EP2595925A2 - Dénitrification et contrôle du ph à l'aide de systèmes bio-électrochimiques - Google Patents

Dénitrification et contrôle du ph à l'aide de systèmes bio-électrochimiques

Info

Publication number
EP2595925A2
EP2595925A2 EP11810413.2A EP11810413A EP2595925A2 EP 2595925 A2 EP2595925 A2 EP 2595925A2 EP 11810413 A EP11810413 A EP 11810413A EP 2595925 A2 EP2595925 A2 EP 2595925A2
Authority
EP
European Patent Office
Prior art keywords
bio
electrochemical system
stream
cathode
chamber
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Withdrawn
Application number
EP11810413.2A
Other languages
German (de)
English (en)
Other versions
EP2595925A4 (fr
Inventor
Matthew Silver
Justin Buck
Patrick Kiely
Juan J. Guzman
Zhen Huang
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Cambrian Innovation LLC
Original Assignee
Cambrian Innovation LLC
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by Cambrian Innovation LLC filed Critical Cambrian Innovation LLC
Publication of EP2595925A2 publication Critical patent/EP2595925A2/fr
Publication of EP2595925A4 publication Critical patent/EP2595925A4/fr
Withdrawn legal-status Critical Current

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Classifications

    • 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
    • A—HUMAN NECESSITIES
    • A01—AGRICULTURE; FORESTRY; ANIMAL HUSBANDRY; HUNTING; TRAPPING; FISHING
    • A01K—ANIMAL HUSBANDRY; CARE OF BIRDS, FISHES, INSECTS; FISHING; REARING OR BREEDING ANIMALS, NOT OTHERWISE PROVIDED FOR; NEW BREEDS OF ANIMALS
    • A01K63/00—Receptacles for live fish, e.g. aquaria; Terraria
    • A01K63/04—Arrangements for treating water specially adapted to receptacles for live fish
    • 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
    • C02F3/30—Aerobic and anaerobic processes
    • C02F3/302—Nitrification and denitrification treatment
    • C—CHEMISTRY; METALLURGY
    • C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F1/00—Treatment of water, waste water, or sewage
    • C02F1/38—Treatment of water, waste water, or sewage by centrifugal separation
    • C02F1/385—Treatment of water, waste water, or sewage by centrifugal separation by centrifuging suspensions
    • C—CHEMISTRY; METALLURGY
    • C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F1/00—Treatment of water, waste water, or sewage
    • C02F2001/007—Processes including a sedimentation step
    • C—CHEMISTRY; METALLURGY
    • C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F1/00—Treatment of water, waste water, or sewage
    • C02F1/46—Treatment of water, waste water, or sewage by electrochemical methods
    • C02F1/461—Treatment of water, waste water, or sewage by electrochemical methods by electrolysis
    • C02F1/46104—Devices therefor; Their operating or servicing
    • C02F1/46109—Electrodes
    • C02F2001/46133—Electrodes characterised by the material
    • C—CHEMISTRY; METALLURGY
    • C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F1/00—Treatment of water, waste water, or sewage
    • C02F1/46—Treatment of water, waste water, or sewage by electrochemical methods
    • C02F1/461—Treatment of water, waste water, or sewage by electrochemical methods by electrolysis
    • C02F1/46104—Devices therefor; Their operating or servicing
    • C02F1/46109—Electrodes
    • C02F2001/46133—Electrodes characterised by the material
    • C02F2001/46138—Electrodes comprising a substrate and a coating
    • 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
    • C02F2201/00—Apparatus for treatment of water, waste water or sewage
    • C02F2201/46—Apparatus for electrochemical processes
    • C02F2201/461—Electrolysis apparatus
    • C02F2201/46105—Details relating to the electrolytic devices
    • C02F2201/46115—Electrolytic cell with membranes or diaphragms
    • C—CHEMISTRY; METALLURGY
    • C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F2209/00—Controlling or monitoring parameters in water treatment
    • C02F2209/22—O2
    • C—CHEMISTRY; METALLURGY
    • C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F2301/00—General aspects of water treatment
    • C02F2301/08—Multistage treatments, e.g. repetition of the same process step under different conditions

Definitions

  • the invention relates to methods and devices for the treatment of nitrogenous waste components and reduced organic compounds in wastewater from industrial water treatment facilities.
  • the present invention includes reactor design, component designs, and operating schemes for removing nitrates and reduced organic compounds from any suitable wastewater stream.
  • the invention also describes reactor designs, component designs, and operating schemes designed to modify and improve pH and water quality in wastewater streams.
  • nitrogen in its various forms is an increasingly important objective in wastewater treatment.
  • nitrogen can caused algal blooms in oceans, pollute lakes and rivers, and pollute drink wells and reservoirs.
  • Two areas where nitrogen is particularly difficult to address involves public and private treatment works, and anaerobic digestion fish farming (aquaculture).
  • Nitrogen can be a problem in integrated treatment works, particularly where biogas is produced. Because much of the carbon is removed from wastewater in the form of carbon dioxide and methane, the bulk solution can develop high levels of ammonia and low
  • C:N carbon/nitrogen
  • Ammonia can be nitrified using aeration, but this then requires addition of a carbon source (such as methanol) to remove the remaining nitates if C:N ratios are low.
  • a carbon source such as methanol
  • C:N ratios carbon/nitrogen ratios
  • RAS re-circulating aquaculture systems
  • economical and efficient wastewater treatment is a critical bottleneck to the sustainable growth of the RAS and semi-RAS industry in the U.S. and worldwide.
  • RAS, and other such closed-loop systems produce high concentrations of dissolved nitrogenous waste components and reduced organic compounds, which in turn stress the chemical oxygen demand (COD) and biological oxygen demand (BOD) in the system.
  • COD chemical oxygen demand
  • BOD biological oxygen demand
  • nitrates can affect fish in re-circulating systems. In flow-through systems they can result in high fees charged to the operator, depending on the region. In Europe, nitrates are highly regulated with active monitoring in discharge waters and in the United States there is anticipation of increased enforcement of the 10 mg/L regulation imposed by the
  • Nitrates can be removed via water exchange, but this must often be as high as 10 - 20% of the system volume per day. As regulations become stricter, the release of nitrates at end of pipe will likely be treated with increasing stringency. Nitrates can be removed via anaerobic
  • sludge organic matter from the same facility can be used in the place of methanol in up- flow anaerobic sludge blanket reactors (UASB).
  • UASB up- flow anaerobic sludge blanket reactors
  • the sludge is often in particulate form.
  • hydrolysis and fermentation must be applied to convert the sludge into volatile fatty acids and other molecules more easily consumed by denitrifying organisms, adding complexity and cost to the operation.
  • EOP treatment is another particularly important kind of treatment common to RAS and semi-RAS.
  • EOP treatment is defined as treatment for wastewater leaving an aquaculture facility and entering the environment.
  • Most end-of-pipe flows have common cause in the concentrated discharge from primary treatment technologies, such drum filters, belt filters, bio-filters, or settling tanks.
  • Aeration technology might be used to treat EOP wastewater.
  • this is often uneconomical at the scale of fish-farming, and it is exceedingly energy intensive. It also results in a solids stream which must also be managed.
  • Some new systems have been developed - for example, a Geotube ® system is available which can treat BOD, nitrogen and nitrates (Tencate).
  • the GeoTube ® uses a high cationic polymer to precipitate end-of-pipe streams. At large scale, this polymer becomes expensive and risks harming fish if wash-back occurs.
  • EOP treatment is particularly important for the future of the aquaculture industry because current advances in treatment systems continue to create concentrated streams that must be dealt with economically. As concerns over our nations water quality grows, the economic needs of the industry will be increasingly at odds with societal needs for unpolluted waterways.
  • the present invention provides improved bio-electrochemical systems and methods for removing nitrates and reduced organic compounds from wastewater streams such as those produced by industrial water treatment facilities.
  • the present invention provides improved reactor designs, component designs, and operating schemes for removing nitrates and reduced organic compounds from any suitable wastewater stream.
  • the invention also describes reactor designs, component designs, and operating schemes designed to modify and improve pH and water quality in wastewater streams.
  • the bio-electrochemical system for treating wastewater include at least one reaction module comprising two electrode chambers of the same polarization and one electrode chamber of a different polarization, each of the electrode chambers being arranged succession in substantial proximity to the other.
  • the bio-electrochemical system can include a cathode chamber housing a cathode and two anode chambers, each housing an anode, with the cathode chamber being sandwiched between the two anode chambers.
  • the bio- electrochemical system can include an anode chamber housing an anode and two cathode chambers, each housing a cathode, with the anode chamber being sandwiched between the two cathode chambers.
  • Each of the electrode chambers can be arranged in vertical succession (e.g., stacked), or in horizontal succession (e.g., side by side).
  • the electrode chambers are coupled together via external circuitry.
  • two or more of the electrode chambers in the reaction module are electrically connected in series.
  • two or more of the electrode chambers in the reaction module can be electrically connected in parallel.
  • One or more of the electrode chambers can include at least one electrogenic microbe in proximity to the electrode housed within.
  • the bio-electrochemical system of the invention includes comprises a plurality of reaction modules, each reaction module including two electrode chambers of the same polarization and one electrode chamber of a different polarization.
  • the plurality of reaction modules are preferably arranged in succession in substantial proximity to the other.
  • the plurality of reaction modules can be arranged in vertical succession (e.g., stacked) or in horizontal succession (e.g., side by side).
  • one or more of the plurality of reaction modules are configured to be removable/interchangeable from the bio- electrochemical system.
  • the reaction module(s) can be of any length or width. In a particular embodiment, the reaction module has a substantially flat configuration/shape.
  • a selectively permeable membrane can be disposed between the electrode chambers within one or more of the reaction modules.
  • the selectively permeable membrane can be a proton exchange membrane, or an ion (e.g., cation, anion) exchange membrane.
  • the selectively permeable membrane is adapted to be removable/interchangeable from the system.
  • the electrodes housed with the electrode chambers can be made of one or more materials including but not limited to carbon cloth, carbon mesh, a solid support coated on at least one side with a conductive material, activated carbon, graphite granules, charcoal, biochar and stainless steel.
  • the electrodes of the same polarization and different polarization can each be made of the same material or different material.
  • the bio-electrochemical system of the invention can include two anodes, each comprised of carbon cloth, and a cathode comprised of graphite granules.
  • at least one of the electrodes (e.g., a cathode) comprises a combination of graphite or carbon-based material, and stainless steel.
  • one or more of the electrodes are made of a solid support (e.g., plastic) coated on at least one side with a conductive material, such as carbon paint or carbon epoxy.
  • the bio-electrochemical systems of the invention can further include at least one pre- treatment tank coupled to the bio-electrochemical system for pre-treating the wastewater.
  • the bio-electrochemical the system includes a plurality of reaction modules
  • at least one common pre-treatment tank can be coupled to all electrodes of the same polarization within the plurality of reaction modules and a separate treatment tank coupled to all the electrodes of a different polarization within the plurality of reaction modules.
  • a splitting manifold can be used to split the pre-treated wastewater stream from the pre-treatment tank into the respective electrodes within the plurality of reaction modules.
  • a power source is coupled to the bio-electrochemical system to apply a voltage to the electrodes within the plurality of reaction modules. The same voltage can be applied across the plurality of reaction modules. Alternatively, a different voltage is selectively applied across the plurality of reaction modules.
  • the bio-electrochemical system is configured to funnel a reaction product produced at in an anode chamber (e.g., C0 2 ) into a cathode chamber.
  • one or more of the electrodes in the bio-electrochemical system of the invention are configured to operate at a poised potential.
  • At least one of the electrode chambers within the bio- electrochemical system of the invention can include an ammonia oxidizing bacteria.
  • the present invention provides a method for removing nitrogenous waste and reduced organic compounds from a wastewater source, by providing a bio- electrochemical system comprising at least one anode chamber and at least one cathode chamber, each chamber being arranged in substantial proximity to each other coupled via external circuitry; separating the wastewater source into a first stream comprising a high biological oxygen demand (e.g., a stream having a high concentration of solid organic compounds) and a second stream comprising a high chemical oxygen demand (e.g., a stream having high concentration of ammonia and nitrates); and flowing the first stream through the anode chamber and the second stream through the cathode chamber of the bio-electrochemical system.
  • a bio- electrochemical system comprising at least one anode chamber and at least one cathode chamber, each chamber being arranged in substantial proximity to each other coupled via external circuitry
  • separating the wastewater source into a first stream comprising a high biological oxygen demand (e.g., a stream having a high concentration of solid
  • Oxidation reactions in the anode chamber and reduction reactions in the cathode chamber reduce the biological oxygen demand in the first stream and the chemical oxygen demand in the second stream, thereby treating the wastewater source.
  • a device such as a mechanical filter, a settling filter, a drum or canister filter or a centrifugation-based filter can be used to separate the wastewater into the first and second streams. Once separated, the first and second streams do not mix throughout the treatment process.
  • the methods of the invention are particularly suited for recirculating or semi- recirculating industrial water treatment facilities, including but not limited to aquacultures and municipal water treatment facilities.
  • the bio-electrochemical system can be disposed externally from the wastewater source.
  • the bio-electrochemical system is at least partially disposed within the wastewater source.
  • a cathode chamber is disposed within the wastewater source.
  • a nitrifying reactor can be coupled to the bio-electrochemical system upstream of the cathode chamber, such that the second stream flows through the nitrifying reactor prior to flowing through the cathode chamber.
  • An oxygen monitor/feedback system can be coupled to the bio-electrochemical system upstream of the anode chamber such that the first stream flows through the oxygen monitor prior to flowing through the anode chamber.
  • the bio-electrochemical system includes a selectively permeable membrane disposed between the at least one anode chamber and the at least one cathode chamber.
  • the selectively permeable membrane is an ion exchange membrane such as a cation exchange membrane or an anion exchange membrane.
  • the effluent from the at least one anode chamber is re-circulated to the wastewater treatment source.
  • Figure 1 depicts a schematic of a typical semi-re-circulating aquaculture process design.
  • Figure 2 depicts a general schematic for treating biological oxygen demand of a wastewater stream at the anode and nitrates (chemical oxygen demand) at the cathode of a bio- electrochemical system.
  • Figure 3 depicts an exemplary embodiment of a bio-electrochemical system according to the invention that utilizes multiple, flat 3-electrode (e.g., anode - cathode - anode) modules.
  • multiple, flat 3-electrode e.g., anode - cathode - anode
  • Figures 4A and 4B are flow diagrams depicting the treatment of separate streams from a single wastewater.
  • Figure 5 is depicts the treatment of separate streams in an aquaculture context using an exemplary embodiment of a bio-electrochemical system according to the invention.
  • Figure 6 depicts the treatment of separate streams from an aquaculture using an exemplary embodiment of a bio-electrochemical system according to the invention.
  • Figures 7A and 7B depict exemplary configuration of a bio-electrochemical system according to the invention coupled with an anaerobic digester.
  • Figure 8 is a flow diagram of a proposed wastewater treatment system layout utilizing an exemplary embodiment of a bio-electrochemical system according to the invention.
  • Figures 9A and 9B each depict an exemplary embodiment of a bio-electrochemical system according to the invention.
  • Figure 10 is an exemplary embodiment of a removable/interchangeable reaction module for a bio-electrochemical system in accordance with the invention.
  • the present invention provides novel architecture and components for an electrogenic system for improving wastewater treatment rates and are particularly useful for industrial scale water treatment facilities, such as aquaculture systems, and municipal water treatment plants.
  • the architectures of the bio-electrochemical systems (BES) described herein enhance waste water treatment rates by leveraging newly discovered electrically active bacteria and reactor design to simultaneously denitrify culture tank water, remove end-of-pipe biological oxygen demand (EOP BOD) without crossing wastewater streams, and generate electricity.
  • the reactor can anaerobically nitrify in an anode using anaerobic ammonia oxidizing bacteria and anaerobically denitrify in a cathode using nitrate and nitrite reducing bacteria.
  • an aeraobic nitrification step is placed in a first stage cathode (e.g., a bio- air cathode) followed by an anaerobic denitrifying cathode (see e.g., FIGS 9A and 9B).
  • a first stage cathode e.g., a bio- air cathode
  • an anaerobic denitrifying cathode see e.g., FIGS 9A and 9B.
  • FIG. 1 An example of a typical semi-re-circulating aquaculture process design (semi-RAS) is depicted in FIG. 1.
  • the bio-electrochemical systems and processes described herein addresses nitrate accumulation in the main re-circulation loop of an RAS, semi-RAS or other such closed- loop system, as well as concentrated end-of-pipe BOD (e.g., sludge water).
  • BESs bio-electrochemical systems
  • BESs bio-electrochemical systems
  • Electrodes to transfer electrons to electrodes or accept electrons from electrodes while consuming organic matter. Similar to a chemical fuel cell, an oxidation reaction in the anodic chamber releases energy, electrons and ions. These migrate to the cathodic region where they are reduced to form a substance with lower free energy of formation.
  • BESs typically consist of electrodes, such as anode and cathodes, both or individually coated in biofilms with the ability to transfer or accept electrons from electrodes. Electrodes may also be coated in noble metals to catalyze one of the reactions taking place. The electrodes can be separated by an electrolyte which conveys ions between them (ion selective membrane can be included, but membrane-less systems also work). Electrodes, biofilms, electrolytes, and catalysts may or may not be enclosed in a casing. Each of these elements, which include the casing, can be connected to external circuits, control systems, or other reactors for use in combined systems. The geometrical configuration of the elements in a BES and their material definition can together be defined as the "architecture" of the system. It should be noted that the terms "bio-electrochemical system”, “microbial fuel cell”, and “reactor” are sometimes used interchangeably herein.
  • the typical BES is a two-chamber system, consisting of both anode and cathode chambers separated by a selectively permeable membrane. Modifications to applied potentials and architecture have allowed BESs to carry out a variety of tasks including hydrogen, methane, and hydrogen peroxide production, as well as water desalination and nitrogen removal.
  • BESs have been successfully operated when supplied a wide array of waste streams such as domestic, winery and potato chip. In these cases, BOD is oxidized at a biological anode with the cathode reducing a range of substrates, often 0 2 .
  • the present invention provides novel reactor designs for BESs in which the EOP water is oxidized in the anode chamber of the BES, while nitrate-rich water is reduced in the cathode chamber (see e.g., FIG. 2).
  • a circuit connecting anode and cathode captures energy.
  • the bio-electrochemical systems described herein work by providing an electrically conductive media on which certain species of microbes will attach and use the electrode as either an electron sink or electron source, depending on whether they are effecting an oxidation or reduction reaction, respectively.
  • Oxidative metabolic processes occur in the anode compartment, where electricigen microbes consume reduced organic compounds, liberating high-potential electrons that are used for their internal metabolic processes, but must ultimately be transferred to a terminal electron acceptor at a lower potential.
  • microbes A variety of electricigen microbes have been catalogued and are known to those of ordinary skill in the art, including but not limited to microbes from the Geobacter, Clostridia, Rhodeferax and E. coli families. Such microbes can be utilized in the BESs of the present invention. Alternatively, multi-strain communities of electricigen microbes naturally present in wastewater streams can serve as a source of electrigen microbes in the bio-electrochemical systems of the invention. Because the reactor volume is kept in an anaerobic or anoxic (low- oxygen) state, microbes utilize the anodic electrode surface as an electron sink. External circuitry provides these electrons with a path to the cathodic electrode, which is colonized by a separate consortium of microbes that accept these electrons for use in the reduction of low potential chemical species, in this case generally nitrate and oxygen.
  • the amount of power generated by a bio-electrochemical system is a function of the potential difference between the free energy of formation of the oxidants and reductants (in this case complex organics (acetate) and nitrate), as well as the reaction rates. Given the numerous benefits associated with the overall process, it is often more advantageous to maximize treatment rate (e.g. denitrification) rather than total power.
  • Stand-out advantages of the reactor designs and component designs describe herein include the following: (i) the use of electrons from end-of- pipe BOD to reduce nitrates, therefore unlike UASB technology there is no requirement for carbon addition (such as methanol); (ii) there is no requirement for operators to mix EOP streams with culture tank water, thus removing the need for extensive and costly pathogen removal; (iii) and decreased requirement for caustic alkalinity addition to adjust pH of denitrified culture water stream. Design of Reactor and Components
  • the bio-electrochemical systems of the invention generally include at least reaction modules housing 3-electrode chambers, where two electrode chambers of the same polarization sandwich another electrode chamber of a different polarization.
  • a BES of the invention can include a single cathode chamber with two anode chambers on opposing sides.
  • a BES of the invention can include a single anode chamber with two cathode chambers on opposing sides.
  • the electrodes can be arranged in vertical succession.
  • the electrodes are arranged in horizontal succession.
  • the electrodes can be electrically coupled/connected either in series or in parallel.
  • the bio-electrochemical systems of the invention include a plurality of reaction modules, each comprising 3 electrode chambers, where two electrode chambers of the same polarization sandwich another electrode chamber of a different polarization.
  • the plurality of reaction modules are arranged in succession in substantial proximity to each other.
  • the plurality of reaction modules can be arranged in vertical succession, or horizontal succession.
  • the plurality of reaction modules are configured to be removable/interchangeable from the BES.
  • a selectively permeable membrane is disposed between the electrodes within the one or more reaction modules.
  • a cation exchange membrane will prevent nitrates from moving across.
  • an anion exchange membrane may be useful for shuttling nitrates into the anode chamber, thus enabling preferential concentration and removal of nitrates into the COD laden anode stream in addition to cathodic nitrate reduction.
  • the selectively permeable membrane can be permanently integrated with the system or removable/interchangeable.
  • the membrane is in the form of an interchangeable cassette that can be removed from the system for cleaning, and/or swapped out for a different type of membrane, depending on the desired application of the BES system.
  • the membrane cassette can itself be sandwiched by conductive wire mesh that serves to both support the membrane and act as an electrode.
  • the length and width of the chambers is constant for all test cells, and can be any suitable length and width ranging from several centimeters of tens of centimeters in width, and a length of several meters per module.
  • each chamber can have a width ranging from 1-1000 cm, 1-500 cm, 1-250 cm, 1-100, 1-90 cm, 1-80 cm, 1-70 cm, 1-60 cm, 1-50, 1-40 cm, 1-30 cm, 1-20 cm, 1-10 cm, or any specific value in between these ranges; and length ranging from 1-10 m, 1-5 m, 1-3 m or any specific value within these ranges (e.g., 2 m).
  • the chamber thickness and resulting membrane spacing can be a fixed membrane spacing between the different electrodes, or can vary between the different electrodes.
  • the electrode chambers and resulting membrane spacing have a suitable length and width such that the electrode chambers are flat, or substantially flat in shape (see e.g., FIG. 3).
  • the electrodes can be constructed from the same material.
  • both the anode and cathode can be any flat or granular conductive material including but not limited to: carbon cloth, carbon mesh, plastic sheet with paintable carbon applied, activated carbon, graphite granules, charcoal, biochar, and stainless steel.
  • the electrodes can be constructed from different materials.
  • the anode can be carbon cloth, while the cathode is granular graphite.
  • the cathode electrode can include a combination of graphite or carbon-based material and stainless steel, or some similar catalyzing metal.
  • the electrode is composed of a rigid substrate/solid support structure such as plastic, coated in a conductive material such carbon paint or carbon epoxy.
  • the conductive material can be sprayed onto the solid support structure with enough coats to achieve a desire resistance.
  • the electrodes can include a conductive wire such as copper sheathed in plastic and allowed to protrude from the plastic in certain places in order to make contact with the conductive coating and collect current.
  • the electrodes can include a combination of the elements above in a removable cassette designed to clean the membrane when it is removed. For example, graphite brush can be placed on a carbon-epoxy coated electrode.
  • the membrane and electrodes can be designed to minimize labor associated with cleaning and maintaining.
  • the electrodes can include a carbon cloth on a solid support, and the solid support can be clamped loosely to the membrane and removed so as to apply pressure to the membrane and clean it of biofilm.
  • the two electrodes and the membrane can be cassettes that are placed in the reactor and easily removed (see FIG. 10).
  • the electrodes can be arranged in one of two preferred embodiments: 1) flat against the membrane; or 2) one or two centimeters away from the membrane.
  • the second preferred embodiment is particularly useful if a anion exchange membrane is used, as it provides space between the electrodes and membrane for denitrification to occur based on nitrates shuttling into the anode chambers.
  • the anode electrode is constructed using carbon cloth material (Type B-1B, E-TEK) and is positioned flush against the membrane. This arrangement will allow for reduced internal resistance and increased current densities in the system as the distance between anode and cathode electrode pairings will be minimized.
  • the volume of the cathode chamber is half filled with graphite granules with a graphite rod used as a current collector (Graphitesales Inc, EC 100).
  • FIG. 3 An example of a denitrification BES according to the invention is depicted in FIG. 3.
  • the BES uses multiple three-chamber, flat modules.
  • Each module has two anodes (outside) and one cathode (inside) (i.e., a cathode sandwiched by two anodes).
  • the anode is used to oxidize COD and the cathode is used to reduce nitrates to nitrogen gas.
  • the width of these chambers has a ratio of about 1:2: 1 (anode: cathode: anode), for example 2 centimeters: 4 centimeters: 2 centimeters.
  • the modules are separated by a permeable membrane (either anion exchange or cation exchange) that selectively allows ions to pass.
  • pre-treatment of wastewater streams may be necessary before feeding volumes into the reactors.
  • a pre-treatment tank can be coupled to the bio- electrochemical systems of the invention.
  • Pre-treatment for the anode and cathode streams can be carried out separately using separate pre-treatment tanks.
  • a pre-treatment tank common to all anodes within the plurality of reaction modules or all cathodes within the plurality of reaction modules can be used.
  • a splitting manifold can split the stream from each tank into each anode and/or cathode within the plurality of reaction modules, respectively.
  • Pre-treatment for the anode chamber can be without re-circulation so as to promote the settling of solids and anaerobic fermentation processes. Solids can therefore be removed from the bottom of this vessel without entering the BES system.
  • the chamber for the cathode chamber can be a constantly mixed tank thus promoting complete nitrification of the influent stream.
  • the system can be operated with dynamic control the takes treatment rates, pH or other parameters as an input, and changes the operating characteristics such as flow rate, external resistance, or other parameters.
  • the system can be operated by poising potentials, particularly cathode potentials, at the optimal potential for COD removal or denitrification.
  • poising potentials particularly cathode potentials
  • the reduction potential for denitrification being close to that of oxygen (NO 3 -/N2 at +0.74V versus +0.82V for O2/H2O), and poising the cathode at this potential would be suitable.
  • One way to poise potentials economically is to measure the cathode potential against a reference electrode and then continuously and dynamically adjust the external resistance between the anode and the cathode so as to ensure the cathode potential stays as close to the desired potential as possible.
  • the present invention also provides a novel methods for the simultaneous treatment of nitrogenous (nitrogen-containing) waste components and reduced organic compounds, commonly measured as chemical oxygen demand (COD) or biological oxygen demand (BOD).
  • COD chemical oxygen demand
  • BOD biological oxygen demand
  • the methods described herein take advantage of the existence of two separate treatment streams in most re-circulating and semi-re-circulating industrial facilities, such as aquaculture systems and wastewater treatment works.
  • settling tanks increase the solids and BOD loading
  • anaerobic digesters will decrease the C:N ratio while aerobic systems will help remove ammonia via nitrification but they will also generate nitrates.
  • aerobic systems will help remove ammonia via nitrification but they will also generate nitrates.
  • the stream higher in nitrates can be put through the cathode and the stream higher in BOD can be put through the anode.
  • the cathode can itself be oxygenated in some places, so that the chamber serves as a bio-air cathode while also nitrifying (see FIGS. 9 A and 9B, each employing filtration membranes or porous separators).
  • the two chambers of the reactor can be used partially or primarily to increase or decrease the pH of the input stream, thereby reducing costs associated with pH management (as described in more detail below).
  • the present invention provides bio-electrochemical systems and methods for the simultaneous treatment of BOD and COD using a bio-electrochemical system that includes at least one anode chamber or compartment and at least one cathode chamber compartment.
  • a wastewater stream high in reduced organics i.e., BOD
  • BOD reduced organics
  • a separate aquaculture wastewater stream high in nitrate is flowed over the cathodic electrode (i.e., the cathodic waste stream)
  • a selective membrane allows protons to transfer from the anode to the cathode and provides charge balance for the electrons flowing to the cathode.
  • the selective membrane also advantageously prevents the transference of other ions or microbes between the two streams.
  • the anodic and cathodic waste streams may be collected or prepared in one of several ways.
  • the anodic waste stream is generally higher in solids because these form a major component of the BOD in aquaculture effluent. Therefore one of several methods to separate or concentrate solids in the anodic waste stream may be employed, including but not limited to, mechanical filtration, a settling filter, a drum or canister filter or a centrifugation-based filter.
  • the high BOD stream becomes the anodic stream, and may be used as is when it exits the primary separation system, or may be further altered for optimal use in the anodic chamber.
  • a system for removing the oxygen from the anodic stream may be employed.
  • Such a system would include in-line oxygen concentration monitoring through the use of an oxygen probe, electrode or other device and a method for reducing the concentration of oxygen in the stream based on feedback from the monitoring system.
  • This could take on several forms, including but not limited to: an oxygen absorbing resin or column; a system to sparge the waste stream with anaerobic gas to drive the oxygen out of solution; a pre-treatment reactor designed to allow microbial growth or metabolism to use the oxygen in the stream before entering; or a combination of two or more such methods.
  • the cathodic waste stream may include, but is not limited to, one of the following:
  • effluent from anaerobic digestion aeration may need to be nitrified before denitrification can occur.
  • a bio-air cathode can be used in the nitrification portion of the cathode and a nitrate removing cathode can used afterwards.
  • the anode input can include, but is not limited to, one or more of the following: the reduced- solids effluent from a mechanical filter, settling filter, drum filter or centrifugation filter, used to separate high BOD solids; or culture water while still inside the main aquaculture vessel.
  • Oxygen can be detrimental to the cathodic reaction because it lowers the amount of nitrate that will be used for cathodic reduction, but is less detrimental than oxygen at the anode because it will not fundamentally alter the way that the cathodic reaction works, just the chemical species being reduced.
  • the bio-electrochemical systems described herein can be used as a treatment reactor for the combined treatment of carbon and nitrogen wastes from industrial facilities, such as an aquaculture system, that is separate and distinct from the main aquaculture vessel.
  • An example of the process design for RAS aquaculture in which the EOP stream is passed through the anode and the culture tank water is passed through the cathode is depicted in FIG. 4A.
  • FIG. 4B the process flow is similar to that depicted in FIG. 4A, however, as shown in FIG. 4B, the anode can be sandwiched by two cathodes.
  • FIG. 5 depicts an exemplary embodiment of reactor architecture/components that can be used to co-treat nitrogenous and organic wastes from an aquaculture system 1 without mixing of streams once separated.
  • the system is configured to allow settling and clarification to occur before nitrification.
  • the reactor shown in FIG. 5 includes an anode chamber 2, a cathode chamber 3, and a membrane 4 serving as a selective barrier between the two chambers that allows protons, but not water contaminants, to pass between the chambers.
  • Each of the anodic and cathodic chambers (2 and 3, respectively) contains an electrode, or several electrodes, composed of one or more electrically conductive materials and generally with a large surface area for microbial attachment.
  • Anodic and cathodic electrodes are connected to each other through external circuitry 5.
  • Each of the anode chamber 2 and cathode chamber 3 also contains at least two ports or connections for fluid-containing tubes to be connected, and a path for liquid to traverse from one or more of the ports to one or more of the remaining ports; this path may be through a porous electrode material.
  • BOD reduced organics
  • a nitrifying reactor 6 is employed upstream of the cathode chamber 3 to oxidize ammonia present in the waste to nitrate, which treats the toxic ammonia while also increasing the concentration of nitrate.
  • Such a nitrifying reactor could also employ an oxygen sensor 7 to adjust the amount of oxygen available in the nitrifying reactor for aerobic ammonia oxidation to supply marginally more oxygen than is necessary to oxidize all of the ammonia, without introducing extra oxygen that would poison the cathodic reaction.
  • a monitoring/feedback controller and/or 0 2 scrubber system 8 can also be employed to ensure that the anode is anaerobic or anoxic.
  • a liquid stream high in nitrate B flows from the aquaculture system 1 to a nitrifying reactor 6 to oxidize ammonia present in the waste to nitrate, and an oxygen sensor 7 to adjust the amount of oxygen available in the nitrifying reactor for aerobic ammonia oxidation, and into the cathode chamber 3.
  • a separate liquid/solid stream C which is high in BOD, flows from the aquaculture system 1 through a monitoring/feedback controller and/or 0 2 scrubber system 8, and into the anode chamber 2.
  • the present invention provides a treatment reactor for the combined treatment of carbon and nitrogen wastes from industrial facilities, such as an aquaculture system, where the cathodic electrode compartment is located within the main aquaculture vessel.
  • a sediment-like electrode material e.g., graphite granules, graphite spheres or graphite cubes
  • a sediment-like electrode material e.g., graphite granules, graphite spheres or graphite cubes
  • oxygen will be depleted by microbial activity before it can diffuse to the bottom layers of the electrode material.
  • ammonia can be oxidized to nitrite and then nitrate in the upper, aerobic sediment layer while the nitrate created will diffuse downward where it can be reduced to nitrogen gas and water by microbial activity by electrons donated from the electrode.
  • a non- conductive layer of sediment may be included above the conductive sediment to prevent electrons from being used solely to reduce oxygen in the aerobic layer.
  • a proton exchange membrane can be used to separate the anode and cathode chambers while allowing proton mobility to the cathode.
  • the aquaculture vessel can contain a proton exchange membrane in a wall of the floor to allow for incorporation of the biotic cathode within an anoxic or anaerobic electrically conductive substrate, such as the cathodic electrode.
  • an oxygen monitoring and reduction system leading into the anode can be used to prevent the anodic reaction from being poisoned by oxygen.
  • the present invention provides a treatment reactor for the combined treatment of carbon and nitrogen wastes from industrial facilities, such as an aquaculture system, where the treatment reactor includes two biotic cathode chambers for increased versatility in managing aquaculture wastes (FIG. 6), with the anode chamber sandwiched between.
  • a liquid stream high in nitrate B flows from the aquaculture system 1 to a first nitrifying reactor 6a to oxidize ammonia present in the waste to nitrate and into the first cathode chamber 3a.
  • a separate liquid/solid stream C which is high in BOD, flows from the aquaculture system 1 through a monitoring/feedback controller and/or 0 2 scrubber system 8, and into the anode chamber 2.
  • Ammonia may be present in both streams exiting the separator 9, and the anode reaction will generally not remediate substantial amounts of ammonia.
  • a monitor 11 is present to divert anode effluent high in ammonia (or nitrate) to a second nitrifying reactor 6b for ammonia oxidation and then to the second cathode chamber 3b for nitrate oxidation (FIG. 6).
  • a feedback system/control 12 for oxygen and effluent recirculating into the second cathode 3b can be disposed upstream the second cathode 3b.
  • the second cathode chamber 3b can be made anaerobic or somewhat aerobic by monitoring and controlling the amount and composition of air in the second nitrifying reactor 2b, and feedback system 12. Allowing some oxygen in the second cathode chamber 3b provides the anode 2 with a more rapid electron sink and could lead to increased BOD treatment rates without impacting the level of nitrate treatment in the first cathode 3a that recirculates to the aquaculture system 1. Since the cathode is generally limiting in microbial fuel cells, this dual cathode system could boost power output and treatment rates significantly.
  • a monitor/valve 13 can be positioned downstream of the second cathode 3b to recirculate the second cathode effluent, dump to waste, or route to the first cathode 3a for additional treatment/reuse.
  • the BESs according to the invention can be placed after an anaerobic digester, or along side an anaerobic digester, with the purpose of removing nitrogen and/or nitrate while generating electricity.
  • the anode stream can be either the input to a primary clarify or the input to the anaerobic digester.
  • the anode stream can be the output of the anaerobic digester. If the anode stream is the output of the anaerobic digester, ammonia oxidizing bacteria can be used in the anode chamber to help remove ammonia.
  • a bio- air cathode can be used to remove residual ammonia, and a denitrifying cathode can be used to remove nitrates (see FIGS. 7A and 7B, embodiments in which the system is used as a polishing step for anaerobic digestion. Aeration is used to nitrify in a bio-air cathode and then cathode denitrification can occur).
  • the BESs according to the invention can be placed after or alongside a nitrate concentrating system (e.g., electrodialysis) for the purpose of treating nitrates.
  • a nitrate concentrating system e.g., electrodialysis
  • the system can be used to capture or remove C0 2 in biogas or otherwise.
  • C0 2 produced at the anode can be bubbled into the cathode.
  • the cathode microbes can use the C0 2 as a carbon source for growth or other reactions.
  • Methane produced in an anaerobic digester can also be bubbled through the cathode, and the microbes will use the C0 2 .
  • the biogas may or may not be purified or separated from the C0 2 in some way beforehand.
  • Most generally bubbling biogas and/or C0 2 through a denitrifying reactor can be a way to remove or sequester C0 2 particularly if a bio-cathode is present to provide electrons.
  • the reactor is operated with positive pressure from the cathode to the anode, so that the nitrate laden stream is always pushed into the anode in the event of any membrane tears or breaches.
  • Denitrification for the removal of the toxic ammonia results in a decrease in the pH of the culture water. Typically, this acidification must be countered with the addition of alkalinity through the use of caustic and/or carbonate. Denitrification treatment technologies will generally mitigate the requirement for pH adjustment, although the exact degree depends on the method and carbon source used. Thus, an important feature of a denitrification used for aquaculture wastewater treatment is a reduction in the amount of pH correction required.
  • the BESs described herein can be used to remove COD (anode), nitrate (cathode) and also improve pH quality in process waster and wastewater.
  • the system can therefore operate at a maximum rate for nitrate removal, COD removal, or pH management depending on the exact needs.
  • a hydraulic retention time (HRT) suitable for optimizing pH might be used and in that case, only partial de-nitrification and partial COD removal favored. This depends on the economics of the site in question.
  • the influent for the reactors originate from two separate streams from the onsite aquaculture tanks or related facilities. These streams can run into separate holding tanks (e.g., 1,000 L each), allowing for a HRT of around 60 hours. This allows for monitoring of pH, temperature, conductivity, COD and nitrate concentrations. If required, this also allows for pre-treatment before being fed into a BES according to the invention.
  • the anode(s) and cathode(s) can be pre-treated separated (see e.g., FIG. 8).
  • the pre-treatment tank for the anode chambers can be left without mixing in order to promote anaerobic fermentation processes, to help optimize performance of the anodic electrogenic biofilm.
  • the cathode pre- treatment tank can be mixed to promote the complete nitrification of the stream and the generation of an anaerobic environment suitable for denitrification.
  • Pumps are used to transfer the monitored solution from the tanks to the reactor chambers.
  • Injection ports and mixing segments can be installed in the influent lines to allow for nutrient and acid dosing.
  • the BESs described herein include a blowdown tank large enough to hold the waste streams over 60 hours in order to be properly treated before being returned to the waste disposal stream.
  • Lines can be installed to feed the cathode effluent back to the aquaculture tank recirculation lines.
  • Solids Handling Solids are known to be a critical issue for biological reactors, including BES-based technologies.
  • the BESs according to the invention can include safety measures to deal with solids.
  • a grit strainers and/or a flow-through filtration unit can be employed.
  • the influent streams travel through grit strainers and a flow-through filtration unit to remove large solids.
  • the BESs according to the invention can also be designed to include a backflow purge to wash out solids accumulating inside the reactor.
  • pressure gauges can be installed on the inlets and outlets of all pumps and reactors.
  • Removable view-pipes can also be installed to observe solids buildup.
  • pre-treatment of wastewater streams may be necessary before feeding volumes into the reactors.
  • Pre-treatment for anode and cathode chambers can be carried out separately.
  • Pre-treatment for the anode chamber can be without recirculation so as to promote the settling of solids and anaerobic fermentation processes. Solids will be removed from the bottom of this vessel without entering the BES system.
  • the chamber for the cathode chamber can be a constantly mixed tank thus promoting complete nitrification of the influent stream.
  • the BES systems of the invention include pre-treatment tanks that are hold enough volume for several days of operation (e.g., 1,000 L in volume). With such a large volume, temporal changes in the source volume will be minimized.
  • the pre-treatment tanks facilitate normalizing pH, temperature, COD, nitrate, and other nutrients critical for operation.
  • pumps can be utilized to transfer the volumes to the reactors.
  • System Connectivity Te-In Locations.
  • the BESs according to the invention can be designed with ease of connection as a high priority.
  • Hoses can be used to transfer volumes between the pre-treatment tanks and reactors, or other process units.
  • cam-and- groove couplings can be used to allow for quick connections during operation and allow for flexible placement of units.
  • hoses with couplings is an advantage as opposed to hard-line cemented PVC since flexibility is achieved by the reactor design described herein. This will allow the reactors to be placed in series or separated entirely for different scenarios and/or applications.
  • the BESs described herein can include water sampling access points along various locations in the system.
  • the system can be designed to allow for water samples to be taken from the pre-treatment tank during preparation, continuously from the reactor at the input, output, and a number of locations along its length.
  • Each of the parallel systems can be independently run by a multichannel I/O programmable logic controller. This controller can be used to control the pumps, collect temperature, pH, reference electrode, COD, and nitrate, conductivity, and pressure readings, and relay the data over the internet to a remote data server. Supervisory Control & Automated Data Acquisition (SCAD A) capabilities can also be included are envisioned within the scope of the present invention.
  • SCAD A Supervisory Control & Automated Data Acquisition
  • the BESs according to the invention are preferably run at low resistance in order to maximize current. However, in larger scale systems when power must be used, power management systems can be used to up-convert the low voltage (-0.25V) to the necessary higher voltages for process units.
  • Gas Handling Gas production from the cathode is expected to be approximately 1 scf / day (based on denitrification rates) with similar rates expected from the anode. No processing of the produced gases is necessary. Gas produced in the cathode of the reactor (principally N 2 ) will rise to the top and be purged through a gas trap and released. Gas flow can be quantified with a gas rotameter and purged to the exterior of the reactor. Gas from the anode is primarily C0 2 , however methane and hydrogen sulfide can also be produced. This gas will also be vented to the exterior following collection and metering. Exact venting requirements can be evaluated during process safety review. Gas sampling locations can be included following gas traps so the composition may be periodically monitored.
  • Pressure gauges and flow meters can be installed at critical points in the system, with pressure-maintaining release valves and rupture discs, to facilitate observation of pressure and flow in the reactors.

Abstract

La présente invention concerne des conceptions de réacteur, des conceptions de composants, et des schémas de fonctionnement pour éliminer les nitrates et la demande chimique en oxygène de tout courant d'eaux usées approprié. L'invention concerne également des conceptions de réacteur, des conceptions de composants, et des schémas de fonctionnement conçus pour modifier et améliorer le pH et la qualité de l'eau des courants d'eaux usées.
EP11810413.2A 2010-07-21 2011-07-21 Dénitrification et contrôle du ph à l'aide de systèmes bio-électrochimiques Withdrawn EP2595925A4 (fr)

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PCT/US2011/044872 WO2012012647A2 (fr) 2010-07-21 2011-07-21 Dénitrification et contrôle du ph à l'aide de systèmes bio-électrochimiques

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