CN103332768A - Method for synchronously removing arsenite and arsenate from water - Google Patents
Method for synchronously removing arsenite and arsenate from water Download PDFInfo
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Abstract
The invention belongs to the field of water quality purification, and discloses a method for synchronously removing arsenite and arsenate from water. In the method, a low-cost iron scrap is used as an electrode material; after an electrode is electrified to be electrolyzed, ferrous ions (Fe(II)) are continuously slowly generated in the water to be treated, and the ferrous ions Fe(II) generate an intermediate state oxidizing agent with dissolved oxygen contained in the water through a series of oxidation processes so that As(III) is promoted to be oxidized and become As(V); in addition, the ferrous ions Fe(II) are oxidized to form a nascent state uncertain iron oxide the formula of which is formed by Fe-OH and a triple bond connected with Fe; As(V) is adsorbed through the iron oxide with above formula; and the nascent state iron oxide with adsorbed arsenic is separated from the water. The method disclosed by the invention is a high-efficiency method based on electrochemistry, is economic, effective and simple in step, can complete the oxidation, adsorption and muddy water separation of the arsenite in one reaction tank and can be used for removing the arsenite and the arsenate from underground water and also be suitable for controlling arsenic-containing industrial wastewater.
Description
Technical field
The invention belongs to environment protection, water-treatment technology field, relate to the method for removing arsenic in the water.
Background technology
As(arsenic) being distributed in widely in the earth's crust, is the high malicious carcinogenic substance of generally acknowledging, it is widely used in making Insecticides (tech) ﹠ Herbicides (tech), semiconductor material, sanitas and fodder additives etc.These use approach are incorporated into a large amount of arsenic in the environment, have increased concentration and the distribution range of As in environment water.In the world wide, the Arsenic Contamination in Groundwater problem is just threatening the health that surpasses 1.4 hundred million populations, has been considered to one of the widest water quality safety problem of influence.
EPA, the World Health Organization and China all are down to 10 μ g/L to the maximum permissible concentration of arsenic in the tap water from 50 μ g/L, and the limit value of arsenic still keeps 50 μ g/L in the small-sized centralized water supply in China rural area and the water dispersion type.Yet the result of Environmental Sanitation Inst., China Preventive Medical Science Academy shows that the concentration of arsenic surpasses 5,500,000 greater than the exposure population of 50 μ g/L in the Drinking Water in China.Therefore, seek cheapness, efficient, to pollute few Removal of Arsenic in Drinking Water technology extremely urgent.
Two kinds of common oxidation state of arsenic are respectively the arsenite (As (III)) of trivalent and the arsenate (As (V)) of pentavalent.As in the underground water (III) often accounts for more than the 67-99% of total As.The toxicity of As (III) is than As(V) high 60 times, and when pH was positioned at neutral range, As (III) was mainly with molecule (H
3AsO
3) form exist, be difficult for being removed, therefore, need earlier As(III usually) be oxidized to easy removed As(V), again by methods such as sorption-coprecipitations with As(V) remove, complex procedures is invested higher.Therefore, to adsorb integrated arsenic removal technology imperative in the exploitation oxidation.
Find have the removal method of arsenic in the water to mainly contain following several through the literature search to prior art:
(1) to remove be that (Yao Juanjuan etc. were Chinese water supply and drainage 2007 years for one of modal arsenic removal technology to the molysite coagulation, VOl.23(21), the 15-18 page or leaf, " the emergency handling process research of the former water of arsenic contamination " delivered), this method shows that the molysite coagulation can effectively remove arsenate (As(V)), for As(III) remove undesirable, under the situation 10 times of former water As content overproofs and 50 times, can't be by the throwing amount that improves coagulating agent with the control of water outlet A s (III) concentration below 10 μ g/L.This is that As (III) is mainly with H because in the neutral pH scope
3AsO
3Form exist, in order to remove the A s (III) in the water effectively, must take the preoxidation measure, therefore can bring treatment step loaded down with trivial details, problems such as equipment manufacturing cost height.
(2) Tang Yulin etc. is at " Characteristics and model studies for fluoride and arsenic adsorption on goethite " (Environ Sci-China 2010,22 (11), 1689-1694), use commercial pyrrhosiderite that arsenic is adsorbed, but maximum adsorption capacity has only 0.941mg/g, and loading capacity is not satisfactory, need expend a large amount of medicaments, both uneconomical, also easily bring serious secondary pollution.
(3) Chinese patent application number: 200810226082.6, patent name is: electrochemical reactor and the method for removing arsenic and fluorine contaminant in the water simultaneously, this patent readme is: " can remove fluorine and arsenic contamination in the water simultaneously ", but what this method was used is the iron plate electrode, price is higher relatively, and the inhomogeneous local perforations that causes of electrolysis may occur and cause the utilization ratio of iron plate lower; In addition, the specific surface area of iron plate electrode is less, and operating power consumption is relatively also higher.
(4) also compared gac among " Removal of Arsenic in Drinking Water technical study new development " (process water and waste water, 2007,38(4) 1-5) that Yao Juanjuan etc. delivers, sorbing materials such as zeolite find that its adsorptive power is all quite limited.
The removal technology of other arsenic all exists expense than problems such as height as ion-exchange, film processing etc.
Summary of the invention
The objective of the invention is at prior art treatment effect or the relatively poor characteristics of economy, propose a kind ofly to use cheap iron plane flower as electrode materials, remove As(III in the water synchronously based on electrochemical method) and water treatment method As(V).This invention can effectively overcome the poor removal effect that exists in the prior art, cost height, defective such as secondary pollution is big.
For realizing goal of the invention, the technical solution adopted in the present invention is:
The method of the method for arsenite and arsenate in a kind of synchronous removal water,
In pending water, facilitate following reaction:
Fe(II)+O
2→O
2 .-+Fe(III) （1）
Fe(II)+O
2 .-+2H+→Fe(III)+H
2O
2 （2）
Fe (II)+H
2O
2→ intermediate state oxygenant (3)
As (III)+intermediate state oxygenant → As (V) (4)
≡Fe-OH+As→≡Fe-As (5)
That is: in pending water, add ferrous ion (Fe(II)), make ferrous ion Fe(II) generate the intermediate state oxygenant with dissolved oxygen in the water through serial oxidising process, impel As(III) oxidation becomes As(V); Simultaneously, ferrous ion Fe(II) oxidation formation nascent state ambiguity ferriferous oxide ≡ Fe-OH, by the As(V of ≡ Fe-OH) adsorb, will be adsorbed with the nascent state ferriferous oxide of arsenic by separating in the water.
Further, adopt the iron plane flower to make electrode, the electrolysis of in pending water, switching on, iron plane flower anode loses electronics and generates ferrous ion Fe(II).
After by stirring the nascent state ferriferous oxide that is adsorbed with arsenic fully being flocculated, realize solid-liquid separation, the oxidation of integrated realization arsenic, absorption and solid-liquid separation by precipitation.
Adopt the method realization of filtering to be adsorbed with the separation of the nascent state ferriferous oxide of arsenic.
Spending crosslinked compression to make density iron plane is 200-500g/dm
3The modularization electrode.
The pH value of adjusting pending water before the electrolysis is 7.0-8.5, and the strength of current during electrolysis is 0.01-0.2A.
Electrolysis stops the back and continue to stir 1-2h and reach adsorption equilibrium to arsenic.
Adopt 1-2mg/L in the aluminate coagulating of aluminium the nascent state ferriferous oxide that is adsorbed with arsenic to be separated, sedimentation time is 1-2h, to reach corresponding water outlet requirement.
Described aluminium salt is aluminum chloride or Tai-Ace S 150.
Further specifically:
(1) iron plane being spent crosslinked compacting make density is 200-500g/dm
3The modularization electrode;
(2) the pH value of adjusting pending water before the electrolysis is 7.0-8.5, and the strength of current during electrolysis is 0.01-0.2A, and generally speaking, it is more high As(III) to account for total arsenic ratio, and the strength of current value is more low, and it is more low As(III) to account for total arsenic ratio, and the strength of current value is more high; It is definite that the electrolysis required time needs the selected parameter of basis and initial arsenic concentration and target to go out water concentration, and generally speaking, the pH value is more high, and the electrolysis required time is more short, and strength of current is more low, and the electrolysis required time is more long, can determine definite electrolysis time by testing.
(3) during electrolysis, strength of current during electrolysis is 0.01-0.2A, iron plane flower anode loses electronics and slowly generates ferrous ion (Fe(II) continuously), Fe(II) can with water in dissolved oxygen generate intermediate state oxygenant (shown in (1)-(3)) through serial oxidising process, impel As(III) oxidation becomes As(V) (formula (4)); Simultaneously, Fe(II) oxidation forms nascent state ambiguity ferriferous oxide (representing with ≡ Fe-OH), and ≡ Fe-OH can be to As(V) efficiently adsorb (formula (5)), thereby reach As(III) and the purpose of synchronous removal As(V);
Fe(II)+O
2→O
2 .-+Fe(III) （1）
Fe(II)+O
2 .-+2H+→Fe(III)+H
2O
2 （2）
Fe (II)+H
2O
2→ intermediate state oxygenant (3)
As (III)+intermediate state oxygenant → As (V) (4)
≡Fe-OH+As→≡Fe-As (5)
(4) need after electrolysis stops to continue to stir the adsorption equilibrium that 1-2h guarantees arsenic, generally speaking, pH is more high as this moment, and it is shorter then to continue churning time; PH is lower as this moment, then continues to stir longer;
(5) adopt 1-2mg/L aluminium salt (in aluminium) coagulation that the nascent state ferriferous oxide that is adsorbed with arsenic is separated at last, sedimentation time is 1-2h, can select according to the supernatant liquor opacity, and is higher as supernatant liquor liquid opacity, proper extension sedimentation time then is to reach corresponding water outlet requirement.
Allow as economic condition, also can adopt the high efficiency separation of the method realization nascent state ferriferous oxide of filtration.
Owing to adopted aforesaid method, the present invention to have the following advantages and beneficial effect:
Can select lathe waste material iron plane flower for use as the iron plane flower of electrode materials among the present invention, the electrode materials iron plate that cost is conventional etc. is saved over half.Iron plane flower specific surface area is big, and resistance is less during electrolysis, so the power consumption in the operational process is also lower than iron plate etc.The intermediate state oxygenant that generates in the electrolytic process As(III in can oxidizing water), form the easier As(V that is adsorbed removal), improved the removal efficient of arsenic.The high 10-1000 of loading capacity of the more conventional sorbent material of nascent state ferriferous oxide that produces in the electrolytic process times, a spot of ferriferous oxide can be realized the removal preferably of arsenic, not only saves cost, also brings less secondary pollutions such as mud.Present invention can be implemented in the oxidation, absorption and the solid-liquid separation that realize arsenic in the reaction tank, not only removal effect is good, and expenses such as capital construction are also lower, further reduced the processing cost of arsenic-containing water.
Description of drawings
Fig. 1 is the synoptic diagram of a kind of embodiment of the present invention.
Wherein 1 is iron plane flower electrode module, and 2 is stirring rake, and 3 is motor, and 4 is power supply, and 5 is water inlet pipe, and 6 is chemical feed pipe, and 7 is rising pipe, and 8 is shore pipe, and 9 is bucket.
Embodiment
The present invention is described in further detail below in conjunction with the accompanying drawing illustrated embodiment.
At first advance pending water by 5 pairs for the treatment of systems of water inlet pipe, spend electrode module 1 as electrode with iron plane simultaneously, connect 4 pairs of system's energisings of power supply and produce the active iron oxide compound, and open motor 3 and stir by stirring rake 2, treat that water stops into water after adding to design water level, and continue to switch on, deenergization 4 stops energising producing the active iron oxide compound of enough concentration when system after, and 1-2h is stirred in continuation, the back adds aluminium salt by chemical feed pipe 6, as aluminum chloride, coagulating sedimentation effect by aluminium salt is carried out precipitation separation to bucket 9 to ferriferous oxide, and supernatant liquor (water of namely having handled well) carries out spoil disposal by shore pipe 8 at last by rising pipe 7 outputs, this moment, system finished one action, can carry out the processing of next cycle.
The present invention is very desirable to the removal effect of the arsenic contamination in the underground water, is particularly suitable for the solution of the Arsenic Contamination in Groundwater problem of economically underdeveloped areas such as rural area.In addition, also be applicable to Industrial Wastewater Treatment.
Certain underground water, initial As(III) and content As(V) be respectively 450 μ g/L and 0 μ g/L, calcium ion content 56mg/L, phosphate radical 1.9mg/L, silicate 22mg/L, the pH value is 7.0.Electric current is under the 0.05A, slowly behind stirring and the energising 35min, add 2mg/L Tai-Ace S 150 after stopping energising and continuing to stir 120min, and stir l min fast it is mixed, after stirring 20min then at a slow speed it fully being flocculated, realize solid-liquid separation by precipitation, be purified water and discharge mud.The arsenic clearance is more than 90%, and the residue arsenic concentration meets the limit value (GB5049-2006) of arsenic in the small-sized centralized water supply in China rural area and the water dispersion type.
Laboratory water distribution, initial As(III) and content As(V) be respectively 0 μ g/L and 500 μ g/L, calcium ion content 200mg/L, magnesium ion content 100mg/L, silicate 40mg/L, the pH value is 8.Electric current is under the 0.05A, slowly stir and the 4min that switches on after, add 1mg/L Tai-Ace S 150 after stopping energising and continue stirring 60min, and stir l min fast it is mixed, after stirring 20min then at a slow speed it fully being flocculated, realize solid-liquid separation by precipitation, be purified water and discharge mud.The arsenic clearance is more than 90%, and the residue arsenic concentration meets the limit value (GB5049-2006) of arsenic in the small-sized centralized water supply in China rural area and the water dispersion type.
Laboratory water distribution, initial As(III) and content As(V) be respectively 0 μ g/L and 500 μ g/L, calcium ion content 200mg/L, magnesium ion content 100mg/L, phosphate radical 3mg/L, silicate 20mg/L, the pH value is 8.Electric current is under the 0.05A, slowly behind stirring and the energising 12min, add 2mg/L Tai-Ace S 150 after stopping energising and continuing to stir 60min, and stir l min fast it is mixed, after stirring 20min then at a slow speed it fully being flocculated, realize solid-liquid separation by precipitation, be purified water and discharge mud.The arsenic clearance is more than 90%, and the residue arsenic concentration meets the limit value (GB5049-2006) of arsenic in the small-sized centralized water supply in China rural area and the water dispersion type.
Initial As(III in the pending water) and content As(V) be respectively 0 μ g/L and 500 μ g/L, calcium ion content 200mg/L, magnesium ion content 100mg/L, phosphate radical 3mg/L, silicate 30mg/L, the pH value is 7.5.Electric current is under the 0.05A, slowly behind stirring and the energising 30min, add 1mg/L Tai-Ace S 150 after stopping energising and continuing to stir 80min, and stir l min fast it is mixed, after stirring 20min then at a slow speed it fully being flocculated, realize solid-liquid separation by precipitation, be purified water and discharge mud.The arsenic clearance is more than 98%, and the residue arsenic concentration meets Drinking Water in China hygienic standard (GB5749-2006).
Initial As(III in the pending water) and content As(V) be respectively 0 μ g/L and 3mg/L, calcium ion content 200mg/L, magnesium ion content 100mg/L, phosphate radical 3mg/L, silicate 30mg/L pH value is 8.Electric current is under the 0.2A, slowly stir and the 4min that switches on after, add 1mg/L Tai-Ace S 150 after stopping energising and continue stirring 60min, and stir l min fast it is mixed, after stirring 20min then at a slow speed it fully being flocculated, realize solid-liquid separation by precipitation, be purified water and discharge mud.The arsenic clearance is more than 90%.
Initial As(III in the pending water) and content As(V) be respectively 500 μ g/L and 0 μ g/L, calcium ion content 50mg/L, magnesium ion content 100mg/L, phosphate radical 3mg/L, silicate 30mg/L pH value is 8.Electric current is under the 0.1A, slowly behind stirring and the energising 14min, add 2mg/L Tai-Ace S 150 after stopping energising and continuing to stir 60-120min, and stir l min fast it is mixed, after stirring 20min then at a slow speed it fully being flocculated, realize solid-liquid separation by precipitation, be purified water and discharge mud.The arsenic clearance is more than 90%.The residue arsenic concentration meets the limit value (GB5049-2006) of arsenic in the small-sized centralized water supply in China rural area and the water dispersion type.
Certain underground water, initial As(III) and content As(V) be respectively 320 μ g/L and 110 μ g/L, calcium ion content 32mg/L, magnesium ion content 18mg/L, phosphate radical 2.8mg/L, silicate 11mg/L, the pH value is 6.3.At first regulate pH to 7.5, electric current is under the 0.2A, slowly behind stirring and the energising 40min, add 1.5mg/L Tai-Ace S 150 after stopping energising and continuing to stir 90min, and stir l min fast it is mixed, after stirring 20min then at a slow speed it fully being flocculated, realize solid-liquid separation by precipitation, be purified water and discharge mud.The arsenic clearance is more than 92%.The residue arsenic concentration meets the limit value (GB5049-2006) of arsenic in the small-sized centralized water supply in China rural area and the water dispersion type.
Initial As(III in the pending water) and content As(V) be respectively 500 μ g/L and 0 μ g/L, calcium ion content 50mg/L, magnesium ion content 50mg/L, phosphate radical 3mg/L, silicate 30mg/L, the pH value is 8.5.Electric current is under the 0.015A, slowly behind stirring and the energising 60min, add 2mg/L Tai-Ace S 150 after stopping energising and continuing to stir 100min, and stir lmin fast it is mixed, after stirring 20min then at a slow speed it fully being flocculated, realize solid-liquid separation by precipitation, be purified water and discharge mud.The arsenic clearance is more than 90%.The residue arsenic concentration meets the limit value (GB5049-2006) of arsenic in the small-sized centralized water supply in China rural area and the water dispersion type.
Certain trade effluent, initial As(III in the pending water) and content As(V) be respectively 3000 μ g/L and 1000 μ g/L, receive ion content 120mg/L, magnesium ion content 80mg/L, the pH value is 8.5.Electric current is under the 0.015A, slowly behind stirring and the energising 50min, add 1mg/L Tai-Ace S 150 after stopping energising and continuing to stir 120min, and stir lmin fast it is mixed, after stirring 20min then at a slow speed it fully being flocculated, realize solid-liquid separation by precipitation, be purified water and discharge mud.The arsenic clearance is more than 90%.
Find out that by above-described embodiment the present invention can remove As(III in the water synchronously) and As(V), handle underground water and can reach world health organization, the up-to-date drinking water standard of American National Environmental Protection Agency relevant criterion and China (GB5749 1).Also can be used for Industrial Wastewater Treatment, clearance is greater than 90%.
The above-mentioned description to embodiment is can understand and apply the invention for ease of those skilled in the art.The person skilled in the art obviously can easily make various modifications to these embodiment, and needn't pass through performing creative labour being applied in the General Principle of this explanation among other embodiment.Therefore, the invention is not restricted to the embodiment here, those skilled in the art are according to announcement of the present invention, and not breaking away from the improvement that category of the present invention makes and revise all should be within protection scope of the present invention.
Claims (9)
1. method of removing synchronously the method for arsenite and arsenate in the water is characterized in that:
In pending water, facilitate following reaction:
Fe(II)+O
2→O
2 .-+Fe(III) （1）
Fe(II)+O
2 .-+2H+→Fe(III)+H
2O
2 （2）
Fe (II)+H
2O
2→ intermediate state oxygenant (3)
As (III)+intermediate state oxygenant → As (V) (4)
≡Fe-OH+As→≡Fe-As (5)
That is: in pending water, add ferrous ion Fe(II), make ferrous ion Fe(II) generate the intermediate state oxygenant with dissolved oxygen in the water through serial oxidising process, impel As(III) oxidation becomes As(V); Simultaneously, ferrous ion Fe(II) oxidation formation nascent state ambiguity ferriferous oxide ≡ Fe-OH, by the As(V of ≡ Fe-OH) adsorb, will be adsorbed with the nascent state ferriferous oxide of arsenic by separating in the water.
2. method according to claim 1 is characterized in that: adopt the iron plane flower to make electrode, and the electrolysis of in pending water, switching on, iron plane flower anode loses electronics and generates ferrous ion Fe(II).
3. method according to claim 1 is characterized in that: after by stirring the nascent state ferriferous oxide that is adsorbed with arsenic fully being flocculated, realize solid-liquid separation, the oxidation of integrated realization arsenic, absorption and solid-liquid separation by precipitation.
4. method according to claim 1 is characterized in that: adopt the method realization of filtering to be adsorbed with the separation of the nascent state ferriferous oxide of arsenic.
5. method according to claim 2, it is characterized in that: spending crosslinked compression to make density iron plane is 200-500g/dm
3The modularization electrode.
6. method according to claim 2 is characterized in that: the pH value of adjusting pending water before the electrolysis is 7.0-8.5, and the strength of current during electrolysis is 0.01-0.2A.
7. method according to claim 2 is characterized in that: electrolysis stops the back and continues to stir 1-2h and reach adsorption equilibrium to arsenic.
8. method according to claim 3 is characterized in that: adopt 1-2mg/L in the aluminate coagulating of aluminium the nascent state ferriferous oxide that is adsorbed with arsenic to be separated, sedimentation time is 1-2h, to reach corresponding water outlet requirement.
9. method according to claim 8, it is characterized in that: described aluminium salt is aluminum chloride or Tai-Ace S 150.
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| CN107129018A (en) * | 2017-06-27 | 2017-09-05 | 中国科学院沈阳应用生态研究所 | The method for concentration of arsenic in a kind of arsenic-containing waste water |
| CN107311363A (en) * | 2017-08-22 | 2017-11-03 | 天津理工大学 | A kind of purification and reuse technology of the sour waste acid containing pozzuolite |
| CN112194279A (en) * | 2020-09-08 | 2021-01-08 | 天津大学 | Method for adsorbing arsenic in arsenic-containing wastewater |
| CN112194279B (en) * | 2020-09-08 | 2022-10-14 | 天津大学 | Method for adsorbing arsenic in arsenic-containing wastewater |
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| CN113461136B (en) * | 2021-09-06 | 2021-12-07 | 湖南博世科环保科技有限公司 | Method for treating organic industrial wastewater by using gamma-FeOOH catalyst |
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