CN110143673B - Iron ore supported method for fixing hexavalent chromium by microorganisms - Google Patents
Iron ore supported method for fixing hexavalent chromium by microorganisms Download PDFInfo
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- CN110143673B CN110143673B CN201910440932.0A CN201910440932A CN110143673B CN 110143673 B CN110143673 B CN 110143673B CN 201910440932 A CN201910440932 A CN 201910440932A CN 110143673 B CN110143673 B CN 110143673B
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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
- C02F3/28—Anaerobic digestion processes
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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
- C02F3/34—Biological treatment of water, waste water, or sewage characterised by the microorganisms used
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- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2101/00—Nature of the contaminant
- C02F2101/10—Inorganic compounds
- C02F2101/20—Heavy metals or heavy metal compounds
- C02F2101/22—Chromium or chromium compounds, e.g. chromates
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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
- C02F2103/00—Nature of the water, waste water, sewage or sludge to be treated
- C02F2103/06—Contaminated groundwater or leachate
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Abstract
The embodiment of the specification provides a material for fixing hexavalent chromium in underground water and a method for fixing hexavalent chromium by using microorganisms supported by iron ore. Wherein the material comprises at least a microorganism and iron ore, the iron ore being at least used as an inorganic electron donor when the microorganism reduces hexavalent chromium. The method comprises the following steps: at least microorganisms and iron ore as an inorganic electron donor for the reduction of hexavalent chromium by said microorganisms are dosed into groundwater containing hexavalent chromium in an ionic state, so that said microorganisms reduce said hexavalent chromium to precipitable trivalent chromium.
Description
Technical Field
One or more embodiments of the present specification relate to the field of groundwater treatment technology, and more particularly, to a material for fixing hexavalent chromium in groundwater, and a method for fixing hexavalent chromium using iron ore-supported microorganisms.
Background
The existing hexavalent chromium removal methods comprise a physical method, a chemical method and a biological method, wherein the traditional physical method and the traditional chemical method comprise heat treatment, direct reduction, electrolytic activated carbon adsorption and the like, but the methods have high cost and are easy to generate secondary pollution. Biological methods include microbial reduction, which is cost effective and convenient to use relative to traditional physical and chemical methods. However, microorganisms rely on electron donors such as organic glucose acetate, gaseous electron donors such as hydrogen, etc., wherein the utilization of organic bound microorganisms is low, timed replenishment is required, excessive biomass is produced, which tends to block aquifers, gaseous electron donors are cumbersome to handle, and the removal rate is low.
Therefore, there is a need for an improved approach based on microbial reduction that optimizes the treatment of hexavalent chromium in groundwater.
Disclosure of Invention
One or more embodiments of the present specification describe a material for fixing hexavalent chromium in groundwater and a method for fixing hexavalent chromium using iron ore-supported microorganisms, which eliminates at least one of the above-mentioned drawbacks of the prior art.
According to a first aspect, there is provided a material for immobilising hexavalent chromium in groundwater, the material comprising at least a microorganism and iron ore, the iron ore being at least used as an inorganic electron donor when the microorganism reduces hexavalent chromium.
In one possible implementation, the iron ore is also used to chemically react directly with the hexavalent chromium to remove the hexavalent chromium.
In one possible implementation, the iron ore includes one or more of: pyrite, marynonete, wustite and magnetite.
In one possible implementation, the material further comprises a carbon source that supports the growth and reproduction of the microorganism.
In one possible implementation, the carbon source comprises an inorganic carbon source comprising sodium bicarbonate or seashell.
In one possible implementation, the microorganisms include facultative bacteria and/or anaerobic bacteria.
According to a second aspect, there is provided a method for the fixation of hexavalent chromium by iron ore-supported microorganisms, the method comprising: at least microorganisms and iron ore as an inorganic electron donor for the reduction of hexavalent chromium by said microorganisms are dosed into groundwater containing hexavalent chromium in an ionic state, so that said microorganisms reduce said hexavalent chromium to precipitable trivalent chromium.
In one possible implementation, the method for delivering at least microorganisms and iron ore as an inorganic electron donor for reducing hexavalent chromium by the microorganisms into groundwater containing hexavalent chromium in an ionic state comprises: the microorganisms, the iron ore and a carbon source supporting the growth and reproduction of the microorganisms are put into groundwater containing hexavalent chromium in an ionic state.
In one possible implementation, the method for delivering at least microorganisms and iron ore as an inorganic electron donor for reducing hexavalent chromium by the microorganisms into groundwater containing hexavalent chromium in an ionic state comprises: feeding anaerobic sludge comprising the microorganisms and the iron ore into groundwater containing pentavalent vanadium in an ionic state.
In one possible implementation manner, the initial concentration of hexavalent chromium in the underground water containing ionic hexavalent chromium is 10mg/L to 50mg/L, and the ionic hexavalent chromium comprises Cr6 +And/or C r2O7 2-。
The scheme provided by the embodiment of the specification can obviously improve the removal efficiency of hexavalent chromium in the underground water, and meanwhile, the reduction product and the oxidation product can be naturally precipitated in the underground water, so that secondary pollution of the underground water is effectively prevented.
Drawings
In order to more clearly illustrate the technical solutions of the embodiments of the present invention, the drawings needed to be used in the description of the embodiments are briefly introduced below, and it is obvious that the drawings in the following description are only some embodiments of the present invention, and it is obvious for those skilled in the art to obtain other drawings based on these drawings without creative efforts.
FIG. 1 shows an experimental setup of a pre-experiment according to one embodiment;
FIG. 2 illustrates a potential column experimental setup and a penetration curve experimental setup according to one embodiment.
Detailed Description
It is to be understood that the scope of the invention is not to be limited to the specific embodiments described below; it is also to be understood that the terminology used in the examples is for the purpose of describing particular embodiments, and is not intended to limit the scope of the present invention; in the description and claims of the present application, the singular forms "a", "an" and "the" include plural referents unless the context clearly dictates otherwise.
When numerical ranges are given in the examples, it is understood that both endpoints of each of the numerical ranges and any value therebetween can be selected unless the invention otherwise indicated. Unless defined otherwise, all technical and scientific terms used herein have the same meaning as commonly understood by one of ordinary skill in the art to which this invention belongs. In addition to the specific methods, devices, and materials used in the examples, any methods, devices, and materials similar or equivalent to those described in the examples may be used in the practice of the invention in addition to the specific methods, devices, and materials used in the examples, in keeping with the knowledge of one skilled in the art and with the description of the invention.
As described above, the microorganism is still dependent on the electron donor, but the use of the organic electron donor and the gaseous electron donor has the problems of low removal efficiency, complicated operation, easy secondary pollution, and the like. Accordingly, the inventors have creatively proposed the use of natural iron ore as an electron donor for microorganisms for removing hexavalent chromium (including Cr) in groundwater6 +、C r2O7 2-And the like), and meanwhile, the inventor finds that the natural iron ore is used for supporting microorganisms to fix hexavalent chromium through experiments, so that the operation is simple and convenient, the removal efficiency is high, and meanwhile, the secondary pollution can be avoided.
The technical solutions of the embodiments of the present invention will be described in more detail with reference to specific examples.
Example 1 preliminary experiments prove that the combined removal efficiency of the natural iron ore and the microorganisms is high
Design thought of preliminary experiment: as is clear from the data described in the relevant documents, the removal rate of hexavalent chromium by the combination of organic substances and microorganisms is about 0.1. + -. 0.02 mg/L.h, and the removal rate of hexavalent chromium by the combination of gaseous electron donors and microorganisms is about 0.03 mg/L.h. Based on this, a plurality of iron ores were selected in preliminary experiments, and combined with microorganisms to determine a plurality of removal rates, and then compared with the removal rates described in the above documents.
In a specific embodiment, one or more of the following iron ores may be selected in the preliminary experiment: pyrite (FeS)2) Marynodite (FeS), wustite (FeO) and magnetite (F)e3O4)。
In a specific embodiment, the microorganisms (hereinafter collectively referred to as anaerobic consortia) may include anaerobesSuch as obligate anaerobes, facultative anaerobes, or aerotolerant anaerobes. In one example, anaerobic bacteria and facultative bacteria may be included. Further, anaerobic organisms are autotrophic, and thus in the combination of microorganisms and iron ore, a carbon source may also be added to support the growth and reproduction of the microorganisms. In one example, sodium bicarbonate (NaHCO) may be used3) Or shells as carbon source. In another specific example, anaerobic sludge including anaerobic biomass can be selected for direct use as the test material.
According to a specific example, see fig. 1 (in which the tinfoil outside the bottles has been torn off for easy photographing), in a preliminary experiment, 4 250ml glass bottles (e.g. serum bottles) were prepared, covered with tinfoil, each of which was charged with 5g of pyrite, 5g of markenoite, 5g of wustite, 5g of magnetite, and 50ml of anaerobic biomass and 10mg of sodium bicarbonate. The substances for removing hexavalent chromium included in the 4 glass bottles are shown in table 1 below.
TABLE 1
200ml of simulated underground water containing hexavalent chromium is added into the four glass bottles respectively, and more specifically, the simulated underground water can contain potassium dichromate, magnesium chloride hexahydrate, sodium chloride, calcium chloride, potassium dihydrogen carbonate and the like, so as to realize real simulation of the underground water, and then the concentration of the hexavalent chromium in the bottles is detected regularly. Experimental data obtained from preliminary experiments in table 1 show that the removal efficiency of the combination of natural iron ore and microorganisms is significantly improved compared to the aforementioned organic matter plus microorganisms and gaseous electron donor plus microorganisms. In addition, it has also been shown that marynoite works better than other natural iron-containing ores.
Then, 5g of mackerel, 50ml of anaerobic biomass and 50ml of sterilized anaerobic biomass were added to 3 glass bottles of 250ml, respectively, which were prepared again, as controls, to further verify the effectiveness of the ore-binding microorganisms in removing hexavalent chromium. The experimental data show that the removal rates of the three control groups are low and gradually decrease to almost no removal in a short time.
Example 2, column experiments further demonstrate the excellent effect of iron ore on the immobilization of hexavalent chromium in groundwater by microorganisms
Design idea of column experiment: and (4) taking the concentration of hexavalent chromium, the hydraulic retention time and other pollutants as experimental variables to judge the influence degree of the experimental variables on the capability of removing the pentavalent vanadium by the mixed culture of the microorganisms.
In a specific embodiment, the concentration of the pentavalent vanadium can be 10mg/L to 50 mg/L. In a specific embodiment, the hydraulic retention time can be 12-24 h. In a specific embodiment, the other contaminants may be selected from nitrates and the like.
According to a specific example, a polyethylene column (see a cylindrical tube with a bottom diameter of 5cm and a height of 25cm, reference numeral 203 in FIG. 2, three side sampling ports for conveniently taking out microorganisms) was prepared, covered with tinfoil paper, 50g of 1-3mm shell was added as an inorganic carbon source, and 50ml of anaerobic biomass and 200g of Marinolite were added. Quartz sand (1-2mm) was added to mix all media and adjust porosity (e.g., to 36.0% or 36.7%). The synthesized hexavalent chromium-contaminated groundwater free of bicarbonate was passed into the column in an up-flow manner by a peristaltic pump (corresponding to reference numeral 202 in fig. 2). The run time was 180 days in duration and was divided into five stages as shown in table 2 to study the effects of groundwater chemistry and hydrodynamics. Hexavalent chromium removal, chemicals and microbial communities in the aqueous phase are monitored at each stage. In stage 5, the solid reaction products and functional genes were analyzed in depth.
TABLE 2
The results of the column experiments shown in table 2 indicate that hexavalent chromium concentration, hydraulic retention time, and other contaminants such as nitrate affect the removal efficiency, but even though hexavalent chromium concentration is high, hydraulic retention time is short, and the removal rate of hexavalent chromium (23.1 ± 1.22 corresponding to the 4 th stage shown in table 1) is still considerable in the presence of other contaminants.
By sampling and analyzing the filler in the column test, the specific analysis experiment means can comprise XRD, EDS and XTS, and the reduction product trivalent chromium (Cr (OH) is generated in the process of fixing hexavalent chromium)3And CrO (OH) form, ferric iron (as Fe (OH)) as an oxidation product of marynodie3And FeO (OH) form) and harmless Sulfates (SO)4 2-). The products can be naturally precipitated in the underground water, and the secondary pollution of the underground water is effectively prevented.
Furthermore, analysis of the microbial community, related functional genes and metabolites showed that the concentration of bacteria associated with hexavalent chromium reduction such as Geobacter, functional genes such as chrA, YieF, functional gene soxB associated with sulfur-trophism, and cytochrome C associated with ferrous oxidation were significantly increased compared to the concentration in the original anaerobic consortium. This indicates that the synergistic effect of autotrophic and heterologous microorganisms is very important for hexavalent chromium removal. The method has high guiding significance for subsequent experiments and application.
Example 3 penetration Curve experiments further discuss biological and non-biological processes of iron ores and microorganisms in hexavalent chromium removal
Two identical volume polyethylene columns (corresponding to 204 and 205 in fig. 2) were prepared and four evenly distributed sampling ports were added laterally for penetration curve studies. One column was packed with the same components as the column experiment described above in example 2, and the other column was depleted of 50ml anaerobic biomass. For 1PV (pore volume), the hydraulic retention time was set to 2 hours. Continuously detecting the concentration of hexavalent chromium in the water. Thus determining the proportion of biological and non-biological processes in the hexavalent chromium removal process.
In addition, it should be noted that the water inlet air bag 201, the peristaltic pump 202 and the water outlet air bag 205 in fig. 2 are used for maintaining an anaerobic environment during operation.
The penetration curve research result shows that the biological process plays a main role in the hexavalent chromium removal process, and the biological process accounts for 76.0 +/-1.12 percent, and the non-biological process accounts for 24.1 +/-1.43 percent. The addition of the microbiome hexavalent chromium penetrated at 168PV and the non-addition of the microbiome at 33PV, indicating that the combination of biological and chemical (non-biological) processes is achieved by the combination of iron ore plus microorganisms, significantly improving the performance and longevity of the hexavalent chromium removal system.
From the above, it can be seen that the method for fixing hexavalent chromium by using iron ore-supported microorganisms, provided in one or more embodiments of the present disclosure, can significantly improve the treatment efficiency of hexavalent chromium in the groundwater, make the operation simpler and more convenient, and avoid secondary pollution.
The foregoing embodiments are merely illustrative of the principles and utilities of the present invention and are not intended to limit the invention. Any person skilled in the art can modify or change the above-mentioned embodiments without departing from the spirit and scope of the present invention. Accordingly, it is intended that all equivalent modifications or changes which can be made by those skilled in the art without departing from the spirit and technical spirit of the present invention be covered by the claims of the present invention.
Claims (4)
1. A material for fixing hexavalent chromium in groundwater, characterized in that the material comprises at least a microorganism and iron ore, the iron ore being at least used as an inorganic electron donor when the microorganism reduces hexavalent chromium;
the iron ore is Makinuo ore (FeS);
the specific using method of the material comprises the following steps: preparing a polyethylene column with the bottom surface diameter of 5cm and the height of 25cm, covering the polyethylene column with tinfoil paper, adding 50g of shells with the diameter of 1-3mm as an inorganic carbon source, and then adding 50ml of anaerobic synbiotic and 200g of mackenoite; adding quartz sand with the particle size of 1-2mm, mixing all media and adjusting the porosity to 36.0%; enabling the synthesized hexavalent chromium polluted underground water without bicarbonate to flow into a column in an up-flow manner through a peristaltic pump; the running time lasts 180 days and is divided into five stages; wherein, the 1 st stage is that the running time is 0 to 50 days, the hydraulic retention time is 24 hours, the concentration of inlet hexavalent chromium is 10mg/L, and the concentration of initial nitrate is 0 mg/L; the 2 nd stage is that the running time is 51 to 80 days, the hydraulic retention time is 24 hours, the concentration of the inlet hexavalent chromium is 50mg/L, and the initial nitrate concentration is 0 mg/L; the 3 rd stage is that the running time is 81-107 days, the hydraulic retention time is 12 hours, the concentration of inlet hexavalent chromium is 50mg/L, and the initial nitrate concentration is 0 mg/L; the 4-stage is that the operation time is 108-150 days, the hydraulic retention time is 24 hours, the concentration of the fed water hexavalent chromium is 50mg/L, and the initial nitrate concentration is 10 mg/L; the 5 stage is that the operation time is 151-year, the hydraulic retention time is 24 hours, the concentration of inlet hexavalent chromium is 10mg/L, and the initial nitrate concentration is 0 mg/L;
deep analysis is carried out on the solid reaction product and the functional gene in the 5 th stage, and sampling analysis is carried out on the filler in the column, so that the concentrations of the bacteria Geobacter related to hexavalent chromium reduction, the functional genes chrA and yieF, the functional gene soxB related to sulfur oxidation and cytochrome C related to ferrous oxidation are obviously improved compared with the concentration in the original anaerobic symbiont.
2. The material according to claim 1, characterized in that the iron ore is also used to chemically react directly with the hexavalent chromium for removing it.
3. The material of claim 1, further comprising a carbon source that supports growth and reproduction of the microorganism.
4. The material of claim 3, wherein the carbon source comprises an inorganic carbon source comprising sodium bicarbonate or seashell.
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| CN101367576B (en) * | 2008-09-23 | 2010-09-01 | 浙江大学 | Method for removing Cr(VI) in water |
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| CN104129850B (en) * | 2014-08-14 | 2016-09-28 | 合肥工业大学 | A kind of method of azotate pollution in in-situ remediation of underground water |
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| CN104845928A (en) * | 2015-05-28 | 2015-08-19 | 广东工业大学 | Method for processing hexavalent chromium pollution employing synergistic effects of mixed bacteria |
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