CN102921374B - Adsorbing material capable of removing dissolved heavy metal in road runoff - Google Patents
Adsorbing material capable of removing dissolved heavy metal in road runoff Download PDFInfo
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- CN102921374B CN102921374B CN201210341957.3A CN201210341957A CN102921374B CN 102921374 B CN102921374 B CN 102921374B CN 201210341957 A CN201210341957 A CN 201210341957A CN 102921374 B CN102921374 B CN 102921374B
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- heavy metal
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- cymbopogon citratus
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Abstract
The invention discloses an adsorbing material capable of removing dissolved heavy metal in road runoff. The adsorbing material is prepared by the following steps of: 1) stirring lemon grass until the lemon grass is crushed; 2) carbonizing the crushed lemon grass by using a hydrothermal autoclave; and 3) drying the carbonized lemon grass by using an air oven, and sieving by using a screen of which the pore diameter is 2mm to obtain the carbonized lemon grass of which the particle size is less than or equal to 2mm, namely the adsorbing material capable of removing the dissolved heavy metal in the road runoff. The adsorbing material is high in capacity of adsorbing dissolved Cu, Zn, and Cd ions in the road runoff.
Description
Technical field
The invention belongs to Phytochemistry, adsorption science and pavement runoff process field, be specifically related to the sorbing material of solubilised state heavy metal in a kind of highway runoff.
Background technology
Study and show both at home and abroad, due to the impact of atmosphere dried wet deposition, the advance factors such as middle vehicle and ground surface material, expressway surface runoff contains the pollutants such as a considerable amount of suspended solids, organic pollution, nitrogen and phosphorous nutrient, heavy metal, polycyclic aromatic hydrocarbon and oils.These pollutants are in line to be received after environment and will be had a strong impact on the self-purification function of environmental system, the welding ecological balance, and the difficult degradation pollutant such as heavy metal finally also may enter human body by food chain, harm humans living safety.
Highway runoff heavy metal is mainly derived from atmospheric sedimentation and road surface deposit etc.The atmospheric wet deposition of rainwater drip washing when dry deposition when atmospheric sedimentation comprises fine day and rainfall.When fine day, in atmosphere, heavy metal can be deposited on road surface by modes such as sedimentations, and they mainly come from the weathering migration of topsoil and industry, enterprise's discharge etc.When rainy day, atmosphere heavy metal is migrated to earth's surface with the suspended particulate of its adhesion by rainfall drip washing.Roadbed subsidence thing contains various heavy pollutant, and mostly is traffic activity and causes as institutes such as automotive emission, fuel drop out, vehicle and tire wear, road degeneration, pavement garbage, pavement preservations.
Visible, pavement runoff heavy metal pollution belongs to pollution of area source, and in general heavy metal pollution kind is many, concentration is high, and change in time and space is large, and discharge rule complexity, is polluted the features such as lasting at strong toxicity.Runoff heavy metal concentration is obviously different with the difference of rainfall, rainfall intensity, air pollution index etc.Also there is larger difference in the runoff heavy metal concentration of same catchment different location.
Pavement runoff heavy metal contaminants is of a great variety, complicated component; Comprise copper (Cu), zinc (Zn), plumbous (Pb), cadmium (Cd), chromium (Cr), nickel (Ni) and mercury (Hg) etc.Table 1 has been listed the maximum range of the pavement runoff heavy metal event mean concentrations (Event Mean Concentrations, EMCs) of domestic and international some scholars monitoring.
Pavement runoff Heavy Metals can be divided into solubilised state (<0.45 μ m) and particulate form (>0.45 μ m), most research shows that Cu in pavement runoff, Zn, Cd exist mainly with solubilised state, and Pb, Hg etc. exists mainly with particulate form.
Solubilised state heavy metal has stronger biology to property, easily absorbed by aquatile, enter human body enrichment by approach such as food chains, after reaching finite concentration, will produce toxic action to human body, and particulate form heavy metal can be present in water body sediment equally lastingly, change solubilised state under certain condition into and enter water environment.Therefore, pavement runoff heavy metal is in line to be received after environmental system and will be produced lasting pollution, and particularly the pollution of solubilised state heavy metal is more direct.
At present, more extensive for the research of pavement runoff treatment process both at home and abroad, overview gets up to mainly contain vegetation control, delaying basin, filtration system, oxidation pond, wet land system etc.Although these several treatment process have advantages of separately all do not possess the features such as flexible, removable, and change difficulty, after accumulating over a long period, easily become new pollution sources.Up to now, researcher is not too much absorbed in the removal of highway runoff solubilised state heavy metal.Therefore, in highway runoff, the absorption of solubilised state heavy metal research has become one of pavement runoff pollution control important research content urgently to be resolved hurrily.
Lemon grass (Cymbopogon citratus) is grass family, is herbaceos perennial, evergreen all the year round, and well developed root system has blue or green fragrance, and 300～500 meters of height above sea level, 5～40 degree Celsius can growth and breeding.It is rich in citronellal, geraniol, nerol, the fragrant ethyl ester of acetic acid, citral, d-citronellol, L-lemon alkene, L-Borneol etc.In dry lemon grass (Cymbopogon citratus), contain 1～2% essential oil, essential oil is mainly made up of citral (neral and spiceleaf isomer).For many years, lemon grass (Cymbopogon citratus) through refinement be usually applied in the fields such as food, cosmetics, medicine, bring good economy, society and environmental benefit, but in prior art also not using the application of sorbing material in water treatment after lemon grass (Cymbopogon citratus) modification.
Summary of the invention
Technical problem: the present invention is directed to highway runoff heavy metal pollution state and prior art deficiency thereof, the sorbing material of solubilised state heavy metal in a kind of removal highway runoff that can effectively remove solubilised state heavy metal, the recycling of realizing lemon grass (Cymbopogon citratus) and highway runoff Heavy Metal Pollution is provided.
Technical scheme: the sorbing material of solubilised state heavy metal in removal highway runoff of the present invention, is prepared by following methods:
1) lemon grass (Cymbopogon citratus) is blended;
2) adopt hydro-thermal autoclave to carry out charing processing to the lemon grass (Cymbopogon citratus) blending, concrete grammar is as follows: temperature is risen to 180～220 ℃ by the speed with 25～30 ℃/min, protect constant temperature 60～70min, then after hydro-thermal autoclave is completely cooling, can obtain charing lemon grass (Cymbopogon citratus);
3) with air-oven, charing lemon grass (Cymbopogon citratus) is dried, then adopting aperture is that the screen cloth of 2mm sieves, and obtains the charing lemon grass (Cymbopogon citratus) that particle diameter is not more than 2mm, is the sorbing material of removing solubilised state heavy metal in highway runoff.
Beneficial effect: the present invention compared with prior art, has the following advantages:
For effectively solving the limitation of above sorbing material, the present invention utilizes charring process, and lemon grass (Cymbopogon citratus) is carried out to charing.Do like this ease of solubility substance not only making in lemon grass (Cymbopogon citratus) and fully removed, avoid the adsorbent take plant as raw material to cause secondary pollution to water quality; Also changed the surface nature of lemon grass (Cymbopogon citratus), effectively improved the removal efficiency of solubilised state heavy metal simultaneously.In addition, sorbing material of the present invention is charing particle, is convenient in actual applications recycling, and these have solved existing vegetalitas sorbing material easily causes water pollution once again problem to recycling rate variance, precipitate.
1. the present invention utilizes charing means to prepare sorbing material, different from existing preparation method, have simple to operate, transformation efficiency advantages of higher, the less pollution that simultaneously preparation process causes, has possessed the condition of cleaner production.
2. the present invention adopts this plant of lemon grass (Cymbopogon citratus), draw materials conveniently, cheap, also can with combine as other industries such as pharmacy, can effectively utilize the refuse after relevant industries activity in production, avoided because of in existing sorbing material preparation process to raw-material a large amount of wastes, reached the object that resource-conserving is produced.
3. the present invention adopts the sorbing material of charing lemon grass (Cymbopogon citratus) after treatment as solubilised state heavy metal in highway runoff, compared with existing liquid-type sorbing material, can be applied in existing runoff treatment device, do like this and can effectively improve the removal effect of solubilised state heavy metal, greatly reduce runoff and received the risk of toxicity of environment, solved existing treating apparatus dissolved pollutant is removed to not good difficult problem.
Accompanying drawing explanation
Fig. 1 is the removal effect figure of the sorbing material prepared of embodiment 1 to heavy metal.
Fig. 2 is the removal effect figure of the sorbing material prepared of embodiment 2 to heavy metal.
Fig. 3 is the adsorption effect figure of the sorbing material prepared of embodiment 3 to heavy metal.
Fig. 4 is the forward and backward Fu Shi conversion infrared spectrum comparison diagram of the sorbing material adsorbing metal of preparation in undressed lemon grass (Cymbopogon citratus) and embodiment 2.
Fig. 5 is the effect comparison diagram of embodiment 3 gained sorbing material absorption mixed solutions and actual pavement runoff heavy metal.
The specific embodiment
Below in conjunction with drawings and Examples, the present invention is further described.
The sorbing material of solubilised state heavy metal in removal highway runoff of the present invention, is prepared by following methods:
1) lemon grass (Cymbopogon citratus) is blended;
2) adopt hydro-thermal autoclave to carry out charing processing to the lemon grass (Cymbopogon citratus) blending, concrete grammar is as follows: temperature is risen to 180～220 ℃ by the speed with 25～30 ℃/min, insulation 60～70min, then after hydro-thermal autoclave is completely cooling, can obtain charing lemon grass (Cymbopogon citratus);
3) with air-oven, charing lemon grass (Cymbopogon citratus) is dried, then adopting aperture is that the screen cloth of 2mm sieves, and obtains the charing lemon grass (Cymbopogon citratus) that particle diameter is not more than 2mm, is the sorbing material of removing solubilised state heavy metal in highway runoff.
25 ℃ of the prepared sorbing materials of the inventive method, rotating speed is 200rpm, and dosage is 2g/L, and pH is 5.5, and adsorption time is in the time of 100min, and the clearance of solubilised state heavy metal Cu, Zn, Cd can reach more than 90%.In the actual rainfall runoff of processing, in pavement runoff, most dissolved pollutant concentration is all in the allowed band of relevant criterion.CLG removes the efficiency of actual pavement runoff heavy metal ion all a little less than the efficiency of removing heavy metal ion in mixed solution.
The present invention makes full use of lemon grass (Cymbopogon citratus), and after charing modification, as the sorbing material of highway runoff solubilised state heavy metal Cu, Zn, Cd, it possesses good adsorption capacity, can obtain good adsorption effect.
The preparation and the absorption property that are below the sorbing material of solubilised state heavy metal in removal highway runoff of the present invention detect the explanation of testing.
Material is prepared: adopt respectively the pure Copper dichloride dihydrate (CuCl of top grade
22H
2o, Merck), zinc chloride (ZnCl
2, Fluda), Cadmium sulfate hydrate (3CdSO
48H
2o, Merck) prepare the storing solution of heavy metal Cu, Zn and Cd solution.Required test material (lemon grass (Cymbopogon citratus)) is all bought in Singapore supermarket.
Obtain solution: adopt 250ml conical flask as reaction vessel, carry out respectively the test of relation between pH value, quantity of sorbent and time of equilibrium adsorption and heavy metal removal.In single heavy metal solution and mixture-metal solution, Cu, Zn and Cd concentration are 10mg/L.Adsorbent mass is known.Use 0.1M HCl and 0.1M NaOH solution that heavy metal solution pH value is changed in 3 to 7 scopes.The conical flask that fills heavy metal solution and adsorbent is placed on shaking table, and vibrates some hours under 200rpm, 25 ℃ of conditions.Then, use 0.45 μ m water system membrane filtration mixed liquor.Finally, use the concentration of heavy metal ion to be measured in ICP-OES analysis-e/or determining filtrate.
Pavement runoff sampling and feature thereof: use vinyon bottle respectively at the mixed sample that has gathered three catchment pavement runoffs between in July, 2011 to December from Singapore inscription on ancient bronze objects Tai Lu.Adopt the collected water sample of 0.45 μ m water system membrane filtration to remove the particle in water sample.Adopt ICP-OES analyzer to measure filtering light metal ion (Na, K, Ca and Mg) in rear water sample and the concentration of heavy metal ion (Cu, Zn and Cd).Adopt QUITCHEM8500 type ion chromatograph to measure the anion concentration (NO filtering in rear water sample
3-, PO
4 3-, Cl-and SO
4 2-).Adopt the intelligent acidometer of pH-110 standard to measure runoff water sample pH value.Setting the water sample of collecting July is No. 1 water sample, and the water sample that collect September is No. 2 water samples, and the water sample that collect December is No. 3 water samples.The concentration of runoff pH value, solubilised state metal ion and anion is as shown in table 2.
PH value, solubilised state metal ion and anion concentration in table 2 pavement runoff
Embodiment 1: adopt preparation method of the present invention to obtain the charing lemon grass (Cymbopogon citratus) of carbon containing 75%, adopt domestic stirrer to blend lemon grass (Cymbopogon citratus), then adopt hydro-thermal autoclave (Pall Corporation of the U.S., 500ml) carry out charing processing, reaction condition is as follows: the speed with 30 ℃/min rises to temperature 200 ℃ rapidly, then constant temperature 1 hour, cool the temperature to again reactor completely cooling after, can obtain respectively charing lemon grass (Cymbopogon citratus) (CLG), finally dried under 60 ℃ of conditions by air-oven, and to adopt aperture be that the stainless steel sift of 2mm sieves, finally obtain the sorbing material that particle diameter is all not more than 2mm highway runoff solubilised state heavy metal.
Adsorption test:
Prepared by embodiment 1 sorbing material add respectively 10mg/L Cu solution, 10mg/L Zn solution, 10mg/L and Cu, Zn, Cd concentration to be in 10mg/L mixture-metal solution, under given pH value of solution=6.0, quantity of sorbent 2g/L and time of contact 180min condition to solution in Cu, Zn and Cd carry out adsorption test.
Embodiment 2: adopt preparation method of the present invention to obtain the charing lemon grass (Cymbopogon citratus) of carbon containing 80%, wherein the reaction condition of charing processing is as follows: the speed with 25 ℃/min rises to temperature 220 ℃ rapidly, then constant temperature 70min, cool the temperature to again reactor completely cooling after, can obtain respectively charing lemon grass (Cymbopogon citratus).
Adsorption test:
Sorbing material prepared by embodiment 2 adds respectively 10mg/L Cu solution, 10mg/L Zn solution, 10mg/L and Cu, Zn, Cd concentration to be in 10mg/L mixture-metal solution, under given pH value of solution=6.0, quantity of sorbent 2g/L and time of contact 180min condition to solution in Cu, Zn and Cd carry out adsorption test.
Embodiment 3: adopt preparation method of the present invention to obtain the charing lemon grass (Cymbopogon citratus) of carbon containing 85%, wherein the reaction condition of charing processing is as follows: the speed with 27 ℃/min rises to temperature 180 ℃ rapidly, then constant temperature 65min, cool the temperature to again reactor completely cooling after, can obtain respectively charing lemon grass (Cymbopogon citratus).
Adsorption test:
Sorbing material prepared by embodiment 3 adds respectively 10mg/L Cu solution, 10mg/L Zn solution, 10mg/L and Cu, Zn, Cd concentration to be in 10mg/L mixture-metal solution, under given pH value of solution=6.0, quantity of sorbent 2g/L and time of contact 180min condition to solution in Cu, Zn and Cd carry out adsorption test.
Can find by above three embodiment: the charing lemon grass (Cymbopogon citratus) that phosphorus content is higher is better to the removal effect of heavy metal.
The sorbing material of drying again after sorbing material prepared by lemon grass (Cymbopogon citratus) raw material, embodiment 3 and Adsorption of Heavy Metals mixes with the ratio of 1:100 with KBr respectively, then mixture being placed in to agate mortar grinds, again by abrasive material 10 tons of pressure lower compression 5min with form material sheet, finally at 400～4000cm
-1under wave number, measure the FTIR collection of illustrative plates of these three kinds of contrast materials.
Lemon grass (Cymbopogon citratus) raw material collection of illustrative plates is 3388.9,2922.1,2360.9,1726.3,1610.6,1514.1,1249.9,1037.7,896.9 and 669.3cm
-1there is peak value in place; This shows that initial lemon grass (Cymbopogon citratus) surface contains several functions group.The larger 3200cm of scope in collection of illustrative plates
-1to 3600cm
-1there is larger absorption peak in section, may be overlapping relevant with the collection of illustrative plates of O-H key or N-H key; This with the collection of illustrative plates of indication alcohol C-O key and C-N key in 1249,1037cm
-1place's peak value is corresponding.Visible, should there is hydroxyl and amino group in lemon grass (Cymbopogon citratus) surface.1610.6,1726.3cm
-1the peak value at place shows that the C=O key in carboxyl and aliphatic group may be present in lemon grass (Cymbopogon citratus).2922.1,1514.1cm
-1the peak value at place shows the material that in lemon grass (Cymbopogon citratus), existence contains c h bond and N-H key.
CLG contains on surface several functions group.The larger 3200cm of scope in collection of illustrative plates
-1to 3600cm
-1there is stronger absworption peak in section, may be overlapping relevant with the collection of illustrative plates of O-H key or N-H key, in this and collection of illustrative plates 1249,1037cm
-1place's indication alcohol C-O key is corresponding with the peak value of C-N key.Wherein, in CLG collection of illustrative plates at 3417.9cm
-1place's absworption peak is the highest, in CLG 1161.1,1112.9cm
-1the peak value at place is all relevant to alcohol C-O key.In CLG collection of illustrative plates 1205.5,1058.9,1033.6cm
-1the peak value at place is at 1274.9cm
-1peak value all in CLG collection of illustrative plates relevant to aralkyl C-O key at 1631.8cm
-1the peak value at place is at 1606.7cm
-1all all there is significant change to the CLG collection of illustrative plates after the relevant Adsorption of Heavy Metals of carboxyl anion C=O key compared with before absorption in the peak value at place.After Adsorption of Cu, Zn, Cd and hybrid metal, in CLG collection of illustrative plates at 1631.8cm
-1the peak value of place's indication carboxyl anion C=O key is transferred to respectively 1629.8cm
-1(single heavy metal) and 1627.9cm
-1(mixture-metal) located; At 1427.3cm
-1the peak value of place's indication carboxylic acid O-H key is all transferred to 1425.4cm
-1place.Meanwhile, in FTIR collection of illustrative plates, indicate the peak value of the collection of illustrative plates lap of O-H key or N-H key also all to change, but the concrete group changing is difficult to be determined equally.Visible, carboxyl, hydroxyl and amino groups Adsorption of Heavy Metals that CLG mainly relies on surface to exist.
In highway runoff, solubilised state heavy metal is compared with common solubilised state heavy metal, its SS concentration compared with high, pollutant levels change in time and space is large, these suspended particulates will affect the surface nature of sorbing material, reduce the contact area of itself and solubilised state heavy metal, thereby have affected adsorption effect.A difficult problem for heavy metal ion adsorbing material maximum is just to reclaim rate variance and secondary pollution problems at present.
Charing lemon grass (Cymbopogon citratus) prepared by embodiment 3 is applied in actual pavement runoff, and result as shown in Figure 5.Although the efficiency that CLG removes actual pavement runoff heavy metal ion all, a little less than removing heavy metal ion in mixed solution, still has obvious removal to actual pavement runoff heavy metal.
Experimental result shows, the prepared phosphorus content of the inventive method is 75%, 80% and 85% sorbing material under given pH value of solution=6.0, quantity of sorbent 2g/L and time of contact 180min condition time, the clearance of solubilised state heavy metal Cu, Zn, Cd can basic guarantee more than 80%.
In the actual rainfall runoff of processing, this sorbing material is removed the efficiency of actual pavement runoff heavy metal ion all a little less than the efficiency of removing heavy metal ion in mixed solution, but still can control its dissolved pollutant concentration all in the allowed band of relevant criterion.
Visible, the present invention makes full use of lemon grass (Cymbopogon citratus), and after charing modification, as the sorbing material of highway runoff solubilised state heavy metal Cu, Zn, Cd, it possesses good adsorption capacity, can obtain good adsorption effect.
Claims (1)
1. a sorbing material of removing solubilised state heavy metal in highway runoff, is characterized in that, this sorbing material is prepared by following methods:
1) lemon grass (Cymbopogon citratus) is blended;
2) adopt hydro-thermal autoclave to carry out charing processing to the lemon grass (Cymbopogon citratus) blending, concrete grammar is as follows: temperature is risen to 180 ~ 220 ℃ by the speed with 25 ~ 30 ℃/min, insulation 60 ~ 70 min, then after hydro-thermal autoclave is completely cooling, can obtain charing lemon grass (Cymbopogon citratus);
3) with air-oven, charing lemon grass (Cymbopogon citratus) is dried, then adopting aperture is that the screen cloth of 2mm sieves, and obtains the charing lemon grass (Cymbopogon citratus) that particle diameter is not more than 2mm, is the sorbing material of removing solubilised state heavy metal in highway runoff.
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