EP3390692B1 - Elektrochemische zelle und verfahren - Google Patents

Elektrochemische zelle und verfahren Download PDF

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Publication number
EP3390692B1
EP3390692B1 EP16788728.0A EP16788728A EP3390692B1 EP 3390692 B1 EP3390692 B1 EP 3390692B1 EP 16788728 A EP16788728 A EP 16788728A EP 3390692 B1 EP3390692 B1 EP 3390692B1
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EP
European Patent Office
Prior art keywords
volume
electrochemical cell
catalyst
anode
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.)
Not-in-force
Application number
EP16788728.0A
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English (en)
French (fr)
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EP3390692A1 (de
Inventor
Timothy Hughes
Ian Wilkinson
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Siemens AG
Siemens Corp
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Siemens AG
Siemens Corp
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    • 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
    • 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
    • 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

Definitions

  • the present invention relates to electrochemical cells, particularly electrochemical cells for synthesis of ammonia NH 3 .
  • the present invention also relates to processes for synthesis of ammonia NH 3 .
  • WO 2015/164730 and JP 2009084615 also describe cell arrangements and methods for the production of ammonia.
  • the present invention seeks to provide alternative methods and apparatus for the synthesis of ammonia from water and nitrogen N 2 .
  • FIG. 1 The embodiment of the invention shown in Fig. 1 comprises an electrochemical cell 10 with three porously partitioned volumes 1-3.
  • the first volume 1 contains a nitride conductor 20 such as a molten salt eutectic, for example LiCl/KCl/Li 3 N.
  • a nitride conductor 20 such as a molten salt eutectic, for example LiCl/KCl/Li 3 N.
  • steam H 2 O is introduced into this first volume through a steam inlet 5.
  • a steam diffuser 22 may be provided to ensure wide distribution of inlet steam.
  • the second volume 2 is a cathode gas electrode. Nitrogen gas N 2 26 is introduced into this gas electrode, on a surface of the porous electrode 24 away from the nitride conductor 20.
  • the third volume 3 is an anode gas electrode.
  • a porous electrode 28 is in contact with the nitride conductor 20 on one side.
  • a DC power supply 7 applies a potential difference between the two porous electrodes 24, 28, with the more positive voltage +V being applied to the anode gas electrode 3 and the more negative voltage -V being applied to the cathode gas electrode 2.
  • the applied potential difference may be in the region of 0.5 V to 2 V.
  • the nitride ions migrate towards the anode under the influence of the voltage gradient between the anode and the cathode.
  • Ammonia is accordingly produced from nitrogen gas and steam.
  • the ammonia diffuses through the nitride conductor 20 to be evolved at the surface of the nitride conductor.
  • An enclosure 6 traps the evolved ammonia gas and allows it to be harvested.
  • the resulting oxide ions migrate towards the anode under the potential gradient between the electrodes.
  • Ammonia gas diffuses through nitride conductor 20 and is trapped in enclosure 6. It may be dried and cleaned as necessary, and may be stored for later use.
  • the structure of the electrochemical cell of the present invention allows steam H 2 O to be used as the source of hydrogen in the ammonia product, rather than hydrogen H 2 as was commonly the case in conventional methods and apparatus for synthesising ammonia. This enables the electrochemical synthesis of ammonia NH 3 without requiring a separate electrolysis stage to generate hydrogen H 2 , or the need to buy and store hydrogen H 2 , resulting in a much simpler system design.
  • a particular feature of the present invention is the solid catalyst 4 provided within the first volume 1.
  • the solid catalyst is provided in the form of a 3D grid structure. In another embodiment of the invention, the solid catalyst is provided in the form of a wool structure. Other structures may be used, such as spheres or other shapes made of, or coated with, a catalyst material.
  • the catalyst is provided on a relatively open structure: a 3D grid, a wool structure, spheres or other shapes and so on.
  • the structure may be made of the catalyst.
  • the relatively open structure ensures that fluids can pass through the catalyst structure relatively freely, in close proximity to the catalyst.
  • the structure such as the 3D grid, wool, spheres, other shapes etc. enables the catalyst to effectively be suspended in the nitride solution in such a way that (a) the steam injected through the inlet structure 22 has a good chance of interacting with the catalyst 4; (b) that the ion movement through the nitride conductor 20 is not significantly impeded by the presence of the catalyst and (c) ammonia NH 3 which is produced in the nitride conductor and at the surface of the catalyst can rise upwards to the enclosure 6 for collection.
  • Suitable catalyst materials include known Fe-based catalysts and Ru-based catalysts. A discussion of suitable catalysts is provided in reference [7].
  • the electrochemical cell and the synthesis method, of the present invention may be applied to the production of other gaseous products from first and second ionic components.
  • means are provided for introducing a first source material 5 (in the above example, steam H 2 O) into the first volume 1 and means are provided for introducing a second source material 26 (in the above example, nitrogen N 2 ) to a cathode 24.
  • An electrolyte in the above example in the form of the nitride conductor
  • Voltages +V and -V are applied respectively to the anode and cathode.
  • a first ionic component in the above example, N 3-
  • the first ionic component traverses the electrolyte under the influence of the voltage gradient between the anode and the ground electrode, towards the anode.
  • the first ionic component encounters the first source material, and a reaction takes place to generate a product (in the above example, ammonia NH 3 ) and an ionic by-product (in the above example, oxide ions O 2- ).
  • the ionic by-product continues to traverse the electrolyte under the influence of the voltage gradient between the anode and the ground electrode, towards the anode.
  • the ionic by-product gives up its charge and becomes an evolved by-product (in the above example, oxygen O 2 ).
  • Means should be provided to collect the product and preferably also the evolved by-product. Means may also be provided to collect any by-products generated at the anode or cathode.
  • anode is described as a gas electrode arranged for collection of a gaseous by-product, such arrangement may not be necessary in electrochemical cells set up to perform a different reaction. In such cases, it may be sufficient to provide a solid cathode, in which case the third volume 3 may be omitted.

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • Materials Engineering (AREA)
  • Metallurgy (AREA)
  • Organic Chemistry (AREA)
  • Inorganic Chemistry (AREA)
  • Electrolytic Production Of Non-Metals, Compounds, Apparatuses Therefor (AREA)
  • Catalysts (AREA)
  • Electrodes For Compound Or Non-Metal Manufacture (AREA)

Claims (13)

  1. Elektrochemische Zelle (10), die ein erstes Volumen aufweist, das den jeweiligen Oberflächen einer Anode (28) und einer Kathode (24) ausgesetzt ist, wobei die elektrochemische Zelle auch mit einem Dampfeinlass (5) versehen ist, um Dampf in das erste Volumen hineinzulassen, dadurch gekennzeichnet, dass die elektrochemische Zelle ferner Folgendes aufweist:
    - eine Umhausung (6), um ein innerhalb des ersten Volumens produziertes gasförmiges Produkt einzufangen, und
    - eine Struktur (4), die innerhalb des ersten Volumens unter der Umhausung (6) einen festen Katalysator aufweist, sodass ein auf einer Oberfläche des Katalysators freigesetztes gasförmiges Produkt durch die Umhausung (6) eingefangen wird,
    wobei der Katalysator eine relativ offene Struktur hat, sodass Fluide in unmittelbarer Nähe zu dem Katalysator die Katalysatorstruktur passieren können, wobei der Katalysator in dem ersten Volumen effektiv suspendiert ist.
  2. Elektrochemische Zelle nach Anspruch 1, wobei der feste Katalysator einen Fe-basierten Katalysator und/oder Rubasierten Katalysator, dem ersten Volumen ausgesetzt, aufweist.
  3. Elektrochemische Zelle nach Anspruch 1, wobei die Struktur (4), die einen festen Katalysator aufweist, in Form einer 3D-Gitterstruktur bereitgestellt wird.
  4. Elektrochemische Zelle nach Anspruch 1, wobei die Struktur (4), die einen festen Katalysator aufweist, in Form einer Wollstruktur bereitgestellt wird.
  5. Elektrochemische Zelle nach Anspruch 1, wobei die Struktur (4), die einen festen Katalysator aufweist, in Form von Kugeln oder anderen Formen, die aus einem Katalysatormaterial hergestellt oder damit beschichtet sind, bereitgestellt wird.
  6. Elektrochemische Zelle nach einem der vorhergehenden Ansprüche, wobei die Kathode (24) eine Gaselektrode ist, die eine poröse Kathode und ein zweites Volumen (2) aufweist.
  7. Elektrochemische Zelle nach einem der vorhergehenden Ansprüche, wobei die Anode (28) eine Gaselektrode ist, die eine poröse Anode und ein drittes Volumen (3) aufweist.
  8. Elektrochemische Zelle nach einem der vorhergehenden Ansprüche, wobei der Dampfeinlass (5) mit einem Dampfdiffusor versehen ist.
  9. Anordnung zur Herstellung eines gasförmigen Produkts aus ersten und zweiten Ausgangsstoffen, die Folgendes umfasst:
    - eine elektrochemische Zelle (10) nach einem der vorhergehenden Ansprüche 1 bis 8,
    - Mittel (5, 22) zum Einführen eines ersten Ausgangsstoffs in das erste Volumen (1)
    - Mittel (2, 24) zum Einführen eines zweiten Ausgangsstoffs (26) in das erste Volumen (1) und
    - einen in dem erstem Volumen bereitgestellter Elektrolyt (20)
  10. Anordnung nach Anspruch 9, ferner umfassend:
    - eine Stromversorgung (7), die angeordnet ist, um eine positive Spannung +V an die Anode (28) anzulegen und um eine negative Spannung -V an die Kathode (24) anzulegen.
  11. Verfahren zur Herstellung eines gasförmigen Produkts unter Verwendung einer Anordnung nach Anspruch 9, das die folgenden Schritte umfasst:
    - Anlegen einer positiven Spannung +V an die Anode (28),
    - Anlegen einer negativen Spannung -V an die Kathode (24),
    - Einführen des ersten Ausgangsstoffs in das erste Volumen (1),
    - Einführen des zweiten Ausgangsstoffs in ein zweites Volumen (2), das einer porösen Kathode ausgesetzt ist, wobei der zweite Ausgangsstoff an der Kathode reagiert, um in dem Elektrolyt in dem ersten Volumen (1) eine ionische Komponente bereitzustellen,
    - Erzeugen des gasförmigen Produkts durch Reaktion zwischen der ersten ionischen Komponente und dem ersten Ausgangsstoff und
    - Sammeln (6) des in dem ersten Volumen hergestellten gasförmigen Produkts.
  12. Verfahren nach Anspruch 11, ferner umfassend den Schritt des Sammelns eines an der Anode erzeugten Nebenprodukts.
  13. Verfahren nach einem der Ansprüche 11 bis 12, wobei
    - der erste Ausgangsstoff Dampf H2O ist,
    - die erste ionische Komponente Nitridionen N3- ist,
    - der zweite Ausgangsstoff Stickstoff N2 ist und
    - das gasförmige Produkt Ammoniak NH3 ist.
EP16788728.0A 2015-12-16 2016-11-02 Elektrochemische zelle und verfahren Not-in-force EP3390692B1 (de)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
GB1522169.0A GB2545444B (en) 2015-12-16 2015-12-16 An electrochemical cell with a steam inlet and a solid catalyst structure
PCT/EP2016/076452 WO2017102167A1 (en) 2015-12-16 2016-11-02 Electrochemical cell and process

Publications (2)

Publication Number Publication Date
EP3390692A1 EP3390692A1 (de) 2018-10-24
EP3390692B1 true EP3390692B1 (de) 2019-09-18

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EP16788728.0A Not-in-force EP3390692B1 (de) 2015-12-16 2016-11-02 Elektrochemische zelle und verfahren

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EP (1) EP3390692B1 (de)
JP (1) JP6952698B2 (de)
AU (1) AU2016369851B2 (de)
GB (1) GB2545444B (de)
WO (1) WO2017102167A1 (de)

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* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN113061912A (zh) * 2019-12-15 2021-07-02 中国科学院大连化学物理研究所 一种基于膜概念的中温电催化合成氨反应器

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JPS552765A (en) * 1978-06-23 1980-01-10 Natl Res Inst For Metals Production of hydrogen sulfide by electrolysis
US6881308B2 (en) * 2002-03-04 2005-04-19 Lynntech, Inc. Electrochemical synthesis of ammonia
WO2005078160A1 (ja) * 2004-02-18 2005-08-25 Ebara Corporation 水素の製造方法及び装置
JP5127385B2 (ja) * 2007-09-28 2013-01-23 学校法人同志社 アンモニア電解合成装置
JP5604204B2 (ja) * 2010-07-21 2014-10-08 日立造船株式会社 アンモニアの合成方法
WO2012129472A2 (en) * 2011-03-23 2012-09-27 Ceramatec, Inc. Ammonia synthesis using lithium ion conductive membrane
US10221491B2 (en) * 2012-06-29 2019-03-05 Australian Biorefining Pty Ltd Process and apparatus for generating or recovering hydrochloric acid from metal salt solutions
US10982339B2 (en) * 2014-04-25 2021-04-20 C2Cnt Llc Process for the production of ammonia from air and water

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Publication number Publication date
AU2016369851B2 (en) 2021-12-02
GB201522169D0 (en) 2016-01-27
GB2545444B (en) 2018-05-30
EP3390692A1 (de) 2018-10-24
WO2017102167A1 (en) 2017-06-22
GB2545444A (en) 2017-06-21
JP2019505663A (ja) 2019-02-28
JP6952698B2 (ja) 2021-10-20
AU2016369851A1 (en) 2018-05-17

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