CN115677017B - A pretreatment method for reverse osmosis desalination of seawater - Google Patents
A pretreatment method for reverse osmosis desalination of seawater Download PDFInfo
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Abstract
本发明公开了一种用于反渗透海水淡化的预处理方法。本发明的用于反渗透海水淡化的预处理方法，包括如下步骤：先将过一硫酸盐加入海水中反应2～6h，再将反应体系的pH调节至≥9.5，继续反应0.5～1.5h，即获得预处理后的海水；所述反应体系中过一硫酸盐的浓度为0.5～10mmol/L。本发明用于反渗透海水淡化的预处理方法，以过一硫酸盐与海水中的氯离子反应生成次氯酸，进而有效杀死海水中的微生物；同时通过调节反应体系的pH产生具有更强降解能力的单线态氧充分降解海水中的有机物，进而减轻反渗透处理负荷，维持稳定的出水渗透率，保持长时间稳定的渗透出水量，提高生产效率。
The present invention discloses a pretreatment method for reverse osmosis seawater desalination. The pretreatment method for reverse osmosis seawater desalination of the present invention comprises the following steps: firstly, peroxymonosulfate is added to seawater for reaction for 2 to 6 hours, then the pH of the reaction system is adjusted to ≥9.5, and the reaction is continued for 0.5 to 1.5 hours, so as to obtain pretreated seawater; the concentration of peroxymonosulfate in the reaction system is 0.5 to 10 mmol/L. The pretreatment method for reverse osmosis seawater desalination of the present invention uses peroxymonosulfate to react with chloride ions in seawater to generate hypochlorous acid, thereby effectively killing microorganisms in seawater; at the same time, singlet oxygen with stronger degradation ability is generated by adjusting the pH of the reaction system to fully degrade organic matter in seawater, thereby reducing the reverse osmosis treatment load, maintaining a stable effluent permeability, maintaining a long-term stable osmotic effluent, and improving production efficiency.
Description
Technical Field
The invention relates to the technical field of water treatment, in particular to a pretreatment method for reverse osmosis seawater desalination.
Background
Fresh water resource shortage is one of the important factors affecting human production and life, and sea water desalination increases an effective way of fresh water supply. Compared with other sea water desalination technologies, the reverse osmosis sea water desalination technology has the characteristics of low equipment investment, low energy consumption, short construction period, low water production cost, flexible water supply application and the like, and is widely applied to sea water desalination treatment.
However, a great amount of inorganic ions, suspended matters, organic matters, microorganisms and the like exist in the seawater, so that irreversible membrane pollution, including inorganic pollution, colloid pollution, organic pollution and biological pollution, is easily caused to a reverse osmosis membrane which is a key component in reverse osmosis seawater desalination treatment, thereby causing high energy consumption and high maintenance cost in the production process, further limiting the further development and application of reverse osmosis seawater desalination technology, especially biological pollution, being most difficult to control and having serious influence on the reverse osmosis membrane, and killing and inhibiting the growth of microorganisms by adding active chlorine or oxide are generally adopted at present.
For example, the prior art discloses a water treatment method for removing micro-pollutants by activating persulfate, which comprises the following steps: adding chloride or sulfate into a water body containing micro-pollutants, fully mixing, adding zero-valent iron powder into the water body, then adding persulfate into the water body, stirring and fully mixing to remove the micro-pollutants in the water body, wherein the chloride or sulfate is mainly used for improving the adsorption of the micro-pollutants on the surfaces of iron and iron oxides and promoting free radicals generated by activating persulfate on the surfaces of the iron and the iron oxides to kill the micro-pollutants, but research proves that even if the sterilization rate reaches 99%, the residual tiny microorganisms still can take the organic matters in the water as nutrient sources to grow and reproduce quickly, namely the traditional oxidation method is difficult to remove the microorganisms in the water effectively and thoroughly, so that development of a method capable of killing the microorganisms in the water is needed.
Disclosure of Invention
The invention aims to overcome the defect and the defect that the existing persulfate is difficult to effectively remove microorganisms in seawater, and provides a pretreatment method for reverse osmosis seawater desalination, wherein the method adopts the reaction of the persulfate and chloride ions in the seawater to generate hypochlorous acid, so that a persulfate-hypochlorous acid-chloride ion composite system is formed, and the microorganisms in the seawater are effectively killed; meanwhile, the pH value of the reaction system is regulated to enable part of peroxymonosulfate to be decomposed to generate singlet oxygen with stronger degradation capability, so that organic matters in seawater are fully degraded, and therefore, the residual extremely small amount of microorganisms are prevented from growing and propagating rapidly by taking the organic matters in the seawater, the cleanliness of a reverse osmosis membrane in the seawater desalination production process is further ensured, the reverse osmosis treatment load is lightened, the stable water permeability is maintained, the long-time stable osmotic water yield is maintained, and the production efficiency is improved.
The above object of the present invention is achieved by the following technical scheme:
The invention provides a pretreatment method for reverse osmosis sea water desalination, which comprises the following steps:
Adding peroxymonosulfate into seawater to react for 2-6 h, adjusting the pH value of a reaction system to be more than or equal to 9.5, and continuing to react for 0.5-1.5 h to obtain pretreated seawater;
wherein the concentration of the peroxymonosulfate in the reaction system is 0.5-10 mmol/L.
According to the invention, the peroxymonosulfate reacts with chloride ions in the seawater to generate hypochlorous acid to form a peroxymonosulfate-hypochlorous acid-chloride ion composite system, bacterial microorganisms in the seawater are effectively killed by the action of the hypochlorous acid, and then the pH value of the reaction system is regulated to enable part of peroxymonosulfate to be decomposed to generate singlet oxygen with stronger degradation capability so as to fully degrade organic matters in the seawater, thereby preventing the residual extremely small amount of bacterial microorganisms from rapidly growing and propagating by taking the organic matters in the seawater, further ensuring the cleanliness of a reverse osmosis membrane in the seawater desalination production process, reducing reverse osmosis treatment load, maintaining stable water permeability, maintaining long-time stable osmotic water yield and improving production efficiency.
When the reaction time of adding the peroxymonosulfate into the seawater is too short or the reaction time is too short after the pH is regulated, bacteria in the seawater are difficult to kill effectively, and organic pollutants in the seawater are difficult to degrade fully; when the pH is less than 9.5, singlet oxygen cannot be generated, and refractory organic matters in the seawater cannot be effectively degraded.
Preferably, the concentration of the peroxymonosulfate in the reaction system of the present invention is 1.5 to 5mmol/L.
Preferably, the pH of the reaction system according to the invention is between 9.5 and 10.
In a specific embodiment, the seawater of the present invention contains microorganisms, which are vibrio and/or marine heterotrophic bacteria.
In a specific embodiment, the number of bacterial colonies of the vibrio genus is 56-268 CFU.mL -1.
In a specific embodiment, the number of the bacterial colonies of the marine heterotrophic bacteria is 75-190 CFU.mL -1.
In a specific embodiment, the peroxymonosulfate in the peroxymonosulfate solution of the present invention is one or more of potassium peroxymonosulfate, sodium peroxymonosulfate, and ammonium peroxymonosulfate.
In a specific embodiment, the seawater has a total organic carbon content of 6.88-7.35, an oxidation-reduction potential of 78.1-98.7 mV, an actual salinity of 21.22-32.26 g/L, a turbidity of 2.55-44.11 NTU and a pH of 7.29-7.96.
Compared with the prior art, the invention has the following beneficial technical effects:
The pretreatment method for reverse osmosis seawater desalination of the invention uses the reaction of the peroxymonosulfate and the chloride ions in the seawater to generate hypochlorous acid, thereby forming a peroxymonosulfate-hypochlorous acid-chloride ion composite system, and further effectively killing microorganisms in the seawater; meanwhile, the pH value of the reaction system is regulated to enable part of peroxymonosulfate to be decomposed to generate singlet oxygen with stronger degradation capability, so that organic matters in seawater are fully degraded, and therefore, the residual extremely small amount of microorganisms are prevented from growing and propagating rapidly by taking the organic matters in the seawater, the cleanliness of a reverse osmosis membrane in the seawater desalination production process is further ensured, the reverse osmosis treatment load is lightened, the stable water permeability is maintained, the long-time stable osmotic water yield is maintained, and the production efficiency is improved.
Drawings
FIG. 1 is a schematic flow chart of the reverse osmosis sea water desalination process of natural sea water.
FIG. 2 is a graph showing the degradation rate of organic matters with time in examples 1 to 3 of the present invention.
FIG. 3 is an inactivation chart of Vibrio in examples 1 to 3 of the present invention.
FIG. 4 shows the inactivation patterns of heterotrophic sea bacteria in examples 1 to 3 of the present invention.
FIG. 5 is a graph showing the variation of the desalination permeation quantity with time of the present invention in example 1 and comparative example 4.
FIG. 6 shows the surface contamination of reverse osmosis membranes after desalination of sea water in example 1 and comparative example 4 of the present invention.
FIG. 7 shows the results of the detection of singlet oxygen produced by the addition of peroxomonosulfate to seawater at pH 10 according to the present invention.
Detailed Description
The invention will be further described with reference to the following specific embodiments, but the examples are not intended to limit the invention in any way. Raw materials reagents used in the examples of the present invention are conventionally purchased raw materials reagents unless otherwise specified.
Example 1
A pretreatment method for reverse osmosis seawater desalination, comprising the steps of:
Adding potassium persulfate into seawater to react for 4 hours, then adopting a sodium hydroxide solution with the concentration of 2mol/L to adjust the pH value of a reaction system to 10, and continuing to react for 1 hour to obtain pretreated seawater; the concentration of potassium peroxymonosulfate in the reaction system is 1.5mmol/L;
wherein, the main physical and chemical parameters of the seawater are shown in table 1:
TABLE 1
Example 2
A pretreatment method for reverse osmosis seawater desalination, comprising the steps of:
Adding potassium persulfate into seawater to react for 4 hours, then adopting a sodium hydroxide solution with the concentration of 2mol/L to adjust the pH value of a reaction system to 10, and continuing to react for 1 hour to obtain pretreated seawater; the concentration of potassium peroxymonosulfate in the reaction system is 1.5mmol/L;
wherein, the main physical and chemical parameters of the seawater are shown in table 2:
TABLE 2
Example 3
A pretreatment method for reverse osmosis seawater desalination, comprising the steps of:
Adding potassium persulfate into seawater to react for 4 hours, then adopting a sodium hydroxide solution with the concentration of 2mol/L to adjust the pH value of a reaction system to 10, and continuing to react for 1 hour to obtain pretreated seawater; the concentration of potassium peroxymonosulfate in the reaction system is 1.5mmol/L;
wherein, the main physical and chemical parameters of the seawater are shown in table 3:
TABLE 3 Table 3
Example 4
A pretreatment method for reverse osmosis seawater desalination, comprising the steps of:
Adding potassium persulfate into seawater to react for 4 hours, then adopting a sodium hydroxide solution with the concentration of 2mol/L to adjust the pH value of a reaction system to 10, and continuing to react for 1 hour to obtain pretreated seawater; the concentration of potassium peroxymonosulfate in the reaction system is 0.5mmol/L; wherein the seawater was the same as in example 1.
Example 5
A pretreatment method for reverse osmosis seawater desalination, comprising the steps of:
adding potassium persulfate into seawater to react for 4 hours, then adopting a sodium hydroxide solution with the concentration of 2mol/L to adjust the pH value of a reaction system to 10, and continuing to react for 1 hour to obtain pretreated seawater; the concentration of potassium peroxymonosulfate in the reaction system is 5mmol/L; wherein the seawater was the same as in example 1.
Example 6
A pretreatment method for reverse osmosis seawater desalination, comprising the steps of:
Adding potassium persulfate into seawater to react for 4 hours, then adopting a sodium hydroxide solution with the concentration of 2mol/L to adjust the pH value of a reaction system to 10, and continuing to react for 1 hour to obtain pretreated seawater; the concentration of potassium peroxymonosulfate in the reaction system is 10mmol/L; wherein the seawater was the same as in example 1.
Example 7
A pretreatment method for reverse osmosis seawater desalination, comprising the steps of:
Adding potassium persulfate into seawater to react for 4 hours, and then adopting a sodium hydroxide solution with the concentration of 2mol/L to adjust the pH value of a reaction system to 9.5, and continuing to react for 1 hour to obtain pretreated seawater; the concentration of potassium peroxymonosulfate in the reaction system is 1.5mmol/L; wherein the seawater was the same as in example 1.
Comparative example 1
A pretreatment method for reverse osmosis seawater desalination, comprising the steps of:
Adding potassium persulfate into seawater to react for 4 hours, then adopting a sodium hydroxide solution with the concentration of 2mol/L to adjust the pH value of a reaction system to 10, and continuing to react for 1 hour to obtain pretreated seawater; the concentration of potassium peroxymonosulfate in the reaction system is 0.1mmol/L; wherein the seawater was the same as in example 1.
Comparative example 2
A pretreatment method for reverse osmosis seawater desalination, comprising the steps of:
Adding potassium persulfate into seawater to react for 4 hours, and then adopting a sodium hydroxide solution with the concentration of 2mol/L to adjust the pH value of a reaction system to 8.5, and continuing to react for 1 hour to obtain pretreated seawater; the concentration of potassium peroxymonosulfate in the reaction system is 1.5mmol/L; wherein the seawater was the same as in example 1.
Comparative example 3
A pretreatment method for reverse osmosis seawater desalination, comprising the steps of:
Adding potassium peroxodisulfate into seawater for reaction for 4 hours, then adopting 2mol/L sodium hydroxide solution to adjust the pH value of a reaction system to 10, and continuing the reaction for 1 hour to obtain pretreated seawater; the concentration of the peroxymonosulfate in the reaction system is 1.5mmol/L; wherein the seawater was the same as in example 1.
Comparative example 4
A pretreatment method for reverse osmosis seawater desalination, comprising the steps of:
Stirring the seawater for 4 hours, adjusting the pH value of a reaction system to 10 by adopting a sodium hydroxide solution with the concentration of 2mol/L, and continuing to react for 1 hour to obtain pretreated seawater; wherein the seawater was the same as in example 1.
Result detection
The pretreated seawater obtained by the pretreatment methods for reverse osmosis seawater desalination of examples 1 to 7 and comparative examples 1 to 4 was subjected to performance test, and the specific test procedures are shown below, and the test results are shown in table 4.
(1) Organic pollutant degradation rate test
The specific test method comprises the following steps:
the content of organic pollutants in seawater is tested through the total organic carbon content, 50mL of real seawater is taken to be put into a clean beaker for stirring, peroxymonosulfate is added for starting timing, 10mL of seawater is taken out respectively at 0h,1h,2h and 4h, the total organic carbon content in the seawater is measured by using a TOC-L total organic carbon content tester, and the degradation rate of the organic pollutants is determined by comparing the total organic carbon content before and after degradation, wherein the specific calculation formula is as follows:
Organic pollutant degradation rate= (total organic carbon content before degradation-total organic carbon content after degradation)/total organic carbon content before degradation.
As can be seen from FIG. 2, after the peroxymonosulfate is added to the seawater in examples 1 to 3, the TOC degradation rate increases rapidly with the increase of the reaction time within 0 to 1 h; the TOC degradation rate is slightly increased within 1-4 h along with the increase of the reaction time and is basically unchanged. When the pH of the seawater is regulated to 10.0, the reaction is continued for 1 hour, the TOC degradation rate is obviously improved, namely, organic pollutants in the seawater are further degraded, and the influence of the pH of a reaction system on effectively degrading the organic pollutants in the seawater is fully illustrated.
(2) Colony count test
The specific test method comprises the following steps:
vibrio genus: 8mL of seawater is taken to be placed into a sterilizing test tube to be continuously vibrated, peroxymonosulfate is added to start timing, after the reaction time reaches 1h, 100 mu L of sample is taken out of the test tube to be uniformly coated on a thiosulfate-citrate-bile salt-sucrose agar culture medium flat plate, the process is repeated three times, the sample is placed into a constant temperature incubator at 30 ℃ to be cultured for 24h, then bacterial colonies appearing on the flat plate are manually counted, the average value of the bacterial colonies is calculated and recorded as N 1, and finally the bacterial colony number of vibrio in the seawater is obtained by the calculation formula:
The number of Vibrio colonies (CFU.mL -1)＝N1.times.10)
Marine heterotrophic bacteria: 8mL of seawater is taken to be placed into a sterilization test tube to be continuously vibrated, peroxymonosulfate is added to start timing, when the reaction time reaches 1h, 100 mu L of sample is taken out of the test tube to be uniformly coated on a marine broth agar culture medium flat plate, the process is repeated three times, the sample is placed into a constant temperature incubator at 37 ℃ to be cultured for 24h, then the colony appearing on the flat plate is manually counted, the average value of the count is recorded as N 2, and finally the bacterial colony number calculation formula of marine heterotrophic bacteria in the seawater is obtained:
Marine heterotrophic bacteria colony number (CFU.mL -1)＝N2. Times.10)
As can be seen from fig. 3 and 4, compared with untreated seawater, vibrio and marine heterotrophic bacteria present in the seawater treated with peroxymonosulfate are all killed, demonstrating that the pretreatment method of the present invention is a method that can be sterilized with high efficiency.
(3) Penetration test
The specific test method comprises the following steps:
Firstly, a reverse osmosis membrane is soaked in deionized water for 40 minutes and is installed in a clean sea water desalting device (shown in figure 1), wherein the cross section area of the membrane is 12.56cm 2, 300mL of sea water is added into the device, the fresh water is permeated from the bottom end of the device to be produced by providing 40bar of pressure through high-pressure nitrogen, the fresh water amount within 5 minutes is collected and weighed, the average value is repeatedly obtained three times and recorded as M, and the fresh water permeation amount of the system is obtained according to the following calculation formula:
The permeation quantity (L/M 2/h/bar) =m/1000/(12.56/10000)/(5/60)/40= 0.2388M.
As can be seen from fig. 5, the fresh water permeation rate of example 1 can be maintained stable and at a higher level for a long period of time as compared with comparative example 4, whereas in comparative example 4, since the pretreatment with monosulfate was not performed, the fresh water permeation rate was significantly reduced after 20 hours; as can be seen from fig. 6, the surface of the reverse osmosis membrane after the seawater is subjected to the dilute water production by using the peroxymonosulfate pretreatment is kept clean and is basically similar to the surface state of the original reverse osmosis membrane, and turbidity appears on the surface of the reverse osmosis membrane without pretreatment, which fully illustrates that the long-term cleanliness of the membrane can be maintained by adopting the peroxymonosulfate for the reverse osmosis seawater desalination pretreatment, and has positive significance in reducing the maintenance cost of the membrane components in actual production.
(4) Detection of singlet oxygen
The specific test method comprises the following steps:
50. Mu.L of TEMP or 10. Mu.L of DMPO was added to 1mL of seawater, 10. Mu.L of 150mol/L peroxymonosulfate was added thereto, the solution was sucked out by a capillary tube, and the solution was tested by an electron paramagnetic resonance apparatus.
As can be seen from fig. 7, with TEMP as the singlet oxygen scavenger, at pH 10.0, the addition of peroxymonosulfate to seawater when TEMP is added can produce a triplet peak with peak intensity of 1:1:1, which is due to singlet oxygen trapped by TEMP, whereas when peroxymonosulfate and seawater are present alone, there is no singlet oxygen present; in addition, when the pH is 8.5, no singlet oxygen is produced even if the peroxymonosulfate is added to seawater. In combination with the above results, it can be demonstrated that the pH adjustment to 10.0 in examples 1 to 3 can produce a further degradation effect due to the singlet oxygen produced, while demonstrating the importance of the peroxymonosulfate in the system.
TABLE 4 Table 4
As is clear from examples 1 and 4 to 6, the degradation effect on organic pollutants is gradually enhanced with an increase in the concentration of potassium persulfate, the sterilization effect on bacteria of the genus Vibrio and marine heterotrophic bacteria is maintained substantially stable, and the concentration of potassium persulfate is preferably 1.5 to 5mmol/L in consideration of the corrosive effect caused by potassium persulfate.
As is clear from examples 1, 7 and 2, the reaction system has good degradation effect on organic pollutants when the pH value is 9.5-10, and can effectively kill vibrio bacteria and marine heterotrophic bacteria; when the pH value of the reaction system is less than 9.5, organic pollutants cannot be effectively degraded, and residual organic pollutants can be used as nutrient substances to revive bacterial microorganisms, so that the fresh water transmittance is reduced; as is clear from comparative example 3, not only does organic contaminants fail to be degraded but also it is difficult to effectively kill Vibrio bacteria and marine heterotrophs using peroxodisulfate.
It is to be understood that the above examples of the present invention are provided by way of illustration only and not by way of limitation of the embodiments of the present invention. Other variations or modifications of the above teachings will be apparent to those of ordinary skill in the art. It is not necessary here nor is it exhaustive of all embodiments. Any modification, equivalent replacement, improvement, etc. which come within the spirit and principles of the invention are desired to be protected by the following claims.
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