WO2015082527A1 - Electrolytic cell equipped with concentric electrode pairs - Google Patents

Electrolytic cell equipped with concentric electrode pairs Download PDF

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Publication number
WO2015082527A1
WO2015082527A1 PCT/EP2014/076369 EP2014076369W WO2015082527A1 WO 2015082527 A1 WO2015082527 A1 WO 2015082527A1 EP 2014076369 W EP2014076369 W EP 2014076369W WO 2015082527 A1 WO2015082527 A1 WO 2015082527A1
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WIPO (PCT)
Prior art keywords
electrode
external
internal
electrodic
cell
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.)
Ceased
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PCT/EP2014/076369
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English (en)
French (fr)
Inventor
Mariachiara Benedetto
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.)
Industrie de Nora SpA
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Industrie de Nora SpA
Priority date (The priority date 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 date listed.)
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Publication date
Priority to CN201480064850.6A priority Critical patent/CN105793474B/zh
Priority to EP14806272.2A priority patent/EP3077577B1/en
Priority to AU2014359318A priority patent/AU2014359318B2/en
Priority to HK16109384.7A priority patent/HK1221268B/xx
Priority to ES14806272.2T priority patent/ES2663499T3/es
Priority to JP2016536698A priority patent/JP6511053B2/ja
Priority to EA201691158A priority patent/EA030848B1/ru
Priority to BR112016009720-3A priority patent/BR112016009720B1/pt
Application filed by Industrie de Nora SpA filed Critical Industrie de Nora SpA
Priority to US15/032,701 priority patent/US10023966B2/en
Priority to KR1020167017119A priority patent/KR102277620B1/ko
Priority to MX2016005653A priority patent/MX357177B/es
Publication of WO2015082527A1 publication Critical patent/WO2015082527A1/en
Priority to IL245083A priority patent/IL245083B/en
Anticipated expiration legal-status Critical
Ceased legal-status Critical Current

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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
    • C25B9/00—Cells or assemblies of cells; Constructional parts of cells; Assemblies of constructional parts, e.g. electrode-diaphragm assemblies; Process-related cell features
    • C25B9/70—Assemblies comprising two or more cells
    • C25B9/73—Assemblies comprising two or more cells of the filter-press type
    • C25B9/75—Assemblies comprising two or more cells of the filter-press type having bipolar electrodes
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    • C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F1/00—Treatment of water, waste water, or sewage
    • C02F1/46—Treatment of water, waste water, or sewage by electrochemical methods
    • C02F1/461—Treatment of water, waste water, or sewage by electrochemical methods by electrolysis
    • C02F1/46104—Devices therefor; Their operating or servicing
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    • C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F1/00—Treatment of water, waste water, or sewage
    • C02F1/46—Treatment of water, waste water, or sewage by electrochemical methods
    • C02F1/461—Treatment of water, waste water, or sewage by electrochemical methods by electrolysis
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    • C02F1/46109—Electrodes
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    • C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
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    • C02F1/00—Treatment of water, waste water, or sewage
    • C02F1/46—Treatment of water, waste water, or sewage by electrochemical methods
    • C02F1/461—Treatment of water, waste water, or sewage by electrochemical methods by electrolysis
    • C02F1/467—Treatment of water, waste water, or sewage by electrochemical methods by electrolysis by electrochemical disinfection; by electrooxydation or by electroreduction
    • C02F1/4672—Treatment of water, waste water, or sewage by electrochemical methods by electrolysis by electrochemical disinfection; by electrooxydation or by electroreduction by electrooxydation
    • C02F1/4674—Treatment of water, waste water, or sewage by electrochemical methods by electrolysis by electrochemical disinfection; by electrooxydation or by electroreduction by electrooxydation with halogen or compound of halogens, e.g. chlorine, bromine
    • 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
    • C25B1/24—Halogens or compounds thereof
    • C25B1/26—Chlorine; Compounds thereof
    • C—CHEMISTRY; METALLURGY
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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
    • C25B1/34—Simultaneous production of alkali metal hydroxides and chlorine, oxyacids or salts of chlorine, e.g. by chlor-alkali electrolysis
    • C25B1/46—Simultaneous production of alkali metal hydroxides and chlorine, oxyacids or salts of chlorine, e.g. by chlor-alkali electrolysis in diaphragm cells
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    • C25B11/00—Electrodes; Manufacture thereof not otherwise provided for
    • C25B11/02—Electrodes; Manufacture thereof not otherwise provided for characterised by shape or form
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    • C25B11/00—Electrodes; Manufacture thereof not otherwise provided for
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    • C25B11/036—Bipolar electrodes
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    • C25B11/055—Electrodes formed of electrocatalysts on a substrate or carrier characterised by the substrate or carrier material
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    • C25B11/073—Electrodes formed of electrocatalysts on a substrate or carrier characterised by the electrocatalyst material
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    • C25B11/073—Electrodes formed of electrocatalysts on a substrate or carrier characterised by the electrocatalyst material
    • C25B11/075—Electrodes formed of electrocatalysts on a substrate or carrier characterised by the electrocatalyst material consisting of a single catalytic element or catalytic compound
    • C25B11/081—Electrodes formed of electrocatalysts on a substrate or carrier characterised by the electrocatalyst material consisting of a single catalytic element or catalytic compound the element being a noble metal
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    • C25B15/02—Process control or regulation
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    • 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
    • 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
    • C25B9/60—Constructional parts of cells
    • C25B9/65—Means for supplying current; Electrode connections; Electric inter-cell connections
    • C—CHEMISTRY; METALLURGY
    • C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
    • C25C—PROCESSES FOR THE ELECTROLYTIC PRODUCTION, RECOVERY OR REFINING OF METALS; APPARATUS THEREFOR
    • C25C1/00—Electrolytic production, recovery or refining of metals by electrolysis of solutions
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    • C25C7/00—Constructional parts, or assemblies thereof, of cells; Servicing or operating of cells
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    • C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
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    • C25C7/00—Constructional parts, or assemblies thereof, of cells; Servicing or operating of cells
    • C25C7/02—Electrodes; Connections thereof
    • C—CHEMISTRY; METALLURGY
    • C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
    • C25C—PROCESSES FOR THE ELECTROLYTIC PRODUCTION, RECOVERY OR REFINING OF METALS; APPARATUS THEREFOR
    • C25C7/00—Constructional parts, or assemblies thereof, of cells; Servicing or operating of cells
    • C25C7/04—Diaphragms; Spacing elements
    • C—CHEMISTRY; METALLURGY
    • C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F1/00—Treatment of water, waste water, or sewage
    • C02F1/46—Treatment of water, waste water, or sewage by electrochemical methods
    • C02F1/461—Treatment of water, waste water, or sewage by electrochemical methods by electrolysis
    • C02F1/46104—Devices therefor; Their operating or servicing
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    • C02F2001/46128—Bipolar electrodes
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    • C02F1/46—Treatment of water, waste water, or sewage by electrochemical methods
    • C02F1/461—Treatment of water, waste water, or sewage by electrochemical methods by electrolysis
    • C02F1/46104—Devices therefor; Their operating or servicing
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    • C02F1/00—Treatment of water, waste water, or sewage
    • C02F1/46—Treatment of water, waste water, or sewage by electrochemical methods
    • C02F1/461—Treatment of water, waste water, or sewage by electrochemical methods by electrolysis
    • C02F1/46104—Devices therefor; Their operating or servicing
    • C02F1/46109—Electrodes
    • C02F2001/46133—Electrodes characterised by the material
    • C02F2001/46138—Electrodes comprising a substrate and a coating
    • C02F2001/46142—Catalytic coating
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    • C02F1/46—Treatment of water, waste water, or sewage by electrochemical methods
    • C02F1/461—Treatment of water, waste water, or sewage by electrochemical methods by electrolysis
    • C02F1/46104—Devices therefor; Their operating or servicing
    • C02F1/46109—Electrodes
    • C02F2001/46133—Electrodes characterised by the material
    • C02F2001/46138—Electrodes comprising a substrate and a coating
    • C02F2001/46147—Diamond coating
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    • C02F1/00—Treatment of water, waste water, or sewage
    • C02F1/46—Treatment of water, waste water, or sewage by electrochemical methods
    • C02F1/461—Treatment of water, waste water, or sewage by electrochemical methods by electrolysis
    • C02F1/46104—Devices therefor; Their operating or servicing
    • C02F1/46109—Electrodes
    • C02F2001/46152—Electrodes characterised by the shape or form
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    • C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F1/00—Treatment of water, waste water, or sewage
    • C02F1/46—Treatment of water, waste water, or sewage by electrochemical methods
    • C02F1/461—Treatment of water, waste water, or sewage by electrochemical methods by electrolysis
    • C02F1/46104—Devices therefor; Their operating or servicing
    • C02F1/46109—Electrodes
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    • C02F2201/00—Apparatus for treatment of water, waste water or sewage
    • C02F2201/46—Apparatus for electrochemical processes
    • C02F2201/461—Electrolysis apparatus
    • C02F2201/46105—Details relating to the electrolytic devices
    • C02F2201/4612—Controlling or monitoring
    • C02F2201/46125—Electrical variables
    • C02F2201/4613—Inversing polarity
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    • C02F2201/46—Apparatus for electrochemical processes
    • C02F2201/461—Electrolysis apparatus
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    • C02F2201/46—Apparatus for electrochemical processes
    • C02F2201/461—Electrolysis apparatus
    • C02F2201/46105—Details relating to the electrolytic devices
    • C02F2201/4616—Power supply

Definitions

  • the invention relates to a bipolar-type electrochemical cell and to a method of carrying out electrolytic processes therein.
  • the invention relates to a bipolar electrolytic cell suitable for electrochemical processes carried out with periodic reversal of the polarity.
  • the periodic polarity reversal of electrochemical cells whereby each of the electrodes works alternatively as anode and as cathode for preset intervals of time, is a measure known in the art especially for preventing the formation of scaling of various kind on the surface of one of the electrodes, usually the cathode.
  • the anode is often subjected to the deposition of polluting films, in this case consisting of organic residues which tend to oligomerise upon the electrode surface, and which sometimes may be removed by the mechanical and chemical action of nascent hydrogen in the subsequent cathodic cycle.
  • polluting films in this case consisting of organic residues which tend to oligomerise upon the electrode surface, and which sometimes may be removed by the mechanical and chemical action of nascent hydrogen in the subsequent cathodic cycle.
  • the electrodes installed in the cells destined to work alternatingly as anodes and as cathodes, besides being spaced at constant gap must preferably be of the same size, so that it is possible to keep both current supplied and operating voltage constant (except for the change of sign).
  • the invention relates to a bipolar electrolysis cell delimited by an external body housing in its interior:
  • an external electrodic pair subdivided into two electrodes, separated at the edges by means of insulating elements, destined to operate alternatingly the one as the cathode and the other as the anode, and vice versa;
  • an internal electrode pair concentric to the first two, so as to delimit a second gap of generally constant width with the intermediate electrode pair;
  • the internal electrode pair being also subdivided into two electrodes, separated at the edges by means of insulating elements, destined to operate alternatingly the one as the cathode and the other as the anode, and vice versa, each of the two electrodes of the pair facing one of two electrodes of the intermediate pair;
  • the external cell body has an elongated shape and the electrode pair have prismatic or cylindrical shape.
  • the external cell body and the electrode pairs have a spheroidal shape.
  • both the anodic area and the cathodic area correspond to the sum of the areas of half the external electrode pair and half the internal electrode pair: by reversing the electrode polarity, the values of the anodic and of the cathodic area are unchanged.
  • both the cell body and the electrode pairs have either a prismatic or a cylindrical shape. It can be advantageous for instance to couple a cylindrical cell body with electrode pairs also cylindrical, in order to minimise the cell volume not engaged in the electrolysis reaction.
  • the two concentric electrode pairs are coaxial to the cell body. This can also have the advantage of minimising the cell volume not engaged in the electrolysis reaction.
  • all the electrodes of the cell are made of titanium or other valve metal coated with a catalytic composition containing one or more components selected from the group of platinum such as platinum metal or oxides of platinum, ruthenium or iridium.
  • the above catalytic composition also contains oxides capable of favouring the growth of compact and protective films, for instance oxides of titanium, tantalum, niobium or tin.
  • oxides capable of favouring the growth of compact and protective films for instance oxides of titanium, tantalum, niobium or tin.
  • electrode made of titanium or other valve metals is used to designate an electrode obtained starting from a substrate of titanium or other valve metal (such as for example niobium, tantalum or zirconium) either pure or differently alloyed.
  • all the electrodes of the cell are made of conductive diamond, for instance boron-doped diamond, either in massive form or supported on a suitable conductive substrate, for instance of niobium or other valve metal.
  • the specified materials have the advantage of working in an optimum fashion for the vast majority of known anodic applications, involving the evolution of anodic products such as chlorine, oxygen, ozone or peroxides, at the same time guaranteeing a correct functioning also as cathodes.
  • the first and second gap have a generally constant width independently ranging between 1 and 20 mm, depending on the needs of each process, as it will be clear to a person skilled in the art.
  • the invention relates to the method of execution of an electrolytic process comprising feeding a process electrolyte inside the gaps of an electrolysis cell as hereinbefore described and supplying direct electric current to the cell poles, varying the direction of the applied current at preset time intervals, for instance every 1 -120 minutes.
  • the electrolytic process according to the invention consists of the electrolysis of a salt solution with production of active chlorine. In one alternative embodiment, the electrolytic process according to the invention consists of a wastewater treatment with degradation of organic substances. In a further embodiment, the electrolytic process according to the invention consists of a metal recovery by cathodic electrodeposition, with optional simultaneous degradation of organic species.
  • Fig. 1 shows a top-view of a section of a cell according to one embodiment of the invention comprising a cylindrical body and prism-shaped electrode pairs.
  • Fig. 2 shows a top-view of a section of a cell according to one embodiment of the invention comprising a cylindrical body and cylinder-shaped electrode pairs.
  • FIG. 1 shows a top-view of a section of one embodiment of the invention consisting of a cell delimited by a cylindrical body 100 in whose interior three parallelepiped-shaped electrode pairs are housed, namely: an internal pair consisting of electrodes 301 and 401 separated at the edges by means of insulating elements 101 , an intermediate pair consisting of electrodes 501 and 502 and an external pair coaxial to the internal pair consisting of electrodes 302 and 402; also the electrodes of the intermediate and of the external pair are separated at the edges by means of equivalent insulating elements 101 .
  • Insulating elements 101 keep the electrodes in fixed position, preventing the short- circuiting thereof: besides performing these functions, elements 101 avoid current to be concentrated at the facing edges of each electrode pair. For such reason, elements 101 must be suitably dimensioned: inventors found out that for most of tested applications, it can be advantageous to dimension elements 101 so that the distance between the facing edges of each electrode pair is at least equal to the width of respective gaps 102 and 1 12. Electrodes 402 and 501 face each other, just like electrodes 302 and 502, so as to define first gap 102, of generally constant width except for the corner regions.
  • electrodes 302 and 501 face each other, just like electrodes 401 and 502, so as to define second gap 1 12, of generally constant width except for the corner regions.
  • Electrode 301 of the internal pair and electrode 302 of the external pair not facing bipolar electrode 501 in its turn facing the same electrode 301 are connected to one pole 300 of a direct power supply 200 provided with means for reversing the direction of current at preset intervals of time; similarly, the other electrode 401 of the internal pair and the other electrode 402 of the external pair are connected to the other pole 400 of direct power supply 200.
  • Regions 103 and 104 of the cell body outside the two adjacent gaps 102 and 1 12 are filled with insulating material, so as to confine the process electrolyte inside said gaps constituting the zone of reaction.
  • the cell can be fed from a terminal part of cylindrical body 100 with the outlet on the opposite site and can optionally operate in continuous mode, with a single pass of electrolyte, or in batch mode.
  • Fig. 2 shows a top-view of a section of a similar embodiment of the invention, differing from the previous one in the cylindrical shape of electrode pairs. This has the advantage of keeping the width of gaps 102 and 1 12 constant, eliminating the corner regions besides maximising the ratio of active electrode surface to total cell volume.
  • a cell corresponding to the embodiment of Fig.2 except for being equipped with two intermediate pairs of bipolar electrodes was fed from the relative gaps with a brine solution prepared from tap water containing 19 g/l of NaCI.
  • the cell was equipped with a 60 mm diameter external electrode pair, a 30 mm diameter internal electrode pair and with 50 mm and 40 mm diameter intermediate bipolar electrode pairs, respectively, defining gaps of approximately 4 mm in width. All electrode pairs had a height of 50 mm.
  • All electrodes of the various pairs consisted of a titanium sheet activated on the side facing the gap with a mixture of oxides of ruthenium, palladium and titanium according to the prior art.
  • the total reaction volume, corresponding to the volume of the two gaps, was 32.5 ml.

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PCT/EP2014/076369 2013-12-03 2014-12-03 Electrolytic cell equipped with concentric electrode pairs Ceased WO2015082527A1 (en)

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EA201691158A EA030848B1 (ru) 2013-12-03 2014-12-03 Электролитическая ячейка, снабженная концентрическими электродными парами
AU2014359318A AU2014359318B2 (en) 2013-12-03 2014-12-03 Electrolytic cell equipped with concentric electrode pairs
HK16109384.7A HK1221268B (en) 2013-12-03 2014-12-03 Electrolytic cell equipped with concentric electrode pairs
ES14806272.2T ES2663499T3 (es) 2013-12-03 2014-12-03 Celda electrolítica equipada con pares de electrodos concéntricos
JP2016536698A JP6511053B2 (ja) 2013-12-03 2014-12-03 同心状電極対を装備した電解セル
BR112016009720-3A BR112016009720B1 (pt) 2013-12-03 2014-12-03 Pilha de eletrólise bipolar e método de execução de um processo eletrolítico em uma pilha
US15/032,701 US10023966B2 (en) 2013-12-03 2014-12-03 Electrolytic cell equipped with concentric electrode pairs
CN201480064850.6A CN105793474B (zh) 2013-12-03 2014-12-03 配备有同轴电极对的电解槽
EP14806272.2A EP3077577B1 (en) 2013-12-03 2014-12-03 Electrolytic cell equipped with concentric electrode pairs
KR1020167017119A KR102277620B1 (ko) 2013-12-03 2014-12-03 동심 전극 쌍들을 구비한 전해 셀
MX2016005653A MX357177B (es) 2013-12-03 2014-12-03 Celula electrolitica equipada con pares de electrodos concentricos.
IL245083A IL245083B (en) 2013-12-03 2016-04-13 An electrolytic cell equipped with concentric electrode pairs

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IT002015A ITMI20132015A1 (it) 2013-12-03 2013-12-03 Cella elettrolitica dotata di coppie concentriche di elettrodi
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EP3077577A1 (en) 2016-10-12
ES2663499T3 (es) 2018-04-13
EA030848B1 (ru) 2018-10-31
JP2017503916A (ja) 2017-02-02
US20160251763A1 (en) 2016-09-01
US10023966B2 (en) 2018-07-17
BR112016009720B1 (pt) 2021-10-13
EP3077577B1 (en) 2018-02-07
EA201691158A1 (ru) 2016-09-30
IL245083A0 (en) 2016-06-30
MX2016005653A (es) 2016-08-11
AU2014359318B2 (en) 2018-08-02
CN105793474B (zh) 2017-11-10
HK1221268A1 (zh) 2017-05-26
JP6511053B2 (ja) 2019-05-08
TW201522715A (zh) 2015-06-16
TWI652374B (zh) 2019-03-01
KR102277620B1 (ko) 2021-07-19
IL245083B (en) 2019-01-31
ITMI20132015A1 (it) 2015-06-04
MX357177B (es) 2018-06-28
BR112016009720A2 (enExample) 2017-08-01
CN105793474A (zh) 2016-07-20
KR20160093650A (ko) 2016-08-08

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