CN111320259B - Micro-aerobic granular sludge and bioelectrode coupling coking wastewater enhanced treatment method and treatment device - Google Patents
Micro-aerobic granular sludge and bioelectrode coupling coking wastewater enhanced treatment method and treatment device Download PDFInfo
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Abstract
The invention relates to a method and a device for strengthening treatment of coking wastewater by coupling micro-aerobic granular sludge and a biological electrode. By relying on the microenvironment advantages of high-activity and high-concentration micro-aerobic granular sludge in the two-stage micro-aerobic granular sludge reactor, the advantages of enriched microbial flora, the advantages of interspecies enhanced mass transfer and the advantages of muddy water enhanced mass transfer, the synchronous and efficient removal of COD, ammonia nitrogen, TN, phenols, thiocyanide, cyanide and the like in the coking wastewater is realized; the removal of the difficultly degraded COD and the accumulated ammonia nitrogen, nitrate and sulfate in the system is further enhanced by means of a three-pair bioelectrode coupling system, so that the high-efficiency and low-consumption treatment and recycling of the coking wastewater are realized.
Description
Technical Field
The invention relates to the technical field of environmental protection, in particular to a method for strengthening treatment of coking wastewater by coupling micro-aerobic granular sludge and a bioelectrode and a treatment device suitable for the treatment method.
Background
The wastewater treatment in the coking industry not only needs to consider the problem that the treated wastewater reaches the integrated wastewater discharge standard, but also relates to the problem that the wastewater cannot be discharged after being recycled. Coking wastewater contains a great amount of intractable toxic pollutants such as phenols, nitrogen-containing heterocyclic substances, polycyclic aromatic hydrocarbon substances, sulfate, thiocyanide, cyanide and the like, and the substances are discharged into the environment if not treated properly, thereby seriously threatening the water body safety and public health.
The treatment of the coking wastewater is a worldwide problem. A adopted in the present biological treatment of coking wastewater2In the process, A1、A2Both the O-stage and the O-stage can be considered to employ activated sludge systems, biofilm systems, or a combination of both. Although the process can remove pollutants in the coking wastewater to a certain degree, the COD of the effluent is difficult to drop after the COD is reduced to a certain degree, and the effluent is difficult to reach the national discharge standard. Most importantly, however, these residual COD's contain significant amounts of toxic, carcinogenic substances such as naphthalenes, polycyclic aromatics, SCN, etc. That is to say, COD standard discharge becomes a major difficulty of breakthrough in the coking wastewater treatment at present, and a new process must be considered and developed to further solve the problem of removing the pollutants in the coking wastewater.
If the subsequent recycling is considered, the problem of difficultly degraded COD, the problem of nitrate accumulation caused by ammonia nitrogen (the TN removal rate is difficult to improve), and the problem of high sulfate content (causing corrosion and perforation of the equipment pipeline and further influencing the recycling) are all needed to be mainly solved.
The advanced treatment process is generally considered to solve the problems in the industry at present. Common advanced treatment processes comprise a coagulating sedimentation method, an adsorption method, an advanced oxidation method, a membrane separation method and the like, but the treatment effect of a single method cannot meet the requirement, and each method has the problem of higher treatment cost. The combined process has the problems of complex flow, high operating cost, secondary pollution and the like.
Aiming at the current situation that the coking wastewater adopts a complex treatment process flow (physicochemical pretreatment (deslagging, oil removal, dephenolization, ammonia distillation) + biological treatment + post-coagulation precipitation process) and can only meet the basic standard discharge, and the discharged coking wastewater can still generate adverse effect on a water body, a solution can not simply consider to continuously increase subsequent treatment units, especially increase some treatment units (membrane process, advanced oxidation method and the like) with high investment and operation cost, and thus the whole process flow is inevitably more and more complex.
An effective method is to consider the optimization of a main stream treatment process, namely a biological treatment unit, and finally solve the problem of coking wastewater treatment by relying on a simpler, energy-saving and efficient process flow. Therefore, the coking wastewater recycling process and equipment which are simple in process flow, energy-saving, environment-friendly and efficient are researched and developed necessarily aiming at the characteristics that the coking wastewater is large in water quantity and complex in components, contains high-concentration ammonia nitrogen and a plurality of nonbiodegradable organic matters, and has large harm to the environment due to some toxic and harmful pollutants (including corrosive sulfate).
Disclosure of Invention
The invention aims to provide a method for strengthening treatment of micro-aerobic granular sludge and bioelectrode coupled coking wastewater so as to finally realize high-efficiency and low-consumption treatment and recycling of the coking wastewater.
The invention provides a treatment device suitable for the micro-aerobic granular sludge and bioelectrode coupling coking wastewater enhanced treatment method, which is another object of the invention.
The invention provides a method for strengthening treatment of micro-aerobic granular sludge and bioelectrode coupling coking wastewater.
a. Two reactors are respectively used as a first-stage reactor and a second-stage reactor, granular sludge is filled in the two reactors, and a micro-aerobic expanded granular sludge bed is formed by means of effluent circulation under the micro-aerobic condition; respectively arranging a first biological anode and a second biological anode at different heights in the primary reactor; and a biological cathode which is also attached with microorganisms is arranged in the secondary reactor along the central shaft, and an annular third biological anode which is coaxial with the biological cathode is arranged close to the inner wall of the secondary reactor.
The biological cathode in the secondary reactor forms two pairs of chambered biological electrodes with the first biological anode and the second biological anode in the primary reactor respectively, and forms a pair of same-chamber biological electrodes with the third biological anode in the secondary reactor.
b. The coking wastewater enters the primary reactor from the bottom of the primary reactor, pollutants in the coking wastewater are degraded through the biodegradation of the micro-aerobic expanded granular sludge bed and the bioelectrochemical coupling of the two pairs of chambered bioelectrode, and the obtained primary treated water is discharged from the top.
c. One part of the formed primary treatment water enters a primary aeration reflux column, and after aeration, the primary treatment water flows back into the primary reactor from the bottom of the primary reactor, and the other part of the primary treatment water enters the secondary reactor from the bottom of the secondary reactor.
d. And (3) the water enters a primary treatment water in a secondary reactor, wherein the residual pollutants are degraded again through the biological degradation effect of the micro-aerobic expanded granular sludge bed and the bioelectrochemical coupling effect of the two pairs of chambered bioelectrode and the same chamber bioelectrode, and the obtained secondary treatment water is discharged from the top.
e. And part of the formed secondary treatment water enters a secondary aeration reflux column, is aerated and then flows back into the secondary reactor from the bottom of the secondary reactor, and part of the formed secondary treatment water returns to the primary reactor from the bottom of the primary reactor, and part of the formed secondary treatment water is directly discharged.
In unit time, the volume of the directly discharged secondary treatment water is the same as that of the coking wastewater entering the primary reactor; the volume of primary treatment water entering the secondary reactor is equal to the sum of the volume of coking wastewater entering the primary reactor and the volume of secondary treatment water returning to the primary reactor.
The above process is carried out continuously.
In the method for strengthening the treatment of the coking wastewater, the primary reactor and the secondary reactor are used for treating the wastewater in a micro-aerobic state all the time, and the method for keeping the micro-aerobic state in the reactors is used for supplying oxygen to the reflux water entering the reactors in a proper amount in an aeration mode.
Furthermore, the invention controls the aeration quantity in the first-stage aeration reflux column and the second-stage aeration reflux column by monitoring the oxidation-reduction potential in the first-stage reactor and the second-stage reactor so as to realize the supply of oxygen to the respective reactors in a proper amount.
Specifically, the oxidation-reduction potential in the first-stage reactor is controlled to be-30 to 90mV, and the oxidation-reduction potential in the second-stage reactor is controlled to be-15 to 150mV by properly adjusting the aeration quantity.
In the three pairs of bioelectrodes, the bioelectrode degrades pollutants through the electricity-generating microorganisms and transmits the generated electrons to the cathode through the anode, and the cathode is responsible for receiving the electrons and transmitting the electrons to the electron acceptor, so that pollutants are degraded, and meanwhile, the microorganisms attached to the cathode can further enhance the electron receiving and transmitting and further enhance the removal of the pollutants.
The invention gradually realizes the conversion from 'easily degradable COD as an anode electron donor' to 'ammonia nitrogen as an anode electron donor' from the lower part to the upper part of the reactor by arranging the biological anodes at different heights in the primary reactor and respectively forming the chambered biological electrode with the biological cathode in the secondary reactor. Then, a pair of inner and outer coaxial lantern rings arranged in the middle of the secondary reactor are used as the co-chamber bioelectrode with outer anode and inner cathode, so that the nondegradable COD is used as the electron donor of the anode.
Specifically, in the bioelectrode of the present invention, the height positions and the anode surface areas of the two bioanodes in the primary reactor can be adjusted according to the pollutant removal effect; furthermore, the relative areas of the two bioanode in the first stage reactor and the biocathode in the second stage reactor and the relative areas of the bioanode and the biocathode in the second stage reactor can be adjusted according to the pollutant removal effect.
Aiming at the defects that the traditional coking wastewater biochemical and advanced treatment process has complex flow and high energy consumption and does not meet the low-carbon economic requirement, the invention provides the integrated process for coupling the micro-aerobic granular sludge and the bioelectrode, which has simple process, compact structure, low operation cost and good treatment effect and can synchronously and efficiently treat high-concentration ammonia nitrogen, sulfate and various toxic and non-degradable harmful pollutants in the coking wastewater.
The coking wastewater enhanced treatment method adopts a two-stage muddy water high-efficiency mass transfer reactor configuration, and utilizes a combined system formed by chamber coupling and same-chamber coupling of the micro-aerobic granular sludge and the biological electrode to efficiently treat coking wastewater. On one hand, the synchronous and efficient removal of COD, ammonia nitrogen, TN, phenols, thiocyanide, cyanide and the like in the coking wastewater is realized by relying on the microenvironment advantage, the enriched microbial flora advantage, the interspecies enhanced mass transfer advantage and the muddy water enhanced mass transfer advantage of high-activity and high-concentration micro-aerobic granular sludge in the two-stage micro-aerobic granular sludge reactor; on the other hand, the removal of the difficultly degraded COD and the accumulated ammonia nitrogen, nitrate and sulfate in the system is further enhanced by depending on a three-pair bioelectrode coupling system, so that the high-efficiency and low-consumption treatment and recycling of the coking wastewater are finally realized.
Furthermore, the present invention utilizes two-stage reactors to form ∙ L of 40-50 g-1The concentration of the high-activity granular sludge, the high-efficiency mass transfer (including substances and electrons) in the granular sludge which is a special microbial polymer, countless anaerobic-anoxic-aerobic coexisting microenvironments formed under the micro-aerobic condition, and the effective coupling of biological treatment and bioelectrochemistry can be realized, so that the coking wastewater can be efficiently treated at the normal temperature of 22-26 ℃. Although the temperature of the reactor can be further increased to about 30 ℃, the conventional medium-temperature operation condition of about 35 ℃ is not required to be maintained, and the energy consumption can be greatly reduced.
Furthermore, the invention also provides a device for strengthening treatment of the micro-aerobic granular sludge and biological electrode coupled coking wastewater, which is suitable for the strengthening treatment method of the micro-aerobic granular sludge and biological electrode coupled coking wastewater and is formed by connecting the following treatment units.
a. The bottom of the first-stage reactor is provided with a water distribution device connected with a water inlet pipe of the first-stage reactor; the inner wall of the middle upper part of the reactor is provided with a lug which divides the reactor into a reaction zone and a precipitation zone; the reaction zone is filled with granular sludge, and a sludge bed formed by the granular sludge is in an expansion state under the micro-aerobic condition and under the action of liquid ascending flow velocity; respectively arranging a first biological anode and a second biological anode at different heights in the reaction zone; the three-phase separation device is arranged in a settling zone at the upper part of the reactor and is used for separating gas, liquid and solid in the reactor together with the lugs; a water outlet tank is arranged at the upper part of the settling zone, and a water outlet pipe of the primary reactor is connected with the bottom of the water outlet tank; the primary treated water produced by the primary reactor flows from the sedimentation zone to the effluent tank through the effluent weir on the effluent tank and is discharged out of the primary reactor.
b. The primary aeration reflux column is internally provided with an aeration head, the inlet of the primary aeration reflux column is connected with a primary reactor water outlet pipe, and the outlet of the primary aeration reflux column is connected with a primary reactor water inlet pipe, and is used for supplying oxygen to the primary treatment water flowing into the aeration device appropriately and then refluxing to the primary reactor.
c. The bottom of the secondary reactor is communicated with a water outlet pipe of the primary reactor through a water inlet pipe of the secondary reactor connected with the water distribution device and used for introducing primary treated water into the secondary reactor; the inner wall of the middle upper part of the secondary reactor is provided with a lug to divide the reactor into a reaction zone and a precipitation zone; the reaction zone is filled with granular sludge, and a sludge bed formed by the granular sludge is in an expansion state under the micro-aerobic condition and under the action of liquid ascending flow velocity; a biological cathode is arranged in the middle of the reaction zone along a central shaft, and a third biological anode which is arranged close to the inner wall of the secondary reactor and is coaxial with the biological cathode in a lantern ring manner is arranged; the three-phase separation device is arranged in a settling zone at the upper part of the reactor and is used for separating gas, liquid and solid in the reactor together with the lugs; a water outlet tank is arranged at the upper part of the settling zone, and a water outlet pipe of the secondary reactor is connected with the bottom of the water outlet tank; and the secondary treated water generated by the secondary reactor flows from the sedimentation zone to the water outlet groove through the water outlet weir on the water outlet groove and is discharged out of the secondary reactor.
d. The second-stage aeration reflux column is internally provided with an aeration head, the inlet of the second-stage aeration reflux column is connected with the water outlet pipe of the second-stage reactor, and the outlet of the second-stage aeration reflux column is connected with the water inlet pipe of the second-stage reactor, and is used for supplying oxygen to the second-stage treated water flowing into the aeration device properly and then refluxing to the second-stage reactor.
e. And the return pipe is connected between the water outlet pipe of the secondary reactor and the water inlet pipe of the primary reactor and is used for returning part of secondary treated water into the primary reactor.
Furthermore, the device for strengthening treatment of coking wastewater by coupling micro-aerobic granular sludge and a biological electrode can also comprise a wastewater storage tank for storing the coking wastewater, wherein a water outlet of the wastewater storage tank is connected with a water inlet pipe of a primary reactor on the primary reactor and is used for introducing the coking wastewater into the primary reactor.
The gas collecting pipe is connected above the two three-phase separation devices and is used for collecting gas generated in the coking wastewater treatment process.
The upper parts of the first-stage aeration reflux column and the second-stage aeration reflux column are provided with air release pipes for discharging redundant air in the aeration process.
Furthermore, in the processing apparatus of the present invention, the first bioanode and the second bioanode disposed in the first-stage reactor are both graphite brushes, wherein the first bioanode is disposed at the lower portion of the reactor, and the second bioanode is disposed above the first bioanode.
The third biological anode in the secondary reactor is a stainless steel woven mesh arranged in the middle of the reactor and wrapped on the inner wall of the reactor, and the biological cathode is a stainless steel bar arranged at the central axis position in the middle of the reactor.
Conventionally, a water pump is arranged on each connecting pipeline for connecting the processing unit with the processing device, and the water pump is used for driving water to flow, and a valve is arranged for controlling and adjusting water flow in the pipeline.
The invention adopts the method and the device for strengthening treatment of the coking wastewater by coupling the micro-aerobic granular sludge and the double biological electrodes, and successfully realizes the same-chamber and chamber-divided double coupling of a biological 'double-catalysis' electrolysis system and a micro-aerobic granular sludge biological system. By means of a micro-aerobic granular sludge biological system, the high-efficiency removal of COD, ammonia nitrogen, phenols, thiocyanide and cyanide in the coking wastewater is synchronously realized; the removal of COD, ammonia nitrogen, phenols, thiocyanide and cyanide in the coking wastewater is further enhanced by virtue of the capability of a biological 'double-catalysis' electrolysis system for more rapidly releasing electrons, transferring electrons and receiving electrons, and the chambered coupling and the same-chamber coupling of the biological electrolysis system and a micro-aerobic biological system.
More importantly, the method strengthens the synchronous and efficient removal of the difficultly degraded COD, the accumulated nitrite and the sulfate in the coking wastewater. Further realizes the omnibearing high-efficiency treatment of micro-energy consumption (micro-oxygen aeration and external micro-voltage) coking wastewater, including high-concentration ammonia nitrogen, high-concentration nondegradable pollutants, toxic and harmful pollutants, accumulated nitrate, accumulated corrosive sulfate and the like.
The invention solves the problems of complex process flow, high investment and operating cost of an advanced treatment unit and influence on subsequent recycling by corrosive high sulfate in the traditional coking wastewater treatment process, and has the characteristics of simple process flow, compact integral system structure, small occupied area, high system treatment efficiency, low energy consumption and accordance with low-carbon economic requirements.
One of the characteristics of the invention is that the 'multiple coupling' is realized by relying on a two-stage micro-aerobic granular sludge reactor, and the synchronous removal of COD, ammonia nitrogen, phenols, thiocyanide and cyanide in the coking wastewater is enhanced.
As is known to all, the coking wastewater has complex water quality and contains a large amount of toxic pollutants, and the treatment of the coking wastewater needs to pay attention not only to the problem of deamination but also to the problem of denitrification. Traditional coking wastewater treatment A2/O, A/O or A2/O2The process, even if the A or O section is strengthened by adopting the biological membrane, the COD and ammonia nitrogen of the effluent are still difficult to reach the discharge standard. There is a need to pay more attention to the structural optimization and microbiological optimization of the reactor. The invention enhances the removal of various pollutants in the coking wastewater by means of multiple coupling. Coupling one: the micro-oxygen is coupled with the granular sludge. The micro-aerobic condition can form aerobic-micro-aerobic-anaerobic conditions on the surface and at different depths of the granular sludge by means of the structure of the granular sludge, and further can form countless aerobic-micro-aerobic conditions in the granular sludge reactorAn anaerobic microenvironment, and synchronous and efficient removal of various pollutants in the coking wastewater is realized. Coupling two: coupling of high-concentration sludge and high-richness microbial flora. The advantages of the reactor configuration of the invention ensure high sludge concentration in the reactor on one hand, ensure compact structures of different metabolic populations and high activity of various microbial floras in granular sludge on the other hand, and promote high-abundance microbial floras in the granular sludge microstructure further under the condition of micro-oxygen, thereby strengthening the removal of various pollutants in coking wastewater by means of the coupling of the high-concentration sludge and the high-abundance microbial floras. Coupling three: coupling of inter-species electron transfer and inter-species mass transfer. The granular sludge with a compact structure ensures the efficient inter-species electron transfer among various microbial floras and the timely transfer of inter-species metabolites, thereby ensuring the efficient performance of various microbial reactions and strengthening the removal of various pollutants in the coking wastewater.
The invention is characterized in that the removal of nitrate is enhanced by coupling in multiple ways so as to solve the problem of nitrate accumulation in the secondary reactor.
Nitrate accumulation is a direct factor that the removal rate of TN in the biological treatment of the coking wastewater is difficult to improve. The final material carrier for biological removal of nitrate is N2However, an electron donor is necessary to accomplish this material conversion. In the traditional denitrification, an organic carbon source is used as an electron donor, but for coking wastewater, nitrate is accumulated in a secondary bioreactor under the condition of extreme shortage of the organic carbon source, so that the normal denitrification cannot be ensured under the condition, and finally, the TN removal rate of a two-stage biological treatment system is difficult to improve. The method solves the problem of nitrate accumulation by coupling multiple modes such as reflux denitrification (without adding an organic carbon source), anaerobic ammonia oxidation, bioelectrode nitrate reduction and the like, and further improves the TN removal rate. The first coupling mode: and (3) no organic carbon source is added, the effluent containing high nitrate in the secondary reactor flows back to the primary reactor, and high-efficiency denitrification is completed by utilizing high-concentration easily-degradable COD in the primary reactor. A second coupling mode: the ammonia nitrogen and the nitrate are simultaneously obtained in the two-stage reactor through anaerobic ammonia oxidation without consuming an organic carbon sourceHigh-efficiency removal. A third coupling mode: the nitrate reduction is realized by accepting electrons transmitted to a biological cathode by a biological anode in a secondary reactor without consuming an organic carbon source (the anode electron source can depend on organic pollutants on the one hand, and more importantly on ammonia nitrogen on the other hand, namely the invention more importantly realizes the effective electron transmission of the ammonia nitrogen to the nitrate by a biological double electrode!).
The invention is characterized in that the sulfate removal is enhanced by multi-mode coupling so as to solve the problem of sulfate accumulation in the secondary reactor.
The coking wastewater contains a large amount of sulfate and a large amount of sulfate is generated in the process of degrading the thiocyanide. The problem of high-concentration sulfate accumulation cannot be solved in the traditional biological treatment process of the coking wastewater, and the discharge of the high-concentration sulfate not only influences the water safety, but also influences the recycling of the coking wastewater due to the corrosivity of the high-concentration sulfate. On one hand, the high-sulfate effluent of the secondary reactor flows back to the primary reactor, the sulfate is reduced and degraded by high-concentration easily-degradable COD in the primary reactor, on the other hand, the sulfate is reduced in the secondary reactor by receiving electrons transmitted to a biological cathode by a biological anode, and more importantly, the high-efficiency reduction of the sulfate is realized by the biological enhancement effect of the biological cathode. Meanwhile, compared with nitrate, sulfate is in the disadvantage of competing for organic carbon sources in reduction in a primary reactor, so that for sulfate reduction, the reduction is completed by obtaining electrons transmitted to a biological cathode by a biological anode (the electrons can be supported by organic matters as well as ammonia nitrogen and other substances) and by the biological enhancement of sulfate reducing bacteria of the biological cathode.
The invention is characterized in that enrichment of cathode sulfate reducing bacteria is used for enhancing the reception of electron reduction of sulfate supported cathode, thereby avoiding competition of organic matters with methane bacteria.
The sulfate removal rate of the traditional biological treatment system for the coking wastewater is low mainly because the biodegradability of the coking wastewater is low, and the organic matters capable of being used for reducing nitrate or sulfate are few, and compared with sulfate, nitrate is easier to obtain the organic matters for reduction. For this reason, when a large amount of nitrate is accumulated in the biological treatment system for coking wastewater, it is difficult to achieve high removal of sulfate. Furthermore, when the problem of nitrate accumulation in the system is solved, the sulfate reducing bacteria compete with methanogens for organic matters, but due to the existence of the granular sludge, the advantage conditions of methanogens depending on the internal environment of the granular sludge are ensured (meanwhile, the sulfate reducing bacteria are not easy to attach to the surface of the granular sludge and are easy to lose). But because the range of the substrate used by the sulfate reducing bacteria is wide, the sulfate reducing bacteria can be kept to be complementary and coexist with methanogens under certain conditions. The invention further relies on a biocatalytic electrolysis system, and relies on the transfer of biologically enhanced electrons from the anode to the cathode and then to the sulfate reducing bacteria, thereby ensuring the efficient removal of sulfate without competing with methanogenic bacteria for electrons (organic matter).
The method is characterized in that the removal of the nondegradable COD in the coking wastewater is enhanced by coupling micro-aerobic digestion and biological electrolysis.
Firstly, the embedding of a biological electrolysis system can enrich the microbial flora of the original micro-aerobic digestion system and strengthen the treatment of the refractory toxic pollutants; secondly, the removal of the difficultly degraded COD is further enhanced by relying on the strong capability of degrading toxic difficultly degraded pollutants of the anode electrogenesis flora and combining with a rapid interspecies electron transfer channel formed by methanogens in the micro-aerobic digestion system.
The invention is characterized in that the enhanced removal of the difficultly degraded COD in the coking wastewater is realized by depending on the chambered coupling and the same-chamber coupling of the biological anode and the biological cathode.
The biodegradability of the coking wastewater is relatively low, and the invention fully utilizes the coupling of the biological anode and the biological cathode to strengthen the removal of the nondegradable COD in the coking wastewater on the basis of the unique mechanical and kinetic advantages of the micro-aerobic granular sludge on the conversion of various matrixes (ensuring the high activity of various microbial flora and the strong degradability on pollutants, especially on some toxic nondegradable pollutants).
The most core of the biological anode is an attached electrogenesis flora, the flora is a group of bacteria with an extracellular electron transfer function, the bacteria rely on the anode, not only have very strong capacity of degrading organic pollutants, but also can directly reduce high-molecular complex organic matters into low-molecular organic matters to strengthen the degradation effect of the hardly degradable toxic pollutants, and can timely transfer electrons to a cathode by relying on the efficient electron transfer capacity of the anode to further strengthen the removal effect of the hardly degradable toxic pollutants. The most core of the biological cathode is the microbial flora based on an electron acceptor in the secondary reactor, and the dominant flora in the system is nitrate reducing bacteria and sulfate reducing bacteria. The electron transfer and receiving utilization efficiency of the cathode position is enhanced by the dominant bacteria, and then the removal of pollutants is enhanced. Therefore, the invention realizes the reinforced removal of the difficultly degraded COD in the secondary reactor by depending on the chamber coupling of the biological anode in the primary reactor and the biological cathode in the secondary reactor and the same-chamber coupling of the biological anode and the biological cathode in the secondary reactor.
The invention is characterized in that the inner and outer coaxial lantern rings of the biological anode and the biological cathode in the secondary reactor are arranged.
For bioelectrode systems, the bioanode is a rate limiting electrode, for which increasing the relative surface area of the anode is critical. The invention adopts a structure that the biological anode and the biological cathode are coaxially arranged in the secondary reactor by the inner lantern ring and the outer lantern ring, the cathode is arranged inside, the anode is arranged outside, the area advantage of the anode and the distance advantage between the two electrodes can be simultaneously ensured, and the removal of the difficultly degraded COD in the secondary reactor is enhanced.
Drawings
FIG. 1 is a schematic structural diagram of a device for strengthening treatment of wastewater from coupled coking of micro-aerobic granular sludge and a bioelectrode.
Detailed Description
The following examples further describe embodiments of the present invention. The following examples are only for illustrating the technical solutions of the present invention more clearly, and do not limit the scope of the present invention. Various changes, modifications, substitutions and alterations to these embodiments will be apparent to those skilled in the art without departing from the principles and spirit of this invention.
Example 1.
The structure of the micro-aerobic granular sludge and bioelectrode coupling coking wastewater strengthening treatment device is shown in figure 1 and comprises a wastewater storage tank 1, a primary reactor 5, a primary aeration reflux column 11, a secondary reactor 17 and a secondary aeration reflux column 24.
The wastewater storage tank 1 is used for storing coking wastewater, and the water outlet of the wastewater storage tank is connected with a primary reactor water inlet pipe 3 on a primary reactor 5 through a valve 27 and a primary reactor water inlet pump 2 and is used for introducing the coking wastewater into the primary reactor 5.
The primary reactor 5 and the secondary reactor 17 both comprise a reaction zone and a precipitation zone, wherein the volume ratio of the reaction zone to the precipitation zone is 2:1, and the inner diameter ratio is 0.7: 1; the height-diameter ratio of the reaction zone is 17: 1; the height-diameter ratio of the precipitation zone was 4.5: 1. Micro-oxygen granular sludge for degrading pollutants in the coking wastewater is filled in the reaction zones of the primary reactor 5 and the secondary reactor 17.
The bottoms of the primary reactor 5 and the secondary reactor 17 are respectively provided with a water distribution device 4, and the lower parts of the two water distribution devices 4 are respectively connected with a primary reactor water inlet pipe 3 and a secondary reactor water inlet pipe 16; the upper part is provided with a lug 7 and a three-phase separation device 8 respectively. Wherein the lug 7 is arranged between the reaction zone and the precipitation zone, and the three-phase separation device 8 is arranged in the precipitation zone and is used for carrying out gas-liquid-solid separation in the reactor. And a gas collecting pipe 14 is also connected above the two three-phase separation devices 8 and is used for collecting gas generated in the coking wastewater treatment process. The upper parts of the settling zones of the primary reactor 5 and the secondary reactor 17 are respectively provided with a water outlet groove 22 of a water outlet weir 28, and a water outlet pipe 29 of the primary reactor and a water outlet pipe 21 of the secondary reactor are respectively connected with the bottom of the water outlet groove 22 of the respective reactors and are respectively used for discharging primary treatment water and secondary treatment water.
The lower part and the upper part of the reaction zone of the first-stage reactor 5 are respectively provided with a first biological anode 6 and a second biological anode 9 which are respectively connected with an external power supply 20 and respectively form two pairs of chambered biological electrodes with biological cathodes 18 in the second-stage reactor for carrying out bioelectrochemical action between the two reactors.
The bottom of the secondary reactor 17 is provided with a secondary reactor inlet pipe 16 which is connected with a primary reactor outlet pipe 29 at the bottom of a primary reactor settling zone water outlet tank, and the secondary reactor inlet pipe enters the bottom of the secondary reactor through a valve 27 and a secondary reactor inlet pump 15 and is used for conveying primary treatment water to the bottom of the secondary reactor. A pair of same-chamber biological electrodes are coaxially sleeved inside and outside the middle position of the reaction zone of the secondary reactor 17, wherein the outer ring close to the inner wall of the secondary reactor is a third biological anode 19, and a biological cathode 18 is arranged at the position of the inner central axis and is respectively connected with an external power supply 20 for carrying out bioelectrochemical action in the secondary reactor.
Aeration heads 12 are respectively arranged in the first-stage aeration reflux column 11 and the second-stage aeration reflux column 24 and are used for appropriately supplying oxygen to the wastewater in the aeration device; the two aeration reflux columns are provided with air release pipes 10 with valves 27.
The inlet of the first-stage aeration reflux column 11 is connected with a first-stage reactor water outlet pipe 29, the outlet of the first-stage aeration reflux column is connected with a first-stage reactor water inlet pipe 3, part of first-stage treated water is conveyed to the first-stage aeration reflux column 11 through a valve 27, and after the first-stage treated water is completely conveyed to the bottom of the first-stage reactor 5 through the first-stage reactor water inlet pipe 3 by a first-stage reactor reflux pump 13 and is used for providing dissolved oxygen for the first-stage reactor.
The inlet of the secondary aeration reflux column 24 is connected with a secondary reactor water outlet pipe 21, the outlet is connected with a secondary reactor water inlet pipe 16, part of secondary treated water is conveyed to the secondary aeration reflux column 24 through a valve 27, and after the secondary treated water is completely conveyed to the bottom of the secondary reactor 17 through a secondary reactor reflux pump 25 and the secondary reactor water inlet pipe 16, the secondary treated water which is properly aerated flows back to the bottom of the secondary reactor 17 for providing dissolved oxygen for the secondary reactor.
A return pipe 23 from the secondary reactor to the primary reactor is also arranged between the water outlet pipe 21 of the secondary reactor and the bottom of the primary reactor 5, and part of secondary treatment water flows back to the bottom of the primary reactor 5 through a return pump 26 from the secondary reactor to the primary reactor through a valve 27.
The coking wastewater entering the first-stage reactor 5 is degraded by the biodegradation of the micro-aerobic expanded granular sludge bed and the bioelectrochemical coupling of the two pairs of chamber-separated biological electrodes to obtain first-stage treated water. The micro-aerobic granular sludge, the primary treated water and the gas generated in the treatment process are separated by a bump 7 positioned at the upper part of the reactor and a three-phase separator device 8. Wherein the gas is collected or directly discharged through the gas collecting pipe 14, the micro-aerobic granular sludge is returned to the primary reactor 5 after being thoroughly separated from the primary treated water, the primary treated water is divided into two parts, one part enters the primary aeration reflux column 11, after being properly aerated, the primary treated water returns to the primary reactor from the bottom of the primary reactor 5 through the water distribution device, and the other part directly enters the secondary reactor 17.
The primary treated water entering the primary aeration reflux column 11 is fully aerated and then refluxed into the primary reactor 5 through a primary reactor reflux pump 13.
The primary treated water entering the secondary reactor 17 is degraded again to obtain secondary treated water through the biodegradation of the micro-aerobic expanded granular sludge bed and the bioelectrochemical coupling action of the two pairs of chambered bioelectrodes and the same pair of chambered bioelectrodes. After micro-oxygen granular sludge, secondary treatment water and gas generated in the treatment process are separated by a bump 7 and a three-phase separation device 8 which are positioned at the upper part of the reactor, the micro-oxygen granular sludge returns to a secondary reactor 17, the gas is collected by a gas collecting pipe 14 or directly discharged, the secondary treatment water is divided into three parts, one part is directly discharged, the other part enters a secondary aeration reflux column 24, after proper aeration, the part returns to the secondary reactor from the bottom of the secondary reactor 17 through a water distribution device, the other part is used as reflux water of the secondary reactor to a primary reactor, and the reflux water directly flows back to the primary reactor 5 from a water inlet pipe 3 of the primary reactor through a reflux pipe 23 by a reflux pump 26.
The second-stage treated water entering the second-stage aeration reflux column 24 is fully aerated and then refluxed into the second-stage reactor 17 through the second-stage reactor water inlet pipe 16 by the second-stage reactor reflux pump 25.
The above process is carried out continuously.
The whole operation process of the micro-aerobic granular sludge and biological electrode coupled coking wastewater enhanced treatment device can consider two stages of starting and stable operation. Wherein the starting stage is mainly the domestication culture of anode electrogenesis functional bacteria, cathode electrogenesis functional bacteria and micro-aerobic granular sludge in the two-stage reactor. In the actual operation process, the domestication culture of the anode electrogenesis function flora and the cathode electrogenesis function flora can be considered by adopting a culture medium, and after the domestication culture, the electrodes attached with the electrogenesis function flora and the cathode electrogenesis function flora are inserted into the reactor to stably operate. And the micro-aerobic granular sludge reactor directly operating the two-stage coupling electrode can also be considered to directly treat the coking wastewater to culture the electricity generating functional flora and the electricity receiving functional flora. The anode culture medium adopts some easily degradable low-carbon substances, such as sodium acetate; the cathode culture medium needs to be considered to ensure the sulfate concentration close to that of a bioreactor for treating the coking wastewater in actual operation; the micro-aerobic granular sludge can be taken from a granular sludge reactor which is used for treating coking wastewater and stably operates.
Example 2.
Taking coking wastewater of a regulating reservoir of a certain coking plant in Taiyuan as water to be treated, wherein COD and NH of the coking wastewater3-N, volatile phenol, cyanide and SCN-The concentration is 1120-2940 mg.L respectively-1、32～258mg·L-1、253～624mg·L-1、0.08～4.36mg·L-1152 to 404 mg.L of a sum-1The pH value is between 8.31 and 9.13.
The granular sludge is taken from a granular sludge reactor for treating coking wastewater, and the granular sludge reactor is filled with a primary reactor and a secondary reactor.
Coking wastewater enters the aerobic granular sludge and biological electrode coupling coking wastewater strengthening treatment device (at the moment, the electrode is in the state of external domestication culture of electrogenesis functional flora and electrogenesis functional flora, wherein, the anode culture medium adopts sodium acetate for domestication, the cathode culture medium adopts sulfate for domestication, the primary reactor and the secondary reactor are in the state of pure aerobic granular sludge, wherein, the aeration rate of the reflux column of the primary reactor is 10000mL min-1The aeration rate of the reflux column of the secondary reactor is 8000 mL/min-1) Stable operation at 22-26 deg.C, HRT 12.0h, COD, ammonia nitrogenThe removal rates of phenols, SCN, CN and nitrate are 69.1-76.5%, 76.2-88.4%, 82-87.4%, 81.8-91.1%, 87.9-92.0% and 83.6-89.2%, and the accumulation of sulfate reaches 54.5%.
After 2 microbial electrodes which are domesticated and attached with anode functional bacteria are inserted into a primary reactor (functional bacteria are not attached to a cathode in a secondary reactor), the operation effect of the reactor is not obviously changed, the ammonia nitrogen removal rate is slowly increased after the reactor operates for 10 days, the COD removal rate is also slowly increased after the reactor operates for 20 days, and the accumulation of sulfate begins to slowly decrease. On the 28 th day, the removal rates of COD and ammonia nitrogen are respectively increased to 72.7-79.6%, and the accumulation of sulfate is reduced to 7.5%.
Inserting a microbial anode attached with anode functional bacteria into a secondary reactor, replacing the original cathode of the secondary reactor with a biological cathode attached with cathode functional bacteria, acclimatizing and adapting for 10 days, further improving the COD removal rate, positively removing sulfate, and then gradually improving, so that the micro-aerobic granular sludge and biological electrode coupling coking wastewater enhanced treatment device can always run efficiently and stably, and the removal rates of COD, ammonia nitrogen, phenols, SCN, CN, nitrate and sulfate are respectively 84.5-92.8%, 89.8-100%, 97.6-99.7%, 94.7-100%, 87.6-96.9% and 45.6-62.7%.
Example 3.
Taking coking wastewater of a regulating reservoir of a certain coking plant in Taiyuan as water to be treated, wherein COD and NH of the coking wastewater3-N, volatile phenol, cyanide and SCN-The concentration of (A) is 1120-2940 mg.L-1、32～258mg·L-1、253～624mg·L-1、0.08～4.36mg·L-1152 to 404 mg.L of a sum-1The pH value is between 8.31 and 9.13.
The granular sludge is taken from a granular sludge reactor for treating coking wastewater, and the granular sludge reactor is filled with a primary reactor and a secondary reactor.
The coking wastewater to be treated enters the aerobic granular sludge and biological electrode coupling coking wastewater strengthening treatment device (the electrodes are in the states of external domestication culture of electricity generating functional flora and electricity receiving functional flora and are not arranged in the electrodesIn the excess sludge treatment reactor, taking water from the primary reactor, acclimating and culturing two anodes of the primary reactor; water taken from the secondary reactor is required to be domesticated and cultured by a pair of electrodes arranged in the secondary reactor. The primary reactor and the secondary reactor are both in a pure micro-aerobic granular sludge state, wherein the aeration rates of the reflux columns of the primary reactor and the secondary reactor are both 10000 mL-min-1) The method is characterized in that the method stably operates at the operating temperature of 29-31 ℃ for HRT 12h, then the domesticated microbial electrodes attached with the anode electrogenesis functional flora and the cathode electrogenesis functional flora are respectively inserted into a first-stage reactor and a second-stage reactor, stable and efficient operation is realized after a rapid adaptation period of 10-15 days, and the removal rates of COD, ammonia nitrogen, phenols, SCN, CN, nitrate and sulfate are respectively 85.3% -91.8%, 89.8% -98.7%, 98.7% -100%, 96.6% -99.8%, 96.7% -100%, 88.6% -95.9% and 48.6% -68.7%.
Example 4.
Coking wastewater which is treated by ammonia distillation and oil removal by a certain coking company in Taiyuan City is taken as water to be treated, and COD and NH of the coking wastewater3-N, volatile phenol, cyanide and SCN-The concentration of (a) is 548-1927 mg.L respectively-1、37～103mg·L-1、5.37～352.5mg·L-1、0.1～5.93mg·L-1And 205.5 to 539.9 mg.L-1The pH value is between 8.86 and 9.71.
The granular sludge is taken from a granular sludge reactor for treating coking wastewater, and the granular sludge reactor is filled with a primary reactor and a secondary reactor. The coking wastewater to be treated enters the aerobic granular sludge and bioelectrode coupling coking wastewater strengthening treatment device (the electrodes are directly arranged in the two-stage reactor, the aeration rate of the reflux column of the two-stage reactor is 10000 mL/min-1) When the device operates in an environment at 29-31 ℃ and HRT is 12h, the removal rates of COD, ammonia nitrogen, phenols, SCN, CN, nitrate and sulfate are gradually increased from 65.1-72.5%, 74.2-85.4%, 84.6-89.4%, 82.8-89.1%, 86.4-91.2%, 84.6-90.2% and (-7.5%) -1.7% to 84.8-90.2%, 89.8-98.7%, 98.9-99.8%, 97.6-99.5%, 98.7-100%, 89.6-96.5% and 52.4-68.7%, and the device stably and efficiently operates.
Claims (9)
1. A method for strengthening treatment of micro-aerobic granular sludge and biological electrode coupled coking wastewater,
a. two reactors are respectively used as a first-stage reactor and a second-stage reactor, granular sludge is filled in the two reactors, and a micro-aerobic expanded granular sludge bed is formed by means of effluent circulation under the micro-aerobic condition; respectively arranging a first biological anode and a second biological anode at different heights in the primary reactor; arranging a biological cathode which is also attached with microorganisms in the secondary reactor along a central shaft, and arranging an annular third biological anode which is coaxial with the biological cathode and is close to the inner wall of the secondary reactor;
wherein, the biological cathode in the secondary reactor forms two pairs of chambered biological electrodes with the first biological anode and the second biological anode in the primary reactor respectively, and forms a pair of same-chamber biological electrodes with the third biological anode in the secondary reactor;
b. the coking wastewater enters a primary reactor from the bottom of the primary reactor, pollutants in the coking wastewater are degraded through the biodegradation effect of a micro-aerobic expanded granular sludge bed and the bioelectrochemical coupling effect of two pairs of chambered bioelectrodes, and the obtained primary treated water is discharged from the top;
c. one part of the formed primary treatment water enters a primary aeration reflux column, is aerated and then flows back into the primary reactor from the bottom of the primary reactor, and the other part of the formed primary treatment water enters the secondary reactor from the bottom of the secondary reactor;
d. the residual pollutants are degraded again through the biological degradation of the micro-aerobic expanded granular sludge bed and the bioelectrochemical coupling action of the two pairs of chambered bioelectrodes and the same chamber bioelectrode, and the obtained secondary treated water is discharged from the top;
e. part of the formed secondary treatment water enters a secondary aeration reflux column, after aeration, the secondary treatment water flows back into a secondary reactor from the bottom of the secondary reactor, and part of the formed secondary treatment water returns to enter a primary reactor from the bottom of the primary reactor, and part of the formed secondary treatment water is directly discharged;
in unit time, the volume of the directly discharged secondary treatment water is the same as that of the coking wastewater entering the primary reactor; the volume of the primary treatment water entering the secondary reactor is equal to the sum of the volume of the coking wastewater entering the primary reactor and the volume of the secondary treatment water returning to the primary reactor;
the above process is carried out continuously.
2. The method for strengthening treatment of coking wastewater according to claim 1, wherein the amount of aeration in the primary and secondary aerated reflux columns is controlled by monitoring the oxidation-reduction potential in the primary and secondary reactors, so as to supply a suitable amount of oxygen to the respective reactors.
3. The method of claim 2, wherein the oxidation-reduction potential in the primary reactor is controlled to be-30 to 90mV, and the oxidation-reduction potential in the secondary reactor is controlled to be-15 to 150 mV.
4. The device for strengthening treatment of the micro-aerobic granular sludge and the biological electrode coupled coking wastewater, which is used for the strengthening treatment method of the micro-aerobic granular sludge and the biological electrode coupled coking wastewater of claim 1, is formed by connecting the following treatment units:
a. the bottom of the first-stage reactor is provided with a water distribution device connected with a water inlet pipe of the first-stage reactor; the inner wall of the middle upper part of the reactor is provided with a lug which divides the reactor into a reaction zone and a precipitation zone; the reaction zone is filled with granular sludge, and a sludge bed formed by the granular sludge is in an expansion state under the micro-aerobic condition and under the action of liquid ascending flow velocity; respectively arranging a first biological anode and a second biological anode at different heights in the reaction zone; the three-phase separation device is arranged in a settling zone at the upper part of the reactor and is used for separating gas, liquid and solid in the reactor together with the lugs; a water outlet tank is arranged at the upper part of the settling zone, and a water outlet pipe of the primary reactor is connected with the bottom of the water outlet tank; the primary treatment water generated by the primary reactor flows from the sedimentation zone to the effluent tank through the effluent weir on the effluent tank and is discharged out of the primary reactor;
b. the primary aeration reflux column is internally provided with an aeration head, the inlet of the primary aeration reflux column is connected with the water outlet pipe of the primary reactor, and the outlet of the primary aeration reflux column is connected with the water inlet pipe of the primary reactor, and the primary aeration reflux column is used for supplying oxygen to the primary treated water flowing into the aeration device properly and then refluxing the primary treated water into the primary reactor;
c. the bottom of the secondary reactor is communicated with a water outlet pipe of the primary reactor through a water inlet pipe of the secondary reactor connected with the water distribution device and used for introducing primary treated water into the secondary reactor; the inner wall of the middle upper part of the secondary reactor is provided with a lug to divide the reactor into a reaction zone and a precipitation zone; the reaction zone is filled with granular sludge, and a sludge bed formed by the granular sludge is in an expansion state under the micro-aerobic condition and under the action of liquid ascending flow velocity; a biological cathode is arranged in the middle of the reaction zone along a central shaft, and a third biological anode which is arranged close to the inner wall of the secondary reactor and is coaxial with the biological cathode in a lantern ring manner is arranged; the three-phase separation device is arranged in a settling zone at the upper part of the reactor and is used for separating gas, liquid and solid in the reactor together with the lugs; a water outlet tank is arranged at the upper part of the settling zone, and a water outlet pipe of the secondary reactor is connected with the bottom of the water outlet tank; the secondary treated water generated by the secondary reactor flows from the sedimentation zone to the water outlet groove through the water outlet weir on the water outlet groove and is discharged out of the secondary reactor;
d. the secondary aeration reflux column is internally provided with an aeration head, the inlet of the secondary aeration reflux column is connected with the water outlet pipe of the secondary reactor, and the outlet of the secondary aeration reflux column is connected with the water inlet pipe of the secondary reactor and is used for supplying oxygen to the secondary treated water flowing into the aeration device properly and then refluxing the secondary treated water into the secondary reactor;
e. and the return pipe is connected between the water outlet pipe of the secondary reactor and the water inlet pipe of the primary reactor and is used for returning part of secondary treated water into the primary reactor.
5. The coking wastewater enhanced treatment device as recited in claim 4, further comprising a wastewater storage tank for storing coking wastewater, wherein a water outlet of the wastewater storage tank is connected with a water inlet pipe of the primary reactor on the primary reactor for introducing coking wastewater into the primary reactor.
6. The coking wastewater enhanced treatment device according to claim 4, characterized in that a gas collecting pipe is connected above the two three-phase separation devices and is used for collecting gas generated in the coking wastewater treatment process.
7. The coking wastewater enhanced treatment device according to claim 4, characterized in that the upper parts of the primary aeration reflux column and the secondary aeration reflux column are provided with gas release pipes for discharging excessive gas in the aeration process.
8. The coking wastewater enhanced treatment device of claim 4, wherein the first biological anode and the second biological anode are graphite brushes, wherein the first biological anode is arranged at the lower part of the reactor, and the second biological anode is positioned above the first biological anode.
9. The coking wastewater strengthening treatment device of claim 4, wherein the third biological anode is a stainless steel mesh grid arranged in the middle of the reactor and wrapped on the inner wall of the reactor, and the biological cathode is a stainless steel bar arranged at the central axis of the middle of the reactor.
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