CN109052620A - A kind of method of cadmium ion in removal heavy metal wastewater thereby - Google Patents

A kind of method of cadmium ion in removal heavy metal wastewater thereby Download PDF

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CN109052620A
CN109052620A CN201810764489.8A CN201810764489A CN109052620A CN 109052620 A CN109052620 A CN 109052620A CN 201810764489 A CN201810764489 A CN 201810764489A CN 109052620 A CN109052620 A CN 109052620A
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mec
mfc
cadmium
cathode
heavy metal
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刘维平
潘璐璐
吴丹菁
梁国斌
陈娴
路娟娟
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Jiangsu University of Technology
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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
    • C02F3/00—Biological treatment of water, waste water, or sewage
    • C02F3/005—Combined electrochemical biological processes
    • 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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Abstract

The invention discloses a kind of methods of cadmium ion in removal heavy metal wastewater thereby, heavy metal wastewater thereby containing cadmium is handled using the electrical energy drive microorganism electrolysis cell that microbiological fuel cell degradation of organic substances generates, overall process does not consume external electric energy, secondary pollution is not generated, is a kind of environmental-friendly new method of heavy metal containing wastewater treatment containing cadmium.This method comprising the following three steps: 1, the determination of MFC operating parameter；2, building of the MFC-MEC from driving coupled system；3, the processing of the heavy metal wastewater thereby containing cadmium: by step 1 and 2, heavy metal wastewater thereby containing cadmium is handled using MEC cathode reaction, catholyte is heavy metal wastewater thereby containing cadmium, and pH value is 1~5, and anode uses carbon paper, and cathode material uses stainless steel, titanium plate and carbon paper.After reaction to MEC, cathode is taken out, MEC cathode reduction products is collected, is detected through XRD, MEC cathode product is cadmium carbonate, and cadmium ion removal rate is 89.5%.

Description

A kind of method of cadmium ion in removal heavy metal wastewater thereby
Technical field
The present invention relates to bioelectrochemistry and heavy metal containing wastewater treatment field, cadmium in specially a kind of removal heavy metal wastewater thereby The method of ion.
Background technique
With the rapid development of our country's economy, process of industrialization is constantly accelerated, and people's lives level is greatly improved, But consequently also bring water environment pollution problem.In the industrial processes such as plating, metallurgy, chemical industry, it can generate a large amount of useless Water, these waste water composition complicated components, in addition to containing organic contamination beyond the region of objective existence difficult to degrade, also containing an a large amount of poisonous and hazardous huge sum of moneys Belong to substance, if this kind of waste water is dealt with improperly, it will cause great harm to ecology, environment, human health.
Cadmium toxicity in waste water is big, is easily absorbed by the body, and accumulates in human body, can damage renal tubule, will lead to when serious Renal failure.Itai-itai event in Japan occurred to 1977 for nineteen fifty-five, was typical chronic cadium poisoning event, more than 20 It is dead to cause more than 200 people by Nian Jian.Thus, cadmium once enters environment, will result in biggish harm.Also occurred in China Serious cadmium pollution event, therefore the processing of the heavy metal wastewater thereby containing cadmium is very urgent, must be handled before discharge of wastewater, with Reach discharge standard, avoids pollution the generation of event.The common technology of heavy metal containing wastewater treatment containing cadmium includes changing both at home and abroad at present Learn the precipitation method, ferrite process, ion-exchange, electric flocculation method, membrane separation process, absorption method, bioanalysis etc., some technology and methods It has successfully been applied in the processing of the heavy metal wastewater thereby containing cadmium.
Patent (CN104211221A) is directed to low concentration heavy metal wastewater thereby containing cadmium, by sequentially adding aluminium polychloride, phosphorus It is stirred after sour sodium, anion, finally precipitating filtering, this method has many advantages, such as at low cost, without secondary pollution.
Patent (CN103466776A) is directed to the heavy metal wastewater thereby containing cadmium of high concentration, and sodium hydroxide and three polysulfide cyanogen are added Sour sodium, this method have good removal effect to the cadmium of various forms in water body.
Patent (CN102464396A) is fixed on carrier by the emulsion for being prepared into foaming agent, organic solvent, auxiliary agent On, for handling heavy metal wastewater thereby containing cadmium, this process flow is simply, at normal temperature carry out, noiseless, and agents useful for same is nontoxic, nothing Harmful, non-volatile, lotion can be recycled, and treatment effect is obvious.
Patent (CN104478128A) based on existing chemical precipitation and coagulation and filtration technique, without or be difficult into Under conditions of the transformation of row Large scale processes, change dispensing and mode of operation and pH value control mode, solves Trace Cadmium in waste water and reach Mark the problem of discharge.With using varieties of reagent few, reagent dosage is few, and raw materials used economical and easily available, does not add into system Any harmful element, at low cost, high treating effect.
Patent (CN101367575) cooperates with quickly processing absorption cadmium using frustule wall and bacterium cell wall, realizes in waste water The removal of cadmium, this method can be widely applied to the cleaning treatment of heavy metal wastewater thereby containing cadmium and resource utilization of industrialized production.It is raw Object electro-chemical systems include microbiological fuel cell (Microbial Fuel Cell, MFC) and microorganism electrolysis cell (Microbial Electrolytic Cell, MEC).The MFC of early stage is concentrated mainly on anode chamber in terms of wastewater treatment, leads to Anode microbial action degradation of organic waste water is crossed, is produced electricl energy while realizing wastewater treatment.With the development of bioelectrochemistry, It was found that many heavy metal ion can also be used as cathode electronics receptor, the application range further expansion of MFC.With this technology Development, the electricity generation ability of MFC improves, and the configuration of device is also more diversified, has also appeared at the same time more The experimental exploring that kind MFC and other technologies are coupled, such as photosynthetic type MFC (Photo-MFC), phytomicroorganism fuel cell (PMFC), anaerobic fluidized bed microbiological fuel cell (AFB-MFC) etc..MFC-MEC is exactly that it constantly explores lower one kind constructed New coupled mode, i.e., produced electricl energy by MFC, and driving MEC operation not only utilizes the electric energy of MFC, but also be able to achieve different redox The removal and recycling of current potential heavy metal ion.Although there are many treating method of the heavy metal wastewater thereby containing cadmium, simple improvement can disappear Very high cost is consumed, is resulted in waste of resources.
Summary of the invention
To solve the above-mentioned problems, the present invention is a kind of emerging clean energy resource and waste water using MFC-MEC coupled system Processing technique.It is calculated according to Nernst equation, Cu2+Electrode potential be positive, reaction spontaneous can carry out, meet MFC reducing condition, And produce electricl energy, with Cu2+When for cathode electronics receptor, MFC's is stabilized the output voltage as 200~750mV, and Cd2+Reduction electricity Position is -0.403V, and the electric energy that MFC is generated is the operation that can drive MEC.Using this feature, MFC is connected with MEC, is realized Cadmium ion in heavy metal wastewater thereby, is restored removal by running from driving for coupled system in the form of cadmium carbonate.By utilizing MFC Electricity production driving MEC operation, while realizing the removal of removal of Cadmium from wastewater, to achieve the purpose that administer water pollution, whole process Without additional electric energy, cleanliness without any pollution.
A method of removal heavy metal wastewater thereby cadmium ion, include the following three steps:
1) MFC and MEC parameter is determined；
2) MFC-MEC series coupled；
3) MFC-MEC handles heavy metal wastewater thereby containing cadmium from driving coupled system；
Wherein the anode of MFC is connected with the cathode of MEC by conducting wire, and the cathode of MFC and the anode of MEC pass through series resistance Coupling is connected；Series circuit is constituted, is run using the electrical energy drive MEC that MFC is generated.
The anode inoculum of the MFC and MEC is activated sludge, and the anode activity that anolyte is volume ratio 1:2-1:4 is dirty The mixed liquor of mud and anode substrate sodium acetate；
The catholyte of the MFC is copper-containing solution, and the catholyte of the MEC is cadmium-containing solution.
Wherein, the determining MFC and MEC parameter comprises the steps of,
The dischargeable capacity of the anode chamber MFC and cathode chamber is 300~500mL, and the catholyte copper ion initial concentration is 500 ~2000mg/L, pH value are 3~5, and saturated sodium chloride solution is used to adjust conductivity for 5~8.5mS/cm, between anode and cathode Away from for 6~8cm；
The dischargeable capacity of the anode chamber MEC and cathode chamber is 100~500mL, and the cadmium wastewater cadmium ion initial concentration is 900~1000mg/L, pH value are 1~5；
The anode material of MFC and MEC is carbon paper, and cathode is using one of stainless steel, titanium plate or carbon paper, anode and cathode Spacing is 6~8cm, is separated by between two Room by anion-exchange membrane；
MFC-MEC series coupled is, when to MFC output voltage stabilization being 200~700mV, preferably 500~700mv, passes through MEC is connected by series resistance coupled modes with MFC, and the resistance is 800-1000 Ω；
It is by the MFC-MEC system of series coupled that MFC-MEC, which handles heavy metal wastewater thereby containing cadmium from driving coupled system, It runs at normal temperatures and pressures, to after reaction, take out MEC cathode, collects cathode reduction products.
The anode substrate sodium acetate solution concentration is 0.9~1g/L；
The anode activated sludge is the sludge containing electricity production bacterium, and the dehydration for being derived from sewage treatment plant's dehydration machine room is dirty Culture domestication liquid is added in the dewatered sludge, cultivates the volume ratio of domestication liquid and dewatered sludge are as follows: 1:5~2:5 for mud；, training Support domestication liquid constituent: 0.2~0.4g/L sucrose, 0.2~0.4g/L potassium dihydrogen phosphate, 0.15~0.35g/L phosphoric acid hydrogen two Potassium, 0.1~0.2g/L triammonium citrate, 0.01~0.3g/L sodium chloride, 0.3~0.5g/L magnesium chloride, 0.1~0.2g/L chlorination Calcium, 0.10~0.40g/LNH4Cl, 0.9~1g sodium acetate, after nitrogen deoxidation with inoculum in anaerobic, be protected from light, normal temperature state Lower domestication is cultivated 5~7 days.
Technical scheme the utility model has the advantages that
1. the electrical energy drive MEC operation generated with MFC, the electric energy that MEC utilizes MFC to generate in situ realize removal of Cadmium from wastewater Removal, realize coupled system from driving operation, whole process does not consume external electric energy, without secondary pollution.
2.MFC maximum power density is up to 22278.4mW/m2, COD removal rate 83.3%, MFC tough cathode ion remaval rate 93.7%, MEC cathode cadmium ion remaval rate 89.5%.
3.MEC cathode surface precipitate is detected as CdCO through XRD3, it was demonstrated that the cadmium ion in waste water passes through MEC cathodic reduction With CdCO after reaction3Precipitated product is precipitated, to realize the removal of removal of Cadmium from wastewater.
Detailed description of the invention
Fig. 1 MFC-MEC coupled system schematic diagram；
Fig. 2 MFC power density curve；
Fig. 3 MEC cathode product XRD spectrum.
Specific embodiment
MFC and MEC is equipped with cathode chamber and anode chamber in embodiment, by HMED-05181 anion-exchange membrane phase between two Room Every wherein MFC catholyte is copper ions solution, and the catholyte of MEC is the waste water containing cadmium ion, and catholyte uses dilute sulfuric acid Adjust pH value；The anode activated sludge and anode substrate sodium acetate that the anolyte of MFC and MEC is volume ratio 1:2-1:4.
Wherein the anode of MFC is connected with the cathode of MEC by conducting wire, and the cathode of MFC and the anode of MEC are by connecting 1000 The coupling of Ω resistance is connected；Series circuit is constituted, is run using the electrical energy drive MEC that MFC is generated.The anode material of MFC and MEC is Carbon paper, cathode material are one of stainless steel, titanium plate or carbon paper.Conductivity is adjusted using saturated sodium chloride solution.
The amberplex is HMED-05181 anion-exchange membrane, and film effective area is 12cm2, first impregnated using preceding In deionized water for 24 hours more than, make the abundant aquation of film and expansion, take the film out in the NaCl solution for being immersed in 5%, save it is standby With.
The anode substrate sodium acetate solution concentration is 1g/L；
The anode activated sludge is to be derived from Changzhou Qing Tan sewage treatment plant dehydration machine room containing the sludge of electricity production bacterium Culture domestication liquid is added in dewatered sludge in the dewatered sludge, and the volume ratio for cultivating domestication liquid and dewatered sludge is 2:5；Training Support domestication liquid constituent: 0.38g/L sucrose, 0.21g/L K2HPO4·3H2O、0.21g/L KH2PO4、0.12g/L C6H5O7 (NH4)3、0.07g/L NaCl、0.40g/L MgCl2·6H2O、0.12g/L CaCl2、0.40g/L NH4Cl, 1.00g/L acetic acid Sodium.After nitrogen deoxidation with inoculum anaerobic, be protected from light, under normal temperature state domestication culture 7 days.
Influence of the embodiment 1:MEC cathode material to MFC-MEC coupled system processing cadmium wastewater
Change the cathode material of MEC: first group of cathode material is stainless steel, and second group of cathode material is titanium plate, third group Cathode material is carbon paper, constructs three groups of coupling devices.MFC, MEC dischargeable capacity are the anode and yin of 500mL, MFC and MEC The volume ratio of interpolar distance 8cm, activated sludge and substrate is 1:4；MFC catholyte copper ion concentration is 1280mg/L, conductivity For 5mS/cm, pH value 5；MEC catholyte concentration of cadmium ions is 985mg/L, pH value 4.9.It is 700mV to MFC output voltage When, MEC is connected with MFC by series system, coupled system is run at normal temperatures and pressures, when cathode material is titanium plate, MEC Cadmium ion removal rate is 51.5% in catholyte, compared with stainless steel, the coupled system that carbon paper is MEC cathode, Cd2+Removal rate point 10.2%, 8.1% is not improved, and it is as shown in Figure 2 that MFC electricity production effect connected in series is shown in Table 1, MFC power density curve.System Cathode is taken out after end of run, collects MEC cathode reduction products, cathode product is analyzed using XRD diffractometer, is in 2 θ There is diffraction maximum at 23.49 °, 30.27 °, 36.42 °, 43.81 °, 49.51 °, 49.90 °, 49.51 °, 58.27 °, as seen Fig. 3 institute Show, it is consistent with the characteristic peak of cadmium carbonate by computer search.
Influence of the embodiment 2:MEC catholyte pH to MFC-MEC coupled system processing cadmium wastewater
In addition to following difference, other conditions are identical for embodiment 2 and embodiment 1.The volume of MFC, MEC activated sludge and substrate Than being 1:2, cathode material is carbon paper, and MFC catholyte copper ion concentration is 512mg/L, pH value 3, conductivity 8.1mS/ Cm, MEC catholyte concentration of cadmium ions are 985mg/L.It adjusts MEC catholyte pH value and is respectively as follows: pH=1, pH=3 and pH=5.It is real It tests when the results are shown in Table 2, pH=5, cadmium ion removal rate is 89.5%, and cathode product is detected as cadmium carbonate through XRD diffractometer.
Influence of 1 cathode material of table to coupled system
The influence that 2 pH value of table removes coupled system electrical property and cadmium ion
MEC catholyte pH Open-circuit voltage (mV) Internal resistance (Ω) Cadmium ion removal rate (%)
1 254 672 45.2
3 343 1263 82.4
5 304 1291 89.5
The present invention is by handling MFC and MEC series coupled cadmium wastewater, not consuming it can be seen from table one and table two Cadmium ion removal rate can be up to 89.5% in the case where expense external electric energy, while the catholyte anolyte of MFC and MEC is sludge Or sewage, with current consumption mass energy, the existing method for removing cadmium for generating new pollutant is completely different.The present invention is weight containing cadmium The processing of metallic wastewater provides more feasible more environmentally-friendly new method.Obviously, above-described embodiment be only be clearly to say Bright example, and do not limit the embodiments.For those of ordinary skill in the art, in above description On the basis of can also make other variations or changes in different ways.There is no need and unable to give all embodiments Exhaustion.And obvious changes or variations extended from this are still within the protection scope of the invention.

Claims (3)

1.一种去除重金属废水镉离子的方法，其特征在于，包含以下三个步骤：1. A method for removing heavy metal wastewater cadmium ions, characterized in that it comprises the following three steps: 1)确定MFC和MEC参数；1) Determine the MFC and MEC parameters; 2)MFC-MEC串联耦合；2) MFC-MEC series coupling; 3)MFC-MEC自驱动耦合系统处理含镉废水；3) MFC-MEC self-driven coupling system to treat cadmium-containing wastewater; 其中MFC的阳极与MEC的阴极耦合相连，MFC的阴极与MEC的阳极通过串联电阻耦合相连；The anode of the MFC is coupled to the cathode of the MEC, and the cathode of the MFC is coupled to the anode of the MEC through a series resistor; 所述MFC和MEC的阳极液为体积比1:2-1:4的阳极活性污泥与阳极底物乙酸钠的混合液；The anolyte of described MFC and MEC is the mixed liquor of the anode activated sludge of volume ratio 1:2-1:4 and anode substrate sodium acetate; 所述MFC的阴极液为含铜溶液，所述MEC的阴极液为含镉废水。The catholyte of the MFC is a solution containing copper, and the catholyte of the MEC is wastewater containing cadmium. 2.根据权利要求1所述的去除重金属废水镉离子的方法，其特征在于：2. the method for removing heavy metal wastewater cadmium ions according to claim 1, is characterized in that: 所述确定MFC和MEC参数包含以下步骤，The determination of MFC and MEC parameters comprises the following steps, 所述MFC阳极室和阴极室的有效容积为300～500mL，所述阴极液铜离子初始浓度为500～2000mg/L，pH值为3～5，电导率为5～8.5mS/cm；The effective volume of the MFC anode chamber and cathode chamber is 300-500mL, the initial copper ion concentration of the catholyte is 500-2000mg/L, the pH value is 3-5, and the conductivity is 5-8.5mS/cm; 所述MEC阳极室和阴极室的有效容积为100～500mL，所述含镉废水镉离子初始浓度为900～1000mg/L，pH值为1～5；The effective volume of the MEC anode chamber and cathode chamber is 100-500mL, the initial concentration of cadmium ions in the cadmium-containing wastewater is 900-1000mg/L, and the pH value is 1-5; 所述MFC和MEC的阳极材料为碳纸，阴极采用不锈钢、钛板或碳纸中的一种，阳极和阴极间距为6～8cm，两室之间由阴离子交换膜相隔；The anode material of the MFC and MEC is carbon paper, the cathode adopts one of stainless steel, titanium plate or carbon paper, the distance between the anode and the cathode is 6-8cm, and the two chambers are separated by an anion exchange membrane; 所述MFC-MEC串联耦合为，待MFC输出电压为200～700mV时，通过串联电阻耦合方式将MEC与MFC相连接，所述电阻为0.01-1000Ω；The series coupling of the MFC-MEC is that when the output voltage of the MFC is 200-700mV, the MEC is connected to the MFC through a series resistance coupling, and the resistance is 0.01-1000Ω; 所述MFC-MEC自驱动耦合系统处理含镉重金属废水为将已经串联耦合的MFC-MEC系统在常温常压下运行，待反应结束后，取出MEC阴极，收集阴极还原产物。The MFC-MEC self-driven coupling system for treating cadmium-containing heavy metal wastewater is to operate the series-coupled MFC-MEC system at normal temperature and pressure. After the reaction is completed, the MEC cathode is taken out to collect cathode reduction products. 3.根据权利要求1或2所述的去除重金属废水镉离子的方法，其特征在于：3. the method for removing heavy metal wastewater cadmium ions according to claim 1 or 2, is characterized in that: 所述阳极底物乙酸钠溶液浓度为0.9～1g/L；The concentration of the anode substrate sodium acetate solution is 0.9～1g/L; 所述阳极活性污泥为含有产电细菌的污泥，取自污水处理厂脱水机房的脱水污泥，在所述脱水污泥中加入培养驯化液，培养驯化液与脱水污泥的体积比为：1:5～2:5；，培养驯化液组成成分：0.2～0.4g/L蔗糖、0.2～0.4g/L磷酸二氢钾、0.15～0.35g/L磷酸氢二钾、0.1～0.2g/L柠檬酸三胺、0.01～0.3g/L氯化钠、0.3～0.5g/L氯化镁、0.1～0.2g/L氯化钙、0.10～0.40g/L NH4Cl、0.9～1g/L乙酸钠，经氮气脱氧后与接种物在无氧、避光、常温状态下驯化培养5～7天。The anode activated sludge is sludge containing electricity-producing bacteria, which is taken from the dewatered sludge in the dehydration machine room of the sewage treatment plant, and the cultivation and acclimatization liquid is added to the dewatered sludge, and the volume ratio of the cultivation and acclimation liquid to the dewatered sludge is : 1:5～2:5;, composition of culture acclimation solution: 0.2～0.4g/L sucrose, 0.2～0.4g/L potassium dihydrogen phosphate, 0.15～0.35g/L dipotassium hydrogen phosphate, 0.1～0.2g /L triamine citrate, 0.01～0.3g/L sodium chloride, 0.3～0.5g/L magnesium chloride, 0.1～0.2g/L calcium chloride, 0.10～0.40g/L NH 4 Cl, 0.9～1g/L Sodium acetate, deoxygenated by nitrogen, and the inoculum were acclimatized and cultured for 5-7 days under anaerobic, light-proof and normal temperature conditions.
CN201810764489.8A 2018-07-12 2018-07-12 A kind of method of cadmium ion in removal heavy metal wastewater thereby Pending CN109052620A (en)

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CN115763832A (en) * 2022-09-15 2023-03-07 云南师范大学 Coupling device of MEC and MFC with shared electrode and application
CN116655059A (en) * 2023-05-06 2023-08-29 山东科技大学 Wastewater treatment device and method for synchronously removing high-concentration heavy metals and sulfate radicals

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Application publication date: 20181221