CN110156147B - Efficient denitrification and electrogenesis wastewater treatment method - Google Patents

Efficient denitrification and electrogenesis wastewater treatment method Download PDF

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CN110156147B
CN110156147B CN201910374601.1A CN201910374601A CN110156147B CN 110156147 B CN110156147 B CN 110156147B CN 201910374601 A CN201910374601 A CN 201910374601A CN 110156147 B CN110156147 B CN 110156147B
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anolyte
anaerobic
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denitrification
chamber
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CN110156147A (en
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付志敏
孔志远
章院灿
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Inner Mongolia University
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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
    • C02F3/00—Biological treatment of water, waste water, or sewage
    • C02F3/28—Anaerobic digestion processes
    • C02F3/2866—Particular arrangements for anaerobic reactors
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/16—Biochemical fuel cells, i.e. cells in which microorganisms function as catalysts
    • 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
    • C02F2101/16—Nitrogen compounds, e.g. ammonia
    • 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
    • C02F2101/16—Nitrogen compounds, e.g. ammonia
    • C02F2101/166—Nitrites
    • C—CHEMISTRY; METALLURGY
    • C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
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    • C02F2305/00—Use of specific compounds during water treatment
    • C02F2305/06—Nutrients for stimulating the growth of microorganisms
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    • Y02E60/30—Hydrogen technology
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    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
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Abstract

The invention discloses a high-efficiency denitrification and power generation wastewater treatment method, which is based on an anode highly-efficient denitrification microbial fuel cell coupled with an anaerobic ammonia oxidation technology and comprises a conventional double-chamber microbial fuel cell, a magnetic stirring system, an external circuit and a data acquisition system. The invention intermittently operates, a certain amount of organic matters are added after the consumption of the inorganic matrix is finished to excite the hydrolytic acidification of the sludge and the activity of heterotrophic electrogenic bacteria, the device has simple structure, and compared with the traditional anode anaerobic ammonia oxidation MFC, the device has obvious denitrification effect, obviously improved nitrogen load and good electrogenic effect.

Description

Efficient denitrification and electrogenesis wastewater treatment method
The technical field is as follows: the invention relates to a high-efficiency denitrification and power generation wastewater treatment method.
Background art:
energy shortage and environmental pollution restrict the sustainable development of human society. The Microbial Fuel Cell (MFC) technology takes anode electrogenesis microorganisms as a catalyst, directly converts chemical energy stored in pollutants into electric energy through biodegradation, and has two functions of energy generation and pollution treatment. The anaerobic ammonia oxidation (ANAMMOX) technology can directly convert ammonia nitrogen and nitrite nitrogen into nitrogen under anaerobic conditions, and is the most economical and efficient denitrification process so far. Anaerobic ammonia oxidation and MFC technology are combined, synchronous denitrification and power generation can be realized, and the method is a research hotspot in the field of current energy and environment.
The coupling of MFC to Anammox technology is divided into 2 forms of denitrification at the cathode and anode. The cathode coupling denitrification is to inoculate Anammox sludge to an MFC cathode chamber, inoculate electrogenesis microorganisms to the anode chamber, add organic matters such as sodium acetate (-1000 mg/L) and the like as fuel, anode output electrons are transmitted to a cathode through an external circuit, nitric acid nitrogen generated by Anammox reaction receives electrons, autotrophic denitrification generates nitrogen, the quality of effluent water is optimized, the total nitrogen removal rate of the system is improved, the cathode coupling type MFC has good electrogenesis performance, but the nitrite nitrogen can also receive electrons to perform autotrophic denitrification, so that the ammonia nitrogen removal rate is reduced. The anode coupling denitrification is to inoculate Anammox bacteria activated sludge to an MFC anode chamber, ammonia nitrogen is used as fuel to generate electrons, and a cathode electron acceptor can be potassium ferricyanide, potassium permanganate or oxygen in the air. However, the voltage output is quite limited due to the small amount of energy released by the Anammox process. In addition, 11% of nitrate nitrogen is generated in the ANAMMOX reaction process, so that the total nitrogen of effluent of system effluent is difficult to stably reach the standard. Although exogenous organic matters are added into the ANMMOX system, the nitrogen concentration of the effluent of the system can be reduced, but the treatment cost of the wastewater is increased.
Aiming at the problem of lower voltage output of the existing anode Anammox coupling type MFC denitrification technology, the method rapidly stimulates the hydrolysis acidification power generation of the activated sludge by utilizing the mode of subsequently adding a carbon source, realizes the synchronous wastewater denitrification and the biological power generation, and obviously improves the output voltage and current of the system; the organic matter generated by in-situ hydrolysis and acidification of the sludge is used as an electron donor in the heterotrophic denitrification process, so that the operation cost of the ANAMMOX system can be effectively reduced, the in-situ electric field of the microbial cell is used for stimulating the activity of functional bacteria, and the operation stability of the anode ANAMMOX coupled MFC denitrification system is improved; the in-situ hydrolysis and acidification of the activated sludge reduce the yield of the excess sludge.
The invention content is as follows:
the invention aims to overcome the defects of the prior art and provide a microbial fuel cell based on anaerobic ammonia oxidation.
The main device of the microbial fuel cell is a double chamber, wherein the main device comprises an anaerobic anode reaction chamber and a chemical cathode reaction chamber; the anaerobic anode reaction chamber is connected with the chemical cathode reaction chamber through a flange, and a cation exchange membrane is fixed on the flange for separation; the inside of the anaerobic anode reaction chamber is provided with anolyte and an anode, the anolyte is inoculated with anaerobic ammonia oxidation sludge, the anaerobic anode is attached with the anaerobic ammonia oxidation sludge, the upper side wall of the anaerobic anode reaction chamber is provided with a water inlet pipe, the lower side wall of the anaerobic anode reaction chamber is provided with a water outlet pipe, the chemical cathode reaction chamber is internally provided with catholyte and a cathode, the upper side wall of the chemical cathode reaction chamber is provided with a water inlet pipe, and the lower side wall of the chemical cathode reaction chamber is provided with a water outlet pipe; two ends of the load are respectively connected with the anaerobic anode and the cathode through leads; the data collected at the two ends of the load are recorded in a computer through a data collector. The main body device is provided with a constant-temperature magnetic stirrer body and a magnetic stirrer.
The efficient denitrogenation and electricity generating waste water treating process features that the anode chamber is reacted in stages, the initial stage includes anaerobic ammoxidation of the anode liquid in the anaerobic anode chamber to produce nitrogen, and after the reaction, the solution containing high concentration organic matter is injected into the anode reaction chamber to produce electricity via anaerobic hydrolysis and acidification of active sludge. The method comprises the following specific steps: firstly, an electrochemical system is assembled, anolyte is added through a water inlet pipe of an anaerobic anode reaction chamber, inorganic matrix is consumed after reaction is finished for a period of time, and a solution of a certain amount of high-concentration organic matters in the anolyte is added through the water inlet pipe of the anaerobic anode reaction chamber to excite the activity of electrogenesis bacteria to generate electricity. Electrons generated by the anode reaction are transmitted to the cathode through an external circuit, the transmission of the electrons accelerates the hydrolysis and acidification of the activated sludge in the anode chamber, organic matters generated by the hydrolysis and acidification improve the denitrification efficiency, and current is generated to recover energy. And after the electricity generation is finished, removing the anolyte, and introducing a new anolyte to start the next period.
The anolyte (4) is wastewater containing ammonia and nitrite, and the concentration ratio of organic matter COD and nitrogen is lower than 1.
Further, the high-efficiency denitrification and electricity generation wastewater treatment method comprises the following steps: after the consumption of the inorganic matrix in the anolyte is finished for 1-12h, adding a certain amount of high-concentration volatile fatty acid salt solution into the anolyte to ensure that the COD concentration of the anolyte reaches 80-400mg/L, and exciting the activity of the electrogenic bacteria.
Further, the high-efficiency denitrification and electricity generation wastewater treatment method comprises the following steps: the ratio of the time of the anaerobic ammonia oxidation reaction stage to the time of the sludge hydrolytic acidification power generation stage is 4: 1-1: 4.
Further, the high-efficiency denitrification and electricity generation wastewater treatment method comprises the following steps: the anaerobic anode and the chemical cathode are made of sheet conductive materials such as carbon paper, carbon cloth, carbon felt and graphite felt inserted with metal wires or meshes.
Further, the high-efficiency denitrification and electricity generation wastewater treatment method comprises the following steps: the catholyte is potassium ferricyanide, potassium permanganate or dissolved oxygen.
The invention has the beneficial effects that:
(1) through the coupling of the anaerobic ammonia oxidation process and the hydrolysis acidification of the activated sludge, high voltage can be output while wastewater containing nitrite nitrogen, ammonia nitrogen and low COD is treated.
(2) The activated sludge hydrolytic acidification provides endogenous organic carbon for denitrification, so that the denitrification efficiency of the system can be effectively improved, and the denitrification operation stability of the system is improved.
(3) The in-situ hydrolysis and acidification of the activated sludge reduce the yield of the excess sludge.
Description of the drawings:
FIG. 1 is a schematic diagram of a high efficiency denitrification and electricity generation microbial fuel cell system;
FIG. 2 shows an example of using a catalyst containing 50mg/L NH4 +-N、64mg/L NO2 --N; using 75mg/L COD low-carbon nitrogen load waste water as anolyte, taking a cycle of 24h, adding sodium acetate when the period is 12h to ensure that the COD concentration of the anolyte reaches 100mg/L, and running a cycle of power generation schematic diagram when the sodium acetate is not added.
FIG. 3 shows that in the above examples, a catalyst containing 50mg/L NH was used4 +-N、64mg/L NO2 --N; 75mg/L COD low-carbon nitrogen load waste water is used as anolyte, 24h is a period, sodium acetate is not added to be used as a stage I, sodium acetate is added to ensure that the COD concentration of the anolyte reaches 100mg/L to be used as a stage II when 12h is carried out, and a water outlet nitrogen concentration graph is obtained during continuous operation.
The specific implementation mode is as follows:
the embodiments of the present invention will be explained with reference to the drawings, but the invention is not limited thereto. The main body device is a double-chamber microbial electrochemical reactor, which comprises two independent reaction areas, namely an anaerobic anode reaction chamber (1) and a chemical cathode reaction chamber (2); a cation exchange membrane (3) is fixed between the anaerobic anode reaction chamber (2) and the chemical cathode reaction chamber (3) for separation; an anolyte (4) and an anode (5) are arranged in the anaerobic anode reaction chamber (2), anaerobic ammonia oxidation sludge is inoculated in the anolyte (4), anaerobic ammonia oxidation sludge is attached to the anaerobic anode (5), a water inlet pipe (6) is arranged on the side wall of the lower part of the anaerobic anode reaction chamber (2), and a water outlet pipe (7) is arranged on the side wall of the upper part of the anaerobic anode reaction chamber; a cathode liquid (10) and a cathode (11) are filled in the chemical cathode reaction chamber (3), a water inlet pipe (12) is arranged on the side wall of the lower part of the chemical cathode reaction chamber (3), and a water outlet pipe (13) is arranged on the side wall of the upper part of the chemical cathode reaction chamber; an opening (19) at the upper part of the anaerobic anode reaction chamber (2) is connected with a gas guide pipe (20) to a water-sealed bottle (21) to lead out generated gas and ensure the sealed environment of the anode chamber. The bottom of the anaerobic anode reaction chamber (2) and the chemical cathode reaction chamber (3) is provided with a constant temperature magnetic stirrer body (9) and a magnetic stirrer (8). Two ends of the load (14) are respectively connected with the anaerobic anode (5) and the cathode (11) through leads (15); the data collected at two ends of the load (14) are connected with a data collector (16) through a wire (15), and the data collector (16) is recorded in a computer (18) through a data transmission line (17).
Referring to fig. 1, the anode highly efficient denitrified microbial fuel cell coupled with the anammox technology comprises a conventional two-chamber microbial fuel cell, a magnetic stirring system, an external circuit and a data acquisition system. The method comprises the following specific steps: according to the figure 1, a microbial fuel cell system is assembled, anaerobic ammonia oxidation sludge is inoculated in an anode reaction chamber 1, the inoculation volume is 20%, anolyte 4 containing ammonia nitrogen and nitrite nitrogen and low COD is added, catholyte 5 containing potassium ferricyanide is inoculated in a cathode reaction chamber 2, and the catholyte 5 enters from a water inlet 12 and exits from a water outlet 13 at a certain speed. After the anolyte 4 reacts for 12 hours, high-concentration sodium acetate is added until the COD concentration of the anolyte reaches 100mg/L, and after the sodium acetate is added for 12 hours, the anolyte is removed and replaced by new solution.

Claims (1)

1. A high-efficiency denitrification and power generation wastewater treatment method is characterized by comprising the following steps: the method comprises the following steps of utilizing a double-chamber microbial fuel cell device, carrying out reactions in an anode chamber in stages, carrying out anaerobic ammoxidation on anolyte in an anaerobic anode chamber in an initial stage to generate nitrogen, and injecting a solution containing high-concentration organic matters into an anode reaction chamber after the reactions are finished to cause anaerobic hydrolytic acidification of activated sludge to generate electricity; the ratio of the time of the anaerobic ammonia oxidation reaction stage to the time of the sludge hydrolytic acidification power generation stage is 4: 1-1: 4;
the method comprises the following specific steps: firstly, assembling an electrochemical system, adding anolyte through a water inlet pipe of an anaerobic anode reaction chamber, reacting for a period of time, finishing the consumption of inorganic matrix, adding a solution containing a certain amount of high-concentration organic matters into the anolyte through the water inlet pipe of the anaerobic anode reaction chamber, and exciting the activity of electrogenic bacteria to generate electricity; electrons generated by the anode reaction are transmitted to the cathode through an external circuit, the transmission of the electrons accelerates the hydrolysis and acidification of the activated sludge in the anode chamber, organic matters generated by the hydrolysis and acidification improve the denitrification efficiency, and current is generated to recover energy; after the electricity generation is finished, discharging the anolyte, and adding new anolyte to start the next period; the anolyte is wastewater containing ammonia and nitrite, and the concentration ratio of organic matter COD to nitrogen is lower than 1;
after the anaerobic ammonia oxidation reaction of the anolyte is finished, namely after the inorganic matrix of the anolyte is consumed for 1-12 hours, adding a certain amount of high-concentration volatile fatty acid salt solution into the anolyte to ensure that the COD concentration of the anolyte reaches 80-400mg/L, and exciting the activity of electrogenic bacteria.
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Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN101667649A (en) * 2009-09-29 2010-03-10 南开大学 Microbe fuel cell inoculation and acclimation starting method for energizing organic waste water
CN102276064A (en) * 2011-07-18 2011-12-14 北京师范大学 Anaerobic-aerobic integrated microbial fuel cell wastewater treatment system
CN103094597A (en) * 2013-01-25 2013-05-08 浙江大学 Microbial fuel cell with function of efficiently and synchronously removing nitrogen and carbon
KR20170054781A (en) * 2015-11-10 2017-05-18 한양대학교 산학협력단 Method for treating wastewater using microbial fuel cell with dual electrode structure
CN206607130U (en) * 2017-03-30 2017-11-03 重庆交通大学 A kind of sewage disposal purifier

Patent Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN101667649A (en) * 2009-09-29 2010-03-10 南开大学 Microbe fuel cell inoculation and acclimation starting method for energizing organic waste water
CN102276064A (en) * 2011-07-18 2011-12-14 北京师范大学 Anaerobic-aerobic integrated microbial fuel cell wastewater treatment system
CN103094597A (en) * 2013-01-25 2013-05-08 浙江大学 Microbial fuel cell with function of efficiently and synchronously removing nitrogen and carbon
KR20170054781A (en) * 2015-11-10 2017-05-18 한양대학교 산학협력단 Method for treating wastewater using microbial fuel cell with dual electrode structure
CN206607130U (en) * 2017-03-30 2017-11-03 重庆交通大学 A kind of sewage disposal purifier

Non-Patent Citations (1)

* Cited by examiner, † Cited by third party
Title
《微生物燃料电池同步脱氮产电性能及机理研究》;张吉强;《中国博士学位论文全文数据库 工程科技 I辑》;20141215;第五章第5.1、5.3节，图5.1 *

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