WO1997031682A1 - Procede de decomposition microbienne de substances nuisibles contenues dans des milieux, et micro-organismes appropries a ce procede - Google Patents

Procede de decomposition microbienne de substances nuisibles contenues dans des milieux, et micro-organismes appropries a ce procede Download PDF

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Publication number
WO1997031682A1
WO1997031682A1 PCT/EP1997/001017 EP9701017W WO9731682A1 WO 1997031682 A1 WO1997031682 A1 WO 1997031682A1 EP 9701017 W EP9701017 W EP 9701017W WO 9731682 A1 WO9731682 A1 WO 9731682A1
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WO
WIPO (PCT)
Prior art keywords
fermenter
degradation
microorganism
formaldehyde
dsm
Prior art date
Application number
PCT/EP1997/001017
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German (de)
English (en)
Inventor
Peter Bartholmes
Kerstin Heesche-Wagner
Michael Kaufmann
Thomas Schwarz
Original Assignee
Bitop Gesellschaft Für Biotechnische Optimierung Mbh
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.)
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Publication date
Application filed by Bitop Gesellschaft Für Biotechnische Optimierung Mbh filed Critical Bitop Gesellschaft Für Biotechnische Optimierung Mbh
Priority to EP97906145A priority Critical patent/EP0885032A1/fr
Priority to JP9530634A priority patent/JP2000505341A/ja
Publication of WO1997031682A1 publication Critical patent/WO1997031682A1/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
    • C02F3/34—Biological treatment of water, waste water, or sewage characterised by the microorganisms used
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
    • B01D53/34—Chemical or biological purification of waste gases
    • B01D53/74—General processes for purification of waste gases; Apparatus or devices specially adapted therefor
    • B01D53/84—Biological processes
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B09—DISPOSAL OF SOLID WASTE; RECLAMATION OF CONTAMINATED SOIL
    • B09C—RECLAMATION OF CONTAMINATED SOIL
    • B09C1/00—Reclamation of contaminated soil
    • B09C1/10—Reclamation of contaminated soil microbiologically, biologically or by using enzymes
    • 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
    • Y02A—TECHNOLOGIES FOR ADAPTATION TO CLIMATE CHANGE
    • Y02A50/00—TECHNOLOGIES FOR ADAPTATION TO CLIMATE CHANGE in human health protection, e.g. against extreme weather
    • Y02A50/20—Air quality improvement or preservation, e.g. vehicle emission control or emission reduction by using catalytic converters

Definitions

  • the invention relates to a method for microbial degradation of pollutants in pollutant-laden media in air, wastewater or soil purification and a device for carrying out this method.
  • the invention further relates to microorganisms suitable for carrying out the method and their use.
  • remediation processes The methods for the reduction of pollutants in polluted media (air, waste water, soil) are referred to as remediation processes. These methods include both the thermal, physical or chemical treatment of the contaminated medium and the biological elimination of pollutants, in which the pollutants contained in the medium are decomposed by the microorganisms or converted into other substances, the disposal of which is less problematic.
  • Microorganisms suitable for the efficient degradation of pollutants must have an optimal pollutant tolerance and the highest possible genetic stability in addition to their specific degradability. In addition, suitable strains must not be pathogenic and must not form dangerous end or intermediate products.
  • microorganisms belonging to the site are often used for biological pollutant elimination.
  • on-site microorganisms often have the disadvantage that they are unsuitable for use in environmental engineering because of their low breakdown rates, their low toxin tolerance or their susceptibility to foreign germs Systems not suitable For this reason, more and more "special cultures" are used in microbial pollutant elimination, which have both higher degradation rates and less susceptibility to foreign germs, a relatively high level of genetic stability and / or a high toxin tolerance Special crops can achieve a certain increase in the degradation performance of the biocoenosis and a shortening of the approach tents of degradation systems
  • a further object of the invention is to develop microorganisms, which are suitable for carrying out the method according to the invention, and to provide their use and a device for carrying out the method
  • the task is solved by a process for the degradation of pollutants in pollutant-laden media during air, wastewater or soil cleaning, in which continuous degradation fermentation is carried out using contaminated pollutants
  • Microorganism culture is carried out in a degradation fermenter, the pollutant concentration in the degradation fermenter being controlled with the aid of a control loop during the degradation fermentation
  • This control can be carried out either by keeping the pollutant concentration constant between an upper and a lower threshold value (f-oxinostatic fermentation) or by using the vitality of the biomass as a leader to regulate the toxin concentration (toxinodynamic fermentation)
  • Toxinodynamic fermentation for example, oxygen consumption or cell respiration serve as vitality parameters.
  • the above-mentioned regulations for the pollutant concentration in the fermenter allow the selection pressure to be maintained during the process.
  • the fermenter is used for continuous sampling for on-line purposes. Measurement of the pollutant concentration, the type of measurement of course depending on the pollutant to be detected.
  • the control can be parameterized in such a way that when a certain threshold value is reached, it is reduced the pollutants are pumped into the reactor while the inflow of the pollutants is reduced when a second, upper concentration threshold value is reached
  • FIG. 1 shows the phenol and formaldehyde concentration in the course of a toxinostatic fermentation.
  • Curve A shows the measurement signal of the concentration of phenol and curve B shows the measurement signal of the concentration of formaldehyde in the fermenter.
  • the black blocks show the duration of the pumping intervals of the substrate feed on
  • the process according to the invention under the control of toxinostatic fermentation brings two essential advantages for industrial pollutant degradation in a continuous reactor.
  • a suitable setpoint for the pollutant concentration in the reactor outflow by specifying a suitable setpoint for the pollutant concentration in the reactor outflow, prescribed receiving water limit values can be observed.
  • the lower threshold value of the pollutant concentration in the degradation fermenter is preferably not below the okotoxicity limit of any microorganisms which are present in the degradation fermenter but which do not contribute to pollutant degradation
  • the okotoxicity limit is the pollutant concentration at which the total metabolism of the examined biological material breaks down
  • the polluted medium contains formaldehyde and the added microorganism culture contains the microorganisms DSM 11423 and / or DSM 11424 or mutants or variants of these microorganisms
  • Formaldehyde in aqueous solution has an extremely toxic effect on microorganisms and is one of the best disinfectants, preservatives and stabilizers.
  • the formaldehyde tolerance values of the microorganisms described so far are far below the formalin concentrations normally found in problematic waste water and waste Microbial degradation of formaldehyde in high concentrations has not been possible until now.
  • a microorganism culture is developed which is capable of formaldehyde concentrations of up to 5,500 mg / l tolerate and degrade the pollutant at high speed
  • the pollutant-containing medium contains phenol and the microorganism culture contains the microorganism DSM 11425 or mutants or variants of this microorganism.
  • the degradation of formaldehyde and phenol during the same fermentation is carried out with simultaneous use of DSM 11425 with DSM 11423 and / or DSM 11424 also possible
  • microorganisms DSM 11423, DSM 11424 and DSM 11425 were deposited on 21.02.1997 with the DSMZ - German Collection of Microorganisms and Cell Cultures Mascheroder Weg 1 b, D-38124 Braunschweig. The physiological and bacterological properties of these microorganisms are shown in Tables 1 and 2 referenced
  • the microorganism DSM 11423 was isolated from a formalin-impregnated tissue sample and initially identified as Methylobacterium ⁇ xtorquens. In degradation fermentations under different conditions, DSM 11423 shows a maximum degradation rate for formaldehyde of 1612 nmol / min * mg and a tolerance limit for this pollutant of 10 mM.
  • DSM 11423 has the highest degradation rate and the lowest Ks value of the formaldehyde-degrading strains investigated in the context of the invention (696 ⁇ M) and is able to reduce the formaldehyde content of a formaldehyde-contaminated medium to almost zero by degradation.
  • the pollutant tolerance is low at 10 mM (300 mg / l).
  • the formaldehyde is broken down by oxidation to formic acid, catalyzed by the glutathione-dependent formaldehyde dehydrogenase.
  • the specific activity of this enzyme in the crude extract is very high at around 1.6 lU / mg protein.
  • the microorganism DSM 11424 was also isolated from a formalin-impregnated tissue sample and initially identified as Pseudomonas putida. When degradation was observed under various conditions, DSM 11424 showed a maximum degradation rate for formaldehyde of 784 nmol / min * mg and a tolerance limit for this pollutant of 100 mM. Compared to other formaldehyde-degrading strains investigated, DSM 11423 has an average degradation rate but the highest K s value (11643 ⁇ M) and is able to decompose formaldehyde even at very high concentrations.
  • the formaldehyde content of the medium can be reduced to approximately 200 mg / l by pure culture of this microorganism.
  • the formaldehyde degradation takes place in the first step via oxidation to formic acid, catalyzed by the glutathione-dependent formaldehyde dehydrogenase. The specific activity of this enzyme in the crude extract is only low.
  • the microorganism DSM 11425 was isolated from a soil sample and is able to convert phenol with a significantly higher degradation rate than the microorganisms on site.
  • the partial sequencing of the 16S rRNA of this microorganism showed a similarity of 99.1% to the type strain Klebsiella oxytoca.
  • the aerobic phenol degradation takes place in a first step by means of an NADH- or NADPH-dependent orf / 70-hydroxylation of the phenol which is catalyzed by the phenol hydroxylase.
  • the product is catechol, a key intermediate in most aromatics routes.
  • Catechol is metabolized in two ways: first through the chromosome-encoded o / t ⁇ o cleavage, and also via the plasmid-encoded mete-cleavage, the ort ⁇ o cleavage being induced by its product, cis. ⁇ s-muconic acid and the mete-cleavage by phenol.
  • the medium flowing out of the degradation fermentation is subjected to a second degradation fermentation, the lower threshold value of the pollutant concentration in the degradation fermenter being lower in the second degradation fermentation than in the first degradation fermentation.
  • An increase in the degradation efficiency is achieved by the pollutant concentration in the first fermenter, independent of that of the second fermenter, so that an optimal enzyme induction and thus a correspondingly high degradation rate is achieved.
  • the pollutant concentration in the second fermenter is then set so that the pollutant concentration in the process corresponds to the prescribed introduction limit
  • the microorganism culture Before being added to the pollutant-laden medium, the microorganism culture is preferably cultured in a mutation fermenter containing a nutrient-rich medium and subjected to a mutagenic treatment and stabilized and then in a selection fermenter which contains a nutrient-poor medium enriched with the pollutant (s). subjected to a selection whereby part of the culture from the selection fermenter is continuously returned to the mutation fermenter until a microorganism culture with the desired pollutant degradation performance and tolerance has been established
  • the degradation fermentation is preceded by a method for growing microorganisms which is based on the principle of evolutionary optimization.
  • a method for growing microorganisms which is based on the principle of evolutionary optimization.
  • the microorganisms DSM 11423, DSM 11424 and DSM 11425 described above are used according to the invention for the cultivation of mutants or variants. Cultivation can take place, for example, by selecting spontaneously occurring mutations. Other possibilities include, for example, mutation through the action of chemical substances and / or radioactive radiation and / or UV light. This allows mutants and variants to be obtained which have improved properties, for example with regard to the pollutant degradation performance or the pollutant tolerance.
  • microorganisms DSM 11423 and DSM 11424 are used as donor organisms for genetic material, in particular for inserting a gene coding for a formaldehyde dehydrogenase or formaldehyde dismutase and / or the associated promoter sequence into a microorganism or a cell.
  • the gene is incorporated into the recipient organism using the methods customary in microbiology, e.g. using a vector.
  • larger amounts of an enzyme relevant for the degradation of pollutants for example formaldehyde dehydrogenase, can be produced.
  • the aforementioned microorganisms are also used to obtain a gene encoding a formaldehyde dehydrogenase or formaldehyde dismutase and / or the associated promoter sequence for the purpose of sequence analysis.
  • the biomass obtained by carrying out the method according to the invention can advantageously be used for / n-s / Y-z soil remediation, in which the pollutants of degradable microorganisms are broken down directly in the soil without removing the soil and thus changing the soil structure.
  • an apparatus for carrying out the method according to the invention which contains at least one degradation fermenter and means for regulating the pollutant concentration in the degradation fermenter or fermenters.
  • the device contains a degradation fermenter and the associated means for regulating the concentration of pollutants in the fermenter, but several parallel fermenters are also conceivable, which can be loaded and inoculated with pollutant-laden medium at the same time.
  • two successive decomposition fermenters are provided, in which the pollutant concentration is set independently of one another by corresponding control loops.
  • a device which contains a mutation fermenter for the cultivation, mutagenic treatment and stabilization of the microorganism culture, a selection fermenter, means for returning part of the culture from the selection fermenter to the mutation fermenter, means for regulating the pollutant concentration in the selection fermenter contains at least one degradation fermenter and means for regulating the pollutant concentration in the degradation fermenter (s).
  • a fermenter with a reactor volume greater than 10 1 is continuously fed with hospital wastewater which contains formaldehyde in fluctuating concentrations between 50 g / 1 and 200 g / 1.
  • the water contains various other organic substances.
  • the following media components are added to the wastewater before the reactor is introduced:
  • the formaldehyde-containing solution introduced does not contain any viable microorganisms due to its high toxicity, but for safety reasons it is exposed to lethal doses before UV radiation is introduced.
  • the reactor is inoculated with a mixed culture containing the microorganisms DSM 11423 and DSM 11424.
  • the process is carried out in the range from pH 5.0 to 8.5 and under p ⁇ 2 regulation up to 10% of the maximum oxygen saturation concentration of the waste water.
  • Degradation fermentation takes place at temperatures between 5 and 45 ° C, in particular between 22 and 30 ° C.
  • the culture is carried out aerobically, continuously and in a toxin-static mode: the formaldehyde concentration in the reactor is measured continuously and kept constant by regulating the inflow between an upper threshold value and a lower threshold value. This pollutant concentration requires a relatively high pollutant tolerance from the microorganisms.
  • Microbial formaldehyde degradation has the effect that the difference between the pollutant concentration of the waste water introduced into the system and the concentration in the outlet is very high is high is high.
  • the water flowing out of the reactor contains a residual concentration of formaldehyde, which is completely degraded microbially in a secondary clarifier
  • a large-scale fermenter is continuously fed with industrial wastewater from bakelite production, which contains formaldehyde in fluctuating concentrations between 8 g / 1 and 12 g / 1.
  • the wastewater contains phenol in a concentration of 40 g / 1 and various Other organic components
  • the media components specified above are added to the wastewater before the reactor is introduced.
  • the introduced formaldehyde and phenol-containing solution contains no viable microorganisms due to its high toxicity, but it is released as a lethal dose for safety reasons before UV radiation is introduced set
  • the reactor is inoculated with a mixed culture that contains the microorganisms DSM 11423, DSM 11424 and DSM 11425.
  • the degradation process is carried out as indicated above.
  • the formaldehyde concentration in the reactor is measured continuously and is kept constant by regulating the inflow between an upper threshold value and a lower threshold value. This pollutant concentration requires a relatively high tolerance to pollutants from the microorganisms.
  • the microbial formaldehyde degradation has the effect that the difference between the pollutant concentration of the waste water introduced into the system and the concentration in the outlet is very high. Simultaneous to formaldehyde degradation, microbiological phenol degradation takes place in the reactor.
  • the water flowing out of the reactor contains a residual concentration of formaldehyde and / or phenol, which is broken down microbially in a secondary clarifier Example 3:
  • Meat extract 3.0 g / pH 7.0
  • This culture serves as the seed culture for the following toxinostatic fermentation
  • a mixed culture under periodic ultraviolet radiation is optimized in a fermentation process carried out in a continuously toxinostatic manner.
  • the formaldehyde concentration set in the fermenter via a control loop is gradually increased during this period depending on the vitality of the overall culture.
  • the originally selected strains have a very high formaldehyde resistance of 500-6000 mg / l formaldehyde for naturally occurring microorganisms. During the fermentation, resistance and degradation rates of the original culture can be increased by a factor of 10 each
  • a production plant glues its products with formaldehyde- and phenol-containing adhesives.
  • the adhesive residues are collected and regularly transported to a central biological disposal facility.
  • the waste is biologically disposed of together with other liquid formaldehyde- and / or phenol-containing waste batches from different sources.
  • the waste stream supplied to the plant fluctuates very strongly due to the heterogeneity of the waste batches in relation to the formaldehyde and phenol concentration
  • the phenol index and the formaldehyde concentration are measured "on-line" and continuously in the bioreactor of the disposal system. If one of the two measurement parameters reaches the permissible upper limit concentration, the supply of pollutants into the reactor is stopped until the upper threshold value is again fallen below if the phenol index falls and / or the formaldehyde concentration to a fixed lower concentration value, this is raised again above the lower threshold value by increasing the flow rate or by additionally adding the respectively limited pollutant. In this way, despite charging the bioreactor with qualitatively very different wastewater batches degrading special culture can be stabilized
  • the formaldehyde-contaminated air in the vicinity of a production and processing facility must be cleaned in order to get below the permissible MAK values in the air.
  • the formaldehyde pollution in the air fluctuates
  • An air washer is used to clean the air, which removes the gaseous formaldehyde from the medium Air is transferred into the medium of water
  • the wash water contaminated with formaldehyde is finally fed to a toxinostatically regulated biological clarification stage, where the formaldehyde is biologically eliminated.
  • the washing water thus regenerated is then fed back to the air washer system in order to again take up formaldehyde from the air
  • Glutaraldehyde is used in the hospital area for cleaning and disinfecting work surfaces. Running washing water contaminated with glutaraldehyde is operated in a toxinostatic manner (the standard size is the glutaraldehyde concentration)
  • a floor contaminated with benzene is cleaned in a floor washing system.
  • the washing water contaminated with benzene is fed to a toxinostatically operated bioreactor (standard size is the benzene concentration). After the biological removal of a large part of the benzene in the washing water, it is used again for washing the floor
  • toxinostatically operated bioreactor standard size is the benzene concentration
  • a groundwater stream contaminated with various polyaromatic hydrocarbons is produced. This is conveyed to the surface via groundwater lances with the aid of suction pumps and fed to a biological clarification stage operated by toxins.
  • a sample stream is continuously withdrawn from the bioreactor and this is continuously analyzed for high-quality liquid chromatography (HPLC) coupled with fluorescence chromatography for quality and quantity of the various PAHs contained.
  • HPLC high-quality liquid chromatography
  • the PAK species which is most highly concentrated in the overall spectrum of PAHs is used at all times as the controlled variable of the toxinatic control.
  • Gram staining - Gram staining: - small round smooth medium-sized light colonies frayed colonies small coconut sticks chopsticks
  • API 20 NE
  • Arginine dihydrolase urease aesculin gelatin p-nitrophenyl- ⁇ -D-galactopyranoside. Assimilation tests glucose arabinose mannose mannitol

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  • Environmental & Geological Engineering (AREA)
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  • Purification Treatments By Anaerobic Or Anaerobic And Aerobic Bacteria Or Animals (AREA)
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Abstract

L'invention concerne un procédé permettant d'obtenir la décomposition microbienne de substances nuisibles contenues dans des milieux lors de la purification de l'air, des eaux usées et du nettoyage des sols. Elle concerne également un dispositif permettant la mise en oeuvre dudit procédé, des micro-organismes appropriés auxdits procédés et leur utilisation. L'objectif de l'invention est d'améliorer ledit procédé de façon à obtenir un établissement à long terme des cultures de micro-organismes utilisées pour décomposer les substances nuisibles, tout en parvenant à des taux élevés de décomposition. Pour atteindre cet objectif, il est proposé un procédé selon lequel une fermentation de décomposition continue se fait dans un fermenteur de décomposition au moyen de micro-organismes présents dans le milieu contenant les substances nuisibles et/ou d'une culture de micro-organismes ajoutée audit milieu. Pendant la fermentation de décomposition, la concentration de substances nuisibles dans le fermenteur de décomposition est régulée de façon à être toxistatique ou toxidynamique, au moyen d'un circuit de régulation, en fonction de la vitalité de la biomasse. Pour décomposer le formaldéhyde, il est proposé, selon l'invention, d'utiliser des micro-organismes particuliers qui le décompose. Pour décomposer les phénols, il est proposé, selon l'invention, d'utiliser des micro-organismes particuliers qui les décomposent.
PCT/EP1997/001017 1996-03-01 1997-02-28 Procede de decomposition microbienne de substances nuisibles contenues dans des milieux, et micro-organismes appropries a ce procede WO1997031682A1 (fr)

Priority Applications (2)

Application Number Priority Date Filing Date Title
EP97906145A EP0885032A1 (fr) 1996-03-01 1997-02-28 Procede de decomposition microbienne de substances nuisibles contenues dans des milieux, et micro-organismes appropries a ce procede
JP9530634A JP2000505341A (ja) 1996-03-01 1997-02-28 有害物質を含有する媒体中の有害物質を微生物により分解する方法及びそのために適した微生物

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Application Number Priority Date Filing Date Title
DE19607943.8 1996-03-01
DE19607943 1996-03-01

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WO1997031682A1 true WO1997031682A1 (fr) 1997-09-04

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JP (1) JP2000505341A (fr)
DE (1) DE19708181A1 (fr)
WO (1) WO1997031682A1 (fr)

Cited By (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP2239322A1 (fr) * 2009-04-07 2010-10-13 Basf Se Utilisation d'enzymes pour réduire le formaldéhyde dans des produits contenant du formaldéhyde
CN107158928A (zh) * 2017-06-05 2017-09-15 石河子开发区创客科技咨询服务有限责任公司 一种生物酶快除甲醛剂
CN108744946A (zh) * 2018-05-18 2018-11-06 朱文杰 一种生物酶甲醛清除剂的制备方法
CN112076604A (zh) * 2020-09-21 2020-12-15 嘉兴瓦格纳环保科技有限公司 一种除味除醛剂及其制备方法

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JP4679413B2 (ja) * 2006-03-31 2011-04-27 東洋エンジニアリング株式会社 炭化水素もしくは含酸素化合物の製造プラント廃水の高温処理方法
JP2019018118A (ja) * 2017-07-12 2019-02-07 三木理研工業株式会社 ホルムアルデヒド分解方法
CN107641199A (zh) * 2017-09-26 2018-01-30 广东绿净界新材料科技股份有限公司 一种聚氨基酸‑辅酶‑聚醚共聚物的制备方法

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Cited By (8)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP2239322A1 (fr) * 2009-04-07 2010-10-13 Basf Se Utilisation d'enzymes pour réduire le formaldéhyde dans des produits contenant du formaldéhyde
WO2010115797A1 (fr) * 2009-04-07 2010-10-14 Basf Se Utilisation d'enzymes pour réduire les aldéhydes contenus dans des produits contenant des aldéhydes
CN102459580A (zh) * 2009-04-07 2012-05-16 巴斯夫欧洲公司 酶减少来自含醛产品中醛的用途
CN102459580B (zh) * 2009-04-07 2015-04-29 巴斯夫欧洲公司 酶减少来自含醛产品中醛的用途
US9109200B2 (en) 2009-04-07 2015-08-18 Basf Se Use of enzymes to reduce aldehydes from aldehyde-containing products
CN107158928A (zh) * 2017-06-05 2017-09-15 石河子开发区创客科技咨询服务有限责任公司 一种生物酶快除甲醛剂
CN108744946A (zh) * 2018-05-18 2018-11-06 朱文杰 一种生物酶甲醛清除剂的制备方法
CN112076604A (zh) * 2020-09-21 2020-12-15 嘉兴瓦格纳环保科技有限公司 一种除味除醛剂及其制备方法

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DE19708181A1 (de) 1997-11-06
EP0885032A1 (fr) 1998-12-23

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