CN118202085A - Apparatus and method for producing hydrogen peroxide - Google Patents
Apparatus and method for producing hydrogen peroxide Download PDFInfo
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- CN118202085A CN118202085A CN202280056698.1A CN202280056698A CN118202085A CN 118202085 A CN118202085 A CN 118202085A CN 202280056698 A CN202280056698 A CN 202280056698A CN 118202085 A CN118202085 A CN 118202085A
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- cathode
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- hydrogen peroxide
- gas diffusion
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- MHAJPDPJQMAIIY-UHFFFAOYSA-N Hydrogen peroxide Chemical compound OO MHAJPDPJQMAIIY-UHFFFAOYSA-N 0.000 title claims abstract description 167
- 238000004519 manufacturing process Methods 0.000 title claims description 22
- 239000007789 gas Substances 0.000 claims abstract description 220
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- 229910001868 water Inorganic materials 0.000 claims abstract description 99
- 238000009792 diffusion process Methods 0.000 claims abstract description 88
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims abstract description 65
- 229910052760 oxygen Inorganic materials 0.000 claims abstract description 65
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- QTBSBXVTEAMEQO-UHFFFAOYSA-N Acetic acid Chemical compound CC(O)=O QTBSBXVTEAMEQO-UHFFFAOYSA-N 0.000 description 3
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- IEQIEDJGQAUEQZ-UHFFFAOYSA-N phthalocyanine Chemical compound N1C(N=C2C3=CC=CC=C3C(N=C3C4=CC=CC=C4C(=N4)N3)=N2)=C(C=CC=C2)C2=C1N=C1C2=CC=CC=C2C4=N1 IEQIEDJGQAUEQZ-UHFFFAOYSA-N 0.000 description 2
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- 229910021397 glassy carbon Inorganic materials 0.000 description 1
- JEGUKCSWCFPDGT-UHFFFAOYSA-N h2o hydrate Chemical compound O.O JEGUKCSWCFPDGT-UHFFFAOYSA-N 0.000 description 1
- 150000002431 hydrogen Chemical class 0.000 description 1
- 238000005984 hydrogenation reaction Methods 0.000 description 1
- 238000011065 in-situ storage Methods 0.000 description 1
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- 238000002347 injection Methods 0.000 description 1
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- 229910052741 iridium Inorganic materials 0.000 description 1
- GKOZUEZYRPOHIO-UHFFFAOYSA-N iridium atom Chemical compound [Ir] GKOZUEZYRPOHIO-UHFFFAOYSA-N 0.000 description 1
- XEEYBQQBJWHFJM-UHFFFAOYSA-N iron Substances [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 description 1
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- 229910001925 ruthenium oxide Inorganic materials 0.000 description 1
- WOCIAKWEIIZHES-UHFFFAOYSA-N ruthenium(iv) oxide Chemical group O=[Ru]=O WOCIAKWEIIZHES-UHFFFAOYSA-N 0.000 description 1
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- C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
- C25B1/00—Electrolytic production of inorganic compounds or non-metals
- C25B1/01—Products
- C25B1/28—Per-compounds
- C25B1/30—Peroxides
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- C25B9/00—Cells or assemblies of cells; Constructional parts of cells; Assemblies of constructional parts, e.g. electrode-diaphragm assemblies; Process-related cell features
- C25B9/17—Cells comprising dimensionally-stable non-movable electrodes; Assemblies of constructional parts thereof
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- C25B15/00—Operating or servicing cells
- C25B15/08—Supplying or removing reactants or electrolytes; Regeneration of electrolytes
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- C25B9/00—Cells or assemblies of cells; Constructional parts of cells; Assemblies of constructional parts, e.g. electrode-diaphragm assemblies; Process-related cell features
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- Chemical Kinetics & Catalysis (AREA)
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- Materials Engineering (AREA)
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- Organic Chemistry (AREA)
- Inorganic Chemistry (AREA)
- Electrolytic Production Of Non-Metals, Compounds, Apparatuses Therefor (AREA)
Abstract
The present invention relates to an apparatus for producing hydrogen peroxide comprising one or more electrochemical cells, the apparatus further comprising at least one electrically conductive porous gas transport layer arranged in close proximity to the cathode gas diffusion layer, the gas transport layer being configured to transport an oxygen-containing gas stream towards the cathode gas diffusion layer and configured to collect an electrical current, and water configured to flow through the porous gas transport layer.
Description
Technical Field
The present invention relates to an apparatus and a method for producing hydrogen peroxide. The invention also relates to a system for generating hydroxyl radicals using the apparatus, and a method for producing the apparatus. More specifically, the present invention relates to an improved apparatus and method for producing hydrogen peroxide using oxygen reduction.
Background
Hydrogen peroxide (H 2O2) is a versatile chemical used as an oxidizing agent in pulp and paper, water treatment and agriculture industries. The use of off-the-shelf compounds to produce hydrogen peroxide on site is attractive to these industries because it allows for independent supply and is more sustainable. Electrolytic cells have the unique advantage that they can utilize electricity as an input energy source to produce chemicals in a decentralized facility without the need for large chemical production plants. Its advantages include: the chemicals are produced at the desired location and time, thereby eliminating the need for transportation and storage and facilitating the use of sustainable energy sources such as wind and solar energy.
Electrochemical methods for producing hydrogen peroxide have great advantages over conventional anthraquinone methods, which produce hydrogen peroxide in centralized chemical facilities. Anthraquinone processes involve a large amount of energy, carbon dioxide emissions and chemical waste. Natural gas is the primary source of hydrogen in today's anthraquinone plants. Since production is centralized, it is necessary to transport the hydrogen peroxide to the point of use. For economic reasons, the transport concentration of hydrogen peroxide is typically 30% to 70%, which is dangerous and presents a safety problem. Once shipped to the point of use, it is typically diluted to a concentration of less than 3%.
These problems can be directly addressed by producing the chemicals on site. Electrochemical production can utilize atmospheric water and oxygen to form H 2O2 and only electricity is needed as an energy input, meaning that when CO 2 is used to neutralize electricity this can be a process without CO 2 emissions. Furthermore, in many applications, low concentrations (below 3 wt%) are required, which means that safety problems can be completely avoided if solutions of low concentration are produced from the beginning.
Electrochemical production of hydrogen peroxide generally relies on selective oxygen reduction. Traditionally, there are two main approaches to electrochemically producing hydrogen peroxide, depending on the form of the ion conductor used.
The first method is to use a liquid ionic conductor, typically in the form of an alkaline or neutral salt solution, as described, for example, in "direct continuous production of hydrogen peroxide (Direct and Continuous Production of Hydrogen Peroxide with 93％Selectivity Using aFuel-Cell System)",Angewandte Chemie 2003 with a selectivity of 93% using a fuel cell system". This method produces hydrogen peroxide with high efficiency and high concentration, but with low purity, because it is difficult to separate the salt from the hydrogen peroxide produced.
The second approach is to use solid state ionic conductors, such as polymeric cation exchange membranes, to achieve higher purity, but generally lower achievable concentrations and efficiencies, as described in synthesis (Neutral H2O2Synthesis by Electrolysis of Water and O2)",Angewandte Chemie2008 by H 2O2 neutralization of electrolyzed water and O 2.
Techniques known in the field of membrane electrode assemblies have difficulty achieving sufficiently high flux, which directly affects the size of the required electrode and thus the cost. The main reasons for this are the difficulty in achieving three conditions required for electrochemical hydrogen peroxide production simultaneously: oxygen is uniformly supplied on the cathode electrode, and electric current is uniformly collected from the cathode electrode while hydrogen peroxide is efficiently extracted from the cathode catalyst layer. The methods of the art operate primarily in the following environments:
Vapor phase oxygen, an environment suitable for delivering oxygen to the electrode, results in high current density, but it is difficult to extract hydrogen peroxide from the electrode, resulting in faraday inefficiency. This means that the overall flux is low.
Dissolved oxygen in water- -water helps to extract hydrogen peroxide, resulting in higher Faraday efficiency, but on the other hand, low solubility of oxygen in water means lower current density. The total flux of hydrogen peroxide is low.
To overcome the low flux problem, the methods in the literature have focused on designing electrochemical cells operating in a mixed phase of gas and liquid, such as those disclosed in U.S. patent application No. 2014/013017 Al and U.S. patent No. 5,972,196, U.S. patent No. 5,770,033, U.S. patent No. 2009/114532Al and european patent No. 3,430,182.
These methods involve applying a gas at selected locations of the cathode through a bubbler or fluidizing medium while immersing the remainder, and even the entire cathode, in water. Typically, in these designs, there are electrode areas dedicated to collecting current, other areas dedicated to delivering gas, and still other areas dedicated to extracting hydrogen peroxide. Thus, while such mixed phase operation brings about improvements such as higher faraday efficiency and flux, challenges remain in efficient and uniform current collection, gas application, product flow, and the full area of the cathode is not utilized effectively, resulting in sub-optimal performance and exacerbating degradation. Notably, in the prior art, the presence of water in the gas diffusion layer is undesirable because in the literature design, water can saturate the gas diffusion layer, which can lead to difficulties in delivering oxygen to the cathode catalyst and reduce the productivity of hydrogen peroxide. Accordingly, there remains a need for further improvements to address these and other challenges of hydrogen peroxide production.
Disclosure of Invention
The present invention addresses the challenges of hydrogen peroxide production discussed above by providing an improved apparatus for producing hydrogen peroxide, an improved system for forming hydroxyl radicals, a method of producing hydrogen peroxide using the apparatus of the present invention, and a method of producing the apparatus of the present invention. At least these and other aspects of the invention are described in detail in the appended claims.
More precisely, as will be described in more detail below, a new method for electrochemical cell design is presented herein, which is suitable for the synthesis of hydrogen peroxide from an electrochemical oxygen reduction reaction. Furthermore, the use of a porous conductive layer is described which provides both a uniform oxygen flow and electrical conductivity to the cathode of an electrochemical cell which generates hydrogen peroxide. Water is arranged to flow through the cathode gas diffusion layer, which assists in the removal of hydrogen peroxide from the electrode.
As mentioned above, the second approach is to use solid state ion conductors, such as polymeric cation exchange membranes, to achieve higher purity. As will be further described herein, the present invention proposes the use of a polymeric cation exchange membrane in combination with cathode and anode electrodes in intimate contact with the membrane to form a single mechanical entity, the so-called membrane electrode assembly, thereby allowing for higher purity of the hydrogen peroxide produced, while achieving higher concentrations and conversion efficiencies than are known in the art.
The proposed design of the electrochemical cell for the production of hydrogen peroxide improves current collection and gas transport while facilitating the extraction of hydrogen peroxide from the cathode by the presence of water or forced water flow. This optimizes the utilization of the available electrode area, resulting in higher flux, higher faraday efficiency, and longer electrode life. Other advantages include low High Frequency Resistance (HFR) and very uniform current collection distribution throughout the electrode area.
The apparatus according to the first aspect of the present invention comprises at least one and preferably a plurality of adjacent electrochemical cells, each electrochemical cell comprising an electrode assembly comprising at least one cathode gas diffusion layer, at least one cathode catalyst layer, at least one ion exchange membrane, at least one anode catalyst layer, and at least one anode current collector, the at least one cathode catalyst layer, the at least one ion exchange membrane and the at least one anode catalyst layer being arranged adjacent to each other within the electrode assembly, in sequence along the horizontal axis of the membrane electrode assembly, and at least one gas transport layer arranged adjacent to the cathode gas diffusion layer, the gas transport layer being capable of facilitating flow of an oxygen-containing gas to the cathode air diffusion layer and of collecting current, the cathode gas diffusion layer comprising water.
A system according to another aspect includes an apparatus according to any aspect of the invention discussed herein, and a device that facilitates the combination of hydrogen peroxide generated by the apparatus with ultraviolet light or ozone to facilitate the formation of hydroxyl radicals.
According to another aspect of the invention, methods of producing hydrogen peroxide using the apparatus of the invention and methods of producing the apparatus of the invention are also discussed in detail herein.
Other aspects of the invention are presented in the dependent claims.
In summary, the present invention provides a cathode gas diffusion layer comprising at least one electrically conductive porous gas transport layer that simultaneously collects current from the cathode and uniformly transports oxygen to the cathode, while water is present in the cathode gas diffusion layer. This configuration maximizes the electrode surface for hydrogen peroxide generation and facilitates extraction of the generated hydrogen peroxide, improving performance over configurations known in the art.
Such devices only require the use of readily available materials such as oxygen (from air) and water to generate hydrogen peroxide at the point of use. It has many advantages over purchasing bulk hydrogen peroxide, including supply safety, carbon dioxide neutralization, and safety.
Brief description of the drawings
List of reference numerals:
1. electrochemical cell
2. Cathode plate
3. Gas transport layer
4. Electrode assembly
5. Anode chamber
6. Air inlet
7. Cathode water inlet
8 Cathode water, oxygen and peroxide outlets
9. Anode water inlet
10. Anode water outlet
11. Cathode water inlet
12. Cathode water outlet
13. Gas diffusion layer
14. Catalyst layer
15. Film and method for producing the same
16. Catalyst layer
17. Anode current collector
18. Cathode end plate
19. Cathode current collector
20. Additional gas diffusion layer
21. Anode gasket
22. Anode end plate
23. Cathode of water pump
24 Gas/oxygen pump
25 Cathode water, oxygen and hydrogen peroxide
26. Water pump anode
27. Anode water and oxygen outlet
28. Power supply
29. Hydrogen peroxide sensor
The invention will be described with reference to the accompanying drawings, in which:
Fig. 1 is a schematic view of a portion of the inventive apparatus showing an electrically conductive porous gas transport layer and components of a membrane electrode assembly according to one embodiment of the invention.
Fig. 2 is a schematic illustration of an electrochemical cell design according to another embodiment of the invention.
Fig. 3 is another schematic illustration of a configuration of an electrochemical cell design according to another embodiment of the invention.
Fig. 4 is an exploded view of the electrochemical cell design of fig. 1.
Fig. 5 is a flow chart of a method for producing hydrogen peroxide using the apparatus of the present invention.
The drawings depict various embodiments of the present disclosure for purposes of illustration only. Those skilled in the art will readily recognize from the following discussion that alternative embodiments of the structures and methods illustrated herein may be employed without departing from the principles described herein.
Detailed Description
The following description is presented to enable one of ordinary skill in the art to make and use the disclosed subject matter and to incorporate it in certain applications. Various modifications and various uses in different applications will be readily apparent to those skilled in the art, and the generic principles defined herein may be applied to a wide variety of embodiments. Thus, the present disclosure is not intended to be limited to the embodiments shown, but is to be accorded the widest scope consistent with the principles and novel features disclosed herein.
In the following detailed description, numerous specific details are set forth in order to provide a more thorough understanding of the present disclosure. It will be apparent, however, to one skilled in the art that the present disclosure is not necessarily limited to these specific details, and that in other instances, well-known structures and devices are shown in block diagram form, rather than in detail, in order to avoid obscuring the present disclosure.
All the features disclosed in this specification (including any accompanying claims, abstract and drawings) may be replaced by alternative features serving the same, equivalent or similar purpose, unless expressly stated otherwise. Thus, unless expressly stated otherwise, each feature disclosed is one example only of a generic series of equivalent or similar features.
As used herein, the term "electrochemical cell" refers to, for example, a device that includes at least a positive electrode, a negative electrode, and an electrolyte therebetween that conducts ions (e.g., H +) but electrically insulates the positive and negative electrodes. In some embodiments, the device may include multiple positive electrodes and/or multiple negative electrodes enclosed in a container.
As used herein, the term "positive electrode" refers to an electrode that conducts, flows or moves positive ions (e.g., H +). As used herein, the term "negative electrode" refers to an electrode toward which positive ions (e.g., H +) flow or move during discharge of an electrochemical cell.
Or the application of heat and pressure may ensure that the cathode and membrane are physically attached and the anode and membrane are physically attached.
As used herein, the term "electrolyte" refers to an electrolyte in the form of a cation exchange membrane, such as Nafion, that allows ions (e.g., H +) to migrate through, but does not allow electrons to conduct through.
As used herein, the phrase "directly contacting" refers to the juxtaposition of two materials such that the two materials are in sufficient contact with each other to conduct ionic or electronic current. As used herein, "in direct contact" means that two materials are in physical contact with each other and that there is no third material between the two materials in direct contact.
As used herein, the term "porous" refers to a material that includes pores (e.g., nanopores, mesopores, or micropores).
As used herein, the term "manufacturing" refers to a process or method that forms or results in the formation of a manufactured object. For example, fabricating the energy storage electrode includes a process, process step, or method that results in the formation of an electrode of the energy storage device. The end result of the steps constituting the manufacture of the energy storage electrode is the production of a material with electrode function.
As used herein, the term "providing" refers to providing, generating, presenting, or delivering provided content.
As used herein, the term "solvent" refers to a liquid suitable for dissolving or solvating the ingredients or materials described herein. For example, the solvent includes a liquid, such as toluene, suitable for dissolving components used in the garnet sintering process, such as a binder.
As used herein, the term "water oxidation reaction" refers to, for example
2H2O→O2+4H++4e-
This reaction occurs at the anode.
Other anodic reactions include oxidation of water to hydrogen peroxide or ozone, oxidation of hydrogen, or oxidation of alcohols.
The term "oxygen reduction reaction" as used herein refers to, for example
2O2+4H++4e-→2H2O2
This reaction occurs at the cathode.
The oxygen source includes air, on-site generated oxygen (e.g., via a pressure swing adsorption system), and oxygen cylinders.
In addition to the definitions specified in the sections above, this document also provides other definitions.
The device of the invention comprises a plurality of electrochemical cells, each electrochemical cell 1 comprising at least one electrode assembly 4. The electrode assembly 4 may be a membrane electrode assembly. The membrane electrode assembly includes electrodes where electrochemical reactions occur. The membrane electrode assembly in its most general configuration comprises an anode, a cation exchange membrane and a cathode in contact with each other. Unlike the arrangements known in the art, in the proposed arrangement of the present invention there is no porous ion conducting layer between the cation exchange membrane and the cathode.
The anode serves as the proton source for the cathode, although water is the most common electrolyte reactant, other electrolytes (proton sources) such as alcohols (e.g., methanol, ethanol) or molecular hydrogen may be used in accordance with the present invention. If other proton sources than water are used, the overall cell and half cell reactions will be modified as desired.
Anodes for oxidation of water to oxygen are well known to those skilled in the art. These anodes generally consist of: iridium oxide nanoparticles are deposited directly on the polymer exchange membrane or current collector to form anode catalyst layer 16.
The ion exchange membrane 15 or the polymer exchange membrane 15 should be a proton conducting membrane, such as a Nafion T M ion exchange membrane. The thickness of the film is 10 μm to 1500 μm, preferably 100 μm to 500 μm.
The anode current collector 17 may include a titanium layer or titanium felt having a thickness of 50 μm to 3000 μm. The titanium layer or titanium felt has a porosity to allow oxygen generated at the anode catalyst layer 16 to escape. The sintered titanium layer or titanium felt may also be coated with other materials, such as platinum or gold, to improve electrical contact. The iridium oxide nanoparticles may be combined with or substituted with ruthenium oxide, platinum, and other metals. The deposition of the nanoparticles is performed by spraying, tape casting, and other suitable methods, and may be performed directly on the polymer exchange membrane 15, forming a Catalyst Coated Membrane (CCM) 15, or on the current collector 17, forming the GDE. After the deposition step, the polymer exchange membrane 15 and the sintered titanium layer or titanium felt 17 may be attached to each other with the anode catalyst layer 16 therebetween. The attachment may be mediated by the application of an ionomer solution and the application of heat and/or pressure.
What reduces oxygen to hydrogen peroxide is the cathode. The oxygen may originate from air, an oxygen concentrator or a compressed gas cylinder.
The cathode is composed of a cathode catalyst layer 14 and a cathode gas diffusion layer 13, the layers 13 and 14 being in contact with each other. The cathode gas diffusion layer 13 is porous and made of a conductive material to enable the transport of oxygen, water and hydrogen peroxide to/from the cathode catalyst layer 14. The cathode gas diffusion layer 13 is composed of carbon cloth or fiber. Other suitable cathode gas diffusion layers include metal foams or meshes, for example made of titanium or other metals, or other conductive foams, for example Reticulated Vitreous Carbon (RVC) or graphene oxide. The thickness of the cathode gas diffusion layer is 0.05 to 10mm, preferably between 0.1 and 5mm, even more preferably between 0.5 and 2mm. The cathode gas diffusion layer 14 may be coated with PTFE or other material on one or both sides to alter its properties.
The cathode catalyst layer 14 contains a catalyst for electrochemical reaction, which is located between the cathode gas diffusion layer 13 and the ion polymer exchange membrane 15. The catalyst ink may be deposited on the cathode gas diffusion layer 13 to form a gas diffusion electrode. The catalyst ink (CATALYST INK) comprises an ionomer mixed with a solvent and a catalyst. Typical ionomers include Nafion dispersions. The solvent includes alcohol and/or water. The cathode catalyst should be selective to the reduction of oxygen to hydrogen peroxide and include Pt-Hg, pd-Hg, cu-Hg, ag, au, carbon, graphene, nitrogen doped carbon, sulfur doped carbon, cobalt porphyrin and phthalocyanine, transition metal sulfides and nitrides, and any combination thereof. The catalyst material is in the form of nanoparticles to increase the surface area and promote the deposition process.
In an alternative embodiment, the catalyst ink is sprayed directly onto the polymer exchange membrane to form a catalyst coated membrane, followed by the addition of a gas diffusion layer. It is also possible to combine both the catalyst coated membrane and the gas diffusion electrode.
In the electrochemical cell 1 including the electrode assembly 4, the cathode is placed with its catalyst layer 14 facing the ion polymer exchange membrane 15. In one possible embodiment, it is the application of heat and pressure that ensures physical attachment of the cathode and membrane. Also, heat and pressure can ensure the attachment between the anode and the membrane. Typical values for temperature and pressure are 80-130 degrees celsius and 20-2000kg/cm 2, typically for 2 to 20 minutes. Or an adhesive material may be used to ensure attachment of the layers.
The anode current collector 17 may also be pressed in a single press or bonded to the opposite side of the membrane 15 with an adhesive. This forms a single mechanical entity comprising the cathode and anode electrodes and the polymer exchange membrane. The entity is a Membrane Electrode Assembly (MEA) or an electrode assembly 4.
The electrode assembly 4 is mechanically assembled in the electrochemical cell 1, which electrochemical cell 1 provides a suitable environment in terms of current collection, gas and water transport and peroxide extraction. The components of the gas transport layer 3 and electrode assembly 4 included in the apparatus of the present invention are also assembled as shown in the figures and will be discussed in more detail in connection with the figures. The gas transport layer 3 must be electrically conductive and porous.
The electrochemical cell 1 according to one embodiment of the present invention includes the following configuration: the electrically conductive porous gas transport layer 3, which is in direct contact with the cathode side of the membrane electrode assembly 4, has the dual function of providing a uniform flow of oxygen-containing gas over its entire surface and acts as a current collector. The conductive porous gas transmission layer 3 may be made of any one of aluminum, titanium, graphite, other metals, or post-transition metals. In order to provide a uniform gas flow, the porosity of the conductive porous gas transfer layer 3 should be adapted to the overall gas flow and gas pressure. For an area of 400cm 2, the preferred pressure drop of the electrically conductive porous gas transport layer in the direction through the plane is at least 1 mbar, and preferably higher than 20 mbar, even more preferably higher than 30 mbar. The thickness of the electrically conductive porous gas transport layer is 0.5 to 10mm, preferably 1 to 5mm, even more preferably 1 to 3mm. The pore size of the electrically conductive porous gas transport layer is from 0.1 to 100 microns, preferably from 0.13 to 10 microns, even more preferably from 0.2 to 5 microns. The electrically conductive porous gas transport layer should cover at least 10%, preferably at least 70%, even more preferably at least 95% of the cathode surface. Importantly, water cannot penetrate into the interior of the electrically conductive porous gas transport layer, otherwise it can clog some of the gas channels and oxygen cannot be uniformly delivered to the cathode gas diffusion layer surface. The pores of the conductive porous gas transmission layer are small, a natural hydrophobic surface is formed, water can be repelled, and the water is prevented from entering the conductive porous gas transmission layer and saturating the pores, so that the situation is avoided.
The oxygen-containing gas flows through the porous gas transmission layer 3 to the cathode side of the electrode assembly 4, passes through the cathode gas diffusion layer 13 in the through-plane direction, and reaches the cathode catalyst layer 14. The water flows through the cathode gas diffusion layer 13 in the planar direction thereof. In this way, the cathode may be simultaneously contacted with the oxygen-containing gas, water and electricity. Hydrogen peroxide generated at the cathode dissolves in the flowing water and is pushed out of the cathode catalyst layer 14. Thus, the decomposition of hydrogen peroxide is minimized and the faraday efficiency and flux are improved. The electrically conductive porous gas transfer layer 3 has important advantages in terms of cell assembly and repeatability over previous designs that rely on gas diffusers, as in previous designs, improper assembly of individual gas diffusers or out of the required tolerance range may lead to cell failure. In addition, another advantage is that the electrically conductive porous gas transport layer serves a dual function, both to collect current from and deliver oxygen reactant to the cathode electrode, whereas gas diffusers typically only disperse gas, and additional components are required to collect current.
According to another embodiment of the present invention, at least one additional gas diffusion layer 20 is interposed between the cathode gas diffusion layer 13 and the electrically conductive porous gas transport layer 3 to facilitate water or gas transport, or to facilitate hydrophilicity or hydrophobicity. The first and last layers of the interposed gas diffusion layers are in contact with the electrically conductive porous gas transport layer 3 and the cathode, respectively. Preferably, the gas diffusion layer 13 adjacent to the electrically conductive porous gas transport layer 3 has hydrophobic properties. The gas diffusion layer may also be patterned with teflon or other substances to have selected preferred regions of hydrophobicity. These preferred hydrophobic regions may be in the plane of the gas diffusion layer, or through the plane, or both. Furthermore, any interposed gas diffusion layer may cover at least 10%, preferably at least 70%, even more preferably at least 95% of the area of the cathode. The pore size of the cathode gas diffusion layer should be larger than the pore size of the electrically conductive porous gas transport layer to facilitate the passage of water flow. The pore size of the first and all gas diffusion layers should be from 1 to 1000 microns, preferably from 50 to 1000 microns, even more preferably from 100 to 1000 microns. The permeability of the cathode gas diffusion layer should be 50 to 1000L/m 2 s, preferably 100 to 600L/m 2 s, even more preferably 150 to 500L/m 2 s.
The cathode plate is placed on the opposite side of the conductive porous gas transport layer 3 from the electrode assembly 4. The function of which is to provide mechanical support and electrical contact to the electrically conductive porous gas transport layer 3 and the membrane electrode assembly 4. The cathode plate is made of an electrically conductive material such as aluminum, titanium, stainless steel or graphite. Combinations of injection molded plastic and electrically conductive materials are also suitable for use in the cathode plate. The cathode plate may have a dedicated gas inlet and the gas is directed to the inner cavity from where it is uniformly delivered to the electrically conductive porous gas transport layer 3. Similarly, the cathode plate also includes a liquid inlet and outlet. Water enters the inlet and water flows out of the outlet along with the hydrogen peroxide produced and any excess gas. The water entering through the inlet may contain dissolved air or oxygen, or nanobubbles, which are additional reactants for the cathodic reaction. Importantly, unlike other references known in the art, water should flow in-plane through the cathode gas diffusion layer 13 to facilitate removal of hydrogen peroxide from the cathode.
In some embodiments of the invention, the cathode plate and the electrically conductive porous gas transport layer 3 have inlet and outlet ports in a through plane direction, constituting an internal manifold (manifold).
To facilitate collection of current from the electrically conductive porous gas transport layer, the cathode plate gas cavity may have electrically conductive posts, coarse porous material or mesh in direct contact with the electrically conductive porous gas transport layer 3.
According to another embodiment of the invention, the inlet and outlet of the gas and liquid, respectively, may be incorporated into the gasket without affecting the properties of the invention. Suitable gasket materials include PTFE, EPDM and other polymer-based substances, as well as ABS, PA and other plastics.
In another embodiment of the invention, the electrically conductive porous gas transport layer may be physically connected to the cathode casing by means of, for example, welding or soldering. In some other embodiments, the electrically conductive porous gas transport layer 3 and the cathode casing are simply pressed against each other when assembled. An O-ring, gasket or sealant product may be used therebetween to prevent gas leakage.
The apparatus of the present invention may further comprise an anode chamber that collects current from the electrode assembly, and further comprises an input and an output at the anode side of the electrode assembly. The anode chamber includes an anode input and an anode output. The anode input is used to introduce water into the anode chamber, while the output is used to direct excess water not consumed by the anode and oxygen generated during the electrochemical reaction out of the housing. The anode chamber may be in electrical contact with the anode side of the electrode assembly 4. This may be facilitated by struts or other structures that allow water flow therethrough while in direct contact with the anode. In other embodiments, porous metal or mesh structures may also be used as separate components.
The individual components of the battery are assembled together and secured in place by bolts, clamps or other means.
According to other embodiments of the invention, the cathode plate and the anode plate may be integrated as a unit, i.e. a bipolar plate.
Once the electrochemical cell is assembled, the required reactants and power are delivered to the electrochemical cell.
After the electrochemical cell 1 has been assembled into a housing, an oxygen-containing gas is introduced at the cathode at a flow rate of 0.01 to 100 ml/min/cm electrode area to obtain a pressure of 0.01 to 10 bar. The source of the oxygen-containing gas may be one of ambient air, a pressurized oxygen cylinder or an oxygen concentrator. Water was introduced into the anode at a water flow rate of 0.01 to 50 ml/min/cm electrode area. Preferably, the water used is deionized, has a conductivity of less than 20 μS/cm, even more preferably has a conductivity of less than 1 μS/cm. The flow may be continuous or pulsed so that the anode chamber is only periodically refilled. Water is also introduced into the cathode chamber at a suitable flow rate, typically 0.01 to 50 ml/min/cm electrode area. A voltage is applied between the cathode and anode electrodes, the voltage of each cell being 0.6 to 10V, preferably 1.2 to 5V, even more preferably 1.2 to 3.5V. The current from the battery ranged from 20mA/cm 2 to 1500mA/cm 2. The result is hydrogen peroxide generation at the cathode. The resulting concentration is 200mg/L to 200000mg/L, preferably 1000 to 30000mg/L. The output concentration may vary depending on the applied current and the water flow in the cathode chamber. One or more cells may also be connected in series, parallel, or a combination of both to produce higher flux.
The hydrogen peroxide solution produced may be stored in a reservoir for later use or may be injected directly into the pipeline. Examples of suitable uses are in wastewater treatment, irrigation water treatment or cooling tower water treatment, or in any other application using hydrogen peroxide as an oxidant, biocide and/or oxygen source. The generated hydrogen peroxide can also be combined with ultraviolet rays, fenton-like reagents (such as iron ions) or ozone to generate OH free radicals, and the OH free radicals have higher oxidation potential and are also the basis of advanced oxidation processes. It may also be combined with acetic acid in situ to form peracetic acid. Several electrochemical cells of this configuration may be arranged in parallel or in series, enabling higher total flux. A particularly attractive arrangement is to connect the cells in series in a compact manner, also known as stacking or stacking.
Thus, in order to summarize at least some aspects of the invention described above, according to one embodiment of the invention, the invention relates to an apparatus for producing hydrogen peroxide comprising a plurality of adjacent electrochemical cells 1. Each electrochemical cell 1 comprises an electrode assembly 4, the electrode assembly 4 comprising at least one cathode gas diffusion layer 13, at least one cathode catalyst layer 14, at least one ion exchange membrane 15, at least one anode catalyst layer 16 and at least one anode current collector 17. The at least one cathode catalyst layer 14, the at least one ion exchange membrane 15, and the at least one anode catalyst layer 16 are disposed adjacent to each other within the electrode assembly 4 and are disposed in sequence along the horizontal axis of the membrane electrode assembly 4. The electrochemical cell 1 further comprises at least one electrically conductive gas transport layer 3 arranged adjacent to the cathode gas diffusion layer 13, which gas transport layer 3 is capable of facilitating the flow of an oxygen containing gas towards the cathode gas diffusion layer 13 and of collecting an electrical current. According to one embodiment of the invention, the cathode gas diffusion layer 13 comprises water, preferably flowing water.
The cathode catalyst layer 14 included in the apparatus of the present invention includes one or more catalysts, and the anode catalyst layer 16 included in the apparatus of the present invention also includes one or more catalysts.
According to one embodiment of the present invention, in the membrane electrode assembly 4, a first side of the ion exchange membrane 15 is joined (bind) to a second side of the cathode catalyst layer 14, and the anode catalyst layer 16 is joined to an opposite second side of the ion exchange membrane 15.
According to one embodiment of the invention, the at least one gas transport layer 3 is an electrically conductive porous gas transport layer in direct contact with the first side of the cathode gas diffusion layer 13.
According to one embodiment of the present invention, the arrangement of the apparatus allows water contained in the cathode gas diffusion layer 13 to flow in the planar direction in the cathode gas diffusion layer 13.
According to one embodiment of the present invention, a water oxidation reaction occurs within at least one anode catalyst layer 16 and an oxygen reduction reaction occurs within at least one cathode catalyst layer 14.
The surface of the gas diffusion layer 13 (or the additional gas diffusion layer 20) adjacent to the gas transport layer 3 is covered by the gas transport layer 3 in a proportion of at least 10%, preferably at least 70%, even more preferably at least 95%.
According to one embodiment of the present invention, the pores of the electrically conductive porous gas transport layer 3 are about 0.1 microns to 100 microns.
According to one embodiment of the invention, the electrically conductive porous gas transfer layer 3 causes a pressure drop between the gas chamber from which the oxygen-containing gas is supplied and the cathode gas diffusion layer 13 of at least 1 mbar, preferably at least 20 mbar, even more preferably 100 mbar.
According to one embodiment of the present invention, the electrically conductive porous gas transport layer 3 comprises one of a porous transition metal, a post-transition metal, a carbonaceous material, or a combination thereof.
According to one embodiment of the present invention, the current density at the membrane electrode assembly 4 is about 30mA/cm 2 to 900mA/cm 2.
According to one embodiment of the present invention, the voltage applied between the at least one cathode catalyst layer 14 and the at least one anode catalyst layer 16 is about 1.2 to about 3.5V.
While various features of the various embodiments of the present invention have been discussed in detail above, these and other features will be discussed below in connection with the embodiments of the present invention shown in the drawings.
Fig. 1 is a schematic view of a portion of the inventive apparatus showing an electrically conductive porous gas transport layer and components of a membrane electrode assembly according to one embodiment of the invention.
The apparatus of fig. 1 comprises an electrically conductive porous gas transport and membrane electrode assembly, numeral 3 representing an electrically conductive porous gas transport layer, numeral 13 representing a cathode gas diffusion layer, numeral 14 representing a cathode catalyst layer, numeral 15 representing a polymer exchange membrane, numeral 16 representing an anode catalyst layer, and numeral 17 representing an anode current collector.
The electrically conductive porous gas transport layer delivers gas to the cathode gas diffusion layer while acting as a cathode current collector. The cathode gas diffusion layer has a water flow in a planar direction, as indicated by the arrows, and bubbles from the electrically conductive porous gas transport layer pass through the water to the cathode catalyst layer. The cathode catalyst layer reduces oxygen to hydrogen peroxide, which rapidly leaves the catalyst layer and dissolves in the water flowing through the cathode gas diffusion layer. The anode catalyst layer oxidizes water to protons, which pass through the polymer exchange membrane to the cathode catalyst layer. The anode current collector supplies an electrical signal to the anode catalyst layer.
Fig. 2 is a schematic illustration of an electrochemical cell design according to another embodiment of the invention.
The apparatus of fig. 2 comprises an electrochemical cell, numeral 1 representing the electrochemical cell, numeral 2 representing the cathode plate, numeral 3 representing the electrically conductive porous gas transport layer, numeral 4 representing the membrane electrode assembly, numeral 5 representing the anode chamber, numeral 6 representing the gas inlet, numeral 7 representing the cathode water inlet, numeral 8 representing the cathode water, oxygen and peroxide outlets, numeral 9 representing the anode input, and numeral 10 representing the anode output.
An oxygen-containing gas is introduced through the gas inlet and passes through the electrically conductive porous gas transport layer uniformly dispersed on the cathode side of the membrane electrode assembly. Water flows in through the cathode water inlet and flows in the planar direction of the cathode gas diffusion layer. Excess gas, water and hydrogen peroxide are vented through the cathode outlet. Water also flows in through the anode input to enter the anode chamber where it is oxidized to oxygen and excess water is discharged through the anode output. A voltage difference is applied between the anode side and the cathode side of the membrane electrode assembly.
Fig. 3 is another schematic illustration of a configuration of an electrochemical cell design according to another embodiment of the invention.
The apparatus of fig. 3 comprises an electrochemical cell, numeral 1 representing the electrochemical cell, numeral 2 representing the cathode plate, numeral 3 representing the electrically conductive porous gas transport layer, numeral 4 representing the membrane electrode assembly, numeral 5 representing the anode chamber, numeral 6 representing the gas inlet, numeral 9 representing the anode water inlet, and numeral 10 representing the anode water outlet. Unlike the configuration shown in fig. 1 and 2, in the configuration shown in fig. 3, the cathode water inlet 11 and the cathode water outlet 12 are placed through the electrically conductive porous gas transport layer, as shown by the dotted lines. The oxygen-containing gas is introduced through the gas inlet and directed through the dedicated opening to the electrically conductive porous gas transport layer to be uniformly dispersed on the cathode side of the membrane electrode assembly. Water flows in through the cathode water inlet, through a dedicated path through the cathode plate and the electrically conductive porous gas transport layer, and flows in the planar direction of the cathode gas diffusion layer. Excess gas, water and hydrogen peroxide are vented through the cathode outlet. Water also flows in through the anode input to enter the anode chamber where it is oxidized to oxygen and excess water is discharged through the anode output. A voltage difference is applied between the anode side and the cathode side of the membrane electrode assembly.
Fig. 4 is an exploded view of the electrochemical cell design of fig. 1.
The apparatus of fig. 4 comprises an electrochemical cell, numeral 1 representing the electrochemical cell, numeral 2 representing the cathode plate, numeral 3 representing the electrically conductive porous gas transport layer, numeral 4 representing the membrane electrode assembly, numeral 5 representing the anode compartment, numeral 18 representing the cathode end plate, numeral 19 representing the cathode current collector, numeral 20 representing one or more additional cathode gas diffusion layers, numeral 21 representing the anode gasket, and numeral 22 representing the anode end plate. It has been found that one or even more additional cathode gas diffusion layers significantly improve the performance of the cell.
Figure 5 is a flow chart of a method included in the application, numeral 1 representing an electrochemical cell, numeral 23 representing a cathode pump controlling water flow to the cathode, numeral 24 representing an air pump, oxygen concentrator or air compressor delivering gas to the electrochemical cell, numeral 25 representing a cathode outlet containing water, gas and hydrogen peroxide, numeral 26 representing an anode pump, numeral 27 representing an anode outlet, numeral 28 representing a power source, and numeral 29 representing a hydrogen peroxide sensor. The hydrogen peroxide sensor measures the concentration at the outlet for automatically adjusting the flow rate delivered by the cathode pump 23 and the current at the power supply to maintain a constant concentration.
Hereinafter, exemplary embodiments of a method for manufacturing the apparatus of the present invention will be discussed.
The anode of the electrochemical cell 1 was prepared by depositing iridium oxide nanoparticles on a cationic polymer exchange membrane. The thickness of the polymer exchange membrane is 135 μm and thicker or thinner membranes can be used without affecting the final performance of the electrochemical cell. Preferably, the thickness of the film is from 5 to 500 μm, more preferably from 20 to 200 μm. A current collector was placed on the anode side of the membrane in direct contact with the iridium oxide nanoparticles. The material of the current collector should be selected to withstand the oxidizing conditions, preferably titanium and/or its oxide, tantalum and/or its oxide, gold, carbon, stainless steel or platinum, etc. The current collector material may also be an electrically conductive material coated with platinum, iridium and oxides thereof, titanium and oxides thereof, or tantalum and oxides thereof. The purpose of this coating is to obtain a proper electrical contact with the anode catalyst, which can be facilitated by applying pressure and/or temperature during the cell manufacturing process. In this example, titanium felt was used as the anode current collector.
The cathode is obtained by coating the gas diffusion layer with a suitable catalyst material. The gas diffusion layer may be hydrophilic or hydrophobic and contain a coating of PTFE or other substance to control hydrophobicity. The coating is accomplished by dispersing the appropriate catalyst nanoparticles in ethanol, water, and ionomer to form a catalyst ink, which may then be sprayed or deposited onto the gas diffusion layer in other ways. Suitable cathode catalysts should be selective to the reduction of oxygen to hydrogen peroxide and include Pt-Hg, pd-Hg, cu-Hg, ag, au, carbon, graphene, nitrogen-doped carbon, sulfur-doped carbon, cobalt porphyrin and phthalocyanine, transition metal sulfides and nitrides, and any combination thereof.
The anode current collector and the membrane, and the anode catalyst layer coated on one side of the membrane and the cathode placed on the other side were assembled together, and hot-pressed at 130 degrees celsius for 5 minutes under a pressure of 200kg/cm 2. This results in a membrane electrode assembly that is a single mechanical entity.
After this assembly step, the membrane electrode assembly is placed in a suitable cell housing, as shown in fig. 2. The cell housing consists of an anode compartment in which the anode side of the cell is disposed, an electrically conductive porous gas transport layer in which the cathode side of the cell is disposed, and a cathode housing that provides mechanical support for the electrically conductive porous gas transport layer. During assembly, it is important that the electrically conductive porous gas transport layer be planar and in uniform contact with the cathode gas diffusion layer. This is important because any deviation will cause water to escape from the ideal path in the plane of the cathode gas diffusion layer and take its external path because it provides less resistance and pressure drop. This will result in reduced efficiency in removing hydrogen peroxide from the cathode catalyst layer and reduced overall performance of the electrochemical cell.
Hereinafter, a method of preparing hydrogen peroxide while using the apparatus of the present invention will be discussed.
The apparatus according to the invention produces hydrogen peroxide based on the following half-cell reaction:
Anode: 2H (H) 2O→O2+4H++4e-
And (3) cathode: 2O (2O) 2+4H++4e-→2H2O2
While producing hydrogen peroxide, it is also important to minimize the decomposition of hydrogen peroxide, which can occur through chemical reactions:
2H2O2→2H2O+O2
or by electrochemical reactions:
H2O2+2H++2e-→2H2O
Other proton sources may be used at the anode without affecting the properties of the present invention; these include ethanol, methanol, hydrogen and other substances, as will be apparent to those skilled in the art.
Illustratively, a gas flow of 22ml/min/cm 2 is supplied to the cathode side of the cell, preferably in the range of 0.01 to 100ml/min/cm 2, based on the electrode area. The pressure at the cathode is set between 0.01 bar and 10 bar. A water flow of 0.3ml/min/cm 2 was supplied to the anode, with respect to the electrode area, and may vary from 0.01 to 50ml/min/cm 2. Water is added between the cathode electrode and the ion exchange membrane at a suitable flow rate to produce a hydrogen peroxide concentration of 1000 to 3000mg/L, and preferably, the concentration may be set to 200 to 50000mg/L, even more preferably, 5000 to 30000mg/L. The current density is set to 100mA/cm 2, but may preferably be set to 10 to 500mA/cm 2. The potential corresponding to 100mA/cm 2 was measured as 1.9V.
The foregoing embodiments and examples are illustrative only and not intended to be limiting. Those skilled in the art will recognize, or be able to ascertain using no more than routine experimentation, many equivalents to the specific compounds, materials, devices, and procedures. All such equivalents are considered to be within the scope of the following claims and are covered by the appended claims.
The language used in the specification has been principally selected for readability and instructional purposes, and may not have been selected to delineate or circumscribe the inventive subject matter. Accordingly, the scope of the disclosure is not limited by this detailed description, but rather by any claims that follow upon such application. Accordingly, the disclosure of the embodiments is intended to be illustrative, but not limiting, of the scope of the disclosure, which is set forth in the following claims.
Claim (modification according to treaty 19)
1. An apparatus for producing hydrogen peroxide comprising one or more adjacent electrochemical cells (1),
Each electrochemical cell (1) comprises:
A membrane electrode assembly (4), the membrane electrode assembly (4) comprising at least one cathode gas diffusion layer (13), at least one cathode catalyst layer (14), at least one ion exchange membrane (15), at least one anode catalyst layer (16), at least one anode current collector (17), and a cathode water inlet connected to a cathode pump (23) for transporting water,
Wherein in the membrane electrode assembly (4) a first side of the ion exchange membrane (15) is joined to a second side of the cathode catalyst layer (14) and the anode catalyst layer (16) is joined to an opposite second side of the ion exchange membrane (15) and at least one electrically conductive porous gas transport layer (3) having a hydrophobic surface is flat and uniformly contacts the first side of the cathode gas diffusion layer (13), the gas transport layer (3) being configured to transport a flow of oxygen-containing gas to the cathode gas diffusion layer (13) in a direction through the plane, the gas diffusion layer having a larger pore size than the electrically conductive porous gas transport layer for water flow therethrough and the gas transport layer further being configured to collect current, the cathode gas diffusion layer further comprising water configured to flow through the cathode gas diffusion layer (13) in the plane direction; and
Wherein the gas diffusion layer (13) is adapted to transport oxygen, water and hydrogen peroxide to the cathode catalyst layer (14) or from the cathode catalyst layer (14).
2. The device according to claim 1, comprising at least one additional gas diffusion layer (20) located between the gas transport layer (3) and the cathode gas diffusion layer (13).
3. The apparatus according to claim 1,
Wherein the water oxidation reaction is configured to occur within the at least one anode catalyst layer (16), and
Wherein the oxygen reduction reaction is configured to occur within the at least one cathode catalyst layer (14).
4. The apparatus according to claim 2,
Wherein the surface of the gas diffusion layer (13) (or the additional gas diffusion layer 20) adjacent to the gas transport layer (3) is covered by the gas transport layer (3) in a proportion of at least 10%, preferably at least 70%, even more preferably at least 95%.
5. The apparatus according to claim 1,
Wherein the pores of the conductive porous gas transmission layer (3) are about 0.1 to 100 micrometers and the thickness is 0.5 to 10 millimeters.
6. The apparatus according to claim 1,
Wherein the electrically conductive porous gas transport layer (3) causes a pressure drop of at least 1mbar between the gas chamber from which the oxygen-containing gas is derived and the cathode gas diffusion layer (13).
7. The apparatus according to claim 1,
Wherein the electrically conductive porous gas transport layer (3) comprises one of a porous transition metal, a post-transition metal, a carbonaceous material, or a combination thereof.
8. The apparatus according to claim 1,
Wherein the current density at the membrane electrode assembly (4) is about 30mA/cm 2 to 900mA/cm 2.
9. The apparatus according to claim 1,
Wherein a voltage applied between the at least one cathode catalyst layer (14) and the at least one anode catalyst layer (16) is about 1.2V to about 3.5V per cell.
10. A system, comprising:
The apparatus of claim 1, and
An apparatus that facilitates the combination of hydrogen peroxide produced by the device with ultraviolet light or ozone to facilitate the formation of hydroxyl radicals.
11. A process for the production of hydrogen peroxide,
Use of the device according to claim 1, the gas transport layer (3) delivering a flow of oxygen-containing gas in a direction through the plane to the cathode gas diffusion layer (13) and collecting the current,
Wherein water flows through the cathode gas diffusion layer (13) in the direction of the plane, and wherein hydrogen peroxide is generated by oxygen reduction at the cathode catalyst layer (14) and is dissolved in the flowing water, and wherein the hydrogen peroxide is pushed out of the cathode catalyst layer (14).
12. The method according to claim 11,
Wherein the concentration of hydrogen peroxide is measured and used to automatically adjust the flow of water delivered to the cathode by the cathode pump (23) and the current of the power supply to maintain a constant concentration.
Claims (12)
1. An apparatus for producing hydrogen peroxide comprising one or more adjacent electrochemical cells (1),
Each electrochemical cell (1) comprises:
a membrane electrode assembly (4), the membrane electrode assembly (4) comprising at least one cathode gas diffusion layer (13), at least one cathode catalyst layer (14), at least one ion exchange membrane (15), at least one anode catalyst layer (16) and at least one anode current collector (17),
Wherein in the membrane electrode assembly (4), a first side of the ion exchange membrane (15) is joined to a second side of the cathode catalyst layer (14), and the anode catalyst layer (16) is joined to an opposite second side of the ion exchange membrane (15), and
At least one electrically conductive porous gas transport layer (3) in direct contact with a first side of the cathode gas diffusion layer (13), the gas transport layer (3) being configured to transport a flow of oxygen-containing gas to the cathode gas diffusion layer (13) in a direction through the plane and further configured to collect an electrical current, further comprising water configured to flow through the cathode gas diffusion layer (13) in the direction of the plane; and
Wherein hydrogen peroxide is produced by oxygen reduction at the cathode catalyst layer (14) and is dissolved in flowing water and pushed out of the cathode catalyst layer (14).
2. The device according to claim 1, comprising at least one additional gas diffusion layer (20) located between the gas transport layer (3) and the cathode gas diffusion layer (13).
3. The apparatus according to claim 1,
Wherein the water oxidation reaction is configured to occur within the at least one anode catalyst layer (16), and
Wherein the oxygen reduction reaction is configured to occur within the at least one cathode catalyst layer (14).
4. The apparatus according to claim 2,
Wherein the surface of the gas diffusion layer (13) (or the additional gas diffusion layer 20) adjacent to the gas transport layer (3) is covered by the gas transport layer (3) in a proportion of at least 10%, preferably at least 70%, even more preferably at least 95%.
5. The apparatus according to claim 1,
Wherein the pores of the conductive porous gas transmission layer (3) are about 0.1 to 100 micrometers and the thickness is 0.5 to 10 millimeters.
6. The apparatus according to claim 1,
Wherein the electrically conductive porous gas transport layer (3) causes a pressure drop of at least 1mbar between the gas chamber from which the oxygen-containing gas is derived and the cathode gas diffusion layer (13).
7. The apparatus according to claim 1,
Wherein the electrically conductive porous gas transport layer (3) comprises one of a porous transition metal, a post-transition metal, a carbonaceous material, or a combination thereof.
8. The apparatus according to claim 1,
Wherein the current density at the membrane electrode assembly (4) is about 30mA/cm 2 to 900mA/cm 2.
9. The apparatus according to claim 1,
Wherein a voltage applied between the at least one cathode catalyst layer (14) and the at least one anode catalyst layer (16) is about 1.2V to about 3.5V per cell.
10. A system, comprising:
The apparatus of claim 1, and
An apparatus that facilitates the combination of hydrogen peroxide produced by the device with ultraviolet light or ozone to facilitate the formation of hydroxyl radicals.
11. A method for producing hydrogen peroxide using the apparatus of claim 1,
Wherein the concentration of hydrogen peroxide is measured and used to automatically adjust the flow of water delivered by the cathode pump (23) and the current of the power supply to maintain a constant concentration.
12. A process for the production of hydrogen peroxide,
Providing one or more electrochemical cells (1), the one or more electrochemical cells comprising: a membrane electrode assembly (4), the membrane electrode assembly (4) comprising at least one cathode gas diffusion layer (13), at least one cathode catalyst layer (14), at least one ion exchange membrane (15), at least one anode catalyst layer (16) and at least one anode current collector (17),
Wherein in the membrane electrode assembly (4) a first side of the ion exchange membrane (15) is joined to a second side of the cathode catalyst layer (14) and the anode catalyst layer (16) is joined to an opposite second side of the ion exchange membrane (15) and to at least one electrically conductive gas transport layer (3) in direct contact with a first side of a cathode gas diffusion layer (13),
The gas transport layer (3) delivers a flow of oxygen-containing gas to the cathode gas diffusion layer (13) in a direction through the plane and collects the current, and further comprises flowing water flowing through the cathode gas diffusion layer (13) in the direction of the plane; and
Wherein hydrogen peroxide is produced by oxygen reduction at the cathode catalyst layer (14) and is dissolved in flowing water, and wherein the hydrogen peroxide is pushed out of the cathode catalyst layer (14).
Applications Claiming Priority (4)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| EP21212606.4 | 2021-12-06 | ||
| US17/889,599 | 2022-08-17 | ||
| US17/889,599 US20240060195A1 (en) | 2022-08-17 | 2022-08-17 | Apparatus and method for producing hydrogen peroxide |
| PCT/EP2022/084324 WO2023104680A1 (en) | 2021-12-06 | 2022-12-04 | Apparatus and method for producing hydrogen peroxide |
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| Publication Number | Publication Date |
|---|---|
| CN118202085A true CN118202085A (en) | 2024-06-14 |
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| Application Number | Title | Priority Date | Filing Date |
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| CN202280056698.1A Pending CN118202085A (en) | 2021-12-06 | 2022-12-04 | Apparatus and method for producing hydrogen peroxide |
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| CN (1) | CN118202085A (en) |
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| WO2021034580A2 (en) * | 2019-08-22 | 2021-02-25 | The Regents Of The University Of California | High performance iron electrocoagulation systems for removing water contaminants |
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| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US6149810A (en) * | 1994-11-23 | 2000-11-21 | Lynntech, Inc. | Membrane with supported internal passages |
| CN108779560A (en) * | 2016-03-17 | 2018-11-09 | Hpnow爱普斯学会 | Electrochemical cell for the vapor-phase reactant in liquid environment |
-
2022
- 2022-08-17 US US17/889,599 patent/US20240060195A1/en not_active Abandoned
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