EP4288584A1 - Particularly compact and efficient assembly with separator and electrodes to be used in the electrolysis of water for the production of hydrogen at high pressure - Google Patents
Particularly compact and efficient assembly with separator and electrodes to be used in the electrolysis of water for the production of hydrogen at high pressureInfo
- Publication number
- EP4288584A1 EP4288584A1 EP22702029.4A EP22702029A EP4288584A1 EP 4288584 A1 EP4288584 A1 EP 4288584A1 EP 22702029 A EP22702029 A EP 22702029A EP 4288584 A1 EP4288584 A1 EP 4288584A1
- Authority
- EP
- European Patent Office
- Prior art keywords
- hydrogen
- separator
- compartment
- aqueous solution
- cathode
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
- Pending
Links
- 239000001257 hydrogen Substances 0.000 title claims abstract description 36
- 229910052739 hydrogen Inorganic materials 0.000 title claims abstract description 36
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 title claims abstract description 34
- 238000004519 manufacturing process Methods 0.000 title claims abstract description 9
- 238000005868 electrolysis reaction Methods 0.000 title claims description 16
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 title claims description 10
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims abstract description 16
- 239000001301 oxygen Substances 0.000 claims abstract description 16
- 229910052760 oxygen Inorganic materials 0.000 claims abstract description 16
- KWYUFKZDYYNOTN-UHFFFAOYSA-M Potassium hydroxide Chemical compound [OH-].[K+] KWYUFKZDYYNOTN-UHFFFAOYSA-M 0.000 claims description 34
- HEMHJVSKTPXQMS-UHFFFAOYSA-M Sodium hydroxide Chemical compound [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 claims description 33
- 239000007864 aqueous solution Substances 0.000 claims description 19
- 238000000034 method Methods 0.000 claims description 7
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 claims description 6
- 239000000243 solution Substances 0.000 claims description 6
- 230000015572 biosynthetic process Effects 0.000 claims description 5
- 229910052751 metal Inorganic materials 0.000 claims description 5
- 239000002184 metal Substances 0.000 claims description 5
- 230000008569 process Effects 0.000 claims description 5
- 239000003575 carbonaceous material Substances 0.000 claims description 4
- 229910052759 nickel Inorganic materials 0.000 claims description 3
- 238000000354 decomposition reaction Methods 0.000 claims description 2
- 150000002431 hydrogen Chemical class 0.000 claims description 2
- 239000000463 material Substances 0.000 claims description 2
- 229910052723 transition metal Inorganic materials 0.000 claims description 2
- 150000003624 transition metals Chemical class 0.000 claims description 2
- 239000012528 membrane Substances 0.000 abstract description 19
- 238000005516 engineering process Methods 0.000 abstract description 14
- 238000012423 maintenance Methods 0.000 abstract description 3
- 239000007787 solid Substances 0.000 abstract 1
- 239000003792 electrolyte Substances 0.000 description 11
- 239000007789 gas Substances 0.000 description 11
- 230000008901 benefit Effects 0.000 description 6
- 238000006243 chemical reaction Methods 0.000 description 4
- 239000007788 liquid Substances 0.000 description 4
- 239000011148 porous material Substances 0.000 description 4
- 239000000203 mixture Substances 0.000 description 3
- 238000000926 separation method Methods 0.000 description 3
- 238000005245 sintering Methods 0.000 description 3
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 2
- 229910000831 Steel Inorganic materials 0.000 description 2
- 230000003197 catalytic effect Effects 0.000 description 2
- 150000002500 ions Chemical class 0.000 description 2
- 230000035699 permeability Effects 0.000 description 2
- 239000012466 permeate Substances 0.000 description 2
- 239000010959 steel Substances 0.000 description 2
- 238000003860 storage Methods 0.000 description 2
- ZLMJMSJWJFRBEC-UHFFFAOYSA-N Potassium Chemical compound [K] ZLMJMSJWJFRBEC-UHFFFAOYSA-N 0.000 description 1
- CDBYLPFSWZWCQE-UHFFFAOYSA-L Sodium Carbonate Chemical compound [Na+].[Na+].[O-]C([O-])=O CDBYLPFSWZWCQE-UHFFFAOYSA-L 0.000 description 1
- 230000009471 action Effects 0.000 description 1
- 239000000654 additive Substances 0.000 description 1
- 230000000996 additive effect Effects 0.000 description 1
- 238000000231 atomic layer deposition Methods 0.000 description 1
- 239000002041 carbon nanotube Substances 0.000 description 1
- 229910021393 carbon nanotube Inorganic materials 0.000 description 1
- 230000015556 catabolic process Effects 0.000 description 1
- 230000001351 cycling effect Effects 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 239000011532 electronic conductor Substances 0.000 description 1
- 230000008030 elimination Effects 0.000 description 1
- 238000003379 elimination reaction Methods 0.000 description 1
- 230000007613 environmental effect Effects 0.000 description 1
- 239000002360 explosive Substances 0.000 description 1
- 239000002803 fossil fuel Substances 0.000 description 1
- 229910021389 graphene Inorganic materials 0.000 description 1
- 231100001261 hazardous Toxicity 0.000 description 1
- 239000010416 ion conductor Substances 0.000 description 1
- 238000005342 ion exchange Methods 0.000 description 1
- 238000007648 laser printing Methods 0.000 description 1
- 239000011244 liquid electrolyte Substances 0.000 description 1
- 238000003754 machining Methods 0.000 description 1
- 239000007769 metal material Substances 0.000 description 1
- 150000002739 metals Chemical class 0.000 description 1
- 230000005012 migration Effects 0.000 description 1
- 238000013508 migration Methods 0.000 description 1
- 229940072033 potash Drugs 0.000 description 1
- BWHMMNNQKKPAPP-UHFFFAOYSA-L potassium carbonate Substances [K+].[K+].[O-]C([O-])=O BWHMMNNQKKPAPP-UHFFFAOYSA-L 0.000 description 1
- 235000015320 potassium carbonate Nutrition 0.000 description 1
- 238000000746 purification Methods 0.000 description 1
- 230000007420 reactivation Effects 0.000 description 1
- 239000007784 solid electrolyte Substances 0.000 description 1
- 230000000930 thermomechanical effect Effects 0.000 description 1
Classifications
-
- C—CHEMISTRY; METALLURGY
- C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
- C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
- C25B13/00—Diaphragms; Spacing elements
- C25B13/04—Diaphragms; Spacing elements characterised by the material
- C25B13/05—Diaphragms; Spacing elements characterised by the material based on inorganic materials
-
- C—CHEMISTRY; METALLURGY
- C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
- 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
- C25B1/02—Hydrogen or oxygen
- C25B1/04—Hydrogen or oxygen by electrolysis of water
-
- C—CHEMISTRY; METALLURGY
- C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
- C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
- C25B15/00—Operating or servicing cells
- C25B15/02—Process control or regulation
-
- C—CHEMISTRY; METALLURGY
- C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
- C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
- C25B15/00—Operating or servicing cells
- C25B15/02—Process control or regulation
- C25B15/023—Measuring, analysing or testing during electrolytic production
-
- C—CHEMISTRY; METALLURGY
- C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
- C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
- C25B9/00—Cells or assemblies of cells; Constructional parts of cells; Assemblies of constructional parts, e.g. electrode-diaphragm assemblies; Process-related cell features
- C25B9/05—Pressure cells
-
- C—CHEMISTRY; METALLURGY
- C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
- C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
- 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
- C25B9/19—Cells comprising dimensionally-stable non-movable electrodes; Assemblies of constructional parts thereof with diaphragms
Definitions
- the present invention refers to a negative electrode/separator/positive electrode assembly, in other words a cathode/separator/anode structure to be inserted in an electrolytic cell based on the same principle of operation as the AEM (Alkaline Electrolyte Membrane) technology in place of the classic MEA (Membrane Electrode Assembly).
- AEM Alkaline Electrolyte Membrane
- MEA Membrane Electrode Assembly
- the invention may also be used in sports shoes similar to a ski boot, such as for example snowboard or ski mountaineering boots, cross-country ski shoes, mountain or rock-climbing shoes, shoes for ice or roller skates, cycling shoes and other types of sports shoes.
- the prior-art electrolyzers consist of an internal structure of the electrolytic cell made up of two catalytic layers (electrodes) that respectively are the anode and the cathode.
- the anode is the electrode where the reaction of production of oxygen takes place and the cathode is the electrode where the reaction of production of hydrogen takes place.
- the electrodes are arranged to form a sandwich structure enclosing an ion exchange polymeric membrane (known with the acronym MEA, or Membrane and Electrodes Assembly), acting as a solid electrolyte in addition to being a separator of the two compartments, and thus of the two gases, in the PEM (Proton Electrolyte Membrane) technology and in the AEM (Alkaline Electrolyte Membrane) technology, whereas in the former AEL (Alkaline Electrolyte Liquid) technology a plastic diaphragm is used as a separator and the electrolytic action is performed by a highly conductive liquid, like soda (NaOH) or potash (KOH) at high concentrations (25-30% of weight by weight w/w).
- MEA ion exchange polymeric membrane
- electrolysis is based on the decomposition of water by means of an electrical potential. Hydrogen is generated on the cathode (-) and oxygen on the anode (+). Between the electrodes, the electrolyte acts as ionic conductor. The ions that transmigrate between the electrodes are both H + and OH'. The electrolytic membrane separates the H2 and O2 gases that are generated between the two electrodes. Moreover, it must satisfy important requirements, such as stability in operating conditions, effective separation of the gases, mechanical separation of the electrodes, ionic conduction and mechanical support for the pressure differences between the two sides of the cell, generally lower than 30 bar.
- the electrolyzers based on liquid alkaline electrolyte are the most common because they have the best “performance/price” ratio, thanks to the low cost of components and to the scalability in the large dimensions (large diameter of the electrolytic cell).
- this technology is the current standard for large-scale electrolysis, while the polymeric-membrane based protonic technology (PEM) has the main advantage of simplicity of layout of the system thanks to the high purity achieved, with a mild system of purification.
- AEM membrane-based alkaline technology
- AEL liquid alkaline technology
- PEM protonic polymeric technology
- the technical problem at the basis of the present invention is therefore to devise a system that makes it possible to operate under high pressures while avoiding the problem of the “crossover” phenomenon and the breakage of the polymeric membrane that must sustain high pressure levels.
- a first objective of the present invention is an assembly provided with electrodes that are catalyzers consisting of common (i.e., not noble), and therefore low- cost metals, capable of being used in an alkaline environment for the generation of oxygen at the anode and of hydrogen at the cathode.
- electrodes that are catalyzers consisting of common (i.e., not noble), and therefore low- cost metals, capable of being used in an alkaline environment for the generation of oxygen at the anode and of hydrogen at the cathode.
- a second objective is an apparatus that uses a very resistant separator, selective to the ionic exchange capable of being used in place of membranes or diaphragms used in the prior art alkaline technology with the polymeric-based membrane.
- a third objective is an electrolytic cell comprising said apparatus.
- a further objective is a particularly efficient hydrogen-producing electrolysis process that uses said electrolytic cell.
- FIG. 1 is a schematic view of a cell of the electrolyzer comprising the assembly according to the present invention.
- the electrolytic cell according to the invention is schematically indicated in its more internal components, with particular reference to the assembly 10, indicated with reference numeral 1.
- the electrolytic cell 1 has a sandwich structure in which a sealed container 2 comprises an anodic compartment 3 where the breakdown of water takes place to form oxygen, a cathodic compartment 4 where hydrogen is formed, a separator 5 interposed between said cathodic and anodic compartments, a source of electric current 6 connected to the cathode 40 and to the anode 30 of the respective compartments through appropriate and conventional “current collectors” (not shown in figure 1 ), that have the function of conducting the current from the source to the electrodes.
- the cathodic compartment 4 includes in turn the cathode 40 formed by the catalyzer properly supported, having a first surface 41 in contact with said separator 5.
- a second surface 42 of the cathode, opposite to said first surface is in contact with a first surface 70 of a layer 7 permeable only to hydrogen (H2).
- This layer 7 is structured in such a manner as to have a porosity whose pores have a diameter smaller than 0.26 nanometers, preferably included between 0.1 and 0.19 nanometers.
- said layer is made of sintered metallic material capable of sustaining high pressures in the order of 300 bar and above.
- a second surface 71 of the layer 7 is then turned toward a chamber 43 of the cathodic compartment 4.
- a chamber 43 of the cathodic compartment 4 In said chamber is released hydrogen at high pressure, which will be sent, for example to storage through an outlet 44 of the same cathodic compartment.
- the separator 5 is interposed as in a sandwich between the cathode 40 and the anode 30 of the respective compartments and is permeable to water.
- the pores of the separator have a diameter between 0.2 and 0.28 nanometers so that they can trap a very diluted aqueous solution of KOH (potassium hydroxide) as electrolyte for the electrolysis reaction.
- the separator is metallic, that is consisting of a sintered metal layer. More preferably, the separator metal is nickel-based, possibly coated with carbon-based materials, such as for example graphene and carbon nanotubes.
- the separator can be made up of the above-mentioned carbon-based materials or oxides such as for example transition metals of the “d” or “f” block.
- this separator is capable of sustaining pressures higher than 350 bar, as it must maintain a maximum positive pressure delta in the order of 30-50 bar between the anodic compartment with respect to the cathodic compartment.
- the separator 5 is preferably made by sintering, Atomic Layer Deposition (ADL) or additive laser printing.
- ADL Atomic Layer Deposition
- additive laser printing Each of these methodologies is known in the field and the adjustment of the respective operating parameters such as for example, temperature and pressures, are within the common knowledge of the technician to achieve the above-mentioned dimensions of the pores of the final separator.
- thermomechanical sintering which is carried out inside a mold that works with pressures between 200 and 500 bar and temperatures between 600 and 2,000°C.
- the anodic compartment 3 comprises an anode 30 having a first surface 31 in contact with said separator 5 and a second surface 32 opposite to the first surface and facing a chamber 33 of the anodic compartment itself.
- the chamber 33 includes an inlet 34 to feed at high pressure, over 300 bar, an aqueous mixture di potassium hydroxide (KOH) or sodium hydroxide (NaOH).
- KOH potassium hydroxide
- NaOH sodium hydroxide
- the aqueous solution of KOH or NaOH can advantageously be included between 1% and 5% in weight (w/w).
- the chamber 33, but also the entire cell 1 , of the invention is built so as to sustain high pressures in the order of 350 bar and above, with precision machining processes of the contact surfaces with a very low tolerance and with high performance gaskets which in contact with a perfectly smooth surface and properly and evenly tightened guarantee their air tightness.
- aqueous solution is fed at high pressure into the inlet 34, and at the outlet 35 a liquid-gas separator 36 makes it possible to recover the oxygen produced in the electrolysis reaction by the aqueous solution of potassium or sodium hydroxide; the latter will be reinserted into the inlet through a conventional circuit (non shown).
- the cathode 40 and the anode 30 of the cell according to the present invention are entirely conventional. Thus, they are electronic conductors provided with a catalytic surface adapted to favor the release of hydrogen and oxygen, respectively, and adapted to offer a large surface between a catalyzer and an electrolyte. Moreover, they must have sites that are suitable for the formation of gas bubbles and properties that favor the detachment of gas bubbles so that they separate from the electrolyte when the operating voltage of the cell is achieved.
- the support materials of the anode and the cathode are typically steel and steel cladded with nickel. The large relative surfaces are obtained with the use of sintered structures, screens, perforated plates and plates with electrochemically corrugated surfaces machined by laser.
- a conventional command and control system (not shown in figure 1 ) comprises pressure sensors mounted on the respective anode and cathodic compartments so as to constantly record the pressure and send corresponding signals to a control unit that will regulate the pressure increase of said aqueous solution in the anodic compartment following the pressure increase in the cathodic compartment due to the buildup of hydrogen during the operation of the cell.
- the electrolytic cell is characterized mainly by said assembly 10 consisting of a sandwich-like structure having a separator interposed between the anode and the cathode, in which the separator is a metallic layer 5 with a porosity between 0.2 and 0.28 nanometers so as to only allow the passage of an aqueous solution of KOH or NaOH, but not the oxygen (O2), and the cathode 40 is cladded on its opposite surface 42 with respect to the one in contact with the layer by a layer 7 with a porosity lower than 0.26 nanometers, preferably included between 0.1 and 0.19 nanometers so as to allow the passage to the outside of the apparatus of the hydrogen alone, but not of said aqueous solution.
- the separator is a metallic layer 5 with a porosity between 0.2 and 0.28 nanometers so as to only allow the passage of an aqueous solution of KOH or NaOH, but not the oxygen (O2)
- the cathode 40 is cladded on its opposite surface 42 with respect to
- a further objective of the invention is an electrolysis process comprising the steps of:
- the aqueous solution permeates with a pressure difference between the anodic compartment and the cathodic compartment of more than 30 bar, preferably between 30 bar and 50 bar, passing from the anodic compartment through the anode and the separator permeable to water until it reaches the cathode.
- the hydrogen released is pushed outside the cathode due to the overpressure of the aqueous solution through the layer permeable to the hydrogen.
- the ions OH’ generated are returned toward the anode by the effect of electroosmotic entrainment, where oxygen is formed and mixes with the starting aqueous solution.
- a turbulent motion is promoted by an appropriate speed of the pump that feeds the aqueous solution into the anodic compartment, so as to advantageously obtain the rapid removal of the oxygen formed, which cannot permeate through the separator thanks to the above-mentioned characteristics of the separator itself.
- the above- mentioned high pressure in the anodic compartment is controlled so that there is always the pressure delta between 30 and 50 bar mentioned above during the entire operation of the cell.
- the cathodic compartment is closed by a conventional valve (not shown in figure 1 ), as the formation of hydrogen increases the pressure within it also increases and, as a consequence, the pressure within the anodic compartment must also increase to maintain the delta 30-50 bar necessary to ensure the correct functioning of the electrolysis and of the system as designed.
- the structure of the cell allows a considerable compacting to the advantage of systems in which more cells are used together to produce considerable quantities of hydrogen.
- the cell is sturdier, since the elimination of polymeric membranes substituted with a sintered separator makes it possible to sustain decidedly high pressures.
- the selective permeability of the water of said separator combined with the selective permeability of the hydrogen of the sintered layer on the cathode makes it possible to reduce, if not completely eliminate, the problem of the “crossover”.
- the structure of the cell makes it possible to not only substitute a more fragile polymeric membrane but also to reduce the quantity of electrolyte and of its aqueous concentration.
Landscapes
- Chemical & Material Sciences (AREA)
- Engineering & Computer Science (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Electrochemistry (AREA)
- Materials Engineering (AREA)
- Metallurgy (AREA)
- Organic Chemistry (AREA)
- Automation & Control Theory (AREA)
- Inorganic Chemistry (AREA)
- Analytical Chemistry (AREA)
- Electrolytic Production Of Non-Metals, Compounds, Apparatuses Therefor (AREA)
Abstract
Description
Claims
Applications Claiming Priority (2)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
IT202100002408 | 2021-02-04 | ||
PCT/IB2022/050398 WO2022167880A1 (en) | 2021-02-04 | 2022-01-18 | Particularly compact and efficient assembly with separator and electrodes to be used in the electrolysis of water for the production of hydrogen at high pressure |
Publications (1)
Publication Number | Publication Date |
---|---|
EP4288584A1 true EP4288584A1 (en) | 2023-12-13 |
Family
ID=75439357
Family Applications (1)
Application Number | Title | Priority Date | Filing Date |
---|---|---|---|
EP22702029.4A Pending EP4288584A1 (en) | 2021-02-04 | 2022-01-18 | Particularly compact and efficient assembly with separator and electrodes to be used in the electrolysis of water for the production of hydrogen at high pressure |
Country Status (2)
Country | Link |
---|---|
EP (1) | EP4288584A1 (en) |
WO (1) | WO2022167880A1 (en) |
Family Cites Families (5)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
US4032427A (en) * | 1975-11-03 | 1977-06-28 | Olin Corporation | Porous anode separator |
DE2927566C2 (en) * | 1979-07-07 | 1986-08-21 | Kernforschungsanlage Jülich GmbH, 5170 Jülich | Diaphragm for alkaline electrolysis, process for producing the same and its use |
DE3424203A1 (en) * | 1984-06-30 | 1986-01-16 | Kernforschungsanlage Jülich GmbH, 5170 Jülich | DIAPHRAGMA FOR ALKALINE ELECTROLYSIS AND METHOD FOR PRODUCING THE SAME |
US9011651B2 (en) * | 2010-12-09 | 2015-04-21 | Ut-Battelle, Llc | Apparatus and method for the electrolysis of water |
JP6450636B2 (en) * | 2015-04-20 | 2019-01-09 | デノラ・ペルメレック株式会社 | Electrolysis method |
-
2022
- 2022-01-18 EP EP22702029.4A patent/EP4288584A1/en active Pending
- 2022-01-18 WO PCT/IB2022/050398 patent/WO2022167880A1/en unknown
Also Published As
Publication number | Publication date |
---|---|
WO2022167880A1 (en) | 2022-08-11 |
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