WO2017076282A1 - Appareil à cuve électrolytique utilisant une cathode de réduction d'oxygène - Google Patents

Appareil à cuve électrolytique utilisant une cathode de réduction d'oxygène Download PDF

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Publication number
WO2017076282A1
WO2017076282A1 PCT/CN2016/104284 CN2016104284W WO2017076282A1 WO 2017076282 A1 WO2017076282 A1 WO 2017076282A1 CN 2016104284 W CN2016104284 W CN 2016104284W WO 2017076282 A1 WO2017076282 A1 WO 2017076282A1
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Prior art keywords
cathode
anode
flow field
end plate
separation chamber
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PCT/CN2016/104284
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English (en)
Chinese (zh)
Inventor
卢善富
梁大为
相艳
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北京航空航天大学
卢善富
梁大为
相艳
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Application filed by 北京航空航天大学, 卢善富, 梁大为, 相艳 filed Critical 北京航空航天大学
Publication of WO2017076282A1 publication Critical patent/WO2017076282A1/fr

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    • C—CHEMISTRY; METALLURGY
    • C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F1/00—Treatment of water, waste water, or sewage
    • C02F1/46—Treatment of water, waste water, or sewage by electrochemical methods
    • C02F1/461—Treatment of water, waste water, or sewage by electrochemical methods by electrolysis
    • C02F1/46104—Devices therefor; Their operating or servicing
    • C02F1/46109—Electrodes
    • C—CHEMISTRY; METALLURGY
    • C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F1/00—Treatment of water, waste water, or sewage
    • C02F1/46—Treatment of water, waste water, or sewage by electrochemical methods
    • C02F1/461—Treatment of water, waste water, or sewage by electrochemical methods by electrolysis
    • C—CHEMISTRY; METALLURGY
    • C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F1/00—Treatment of water, waste water, or sewage
    • C02F1/46—Treatment of water, waste water, or sewage by electrochemical methods
    • C02F1/461—Treatment of water, waste water, or sewage by electrochemical methods by electrolysis
    • C02F1/46104—Devices therefor; Their operating or servicing
    • C02F1/46109—Electrodes
    • C02F2001/46133—Electrodes characterised by the material
    • C—CHEMISTRY; METALLURGY
    • C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F1/00—Treatment of water, waste water, or sewage
    • C02F1/46—Treatment of water, waste water, or sewage by electrochemical methods
    • C02F1/461—Treatment of water, waste water, or sewage by electrochemical methods by electrolysis
    • C02F1/46104—Devices therefor; Their operating or servicing
    • C02F1/46109—Electrodes
    • C02F2001/46133—Electrodes characterised by the material
    • C02F2001/46138—Electrodes comprising a substrate and a coating
    • C02F2001/46142—Catalytic coating
    • C—CHEMISTRY; METALLURGY
    • C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F1/00—Treatment of water, waste water, or sewage
    • C02F1/46—Treatment of water, waste water, or sewage by electrochemical methods
    • C02F1/461—Treatment of water, waste water, or sewage by electrochemical methods by electrolysis
    • C02F1/46104—Devices therefor; Their operating or servicing
    • C02F1/46109—Electrodes
    • C02F2001/46152—Electrodes characterised by the shape or form
    • C02F2001/46157—Perforated or foraminous electrodes
    • C02F2001/46161—Porous electrodes
    • C02F2001/46166—Gas diffusion electrodes
    • C—CHEMISTRY; METALLURGY
    • C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F2101/00—Nature of the contaminant
    • C02F2101/30—Organic compounds

Definitions

  • the invention relates to an electrolytic cell device using an oxygen reducing cathode based on a porous gas diffusion electrode, and belongs to the water treatment industrial technology in the field of environmental protection.
  • Electrochemical advanced oxidation is an effective method for treating such industrial wastewater. Electrochemical oxidation can effectively oxidize and degrade water by using free radicals generated on the surface of the electrode (such as direct oxidation of hydroxyl radicals) or generated oxidants (such as indirect oxidation of hypochlorous acid). Organic Pollutants.
  • the method has the characteristics of high processing efficiency, simple operation, environmental friendliness, and the like, and is convenient for technology. However, higher energy consumption has been a bottleneck that has plagued the application of electro-oxidation technology to wastewater treatment.
  • the conventional electrochemical oxidation method uses a hydrogen-producing cathode to generate hydrogen in the electrocatalytic reduction of protons in the cathode. Moreover, since the reaction is carried out in an open electrolytic cell, the hydrogen production of the cathode is not effectively recovered, and the mixing of the by-product oxygen of the anode with the hydrogen production of the cathode is also potentially dangerous.
  • the oxygen cathode used in the present invention has been widely used in industrial production of fuel cells and chlor-alkali. In a oxyhydrogen fuel cell, oxygen is reduced at the cathode to form water, and the cathode includes a gas diffusion layer whose main body is a carbon material and a catalytic layer containing a noble metal catalyst.
  • the invention provides an efficient and economical treatment process for changing traditional refractory organic wastewater.
  • the invention utilizes an electrolytic cell based on an oxygen reduction cathode, and under the condition of an applied voltage of 1-5 volts, the anode is highly mineralized to decompose organic pollutants and ammonia nitrogen in the organic wastewater, and the cathode reduces the oxygen which is introduced into water.
  • the invention is unique in that it is more conventional to use oxygen to reduce the cathode.
  • the higher electrode potential of the hydrogen producing cathode reduces the occurrence of reversible reduction of organic pollutants at the cathode and improves current efficiency.
  • the invention effectively reduces the electrode plate spacing and simultaneously increases the cathode potential, resulting in a significant reduction in the electrolytic cell voltage, greatly improving the economics of the electrochemical oxidation process for treating wastewater.
  • An electrolytic cell device using a porous gas diffusion electrode as a cathode comprising an anode chamber, a separation chamber and a cathode chamber;
  • the anode chamber includes an anode end plate, a separation chamber, a porous anode support material and an anode catalytic layer, the lower end of the water flow chamber is provided with a water inlet, and the upper end is provided with a water outlet; the anode catalytic layer and the porous anode support a material disposed between the anode end plate and the separation chamber; the anode catalytic layer is located on a side of the porous anode support material facing the separation chamber; the porous anode support material is provided An anode current collector, the anode current collector sealing out of the anode end plate;
  • the compartment is made of foamed plastic, PMMA or silica gel material, and the hollow portion is filled with a porous glass fiber material.
  • the anode chamber and the cathode chamber are separated by a compartment.
  • an electrolytic cell apparatus using an oxygen reduction cathode comprising:
  • the anode chamber includes an anode end plate, a porous anode support material and an anode catalytic layer, and an anode flow field groove is disposed on a side of the anode end plate facing the separation chamber, and an inlet end of the anode flow field groove is provided There is an anode water inlet, and an anode water outlet is arranged at the water outlet end of the anode flow field tank.
  • the anode catalytic layer is located between the separation chamber and the porous anode support material,
  • the cathode chamber includes a cathode end plate and a gas diffusion electrode, and a cathode flow field groove is disposed on a side of the cathode end plate facing the separation chamber, and a cathode air inlet is provided at an inlet end of the cathode flow field groove a gas outlet end of the cathode flow field groove is provided with a cathode gas outlet; the porous gas diffusion electrode is disposed between the cathode end plate and the separation chamber,
  • the compartment of the compartment is filled with a glass fiber filler.
  • the cathode chamber includes a cathode end plate and a porous gas diffusion electrode, the porous gas diffusion electrode sealing is disposed between the cathode end plate and the separation chamber; and the cathode end plate faces the porous gas diffusion electrode
  • One side is provided with a cathode flow field groove, and the cathode flow field a cathode inlet is disposed at an inlet end of the tank, a cathode outlet is disposed at an outlet end of the cathode flow field groove, a cathode current collector is disposed in the porous gas diffusion electrode, and the cathode current collector is sealed Outside the cathode end plate;
  • the anode end plate is made of polymethyl methacrylate (PMMA).
  • the porous male support material is a corrosion resistant wire mesh having a mesh number of 50-400 mesh, a wire diameter of 10-500 micrometers, and a wire mesh thickness of 100-1000 micrometers.
  • the anode catalytic layer is RuO 2 -TiO 2 , PbO 2 , SnO 2 -Sb 2 O 3 , Nb 2 O 5 -SnO 2 , SnO 2 -In 2 O 3 , IrO 2 -Ta 2 O 5 , or rare earth metal oxide / Sb 2 or a mixture of a medium 2 O 5 -SnO more.
  • the corrosion resistant wire comprises a tungsten wire, a titanium wire, a molybdenum wire or a twisted wire.
  • the corrosion resistant wire forming mesh is a foamed titanium mesh having a thickness of 300 micrometers to 2000 micrometers;
  • the corrosion-resistant wire forming mesh is a porous titanium plate having a thickness of 500 micrometers to 3000 micrometers and a porosity of more than 40%.
  • the anode flow field groove is designed to be a lateral bottom wide groove and a longitudinal narrow groove, the wide groove width is 3-6 mm, the narrow groove width is 1-3 mm, and the groove depth is 0.5-2.0 mm.
  • the cathode end plate is made of PMMA.
  • the porous gas diffusion electrode is composed of a gas diffusion layer, a hydrophobic skeleton, and a catalyst.
  • Materials constituting the gas diffusion layer include carbon black, graphite, carbon nanotubes, and carbon nanofibers.
  • the materials constituting the hydrophobic skeleton include polytetrafluoroethylene (PTFE), paraffin wax, polyethylene, polypropylene, and wax, and are added in the form of a dry powder additive, a liquid suspension (including a special dispersant), or a spherical shape. In the form of a film on a fiber or a porous substrate.
  • the catalyst is a Pt catalyst suitable for an oxygen reduction reaction.
  • the cathode flow field groove is designed to be a horizontal or vertical serpentine shape and a comb groove arrangement, the groove width is 1-3 mm, the groove depth is 0.5-2.0 mm, and two or three flow channel grooves are arranged in parallel, and the flow field channel is arranged. From the beginning of the water inlet to the end of the water outlet;
  • the cathode chamber and the anode chamber are separated by the separation chamber.
  • a silicon or foam seal that is sealed by the silicone seal between the anode end plate, the separation chamber, and the porous gas diffusion electrode.
  • the present invention employs an oxygen-reducing cathode, and oxygen is reduced at the cathode to form water. Compared with the conventional hydrogen-producing cathode, the voltage of the electrolytic cell can be greatly reduced due to changes in the electrode reaction.
  • Oxygen reduction cathode has higher potential than traditional hydrogen production cathode, effectively avoiding pollutants
  • a reversible redox reaction occurs at the yin and yang poles to improve current efficiency.
  • the electrolytic cell designed in the present invention can greatly reduce the plate spacing and reduce the solution potential drop compared to the conventional open electrolytic cell.
  • FIG. 1 is a diagram showing the structure of an oxygen cathode electrooxidation system according to an embodiment of the present invention.
  • Figure 2 is a development view of the oxygen cathode electrooxidation system of the embodiment shown in Figure 1.
  • Figure 3 is a front elevational view of an anode in accordance with one embodiment of the present invention.
  • Figure 4 is a left side view of the anode shown in Figure 3.
  • an electrolytic cell apparatus using an oxygen-reducing cathode includes a partitioning chamber 7 and a glass fiber filled therein and a cavity therein.
  • an anode flow field tank 2 the inlet end of the anode flow field tank 2 is provided with an anode water inlet 101, and the water outlet end of the anode flow field tank 2 is provided with an anode water outlet 102;
  • the anode catalytic layer 5 is located at the Between the separation chamber 7 and the porous anode support material 4, and is in close contact with the porous anode support material 4; the porous anode support material 4 is provided with an anode current collector 6, the an
  • the porous male support material 4 is a corrosion resistant wire mesh having a mesh number of 50-400 mesh, a wire diameter of 10-500 micrometers, and a wire mesh thickness of 100- 1000 micrometers;
  • the anode catalytic layer 5 is RuO 2 -TiO 2 , PbO 2 , SnO 2 -Sb 2 O 3 , Nb 2 O 5 -SnO 2 , SnO 2 -In 2 O 3 , IrO 2 -Ta 2 O 5 or / Sb one kind of rare earth metal oxide or a mixture of 2 2 O 5 -SnO more.
  • the wire of the corrosion resistant wire mesh is one or more selected from the group consisting of tungsten wire, titanium wire, molybdenum wire or wire.
  • the corrosion-resistant wire forming mesh is a foamed titanium mesh having a thickness of 300 micrometers to 2000 micrometers; or the corrosion-resistant wire mesh is porous titanium.
  • the plate has a thickness of from 500 micrometers to 3000 micrometers and a porosity of greater than 40%.
  • the cathode end plate 11 is made of polymethyl methacrylate (PMMA);
  • the cathode flow field groove 10 is designed as a lateral or longitudinal serpentine, combed groove arrangement,
  • the groove width is 1-3 mm, the groove depth is 0.5-2.0 mm, and two or three flow channel grooves are arranged in parallel to form a flow field channel from the air inlet to the end of the gas outlet;
  • the catalyst of the porous gas diffusion electrode 9 is a Pt catalyst .
  • the oxygen reduction cathode electrolyzer device further comprises a foam seal 3, the anode end plate 1 and the separation chamber 7 being sealed by the foam seal 3
  • the cathode end plate 11 and the separation chamber 7 are also sealed by the foam sealing ring 3.
  • the anode chamber includes an anode end plate 1, an anode flow field groove 10, a foam sealing ring 3, an anode current collector 6, a porous anode support material 4, and an anode catalytic layer 5.
  • the anode end plate 1 is made of PMMA, and the anode flow field groove is formed by a lateral bottom wide groove and a longitudinal narrow groove, the wide groove width is 3-6 mm, the narrow groove width is 1-3 mm, and the groove depth is 0.5-2.0. Millimeter.
  • the porous male support material is a wire mesh, and is made of corrosion-resistant metal wire such as tungsten wire, titanium wire, molybdenum wire, and/or silk wire, and the mesh number is 50-400 mesh, and the wire diameter is 10- 500 microns, the thickness of the wire mesh is from 100 microns to 1000 microns; in one embodiment, a titanium foam mesh is used as the anode support material having a thickness of from about 300 microns to about 2000 microns; in another embodiment, porous titanium is used.
  • a support material made plate having a thickness of 500-3000 microns, a porosity greater than 40%; the anode catalyst layer 5 RuO 2 -TiO 2, PbO 2, SnO 2 -Sb 2 O 3, Nb 2 O 5 -SnO 2, SnO 2 -In 2 O 3 , IrO 2 -Ta 2 O 5 , or a mixture of one or more of rare earth metal oxides/Sb 2 O 5 -SnO 2 .
  • the cathode includes a cathode end plate 11, a cathode flow field groove 10, a foam sealing ring 3, a gas diffusion electrode 9, a cathode current collector 8, a cathode end plate 11 made of PMMA material, and a cathode flow field 10 design different from the anode flow field 2.
  • It is a horizontal or vertical serpentine, comb-groove arrangement with a groove width of 1-3 mm and a groove depth of 0.5-2.0 mm.
  • Two or three flow channel grooves are arranged in parallel, and the flow field channel starts from the air inlet to the outlet.
  • the gas port ends; the gas diffusion electrode 9 is made of PTFE, acetylene black, and Pt catalyst.
  • the cathode chamber and the anode chamber of the electrolytic cell are separated by the partition chamber 7.
  • the partition chamber 7 used is filled with glass fiber and has a thickness of 500-2000 micrometers; the working voltage applied to the electrolytic cell is 1-5 volts, and the electrolytic cell
  • the working current density is 1-120 mA/cm2; the water inlet 101 on the anode plate 1 is connected to the beginning of the anode flow field 2 at the bottom of the electrode plate; the water outlet 102 on the anode plate 1 is disposed on the side of the plate upper portion, and The ends of the anode flow field 2 are connected.
  • the gas inlet port 201 on the cathode plate 11 is connected to the beginning of the cathode flow field 10 at the bottom of the electrode plate; the water outlet port 202 on the anode plate 11 is disposed on the side of the plate upper portion and is connected to the end of the cathode flow field 10.
  • the organic wastewater enters from the water inlet 101 on the anode plate 1 of the oxygen reduction cathode electrolysis cell at a flow rate of 0.02-0.20 ml/(cm 2 ⁇ min), and is degraded and mineralized under the electrooxidation of the anode, and the treated water is discharged from the anode.
  • the water outlet 102 on the plate 1 is discharged.

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  • Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Hydrology & Water Resources (AREA)
  • Engineering & Computer Science (AREA)
  • Environmental & Geological Engineering (AREA)
  • Water Supply & Treatment (AREA)
  • Organic Chemistry (AREA)
  • Electrodes For Compound Or Non-Metal Manufacture (AREA)
  • Catalysts (AREA)
  • Water Treatment By Electricity Or Magnetism (AREA)

Abstract

La présente invention concerne un appareil à cuve électrolytique utilisant une cathode de réduction d'oxygène caractérisé en ce qu'il comporte: une chambre de séparation (7), une chambre d'anode sur un côté de la chambre de séparation (7), et une chambre de cathode sur l'autre côté de la chambre de séparation (7), la chambre d'anode comprenant une plaque à bornes d'anode (1), un matériau poreux de support d'anode (4), et une couche catalytique d'anode (5). Une cuve de champ d'écoulement d'anode (2) est prévue sur un côté, faisant face à la chambre de séparation (7), de la plaque à bornes anode (1), un orifice d'entrée d'eau (101) est prévu à une extrémité d'orifice d'entrée d'eau d'anode au niveau de la cuve de champ d'écoulement d'anode (2) et un orifice de sortie d'eau d'anode (102) est prévu au niveau d'un orifice de sortie d'eau de la cuve de champ d'écoulement d'anode (2). La couche catalytique d'anode (5) est située entre la chambre de séparation (7) et le matériau poreux de support d'anode (4). La chambre de cathode comporte une plaque à bornes de cathode (11) et une électrode de diffusion de gaz (9). Une cuve de champ d'écoulement de cathode (10) est prévue sur un côté faisant face à la chambre de séparation (7), de la plaque à bornes de cathode (11), un orifice entrée de gaz de cathode (201) est prévu à une extrémité d'orifice d'entrée de gaz de la cuve de champ d'écoulement de cathode (10) et un orifice de sortie de gaz de cathode (202) est prévu au niveau d'un orifice de sortie de gaz de la cuve de champ d'écoulement de cathode (10). L'électrode poreuse de diffusion de gaz (9) est disposée entre la plaque à bornes de cathode (11) et la chambre de séparation (7). Une cavité de la chambre de séparation (7) est remplie de charges de fibres de verre.
PCT/CN2016/104284 2015-11-06 2016-11-01 Appareil à cuve électrolytique utilisant une cathode de réduction d'oxygène WO2017076282A1 (fr)

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CN201510751195.8A CN105461023B (zh) 2015-11-06 2015-11-06 一种采用氧还原阴极的电解槽装置
CN2015107511958 2015-11-06

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Cited By (1)

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CN115976553A (zh) * 2022-12-28 2023-04-18 哈尔滨工业大学（威海） 一种带有紊流强化模块的电解水制氢装置及方法

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CN105461023B (zh) * 2015-11-06 2018-08-10 北京航空航天大学 一种采用氧还原阴极的电解槽装置
CN109607694A (zh) * 2018-12-27 2019-04-12 陕西麦可罗生物科技有限公司 一种春雷霉素原药车间浓缩水循环利用装置及方法
CN111058054B (zh) * 2020-01-03 2022-01-18 大连理工大学 一种用盐桥取代Nafion膜的电催化氮还原合成氨的装置及其方法

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* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN115976553A (zh) * 2022-12-28 2023-04-18 哈尔滨工业大学（威海） 一种带有紊流强化模块的电解水制氢装置及方法

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