CN103872368B - Interactive three Room biological fuel cell devices and the method being applied to denitrogenation of waste water thereof - Google Patents
Interactive three Room biological fuel cell devices and the method being applied to denitrogenation of waste water thereof Download PDFInfo
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- H—ELECTRICITY
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- H01M8/16—Biochemical fuel cells, i.e. cells in which microorganisms function as catalysts
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Abstract
The invention discloses a kind of interactive three Room biological fuel cell devices and the method being applied to denitrogenation of waste water thereof, belong to saprobia and repair field, particularly relate to for the denitrification denitrogenation processing method containing nitrate nitrogen waste water。The present invention is on the basis of traditional dual chamber biological fuel cell, and negative electrode uses nitrate to replace oxygen as electron acceptor, and constructs three Room biological fuel cells of grading electrode room, both sides cathode chamber。Simultaneously by Interactive control switch Interactive control grading electrode and the Guan Bi of both sides negative electrode, off-state so that the electrode denitrification of negative electrode and non-electrode denitrification process reasonable coordination carry out。The method produces electric current sustainably and effectively removes nitrate nitrogen, saves the organic carbon source needed for denitrification simultaneously, is a kind of based on energy-saving and cost-reducing Novel sewage treatment method, has good application prospect。
Description
Technical field
The present invention relates to water Treatment and recovery and utilize field, specifically efficiently process containing nitrate nitrogen waste water and realize the recoverable a kind of interactive three Room biological fuel cells of electricity and the method being applied to denitrogenation of waste water thereof simultaneously。
Background technology
The excessive emissions of nitrogen may result in body eutrophication, brings significant damage to the mankind。Since " 12 ", China still adheres to deeply implementing and economizes on resources and protect environment fundamental state policy, develops a circular economy, and " energy-saving and emission-reduction " problem is the focus of research all the time。Therefore, in the face of the pressure of ever-increasing nitrogen in sewage reduction, it would be highly desirable to develop the sewage water denitrification new technique of " energy-saving and emission-reduction "。
Microbiological fuel cell (MFC, also biological fuel cell it is called for short) it is the new and high technology of 21 century water treatment field, it it is a kind of novel saprobia recovery technique, have and remove organic pollution simultaneously and obtain the advantage of energy output, have also been obtained increasing concern in field of waste water treatment in recent years。According to existing achievement in research, MFC will be expected to be applied to actual waste water denitrogenation engineering, become novel denitrogenation of waste water technology energy-conservation, efficient。
In traditional biological denitrification denitrification process, organic carbon source is important restrictive factor。The organic carbon source deficiency and China's municipal sewage plant is generally intake, causes that nitric efficiency is low。If carbon-nitrogen ratio is too high, residual organic substances need to process further；If carbon-nitrogen ratio is low, then denitrification efficiency is low, and has the accumulation of nitrite。
MFC negative electrode denitrification process, owing to introducing the reduction of electrode, a required electronics part can derive from the electronics that organic carbon source produces in microbial metabolism, another part (under biological catalysis) can directly obtain from cathode electrode, therefore MFC available electron donor in actual waste water denitrification process is more extensive, and its denitrification process is non-electrode denitrification and the coefficient result of electrode denitrification。So, use MFC that sewage is carried out denitrification denitrogenation, can effectively reduce carbon-nitrogen ratio, it is possible to the problem that needed for making up sewage denitrification, organic carbon source is not enough。
At present, microbiological fuel cell denitrogenation aspect has been carried out substantial amounts of research by Chinese scholars。Clauwaert etc. confirm that biological-cathode type MFC can be used in denitrification first, achieve the function of denitrogenation simultaneously, de-carbon and electrogenesis, obtain 0.146kg/m every day in MFC3The clearance of nitrate。Virdis etc. by external aerobic nitrification reactor, the A/O technique of tradition denitrogenation and MFC series combination, carry out denitrogenation, de-carbon simultaneously, it may be achieved every day 2kg/m3COD and 0.41kg/m3The clearance of nitrate。Virdis etc. remove additional nitrator subsequently, carry out synchronous biological nitrification and denitrification reaction at cathode chamber, obtain the nitrogen removal efficiency of 94.1%。Xie etc. then construct aerobe negative electrode MFC and Anaerobe negative electrode MFC coupled system, and the clearance of COD, ammonia nitrogen and total nitrogen is respectively reached 98.8%, 97.4% and 97.3%。Huang Xia etc. disclose a kind of Biocathode microbial fuel cell, are made up of anode chamber, aerobic cathode chamber and anoxia cathode chamber, carry out denitrogenation while organics removal and electrogenesis。A kind of microbial fuel cell wastewater treatment system improving denitrification effect is disclosed in Changping etc., inoculate nitrifying sludge to cathode chamber and add embedding aerobic denitrifying bacteria granule, make Nitrification and denitrification work in coordination with a reaction zone to play a role, make full use of DO and the residue carbon source of negative electrode, reach denitrogenation and remove COD purpose further。
But, utilize denitrifying microorganism fuel cell to carry out denitrogenation of waste water, prior art still suffers from many difficult points。Wherein, electrode denitrification and non-electrode denitrification competitiveness in cathode chamber system are main contradiction。Existing research shows, in biological denitrification process, nitrate nitrogen carries out denitrification process using preferentially utilizing organic carbon source (rather than electrodic electron) as electron donor。That is, the organic carbon source of higher concentration is inhibited to electrode denitrification。At cathode chamber, when two kinds of electron donors (organic carbon source and cathode electronics) coexist, non-electrode Denitrification is relatively strong, and electrode Denitrification is more weak, by low for the electricity generation ability making battery, and waste organic carbon source；But then, if not adding organic carbon source, only relying on electrode Denitrification, denitrifying speed is very low again, affects nitric efficiency。This contradiction makes the application prospect of denitrifying microorganism fuel cell receive query。
Summary of the invention
Goal of the invention: it is an object of the invention to build novel combination type biological fuel cell and adopt rational method to realize the denitrifying function of its high-performance bio, overcome the deficiencies in the prior art simultaneously, the contradiction of electrode denitrification and non-electrode two processes of denitrification in cathode chamber in solution prior art, make device efficient electrogenesis, denitrogenation basis on, electron donor can be made full use of, save the consumption of denitrification organic carbon source。
1. an interactive mode three Room biological fuel cell device, including: grading electrode room (5), both sides cathode chamber (1), external circuit and resistance (10), Interactive control switch (11), described grading electrode room (6) includes electrode chamber, intake-outlet, adding mouth, interior inoculation anaerobic sludge, control anaerobic state, and place the anode (6) of carbon felt material；
It is characterized in that:
Described cathode chamber (1), is included into outlet (4), (3), adding mouth (9), and interior inoculation is through the anoxic sludge of domestication, and placement surface is amassed as 28cm2Carbon felt material as negative electrode (2)；
Described both sides cathode chamber (1), including two (1A, the 1B) of specular, volume is 350cm2, separated with anode chamber by the PEM (7) of diameter 20cm respectively；
Anode and two negative electrodes (2A, 2B) are respectively connected with by described external circuit and resistance (10), and external resistance is fixed as 800 ohm, three electrode chambers constitute the biological fuel cell of two specular；
Described Interactive control switchs (11) and is connected with anode (6), and for controlling the negative electrode selecting to be connected with anode, alternately with two negative electrodes composition Guan Bi circuit, and anode is always maintained at the state of operation。
2. the method being applied to denitrogenation of waste water based on above-mentioned interactive three Room biological fuel cell devices, comprises the steps:
Step one: anode chamber (5) are inoculated anaerobic sludge, two cathode chambers (1) all inoculate the anoxic denitrification mud through domestication；
Step 2: alternately enter the both sides cathode chamber (1A of this three Room biological fuel cell with needing the wastewater by sequencing batch formula containing nitrate nitrogen to be processed, 1B), first A side negative electrode (2A) disconnects with anode, A side cathode chamber (1A) intakes, and carries out utilizing the non-electrode denitrification of organic carbon source；
Step 3: after 24h, B side negative electrode (2B) disconnects with anode, B side cathode chamber (1B) intakes, carry out utilizing the non-electrode denitrification of organic carbon source, now, A side cathode chamber (1A) organic carbon approach exhaustion, Interactive control on-off control anode connects with A side negative electrode (2A), A side cathode chamber carries out utilizing the electrode denitrification of cathode electronics, and produces electric energy simultaneously；
Step 4: again after 24h, B side cathode chamber (1B) enters low-carbon-source state, and Interactive control on-off control anode connects with B side negative electrode (2B), B side cathode chamber carries out electrode denitrification, and produce electric energy simultaneously, and the cathode chamber draining of A side, and enter new waste water；
Step 5: repeat the above steps two, three, four, two cathode chamber alternately water inlets, draining, alternately it is in " low-carbon-source " state and " high carbon source " state (during organic carbon source approach exhaustion needed for wherein side cathode chamber denitrification, i.e. so-called entrance " low-carbon-source " state) and coordinate Interactive control switch (11), control anode (6) to be connected with the negative electrode of " low-carbon-source " all the time, make two battery alternate runs, namely, when A side negative electrode (2A) off state enters " low-carbon-source " state (now still having nitrate nitrogen not to be removed in sewage) after carrying out non-electrode denitrification, switch (11) by Interactive control to be connected with A side negative electrode (2A), carry out water outlet after electrode denitrification further, meanwhile, B side cathode chamber (1B) is then in open-circuit condition, organic carbon source is utilized to carry out non-electrode denitrification。
Beneficial effect:
Traditional is applied in denitrifying biological fuel cell, Competition due to two kinds of electron donors (organic carbon source and cathode electronics exist) simultaneously, in cathode chamber, the organic carbon source of higher concentration can suppress electrode denitrification process, and causes system electricity generation ability, acquisition capability to electric energy to reduce；And if rely on merely electrode Denitrification, its reaction rate is slower。
The present invention passes through the sewage water treatment method of the improvement of the structure to microbiological fuel cell and space-time alternative, electrode denitrification process is remained at carry out under " low-carbon-source " state, weaken the competitiveness of two electron-like donors, from space-time, efficiently solve the contradiction between electrode denitrification and non-electrode denitrification。Making system while ensureing high electricity generation ability and efficient denitrification effect, make full use of electron donor, the consumption of organic carbon source needed for saving denitrification, sludge yield is low。Apparatus of the present invention average output power within a reaction time is 27.0mW/cm2, comprehensive denitrification rate 2.62mg/ (L h), the consumed organic carbon source COD/NO of denitrification3 -Less than 4, performance is better than common dual chamber denitrifying microorganism fuel cell comprehensively, and increase under little premise (accompanying drawing) in manufacturing cost, the sewage treating efficiency (water yield) being doubled, it is a kind of based on energy-saving and cost-reducing Novel sewage treatment method, suitable in the process of the nitrate nitrogen waste water of organic carbon source deficiency, there are good environmental benefit and economic benefit。
Accompanying drawing explanation
Fig. 1 is the structure chart of interactive three chamber microbiological fuel cells of the present invention。In figure:
1, cathode chamber two Room 1A and the 1B of symmetry (have), 2, negative electrode, 3, cathode chamber outlet, 4, cathode chamber water inlet, 5, anode chamber, 6, anode, 7, PEM, 8, guidewire port, 9, negative electrode adding mouth, 10, external circuit and resistance, 11, Interactive control switch
Detailed description of the invention
A kind of interactive three Room biological fuel cell devices, including: grading electrode room (5), both sides cathode chamber (1), external circuit and resistance (10), Interactive control switch (11)。
Described grading electrode room (5) includes electrode chamber, intake-outlet, adding mouth, interior inoculation anaerobic sludge, controls anaerobic state, and places the anode (6) of carbon felt material；
Described cathode chamber (1), is included into outlet (4), (3), adding mouth (9), and interior inoculation is through the anoxic sludge of domestication, and placement surface is amassed as 28cm2Carbon felt material as negative electrode (2)；
Described both sides cathode chamber (1), including two (1A, the 1B) of specular, volume is 350cm2, separated with anode chamber by the PEM (7) of diameter 20cm respectively；
Anode and two negative electrodes are respectively connected with by described external circuit and resistance (10), and external resistance is fixed as 800 ohm, three electrode chambers constitute the biological fuel cell of two specular；
Described Interactive control switch (11) is connected with anode (6), for controlling the negative electrode selecting to be connected with anode, alternately with two negative electrode (2A, 2B) composition Guan Bi circuit。
Case study on implementation 1:
Above-mentioned interactive three Room biological fuel cell devices are utilized to carry out testing containing nitrate nitrogen denitrogenation of waste water。
Step one: anode chamber (5) are inoculated anaerobic sludge, anodic dissolution adds NaAc (COD is 1000mg/L) as electron donor, two cathode chambers (1) inoculation anoxic denitrification mud, receive (COD concentration is 200mg/L) and NaNO containing acetic acid in negative electrode water inlet (simulated wastewater)3(NO3N is 70mg/L), it is possible to additionally incorporate the Na of 2g/L2CO3As the inorganic carbon source that the growth of negative electrode denitrifying bacterium is required；
Step 2: alternately enter the both sides cathode chamber (1A of this three Room biological fuel cell catholyte batch-type, 1B), first A side negative electrode (2A) disconnects with anode, and A side cathode chamber (1A) intakes, and carries out utilizing the non-electrode denitrification of organic carbon source；
Step 3: after 24h, B side negative electrode (2B) and anode disconnect B side cathode chamber (1B) water inlet, carry out utilizing the non-electrode denitrification of organic carbon source, now, namely A side cathode chamber organic carbon approach exhaustion (now enters low-carbon-source state), Interactive control on-off control anode connects with A side negative electrode (2A), and A side cathode chamber carries out utilizing the electrode denitrification of cathode electronics, and produces electric energy simultaneously；
Step 4: again after 24h, B side cathode chamber (1B) organic carbon source approach exhaustion, interactive controlling on-off control anode connects with B side negative electrode, B side cathode chamber carries out electrode denitrification, and produce electric energy simultaneously, and the cathode chamber draining of A side, and enter new waste water；
Step 5: repeat the above steps two, three and four, two cathode chamber alternately water inlets, draining, alternately it is in " low-carbon-source " state and " high carbon source " state, and coordinate Interactive control switch (13), control anode (6) to be connected with the negative electrode of " low-carbon-source " all the time, make A, two battery alternate runs of B, namely, when A side negative electrode (2A) off state enters " low-carbon-source " state (now still having nitrate nitrogen not to be removed in sewage) after carrying out non-electrode denitrification 24h, switch (11) by Interactive control to be connected with A side negative electrode (2A), carry out water outlet after electrode denitrification further, meanwhile, B side cathode chamber (1B) is then in open-circuit condition, organic carbon source is utilized to carry out non-electrode denitrification。
With A side negative electrode for investigating object (B side is identical), experimental result following (two processes):
(1) the non-electrode denitrification process in A side (now, B lateral electrode denitrification) process: disconnect anode and A side negative electrode, after reacting 24 hours, negative electrode NO3-N35.5mg/L, COD31.2mg/L, this process denitrification rate is 4.11mg/ (L h), and for non-electrode denitrification, now A side battery does not produce electric energy。
(2) A lateral electrode denitrification process (now, the non-electrode denitrification process in B side): connection anode and A side negative electrode, continues reaction 24 hours, negative electrode NO3-N26.0mg/L, COD28.2mg/L, this process denitrification rate is 0.56mg/ (L h), is mainly electrode denitrification (COD consumes relatively low, and non-electrode denitrification is less)。Now, A battery produces electric energy, average voltage 246mV in 24h, average output power 27.0mW/cm2。
Total process: comprehensive denitrification rate 2.62mg/ (L h) of the total process of A battery, the consumed organic carbon source COD/NO of denitrification3 -Ratio is 3.9, produces electric energy 6.54W, the overall total process electrogenesis energy 13.08W of this device。
Case study on implementation 2:
Using traditional dual chamber denitrification biological fuel cell, other experiment conditions are with embodiment 1, but yin, yang electrode connects all the time, as the comparison with case 1。After reaction 48h, negative electrode water outlet NO3-N28.7mg/L, now COD22.4mg/L, now, average voltage 203.1mV in 48h, average output power 18.4mW/cm2。Comprehensive denitrification rate 2.46mg/ (L h), the consumed organic carbon source COD/NO of denitrification3 -Ratio is 4.3, produces electric energy 4.46W。The property indices such as organic carbon source consumption are below apparatus of the present invention (case 1), and the process water yield also reduces half。
Case study on implementation 3:
Other operating condition, with embodiment 1, does not use Interactive control to switch for this three Room battery so that two batteries simultaneously switch off and Guan Bi, compare with embodiment 1。Divide two processes:
(1) A, B side carries out non-electrode denitrification process simultaneously: disconnect anode and two negative electrodes, after reacting 24 hours, and negative electrode NO3-N35.5mg/L, COD31.2mg/L, this process denitrification rate is 4.11mg/ (L h) (result is with process 1 in case study on implementation 1), now A, B battery all not electrogenesis energy。
(2) A, B side carries out electrode denitrification process simultaneously: connection anode and two negative electrodes, after continuing reaction 24 hours, and single-sided cathodes NO3-N32.9mg/L, COD30.4mg/L, this process denitrification rate is 0.15mg/ (L h), now unilateral battery (on average) electrogenesis energy 2.86W, altogether 5.72W。
Connect two negative electrodes due to Sole anode simultaneously, electric current density dispersion (and unstable) causes that two lateral electrode denitrification rates all reduce, the i.e. method of operation of three Room battery Simultaneous Switchings, from the denitrifying speed of electrode and electricity generation ability, all not as the method for operation of Interactive control on-off control。
Case study on implementation 4:
Other operating condition is with embodiment 1, and the change alternate run time is 12h, 24h, 36h, 48h etc., compares the impact of alt time。
In experiment, when negative electrode COD is lower than 30mg/L, non-electrode denitrification rate is substantially reduced, about to 0.08mg/ (L h), even below electrode denitrification rate 0.1-0.6mg/ (L h)。And (COD concentration is about 200mg/L) and NaNO receive for water inlet acetic acid3(NO3-N is about 70mg/L), in this experiment condition, when process I reacts 24h, just COD is down to about 30mg/L。Non-electrode denitrification overlong time, causes that as 36h, COD are too low non-electrode denitrification rate is very low；Time is too short, and remaining a large amount of organic carbon source affects speed and the production capacity of electrode denitrification process。Therefore, for this flow condition, time optimal control point is 24h。
If the condition such as influent COD, nitrate nitrogen changes, then can pass through adjusting reaction time, find the interaction time control point of optimum to be optimized operation。
Claims (2)
1. an interactive mode three Room biological fuel cell device, including: grading electrode room (5), both sides cathode chamber (1), external circuit and resistance (10), Interactive control switch (11), described grading electrode room (5) includes electrode chamber, intake-outlet, adding mouth, interior inoculation anaerobic sludge, control anaerobic state, and place the anode (6) of carbon felt material；
It is characterized in that:
Described cathode chamber (1), is included into outlet (4), (3), adding mouth (9), and interior inoculation is through the anoxic sludge of domestication, and placement surface is amassed as 28cm2Carbon felt material as negative electrode (2)；
Described both sides cathode chamber (1), including two (1A, 1B) rooms of specular, volume is 350cm2, separated with anode chamber by the PEM (7) of diameter 20cm respectively；
Anode and two negative electrodes (2A, 2B) are respectively connected with by described external circuit and resistance (10), and external resistance is fixed as 800 ohm, three electrode chambers constitute the biological fuel cell of two specular；
Described Interactive control switch (11) is connected with anode (6), and alternately controls Guan Bi and the disconnection of anode and two negative electrodes。
2. the method being applied to denitrogenation of waste water based on the interactive mode three Room biological fuel cell device described in claim 1, comprises the steps:
Step one: anode chamber (5) are inoculated anaerobic sludge, two cathode chambers (1A and 1B) all inoculate the anoxic denitrification mud through domestication；
It is characterized in that also comprising the steps:
Step 2: alternately enter the both sides cathode chamber (1A of this three Room biological fuel cell with needing the wastewater by sequencing batch formula containing nitrate nitrogen to be processed, 1B), first A side negative electrode (2A) disconnects with anode, A side cathode chamber (1A) intakes, and carries out utilizing the non-electrode denitrification of organic carbon source；
Step 3: after 24h, B side negative electrode (2B) disconnects with anode, B side cathode chamber (1B) intakes, carry out utilizing the non-electrode denitrification of organic carbon source, now, A side cathode chamber (1A) organic carbon approach exhaustion, Interactive control on-off control anode connects with A side negative electrode, A side cathode chamber carries out utilizing the electrode denitrification of cathode electronics, and produces electric energy simultaneously；
Step 4: again after 24h, B side cathode chamber (1B) organic carbon approach exhaustion, Interactive control on-off control anode connects with B side negative electrode, B side cathode chamber carries out electrode denitrification, and produce electric energy simultaneously, and the cathode chamber draining of A side, and enter new waste water；
Step 5: repeat the above steps two, three and four, two cathode chamber alternately water inlets, drainings, and coordinate Interactive control switch (11), control anode (6) and be connected with the negative electrode of " organic carbon source approach exhaustion " all the time so that two battery alternate runs。
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| CN105948223B (en) * | 2016-06-30 | 2019-10-15 | 河海大学 | A kind of microbial fuel cell unit of three battery system and its application |
| CN107311294B (en) * | 2017-08-23 | 2020-06-02 | 哈尔滨工业大学 | Device and method for simultaneously treating park sludge and electroplating wastewater in electroplating industrial park |
| CN108195901B (en) * | 2017-12-19 | 2020-05-05 | 清华大学 | Method for early warning of nitrate in water body |
| CN108178328B (en) * | 2017-12-26 | 2021-05-07 | 太原理工大学 | Biological cathode electrochemical system for treating sewage with low C/N ratio and method for treating sewage by using biological cathode electrochemical system |
| CN109160618B (en) * | 2018-10-16 | 2021-08-17 | 中国石油化工股份有限公司 | Bioelectrochemical reactor for quickly deoxidizing oil field wastewater |
| CN111115816A (en) * | 2020-01-06 | 2020-05-08 | 广东电科院能源技术有限责任公司 | Bioelectrochemical device and method for treating organic pollutants containing azobenzene |
| CN111146484B (en) * | 2020-01-21 | 2021-06-25 | 河海大学 | Microbial fuel cell and method for promoting wastewater denitrification of microbial fuel cell |
| CN113387430A (en) * | 2021-07-12 | 2021-09-14 | 国润(广东)生物科技有限公司 | Device and method for treating organic wastewater by using continuous energy supply of microbial fuel cell |
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