WO2019027377A1 - Bioréacteur à membrane de dénitrification mixotrophe à base de soufre élémentaire - Google Patents

Bioréacteur à membrane de dénitrification mixotrophe à base de soufre élémentaire Download PDF

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Publication number
WO2019027377A1
WO2019027377A1 PCT/TR2017/000151 TR2017000151W WO2019027377A1 WO 2019027377 A1 WO2019027377 A1 WO 2019027377A1 TR 2017000151 W TR2017000151 W TR 2017000151W WO 2019027377 A1 WO2019027377 A1 WO 2019027377A1
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WIPO (PCT)
Prior art keywords
sulfur
nitrate
denitrification
bioreactor
methanol
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Application number
PCT/TR2017/000151
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English (en)
Inventor
Adem Yurtsever
Deniz UÇAR
Erkan ŞAHİNKAYA
Original Assignee
Hasan Kalyoncu Üni̇versi̇tesi̇
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Publication of WO2019027377A1 publication Critical patent/WO2019027377A1/fr

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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
    • C02F3/02—Aerobic processes
    • C02F3/12—Activated sludge processes
    • C02F3/1236—Particular type of activated sludge installations
    • C02F3/1268—Membrane bioreactor systems
    • C02F3/1273—Submerged membrane bioreactors
    • C—CHEMISTRY; METALLURGY
    • C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F3/00—Biological treatment of water, waste water, or sewage
    • C02F3/28—Anaerobic digestion processes
    • C02F3/2853—Anaerobic digestion processes using anaerobic membrane bioreactors
    • 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
    • C02F3/305—Nitrification and denitrification treatment characterised by the denitrification
    • 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
    • C02F3/34—Biological treatment of water, waste water, or sewage characterised by the microorganisms used
    • C02F3/345—Biological treatment of water, waste water, or sewage characterised by the microorganisms used for biological oxidation or reduction of sulfur compounds
    • C—CHEMISTRY; METALLURGY
    • C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F2101/00—Nature of the contaminant
    • C02F2101/10—Inorganic compounds
    • C02F2101/16—Nitrogen compounds, e.g. ammonia
    • C02F2101/163—Nitrates
    • 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
    • C02F2101/20—Heavy metals or heavy metal compounds
    • C02F2101/22—Chromium or chromium compounds, e.g. chromates
    • C—CHEMISTRY; METALLURGY
    • C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F2103/00—Nature of the water, waste water, sewage or sludge to be treated
    • C02F2103/16—Nature of the water, waste water, sewage or sludge to be treated from metallurgical processes, i.e. from the production, refining or treatment of metals, e.g. galvanic wastes
    • C—CHEMISTRY; METALLURGY
    • C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F2103/00—Nature of the water, waste water, sewage or sludge to be treated
    • C02F2103/22—Nature of the water, waste water, sewage or sludge to be treated from the processing of animals, e.g. poultry, fish, or parts thereof
    • C02F2103/24—Nature of the water, waste water, sewage or sludge to be treated from the processing of animals, e.g. poultry, fish, or parts thereof from tanneries
    • C—CHEMISTRY; METALLURGY
    • C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F2103/00—Nature of the water, waste water, sewage or sludge to be treated
    • C02F2103/26—Nature of the water, waste water, sewage or sludge to be treated from the processing of plants or parts thereof
    • 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
    • C02F2209/03—Pressure
    • 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
    • C02F2209/42—Liquid level
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E50/00—Technologies for the production of fuel of non-fossil origin
    • Y02E50/30—Fuel from waste, e.g. synthetic alcohol or diesel
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02W—CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO WASTEWATER TREATMENT OR WASTE MANAGEMENT
    • Y02W10/00—Technologies for wastewater treatment
    • Y02W10/10—Biological treatment of water, waste water, or sewage

Definitions

  • This invention is specifically related to the development of elemental-sulfur based mixotrophic denitrifying membrane bioreactor (MBR) process for simultaneous Cr(VI) and nitrate reduction from drinking water
  • the chromium is used in numerous industrial applications, such as stainless steel, metal plating, leather tanning and wood treatment. Chromium contamination of soil, groundwater and surface waters due to unsuitable water and wastewater discharges is a major problem that is widespread all over the world.
  • Cr (VI) and Cr (III) are the most dominant types in the environment, although the chromium oxidation state varies between -2 and +6.
  • the hexavalent chromium which is thought to cause carcinogenic, teratogenic and toxic effects, tends to be mobile in nature.
  • Cr (III) may precipitate in the form of hydroxide (Cr(OH) 3 ), especially at neutral pH.
  • Advanced methods of treatment such as reverse osmosis, ion exchange, membrane filtration and electrodialysis are very effective for chromium removal.
  • the reduction of Cr (VI) using microbial systems is also one of the potential methods used for chromium treatment.
  • high concentrations of Cr (VI) may be toxic to bacteria in long term operation of bioreactor.
  • Cr (VI) has been successfully reduced to Cr (III), but the formed Cr (III) has left the bioreactor because it is not precipitate.
  • Nitrate is one of the most common contaminants in surface and ground waters. The most important sources of nitrate are excessive use of nitrogen-containing fertilizers and discharge of domestic and industrial wastewaters without nutrient removal. According to TS266, the limit values for nitrate and nitrite in drinking water are 1 1 .3 mg/L NO3 -N and 0.15 mg/L NO2 -N, respectively. In many drinking water resources, nitrate and chromate can be found together(Vainshtein et.al. 2003; Baek et.al. 2004). Therefore, it is necessary to develop biological systems which can remove the nitrate and Cr (VI) simultaneously. Recently, there are so many studies on autotrophic biological denitrification processes for nitrate removal from drinking water.
  • SAD sulfur-based autotrophic denitrification
  • Thiobaciilus denitrificans and Thiomicrospira denitricans etc. use the elemental sulfur and nitrate as an electron donor and an acceptor, respectively.
  • nitrate is finally transformed into nitrogen gas, sulfur is transformed into sulfate.
  • CO ⁇ is used as a carbon source and the reaction is simply shown below (Zhang, 2004).
  • the main disadvantages of this process are sulfate and acid generation.
  • the aim of the study is to reduce Cr (VI) to Cr (III) and to remove Cr (III) from the water by precipitating as Cr(OH)3 at neutral pH values.
  • Hydrogen has been used as an electron source for both nitrate and chromium reductive bacteria.
  • Mixotrophic denitrification is a process in which both heterotrophic and sulfur-based autotrophic denitrification processes are combined in a single reactor to eliminate disadvantages of both processes (Sahinkaya et.al. 201 1 ). Alkalinity generated in heterotrophic denitrification may neutralize the acidity generated by the autotrophic process. In addition, since heterotrophic denitrification will consume some nitrate, the amount of sulfate produced by the autotrophic process will also decrease. The most significant advantages of autotrophic denitrification compared to heterotrophic process, especially for drinking water treatment, are the elimination of organic supplementation and reduced bacterial growth, which may decrease the treated water contamination.
  • the sulfur-based mixotrophic denitrification process is a highly advantageous method for nitrate removal from drinking water.
  • nitrate and Cr (VI) can be present together in many groundwater (Vainshtein et.al. 2003; Baek et.al. 2004). For this reason, researchers are also carrying out on systems that removes Cr (VI) and nitrate simultaneously. Since the concentration of contaminants such as Cr (VI) in drinking water is low, the required energy to grow bacteria can not be produced only by chromium reduction. For this reason, nitrate is used as the primary electron acceptor for microorganisms. Denitrifying microorganisms reduce Cr (VI) to Cr (II I) by using it as a secondary electron acceptor.
  • Liu et al. (2009) operated a two-stage denitrification process to eliminate disadvantages of both heterotrophic and autotrophic denitrification processes.
  • the first process in this system is heterotrophic denitrification, some of the nitrate is removed at this stage, and alkalinity is generated.
  • the theoretical C/N ratio for complete heterotrophic denitrification is 2.47 g/g. However, the required ratio is greater than 2.47 due to the presence of oxygen in the water.
  • organic matter remained at the effluent when the organic matter is added to the stoichiometric ratio or more.
  • Membrane Bioreactors are biological processes in suspended growth media in which treated water and biomass are physically separated by a membrane. Biochemical oxidation and water/biomass separation that take place in two separate tanks in the conventional activated sludge process, occurs in a single tank in the MBR. The use of membrane bioreactors for water treatment has begun to be used at an increasing rate in developed and developing countries over the past 10 years.
  • an integrated flat-sheet MBR and reverse osmosis membrane system are used to treat wastewater.
  • wastewater treatment process after textile wastewater is treated in the aerobic reactor, the wastewater was passed through a flat layer MBR separation. After MBR, further treatment with reverse osmosis membrane was applied.
  • the objective of this invention is to develop a process that simultaneously removes nitrate and Cr (VI), which can often be present together in drinking waters, in membrane bioreactors, with the sulfur-based mixotrophic denitrification process.
  • VI nitrate and Cr
  • Another objective of the invention is to provide mixotrophic (autotrophic + heterotrophic) conditions resulting from the combination of autotrophic denitrification and heterotrophic denitrification processes, thus, elimination of alkalinity requirement and excess sulfate generation of sulfur-based autotrophic denitrification process is possible by stimulating simultaneous autotrophic and heterotrophic (mixotrophic) denitrification process by methanol supplementation.
  • heterotrophic nitrate reduction processes organic substances can be remain in the effluent when supplemented in excess amount and these substances can cause microbial growth and undesirable disinfection by-products in the disinfection processes with chlorine in the water distribution networks.
  • Methanol is fed from the methanol feed tank and sulfur is fed to the system from the sulfur feed tank simultaneously.
  • Another object of the invention is to identify the most suitable alternative to reduce the membrane fouling in the membrane bioreactor
  • FIG. 1 Schematic representation of the membrane bioreactor system - overview
  • the powdered elemental sulfur (particle size was around 150 pm) was weekly added to the MBR at a S°/N0 3 -N ratio of 1 .5 g/g.
  • the added elemental sulfur theoretically reduces only 60% of the feed nitrate.
  • the electron source amount was around 15% higher than the theoretical requirement to make sure that electron amount was enough for the complete nitrate reduction and the electron source is also supplied to the reactor to reduce Cr (VI). Therefore, in order to reduce the nitrate present in the feed of the mixotrophic bioreactor (7), less methanol than the required amount and enough sulfur to reduce the remaining nitrate are being fed. Elemental sulfur is not continuously added to the reactor like methanol.
  • the MBR are supplemented with methanol from the methanol feed tank (1 ) as the organic carbon source for heterotrophic denitrifiers and the sulfur from the sulfur feed tank (6) for autotrophic sulfur oxidizing and nitrate reducing microorganisms.
  • the required elemental sulfur is weekly added to the MBR to provide the surface for the bacteria and to help the cleaning of the membrane physically.
  • powdered elemental-sulfur particles size ⁇ 50-150 pm
  • Ther water to be treated is initially pumped into the feed tank (2). From here, the water is fed into the bioreactor (7) by the feed pump (3).
  • methanol stored in the methanol feed tank (1 ) is fed into the bioreactor (7) by the feed pump (3) to provide heterotrophic denitrification and sulfur is weekly supplemented from sulfur feed tank (6) to provide autotrophic denitrification.
  • the decrease of the water level inside the bioreactor (7) is determined by the level sensor (5) and is transmitted to the feed controller (4).
  • the level controller (4) provides the operation of the feed pump (3). In this way, the water influent to the bioreactor (7) is provided.
  • the bioreactor (7) was completely mixed by a stirrer (9) located under the bioreactor (7). It is ensured that the microorganism is fully mixed with the water containing methanol, nitrate and Cr (VI). After the biological oxidation of methanol, nitrate and Cr (VI) in the fully mixed bioreactor (7), the treated water is filtered by the suction pump (1 1 ) through a microfiltration membrane (8) with 0.45 Mm pore size to separate from the microorganism. During water filtration from the membrane (8), the pressure difference between the microfiltration membrane (8) and the suction pump (1 1 ) is measured by the pressure sensor (10) and is stored instantaneously in the computerized monitoring and control system (13).
  • the suction pump (1 1 ) is stopped via the computerized monitoring and control system (13), which prevents damage to the membranes.
  • the effluent is collected in the effluent tank (12).
  • the main function of the membrane (8) in the mixotrophic bioreactor (7) is to keep microorganisms in the bioreactor (7).
  • the SS concentration of the effluent is obtained at very low values by separating the treated water and microorganisms from each other.
  • the system described in detail above is capable of serving the above-mentioned purposes and it can be applied in industry to remove nitrate and Cr (VI) in drinking water.
  • the invention can be used successfully in the treatment of surface and groundwater containing high nitrate level, particularly in drinking water treatment plants that supply drinking water to the public.
  • the invention can be used not only in drinking water, but also in treatment of wastewaters containing high nitrate concentration.

Abstract

La présente invention concerne l'élaboration d'un système pour la réduction simultanée de nitrate et de chromate en combinant les avantages des technologies de dénitrification hétérotrophe à base de soufre, de dénitrification autotrophe et de bioréacteur à membrane (MBR). L'invention a été spécialement conçue pour éliminer les inconvénients de la dénitrification hétérotrophe à base de soufre et de la dénitrification autotrophe avec le procédé mixotrophe qui est un procédé de réduction du nitrate et du Cr (VI). Avec cette invention, le sulfate produit dans la dénitrification autotrophe à base de soufre au-dessous des valeurs limites et l'exigence d'alcalinité ont été éliminées grâce à l'alcalinité produite par le processus de dénitrification hétérotrophe. De plus, grâce à la membrane (8) utilisée dans le système, les microorganismes à taux de croissance lent demeurent dans le bioréacteur (7). Parallèlement, le lessivage des particules de petite taille du système est évité.
PCT/TR2017/000151 2017-08-03 2017-12-29 Bioréacteur à membrane de dénitrification mixotrophe à base de soufre élémentaire WO2019027377A1 (fr)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
TR2017/11429 2017-08-03
TR2017/11429A TR201711429A2 (tr) 2017-08-03 2017-08-03 Elementel kükürt bazli mi̇ksotrofi̇k deni̇tri̇fi̇kasyon membran bi̇yoreaktörü

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Cited By (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN110877927A (zh) * 2019-12-02 2020-03-13 中国地质大学（北京） 一种沉钒废水处理系统、方法及用途
CN113522228A (zh) * 2021-07-20 2021-10-22 南京大学 一种同步脱氮除铬轻质材料及其制备方法和应用
CN114291900A (zh) * 2021-12-31 2022-04-08 中国科学院生态环境研究中心 一种硫自养反硝化颗粒及其制备方法与应用
WO2024021421A1 (fr) * 2022-07-25 2024-02-01 哈尔滨工业大学（深圳） Procédé de régulation de rétrolavage pour filtre de dénitrification autotrophe utilisant des charges soufrées

Families Citing this family (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN115536144B (zh) * 2021-06-29 2024-05-03 中国石油化工股份有限公司 一种硫自养反硝化菌的快速富集方法及装置

Citations (3)

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EP1568662B1 (fr) 2004-02-25 2008-04-09 Bilfinger Berger Umwelttechnik GmbH Bioreacteur à membrane et méthode de traitement des eaux résiduelles
CN102101738A (zh) 2009-12-21 2011-06-22 东丽纤维研究所（中国）有限公司 平板膜生物反应器和反渗透的综合膜集成系统的废水处理工艺
US20160075579A1 (en) * 2014-09-15 2016-03-17 Velocys Technologies, Ltd. Methods of Making Purified Water from the Fischer-Tropsch Process

Patent Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP1568662B1 (fr) 2004-02-25 2008-04-09 Bilfinger Berger Umwelttechnik GmbH Bioreacteur à membrane et méthode de traitement des eaux résiduelles
CN102101738A (zh) 2009-12-21 2011-06-22 东丽纤维研究所（中国）有限公司 平板膜生物反应器和反渗透的综合膜集成系统的废水处理工艺
US20160075579A1 (en) * 2014-09-15 2016-03-17 Velocys Technologies, Ltd. Methods of Making Purified Water from the Fischer-Tropsch Process

Non-Patent Citations (1)

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Title
SAHINKAYA ERKAN ET AL: "A novel elemental sulfur-based mixotrophic denitrifying membrane bioreactor for simultaneous Cr(VI) and nitrate reduction", JOURNAL OF HAZARDOUS MATERIALS, ELSEVIER, AMSTERDAM, NL, vol. 324, 15 February 2016 (2016-02-15), pages 15 - 21, XP029836981, ISSN: 0304-3894, DOI: 10.1016/J.JHAZMAT.2016.02.032 *

Cited By (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN110877927A (zh) * 2019-12-02 2020-03-13 中国地质大学（北京） 一种沉钒废水处理系统、方法及用途
CN113522228A (zh) * 2021-07-20 2021-10-22 南京大学 一种同步脱氮除铬轻质材料及其制备方法和应用
CN114291900A (zh) * 2021-12-31 2022-04-08 中国科学院生态环境研究中心 一种硫自养反硝化颗粒及其制备方法与应用
WO2024021421A1 (fr) * 2022-07-25 2024-02-01 哈尔滨工业大学（深圳） Procédé de régulation de rétrolavage pour filtre de dénitrification autotrophe utilisant des charges soufrées

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