenyl carbazide spectrophotometry to measure (GB7467-87): in Cr (VI) sample solution after 10mL dilution, add the sulphuric acid soln of 0.5mL1:1 and the phosphoric acid solution of 0.5mL1:1 respectively, shake up; Add 2mL200mg/L diphenylcarbazide solution again, shake up, colour developing 5 ~ 10min, at 540nm wavelength place, does reference with water, measures absorbancy.The clearance of Cr (VI) is calculated by absorbance.And the concentration of malachite green adopts ultraviolet visible spectrophotometry, be its clearance of change calculations that 618nm place measures absorbancy at wavelength.
Embodiment 1:
First catalyzer pyrite is carried out fragmentation, grinds, sieved, make its particle radius within the scope of 20 ~ 40 μm; Regulate the water pH value 2 ~ 7 containing heavy metal Cr (VI) and organism malachite green; Under ultraviolet light conditions, to in the water body containing 10mg/L heavy metal Cr (VI) and 30mg/L organism malachite green, add the catalyzer pyrite 1.0g/L processed, under 10 ~ 20W UV-irradiation, average rate is kept to stir, react, reaction 100 ~ 120min, redox is worked in coordination with and is removed Cr (VI) in water body and malachite green.The change of Cr (VI) and malachite green concentration in water body before and after assaying reaction.
In embodiment 1 result as shown in Figure 1, as seen from Figure 1, after reaction 120min, the clearance of Cr (VI) and malachite green presents downward trend along with the rising of pH, wherein, malachite green and Cr (VI) clearance when pH=3 the highest, reach 97.3% and 53.1% respectively.
Comparative example 1:
In this comparative example, adopt pyrite individual curing to contain the water body of malachite green as different from Example 1, add toward reactor the malachite green solution that concentration is 30mg/L, pH value of solution is adjusted to 3, and other condition is identical with embodiment 1.Comparative example 1 result is as shown in table 1, as can be seen from Table 1, during pyrite individual curing malachite green solution, the clearance of malachite green is 76.9%, and when removing Cr (VI) and malachite green at the same time, the existence that its clearance reaches 97.3%, Cr (VI) effectively facilitates the efficiency of pyrite photochemical catalysis malachite green, and Cr (VI) also can realize synchronous removal.
Comparative example 2:
In this comparative example, adopt pyrite individual curing to contain the water body of Cr (VI) as different from Example 1, add toward reactor Cr (VI) solution that concentration is 10mg/L, pH value of solution is adjusted to 3, and other condition is identical with embodiment 1.Comparative example 2 result is as shown in table 1, as can be seen from Table 1, during pyrite individual curing Cr (VI) solution, the clearance of Cr (VI) is 28.5%, and at removal Cr (VI) and malachite green compound tense, its clearance reaches 53.1%, and the existence of malachite green effectively facilitates the efficiency of pyrite photochemical catalysis Cr (VI), and malachite green also can realize synchronous high-efficiency removal.
Table 1. compares for the Cr (VI) under different technology conditions and malachite green removal effect
Embodiment 2:
Difference from Example 1 is, regulate the initial pH value of polluted-water to be 3, the pyritous dosage of catalyzer is 0.5 ~ 1.5g/L, the change of Cr (VI) and malachite green concentration in water body before and after assaying reaction.In embodiment 2 result as shown in Figure 2, as seen from Figure 2, after reaction 120min, the clearance of malachite green and Cr (VI) presents the trend of upper rising along with the increase of the dosage of pyrite photocatalyst, when dosage is 1.0g/L, the clearance of malachite green and Cr (VI) almost reaches maximum value, and when dosage is more than 1.0g/L, the clearance of malachite green and Cr (VI) no longer changes.
Embodiment 3:
Difference from Example 1 is, the concentration ratio that regulate malachite green and Cr (VI) is 12:1 ~ 1:1, the change of Cr (VI) and malachite green concentration in water body before and after assaying reaction.In embodiment 3 result as shown in Figure 3, as seen from Figure 3, after reaction 120min, the clearance of Cr (VI) declines along with the minimizing of concentration ratio, and the removal of malachite green takes the lead in rising along with the minimizing of concentration ratio, when concentration ratio is more than 3:1, the clearance of malachite green but declines along with the minimizing of concentration ratio.Therefore, when malachite green/Cr (VI) is for 3:1, the clearance of malachite green and Cr (VI) reaches maximum value respectively.
Embodiment 4:
Difference from Example 1 is, regulates the initial pH value of polluted-water to be 3, carries out recovery reuse for five times reacted pyrite, the change of Cr (VI) and malachite green concentration in water body before and after each assaying reaction.In embodiment 4 result as shown in Figure 4, as seen from Figure 4, when photochemical catalysis reuses first three time, catalyzer itself also maintains very high activity, and the clearance of malachite green and Cr (VI) maintains more than 95% and 51% level respectively.After the 4th time, all there is downward trend in both clearances, but after reusing the 5th time, the clearance of malachite green and Cr (VI) can also reach 76.5% and 39.4%, and pyrite keeps good catalytic activity.
Claims (8)
1. can work in coordination with the photocatalytic method removing Heavy Metals in Waters-organic pollutant based on Natural pyrite, it is characterized in that, concrete steps are as follows:
(1), first catalyzer pyrite is carried out fragmentation, grinds, sieved, make its particle radius within the scope of 20 ~ 40 μm;
(2) water pH value containing heavy metal Cr (VI) and organism malachite green, is regulated;
(3), under ultraviolet light conditions, to in the water body containing heavy metal Cr (VI) and organism malachite green, add the catalyzer pyrite that step (1) processed, react, redox is worked in coordination with and is removed Cr (VI) in water body and malachite green.
2. the photocatalytic method working in coordination with removal Heavy Metals in Waters-organic pollutant based on Natural pyrite according to claim 1, it is characterized in that, the pH value of step (2) is 2 ~ 7.
3. the photocatalytic method working in coordination with removal Heavy Metals in Waters-organic pollutant based on Natural pyrite according to claim 1 and 2, it is characterized in that, the pH value of step (2) is 3.
4. the photocatalytic method working in coordination with removal Heavy Metals in Waters-organic pollutant based on Natural pyrite according to claim 1, it is characterized in that, the described water body containing heavy metal Cr (VI) and organism malachite green, the mass concentration of Cr (VI) is 2.5 ~ 30mg/L.
5. the photocatalytic method working in coordination with removal Heavy Metals in Waters-organic pollutant based on Natural pyrite according to claim 1, it is characterized in that, the described water body containing heavy metal Cr (VI) and organism malachite green, the mass concentration of malachite green is 30mg/L.
6. the photocatalytic method working in coordination with removal Heavy Metals in Waters-organic pollutant based on Natural pyrite according to claim 1, it is characterized in that, the ultraviolet light conditions described in step (3), ultraviolet ray intensity is 10 ~ 20W.
7. the photocatalytic method working in coordination with removal Heavy Metals in Waters-organic pollutant based on Natural pyrite according to claim 1, it is characterized in that, the catalyzer pyrite that adding described in step (3) processed, dosage is 0.5 ~ 1.5g/L.
8. the photocatalytic method working in coordination with removal Heavy Metals in Waters-organic pollutant based on Natural pyrite according to claim 1, it is characterized in that, the carrying out described in step (3) reacts, and the reaction times is 100 ~ 120min.
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Cited By (11)
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| CN105458294A (en) * | 2016-01-18 | 2016-04-06 | 中国科学院南海海洋研究所 | Nanometer zero-valent iron prepared from iron in acid mine wastewater and preparing method and application thereof |
| CN106957078A (en) * | 2017-02-17 | 2017-07-18 | 湖南有色金属研究院 | A kind of method of the photocatalytic semiconductor sulphide ore degraded beneficiation wastewater Residuals based on iron-oxidizing bacterium |
| CN107611009A (en) * | 2017-08-30 | 2018-01-19 | 常州瑞坦商贸有限公司 | A kind of preparation method of zinc oxide composite semiconductor material |
| CN108439533A (en) * | 2018-05-03 | 2018-08-24 | 温州大学苍南研究院 | A method of the recycling synchronous with chromium of reduction composite drug joint treatment with ultraviolet light trivalent chromium complexing waste water |
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| CN112206790A (en) * | 2020-11-12 | 2021-01-12 | 厦门理工学院 | Preparation method and application of modified pyrite with photocatalytic performance |
| CN112642576A (en) * | 2020-09-17 | 2021-04-13 | 中南大学 | Selective oxidation and flotation separation method for pyrite gangue in sulfide ore |
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| CN113880218A (en) * | 2021-10-12 | 2022-01-04 | 中南大学 | Utilize organic dyestuff effluent disposal system of pyrite tailing |
| CN114702117A (en) * | 2022-05-20 | 2022-07-05 | 中国地质大学（北京） | Method for simultaneously removing heavy metals and organic pollutants from mine by using iron-containing solid waste |
| WO2023175163A1 (en) | 2022-03-18 | 2023-09-21 | Wageningen Universiteit | Process for the generation of hydrogen sulfide in the presence of pyrite as catalyst |
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| CN1040968A (en) * | 1988-09-06 | 1990-04-04 | 厦门大学 | A kind of method of photocatalysis treatment of waste water |
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| CN106957078A (en) * | 2017-02-17 | 2017-07-18 | 湖南有色金属研究院 | A kind of method of the photocatalytic semiconductor sulphide ore degraded beneficiation wastewater Residuals based on iron-oxidizing bacterium |
| CN106957078B (en) * | 2017-02-17 | 2020-06-12 | 湖南有色金属研究院 | Method for degrading residual agent in beneficiation wastewater by photocatalytic semiconductor sulfide ore based on iron-oxidizing bacteria |
| CN107611009A (en) * | 2017-08-30 | 2018-01-19 | 常州瑞坦商贸有限公司 | A kind of preparation method of zinc oxide composite semiconductor material |
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| CN108439533B (en) * | 2018-05-03 | 2020-07-28 | 温州大学苍南研究院 | Method for treating trivalent chromium complex wastewater by reducing composite medicament and combining ultraviolet light and synchronously recycling chromium |
| CN110918102A (en) * | 2019-12-10 | 2020-03-27 | 桂林理工大学 | Preparation method of graphene oxide modified metal sulfide composite photocatalyst |
| CN112642576A (en) * | 2020-09-17 | 2021-04-13 | 中南大学 | Selective oxidation and flotation separation method for pyrite gangue in sulfide ore |
| CN112206790A (en) * | 2020-11-12 | 2021-01-12 | 厦门理工学院 | Preparation method and application of modified pyrite with photocatalytic performance |
| CN112206790B (en) * | 2020-11-12 | 2022-04-22 | 厦门理工学院 | Preparation method and application of modified pyrite with photocatalytic performance |
| WO2022100226A1 (en) * | 2020-11-12 | 2022-05-19 | 厦门理工学院 | Method for preparing modified pyrite with photocatalytic performance and use thereof |
| CN113060817A (en) * | 2021-03-18 | 2021-07-02 | 中南大学 | Method for treating chromium-containing electroplating wastewater by using mineral modified material |
| CN113060817B (en) * | 2021-03-18 | 2022-08-16 | 中南大学 | Method for treating chromium-containing electroplating wastewater by using mineral modified material |
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| WO2023175163A1 (en) | 2022-03-18 | 2023-09-21 | Wageningen Universiteit | Process for the generation of hydrogen sulfide in the presence of pyrite as catalyst |
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