CN102642930A - Method for treatment of metal waste water by sulfate reducing bacteria growing up with electric current - Google Patents

Method for treatment of metal waste water by sulfate reducing bacteria growing up with electric current Download PDF

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CN102642930A
CN102642930A CN2012100919676A CN201210091967A CN102642930A CN 102642930 A CN102642930 A CN 102642930A CN 2012100919676 A CN2012100919676 A CN 2012100919676A CN 201210091967 A CN201210091967 A CN 201210091967A CN 102642930 A CN102642930 A CN 102642930A
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cathode
electrode
waste water
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potentiostat
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CN102642930B (en
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李大平
苏文涛
何晓红
陶勇
张礼霞
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Chengdu Institute of Biology of CAS
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Abstract

The invention belongs to the technical field of treatment of waste water, and particularly relates to a method for reduction of sulfate into sulfide and treatment of metal waste water by sulfate reducing bacteria growing up with electric current. The sulfate reducing bacteria provided by the invention is a mixing bacteria group, which comprises Desulfobulbus propinonicus, geobacter sulfurreducens. Under the condition of lacking organic carbon resource, an electrode is used as the only electronic donator for growing, sulfate is reduced into sulfide via bioelectrical chemistry, and the sulfide is applied to the treatment of metal waste water. According to the method provided by the invention, the defect that organic carbon resource is needed to be used as the electronic donator is overcome, the operation is simple, the secondary pollution is zero, the cost is low, and is particularly suitable for the treatment on organic carbon metal waste water of mine waste water, metal smelting waste water, electric plating waste water and the like.

Description

Utilize the method for the sulphate reducing bacteria processing heavy metal wastewater thereby of electric current growth
Technical field
The invention belongs to technical field of waste water processing, the sulphate reducing bacteria sulphate reducing that is specifically related to utilize the electric current growth is for sulfide and be applied to the method for heavy metal containing wastewater treatment.
Background technology
Along with development of modern industry, all can produce a large amount of heavy metal wastewater therebies every year, and sulfide is the important means of extracting valuable metal.Traditional biological method is to be H through sulphate reducing bacteria alienation sulphate reducing 2S (CN101506104A) or sulphate reducing bacteria are produced biological sulphur iron composite material (CN101935100A); Under different pH controls; Can utilize the selective precipitation of realizing metallic sulfide; Removing heavy metal ions in wastewater and to reclaim valuable metal, it is low that this method has a cost, the strong characteristics of flexibility.
Yet the suitable organic carbon source of the growth needs of sulphate reducing bacteria is as electron donor, and price is more expensive, and production cost is high, and has the secondary pollution problem of organic substrate to processed water that add.Report as the patent that substitutes carbon source (CN101434919B) is existing with solid waste such as straw, but straw needs fermentation pre-treatment in 10-30 days, the cycle is longer.Therefore, organic carbon source capable of using is the especially important factor of low-carbon (LC) waste water of restriction heavy metal contamination.
Bioelectrochemistry is the novel method of a kind of treatment of heavy metal polluted water that biological process and electrochemical process are combined.Its handling principle is to make pollutants in sewage under biological and electrochemistry dual function, obtain degraded, and faint electric current can also stimulate the Metabolic activity of mikrobe.Bio-electrochemical process has obtained development rapidly in recent years as a kind of environmentally friendly method.Sulfate-reducing process with the hydrogen mediation obtains broad research, comprises that the mikrobe assisted electrochemical produces hydrogen (C.M.Cordas et al, 2008; L.Yu et al, 2011) auxiliary hydrogen (Lojou et al, 2002) and the direct hydrogen supply (Xu Huiwei, 2009) of producing of electron shuttle body.Because the water solubility of hydrogen own is low, it is low to exist efficient with hydrogen mediation reduction process, expends shortcomings such as additional energy.
The present invention is directed to the restraining factors that are used for sulfate reduction of hydrogen as electron donor; Supply the sulfate reduction bacteria growing with polarizing electrode as direct electron donor; Propagation, raising enzymic activity and metabolic activity and sulphate reducing are that the phenomenon of sulfide is not also appeared in the newspapers.
Summary of the invention
The objective of the invention is to invent a kind of sulphate reducing bacteria sulphate reducing with the electric current growth is sulfide, and handles the method for heavy metal wastewater thereby.Sulphate reducing bacteria among the present invention is a mixed bacterial, comprises Desulfobulbus propionicus, Geobacter sulfurreducens.It is characterized in that under the condition that lacks organic carbon sulphate reducing bacteria is unique electron donor growth with electrode, through the bioelectrochemistry approach, is sulfide with sulfate reduction, sulfide is applied to the processing of heavy metal wastewater thereby.The present invention overcomes prior art needs the deficiency of organic carbon source as electron donor.
The present invention realizes through following steps:
The structure of bioelectrochemistry device
The bioelectrochemistry device is two chamber reactor configuration (Fig. 1), comprises potentiostat 4, lead 5, cathode compartment 1 and anolyte compartment 2.Insert working electrode 6 and reference electrode 7 in the cathode compartment 1, and add the municipal wastewater treatment plant active sludge; Insert supporting electrode 8 in the anolyte compartment 2; Opened in 3 minutes with barrier film between two Room.
The preparation of cathode compartment and anolyte compartment's solution
The anolyte compartment
0.05mol/L phosphate buffer soln (pH 7.0)
Cathode compartment
Na 2HPO 412H 2O 10.9g L -1, NaH 2PO 43.0g L -1, NaHCO 32.0g L -1, KCl 100mg L -1, MgCl 240mg L -1, NH 4Cl 310mg L -1, CaCl 250mg L -1, NaCl 10mg L -1, FeCl 225mg L -1, CoCl 22H 2O 5mg L -1, MnCl 24H 2O 5mg L -1, AlCl 32.5mg L -1, (NH 4) 6Mo 7O 2415mg L -1, H 3BO 35mg L -1, NiCl 26H 2O 0.5mg L -1, CuCl 22H 2O 3.5mg L -1, ZnCl 25mg L -1, 180～200mg L -1Vitriol is as electron acceptor(EA), and adjusting catholyte pH is 7.2.
The biological-cathode preparation
The extension film of mikrobe
Inoculation municipal wastewater treatment plant active sludge, logical H 2As electron donor, and interpolation vitriol is electron acceptor(EA) enrichment culture 2-3 month.With enrichment to autotrophy sulphate reducing bacteria source be inoculated in the bioelectrochemistry reactor drum cathode compartment of above-mentioned structure, no power continues logical H 2Stir culture.When enriching floras shows the success of extension film to cathode electrode.
The domestication of biological-cathode
Mikrobe feeds argon gas in reactor drum after hanging the film completion on the cathode electrode, drive remaining H away 2, and carry out-400mV (vs.Ag/AgCl) domestication of switching on, when reaching steady state, the removal efficient of vitriol shows that biological-cathode makes up successfully.
The operation of bioelectrochemistry reactor drum
The vitriol substratum that will contain 20mg/L-600mg/L is packed into and is contained the biomembranous cathode compartment of negative electrode; With the phosphate buffer soln anolyte compartment of packing into.Feed 20 minutes argon gas respectively to two Room then and all rush, respectively two Room are sealed again to guarantee the air in the reactor drum.At last, said device is inserted potentiostat through lead, working electrode connects the negative pole of potentiostat, and supporting electrode connects the positive pole of potentiostat, and reference electrode connects the potentiostat reference electrode, sets electrode potential scope-400 to-700mV (vs.Ag/AgCl).Sulfide concentration reaches 50mgL in the catholyte -1Change catholyte when above, the catholyte of the sulfur compound that swaps out is used for treatment of heavy metal ions.
The invention still further relates to the above-mentioned purposes of method in the processing of the low organic carbon heavy metal wastewater thereby of mine wastewater, Metal smelting waste water, electroplating wastewater of utilizing the sulphate reducing bacteria processing heavy metal wastewater thereby of electric current growth.
Beneficial effect of the present invention:
(1) not needing organic carbon source, is that unique electron donor supplies the sulfate reduction bacteria growing with electrode directly, through the bioelectrochemistry approach, is sulfide with sulfate reduction, avoids causing secondary pollution, and simple to operate.
(2) the present invention does not need hydrogen as electron donor, and the electrode potential that provides is low, save energy, and electrode need not to use expensive catalysts, and cost is low.
(3) the present invention has using value for the metals ion of removing in the low organic carbon heavy metal wastewater thereby.
The present invention is specially adapted to the processing of low organic carbon heavy metal wastewater therebies such as mine wastewater, Metal smelting waste water, electroplating wastewater.
Description of drawings
Fig. 1 is a bioelectrochemistry device synoptic diagram of the present invention.1 cathode compartment wherein; 2 anolyte compartments; 3 barrier films; 4 potentiostats; 5 leads; 6 working electrodes; 7 reference electrodes; 8 supporting electrodes
When Fig. 2 was electromotive force-400mV (vs.Ag/AgCl), sulfate reduction and sulfide generated change procedure in time.
Fig. 3 generates over time for adding up electric charge and sulfide.
Fig. 4 is a batch test sulfate reduction cyclic voltammetry scan.
Embodiment:
Come further explain the present invention below in conjunction with accompanying drawing and embodiment.Embodiment is for ease of better understanding the present invention, but is not limitation of the present invention.
Embodiment 1: be the sulfate reduction and the sulfide generation of unique electron donor with electrode
The structure of bioelectrochemistry reaction unit
The bioelectrochemistry device is two chamber reactor configuration (Fig. 1), comprises potentiostat 4, lead 5, cathode compartment 1 and anolyte compartment 2.Insert working electrode 6 and reference electrode 7 in the cathode compartment 1, and add the active sludge of municipal wastewater treatment plant; Insert supporting electrode 8 in the anolyte compartment 2; Opened in 3 minutes with barrier film between two Room.
The preparation of cathode compartment and anolyte compartment's solution
The anolyte compartment
0..05mol/L phosphate buffer soln (pH 7.0)
Cathode compartment
Na 2HPO 412H 2O 10.9g L -1, NaH 2PO 43.0g L -1, NaHCO 32.0g L -1, KCl 100mg L -1, MgCl 240mg L -1, NH 4Cl 310mg L -1, CaCl 250mg L -1, NaCl 10mg L -1, FeCl 225mg L -1, CoCl 22H 2O 5mg L -1, MnCl 24H 2O 5mg L -1, AlCl 32.5mg L -1, (NH 4) 6Mo 7O 2415mg L -1, H 3BO 35mg L -1, NiCl 26H 2O 0.5mg L -1, CuCl 22H 2O 3.5mg L -1, ZnCl 25mg L -1, 180～200mg L -1Vitriol is as electron acceptor(EA), and adjusting catholyte pH is 7.2.
The biological-cathode preparation
The extension film of mikrobe
The active sludge of inoculation municipal wastewater treatment plant, logical H 2As electron donor, and interpolation vitriol is electron acceptor(EA) enrichment culture 2-3 month.With enrichment to autotrophy sulphate reducing bacteria source be inoculated in the bioelectrochemistry reactor drum cathode compartment of above-mentioned structure, no power continues logical H 2Stir culture.When enriching floras shows the success of extension film to cathode electrode.
The domestication of biological-cathode
Mikrobe feeds argon gas in reactor drum after hanging the film completion on the cathode electrode, drive remaining H away 2, and carry out-400mV (vs.Ag/AgCl) energising domestication 30d, when reaching steady state, the removal efficient of vitriol shows that biological-cathode makes up successfully.
The operation of bioelectrochemistry reactor drum
The vitriol substratum that will contain 60mg/L-200mg/L is packed into and is contained the biomembranous cathode compartment of negative electrode; With the phosphate buffer soln anolyte compartment of packing into.Feed 20 minutes argon gas respectively to two Room then and all rush, respectively two Room are sealed again to guarantee the air in the reactor drum.At last, said device is inserted potentiostat through lead, working electrode connects the negative pole of potentiostat, and supporting electrode connects the positive pole of potentiostat, and reference electrode connects the potentiostat reference electrode, sets electrode potential-400mV (vs.Ag/AgCl).
The bioelectrochemistry device carries out a batch test after starting, and changes the minimizing of detection by quantitative vitriol and the generation of sulfide through electrochemical workstation continuous monitoring working electrode electric current.Blank and three batches of test-results are seen table 1:
The clearance of vitriol minimizing and sulfide generation and vitriol in the table 1 batch test
Figure BDA0000149231800000061
Wherein, aOCV: open circuit voltage; bN.D.: do not detect.
Fig. 2 and Fig. 3 are domestication period 3 result, data replication three times, and initial sulfate concentration is 182.70 ± 1.91mg L -1, the reaction times is 10d, sulfate concentration is 34.56 ± 7.17mg L during end -1It is 48.64 ± 4.10mg L that hydrogen sulfide produces concentration -1The electronics mole number of every liter of solution generation hydrogen sulfide is 1173.83C L when 10d finishes -1, the electronics mole number of every liter of solution through cathode electrode is 1838.48C L -1, the electric current utilising efficiency is 71.83%.
To the scan round analysis of biological-cathode electrode, sweep limit is-0.75-0.5V that scanning speed is 5mV s -1As shown in Figure 4; The redox peak of a pair of similar cytochrome protein occurs at 0.10and-0.2V (vs.Ag/AgCl) respectively, has a reduction peak to occur, infers to be the hydrogen reducing peak at-0.7V (vs.Ag/AgCl) current potential place simultaneously; This experiment adopts voltage to be-0.4V (vs.Ag/AgCl); Do not reach go back protohydrogen required-0.7V (vs.Ag/AgCl) voltage, do not detect the existence of hydrogen in the experiment yet, these results can infer that cathode microbial directly obtains from electrode that electronics is used for sulfate reduction through the membranin of bacterium own but not carries out through hydrogen mediation mode.
Embodiment 2: the test of sulfide reducing metal cupric ion
The solvability sulfide that the sulphate reducing bacteria reduction produces has S 2-, HS -, H 2S, their form is relevant with pH, according to bibliographical information, H when pH＜6.5 2S concentration is bigger, HS between the pH 7-13 -Be main, pH＞13 are with S 2-Be main.Carry out the operation that bioelectrochemistry is reacted according to embodiment 1 step, because catholyte contains buffered soln, pH about 8 behind the sulfate reduction, and sulfide should be with HS in the catholyte -Be main, therefore,, the reactor drum water outlet fed according to 1: 1 ratio contain 100mg/L Cu when sulfide concentration in the reactor drum continues to reach 50mg/L when above 2+Low concentration wastewater after form copper sulfide precipitation, detect Cu in the waste water 2+Content, the Cu of post precipitation supernatant 2+Content is lower than 5mg/L, Cu 2+Clearance greater than 95%.

Claims (2)

1. utilize the method for the sulphate reducing bacteria processing heavy metal wastewater thereby of electric current growth, it is characterized in that this method comprises following concrete steps:
(1) structure of bioelectrochemistry device
The bioelectrochemistry device is two chambers reactor configuration, comprises potentiostat (4), lead (5), cathode compartment (1) and anolyte compartment (2), inserts working electrode (6) and reference electrode (7) in the cathode compartment (1), and adding municipal wastewater treatment plant active sludge; Insert supporting electrode (8) in the anolyte compartment (2); Separate with barrier film (3) between two Room;
(2) preparation of cathode compartment and anolyte compartment's solution
The anolyte compartment
0.05mol/L phosphate buffer soln (pH 7.0)
Cathode compartment
Na 2HPO 412H 2O 10.9g L -1, NaH 2PO 43.0g L -1, NaHCO 32.0g L -1, KCl 100mg L -1, MgCl 240mg L -1, NH 4Cl 310mg L -1, CaCl 250mg L -1, NaCl 10mg L -1, FeCl 225mg L -1, CoCl 22H 2O 5mg L -1, MnCl 24H 2O 5mg L -1, AlCl 32.5mg L -1, (NH 4) 6Mo 7O 2415mg L -1, H 3BO 35mg L -1, NiCl 26H 2O 0.5mg L -1, CuCl 22H 2O 3.5mg L -1, ZnCl 25mg L -1, 180～200mg L -1Vitriol is as electron acceptor(EA), and adjusting catholyte pH is 7.2;
(3) biological-cathode preparation
The extension film of A, mikrobe
Inoculation municipal wastewater treatment plant active sludge, logical H 2As electron donor, and interpolation vitriol is electron acceptor(EA) enrichment culture 2-3 month; With enrichment to autotrophy sulphate reducing bacteria source be inoculated in the bioelectrochemistry reactor drum cathode compartment of above-mentioned structure, no power continues logical H 2Stir culture is when enriching floras shows the success of extension film to cathode electrode;
The domestication of B, biological-cathode
Mikrobe feeds argon gas in reactor drum after hanging the film completion on the cathode electrode, drive remaining H away 2, and carry out-400mV (vs.Ag/AgCl) domestication of switching on, when reaching steady state, the removal efficient of vitriol shows that biological-cathode makes up successfully;
(4) operation of bioelectrochemistry reactor drum
The vitriol substratum that will contain 20mg/L-600mg/L is packed into and is contained the biomembranous cathode compartment of negative electrode; With the phosphate buffer soln anolyte compartment of packing into; Feed 20 minutes argon gas respectively to two Room then and all rush, respectively two Room are sealed again to guarantee the air in the reactor drum; At last, said device is inserted potentiostat through lead, working electrode connects the negative pole of potentiostat, and supporting electrode connects the positive pole of potentiostat, and reference electrode connects the potentiostat reference electrode, sets electrode potential scope-400mV to-700mV (vs.Ag/AgCl); Sulfide concentration reaches 50mgL-1 and changes catholyte when above in the catholyte, and the catholyte of the sulfur compound that swaps out is used for treatment of heavy metal ions.
2. the purposes of the described method of claim 1 in the processing of the low organic carbon heavy metal wastewater thereby of mine wastewater, Metal smelting waste water, electroplating wastewater.
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CN102925348A (en) * 2012-11-11 2013-02-13 中国船舶重工集团公司第七二五研究所 Device for detecting concentration of sulfate-reducing bacteria (SRB)
CN103319002A (en) * 2013-06-27 2013-09-25 中国科学院过程工程研究所 Method for biological treatment of sulfate wastewater employing synchronous electric catalysis of anode and cathode
CN103663884A (en) * 2013-12-30 2014-03-26 合肥工业大学 Method for enhancing degradation of organic arsenic in waste water of livestock breeding into pentavalent arsenic by utilizing weak potential
CN103898005A (en) * 2014-01-09 2014-07-02 浙江大学 Electrochemically-active bacterium and screening method thereof
CN104310573A (en) * 2014-11-19 2015-01-28 江南大学 Combination electrode preparation method and application of combination electrode preparation method in bioelectricity Fenton system
CN105060504A (en) * 2015-08-12 2015-11-18 北京化工大学 Method for treating heavy metal wastewater through intermittent non-power-output, parallel connection of two MFCs and voltage increase
CN106345437A (en) * 2016-11-08 2017-01-25 太原理工大学 Preparation method for conductive polymer sulfur fixation material and application thereof in water treatment
CN106630019A (en) * 2016-11-08 2017-05-10 太原理工大学 Method for removing heavy metal ions in wastewater through electric control reduction of elemental sulfur
CN108046427A (en) * 2018-01-09 2018-05-18 衢州学院 Low C/S is than the anaerobic bio-treated method of sulfate-containing organic wastewater under room temperature
CN110078209A (en) * 2019-05-16 2019-08-02 桂林电子科技大学 A kind of method of micro-reduction sulfate formation cadmium sulphur mine
CN111054740A (en) * 2019-12-27 2020-04-24 浙江大学 Device and method for in-situ remediation of cadmium and lead polluted farmland soil by sulfate reduction system driven by microbial electrochemistry
CN111717965A (en) * 2019-03-20 2020-09-29 中国石油化工股份有限公司 Electro-filtration sterilization method for sulfate reducing bacteria
CN113371818A (en) * 2021-06-24 2021-09-10 广东石油化工学院 Method for strengthening nitrogen/sulfur-containing wastewater autotrophic treatment of MEC (methanol-organic carbon) biological cathode
CN113845217A (en) * 2021-11-02 2021-12-28 中山大学 Method and device for removing refractory organic pollutants through sulfur-mediated bioelectrochemistry enhancement
WO2023206841A1 (en) * 2022-04-28 2023-11-02 湖北绿钨资源循环有限公司 Method for separation and impurity removal of tungsten and molybdenum during tungsten smelting process

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CN2852128Y (en) * 2005-12-09 2006-12-27 中国科学院海洋研究所 Dual electrolytic cell for studying hydrogen permeation behavior of metal in sea mud containing sulfate-reducing bacteria
CN101503244A (en) * 2009-03-20 2009-08-12 清华大学 Strengthened autotrophs desulphurization apparatus with complex function
WO2012088503A2 (en) * 2010-12-23 2012-06-28 Stc.Unm Paper-based fuel cell
CN102170006A (en) * 2011-04-07 2011-08-31 重庆大学 Micro-organism fuel battery capable of degrading volatile organic matters

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Publication number Priority date Publication date Assignee Title
CN102925348A (en) * 2012-11-11 2013-02-13 中国船舶重工集团公司第七二五研究所 Device for detecting concentration of sulfate-reducing bacteria (SRB)
CN102925348B (en) * 2012-11-11 2013-10-09 中国船舶重工集团公司第七二五研究所 Device for detecting concentration of sulfate-reducing bacteria (SRB)
CN103319002A (en) * 2013-06-27 2013-09-25 中国科学院过程工程研究所 Method for biological treatment of sulfate wastewater employing synchronous electric catalysis of anode and cathode
CN103663884A (en) * 2013-12-30 2014-03-26 合肥工业大学 Method for enhancing degradation of organic arsenic in waste water of livestock breeding into pentavalent arsenic by utilizing weak potential
CN103898005A (en) * 2014-01-09 2014-07-02 浙江大学 Electrochemically-active bacterium and screening method thereof
CN103898005B (en) * 2014-01-09 2016-11-23 浙江大学 Electro-chemical activity antibacterial and screening technique thereof
CN104310573A (en) * 2014-11-19 2015-01-28 江南大学 Combination electrode preparation method and application of combination electrode preparation method in bioelectricity Fenton system
CN105060504A (en) * 2015-08-12 2015-11-18 北京化工大学 Method for treating heavy metal wastewater through intermittent non-power-output, parallel connection of two MFCs and voltage increase
CN106630019B (en) * 2016-11-08 2018-03-09 太原理工大学 A kind of method of automatically controlled reduction simple substance removal of sulphur heavy metal ions in wastewater
CN106630019A (en) * 2016-11-08 2017-05-10 太原理工大学 Method for removing heavy metal ions in wastewater through electric control reduction of elemental sulfur
CN106345437A (en) * 2016-11-08 2017-01-25 太原理工大学 Preparation method for conductive polymer sulfur fixation material and application thereof in water treatment
CN106345437B (en) * 2016-11-08 2018-12-25 太原理工大学 The preparation and its application in water process that conducting polymer consolidates sulfur materials
CN108046427A (en) * 2018-01-09 2018-05-18 衢州学院 Low C/S is than the anaerobic bio-treated method of sulfate-containing organic wastewater under room temperature
CN111717965A (en) * 2019-03-20 2020-09-29 中国石油化工股份有限公司 Electro-filtration sterilization method for sulfate reducing bacteria
CN111717965B (en) * 2019-03-20 2022-06-28 中国石油化工股份有限公司 Electro-filtration sterilization method for sulfate reducing bacteria
CN110078209A (en) * 2019-05-16 2019-08-02 桂林电子科技大学 A kind of method of micro-reduction sulfate formation cadmium sulphur mine
CN111054740A (en) * 2019-12-27 2020-04-24 浙江大学 Device and method for in-situ remediation of cadmium and lead polluted farmland soil by sulfate reduction system driven by microbial electrochemistry
CN113371818A (en) * 2021-06-24 2021-09-10 广东石油化工学院 Method for strengthening nitrogen/sulfur-containing wastewater autotrophic treatment of MEC (methanol-organic carbon) biological cathode
CN113845217A (en) * 2021-11-02 2021-12-28 中山大学 Method and device for removing refractory organic pollutants through sulfur-mediated bioelectrochemistry enhancement
WO2023206841A1 (en) * 2022-04-28 2023-11-02 湖北绿钨资源循环有限公司 Method for separation and impurity removal of tungsten and molybdenum during tungsten smelting process

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