CN106492748B - A method of for heavy metal in water and polycyclic aromatic hydrocarbon collaboration efficient absorption removal - Google Patents
A method of for heavy metal in water and polycyclic aromatic hydrocarbon collaboration efficient absorption removal Download PDFInfo
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- CN106492748B CN106492748B CN201610895620.5A CN201610895620A CN106492748B CN 106492748 B CN106492748 B CN 106492748B CN 201610895620 A CN201610895620 A CN 201610895620A CN 106492748 B CN106492748 B CN 106492748B
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J20/00—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof
- B01J20/02—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising inorganic material
- B01J20/10—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising inorganic material comprising silica or silicate
- B01J20/16—Alumino-silicates
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J20/00—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof
- B01J20/28—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof characterised by their form or physical properties
- B01J20/28054—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof characterised by their form or physical properties characterised by their surface properties or porosity
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- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F1/00—Treatment of water, waste water, or sewage
- C02F1/28—Treatment of water, waste water, or sewage by sorption
- C02F1/281—Treatment of water, waste water, or sewage by sorption using inorganic sorbents
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- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2101/00—Nature of the contaminant
- C02F2101/10—Inorganic compounds
- C02F2101/20—Heavy metals or heavy metal compounds
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- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2101/00—Nature of the contaminant
- C02F2101/30—Organic compounds
- C02F2101/32—Hydrocarbons, e.g. oil
- C02F2101/327—Polyaromatic Hydrocarbons [PAH's]
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Abstract
The present invention relates to a kind of methods for heavy metal in water and polycyclic aromatic hydrocarbon collaboration efficient absorption removal, and the adsorbent that the method uses is Fe-SBA15 mesopore molecular sieve.Heavy metal is copper in the water.Polycyclic aromatic hydrocarbon is pyrene in the water.Concentration is 5~50mg/L to the copper in water.Concentration is 25~200 μ g/L to the pyrene in water.The amount that Fe-SBA15 mesopore molecular sieve is added in the water is 0.1~2g/L.Method operating method of the invention is simple, easily operated.Various parameters are easy to control, and can adjust operating parameter at any time as needed.Fe-SBA15 mesoporous molecular sieve adsorbent to heavy metal in water and polycyclic aromatic hydrocarbon carry out adsorption treatment excessively in, the removal of two kinds of pollutants has collaboration (mutually promoting) effect.It can continuously use for several times after the regeneration of Fe-SBA15 solid absorbent without influencing adsorption effect, reduce long-time service processing cost.For pH value and ionic strength for pending water without particular/special requirement, the scope of application is larger.
Description
Technical field
The invention belongs to water treatment fields, are related to a kind of for heavy metal in water and polycyclic aromatic hydrocarbon collaboration efficient absorption removal
Method.
Background technique
Heavy metal and polycyclic aromatic hydrocarbon (PAHs) are the persistent pollutants of two quasi-representatives common in environment, polycyclic aromatic hydrocarbon
Chemical structure is extremely stable, and bioavailability is extremely low, and can enter the internal of people via food chain, greatly increases the mankind and suffers from
The risk of cancer.Heavy metal cannot be biodegradable, has very strong toxicity, and they to the mankind and wildlife trace level
It industrially applies and its extensively, causes heavy metal in waste water dense, finally entered in water environment via various approach.
Many research discovery heavy metals and polycyclic aromatic hydrocarbon can be often detected simultaneously in the environment, wherein related soil, river
The two combined pollution effect of lake and its bed mud report is more, and some researches show that heavy metals and polycyclic aromatic hydrocarbon synergy to generate
Combined pollutant it is extremely complex, and toxicity is stronger, and harmfulness is bigger, thus is combined in the environment by heavy metal and polycyclic aromatic hydrocarbon
Combined pollution phenomenon caused by acting on has caused the highest attention of scientists from all over the world.
In recent years, people give very big pass to the reparation of heavy metal in surrounding medium and polycyclic aromatic hydrocarbon composite pollution
Note, especially soil environment, and aggravate in face of China's Heavy Metals in Water Environment and polycyclic aromatic hydrocarbons contaminated degree, cumulative year after year shows
As, most of researchers have only formulated the removal scheme for independent pollutant, but to removing removing heavy metals and polycyclic virtue simultaneously
The concern of hydrocarbon is less.As patent 201510390223.8 disclose the polycyclic aromatic hydrocarbon-degrading bacteria of one plant of resistance to heavy metal, composition and
Its purposes.The bacterium is pale yellow mycobacteria Mycobacterium gilvum, and deposit number is CGMCC No.10941.The bacterium
It can be used for removal or degrading polycyclic aromatic hydrocarbons, the polycyclic aromatic hydrocarbon in the soil that especially removes or degrade, water environment；It can be also used for
It is biological prosthetic in polycyclic aromatic hydrocarbons contaminated soil, water environment, the especially soil or water of heavy metal and polycyclic aromatic hydrocarbon composite pollution.
The bacterium cooperates with the ability that can enhance removal or degrading polycyclic aromatic hydrocarbons with surfactant simultaneously.The patent can only be gone in water removal
Polycyclic aromatic hydrocarbon.And with the accumulation of time, heavy metal and polycyclic aromatic hydrocarbon therein whether there is the problems such as migrating and converting
It is unclear.Therefore, a kind of method that can remove removing heavy metals and polycyclic aromatic hydrocarbon simultaneously is developed to be of great significance.
Summary of the invention
For overcome the deficiencies in the prior art, the present invention provides a kind of efficient for heavy metal in water and polycyclic aromatic hydrocarbon collaboration
The method of Adsorption.This method establishes a kind of synchronization, efficiently removal Heavy Metals in Water Environment and polycyclic aromatic hydrocarbon composite pollution
New method provides application technology for water pollution control.
The present invention provides the following technical solutions:
A method of for heavy metal in water and polycyclic aromatic hydrocarbon collaboration efficient absorption removal, the method uses adsorbent
For Fe-SBA15 mesopore molecular sieve.
It is preferably in the above scheme, heavy metal is copper in the water.
In any of the above-described scheme preferably, polycyclic aromatic hydrocarbon is pyrene in the water.
In any of the above-described scheme preferably, concentration is 5~50mg/L to the copper in water.
In any of the above-described scheme preferably, concentration is preferably 20mg/L to the copper in water.
In any of the above-described scheme preferably, concentration is 25~200 μ g/L to the pyrene in water.
In any of the above-described scheme preferably, concentration is preferably 100 μ g/L to the pyrene in water.
In any of the above-described scheme preferably, the amount that Fe-SBA15 mesopore molecular sieve is added in the water is 0.1~2g/
L。
In any of the above-described scheme preferably, the amount of addition Fe-SBA15 mesopore molecular sieve is preferably in the water
0.5g/L。
In any of the above-described scheme preferably, the adsorbent stirs after being added to the water, and the revolving speed of stirring is 650~
900r/min, time are 0~300min.
In any of the above-described scheme preferably, the adsorbent stirs after being added to the water, and the revolving speed of stirring is preferably
850r/min。
In any of the above-described scheme preferably, solion is added in the water.
In any of the above-described scheme preferably, the solion is Klorvess Liquid.
In any of the above-described scheme preferably, after the Klorvess Liquid is added to the water, the concentration of potassium chloride is 0.005
~0.1mol/L.
In any of the above-described scheme preferably, after the Klorvess Liquid is added to the water, the concentration of potassium chloride is preferably
0.005~0.025mol/L.
In any of the above-described scheme preferably, the pH value for controlling aqueous solution is 2~5.
In any of the above-described scheme preferably, when suction-operated occurs, concussion or stirring are protected from light.
Adsorbent Fe-SBA15 mesopore molecular sieve in the present invention, is with triblock polymer PULLRONIC F68-
Polyoxyethylene (abbreviation P123) is template, and ethyl orthosilicate (TEOS) is the predecessor of silicon, FeCl3·6H2O is Fe predecessor,
In autoclave direct hydrothermal synthesis prepare Fe-SBA15 mesopore molecular sieve, after in Muffle furnace calcining obtain light yellowish-brown toner
End.
Method operating method of the invention is simple, easily operated.Various parameters are easy to control, and can be adjusted at any time as needed
Operating parameter.Fe-SBA15 mesoporous molecular sieve adsorbent to heavy metal in water and polycyclic aromatic hydrocarbon carry out adsorption treatment excessively in, two
The removal of kind pollutant has collaboration (mutually promoting) effect.Fe-SBA15 solid absorbent regeneration after can continuously use for several times and
Adsorption effect is not influenced, long-time service processing cost is reduced.PH value and ionic strength for pending water without particular/special requirement,
The scope of application is larger.
Detailed description of the invention
Fig. 1 is that the present invention is a kind of to be connect for difference in heavy metal in water and the method for polycyclic aromatic hydrocarbon collaboration efficient absorption removal
Adsorption effect schematic diagram of the Fe-SBA15 to copper and pyrene under touching time conditions；
Fig. 2 is Bu Tong first in a kind of method removed for heavy metal in water with polycyclic aromatic hydrocarbon collaboration efficient absorption of the present invention
Adsorption effect schematic diagram of the Fe-SBA15 to copper and pyrene under beginning concentration conditions；
Fig. 3 be the present invention it is a kind of for heavy metal in water and polycyclic aromatic hydrocarbon collaboration efficient absorption removal method in difference from
Adsorption effect schematic diagram of the Fe-SBA15 to copper and pyrene under sub- strength condition；
Fig. 4 is that the present invention is a kind of for difference pH in heavy metal in water and the method for polycyclic aromatic hydrocarbon collaboration efficient absorption removal
Fe-SBA15 influences schematic diagram to the adsorption effect of copper and pyrene under the conditions of value；
Fig. 5 is that the present invention is a kind of to be inhaled for different in heavy metal in water and the method for polycyclic aromatic hydrocarbon collaboration efficient absorption removal
Attached dose of Fe-SBA15 dosage influences schematic diagram to the adsorption effect of copper and pyrene.
Specific embodiment
In order to further appreciate that technical characteristic of the invention, the present invention is explained in detail combined with specific embodiments below
It states.Embodiment only has illustrative effect to the present invention, without the effect of any restrictions, those skilled in the art
The modification for any unsubstantiality made on the basis of the present invention, all should belong to protection scope of the present invention.
Fe-SBA15 mesopore molecular sieve of the invention can be obtained by synthesizing, and specific method is with triblock polymer polyoxy second
Alkene-polyoxypropylene polyoxyethylene (abbreviation P123) is template, and ethyl orthosilicate (TEOS) is the predecessor of silicon, FeCl3·
6H2O is Fe predecessor, and direct hydrothermal synthesis prepares Fe-SBA15 mesopore molecular sieve in autoclave.
The present invention provides a kind of method for heavy metal in water and polycyclic aromatic hydrocarbon collaboration efficient absorption removal, the sides
Method uses adsorbent for Fe-SBA15 mesopore molecular sieve.
Further, heavy metal is copper in the water.
Further, polycyclic aromatic hydrocarbon is pyrene in the water.
Further, concentration is 5~50mg/L to the copper in water.It is preferred that 20mg/L.
Further, concentration is 25~200 μ g/L to the pyrene in water.It is preferred that 100 μ g/L.
Further, the amount that Fe-SBA15 mesopore molecular sieve is added in the water is 0.1~2g/L.Preferably 0.5g/L
Further, the adsorbent stirs after being added to the water, and the revolving speed of stirring is 650~900r/min, time 0
~300min.Revolving speed is preferably 850r/min.
Further, solion is added in the water.
Further, the solion is Klorvess Liquid.
Further, after the Klorvess Liquid is added to the water, the concentration of potassium chloride is 0.005~0.1mol/L.It is excellent
It is selected as 0.005~0.025mol/L.
Further, the pH value for controlling aqueous solution is 2~5.
Further, when suction-operated occurs, concussion or stirring are protected from light.
The embodiment of the present invention 1-5 prepares the mixed solution of heavy metal solution, polycyclic aromatic hydrocarbon solution and the two respectively, adds
Enter adsorbent Fe-SBA15, passes through control pollutant and the time of contact of adsorbent, the initial concentration of pollutant, pH value, ion
The conditions such as intensity and adsorbent dosage realize the efficient synergistic sorption of heavy metal and polycyclic aromatic hydrocarbon removal in water, to illustrate this
The effect of invention.
Embodiment 1:
Typical polycyclic aromatic hydrocarbon (pyrene) solution, representative heavy metal are separately added into the glass beaker that 3 volumes are 500ml
The mixed solution 500ml of (copper) solution and the two, is placed on magnetic stirring apparatus, stirs solution with the revolving speed of 850r/min, to
Adsorbent Fe-SBA15 0.25g is added after stabilization of speed, starts timing, carries out adsorption reaction, was used as 0 moment at this time.Control is dirty
The time of contact for contaminating object and adsorbent, adsorption treatment is carried out under the following conditions:
React target solution volume: 500ml
React target solution concentration: 1, pyrene: 100 μ g/L；2, copper: 20mg/L；3, pyrene: 100 μ g/L+
Copper: 20mg/L
Reaction target solution temperature: 25 DEG C
Reaction solution system: 0.01M Klorvess Liquid
Adsorbent dosage: 0.5g/L
Adsorbent material: Fe-SBA15 powder
Sampling time point: 0,5,15,25,35,45,60,75,90,120,150,180,210,270,300min.
After sampling, it is centrifuged two minutes under the conditions of 5000rmp in supercentrifuge, takes supernatant, measure remaining pollution
Object concentration.As a result as shown in Figure 1.
As shown in Figure 1, Fe-SBA15 adsorbs copper and pyrene, and the adsorbance of pollutant is with time of contact when beginning
Growth and increase, finally tend towards stability.By Fig. 1 a it is found that the adsorbance of copper significantly increases, equilibrium adsorption capacity after pyrene is added
3.78mg/g is increased to by 2.54mg/g, amplification has facilitation to the absorption of copper up to 48.8%, i.e. pyrene；It can be obtained by Fig. 1 b,
After copper is added in pyrene solution, the adsorbance of pyrene is also significantly improved, and equilibrium adsorption capacity increases to 58 μ g/g by 44 μ g/g, increases
Width is 32%, i.e., copper equally has facilitation to the absorption of pyrene.In conclusion copper and pyrene have obviously in adsorption process
The effect mutually promoted, can efficiently cooperate with removal.
Embodiment 2:
The pyrene solution (adding or be not added copper) of a certain concentration gradient is separately added into a series of centrifuge tube that volumes are 30ml
With copper solution (adding or be not added pyrene) 25ml of a certain concentration gradient, in duplicate.Adsorbent Fe-SBA15 is added later
Centrifuge tube is placed on shaking table by 0.0125g, and concussion is protected from light under the conditions of 150rpm.By controlling the initial concentration of pollutant, under
Adsorption treatment is carried out under the conditions of stating:
React target solution volume: 25ml
React target solution concentration: pyrene: 25,50,75,100,125,150,175,200 μ g/L (add or are not added 20mg/L's
Copper solution)；Copper: 5,10,15,20,25,30,35,40,45,50mg/L (the pyrene solution for adding or being not added 100 μ g/L)
Reaction target solution temperature: 25 DEG C
Reaction solution system: 0.01M Klorvess Liquid
Adsorbent dosage: 0.5g/L
Adsorbent material: Fe-SBA15 powder
Sampling time point: for 24 hours
After sampling, it is centrifuged two minutes under the conditions of 5000rmp in supercentrifuge, takes supernatant, measure remaining pollution
Object concentration.As a result as shown in Fig. 2, and data are fitted with Langmuir model, obtain maximum adsorption capacity, formula is such as
Under:
Qe=QmaxbCe/(1+bCe)
In formula, CeFor equilibrium concentration (mg/L or μ g/L)；QmaxFor maximal absorptive capacity (mg/g or μ g/g)；B is absorption system
Number.Acquired results are as shown in the table after fitting.
Cu indicates that copper, Pyr indicate pyrene in table.
By Fig. 2 a it is found that the adsorbance of copper increases with the increase of initial concentration solution, and when pyrene is added in solution,
The adsorbance of copper will significantly increase, and by Biao Ke get, after being fitted, maximal absorptive capacity increases to 6.77mg/ by 4.31mg/g
G, amplification 57.1%, i.e. pyrene have facilitation to the absorption of copper；It can be obtained by Fig. 2 b, it is similar to the absorption situation of copper, pyrene
Adsorbance also with initial concentration solution increase and increase, and when in pyrene solution be added copper after, the adsorbance of pyrene has greatly
Increase, by Biao Ke get, after fitting, 93 μ g/g when maximal absorptive capacity is by individually adsorbing increase to 161 μ g/g, and amplification reaches
73.1%, i.e. copper equally has facilitation to the absorption of pyrene.From the foregoing, it will be observed that in adsorption process, copper and pyrene have and its bright
The aobvious effect mutually promoted can efficiently cooperate with removal.
Embodiment 3:
Prepare a series of system of Klorvess Liquids as reaction solution, concentration is respectively 0,0.001,0.005,0.01,
0.025,0.05,0.1mol/L.Adsorption treatment is divided into three groups while carrying out, and first group of pyrene for containing 100 μ g/L, second group contains
The copper of 20mg/L, pyrene and 20mg/L copper of last group containing 100 μ g/L.Every kind of solution take 25ml in volume be 30ml from
In heart pipe, in duplicate.Adsorbent Fe-SBA15 0.0125g is added later, centrifuge tube is placed on shaking table, 150rpm item
Concussion is protected from light under part.By controlling the ionic strength of solution system, adsorption treatment is carried out.Other conditions are referring to embodiment 2.As a result
As shown in Figure 3.
By Fig. 3 a it is found that with ionic strength increase, the adsorbance of copper reduces, and is added after pyrene, the adsorbance of copper
There is apparent increase, when wherein potassium chloride concentration is 0.005mol/L, the adsorbance of copper increases to 3.02mg/ by 2.13mg/g
G, amplification is minimum, is 31.3%, when potassium chloride concentration is 0.1mol/L, the adsorbance of copper increases to 1.84mg/ by 0.51mg/g
G, amplification is maximum, and up to 260%.；It can be obtained by Fig. 3 b, the adsorbance of pyrene increases with the increase of ionic strength, and copper is added
Later, also there is different degrees of increase in the adsorbance of pyrene, when wherein potassium chloride concentration is 0.005mol/L, the adsorbance of pyrene by
It is 30.8 μ g/g that 25.04 μ g/g, which increase, and amplification is minimum, is 23%, when potassium chloride concentration is 0.025mol/L, the adsorbance of pyrene by
35.18 μ g/g increase to 58.17 μ g/g, and amplification is maximum, are 65.3%.In conclusion in adsorption process, when reaction system
When ionic strength changes, copper and pyrene have the function of extremely significantly mutually promoting, and can efficiently cooperate with removal.
Embodiment 4:
The pyrene solution of 100 μ g/L, the mixed solution of 20mg/L copper solution and pyrene (100 μ g/L) and copper (20mg/L) are prepared,
Every kind of solution takes 25ml in the centrifuge tube that volume is 30ml.Solution ph is transferred to 2,3,4,5 respectively, in duplicate.It
Adsorbent Fe-SBA15 0.0125g is added afterwards, centrifuge tube is placed on shaking table, concussion is protected from light under the conditions of 150rpm.Pass through control
The pH value of solution system processed carries out adsorption treatment.Other conditions are referring to embodiment 2.As a result as shown in Figure 4.
By Fig. 4 a it is found that the adsorbance of copper increases with the increase of pH value, and after addition pyrene, the adsorbance of copper is had not
With the increase of degree, when wherein pH value is 4, the adsorbance of copper increases to 10.11mg/g from 9.03mg/g, and amplification is minimum, is
12%, when pH value is 2, the adsorbance of copper increases to 4.41mg/g by 1.97mg/g, and amplification is maximum, and up to 124%；Fig. 4 b is aobvious
Show, with the raising of pH value, the adsorbance of pyrene can be reduced, while in the presence of having copper, the adsorbance of pyrene will appear increasing slightly
Greatly.It can be obtained from above, in adsorption process, when the pH value of reaction system changes, copper and pyrene still have apparent mutually rush
Into effect, can efficiently cooperate with removal.
Embodiment 5:
The mixed solution of pyrene (100 μ g/L) and copper (20mg/L) are prepared, every kind of solution takes 25ml in volume for 30ml's
In centrifuge tube.It is separately added into a certain amount of Fe-SBA15 according to adsorbent dosage 0.1,0.3,0.5,1.0,1.5,2.0g/L,
In duplicate.Centrifuge tube is placed on shaking table, concussion is protected from light under the conditions of 150rpm.By controlling the dosage of adsorbent, carry out
Adsorption treatment.Other conditions are referring to embodiment 2.As a result as shown in Figure 5.
As shown in Figure 5, when adsorbent dosage increases to 0.3g/L by 0.1g/L, the adsorbance of copper and pyrene all obviously increases
Greatly, and the adsorbance both in 0.3g/L all reaches maximum value, respectively 5.05mg/g and 99.52 μ g/g, later with suction
The increase of attached dose of dosage, the adsorbance of two kinds of pollutants all occur significantly reduce, therefore consider pollutant removal rate and
The utilization rate of adsorbent, the dosage of adsorbent are preferably 0.5g/L.
Claims (4)
1. it is a kind of for heavy metal in water and polycyclic aromatic hydrocarbon collaboration efficient absorption removal method, the method use adsorbent for
Fe-SBA15 mesopore molecular sieve, heavy metal is copper in the water, and polycyclic aromatic hydrocarbon is pyrene in the water, and Fe- is added in the water
The amount of SBA15 mesopore molecular sieve is 0.1~2g/L, and concentration is 5~50mg/L to the copper in water, and concentration is the pyrene in water
25~200 μ g/L, the pH value for controlling aqueous solution is 2~5.
2. the method according to claim 1 for heavy metal in water and polycyclic aromatic hydrocarbon collaboration efficient absorption removal, special
Sign is: the adsorbent stirs after being added to the water, and the revolving speed of stirring is 650~900r/min, and the time is 0~300min.
3. the method according to claim 1 for heavy metal in water and polycyclic aromatic hydrocarbon collaboration efficient absorption removal,
It is characterized in that: solion is added in the water.
4. the method according to claim 3 for heavy metal in water and polycyclic aromatic hydrocarbon collaboration efficient absorption removal, special
Sign is: the solion is Klorvess Liquid.
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