CN111115842B - Method for treating ammonium perchlorate wastewater - Google Patents
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- CN111115842B CN111115842B CN201911320602.4A CN201911320602A CN111115842B CN 111115842 B CN111115842 B CN 111115842B CN 201911320602 A CN201911320602 A CN 201911320602A CN 111115842 B CN111115842 B CN 111115842B
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Abstract
The invention discloses a method for treating ammonium perchlorate wastewater, which comprises the following steps: obtaining intermediate products of hydrogen and volatile fatty acid through an anaerobic digestion hydrogen-producing and acid-producing stage of the kitchen waste; providing an electron donor and a carbon source for the reduction process of ammonium perchlorate by perchlorate reducing bacteria by using intermediate product hydrogen and volatile fatty acid; and reducing the ammonium perchlorate into chloride ions by adopting a three-stage degradation combined process of hydrogen autotrophic reduction, organic acid heterotrophic reduction and iron/sulfur autotrophic reduction, reducing the concentration of the ammonium perchlorate wastewater and finishing the treatment of the ammonium perchlorate wastewater. The invention can obviously improve the removal effect of the ammonium perchlorate wastewater, simultaneously generates the methane as clean energy for life production and use, and has obvious improvement on the aspects of economic rationality and process operability.
Description
Technical Field
The invention belongs to the technical field of environmental biology, relates to an anaerobic digestion and perchlorate biological reduction method, and particularly relates to a method for treating ammonium perchlorate wastewater.
Background
Ammonium perchlorate is used as a strong oxidant and is widely applied to aerospace and military industries such as rocket solid propellant, missile fuel, explosive and the like in recent years. Ammonium perchlorate in waste rocket engines and explosives can generate a large amount of ammonium perchlorate wastewater, and the problem needs to be solved urgently.
At present, the treatment method of ammonium perchlorate wastewater comprises a physicochemical method and a biological method. The physical and chemical methods include activated carbon/biomass adsorption method, ion exchange method, reverse osmosis membrane separation method (reverse osmosis RO, ultrafiltration UF, nanofiltration NF), etc.; the activated carbon adsorbent has limited capacity and high preparation cost, can generate explosive waste carbon to cause secondary pollution, and is not suitable for being used as a treatment technology of large-scale ammonium perchlorate wastewater; the ion exchange method can efficiently remove trace ammonium perchlorate in water, but the high-selectivity ion exchange resin has high cost, the used resin contains perchlorate and needs further treatment, and other coexisting ions in the water easily influence the removal effect of the resin on the ammonium perchlorate; the reverse osmosis membrane method can treat the perchlorate wastewater to the ultrapure water level, but can face the problems of membrane pollution and high-cost preparation of the membrane, the permeation of the perchlorate is influenced by other ions in water, and the residual high-concentration saline water needs to be further treated, so that the membrane filtration is difficult to be used for removing the ammonium perchlorate wastewater on a large scale. Micro-meterThe biological method is known as a feasible technology for treating the ammonium perchlorate wastewater due to low cost, high efficiency and no pollution. Since perchlorate has a high reduction potential (ClO)4 -/Cl-Eo ═ 1.287V), which can act as an ideal metabolic electron acceptor for microorganisms, perchlorate is finally reduced to chloride in reducing bacteria using perchlorate reductase when sufficient organic/inorganic substance is supplied as an electron donor to the reaction system: ClO4 -—ClO3 -—ClO2 -—Cl-+O2。
Perchlorate, as an endocrine disruptor, interferes with the uptake of iodine element by the thyroid gland of a human body, and iodine is an essential element for producing thyroid hormone, which is one of the most important hormones in the human body, and the lack of thyroid hormone causes endocrine dyscrasia and poor development of the central nerve.
In summary, an economical and efficient treatment method is needed to solve the problem of ammonium perchlorate pollution and prevent ammonium perchlorate from entering the environment to cause serious harm. Research has shown that the microbiological method is a feasible method for removing ammonium perchlorate, but needs to consider providing sufficient electron donor for a microbiological system in the biological treatment process, and the electron donor is selected by adopting an external dosing method at present, so that the improvement in economic rationality and process operability needs to be further evaluated.
Disclosure of Invention
The invention aims to provide a method for treating ammonium perchlorate wastewater so as to solve one or more of the technical problems. The invention can obviously improve the removal effect of the ammonium perchlorate wastewater, simultaneously generates the methane as clean energy for life production and use, and has obvious improvement on the aspects of economic rationality and process operability.
In order to achieve the purpose, the invention adopts the following technical scheme:
the invention relates to a method for treating ammonium perchlorate wastewater, which comprises the following steps:
obtaining intermediate products of hydrogen and volatile fatty acid through an anaerobic digestion hydrogen-producing and acid-producing stage of the kitchen waste;
providing an electron donor and a carbon source for the reduction process of ammonium perchlorate by perchlorate reducing bacteria by using intermediate product hydrogen and volatile fatty acid;
and reducing the ammonium perchlorate into chloride ions by adopting a three-stage degradation combined process of hydrogen autotrophic reduction, organic acid heterotrophic reduction and iron/sulfur autotrophic reduction, reducing the concentration of the ammonium perchlorate wastewater and finishing the treatment of the ammonium perchlorate wastewater.
The invention relates to a method for treating ammonium perchlorate wastewater, which comprises the following steps:
in the stage of producing hydrogen and acid from kitchen waste, hydrolyzing macromolecular carbohydrates, proteins and fats in the kitchen waste into micromolecular organic acids and alcohols by using hydrolytic zymogens, and generating an intermediate product under the action of the hydrogen-producing acid-producing bacteria; the intermediate product comprises: hydrogen and volatile fatty acids;
in the methane production stage, methanogens are used to convert hydrogen and volatile fatty acid, which are the products of the hydrogen-producing and acid-producing stage of the kitchen waste, into methane, and bottom slag is obtained;
an ammonium perchlorate reducing bacteria domestication stage, namely, taking the bottom slag in the methane production stage as inoculation mud, adding ammonium perchlorate, and domesticating to obtain ammonium perchlorate reducing bacteria;
in the primary degradation stage of the ammonium perchlorate, the product hydrogen in the hydrogen-producing and acid-producing stage of the kitchen waste is used as an electron donor, and ammonium perchlorate reducing bacteria are used for reducing the ammonium perchlorate into chloride ions;
in the ammonium perchlorate secondary degradation stage, volatile fatty acid which is a product in the kitchen waste hydrogen-producing and acid-producing stage is used as an electron donor and a carbon source, and ammonium perchlorate is reduced into chloride ions by ammonium perchlorate reducing bacteria;
and in the ammonium perchlorate three-stage degradation stage, adding sulfur powder or iron powder, and reducing the ammonium perchlorate into chloride ions by using ammonium perchlorate reducing bacteria.
The invention is further improved in that in the stage of producing hydrogen and acid from kitchen waste, the concentrated residual sludge of an urban domestic sewage treatment plant is added for adjusting the C/N ratio, the buffer capacity and the trace elements of the kitchen waste, so that the kitchen waste anaerobic digestion system can stably operate.
The invention has the further improvement that the ratio of organic components of the kitchen waste to the residual sludge in the whole treatment process is 1: 1.
The invention has the further improvement that the inoculation mud adopted in the anaerobic digestion process of the kitchen waste comes from the digestive juice in the mesophilic digestion tank of the municipal sewage treatment plant; before use, sodium acetate is used as a carbon source for culture, and after the stability of methanogenesis is measured, the strain is used as inoculation mud to be inoculated into an anaerobic digestion system, so that the inoculation rate is ensured to be more than or equal to 5 percent of the matrix.
The invention is further improved in that the bottom slag in the methane production stage is used as an inoculum of the ammonium perchlorate wastewater treatment system; taking sodium acetate as a carbon source, adding ammonium perchlorate with a certain concentration for culturing, and determining that ammonium perchlorate is degraded stably, and then considering that the acclimation of ammonium perchlorate reducing bacteria is successful; inoculating the successfully domesticated strain into an ammonium perchlorate reduction system, wherein the inoculation rate is more than or equal to 5 percent of the matrix.
The invention is further improved in that the operation temperature, pH and oxidation-reduction potential of the kitchen waste hydrogen-producing acid-producing stage, the methane-producing stage and the ammonium perchlorate reducing bacteria domestication stage are controlled to maintain the activity of the hydrogen-producing acid-producing bacteria, the methane-producing bacteria and the ammonium perchlorate reducing bacteria.
The further improvement of the invention is that the treatment method can treat the high-concentration ammonium perchlorate wastewater with the concentration of 100mg/L to zero emission through three-stage combined degradation, and the removal rate can reach more than 98 percent.
Compared with the prior art, the invention has the following beneficial effects:
the treatment method can obviously improve the removal effect of the ammonium perchlorate wastewater, and simultaneously generates methane as clean energy for life production. According to the invention, on the basis of removing perchlorate by a biological method, an anaerobic digestion process of kitchen waste is introduced, the intermediate product of anaerobic digestion is utilized to a great extent, a multi-stage combined degradation process is adopted to jointly remove ammonium perchlorate, a large amount of electron donors are not required to be additionally added, the process operation is simple, and the ammonium perchlorate is thoroughly treated.
The invention provides a new idea and a new prospect for removing ammonium perchlorate in practical application of a biological method. In particular, miningThe method for removing the ammonium perchlorate wastewater does not need to additionally add a large amount of electron donors, and adopts autotrophic heterotrophic multi-stage series treatment, so that the high-concentration ammonium perchlorate wastewater can be completely removed, and the ammonium perchlorate is prevented from entering the environment to cause serious harm. The anaerobic digestion treatment method can be used for effectively carrying out anaerobic digestion on the kitchen waste, reducing the environmental pollution load, simultaneously generating the biogas clean energy, and has important significance for sustainable development of the energy and treatment and disposal of the kitchen waste. In the invention, hydrogen generated by anaerobic digestion of kitchen waste is adopted to perform ammonium perchlorate autotrophic reduction by ammonium perchlorate autotrophic reducing bacteria, and acid generated by anaerobic digestion is adopted as heterotrophic bacteria electron donor and carbon source to perform heterotrophic reduction of ammonium perchlorate. And finally, adding industrial waste sulfur powder or iron powder as an autotrophic electron donor to carry out three-stage degradation so as to deeply treat the residual ammonium perchlorate in the water. The method is simple, convenient, rapid and efficient to operate, fully utilizes the existing resources, and is economic and environment-friendly. H generated in anaerobic digestion process of kitchen waste2And VFAs can respectively provide different types of electron donors for the reduction process of the ammonium perchlorate, and the kitchen waste can provide enough carbon source and nutrient substances for the perchlorate reducing bacteria and is used for the rapid propagation and growth of the perchlorate reducing bacteria. After the kitchen waste is subjected to the hydrogen production and acid production stage, hydrogen is generated and used as an electron donor for the ammonium perchlorate autotrophic reduction, and simultaneously, the generated acid is used as an electron donor and a carbon source for the ammonium perchlorate heterotrophic reduction, and can be further utilized by methanogens to generate methane. The anaerobic digestion hydrogen-production acid-production stage and the methane-production stage of the kitchen waste are separated, so that the growth conditions suitable for different bacteria can be better controlled, the harm of acid accumulation to methanogenic bacteria can be reduced, and the collection of hydrogen and methane is facilitated. The biogas (methane and carbon dioxide) generated in the methane production stage is collected and used for power generation or other energy output for utilization after passing through a purification facility.
In the invention, in order to prevent the system from being damaged in the anaerobic digestion process of the kitchen waste, the concentrated excess sludge of the municipal domestic sewage treatment plant is added for adjusting C/N, buffer capacity and trace elements of the kitchen waste and ensuring the stability and high efficiency of the anaerobic digestion system.
According to the invention, the operation temperature, pH and oxidation-reduction potential of the kitchen waste hydrogen-producing acid-producing stage, the methane-producing stage and the ammonium perchlorate reducing bacteria domestication stage are controlled, so that the activities of the hydrogen-producing acid-producing bacteria, the methane-producing bacteria and the ammonium perchlorate reducing bacteria are maintained, the anaerobic digestion is ensured, and the perchlorate is effectively reduced into chloride ions. Wherein the optimal pH of acid-producing bacteria is 5.8, the proper temperature of methanogen is 37.5 ℃, the pH is kept at 7.0-7.2, the anaerobic condition is strictly controlled, and the oxidation-reduction potential is ensured to be lower than-350 mV. The optimum temperature of the ammonium perchlorate reducing bacteria is 35 ℃, the optimum pH value is 7.5, and the system is ensured to maintain an anaerobic environment.
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In order to more clearly illustrate the embodiments of the present invention or the technical solutions in the prior art, the drawings used in the description of the embodiments or the prior art are briefly introduced below; it is obvious that the drawings in the following description are some embodiments of the invention, and that for a person skilled in the art, other drawings can be derived from them without inventive effort.
FIG. 1 is a schematic block diagram of a process for treating ammonium perchlorate wastewater according to an embodiment of the invention.
Detailed Description
In order to make the purpose, technical effect and technical solution of the embodiments of the present invention clearer, the following clearly and completely describes the technical solution of the embodiments of the present invention with reference to the drawings in the embodiments of the present invention; it is to be understood that the described embodiments are only some of the embodiments of the present invention. Other embodiments, which can be derived by one of ordinary skill in the art from the disclosed embodiments without inventive faculty, are intended to be within the scope of the invention.
The method for treating the ammonium perchlorate wastewater comprises the following steps: (1) the method comprises the steps of (1) a kitchen waste hydrogen-producing and acid-producing stage, (2) a methane-producing stage, (3) an ammonium perchlorate reducing bacteria domestication stage, (4) an ammonium perchlorate primary degradation stage, (5) an ammonium perchlorate secondary degradation stage and (6) an ammonium perchlorate tertiary degradation stage.
After the hydrogen and acid production stage of the kitchen waste is completed, entering a methane production stage; wherein, hydrogen generated in the hydrogen-producing and acid-producing stage of the kitchen waste is supplied to the primary degradation stage of the ammonium perchlorate, and part of acid generated in the hydrogen-producing and acid-producing stage of the kitchen waste is supplied to the secondary degradation stage of the ammonium perchlorate.
After the methanogenesis stage is completed, the bottom slag enters an ammonium perchlorate reducing bacteria domestication section, and then primary degradation, secondary degradation and tertiary degradation are sequentially carried out; wherein, enough industrial waste sulfur powder or iron powder is added in the three-stage degradation to reduce the ammonium perchlorate by autotrophy.
Optionally, inoculating acid-producing bacteria in the stage of producing hydrogen and acid by using kitchen waste; and (4) inoculating methanogenic bacteria at the methanogenic stage, and adjusting the operating conditions suitable for the growth of the acid-producing bacteria and the methanogenic bacteria. And the kitchen waste and the excess sludge are mixed, so that the stability of an anaerobic digestion system is ensured.
Optionally, collecting hydrogen generated in the hydrogen-producing and acid-producing stage of the kitchen waste and entering the primary degradation stage of the ammonium perchlorate; the hydrogen provides an autotrophic electron donor for the ammonium perchlorate reducing bacteria, and perchlorate is reduced into chloride ions.
Optionally, acid generated in the kitchen waste hydrogen-producing acid-producing stage enters the ammonium perchlorate secondary degradation stage synchronously and is consumed as a heterotrophic electron donor and a carbon source by perchlorate heterotrophic reducing bacteria. And (4) allowing the bottom slag in the methane production stage to enter an ammonium perchlorate reducing bacteria domestication section for ammonium perchlorate reducing bacteria domestication. Acid generated in the kitchen waste hydrogen-producing and acid-producing stage enters a methane-producing stage to provide nutrients for methanogens, and the methanogens convert the methanogens into methane.
Collecting the methane generated in the methane generation stage as clean energy for production and living.
In the treatment method, the ammonium perchlorate wastewater which is partially degraded in the primary degradation stage of the ammonium perchlorate continues to enter the secondary degradation stage. And (3) continuously introducing the ammonium perchlorate wastewater subjected to secondary degradation into a third-stage degradation stage, performing sulfur autotrophy or iron autotrophy reduction on the residual ammonium perchlorate by using waste sulfur powder or iron powder as an electron donor in the third-stage degradation stage, and finally discharging the final effluent which completely meets the standard. Compared with the prior art, the invention has the advantages that: the method for removing the ammonium perchlorate wastewater does not need to additionally add a large amount of electron donors, and can completely remove the high-concentration ammonium perchlorate wastewater by adopting autotrophic heterotrophic multi-stage series treatment, thereby preventing the ammonium perchlorate from entering the environment to cause serious harm. The anaerobic digestion treatment method can be used for effectively carrying out anaerobic digestion on the kitchen waste, reducing the environmental pollution load, simultaneously generating the biogas clean energy, and has important significance for sustainable development of the energy and treatment and disposal of the kitchen waste. According to the invention, hydrogen generated by anaerobic digestion of kitchen waste is adopted to perform ammonium perchlorate autotrophic reduction by reducing bacteria, and acid generated by anaerobic digestion is adopted as a heterotrophic electron donor to perform heterotrophic reduction of ammonium perchlorate. And finally, adding waste sulfur powder or iron powder as an autotrophic electron donor to carry out three-stage degradation for deeply treating the residual ammonium perchlorate in the water. The method is simple and convenient to operate, rapid, high in efficiency, economic and environment-friendly, and fully utilizes the existing resources.
In conclusion, the invention discloses a method for treating ammonium perchlorate wastewater, which combines a kitchen waste anaerobic digestion process with a biological ammonium perchlorate wastewater reduction process. The ammonium perchlorate wastewater is completely removed by utilizing three-stage degradation by combining the processes of autotrophic reduction, heterotrophic reduction and autotrophic reduction of ammonium perchlorate. The method avoids the operation of adding a large amount of electron donors and carbon sources in the previous ammonium perchlorate reduction process by a biological method, and utilizes H generated in the anaerobic digestion process of kitchen waste2And VFAs can provide sufficient electron donor for ammonium perchlorate removal while reducing H2And excessive accumulation of VFAs during anaerobic digestion inhibits methanogen activity. Finally, waste sulfur powder or iron powder is adopted to deeply reduce the ammonium perchlorate remained in the water, so that the maximum effective utilization of resources is achieved and the ammonium perchlorate is completely removed. The method fully utilizes the characteristic that the intermediate product in the anaerobic digestion process of the kitchen waste can provide an electron donor for reducing the ammonium perchlorate by a biological method, realizes the synchronous degradation of the kitchen waste and the ammonium perchlorate wastewater, has the advantages of high treatment efficiency, economy, high efficiency and the like, and has strong practical value for the treatment of the ammonium perchlorate wastewater.
Although the present invention has been described in detail with reference to the above embodiments, those skilled in the art can make modifications and equivalents to the embodiments of the present invention without departing from the spirit and scope of the present invention, which is set forth in the claims of the present application.
Claims (5)
1. A method for treating ammonium perchlorate wastewater is characterized by comprising the following steps:
s1: in the stage of producing hydrogen and acid from kitchen waste, hydrolyzing macromolecular carbohydrates, proteins and fats in the kitchen waste into micromolecular organic acids and alcohols by using hydrolytic zymogens, and generating an intermediate product under the action of the hydrogen-producing acid-producing bacteria; the intermediate product comprises: hydrogen and volatile fatty acids;
s2: in the methane production stage, methanogens are used to convert hydrogen and volatile fatty acid, which are the products of the hydrogen-producing and acid-producing stage of the kitchen waste, into methane, and bottom slag is obtained;
s3: in the acclimation stage of the ammonium perchlorate reducing bacteria, the obtained bottom slag is used as inoculation mud, sodium acetate is used as a carbon source, ammonium perchlorate is added, and the ammonium perchlorate reducing bacteria are acclimated to obtain the ammonium perchlorate reducing bacteria;
s4: in the first-stage degradation stage of the ammonium perchlorate, the product hydrogen in the S1 stage is used as an electron donor, and ammonium perchlorate reducing bacteria are used for reducing the ammonium perchlorate into chloride ions;
s5: in the ammonium perchlorate secondary degradation stage, the volatile fatty acid product in the S1 stage is used as an electron donor and a carbon source, and ammonium perchlorate is reduced into chloride ions by ammonium perchlorate reducing bacteria;
s6: and in the ammonium perchlorate three-stage degradation stage, adding sulfur powder or iron powder, and reducing the ammonium perchlorate into chloride ions by using ammonium perchlorate reducing bacteria.
2. The method for treating ammonium perchlorate wastewater according to claim 1, characterized in that the excess sludge concentrated by the municipal sewage treatment plant is added at the S1 stage to adjust the C/N ratio, the buffering capacity and the trace elements of the kitchen waste, so that the kitchen waste anaerobic digestion system can operate stably.
3. The method for treating ammonium perchlorate wastewater according to claim 2, characterized in that the ratio of organic components of the kitchen waste and the excess sludge in the whole treatment process is 1: 1.
4. The method for treating ammonium perchlorate wastewater according to claim 2, characterized in that the inoculation sludge adopted in the anaerobic digestion process of the kitchen waste is from a digestive juice in a mesophilic digestion tank of a municipal sewage treatment plant;
before use, sodium acetate is used as a carbon source for culture, and after the stability of methanogenesis is measured, the strain is used as inoculation mud to be inoculated into an anaerobic digestion system, so that the inoculation rate is ensured to be more than or equal to 5 percent of the matrix.
5. The method for treating ammonium perchlorate wastewater as claimed in claim 1, wherein the operating temperature, pH and oxidation-reduction potential of the S1-S3 stages are controlled to maintain the activity of hydrogen-producing acid-producing bacteria, methanogenic bacteria and ammonium perchlorate-reducing bacteria.
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