CN114195247B - Method for removing Cr (VI) in water body by using nano zero-valent iron mediated by iron dissimilatory reduction bacteria - Google Patents
Method for removing Cr (VI) in water body by using nano zero-valent iron mediated by iron dissimilatory reduction bacteria Download PDFInfo
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- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 title claims abstract description 139
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- 241000894006 Bacteria Species 0.000 title claims abstract description 36
- 238000000034 method Methods 0.000 title claims abstract description 35
- 230000009467 reduction Effects 0.000 title claims abstract description 18
- 230000001404 mediated effect Effects 0.000 title claims abstract description 17
- 229910052742 iron Inorganic materials 0.000 title claims description 21
- 239000002351 wastewater Substances 0.000 claims abstract description 25
- 239000000243 solution Substances 0.000 claims description 24
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- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 claims description 15
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- CYDQOEWLBCCFJZ-UHFFFAOYSA-N 4-(4-fluorophenyl)oxane-4-carboxylic acid Chemical compound C=1C=C(F)C=CC=1C1(C(=O)O)CCOCC1 CYDQOEWLBCCFJZ-UHFFFAOYSA-N 0.000 claims description 5
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- NLXLAEXVIDQMFP-UHFFFAOYSA-N Ammonia chloride Chemical compound [NH4+].[Cl-] NLXLAEXVIDQMFP-UHFFFAOYSA-N 0.000 claims description 4
- 239000007836 KH2PO4 Substances 0.000 claims description 4
- 239000007832 Na2SO4 Substances 0.000 claims description 4
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- -1 polyethylene Polymers 0.000 claims description 4
- GNSKLFRGEWLPPA-UHFFFAOYSA-M potassium dihydrogen phosphate Chemical compound [K+].OP(O)([O-])=O GNSKLFRGEWLPPA-UHFFFAOYSA-M 0.000 claims description 4
- 229910052938 sodium sulfate Inorganic materials 0.000 claims description 4
- 238000005303 weighing Methods 0.000 claims description 4
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- 238000001816 cooling Methods 0.000 claims description 3
- DBLXOVFQHHSKRC-UHFFFAOYSA-N ethanesulfonic acid;2-piperazin-1-ylethanol Chemical compound CCS(O)(=O)=O.OCCN1CCNCC1 DBLXOVFQHHSKRC-UHFFFAOYSA-N 0.000 claims description 3
- 239000004033 plastic Substances 0.000 claims description 3
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- WFCSWCVEJLETKA-UHFFFAOYSA-N 2-piperazin-1-ylethanol Chemical compound OCCN1CCNCC1 WFCSWCVEJLETKA-UHFFFAOYSA-N 0.000 claims 2
- 241001052560 Thallis Species 0.000 claims 2
- 229910052564 epsomite Inorganic materials 0.000 claims 2
- 229940089468 hydroxyethylpiperazine ethane sulfonic acid Drugs 0.000 claims 2
- 229910001873 dinitrogen Inorganic materials 0.000 claims 1
- 239000007791 liquid phase Substances 0.000 claims 1
- VTLYFUHAOXGGBS-UHFFFAOYSA-N Fe3+ Chemical compound [Fe+3] VTLYFUHAOXGGBS-UHFFFAOYSA-N 0.000 abstract description 6
- 150000002500 ions Chemical class 0.000 abstract description 6
- 229910001385 heavy metal Inorganic materials 0.000 abstract description 3
- 238000004065 wastewater treatment Methods 0.000 abstract description 2
- 239000011651 chromium Substances 0.000 description 76
- 230000000694 effects Effects 0.000 description 15
- 238000002161 passivation Methods 0.000 description 15
- 239000000203 mixture Substances 0.000 description 14
- UQSXHKLRYXJYBZ-UHFFFAOYSA-N Iron oxide Chemical compound [Fe]=O UQSXHKLRYXJYBZ-UHFFFAOYSA-N 0.000 description 12
- 239000000126 substance Substances 0.000 description 9
- 230000009257 reactivity Effects 0.000 description 6
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 5
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- 239000000047 product Substances 0.000 description 5
- JKMHFZQWWAIEOD-UHFFFAOYSA-N 2-[4-(2-hydroxyethyl)piperazin-1-yl]ethanesulfonic acid Chemical compound OCC[NH+]1CCN(CCS([O-])(=O)=O)CC1 JKMHFZQWWAIEOD-UHFFFAOYSA-N 0.000 description 4
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- VYZAMTAEIAYCRO-UHFFFAOYSA-N Chromium Chemical compound [Cr] VYZAMTAEIAYCRO-UHFFFAOYSA-N 0.000 description 3
- HEMHJVSKTPXQMS-UHFFFAOYSA-M Sodium hydroxide Chemical compound [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 description 3
- 239000000370 acceptor Substances 0.000 description 3
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 3
- 229910052804 chromium Inorganic materials 0.000 description 3
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- 241000196324 Embryophyta Species 0.000 description 2
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- SZVJSHCCFOBDDC-UHFFFAOYSA-N ferrosoferric oxide Chemical compound O=[Fe]O[Fe]O[Fe]=O SZVJSHCCFOBDDC-UHFFFAOYSA-N 0.000 description 2
- 230000004060 metabolic process Effects 0.000 description 2
- 244000005700 microbiome Species 0.000 description 2
- 238000002156 mixing Methods 0.000 description 2
- KMUONIBRACKNSN-UHFFFAOYSA-N potassium dichromate Chemical compound [K+].[K+].[O-][Cr](=O)(=O)O[Cr]([O-])(=O)=O KMUONIBRACKNSN-UHFFFAOYSA-N 0.000 description 2
- 239000002244 precipitate Substances 0.000 description 2
- 230000001105 regulatory effect Effects 0.000 description 2
- 238000001228 spectrum Methods 0.000 description 2
- 230000001502 supplementing effect Effects 0.000 description 2
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- 206010007269 Carcinogenicity Diseases 0.000 description 1
- 108090000790 Enzymes Proteins 0.000 description 1
- 102000004190 Enzymes Human genes 0.000 description 1
- 229910002588 FeOOH Inorganic materials 0.000 description 1
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 1
- 108010044467 Isoenzymes Proteins 0.000 description 1
- IPWKIXLWTCNBKN-UHFFFAOYSA-N Madelen Chemical compound CC1=NC=C([N+]([O-])=O)N1CC(O)CCl IPWKIXLWTCNBKN-UHFFFAOYSA-N 0.000 description 1
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- 230000007670 carcinogenicity Effects 0.000 description 1
- 230000015556 catabolic process Effects 0.000 description 1
- 230000008859 change Effects 0.000 description 1
- 239000003638 chemical reducing agent Substances 0.000 description 1
- 238000000576 coating method Methods 0.000 description 1
- 150000001875 compounds Chemical class 0.000 description 1
- 239000000356 contaminant Substances 0.000 description 1
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- 235000013305 food Nutrition 0.000 description 1
- 239000003673 groundwater Substances 0.000 description 1
- 230000012010 growth Effects 0.000 description 1
- 239000001257 hydrogen Substances 0.000 description 1
- 229910052739 hydrogen Inorganic materials 0.000 description 1
- 238000011081 inoculation Methods 0.000 description 1
- VBMVTYDPPZVILR-UHFFFAOYSA-N iron(2+);oxygen(2-) Chemical class [O-2].[Fe+2] VBMVTYDPPZVILR-UHFFFAOYSA-N 0.000 description 1
- JEIPFZHSYJVQDO-UHFFFAOYSA-N iron(III) oxide Inorganic materials O=[Fe]O[Fe]=O JEIPFZHSYJVQDO-UHFFFAOYSA-N 0.000 description 1
- HWSZZLVAJGOAAY-UHFFFAOYSA-L lead(II) chloride Chemical compound Cl[Pb]Cl HWSZZLVAJGOAAY-UHFFFAOYSA-L 0.000 description 1
- 239000010985 leather Substances 0.000 description 1
- 231100000053 low toxicity Toxicity 0.000 description 1
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- 229910052751 metal Inorganic materials 0.000 description 1
- 231100000243 mutagenic effect Toxicity 0.000 description 1
- 230000003505 mutagenic effect Effects 0.000 description 1
- 239000002086 nanomaterial Substances 0.000 description 1
- 238000003199 nucleic acid amplification method Methods 0.000 description 1
- 229960002313 ornidazole Drugs 0.000 description 1
- 230000003647 oxidation Effects 0.000 description 1
- 238000007254 oxidation reaction Methods 0.000 description 1
- 238000007747 plating Methods 0.000 description 1
- 231100000719 pollutant Toxicity 0.000 description 1
- 150000008442 polyphenolic compounds Chemical class 0.000 description 1
- 235000013824 polyphenols Nutrition 0.000 description 1
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- 238000005096 rolling process Methods 0.000 description 1
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- 238000004088 simulation Methods 0.000 description 1
- VWDWKYIASSYTQR-UHFFFAOYSA-N sodium nitrate Inorganic materials [Na+].[O-][N+]([O-])=O VWDWKYIASSYTQR-UHFFFAOYSA-N 0.000 description 1
- NGSFWBMYFKHRBD-DKWTVANSSA-M sodium;(2s)-2-hydroxypropanoate Chemical compound [Na+].C[C@H](O)C([O-])=O NGSFWBMYFKHRBD-DKWTVANSSA-M 0.000 description 1
- 239000011550 stock solution Substances 0.000 description 1
- 239000002352 surface water Substances 0.000 description 1
- 239000011573 trace mineral Substances 0.000 description 1
- 235000013619 trace mineral Nutrition 0.000 description 1
- 229910021642 ultra pure water Inorganic materials 0.000 description 1
- 239000012498 ultrapure water Substances 0.000 description 1
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- 238000004073 vulcanization Methods 0.000 description 1
- 239000002023 wood Substances 0.000 description 1
- 239000011592 zinc chloride Substances 0.000 description 1
- JIAARYAFYJHUJI-UHFFFAOYSA-L zinc dichloride Chemical compound [Cl-].[Cl-].[Zn+2] JIAARYAFYJHUJI-UHFFFAOYSA-L 0.000 description 1
Classifications
-
- 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
- C02F1/70—Treatment of water, waste water, or sewage by reduction
- C02F1/705—Reduction by metals
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B22—CASTING; POWDER METALLURGY
- B22F—WORKING METALLIC POWDER; MANUFACTURE OF ARTICLES FROM METALLIC POWDER; MAKING METALLIC POWDER; APPARATUS OR DEVICES SPECIALLY ADAPTED FOR METALLIC POWDER
- B22F9/00—Making metallic powder or suspensions thereof
- B22F9/16—Making metallic powder or suspensions thereof using chemical processes
- B22F9/18—Making metallic powder or suspensions thereof using chemical processes with reduction of metal compounds
- B22F9/24—Making metallic powder or suspensions thereof using chemical processes with reduction of metal compounds starting from liquid metal compounds, e.g. solutions
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B82—NANOTECHNOLOGY
- B82Y—SPECIFIC USES OR APPLICATIONS OF NANOSTRUCTURES; MEASUREMENT OR ANALYSIS OF NANOSTRUCTURES; MANUFACTURE OR TREATMENT OF NANOSTRUCTURES
- B82Y30/00—Nanotechnology for materials or surface science, e.g. nanocomposites
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B82—NANOTECHNOLOGY
- B82Y—SPECIFIC USES OR APPLICATIONS OF NANOSTRUCTURES; MEASUREMENT OR ANALYSIS OF NANOSTRUCTURES; MANUFACTURE OR TREATMENT OF NANOSTRUCTURES
- B82Y40/00—Manufacture or treatment of nanostructures
-
- 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
- C02F2101/22—Chromium or chromium compounds, e.g. chromates
Landscapes
- Chemical & Material Sciences (AREA)
- Engineering & Computer Science (AREA)
- Nanotechnology (AREA)
- Condensed Matter Physics & Semiconductors (AREA)
- Physics & Mathematics (AREA)
- Crystallography & Structural Chemistry (AREA)
- General Physics & Mathematics (AREA)
- Manufacturing & Machinery (AREA)
- Life Sciences & Earth Sciences (AREA)
- Organic Chemistry (AREA)
- Water Supply & Treatment (AREA)
- Environmental & Geological Engineering (AREA)
- Hydrology & Water Resources (AREA)
- Composite Materials (AREA)
- Materials Engineering (AREA)
- Chemical Kinetics & Catalysis (AREA)
- General Chemical & Material Sciences (AREA)
- Purification Treatments By Anaerobic Or Anaerobic And Aerobic Bacteria Or Animals (AREA)
- Micro-Organisms Or Cultivation Processes Thereof (AREA)
Abstract
The invention belongs to the technical field of heavy metal wastewater treatment, and particularly discloses a method for efficiently removing Cr (VI) in water by nano zero-valent iron mediated by a dissimilatory Fe (III) reducing bacterium. Meanwhile, fe (II) generated by reduction can further reduce Cr (VI), so that reduction of the Cr (VI) is accelerated, and finally, efficient treatment of the wastewater containing the Cr (VI) is realized. The method has the characteristics of simplicity, convenience in operation, high reduction efficiency, small influence of coexisting ions in water, wide application prospect and the like, and provides a new idea for efficiently treating Cr (VI) containing wastewater by nano zero-valent iron.
Description
Technical Field
The invention belongs to the technical field of heavy metal wastewater treatment, and particularly relates to a preparation method of environment-friendly nano zero-valent iron and a method for efficiently removing Cr (VI) in water by nano zero-valent iron mediated by iron dissimilatory.
Background
Chromium and its compound are important chemical raw materials, are widely applied to industries of electroplating, leather, printing and dyeing, chemical industry, pharmacy, wood corrosion prevention and the like, and are metal elements with important strategic significance for national economic development. Due to leakage and unreasonable emissions during production, a large amount of chromium enters surface and groundwater environments. Chromium exists in natural environment mainly in two forms of Cr (iii) and Cr (vi), but they exhibit distinct chemical properties and have very different ways of influence on organisms. Cr (vi) has extremely strong water solubility and mobility over the entire pH range and has very strong toxicity, carcinogenicity and mutagenic properties, and is classified by many countries as a priority for controlling contaminants. Cr (III) participates in metabolism of sugar and fat in human and animals, is a trace element necessary for human body, exists mainly in a form of Cr (OH) 3 precipitate in water, and has low solubility and toxicity. Therefore, reduction of highly toxic Cr (VI) to Cr (III) of low water solubility and low toxicity is currently the most commonly used and effective method for controlling Cr (VI) contamination.
In recent years, researches show that nano zero-valent iron is an environment-friendly nano material, and can be used as a strong reducing agent with high reactivity to reduce and remove various organic matters and inorganic matters. And the nano zero-valent iron has magnetism, so that the nano zero-valent iron is convenient to recycle. Therefore, application of nano zero-valent iron to reduction and removal of Cr (VI) pollution in water is one of the research hot spots in recent years.
However, because the nano zero-valent iron particles are small and have high reactivity, the nano zero-valent iron particles are easy to react with oxygen, water and the like, and a thick passivation layer is formed on the surface of the nano zero-valent iron by the generated iron oxide precipitate (Fe (OH) 3、FeOOH、Fe3O4、Fe2O3), so that electron transfer between the nano zero-valent iron and pollutants is hindered, the activity of the nano zero-valent iron is rapidly reduced, and the practical application of the nano zero-valent iron is limited. Therefore, the problem of passivation of the nano zero-valent iron in the reaction process is a key point for determining whether the nano zero-valent iron can be practically applied on a large scale.
At present, the surface passivation of nano zero-valent iron is mainly concentrated on modifying the nano zero-valent iron, and the most common method comprises the following steps: (1) a vulcanization method is used for modifying nano zero-valent iron: the modified vulcanized nano iron has FeS@nano zero-valent iron with a nano zero-valent iron inner core and a FeS shell, namely, a layer of protective film is formed on the surface of the nano zero-valent iron by the sulfide, so that side reaction between the nano zero-valent iron and water is inhibited, the nano zero-valent iron is protected from being oxidized, and the stability and the reactivity of the nano zero-valent iron are improved. (2) modifying nano zero-valent iron by a surface coating method: the nano zero-valent iron surface is coated with a layer of high molecular polymer, and the existence of the high molecular polymer layer can slow down the contact of the nano zero-valent iron and oxygen, enhance the oxidation resistance of the nano zero-valent iron, slow down the formation of a passivation layer and maintain the reactivity of the nano zero-valent iron. The preparation process of the method is complex, the cost is high, and the sulfide and the high molecular polymer used can cause secondary pollution to the environment, so that the practical application of the method is limited. Therefore, developing an environment-friendly low-cost technology to solve the problem of nano zero-valent iron surface passivation is one of the main directions of current researches.
The dissimilatory Fe (III) reducing bacteria have special geochemical action and environmental remediation action, and have attracted extensive attention. Iron-reducing foreign bacteria are widely distributed in various terrestrial, aquatic and underground environments. The dissimilating Fe (III) reducing bacteria are general terms of microorganisms which take organic matters or hydrogen as electron donors, fe (III) oxides as electron acceptors, release energy in the process of reducing Fe (III) into Fe (II), support self growth and realize degradation of organic matters. Research shows that the iron dissimilatory reducing bacteria have strong respiratory metabolism capability, can degrade various toxic and refractory organic matters and can resist various toxic heavy metals. Therefore, the invention aims to reduce the iron oxide in the nano zero-valent iron surface passivation layer to Fe (II) with better solubility by using the dissimilatory Fe (III) reducing bacteria as an electron acceptor, thereby promoting the dissolution of the nano zero-valent iron surface passivation layer and prolonging the reactivity of the nano zero-valent iron surface passivation layer. Meanwhile, fe (II) generated by reduction can further reduce Cr (VI), so that reduction of the Cr (VI) is accelerated, and efficient treatment of the wastewater containing the Cr (VI) is realized. So far, no report of removing Cr (VI) in water body by using nano zero-valent iron mediated by the iron dissimilatory reducing bacteria is seen, and the invention provides a novel method for efficiently treating Cr (VI) containing wastewater by using nano zero-valent iron, and has wide application prospect.
Disclosure of Invention
Aiming at the defects existing in the prior art, the invention aims to solve the passivation problem of nano zero-valent iron in the Cr (VI) reduction process by using a biological method, and has the characteristics of economy, convenience and environmental friendliness.
The invention provides a method for efficiently removing Cr (VI) in a water body by using nano zero-valent iron mediated by iron dissimilatory reduction bacteria, which comprises the following steps:
(1) Preparation of nano zero-valent iron
The invention adopts an environment-friendly method for preparing nano zero-valent iron, namely a method for reducing FeSO 4 solution by green tea extract to prepare nano zero-valent iron. The method comprises the following specific steps: weighing green tea, adding into distilled water (the ratio of the green tea to the distilled water is 6g:100 mL), boiling at 75-85 ℃ for more than 20min, continuously stirring by a magnetic stirrer during boiling, cooling to room temperature, and vacuum filtering to obtain green tea extract. Then slowly adding a certain volume of green tea extract into a certain volume of 0.1mol/L FeSO 4 solution (the volume ratio of the green tea extract to the FeSO 4 solution is 2:1) in a room temperature and nitrogen environment, slowly stirring by using a magnetic stirrer while adding, continuing to react for at least 50min after adding, continuing to stir for at least 80min to obtain black suspension, then vacuum filtering, washing three times by using a mixed solution of ethanol and water (the volume ratio of the ethanol to the water is 1:3), then vacuum drying at 40 ℃ to obtain solid powder, namely nano zero-valent iron, and storing the solid powder in a polyethylene plastic bottle for standby.
(2) Preparation of suspension of iron-reducing bacteria
The iron-reducing bacteria of the invention is a typical iron-reducing bacteria, namely the Ornidazole Shewanella (ShewanellaoneidensisMR-1), which is used because ShewanellaoneidensisMR-1 grows fast, and has the characteristics of wide distribution in nature, strong metabolic capability and the like. ShewanellaoneidensisMR-1 bacterial suspension is prepared by the following steps: activating the bacterial powder with a proper amount of LB culture medium (10 g/L of peptone, 5g/L of yeast extract and 10g/L of sodium chloride) to obtain an activated bacterial liquid, performing amplification culture on the activated bacterial liquid by using the LB culture medium (inoculating 1mL of activated bacterial liquid according to the proportion of 100mL of culture medium), placing the activated bacterial liquid in a constant-temperature oscillator at 30 ℃ and 150rpm for culturing to logarithmic phase, performing centrifugal separation for 5min at 8000r/min to obtain wet bacterial bodies, washing three times by using 10mL of sterilized 20mM HEPES solution with initial pH of 7.0, dispersing the wet bacterial bodies in a certain amount of sterilized BMM culture medium to obtain a suspension, and adjusting the dosage of the wet bacterial bodies so that the absorbance (OD 600) at 600nm is 1.3 to obtain the suspension for standby.
(3) Method for efficiently removing Cr (VI) in water body by using nano zero-valent iron mediated by iron dissimilatory reduction bacteria
Simulation experiment: taking 90-100mL of sterilized BMM culture based on 250mL of blue mouth bottle, adding Cr (VI) to make the initial concentration range of the BMM culture be 40-100mg/L, adding 20mmol/L sodium lactate as a carbon source, adding 0.33-1.98mmol/L nano zero-valent iron, inoculating a certain amount of ShewanellaoneidensisMR-1 suspension to make the OD 600 of the BMM culture be 0.1-0.4, finally supplementing a certain amount of BMM culture medium to make the total volume of the mixed solution be 100-110mL, then filling high-purity nitrogen to deoxidize for 15min, sealing, placing the mixture in a constant-temperature oscillator at 30 ℃ for culture, sampling and analyzing the concentration of Cr (VI) in the solution every day, and calculating the removal rate of Cr (VI);
the composition and concentration of the BMM culture medium
The BMM medium was prepared by mixing each component in Table 1 with water.
The method is practically applied: taking the actual Cr (VI) containing wastewater with the volume V, regulating the pH value of the wastewater to be 7, adding a certain amount of KH2PO4、Na2HPO4、NH4Cl、Na2SO4、MgO4·7H2O、HEPES(4- hydroxyethyl piperazine ethane sulfonic acid to ensure that the final concentration is respectively 2.59-2.75, 4.05-4.30, 0.50-0.54, 0.108-0.114 and 6.80-7.15g/L, adding a certain amount of sodium lactate as a carbon source to ensure that the final concentration is 20mmol/L, adding nano zero-valent iron to ensure that the final concentration is 0.33-1.32mmol/L, and inoculating a certain amount of ShewanellaoneidensisMR-1 suspension to ensure that the OD 600 =0.1-0.3 of the final solution, the volume of the final solution is 1.05-1.10V, pH =7, then filling high-purity nitrogen to deoxidize for 15min, sealing, and placing in a constant temperature oscillator at 30 ℃ for culturing for 5-10d at 150 rpm.
Preferably, the Cr (VI) concentration of the actual Cr (VI) -containing wastewater is 40-80mg/L.
Compared with the prior art, the application has the following advantages and beneficial effects:
the method for efficiently removing Cr (VI) in the water body by using the nano zero-valent iron mediated by the dissimilatory iron reducing bacteria has the characteristics of simplicity, convenience in operation, good reduction effect, small influence of co-existence ions in water, wide application prospect and the like, and provides a new thought for efficiently treating Cr (VI) containing wastewater by using the nano zero-valent iron.
The method solves the passivation problem of nano zero-valent iron in the Cr (VI) reduction process by utilizing the iron dissimilatory reduction bacteria ShewanellaoneidensisMR-1, and has the characteristics of economy and environmental friendliness. Meanwhile ShewanellaoneidensisMR-1 utilizes the iron oxide in the surface passivation layer as an electron acceptor to reduce the iron oxide into Fe (II) with better solubility, so that the activity of nano zero-valent iron can be prolonged, meanwhile, the generated Fe (II) can further reduce Cr (VI), the efficient treatment of Cr (VI) -containing wastewater can be realized, and the method has important environmental benefit and social value.
The iron dissimilatory reducing bacteria are widely distributed in nature and are convenient to apply in practical engineering.
Drawings
FIG. 1 is a scanning electron microscope image of nano zero-valent iron prepared in example 1 of the present invention;
FIG. 2 is an X-ray energy spectrum of nano zero-valent iron prepared in example 1 of the present invention;
FIG. 3 is a graph showing the effect of Cr (VI) removal in different systems in example 2, wherein nZVI is nano zero-valent iron and MR-1 is ShewanellaoneidensisMR-1;
FIG. 4 is a scanning electron microscope image of the reduction product of example 2 of the present invention, wherein nZVI is nano zero-valent iron and MR-1 is ShewanellaoneidensisMR-1;
FIG. 5 is an XPS chart of the reduction product Cr2p in example 2 of the present invention;
FIG. 6 shows the effect of Cr (VI) removal at various initial Cr (VI) concentrations in example 3 of the present invention;
FIG. 7 shows the effect of Cr (VI) removal at various zero-valent iron concentrations in example 4 of the present invention.
Detailed Description
The following detailed description of the present application is provided by applicant in connection with specific embodiments to facilitate a further understanding of the present application by those skilled in the art, but should not be construed or interpreted in any way as limiting the scope of the present application as claimed.
In the following examples:
Source of iron-reducing strain:
The powder of Kaschin-ShewanellaoneidensisMR-1 (number MCC 1A 01706) was purchased from China center for type culture Collection of marine microorganisms.
Green tea (food grade, i.e., obtained by deactivation of enzymes, rolling, and drying processes) was purchased from shandong one cup scented tea industry limited.
The pH was adjusted with 0.1mol/L NaOH solution and/or 0.1mol/L HCl solution.
The composition of the BMM medium used is shown in Table 1.
TABLE 1 BMM composition and concentration of the Medium
The BMM medium was prepared by mixing each component in Table 1 with ultrapure water.
Example 1: a preparation method of nano zero-valent iron comprises the following steps of
Weighing 6g of green tea, adding into 100mL of distilled water, boiling at 80 ℃ for 30min, continuously stirring by a magnetic stirrer during boiling, cooling to room temperature, and vacuum filtering to obtain green tea extract; then, under the environment of room temperature and nitrogen, slowly adding the obtained green tea extract into a certain volume of 0.1mol/L FeSO 4 solution (the volume ratio of the green tea extract to the FeSO 4 solution is 2:1), slowly stirring the green tea extract by using a magnetic stirrer while adding the green tea extract, continuing to react for 60min after adding the green tea extract, continuing to stir the green tea extract for 80min to obtain black suspension, then performing vacuum filtration, washing the black suspension for three times by using a mixed solution of ethanol and water (the volume ratio of the ethanol to the water is 1:3), and performing vacuum drying at 40 ℃ to obtain solid powder, namely nano zero-valent iron (the scanning electron microscope image of the nano zero-valent iron is shown in the figure 1, and the X-ray energy spectrum is shown in the figure 2), and storing the solid powder in a polyethylene plastic bottle for the following examples.
As shown in FIG. 1, the nano zero-valent iron has a particle size in the range of 50-100nm, and as shown in FIG. 2, the nano zero-valent iron contains carbon and oxygen in addition to iron, which is caused by residual tea polyphenols in the green tea extract.
The glassware used in the examples below was used after sterilization at 121℃for 20 min.
Example 2: a method for efficiently removing Cr (VI) in a water body by using nano zero-valent iron mediated by an iron dissimilatory reducing bacterium comprises the following steps:
(1) Preparation of suspension of iron-reducing bacteria
5Mg of Shewanella as one of the above-mentioned bacterial powders (No. MCC 1A 01706) was activated with 2mL of LB medium (composed of peptone, yeast extract, sodium chloride and water, wherein 10g/L of peptone, 5g/L of yeast extract and 10g/L of sodium chloride) in a thermostatic shaker at 30℃and 150rpm for 4 hours to obtain an activated bacterial liquid, then the activated bacterial liquid was subjected to expansion culture (inoculated in a proportion of 1mL of activated bacterial liquid in 100mL of medium) using the above-mentioned LB medium, and placed in a thermostatic shaker at 30℃and 150rpm for cultivation to logarithmic growth phase, and then centrifuged at 8000r/min for 5 minutes to obtain wet bacterial cells, and then 10mL of sterilized 20mM HEPES solution having an initial pH of 7.0 was used for three times, and then the washed wet bacterial cells were dispersed in a predetermined amount of BMM medium after sterilization (sterilization in this step: 121℃for 20min, the same shall not be repeated), and the wet bacterial liquid was adjusted to have an absorbance of 53600 nm (OD 1.600).
(2) Taking 90mL of sterilized BMM culture, adding 10g/L potassium dichromate stock solution prepared by distilled water into a blue mouth bottle (controlling the final reaction volume to be 100 mL) based on 250mL of sterilized BMM culture, so that the initial concentration of Cr (VI) (namely the final concentration after all substances are added and the concentration before the reaction starts, which are not described in detail later), is 80mg/L, regulating the pH value of the mixture to be 7, adding a proper amount of sodium lactate as a carbon source to enable the final concentration of the mixture to be 20mmol/L, adding a proper amount of nano zero-valent iron to enable the final concentration of the mixture to be 1.32mmol/L, inoculating a proper amount of ShewanellaoneidensisMR-1 suspension prepared in the step (1), enabling the OD 600 =0.3 of the solution, and finally supplementing a proper amount of BMM culture medium to enable the total volume of the mixture to be 100mL, wherein the pH value of the mixture is not changed obviously, and is still 7, wherein the final concentration is the concentration at the moment (which is not described later), then filling high pure nitrogen to deoxidize for 15min, sealing, placing the mixture in a constant temperature culture experiment set at 30 ℃ and 150 rpm; meanwhile, a control group with only bacteria (except no nano zero-valent iron, the rest are the same as the experimental group) and only nano zero-valent iron (except no bacteria), and then sampling and analyzing the concentration of Cr (VI) every day, and calculating the removal rate of Cr (VI) under different systems. The Cr (VI) removal effect in different systems is shown in FIG. 3. The scanning electron microscope image of the reduced product (filtered, freeze-dried at 40 ℃ to obtain a solid sample) is shown in fig. 4, and the XPS image of the reduced product Cr2p is shown in fig. 5.
As shown in FIG. 3, the removal rate of 6dCr (VI) was 18.39% in the system with only bacteria; a system only containing nano zero-valent iron, wherein the 6dCr (VI) removal rate is 48.05 percent; and the removal rate of 6dCr (VI) is up to 98.65% in the nano zero-valent iron system mediated by the iron dissimilatory reduction bacteria ShewanellaoneidensisMR-1.
The dissimilatory iron-reducing bacteria ShewanellaoneidensisMR-1 can effectively relieve the passivation problem of nano zero-valent iron in the Cr (VI) reduction process and prolong the activity of the nano zero-valent iron. As shown in FIG. 4, when the iron-reducing bacteria SHEWANELLA ONEIDENSISMR-1 are not added, a large amount of iron oxide clusters are gathered and deposited on the surface of the nano zero-valent iron to form a passivation layer. And after the iron-dissimilating reducing bacteria ShewanellaoneidensisMR-1 are added, the iron oxide in the passivation layer on the surface of the nano zero-valent iron is greatly reduced, which further indicates that the iron-dissimilating reducing bacteria ShewanellaoneidensisMR-1 can promote the dissolution of the iron oxide in the passivation layer on the surface of the nano zero-valent iron and prolong the reactivity of the nano zero-valent iron. As can be seen from FIG. 5, the reduced product of Cr (VI) in example 2 exhibited two peaks at 576.8eV and 586.8eV, which represent Cr (III) 2p1/2 and Cr (III) 2p3/2, respectively, with the main components Cr (OH) 3 and Cr 2O3. This illustrates that the mechanism of Cr (VI) removal in water is that Cr (VI) is reduced to Cr (III) and then precipitated in water as Cr (OH) 3 and Cr 2O3 insolubles, effecting Cr (VI) removal from wastewater.
Example 3: a method for efficiently removing Cr (VI) in a water body by using nano zero-valent iron mediated by an iron dissimilatory reducing bacterium comprises the following steps:
According to the procedure of example 2, only the initial concentrations of Cr (VI) in step (2) of example 2 were adjusted to 40, 60, 80 and 100mg/L, respectively, and the ph=7 of the mixture obtained after all the substances were added was kept unchanged, and the effect of the iron-reducing isozymes ShewanellaoneidensisMR-1 on the removal of Cr (VI) at different initial concentrations was examined, and the results are shown in fig. 6. As is clear from FIG. 6, the removal rates of 6dCr (VI) were 99.80%, 99.56%,98.65% and 77.59% when the initial concentrations of Cr (VI) were 40, 60, 80 and 100mg/L, respectively. It can be seen that the method of the present invention has a good Cr (VI) removing effect when the initial concentration of Cr (VI) is not higher than 80 mg/L.
Example 4: a method for efficiently removing Cr (VI) in a water body by using nano zero-valent iron mediated by an iron dissimilatory reducing bacterium comprises the following steps:
According to the procedure of example 2, the final concentration of nano zero-valent iron in step (2) of example 2 was adjusted to be 0.33, 0.66, 1.32 and 1.98mmol/L, respectively, the other procedures and the amounts were unchanged, the ph=7 of the mixture obtained after all the substances were added, and the effect of the iron-dissimilatory reducing bacteria ShewanellaoneidensisMR-1 on Cr (VI) removal by different nano zero-valent iron concentrations was examined, and the results are shown in fig. 7. As is clear from FIG. 7, when the concentration of nano zero-valent iron is gradually increased in the range of 0.33 to 1.32mmol/L, the removal rate of 6dCr (VI) is significantly increased. When the concentration of nano zero-valent iron is further improved to 1.98mmol/L, the removal rate of Cr (VI) is changed little, so the invention determines that the optimal concentration of nano zero-valent iron is 1.32 mmol/L.
Example 5: a method for efficiently removing Cr (VI) in a water body by using nano zero-valent iron mediated by an iron dissimilatory reducing bacterium comprises the following steps:
According to the procedure of example 2, only the concentration of ShewanellaoneidensisMR-1 suspension in step (2) of example 2 was adjusted to make the OD 600 of the solution be 0.1,0.2,0.3 and 0.4, respectively, the other procedures and the amounts were unchanged, the ph=7 of the mixture obtained after all the substances were added, and the effect of the concentration of different suspensions under the mediation of iron-variant reducing bacteria ShewanellaoneidensisMR-1 on Cr (VI) removal was examined. The results showed that the removal rate of 6dCr (VI) was 84.31%, 93.46% and 98.65% when the concentration of the suspension, namely OD 600, was 0.1,0.2,0.3, respectively. When the concentration of the suspension was further increased to have an OD 600 of 0.4, the change in the removal rate of Cr (vi) was small and was 99.63%, so that the present invention determines that the concentration of the optimum suspension, that is, OD 600 =0.3.
Example 6: a method for efficiently removing Cr (VI) in a water body by using nano zero-valent iron mediated by an iron dissimilatory reducing bacterium comprises the following steps:
according to the procedure of example 2, in the implementation of step (2) of example 2, zn 2+(ZnCl2)、Pb2+(PbCl2)、SO4 2-(NaSO4) and NO 3 -(NaNO3) with final concentrations of 2mM were added as coexisting ions before inoculation of the suspension, and the added substance forms were shown by brackets behind the ions in four groups, other operating conditions and amounts were unchanged, and the pH of the mixture obtained in the four groups after all the substances were 7, and the effect of the iron-dissimilatory reduction bacteria SHEWANELLA ONEIDENSISMR-1 on Cr (VI) removal by the nano zero-valent iron was examined. The results show that the effect of the coexisting ions in the solution on the removal of Cr (VI) is small, and the removal rates of 6dCr (VI) are respectively 98.56%, 98.42%, 97.80% and 92.77% in sequence, which shows that the effect of the coexisting ions in water is small when the Cr (VI) is removed.
Example 7: a method for efficiently removing Cr (VI) in a water body by using nano zero-valent iron mediated by an iron dissimilatory reducing bacterium comprises the following steps:
Taking actual Cr (VI) containing wastewater, adding water to dilute the wastewater by one time, taking out 95mL of the wastewater in a 250mL blue-mouth bottle, firstly adjusting the pH=7 of the wastewater, then adding a proper amount of KH2PO4、Na2HPO4、NH4Cl、Na2SO4、MgO4·7H2O、HEPES(4- hydroxyethyl piperazine ethane sulfonic acid to ensure that the final concentrations of the wastewater are 2.72 g/L, 4.26 g/L, 0.53 g/L, 0.113 g/L and 7.14g/L respectively, then adding a proper amount of sodium lactate as a carbon source to ensure that the final concentration of the wastewater is 20mmol/L, adding nano zero-valent iron to ensure that the final concentration of the wastewater is 1.32mmol/L, and inoculating a certain amount of ShewanellaoneidensisMR-1 suspension to ensure that the OD 600 =0.3, ensuring that the final solution volume is 100mL and pH=7, then filling high-purity nitrogen to deoxidize 15min, sealing, placing the wastewater in a constant-temperature oscillator at 30 ℃ for culture at 150rpm, and carrying out sampling analysis for 6d, wherein the Cr (VI) removal rate is 97.65%.
The actual Cr (VI) containing wastewater of this example was taken from the washing wastewater of the electroplating plant in a plating plant in Hubei province, and analyzed, the Cr (VI) concentration in the wastewater was 154.38mg/L, the total Cr concentration was 168.60mg/L, the Cu 2+ concentration was 42.46mg/L, the Zn 2+ concentration was 34.88mg/L, SO 4 2- =87.41 mg/L, and the pH=5.12.
Claims (1)
1. The method for removing Cr (VI) in water by using nano zero-valent iron mediated by the iron dissimilatory reducing bacteria is characterized by comprising the following steps of:
(1) Preparation of nano zero-valent iron
Weighing green tea, adding into distilled water, weighing green tea and distilled water at a weight ratio of 6g to 100mL, boiling at 75-85deg.C for more than 20min, continuously stirring with magnetic stirrer, cooling to room temperature, and vacuum filtering to obtain green tea extractive solution; then slowly adding a certain volume of green tea extract into a certain volume of 0.1mol/L FeSO 4 solution under the environment of room temperature and nitrogen, wherein the volume ratio of the green tea extract to the 0.1mol/L FeSO 4 solution is 2:1, slowly stirring by a magnetic stirrer while adding, continuing to react for at least 50min after adding, and continuing to stir for at least 80min to obtain black suspension; vacuum filtering the obtained black suspension, and washing with a mixed solution of ethanol and water for three times, wherein the volume ratio of the ethanol to the water is 1:3; vacuum drying at 40deg.C to obtain solid powder which is nanometer zero-valent iron, and storing the solid powder in polyethylene plastic bottle; the particle size of the nano zero-valent iron is 50-100 nm;
(2) Preparation of suspension of iron-reducing bacteria
Activating the powder of the Shewanella oldhamii ShewanellaoneidensisMR-1 with a proper amount of LB culture medium to obtain an activated bacterial liquid; performing expansion culture on the activated bacterial liquid by utilizing an LB (liquid-phase) culture medium, inoculating 1mL of the activated bacterial liquid according to the proportion of 100mL of the LB culture medium, placing the inoculated activated bacterial liquid in a constant-temperature oscillator with the temperature of 30 ℃ and the speed of 150rpm for culturing to a logarithmic growth phase, and performing centrifugal separation for 5min at 8000r/min to obtain wet bacterial bodies; then, washing three times with 10mL of sterilized 20mM 4-hydroxyethyl piperazine ethane sulfonic acid solution with initial pH of 7.0, dispersing wet thalli in a certain amount of sterilized BMM culture medium to obtain a suspension, and adjusting the dosage of the wet thalli to ensure that the absorbance (OD 600) at 600nm is 1.3, thus obtaining the suspension for later use;
The LB culture medium consists of peptone, yeast extract, sodium chloride and water, wherein the concentrations of the peptone, the yeast extract and the sodium chloride are respectively 10g/L, 5g/L and 10g/L; the BMM culture medium consists of KH2PO4、Na2HPO4、NH4Cl、Na2SO4、MgSO4·7H2O、4- hydroxyethyl piperazine ethanesulfonic acid, so that the final concentration is 2.59-2.75g/L, 4.05-4.30g/L, 0.50-0.54g/L, 0.108-0.114g/L and 6.80-7.15g/L respectively;
(3) Specific mode for removing Cr (VI) in water body by using nano zero-valent iron mediated by iron dissimilatory reduction bacteria
The final solution volume was controlled to 100mL: taking Cr (VI) containing wastewater with the volume of V, adjusting the pH value of the wastewater to be 7, and then adding a certain amount of KH2PO4、Na2HPO4、NH4Cl、Na2SO4、MgSO4·7H2O、4- hydroxyethyl piperazine ethanesulfonic acid to ensure that the final concentration is 2.59-2.75g/L, 4.05-4.30g/L, 0.50-0.54g/L, 0.108-0.114g/L and 6.80-7.15g/L in sequence; then adding a certain amount of sodium lactate to make the final concentration of the sodium lactate be 20 mmol/L; adding nano zero-valent iron to make the final concentration of the nano zero-valent iron be 0.33-1.32 mmol/L; inoculating a certain amount of suspension to make OD 600 =0.1-0.3; the final solution volume is 1.05-1.10V, ph=7, wherein the final solution volume is 1.05-1.10V is 100mL; then filling nitrogen gas 10-20 min for deoxidization, sealing and culturing 6 d;
The final concentration refers to a concentration such that the final solution volume is 100mL at ph=7; the initial concentration of Cr (VI) in the wastewater containing Cr (VI) is 40-80mg/L, and the initial concentration refers to the concentration of the wastewater containing Cr (VI) after being added into a BMM culture medium and before starting the reaction.
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