WO2019016837A1 - Appareil pour la réduction et la conversion de polluants gazeux atmosphériques comprenant un système couplé plasma/catalyseur ou plasma/adsorbant - Google Patents

Appareil pour la réduction et la conversion de polluants gazeux atmosphériques comprenant un système couplé plasma/catalyseur ou plasma/adsorbant Download PDF

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Publication number
WO2019016837A1
WO2019016837A1 PCT/IT2017/000151 IT2017000151W WO2019016837A1 WO 2019016837 A1 WO2019016837 A1 WO 2019016837A1 IT 2017000151 W IT2017000151 W IT 2017000151W WO 2019016837 A1 WO2019016837 A1 WO 2019016837A1
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Prior art keywords
plasma
abatement
vocs
catalyst
odours
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PCT/IT2017/000151
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English (en)
Inventor
Francesco Parisi
Katiuscia COSTABELLO
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Grinp S.R.L.
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Priority to EP17794090.5A priority Critical patent/EP3655135A1/fr
Priority to PCT/IT2017/000151 priority patent/WO2019016837A1/fr
Publication of WO2019016837A1 publication Critical patent/WO2019016837A1/fr

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    • 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
    • B01D53/32—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 by electrical effects other than those provided for in group B01D61/00
    • B01D53/323—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 by electrical effects other than those provided for in group B01D61/00 by electrostatic effects or by high-voltage electric fields
    • 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
    • B01D53/86—Catalytic processes
    • B01D53/8621—Removing nitrogen compounds
    • B01D53/8625—Nitrogen oxides
    • B01D53/8631—Processes characterised by a specific device
    • 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
    • B01D53/86—Catalytic processes
    • B01D53/8621—Removing nitrogen compounds
    • B01D53/8634—Ammonia
    • 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
    • B01D53/86—Catalytic processes
    • B01D53/864—Removing carbon monoxide or hydrocarbons
    • 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
    • B01D53/86—Catalytic processes
    • B01D53/8668—Removing organic compounds not provided for in B01D53/8603 - B01D53/8665
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2255/00—Catalysts
    • B01D2255/20—Metals or compounds thereof
    • B01D2255/204—Alkaline earth metals
    • B01D2255/2042—Barium
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2255/00—Catalysts
    • B01D2255/90—Physical characteristics of catalysts
    • B01D2255/91—NOx-storage component incorporated in the catalyst
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2257/00—Components to be removed
    • B01D2257/20—Halogens or halogen compounds
    • B01D2257/206—Organic halogen compounds
    • B01D2257/2066—Fluorine
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2257/00—Components to be removed
    • B01D2257/40—Nitrogen compounds
    • B01D2257/406—Ammonia
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2257/00—Components to be removed
    • B01D2257/50—Carbon oxides
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2257/00—Components to be removed
    • B01D2257/50—Carbon oxides
    • B01D2257/504—Carbon dioxide
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2257/00—Components to be removed
    • B01D2257/70—Organic compounds not provided for in groups B01D2257/00 - B01D2257/602
    • B01D2257/702—Hydrocarbons
    • B01D2257/7022—Aliphatic hydrocarbons
    • B01D2257/7025—Methane
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2257/00—Components to be removed
    • B01D2257/70—Organic compounds not provided for in groups B01D2257/00 - B01D2257/602
    • B01D2257/708—Volatile organic compounds V.O.C.'s
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2257/00—Components to be removed
    • B01D2257/90—Odorous compounds not provided for in groups B01D2257/00 - B01D2257/708
    • 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
    • Y02C—CAPTURE, STORAGE, SEQUESTRATION OR DISPOSAL OF GREENHOUSE GASES [GHG]
    • Y02C20/00—Capture or disposal of greenhouse gases
    • Y02C20/20—Capture or disposal of greenhouse gases of methane

Definitions

  • An apparatus for the abatement and conversion of atmospheric gaseous pollutants comprising a plasma/ catalyst or a plasma/ adsorbent coupled system
  • the present invention relates to the environment sector and, in particular, to the abatement of gaseous atmospheric pollutants such as nitrogen oxides (nitrogen monoxide NO and nitrogen dioxide NO 2 , denoted overall as nitrogen oxides NO x ), volatile organic compounds (VOCs), CO2, NH3, CH 4 and odours.
  • nitrogen oxides nitrogen monoxide NO and nitrogen dioxide NO 2 , denoted overall as nitrogen oxides NO x
  • VOCs volatile organic compounds
  • CO2 NH3, CH 4 and odours.
  • the present invention relates to an apparatus for the abatement at low temperature of gaseous atmospheric pollutants comprising a coupled plasma/ catalyst or plasma/ adsorbent system, integrated.
  • the present invention relates to an apparatus for the abatement and the conversion at low temperature of gaseous atmospheric pollutants comprising a coupled plasma/ catalyst or plasma/ adsorbent system with plasma at atmospheric pressure and heterogeneous adsorbent or catalyst.
  • the present invention also relates to a method for the abatement of volatile organic compounds (VOCs) by means of a coupled plasma/ catalyst system, integrated.
  • VOCs volatile organic compounds
  • the present invention also relates to a method for the abatement and the conversion of CO 2 into different types of chemical substances with high economic interest, such as for example dimethyl ether (DME), by means of a coupled plasma/ catalyst system, integrated.
  • DME dimethyl ether
  • the preferred and advantageous application of the present invention is for the abatement of NO x produced by mobile systems (for example in the combustion chamber of internal combustion engines) and by fixed systems (such as, for example, thermoelectric power plants and industrial plants).
  • the method according to the present invention does not entail the production of carbon dioxide (CO2) and, therefore, considerably reduces the environmental impact of gaseous effluent from mobile and fixed sources.
  • CO2 carbon dioxide
  • a further preferred and advantageous application of the present invention is the total conversion of VOCs into CO2 thanks to the action of the catalytic plasma and also thanks to the oxidizing action of the ozone produced by the lighting of the plasma in air and in the presence of oxygen.
  • a further preferred and advantageous application of the present invention is for the abatement of odours and the conversion into CO2 thanks to the action of the catalytic plasma and also thanks to the oxidizing action of the ozone produced by the lighting of the plasma in air and in the presence of oxygen.
  • a further preferred and advantageous application of the present invention is the abatement and the conversion of CO2 into useful and economically interesting substances such as dimethyl ether (DME) and others.
  • DME dimethyl ether
  • a further preferred and advantageous application of the present invention is the abatement and the conversion of CH 4 into useful and economically interesting substances such as dimethyl ether (DME) and others.
  • DME dimethyl ether
  • a further preferred and advantageous application of the present invention is the abatement and the conversion of NH3.
  • nitrogen protoxide N2O nitrogen monoxide NO
  • nitrogen dioxide NO2 dinotrogen trioxide N2O3
  • dinitrogen pentoxide N2O5 nitrogen protoxide N2O
  • N2O, NO and NO2 are naturally present in the atmosphere yet, while the nitrogen protoxide N2O is relatively inert, nitrogen monoxide NO and nitrogen dioxide NO2 are highly toxic and make an important contribution to many environmental problems such as the formation of smog and acid rain, the destruction of the ozone layer and the greenhouse effect.
  • Nitrogen monoxide NO and nitrogen dioxide NO2 are emitted into the atmosphere mainly from anthropogenic sources, in particular the production of NO x by humans takes place from fixed systems (for example thermoelectric power plants and industrial systems) and mobile systems (for example in the combustion chamber of internal combustion engines).
  • nitrogen oxides NO x are generated by processes of combustion, whatever the fuel used, through direct reaction between the nitrogen and the oxygen present in the air at high temperature (higher than 1,200°C).
  • the processes of combustion emit as main component nitrogen monoxide NO which subsequently, in the presence of ozone, is transformed into nitrogen dioxide NO2.
  • the direct formation of nitrogen dioxide NO2 by the combustion processes instead, is closely linked to the high values of pressure and temperature which occur inside the combustion chambers of engines.
  • Volatile organic compounds comprise a series of chemical compounds of organic nature in the form of vapour or in liquid form but able to evaporate easily at ambient pressure and temperature, which are therefore found in the atmosphere mainly in gaseous phase. They include hydrocarbons (compounds containing only carbon and oxygen such as aliphatic hydrocarbons, such as methane, aromatic hydrocarbons, such as benzene and halogenated hydrocarbons, such as chloroform) and also oxygenated species such as acids, alcohols, aldehydes (such as formaldehyde), ketones and esters.
  • hydrocarbons compounds containing only carbon and oxygen such as aliphatic hydrocarbons, such as methane, aromatic hydrocarbons, such as benzene and halogenated hydrocarbons, such as chloroform
  • oxygenated species such as acids, alcohols, aldehydes (such as formaldehyde), ketones and esters.
  • the natural emissions of the VOCs comprise the direct emission from vegetation and the degradation of organic material while anthropogenic emissions are mainly due to the incomplete combustion of hydrocarbons, to the evaporation of solvents and fuels and to processing industries.
  • VOCs aromatic organic compounds are found to be particularly damaging and which have direct effects on human health.
  • the most polluting species is benzene, relatively stable (average life span approximately four days) and with ascertained carcinogenic properties.
  • VOCs are also responsible for the formation of secondary pollutants.
  • class of alkenes is that of greatest interest in the atmospheric field due to their important role in the formation of oxidizing species.
  • This catalyst is constituted by platinum Pt and barium Ba (in oxide form) supported on gamma alumina ⁇ - AI2O3 with high surface area and is already active starting from 150°C, with maximum efficiency between 300 and 400°C.
  • the catalyst accumulates the NO x on the surface as barium nitrates Ba ( ⁇ 3)2 ⁇
  • a pulse of fuel is fed which acts as reducent and, thanks to the catalytic intervention of the platinum Pt, the NO x accumulated as nitrates are reduced to nitrogen N 2 .
  • the main disadvantage of this type of catalysts lies in the fact of entailing the waste of fuel for the recovery of the capacity of accumulation of the catalyst.
  • a further disadvantage is represented by the use of very costly noble metals.
  • a further disadvantage is due to the oxidizing working conditions, in that the presence of oxygen in the mixture leads to a smaller yield of the reaction of reduction and to a lower selectivity.
  • a further disadvantage is represented by the production of carbon dioxide CO2.
  • the catalysts according to the prior art described above are mainly limited by the fact of having to operate at temperatures higher than ambient temperature, of requiring the use of noble metals, of producing CO2 and of having in any case low efficiencies of conversion of the NO x into N 2 .
  • a gas rich in N0 2 has to arrive at the catalyst to increase the selectivity of the reduction reaction, it is important that the oxidization of NO into NO 2 is complete and, therefore, is conducted into a plasma reactor, specifically a traditional DBD - dielectric barrier discharge - apparatus, which operates in oxidizing conditions, specifically with an incoming flow rich in O 2 .
  • the solution described in this document provides for a successive reduction in NO2 which is performed with traditional techniques in which the catalyst works in the presence of hydrocarbons HC deriving from the fuel.
  • the catalyst is a fixed bed reactor constituted by gamma alumina on which a zeolite named Cu ZSM-5 is deposited.
  • the solution described in this document allows the achieving of a conversion of the NOx of approximately 70%.
  • a plasma reactor which works at 250°C.
  • the flow entering the reactor is a mixture of C3 ⁇ 4 and N 2 .
  • the plasma serves to act as catalyst to the reaction of reduction of the bimolecular nitrogen to NH3, which is the reducent used to complete the reaction of abatement/ conversion of the nitrogen oxides into N 2 .
  • the remaining part of the system is a normal catalytic converter of the SCR (selective catalytic reduction) type.
  • the plasma in this case is used to produce a reaction of oxide-reduction and is a secondary system with respect to that which is the main catalytic system of reduction of NO x , which contains a fairly important quantity of precious metal.
  • a mixed system of the solutions described in the two previous documents is that illustrated in the international application published under no. WO 2006/036311 A2.
  • This system is composed of a normal catalytic converter which works with an SCR catalyst, therefore with feeding of ammonia into the chamber of reduction of the nitrogen oxides with bimolecular nitrogen.
  • the plasma reactor is a quartz tube and the plasma is used as producer of ozone since, lit in air, the plasma acts as catalyst for the following reaction:
  • the ozone produced is a strongly reactive and oxidizing species and, fed into a reaction pre-chamber, serves to convert quantitatively the NO species into NO2 species, making the reduction reaction more efficient in terms of percentage conversion into bimolecular nitrogen.
  • the plasma is not used as reducent of the NO x but only as oxidizer and producer of ozone.
  • Regenerative converters are classic heat converters characterised by the recovery of the heat of the gas in output which, having an effective system of heat recovery, allow a more limited use of methane gas with lower running costs.
  • the problem in this case is however bound by the dimensioning of the system, which allows good conversions and low running costs only if the system is used at full load while, in the opposite case, the running costs of the plant, in terms of use of methane, are very high and serve to heat the gas to be treated.
  • the systems mentioned above provide however for a high production of carbon dioxide, gas obtained from the complete combustion of the various volatile organic molecules VOCs. At the present state of the art systems are not provided for capture and conversion of the CO2 downstream of the combusters.
  • the object of the present invention to simplify and make economically advantageous the abatement of NOx, and also of VOCs, odours, NH3, CO 2 and CH 4 .
  • These objectives are achieved with the apparatus according to the present invention which, advantageously integrating a catalytic plasma reactor at atmospheric pressure with catalyst integrated in the reactor and post-reactor catalyst of the heterogeneous type, allows the achieving of a very high efficiency of abatement of NO x , and also of VOCs, odours, NH3, CO2 and CH 4 , also in conditions of low temperature (for example 20°C).
  • the apparatus thanks to the innovative system which it implements, means that it is the plasma that acts as "super" catalyst of the reaction, in other words the plasma in this case implements both the principles of traditional catalysis and those of photocatalysis. On the one hand therefore it lowers the energy of activation of the reaction in such a way as to make it take place with good yields in the chosen conditions of temperature and pressure, on the other hand it supplies energy in the form of light, therefore providing the energy necessary for the reaction to take place.
  • Preferred embodiments and variants of the apparatus of abatement of nitrogen oxides NO x and/ or of volatile organic compounds VOCs, odours, NH3, CO 2 and CH according to the present invention constitute the object of the dependent claims. More particularly, in a first preferred and advantageous embodiment for the abatement of ⁇ and of CO ⁇ the apparatus according to the present invention provides for the use of a reducing plasma and of an adsorbent. More particularly, in a second preferred and advantageous embodiment for the abatement of VOCs and NH3 and odours and CH 4 , the apparatus according to the present invention provides for the use of an oxidizing plasma and of a catalyst.
  • Another aspect of the present invention relates to a method for the abatement of volatile organic compounds VOCs, odours, NH3, CO 2 and CH 4 by means of an integrated plasma at atmospheric pressure/ heterogeneous catalyst or atmospheric pressure plasma/ heterogeneous adsorbent system.
  • Another aspect of the present invention relates to a method for the abatement and the conversion of CO2 into different types of chemical substances with high economic interest, such as for example dimethyl ether (DME), by means of a coupled plasma/ catalyst, integrated system.
  • DME dimethyl ether
  • the apparatus according to the present invention thanks to its versatility and adaptability to the different types of pollutants and to odours, is suitable for being used in activities of the industrial type (producers of VOCs, painting processes, use of solvents), in energy production plants (incinerators, production of biogas), in agriculture (livestock farms) and in the transport sector (ships, heavy vehicles).
  • the apparatus according to the present invention in fact, it is possible to abate both the pollutants termed as climate change (O3, CO2, CH 4 , N 2 O) and those directly responsible for atmospheric pollution (VOCs, NO x , SO x , PM, NH3).
  • pollutants such as ⁇ and also VOCs, odours, NH3, CO2 and CH independently of the composition of the incoming gas, therefore also of the percentage of oxygen (in the case of the NO x ) or nitrogen (in the case of the VOCs) present;
  • Fig. 1 is a schematic representation of the first embodiment, for the abatement of NO x , of the apparatus according to the invention
  • Fig. 2 is a schematic representation of the first embodiment, for the abatement of NO x , of the apparatus according to the invention, in a first variant which provides an active carbons filter upstream of the same apparatus;
  • Fig. 3 is a schematic representation of the adsorbent used, for the abatement of NO x , of the apparatus according to the invention
  • Fig. 4A is a schematic representation of the first working phase of a second variant of the first embodiment, for the abatement of NO x , of the apparatus according to the invention
  • Fig.4B is a schematic representation of the second working phase of the second variant of the first embodiment, for the abatement of NO x , of the apparatus according to the invention
  • Fig. 4C is a graphic representation of the reducing gas in the two working phases of the apparatus of Figs. 4A and 4B;
  • Fig. 4D is a graphic representation of the plasma in the two working phases of the apparatus of Figs. 4A and 4B;
  • Fig. 5 is a schematic representation of the second embodiment, for the abatement of VOCS, of the apparatus according to the invention.
  • Fig. 6 is a schematic representation of the catalyst used, for the abatement of VOCS, of the apparatus according to the invention.
  • Fig. 7 is a schematic representation of the support media whereon the catalyst of the apparatus according to the invention is deposited;
  • Fig. 8A is a schematic representation of a first configuration of the plasma reactor of the apparatus according to the invention.
  • Fig. 8B is a schematic representation of a second configuration of the plasma reactor of the apparatus according to the invention.
  • Fig. 9 A is a schematic representation of a first type of plasma reactor of the apparatus according to the invention.
  • Fig. 9B is a schematic representation of a second type of plasma reactor of the apparatus according to the invention.
  • Fig. 10 is a schematic representation of the apparatus according to the invention fitted with cooling plate which allows efficient control of the temperature of the system.
  • the apparatus for the abatement of gaseous pollutants such as nitrogen oxides (NO x ) and volatile organic compounds (VOCs), odours, NH3, CO2 and CH 4 of the present invention is based on the innovative concept of abating pollutant compounds by means of the synergic action of plasma and catalyst, whether it is with oxidizing or reducing action according to the types of molecules to be treated.
  • This innovative system allows very high efficiency of abatement and conversion to be achieved, comprised between 97 and 99 %, of the NO x , of the VOCs and of other pollutants such as odours, NH3, CO2 and CH 4 .
  • the inventors have in fact surprisingly and unexpectedly discovered that the use of a plasma coupled with an appropriate catalyst is particularly effective in the abatement and in the conversion of many classes of atmospheric pollutants, such as nitrogen oxides (NOx), volatile organic compounds (VOCs), odours, NH3, CO 2 and CH 4 .
  • nitrogen oxides NOx
  • VOCs volatile organic compounds
  • odours NH3, CO 2 and CH 4 .
  • An important feature of this apparatus lies in the fact of being able to perform the abatement with efficacy, with high conversion, with reduced dimensions and with reduced running costs.
  • the apparatus can be provided with an innovative real-time adapting device which allows operation in optimal conditions both with continuous and discontinuous flow.
  • nitrogen oxides NO x is intended to indicate any mixture of nitrogen monoxide NO and nitrogen dioxide NO 2 in any ratio.
  • the terms “nitrogen oxides NO x " and “mixture of nitrogen monoxide NO and nitrogen dioxide NO 2 ", in the present description, are used indifferently, as synonyms.
  • volatile organic compounds VOCs is intended to indicate any mixture of volatile organic compounds which, at the temperature of 293.15 K (20°C), have a vapour pressure of 0.01 kPa or higher.
  • the term "odours” refers to one or more volatilised chemical compounds also at a very low concentration, which human beings or other animals perceive through the sense of smell.
  • adsorbent is intended to indicate an oxidic material formed by a metal or by a non-metal and by oxygen.
  • An adsorbent as defined here is used in a first embodiment of the invention, as will be described here below, for the abatement of NO x .
  • catalyst is intended to indicate an adsorbent on which a precious metal has been inserted.
  • a “catalyst” as defined here is used in a second embodiment of the invention, as will be described here below, for the abatement of VOCs.
  • heterogeneous adsorbent refers to an adsorbent in solid phase.
  • heterogeneous catalyst refers to a catalyst in solid phase.
  • the general configuration of the apparatus for the abatement of gaseous pollutants, such as nitrogen oxides NO / volatile organic compounds VOCs, odours, NH 3 , CO2 and CH 4 , of the present invention is that of a plasma reactor at atmospheric pressure integrated with a catalyst/ adsorbent. More specifically these are oxidizing systems in the case of the abatement of gaseous substances such as VOCs, CH 4 , particulate, dioxins, perfluorocarbons (PFC) and NH3 and reducing systems for the abatement of gaseous pollutants, such as nitrogen oxides NO / volatile organic compounds VOCs, odours, NH 3 , CO2 and CH 4 , of the present invention is that of a plasma reactor at atmospheric pressure integrated with a catalyst/ adsorbent. More specifically these are oxidizing systems in the case of the abatement of gaseous substances such as VOCs, CH 4 , particulate, dioxins, perfluorocarbons (PFC)
  • the oxidizing systems are able to catalyse the oxidation reaction of the pollutant substance by promoting the loss of atoms of hydrogen H and increasing the quantity of atoms of oxygen O and the presence of oxygen O 2 is necessary in the reaction mixture.
  • the reducing systems instead, are able to catalyse the reaction of oxidation of the pollutant substance by promoting the loss of atoms of oxygen O and increasing the quantity of atoms of hydrogen H.
  • the main part of the apparatus is represented by the plasma reactor, which is made up of two parts:
  • the actual plasma reactor which in turn is composed of different parts and is the zone in which the plasma is generated by means of an electrical discharge passing between two electrodes (cathode and anode), and
  • the materials used for the electrodes can be of different type, such as for example steel and/ or cordierite. Plastic materials resistant to high temperatures can also be used such as transparent or orange Kapton.
  • the plasma reactor is managed by a generator which is an integral part of the system.
  • the plasma generated by the generator can be of the continuous or pulsed type, SDBD (superficial dielectric barrier discharge) or VDBD (volume dielectric barrier discharge) on the basis of the geometry of the plates and of the reactor, which causes a different type of plasma.
  • the DBD plasma can in fact be generated in a volume (VDBD) or on a flat surface (SDBD).
  • VDBD the plasma is generated between two electrodes, for example between two parallel plates with dielectric in the middle; in the SDBD the micro-discharges are generated on the surface of a dielectric, which translates into a very homogeneous plasma.
  • the apparatus 1 comprises:
  • the support media 7 for the heterogeneous catalyst 5, to which reference will also be made as to cathodes, are placed inside the plasma reactor at atmospheric pressure 3 so as to form an integrated system 3,5,7.
  • Fig. 1 the type of apparatus illustrated in Fig. 1 is also suitable for the abatement of C0 2 and that therefore, in the present description, when reference is made to the apparatus for the abatement of NO x if necessary the abatement of C0 2 will also be understood to be included.
  • the apparatus 1 comprises a reactor 3 which uses a reducing plasma GR and an adsorbent 5.
  • the reducing plasma GR is chosen in the group comprising H 2 , He and Ar, and mixtures thereof.
  • the means 9 are preferably liquid heat exchangers.
  • the efficiency of abatement of the content of NO x and/ or CO2 is equal to or higher than 80%.
  • the apparatus 1' comprises:
  • - means 9' for maintaining the operating temperature at a value greater than 20°C, preferably between a minimum value of 20°C and a maximum value of 350°Q and
  • the support media 7' are similar to the support media 7 described in reference to Fig. 1.
  • the means 9' are preferably liquid heat exchangers.
  • the active carbons filter 11 is preferably a substance with high absorbing capacity, thanks to its porosity, most of the organic substances and on the consequent possibility of extracting them using a "vehicle” which is generally vapour.
  • the selective active carbons filter for the oxygen 11 operates so as to eliminate most thereof and have a reaction chamber in which the plasma can work in conditions of excess reducent. In this way collateral reactions, able to originate undesired and potentially damaging chemical species, are avoided.
  • the efficiency of abatement of the content of NO x and/ or CO 2 is equal to or higher than 90%.
  • the structure is noted of the biphasic adsorbent 5;5' used in the first embodiment for the abatement of NO x and/ or CO 2 , which is formed by an inert support medium X, X', chosen in the group comprising oxides and metals, and by an adsorbent Y;Y', chosen in the group of the oxides of alkaline and alkaline earth metals.
  • the inert support medium comprises a porous oxide X;X' and an oxide in nanometric form ⁇ , ⁇ '; preferably the porous oxide X;X' is alumina, aluminium oxide and/ or silicon oxide and the oxide in nanometric form ⁇ , ⁇ ' is barium oxide, an oxide with particular affinity to the nitrogen oxides. This oxide forms with the nitrogen oxide an ionic bond giving rise to nitrate ions with negative charge.
  • the greater the surface area of the adsorbent the greater the number of nitrate ions formed and the greater the efficiency of the system will be and there will be therefore a greater conversion of the reactor in percentage points (%) per unit of time.
  • the biphasic adsorbent 5;5' is deposited on the support media 7;7'.
  • a so-called heterogeneous catalyst/ adsorbent is used, in that it is not in the same phase (solid, liquid or gaseous) in which the reagents are present.
  • the heterogeneous catalyst/ adsorbent is in general formed by different elements.
  • a support medium generally inert, having high surface area and good thermal and mechanical stability
  • the actual catalyst is deposited, whether mono or biphasic, and optionally compounds for preventing the sintering thereof, as well as optional promoters (substances which act in a particular way, improving or modulating the catalytic performance).
  • the particles of heterogeneous catalyst/ adsorbent selected have in general a porous structure, therefore catalysis takes place both on the outer surface of the catalyst and on the inner one. This means that the surface available for the exchange of material is of different orders of greater magnitude with respect to that which would be obtained if the structure of the heterogeneous catalyst were compact (high surface area). Since the inner surface of a heterogeneous catalyst is much more extended than its outer surface, at the stage of design of the apparatus account has to be taken of the transport of material inside the pores of the catalyst.
  • adsorbent 5;5' used in the first embodiment, for the abatement of NO x , and/ or of C02 is constituted by three different phases:
  • a ceramic substrate (aluminium oxide, cerium oxide, silicon oxide, zinc, nickel oxide, magnesium oxide or mixed oxide of these) having high area.
  • structured oxides are also used with porosity of different diameter (from micro to nano) so as to have a further increase in the surface area; these materials are called micro or mesoporous according to the dimension of the pores.
  • a precious metal Au, Pt, Pa, Rh, Fe, Ar, Ru
  • Au precious metal
  • the metal is not however necessary in all the embodiments of the present invention (mention is made in fact of catalyst if this is constituted also by nanoparticles of metal, precious and appropriately dispersed, and supported on mixed oxides.
  • the nanoparticles used are different according to the type of application required and of the type of reaction which is to be produced. The use of nanoparticles of precious metal greatly increases, obviously, the cost of the catalyst).
  • FIG.4A and 4B a second variant of the first embodiment of the apparatus according to the invention is illustrated, which comprises:
  • - means 9,9' are preferably liquid heat exchangers.
  • the two integrated systems 3a,5a,7a;3'a,5'a,7'a and 3b,5b,7b;3'b,5'b,7'b operate in an alternate manner one in relation to the other thanks to the action of the switch 13, for example the first integrated system 3a,5a,7a;3'a,5'a,7'a operates with plasma unlit and the second integrated system b,5b,7b;?)'b,5'b,7'b operates with plasma lit (as can be seen in Fig.
  • the first integrated system 3a,5a,7a;3' 'a,5' 'a,7 'a operates with plasma lit
  • the second integrated system 3b,5b,7b;3'b,5'b,7'b operates with plasma unlit (as can be seen in Fig. 4B).
  • Fig. 4A represents the first operative phase in which, as mentioned previously, the first integrated system 3a,5a,7a;3'a,5'a,7'a operates with plasma unlit and the second integrated system 3b,5b,7b ⁇ 3'b,5'b r 7'b operates with plasma lit
  • Fig.4B represents the second operative phase in which, as mentioned previously, the first integrated system 3a,5a,7a;3'a,5'a,7'a operates with plasma lit and the second integrated system 3b,5b,7b;3'b,5'b,7'b operates with plasma unlit.
  • the flow of gas is conveyed into the first integrated system 3a,5a,7a ⁇ 3' a,5' a,7' a wherein the plasma P is unlit and the flow of reducing gas GR is absent.
  • the molecules of NO x are adsorbed on the surface of the barium oxide, creating NO 3- species.
  • the plasma P is lit and the reducing gas GR is present.
  • the energy supplied by the plasma is used to reduce the NO 3 ⁇ species adsorbed previously according to the conversion reaction (reduction):
  • the second integrated system 3b,5b,7b 3'b,5'b,7'b is open and the reduced gas can exit the reactor.
  • the flow of gas is conveyed now into the second integrated system 3b,5b,7b;3'b,5'b,7'b, which is now closed, and the pollutant gas is adsorbed by the adsorbent material.
  • the reaction of reduction takes place in the first integrated system 3a,5a,7a;3'a,5'a,7'a by the plasma P and the reducing gas GR.
  • the two integrated systems therefore work in an alternate manner with plasma unlit and plasma lit respectively in storage or reduction mode.
  • the apparatus 1;1' constituted by a system with two stages which work in an alternate manner, as illustrated in Figs. 4A and 4B, has the specific advantage of working with good conversions of NOx and in low temperature conditions.
  • the corresponding graphic representations of the reducing gas GR and of the plasma P in the two working phases of the apparatus of Figs. 4A and 4B show that, in the two-stage system, the reactor works in plasma conditions of pulsed type, with moments wherein the plasma P is lit - in ON phase - and moments in which the plasma P is unlit - in OFF phase.
  • the reducing gas GR is inserted in the reaction chamber while the flow of reducing gas GR is blocked when the plasma P is unlit.
  • the apparatus 1" according to the invention comprises:
  • the support media 7" are similar to the support media 7 described in reference to Fig. 1.
  • the apparatus 1" comprises a reactor 3" which uses an oxidizing plasma GO and a catalyst 5".
  • the oxidizing plasma GO is chosen in the group comprising He or Ar with O2, and mixtures thereof.
  • the means 9" are preferably liquid heat exchangers.
  • the efficiency of abatement of the content of VOCs and/or odours is equal to or higher than 97%.
  • the conversion is equal to or higher than 32%.
  • the conversion is higher than 98%.
  • the conversion is higher than 99%.
  • Fig. 5 illustrates, more specifically, a variant of the second embodiment which also comprises, downstream of the integrated system 3",5",7", an additional stage 15 in which the ozone O3 produced in the integrated system 3", 5", 7" acts as promoter for the total conversion of the residual volatile organic compounds (VOCs) into CO2, thus further incrementing the efficiency of the apparatus.
  • VOCs residual volatile organic compounds
  • the structure is noted of the biphasic catalyst 5" used in the second embodiment for the abatement of VOCs and/ or of CH 4 and/ or of odours and/ or of NH 3/ which is formed by an inert support medium X", chosen in the group comprising oxides and metals, and by a catalyst Z", chosen in the group of precious metals.
  • the inert support medium X" is preferably aluminium oxide (gamma alumina) structured with porous base.
  • the catalyst Z" is preferably manganese oxide MnO in nanopowder form.
  • a catalyst of metal type such as gold Au is also deposited in the form of nanopowder on the biphasic system which has been created.
  • the biphasic catalyst 5" is deposited on the support media 7".
  • FIG. 7 a schematic representation is seen of the support media 7;7';7" whereon the adsorbent/ the catalyst 5;5';5" of the apparatus according to the invention is deposited.
  • the adsorbent or catalytic material 5;5';5" in the form of nanometric powder is deposited directly on the support media creating a more or less uniform layer on their surface.
  • the plurality of support media 7;7';7" are flat plates.
  • the support media 7;7';7" can be undulated plates (which have a greater surface area with respect to the flat plates) or fibres, metal or glass, or again beds of ceramic material or glass.
  • the support media 7;7';7" are metal, since they have a greater stability to thermal, chemical and mechanical stresses. These support media are resistant, lightweight, not bulky and capable of large exchange surfaces.
  • ceramic support media 7;7';7" the chosen structure is the honeycomb one and covered in all its points by a porous substance, a mixture of refractory oxides appropriately mixed one with the other, impregnated with precious metals.
  • the degree of dispersion of the noble metal defines the performance of the catalyst: the more it is dispersed, the higher the performance will be.
  • the catalyst 5;5';5" is deposited on the ceramic support media 7;7';7" by means of impregnation, that is to say by means of an operation apt to deposit on the porous ceramic support medium the metal active in the catalysis in the most dispersed form possible.
  • the active metal is typically an element of the group of platinoids but can also be not noble, such as iron or cobalt.
  • each type of catalysis requires a special specific support medium-metal combination.
  • a chemically modified photocatalytic material with oxidizing action is deposited with self-cleaning function of the apparatus 1;1';1".
  • the photocatalytic material is titanium oxide modified with Fe and
  • the apparatus 1; ⁇ ;1" is able to treat different pollutants also present simultaneously in the incoming flow, thus resulting in a multi-pollutant apparatus.
  • This feature is conferred to the apparatus 1;1';1" using appropriate catalysts according to the type of reaction to bring about, whether reducing or oxidizing.
  • the apparatus (1;1';1" comprises also a plug-and-play device so that it is easy to install and to use.
  • the apparatus 1; ;1" also comprises a smart online probe integrated in the same apparatus so as to allow the latter to function in real-time adapting conditions, i.e. adapting the conditions of treatment on the basis of the values of output pollutant gases values.
  • Fig. 8A shows a first configuration of plasma reactor 3i;3i';3i" of the apparatus 1;1';1" according to the invention.
  • plates of different material metal or plastic
  • the electrical current is carried through the cathodes themselves and a passage of voltage is created as illustrated in the drawing.
  • the plasma is lit in a volume and is called VDBD.
  • Fig. 8B shows a second configuration of plasma reactor Sifiifii' of the apparatus 1;1';1" according to the invention.
  • plates of metal material are present constituted by small undulations in sheet meal with different structures.
  • the sheet metal can have thickness varying between 0.02 and 0.2 mm according to the surface area required for the specific application.
  • the drawing shows in detail the zone in which the passage of voltage is created.
  • the plasma is lit only on the surface on the plate and is called SDBD.
  • Fig. 9 A shows a first type of plasma reactor 33;33';33" of the apparatus 1; ; ' according to the invention.
  • This first type provides a quartz tube, connected to earth, in which an electrode is inserted which conducts the high voltage and generates the plasma and the reactor is filled with ceramic or glass spheres (beads) whereon the necessary catalyst is deposited.
  • Fig. 9B shows a second type of plasma reactor 34;34';3 4 " of the apparatus 1;1';1" according to the invention.
  • This second type also provides a quartz tube, connected to earth, in which an electrode is inserted which conducts the high voltage and generates the plasma and, in this case, the reactor is filled with metal fibres whereon the necessary catalyst is deposited.
  • the adhesion of the catalyst nanoparticles on the different types of support medium is made optimal via different types of surface treatment.
  • affinity with the catalytic material such as passivation or electrodeposition of ceramic material by means of which a layer of oxide is created on the metal with affinity through composition with the ceramic material to be deposited.
  • the apparatus 1;1';1" is provided with a cooling or heating plate 17, in whose interior a cooling or heating fluid 17 flows, which allows an efficient control of the temperature of the system.
  • the present invention provides a method for the abatement of volatile organic compounds VOCs and/ or CH 4 and/ or odours and/ or NHb, comprising the steps of:
  • an apparatus 1" comprising a reactor 3" which uses an oxidizing plasma GO and a heterogeneous catalyst 5" according to what is described previously in relation to the treatment of volatile organic compounds VOCs and/or CH 4 and/ or odours and/ or NH3 ⁇ 4
  • the oxidizing plasma GO is chosen in the group comprising He or Ar with O 2 , and mixtures thereof.
  • the efficiency of abatement of the content of volatile organic compounds VOCs and/ or CH 4 and/ or odours and/ or NH3, is equal to or higher than 97% .
  • the present invention provides a method for the abatement and the conversion of CO2, comprising the steps of:
  • an apparatus 1;1' comprising a reactor 3;3' which uses a reducing plasma GR and a heterogeneous catalyst 5;5' according to what is described previously in relation to the treatment of NO x and/ or C02;
  • the efficiency of abatement of CO2 is equal to or higher than 50%.
  • the apparatus according to the present invention can be used as plasma chamber in a method of abatement of nitrogen oxides NO x studied by the same Applicant, which forms the object of a separate yet simultaneous Italian patent application entitled "Method of abatement of NO x by means of a coupled plasma/ adsorbent system".
  • the abatement is very selective and economically advantageous of polluting substances such as VOCs independently of the composition of the incoming gas, therefore also of the percentage of nitrogen present.
  • the abatement is very selective and economically advantageous of polluting substances such as NOx independently of the composition of the incoming gas, therefore also of the percentage of nitrogen present.
  • Example 1 abatement of NO x present in the gaseous effluent of a thermoelectric power plant or an industrial plant
  • An important aspect of the present invention relates to the application of the method with gaseous mixture containing nitrogen oxides NOx coming from a fixed system, for example a thermoelectric power plant or an industrial plant.
  • a mixture comprises nitrogen monoxide NO and nitrogen dioxide NO 2 .
  • thermoelectric power plant or of an industrial plant
  • innovative technical solution described here in reducing configuration has the following advantageous features:
  • Example 2 abatement of VOCs in a painting plant
  • VOC type of pollutant in the gas correlated to the composition of the painting used in the painting booth.
  • Typical examples are painting booths for cars, for the body or for the bumpers.
  • the abatement is very selective and economically advantageous of polluting substances such as VOCs independently of the composition of the incoming gas, therefore also of the percentage of nitrogen present.
  • Example 3 abatement of NH3 on brake pads firing system
  • the abatement is very selective and economically advantageous of polluting substances such as NOx independently of the composition of the incoming gas, therefore also of the percentage of nitrogen present.

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Abstract

L'invention concerne un appareil pour la réduction à basse température de polluants atmosphériques gazeux, tels que des oxydes d'azote (NOx), des composés organiques volatils (COV), NH3, CO2, CH4 et les odeurs, comprenant un système couplé plasma/catalyseur intégré, c'est-à-dire qui constitue une seule phase de travail, le plasma étant un plasma à pression atmosphérique et le catalyseur étant hétérogène. Plus particulièrement, l'appareil selon la présente invention concerne l'utilisation d'un plasma réducteur et d'un adsorbant pour la réduction de NOx et l'utilisation d'un plasma oxydant et d'un catalyseur pour la réduction des COV. L'invention concerne également un procédé de réduction de composés organiques volatils (COV) au moyen d'un système couplé plasma/catalyseur intégré. L'invention concerne également un procédé de réduction et de conversion de CO2 en différents types de substances chimiques avec un intérêt économique élevé, tel que par exemple l'oxyde de diméthyle, au moyen d'un système couplé plasma/catalyseur intégré.
PCT/IT2017/000151 2017-07-21 2017-07-21 Appareil pour la réduction et la conversion de polluants gazeux atmosphériques comprenant un système couplé plasma/catalyseur ou plasma/adsorbant WO2019016837A1 (fr)

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PCT/IT2017/000151 WO2019016837A1 (fr) 2017-07-21 2017-07-21 Appareil pour la réduction et la conversion de polluants gazeux atmosphériques comprenant un système couplé plasma/catalyseur ou plasma/adsorbant

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CN112316941A (zh) * 2020-09-30 2021-02-05 光大环境修复(江苏)有限公司 一种用于氮氧化物和挥发性有机化合物协同净化的双功能催化剂及其制备方法
CN113198317A (zh) * 2021-04-22 2021-08-03 上海玉朗科技有限公司 一种电线电缆阻燃性能测试废气治理系统
CN113975946A (zh) * 2021-10-29 2022-01-28 重庆邮电大学 一种等离子体与光催化剂协同转化二氧化碳的方法
CN114653173A (zh) * 2022-03-28 2022-06-24 南京工业大学 一种应用于co2加氢的等离子体耦合光催化装置
CN117339356A (zh) * 2023-11-20 2024-01-05 安徽申兰华色材股份有限公司 一种铜酞菁合成尾气治理方法及系统

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