WO2021062908A1 - Procédé et dispositif d'élimination de polluants gazeux par oxydation catalytique électro-fenton - Google Patents

Procédé et dispositif d'élimination de polluants gazeux par oxydation catalytique électro-fenton Download PDF

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WO2021062908A1
WO2021062908A1 PCT/CN2019/113912 CN2019113912W WO2021062908A1 WO 2021062908 A1 WO2021062908 A1 WO 2021062908A1 CN 2019113912 W CN2019113912 W CN 2019113912W WO 2021062908 A1 WO2021062908 A1 WO 2021062908A1
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electrode
cathode
gaseous pollutants
electro
anode
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PCT/CN2019/113912
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English (en)
Chinese (zh)
Inventor
张礼知
艾智慧
贾法龙
严义清
严方升
李普煊
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华中师范大学
深圳市普瑞美泰环保科技有限公司
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Publication of WO2021062908A1 publication Critical patent/WO2021062908A1/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
    • B01D53/34—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
    • B01D53/8678—Removing components of undefined structure
    • 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
    • B01D53/92—Chemical or biological purification of waste gases of engine exhaust gases
    • B01D53/94—Chemical or biological purification of waste gases of engine exhaust gases by catalytic processes
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2259/00—Type of treatment
    • B01D2259/80—Employing electric, magnetic, electromagnetic or wave energy, or particle radiation

Definitions

  • the application relates to the technical field of gaseous pollutants, and in particular to a method and device for removing gaseous pollutants by electro-Fenton catalytic oxidation.
  • the gaseous pollutants in the air mainly come from human activities (industrial production, coal burning, motor vehicle exhaust, etc.) and natural process emissions. They are toxic, carcinogenic and malodorous. At the same time, they are produced by photochemical reactions to produce secondary aerosols and ozone.
  • the methods for removing gaseous pollutants mainly include physical adsorption, ozone oxidation, photocatalysis, thermal catalytic oxidation, and plasma methods.
  • these removal methods generally have problems such as high energy consumption, potential safety hazards, and secondary pollution. The scope of application restricted.
  • the main purpose of this application is to provide a method and device for removing gaseous pollutants by electro-Fenton catalytic oxidation, which aims to effectively remove gaseous pollutants and has a wide range of applications.
  • the device for removing gaseous pollutants proposed in this application includes an electrochemical reactor, which includes a power source, an anode, a cathode, a proton exchange membrane, an anode gas flow channel, and a cathode gas flow channel.
  • the exchange membrane is arranged between the anode and the cathode, the anode is arranged in the anode air flow channel, the cathode is arranged in the cathode air flow channel, and the cathode is a porous conductive supporting electro Fenton catalyst Adsorption material electrode.
  • the active component of the electro-Fenton catalyst is at least one of iron, cobalt, nickel, manganese, and cerium oxides, hydroxides, and alloys thereof.
  • the active component of the electro-Fenton catalyst is at least one of a complex of polyphosphoric acid and iron ions, lithium iron phosphate, and a metal organic framework material.
  • the porous conductive adsorption material electrode is one of activated carbon fiber, graphene, carbon nanotube, and nitrogen-doped graphene.
  • the loading range of the electro Fenton catalyst is 0.1%-50%.
  • the anode is at least one of a graphite electrode, a metal electrode, a metal alloy electrode, and a metal oxide electrode.
  • the metal electrode is at least one of a tin electrode, a chromium electrode, a nickel electrode, a manganese electrode, a ruthenium electrode, an iridium electrode, an iron electrode, a rhodium electrode, a palladium electrode, a platinum electrode, a lead electrode, and a tantalum electrode.
  • electrochemical reactors there are multiple electrochemical reactors, and multiple electrochemical reactors are arranged in parallel or in series.
  • a plurality of the electrochemical reactors are provided, and a plurality of the electrochemical reactors are arranged in parallel, and the opposite electrodes of the two adjacent electrochemical reactors are located in the same air flow channel, and are located in the same air flow channel
  • the two electrodes have the same polarity; and/or, the electrochemical reactor is provided with a plurality of the electrochemical reactors are arranged in series, and the opposite electrodes of the two adjacent electrochemical reactors are located in the same gas flow
  • the two electrodes in the channel and located in the same air flow channel have the same polarity.
  • This application also proposes a method for removing gaseous pollutants, which is applied to the device for removing gaseous pollutants as described above, and the method for removing gaseous pollutants includes the following steps:
  • the concentration of gaseous pollutants at the outlet of the cathode gas flow channel is monitored respectively.
  • the cathode adopts a porous conductive adsorption material electrode loaded with an electric Fenton catalyst
  • oxygen can be reduced to hydrogen peroxide.
  • the hydrogen peroxide reacts with the catalyst to generate active species such as hydroxyl radicals and hydroxyl radicals through the Fenton reaction.
  • Active species react with gaseous pollutants to achieve their effective removal.
  • the electro-Fenton catalyst has higher activity and better stability, which helps to improve the removal rate of pollutants.
  • the catalyst can efficiently catalyze and decompose a variety of gaseous pollutants, and has a wide range of applications.
  • Fig. 1 is a schematic structural diagram of an embodiment of a device for removing gaseous pollutants according to the present application
  • FIG. 2 is a schematic structural diagram of another embodiment of the device for removing gaseous pollutants according to the present application.
  • FIG. 3 is a schematic diagram of the degradation rate of benzene pollutants under different voltages in the method for removing gaseous pollutants in this application;
  • FIG. 4 is a schematic diagram of the degradation rate of benzene pollutants at a voltage of 2.2V in the method for removing gaseous pollutants according to the present application, as a function of electrolysis time;
  • Figure 5 shows the degradation rate of benzene with different carbon material electrodes as the cathode matrix under 2.3V voltage
  • Figure 6 shows the total flow rate at which benzene degradation rate reaches 90% at 2.3V voltage with different carbon material electrodes as the cathode matrix
  • Figure 7 shows the degradation rate of benzene pollutants with different electric Fenton catalysts as cathodes at a voltage of 2.2V;
  • Figure 8 shows the degradation rate of benzene pollutants with different electric Fenton catalysts as cathodes at a voltage of 2.2V;
  • Figure 9 shows the degradation rate of benzene pollutants for different anode materials at a voltage of 2.2V
  • Figure 10 shows the applied voltage when the degradation rate of different gaseous pollutants reaches 95%.
  • Attached icon number description Label name Label name 100 Electrochemical reactor 30 Anode gas flow channel 10 anode 40 Cathode airflow channel 20 cathode 50 Proton exchange membrane
  • This application proposes a device for removing gaseous pollutants, which is used to remove gaseous pollutants.
  • the device for removing gaseous pollutants includes an electrochemical reactor 100.
  • the electrochemical reactor 100 includes a power supply, an anode 10, a cathode 20, and a proton exchange membrane 50.
  • the anode air flow channel 30 and the cathode air flow channel 40, the proton exchange membrane 50 is arranged between the anode 10 and the cathode 20, the anode 10 is arranged in the anode air flow channel 30, the cathode 20 is arranged in the cathode air flow channel 40, and the cathode 20 is the load power Porous conductive adsorption material electrode of Fenton catalyst.
  • the power supply here is a DC power supply
  • the cathode 20 uses a carbon material electrode loaded with an electric Fenton catalyst
  • a proton exchange membrane 50 is placed between the cathode 20 and the anode 10
  • the three layers of materials of the anode 10 are clamped
  • the surface of the anode 10 is provided with an anode air flow channel 30, and the surface of the cathode 20 is provided with a cathode air channel 40
  • the anode 10 and the cathode 20 are respectively connected to the positive and negative electrodes of the DC power supply through wires to obtain gaseous pollutant removal Device.
  • the cathode 20 adopts the active components of the supported electric Fenton catalyst, the gaseous pollutants can be fully electrically Fentonized, that is, under the action of direct current, the oxygen is electrochemically reduced on the cathode 20 to generate hydrogen peroxide, and the hydrogen peroxide is further combined with the load.
  • the Fenton catalyst on the surface of the cathode 20 generates hydroxyl radical active species, which then oxidize and remove the gaseous pollutants, and kill pathogenic bacteria and inactivate viruses.
  • the carbon material electrode is used here.
  • the carbon material has a relatively high specific surface area. During the gas phase electro-Fenton reaction, it can effectively adsorb pollutants on its surface and oxidize and degrade; the carbon material has good physical and chemical properties, which can be used in electrochemical reactions. relatively stable.
  • porous conductive adsorbent material may be a porous carbon material or other porous conductive adsorbent materials, all of which fall within the protection scope of the present application.
  • the cathode 20 adopts a carbon material electrode supporting an electric Fenton catalyst, it can reduce oxygen to hydrogen peroxide, and the hydrogen peroxide and the iron-containing catalyst generate hydroxyl radicals through the Fenton reaction. Active species such as hydroxyl radicals and other reactive species react with gaseous pollutants to achieve effective removal.
  • the electro-Fenton catalyst has higher activity and better stability, which helps to improve the removal rate of pollutants.
  • the catalyst can efficiently catalyze and decompose a variety of gaseous pollutants, and has a wide range of applications.
  • the device for removing gaseous pollutants also includes transportation equipment and transportation pipelines.
  • the transportation pipeline communicates with the anode air flow channel 30, and the transportation pipeline communicates with the cathode air flow channel 40.
  • the transportation pipelines are equipped with transportation equipment and transportation equipment. It is a fan, air pump, or water pump.
  • the active component of the electro-Fenton catalyst is at least one of iron, cobalt, nickel, manganese, and cerium oxides, hydroxides, and alloys thereof. Iron, cobalt, nickel, manganese, and cerium oxides, hydroxides and their alloys can all be used as active components of the electro-Fenton catalyst, and one or more of them can be used in combination.
  • the active component of the electro-Fenton catalyst is at least one of a complex of polyphosphoric acid and iron ions, lithium iron phosphate, and a metal organic framework material.
  • Complexes of polyphosphoric acid and iron ions, lithium iron phosphate and metal organic framework materials can also be used as Fenton catalysts, and one or more of them can also be used in combination.
  • the porous conductive adsorption material electrode is one of activated carbon fiber, graphene, carbon nanotube, and nitrogen-doped graphene.
  • activated carbon fiber graphene, carbon nanotube, and nitrogen-doped graphene.
  • the loading range of the electro-Fenton catalyst is 0.1%-50%.
  • the loading of electro-Fenton catalyst is 0.1%, 1%, 10%, 20%, 40% or 50%.
  • the load is 1%-5%, such as 1%, 2%, 3%, 4%, or 5%.
  • the anode 10 is at least one of a graphite electrode, a metal electrode, a metal alloy electrode, and a metal oxide electrode.
  • the metal electrode is at least one of a tin electrode, a chromium electrode, a nickel electrode, a manganese electrode, a ruthenium electrode, an iridium electrode, an iron electrode, a rhodium electrode, a palladium electrode, a platinum electrode, a lead electrode, and a tantalum electrode.
  • a tin electrode a chromium electrode, a nickel electrode, a manganese electrode, a ruthenium electrode, an iridium electrode, an iron electrode, a rhodium electrode, a palladium electrode, a platinum electrode, a lead electrode, and a tantalum electrode.
  • the metal alloys can be alloys of tin, chromium, nickel, manganese, ruthenium, iridium, iron, rhodium, palladium, platinum, lead, and tantalum, and the metal oxides can also be oxides of these metals.
  • multiple electrochemical reactors 100 are provided, and multiple electrochemical reactors 100 are provided in parallel. It is understandable that multiple electrochemical reactors 100 are arranged in parallel here, and two adjacent electrochemical reactors 100 are arranged separately, so that multiple electrochemical reactors 100 can be used to degrade gaseous pollutants at the same time. Increase the gas processing volume per unit time and improve its removal efficiency. It should be noted that the polarities of the opposite electrodes of the two adjacent electrochemical reactors 100 can be the same or opposite, which is not limited here. That is, the opposite electrodes of two adjacent electrochemical reactors 100 can be the same as the cathode 20 and the same as the anode 10, or one is the cathode 20 and the other is the anode 10.
  • multiple electrochemical reactors 100 are provided, and multiple electrochemical reactors 100 are provided in series.
  • the multiple electrochemical reactors 100 are arranged in series, so that the air containing pollutants passes through the multiple electrochemical reactors 100 in sequence, and finally the pollutants are completely removed.
  • the polarities of the opposite electrodes of two adjacent electrochemical reactors 100 can be the same or opposite, which is not limited here.
  • multiple electrochemical reactors 100 are provided, and multiple electrochemical reactors 100 are provided in parallel, and the opposite electrodes of two adjacent electrochemical reactors 100 are located in the same gas flow channel
  • the two electrodes located in the same air flow channel have the same polarity.
  • a plurality of electrochemical reactors 100 are provided, and a plurality of the electrochemical reactors 100 are arranged in series, and the opposite electrodes of two adjacent electrochemical reactors 100 are located in the same gas flow channel , And the two electrodes located in the same air flow channel have the same polarity.
  • such an arrangement can also relatively reduce the occupied size of the overall device, and greatly improve the space utilization of the device.
  • This application also proposes a method for removing gaseous pollutants, which is applied to the device for removing gaseous pollutants as described above, and the method for removing gaseous pollutants includes the following steps:
  • the DC voltage range is preferably 2V-5V, for example, the applied voltage is 2V, 3V, 4V or 5V.
  • the gaseous pollutants are fully electro-Fenton oxidized, so that the removal efficiency of the gaseous pollutants is optimized.
  • the water is electrolyzed at the anode 10 to generate oxygen, which is released into the air and can be recycled to the cathode 20 area for use, so that the recycling of resources can be realized.
  • the air containing gaseous pollutants is continuously passed into the anode airflow channel 30 and the cathode airflow channel 40 here.
  • an instrument is used to detect the concentration of gaseous pollutants at the gas outlets of the anode gas flow channel 30 and the cathode gas flow channel 40.
  • it can also be used to detect the pollution of gaseous pollutants in the air treated by the device.
  • the method for removing gaseous pollutants using the electrochemical reaction device of step (2) includes the following steps: passing benzene-containing gas into the cathode airflow channel, the concentration of organic pollutant benzene is 10ppm, and air is used as the balance gas.
  • the total flow rate is 20mL/min.
  • the water is continuously introduced into the anode gas flow channel through the water pump, and the flow rate is 10 mL/min. Then apply a DC voltage between the cathode and the anode, and monitor the concentration of benzene pollutants at the outlet of the cathode airflow channel when it is stable.
  • the catalytic performance is shown in Figures 3 and 4.
  • porous conductive adsorption material electrodes are used as cathodes to carry out the experiment of removing benzene pollutants.
  • the iron-containing catalyst in the cathode uses iron oxide catalyst
  • the porous conductive adsorption material electrode uses activated carbon fiber, carbon nanotubes, graphene and nitrogen-doped graphene.
  • the specific operation is: ultrasonically disperse 10mg of iron oxide catalyst to 5mL In the mixture of Nafion and isopropanol, the dispersion was sprayed on the surface of 16 square centimeters of activated carbon fibers, carbon nanotubes, graphene, and nitrogen-doped graphene to prepare different cathodes.
  • electro-Fenton catalysts were used to remove benzene pollutants.
  • the electro-Fenton catalyst used iron oxide catalyst, ferroferric oxide catalyst, nickel oxide catalyst, cobalt tetroxide catalyst, manganese dioxide catalyst, ceria catalyst and Nickel iron hydroxide catalyst, nickel iron hydroxide catalyst, chromium oxide catalyst, iron hydroxide catalyst, sodium tetrapolyphosphate, iron sulfate, sodium tripolyphosphate and iron chloride.
  • the carbon material electrode uses activated carbon fiber.
  • the specific operation is: passing the gas containing benzene into the gas flow channel near the surface of the cathode ,
  • the concentration of organic pollutant benzene is 10ppm
  • air is used as the balance gas
  • the total flow rate is controlled to 20mL/min.
  • the water pump is continuously introduced into the channel close to the anode surface with a flow rate of 10 mL/min.
  • the catalytic performance is shown in Figures 7 and 8.
  • the degradation rate of benzene pollutants is different under a certain voltage when different electro-Fenton catalysts are used.
  • iron oxide, cobalt tetroxide, sodium tetrapolyphosphate and iron sulfate are used as electro-Fenton catalysts.
  • the degradation rate is greater than 90%.
  • the anode material can be tin, lead, ruthenium, rhodium, palladium, iridium, platinum, ruthenium-iridium alloy, ruthenium oxide or iridium oxide, and its cathode material, electrochemical reactor
  • the method of assembling and the method of removing benzene contaminants can be referred to the operation of embodiment 1, which will not be repeated here.
  • monitor the concentration of benzene pollutants at the outlet of the cathode airflow channel when it is stable, and the catalytic performance is shown in Figure 9.
  • Example 1 The electrochemical reactor in Example 1 was used for benzene, toluene, m/p-xylene, o-xylene, 1,2,4-trimethylbenzene, styrene, ethylene, propylene, 1,3-
  • the removal test of butadiene, formaldehyde, and acetaldehyde pollutants is carried out.
  • the specific operation can refer to the operation in Example 1.
  • Different DC voltages are applied between the cathode and the anode, and the benzene pollutants at the outlet of the cathode airflow channel are monitored when they are stable. Concentration, record the voltage when the pollutant degradation rate is greater than 95%, and the catalytic performance is shown in Figure 10.

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Abstract

Dispositif et procédé d'élimination d'un polluant gazeux par oxydation catalytique électro-Fenton. Le dispositif comprend un réacteur électrochimique (100) ; le réacteur électrochimique (100) comprend une source d'alimentation, une anode (10), une cathode (20), une membrane échangeuse de protons (50), un canal d'écoulement d'air d'anode (30) et un canal d'écoulement d'air de cathode (40) ; la membrane échangeuse de protons (50) est disposée entre l'anode (10) et la cathode (20) ; l'anode (10) est disposée dans le canal d'écoulement d'air d'anode (30) ; la cathode (20) est disposée dans le canal d'écoulement d'air de cathode (40) ; la cathode (20) est une électrode en matériau adsorbant conducteur poreux pour charger un catalyseur de métal de transition. Le procédé comprend les étapes suivantes : l'introduction d'air contenant le polluant gazeux dans le canal d'écoulement d'air de cathode (40), l'introduction d'eau ou d'air contenant de la vapeur d'eau dans le canal d'écoulement d'air d'anode (30), et l'application d'une tension de courant continu de 0,5 V à 36 V entre l'anode (10) et la cathode (20).
PCT/CN2019/113912 2019-09-30 2019-10-29 Procédé et dispositif d'élimination de polluants gazeux par oxydation catalytique électro-fenton WO2021062908A1 (fr)

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CN201910948066.6 2019-09-30

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