US3879279A - Electrode with exchangeable membrane - Google Patents

Electrode with exchangeable membrane Download PDF

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Publication number
US3879279A
US3879279A US202416A US20241671A US3879279A US 3879279 A US3879279 A US 3879279A US 202416 A US202416 A US 202416A US 20241671 A US20241671 A US 20241671A US 3879279 A US3879279 A US 3879279A
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United States
Prior art keywords
shaft
electrode
membrane
fluid tight
electrode shaft
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US202416A
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English (en)
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Friedrich Gustav Karl Baucke
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Schott AG
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Jenaer Glaswerk Schott and Gen
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    • G—PHYSICS
    • G01—MEASURING; TESTING
    • G01N—INVESTIGATING OR ANALYSING MATERIALS BY DETERMINING THEIR CHEMICAL OR PHYSICAL PROPERTIES
    • G01N27/00—Investigating or analysing materials by the use of electric, electrochemical, or magnetic means
    • G01N27/26—Investigating or analysing materials by the use of electric, electrochemical, or magnetic means by investigating electrochemical variables; by using electrolysis or electrophoresis
    • G01N27/28—Electrolytic cell components
    • G01N27/30—Electrodes, e.g. test electrodes; Half-cells
    • G01N27/333—Ion-selective electrodes or membranes

Definitions

  • the invention relates to an electrode with an exchangeable ion-sensitive membrane for measuring ion activities in solutions. suspensions, pastes. or the like. which electrode may be constructed as measuring electrode or single-bar measuring chain.
  • the invention is characterized in that the membrane is incorporated in the electrode shaft and the surface of the ion-sensitive membrane which is in contact with the solution to be measured forms a portion of the outer wall of the electrode shaft. ln a particular embodiment of the electrode there is provided. in the electrode shaft. two or more exchangeable membranes for the simultaneous measurement of the activities of two or more different ions.
  • lon membranes can be employed in a great variety of types. e.g. they may consist of:
  • porous bodies imbued with a usually organic solution of an ion exchanger 4. porous bodies imbued with a usually organic solution of an ion exchanger.
  • Electrodes for measuring ion activities are known (British Pat. No. 1.198.589) wherein a membrane 1 (FIG. 1a) which separates a solution 4 in the inner space ofthe electrode from the solution to be measured and on the outer surface 111 of which electrode the potential determined by the activity of the ions concerned of the solution to be measured is generated, is fastened by means of an adhesive or cement 2 at the base of the electrode shaft 3.
  • the adhesive or cement 2 must furthermore seal the gap between shaft and membrane to such an extent that the liquid to be measured cannot enter the electrode and thus mix with the inside solutuion thereof.
  • the inside solution must of course not leak from the electrode into the solution to be measured.
  • the present invention overcomes all these disadvantages in the simplest manner by the device that the membrane does not. as was hitherto the case. form the base end, namely a portion of the base of the electrode shaft but is inserted as intermediate ring or as window" in the round or angular shaft of the electrode.
  • the cohesion of the electrode parts namely electrode base, intermediate ring or window (membrane) and electrode top is assured by a screwed joint within the electrode.
  • the seal between the individual parts may consist of elastic gasket rings or an elastic cement.
  • the membrane is not rigidly connected with the shaft but is exchangeable
  • the electrode is shaped as a straight shaft without any projections and can be inserted in appliances or equipment through normal openings provided therefor, such as cuts or inserted tubes.
  • the ratio between the size of the surface and the distance between inner and outer surface can be selected at will within a wide range. This can be of great importance since the ratio between the size of the surface and the distance between inner and outer surface must be adapted to the conductivity of the membrane material used.
  • Membranes with inside contacts by liquids e.g. electrolyte solutions. as well as by solid state bodies. e.g. metals, can be produced.
  • Electrodes with two or more different membranes for simultaneous measurement of activities of different ions can be produced, one of which membranes, insofar as the constancy. in the solution to be measured, of the ion activity which determines its potential is assured, can be used as reference electrode membrane.
  • an electrode for measuring ion activities.
  • the electrode comprises an electrode shaft and an ion sensitive membrane.
  • the electrode shaft is divided into an upper portion and a lower portion.
  • the ion sensitive membrane is located between the upper and lower portions of the shaft.
  • the outer surface of the membrane is adapted to contact the material whose ion activity is to be measured.
  • the ion sensitive membrane is in the form of an annular ring. whereas in another embodiment of the present invention, it is in the form of a window which can have a curved or planar outer surface.
  • the electrode further comprises a second membrane for measuring the activity of a second ion.
  • the outer wall of the electrode shaft is substantially co-extensive with the outer wall of the membrane. This permits the electrodes of the present invention to be inserted into chemical process equipment through the holes characteristically provided for prior art electrodes.
  • the electrode When the electrode contains a single ion sensitive membrane in the form of an annular ring, the top of the ring forms a fluid tight seal with the upper portion of the electrode shaft, whereas the bottom of the ring forms a fluid tight seal with the lower portion of the electrode shaft.
  • the electrode is provided with means for pressing the upper and lower portions of the electrode shaft against the ring in order to maintain fluid seals. This can be accomplished according to one embodiment by a tension shaft and according to another embodiment by providing threads on a portion of the electrode shaft.
  • the tension shaft is preferably fixed to the lower portion of the electrode shaft and extends through the annulus of the ring and through and beyond the hollow upper portion of the electrode shaft.
  • the tension shaft further extends beyond the upper extremity of the upper portion of the electrode shaft.
  • the end of the tension shaft is provided with threads having a nut thereon.
  • a force transmitting member is slidably mounted on the tension shaft between the nut and the upper extremity of the upper portion of the electrode shaft. This force transmitting member extends laterally to contact the upper extremity of the upper portion of the electrode shaft. The force transmitting member exerts a force on this portion of the electrode shaft.
  • the means for pressing the upper and lower portions of the electrode shaft against the ring is accomplished by providing the hollow upper portion of the shaft with internal threads adjacent to the lower extremity of the upper portion.
  • the lower portion of the electrode shaft is provided with an externally threaded member which engages the internal threads of the upper portion.
  • the ion-sensitive membrane in the form of an annular ring surround the externally threaded member.
  • the electrode is provided with a second chamber within the upper portion of the electrode shaft.
  • the first chamber is, or course, formed by the upper and lower portions of the electrode shaft and the membrane.
  • a sensing electrode is located in the first chamber, and a reference electrode is located in the second chamber.
  • the electrode shaft has an intermediate portion in addition to the upper and lower portions.
  • a first ion sensitive membrane is located between the upper and the intermediate portions whereas a second ion-sensitive membrane is located between the lower and the intermediate portions.
  • the sealing is preferably accomplished by providing the upper and lower portions of the electrode shaft each with a planar surface at right angles to the center line of the electrode shaft.
  • the intermediate portion of the electrode shaft is also provided with two such planar surfaces. one designated an upper planar surface. the other designated a lower planar surface.
  • the first ion sensitive membrane is located between the upper and the intermediate portions of the shaft. This ion-sensitive membrane is in the form of an annular ring.
  • the ring has an upper planar surface adapted to form a fluid tight seal with the planar surface of the upper portion of the shaft.
  • the ring also has a lower planar surface adapted to form a fluid tight seal with the planar surface of the intermediate portion of the shaft.
  • the second ion-sensitive membrane is similarly situtated between the intermediate portion of the shaft and the lower portion of the shaft.
  • a first fluid tight chamber is defined by the upper portion of the shaft, the intermediate portion of the shaft. and the first membrane.
  • a second fluid tight chamber is defined by the lower portion of the shaft, the intermediate portion of the shaft, and the second membrane. Electrodes may be located within each of these fluid tight chambers together with appropriate ionic solutions. The electrodes of the present invention are characteristically sold and shipped without the ionic solution in place.
  • FIG. la is a partial cross-sectional diagram of a prior art electrode.
  • FIG. lb is a partial cross-sectional diagram of a second prior art electrode.
  • FIG. 2 illustrates one electrode according to the present invention.
  • FIG. 2a illustrates an alternate embodiment for a base for the device of FIG. 2.
  • FIG. 3 illustrates an alternate electrical connection for the device of FIG. 2.
  • FIG. 4 illustrates another embodiment of the electrode according to the invention using a different membrane level.
  • FIG. 5 illustrates another electrode construction
  • FIG. 6 illustrates the base of an electrode as in FIG. 2, but using a two-layer membrane.
  • FIG. 7 illustrates a single-bar measuring circuit with a ring-shaped electrode.
  • FIG. 8 illustrates a single-bar measuring circuit with a plate-shaped electrode.
  • FIG. 9 illustrates a double electrode with two ringshaped membranes.
  • FIG. 10 illustrates an electrode on whose membrane the electric connection is fastened by means of a solid state element.
  • FIG. 11 illustrates an electrode with a semiconductor membrane.
  • FIG. 2 shows an electrode of the invention with a ring'shaped membrane I whose surface lb is in contact with the inner solution 4 of the electrode and whose surface la is in contact with the solution to be measured.
  • the electrode contains the following parts: a base 5, a membrane 1, gasket rings or elastic cement 2, an electrode shaft 3, electrode head sealings 2a and 211, an electrode cover 8 and one or more supporting discs 10.
  • a nut 9 supported by that portion of shaft 6 which is provided with threads 6a compresses under a pressure of optional value these individual parts of the electrode.
  • the electrode is held together and sealed by a tension and compression arrangement. The tension occurs when nut 9 is tightened along tension shaft 6, upon which nut 9 sits. As the nut is turned, tension is exerted on tension shaft 6 which is fixed to base 5 of the lower portion of the electrode shaft. The tension is therein converted, via the force-transmitting cover 8, into compression conveyed along shaft 3 to rings 2.
  • Shaft 6 which may consist e.g. of plastic, may be a portion of base 5 or may be screwed at 511 into the latter.
  • the construction is centered by a guide 517 in base 5, and a guide 312 in shaft 3.
  • cover 8 of the electrode should contain a guide 8a.
  • the electric connection 12 of an inside shunt electrode 11 projecting into the inner solution 4 of the electrode may either. as shown in FIG. 2, be tightly cemented into cover 8 or, as indicated e.g. in FIGS. 3 and 4, pass through a bore in shaft 6.
  • the top end of the electrode consists suitably of cap 13 which is screwed by means of a thread 13a onto shaft 3 or, if the electric connection 12 passes through shaft 6, onto the spiral section 6a of shaft 6, as shown in FIGS. 3 and 4.
  • Other shapes of the electrode top end are of course also possible.
  • FIG. 3 shows that. e.g., electrode shaft 3 may be provided with a stationary perforated end 8b against which electrode cap 13, which at 6a is provided with a thread. is screwed from the top.
  • the sealing consists in this case also of a gasket ring 2a which is pressed. together with a supporting disc 10, between end 8! and cap 13.
  • FIG. 2a shows an embodiment wherein base 5 is screwed by means of a thread 5d directly, i.e. without the use of a shaft. to a thread within electrode shaft 3, whereby base 5, gasket rings or coment 2, membrane 1 and shaft 3 are pressed together under any pressure and seal the electrode.
  • the section 5e of base 5 which is provided with thread 5d must of course be perforated once or repeatedly in order to make possible a contact of inner solution 4 and surface lb of the membrane. This is shown by a shaded area 5f of FIG. 2a.
  • FIG. 4 shows an embodiment similar to that of FIG. 2.
  • the membrane is positioned at a higher level than in FIG. 2 and arranged between shaft 3 and base 5 which constitutes a portion of shaft 50.
  • This embodiment can be of interest if inner solution 4 of the electrode is to be in contact with a base material. eg a salt with which solution 4 is saturated, but a contact. e.g. at a temperature change, with or without crystallization of this salt on membrane 1 is to be avoided.
  • FIG. 5 shows an electrode construction wherein an-- other ratio between the size of surface la relative to the distance between inner surface lb and outer surface In ofmcmbrane 1 has been chosen, than e.g. in FIG. 2.
  • the membrane thus constitutes also an intermediate ring, its shape is rather that of a perforated round plate.
  • Guidance is in this example provided by means of a groove 1e on the outer edge of membrane 1.
  • FIG. 6 shows the base of an electrode as shown in FIG. 2.
  • the membrane used in the present case is a two-layer membrane consisting of a layer Id which at 1b is in contact with the inner solution and a layer 1c which at la is in contact with the solution to be measured.
  • the advantages of the use of a membrane consisting of two or more layers are described in U.S Pat. application Ser. No. 169,674 filed Aug. 6, I971. The said figure does not show a screwed joint which can be carried out according to the principle of FIG. 2 or FIG. 20.
  • FIGS. 7 and 8 show two embodiments of a single-bar measuring chain with. respectively, a ring-shaped membrane (FIG. 7) and a plate-shaped membrane (FIG. 8).
  • a single-bar measuring chain presents an electrode unit which has a measuring membrane and also a reference electrode. i.e. a membrane which is in contact with the solution to be measured and with the inner shunt, and also a reference electrode in a reference electrode solution.
  • a double shaft 3 of these single-bar measuring chains consists of one piece and can be produced very simply e.g. from glass tubes, but may also consist of another material, e.g. plastic.
  • An opening 16 (FIG. 7) permits the replacement of portions of the electrolyte solution 14 of reference electrode 15 which have leaked through a diaphragm 17 (FIGS. 7 and 8).
  • connection 12 to the inner shunt electrode 11 passes in FIG. 7 through a bore in shaft 6.
  • the connection 15a to reference electrode 15 is tightly cemented into electrode cover 8.
  • the embodiment of FIG. 8 has particularly long insulation paths radially to gasket rings 2.
  • FIG. 9 shows a double electrode with two ringshaped membranes 1 and 18 which respond to different ions in the solution to be measured.
  • Flat. plate-shaped perforated membranes may be used in place of the ring-shaped high membranes.
  • one of the membranes may be used as reference electrode. which is always possible when the activity of one of the ion types to be measured of the solution to be measured is constant.
  • the shaping of an inner shaft 19 which has at its bottom end an expansion 19a with a guide for each of membranes 1 and 18 is particularly simple.
  • one (12) of the feed lines to the shunt electrodes passes through shaft 6, the other (21a) through cover 8 of the electrode.
  • Numeral indicates the electrolyte solution which is in contact with membrane l8 and shunt electrode 21.
  • FIG. 10 shows an embodiment of such an electrode on whose membrane 1 the electric connection 22 is fastened by means of a solid state element If.
  • the membranes used need not necessarily be ringshaped and form a full circle of an ion-sensitive surface; they may also be installed as a window" tapering towardthe outside and having a curved or planar front surface in a round shaft or a shaft provided with planar surfaces.
  • FIG. 11 shows e.g. an embodiment with a semicircular membrane 1 which has planar. parallel front surfaces In and 112.
  • Several different membranes of this type can be incorporated in a shaft. which is particularly simple if each has a solid state contact.
  • An electrode for measuring ion activities comprising:
  • An electrode for measuring ion activities comprising:
  • said ring having: I. an upper flat surface having a plane adapted to form a fluid tight seal with the flat surface having a plane of the upper portion of the electrode shaft.
  • tension shaft fixed to the lower portion of the electrode shaft and extending through the annulus of the ring. through and beyond the hollow upper portion of the electrode shaft and extending beyond the upper extremity of the upper portion of the electrode shaft. the end of the tension shaft having threads.
  • a force transmitting member slidably mounted on the tension shaft between the nut and the upper extremity of the upper portion of the electrode shaft. the force transmitting member extending laterally to contact and exert force on the upper extremity of the upper portion of the electrode shaft,
  • An electrode for measuring ion activities comprising:
  • an electrode shaft comprising:
  • a hollow upper portion having:
  • An electrode for measuring ion activities comprising:
  • An electrode for measuring ion activities of two ions comprising:
  • D. means for axially compressing the two membranes and the three portions of the shaft in order to maintain the fluid tight integrity of the two chambers.
  • An electrode for measuring ion activities of two ions comprising:
  • an intermediate portion having an upper flat surface having a plane and a lower flat surface having a plane
  • a first ion sensitive membrane between the upper and intermediate portions of the shaft wherein the membrane is in the form of an annular ring.
  • said ring having: I. an upper flat surface having a plane adapted to form a fluid tight seal with the flat surface having a plane of the upper portion of the shaft, 2. a lower flat surface having a plane adapted to form a fluid tight seal with the flat surface having a plane of the intermediate portion of the shaft, C. a second ion sensitive membrane between the lower and intermediate portions of the shaft wherein the membrane is in the form of an annular ring.
  • said ring having: 1.
  • a nut on the threads F. a force transmitting member slidably mounted on the tension shaft between the nut and the upper extremity of the upper portion of the electrode shaft. the force transmitting member extending laterally to contact and exert force on the upper extremity of the upper portion of the electrode shaft, wherein a first fluid tight chamber is defined by:
  • a second fluid tight chamber is defined by:

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  • Chemical & Material Sciences (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Health & Medical Sciences (AREA)
  • Biochemistry (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • Physics & Mathematics (AREA)
  • Analytical Chemistry (AREA)
  • Molecular Biology (AREA)
  • General Health & Medical Sciences (AREA)
  • General Physics & Mathematics (AREA)
  • Immunology (AREA)
  • Pathology (AREA)
  • Investigating Or Analyzing Materials By The Use Of Electric Means (AREA)
  • Separation Using Semi-Permeable Membranes (AREA)
  • Physical Or Chemical Processes And Apparatus (AREA)
US202416A 1970-12-03 1971-11-26 Electrode with exchangeable membrane Expired - Lifetime US3879279A (en)

Applications Claiming Priority (1)

Application Number Priority Date Filing Date Title
DE2059559A DE2059559C3 (de) 1970-12-03 1970-12-03 Elektrode mit auswechselbarer Membran zur Messung von lonenaküvitäten

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DE (1) DE2059559C3 (enrdf_load_stackoverflow)
GB (1) GB1304498A (enrdf_load_stackoverflow)
NL (1) NL7115526A (enrdf_load_stackoverflow)

Cited By (17)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US4008141A (en) * 1974-10-04 1977-02-15 Horiba, Ltd. Combination pH electrode
US4052285A (en) * 1975-03-20 1977-10-04 National Research Development Corporation Ion selective electrodes
US4116796A (en) * 1975-04-23 1978-09-26 Radelkis Elektrokemiai Muszergyarto Szovetkezet Selective halide and sulfide sensitive electrodes
US4135999A (en) * 1975-01-27 1979-01-23 Dr. E. Fresenius Chemisch Pharmazeutische Industrie Kg, Apparatebau Kg Ion sensitive electrode and cells for use therewith
US4314895A (en) * 1978-07-17 1982-02-09 Nova Biomedical Corporation Method of making liquid membrane electrode
US4519973A (en) * 1983-08-03 1985-05-28 Medtronic, Inc. Ion selective membranes for use in ion sensing electrodes
WO1986000137A1 (en) * 1984-06-11 1986-01-03 Bukamier Gary L Improvements in electrochemical sensors
US4565666A (en) * 1983-08-03 1986-01-21 Medtronic, Inc. Method of producing combination ion selective sensing electrode
US4565665A (en) * 1983-08-03 1986-01-21 Medtronic, Inc. Flow through ion selective electrode
US4600495A (en) * 1983-08-03 1986-07-15 Medtronic, Inc. Flow through ion selective electrode
US4783252A (en) * 1987-03-02 1988-11-08 Rosemount Inc. Lateral indicator sensor
US4891123A (en) * 1987-04-10 1990-01-02 Frantztech Ltd. Electrochemical analyzer for measuring the concentration of atoms or molecules in a fluid and method of making same
US4908119A (en) * 1986-09-01 1990-03-13 Nippondenso Co., Ltd. Apparatus for determining oxygen concentration
US5558756A (en) * 1994-11-15 1996-09-24 Cominco Ltd. Method for geo-electrochemical sampling
US6398931B1 (en) * 2000-01-31 2002-06-04 Phoenix Electrode Company Combination ion-selective electrode with a replaceable sensing membrane
EP1098192A3 (de) * 1999-11-05 2004-01-14 M.K. Juchheim GmbH & Co. Indikatorelektrode mit einer sensitiven Oberfläche und Verwendung hierfür
CN102265146A (zh) * 2008-12-22 2011-11-30 恩德莱斯和豪瑟尔测量及调节技术分析仪表两合公司 离子选择电极

Citations (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3216915A (en) * 1961-12-12 1965-11-09 Beckman Instruments Inc Flow cell for ion potential measurements
US3591464A (en) * 1968-09-06 1971-07-06 Orion Research Method and apparatus for detecting ionic activity

Patent Citations (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3216915A (en) * 1961-12-12 1965-11-09 Beckman Instruments Inc Flow cell for ion potential measurements
US3591464A (en) * 1968-09-06 1971-07-06 Orion Research Method and apparatus for detecting ionic activity

Cited By (19)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US4008141A (en) * 1974-10-04 1977-02-15 Horiba, Ltd. Combination pH electrode
US4135999A (en) * 1975-01-27 1979-01-23 Dr. E. Fresenius Chemisch Pharmazeutische Industrie Kg, Apparatebau Kg Ion sensitive electrode and cells for use therewith
US4052285A (en) * 1975-03-20 1977-10-04 National Research Development Corporation Ion selective electrodes
US4116796A (en) * 1975-04-23 1978-09-26 Radelkis Elektrokemiai Muszergyarto Szovetkezet Selective halide and sulfide sensitive electrodes
US4314895A (en) * 1978-07-17 1982-02-09 Nova Biomedical Corporation Method of making liquid membrane electrode
US4565665A (en) * 1983-08-03 1986-01-21 Medtronic, Inc. Flow through ion selective electrode
US4565666A (en) * 1983-08-03 1986-01-21 Medtronic, Inc. Method of producing combination ion selective sensing electrode
US4519973A (en) * 1983-08-03 1985-05-28 Medtronic, Inc. Ion selective membranes for use in ion sensing electrodes
US4600495A (en) * 1983-08-03 1986-07-15 Medtronic, Inc. Flow through ion selective electrode
WO1986000137A1 (en) * 1984-06-11 1986-01-03 Bukamier Gary L Improvements in electrochemical sensors
US4908119A (en) * 1986-09-01 1990-03-13 Nippondenso Co., Ltd. Apparatus for determining oxygen concentration
US4783252A (en) * 1987-03-02 1988-11-08 Rosemount Inc. Lateral indicator sensor
US4891123A (en) * 1987-04-10 1990-01-02 Frantztech Ltd. Electrochemical analyzer for measuring the concentration of atoms or molecules in a fluid and method of making same
US5558756A (en) * 1994-11-15 1996-09-24 Cominco Ltd. Method for geo-electrochemical sampling
US5584978A (en) * 1994-11-15 1996-12-17 Cominco Ltd. Collection electrode (collectrode) for geo-electrochemical sampling
EP1098192A3 (de) * 1999-11-05 2004-01-14 M.K. Juchheim GmbH & Co. Indikatorelektrode mit einer sensitiven Oberfläche und Verwendung hierfür
US6398931B1 (en) * 2000-01-31 2002-06-04 Phoenix Electrode Company Combination ion-selective electrode with a replaceable sensing membrane
CN102265146A (zh) * 2008-12-22 2011-11-30 恩德莱斯和豪瑟尔测量及调节技术分析仪表两合公司 离子选择电极
CN102265146B (zh) * 2008-12-22 2014-06-25 恩德莱斯和豪瑟尔测量及调节技术分析仪表两合公司 离子选择电极

Also Published As

Publication number Publication date
GB1304498A (enrdf_load_stackoverflow) 1973-01-24
DE2059559C3 (de) 1975-10-30
DE2059559A1 (de) 1972-06-29
NL7115526A (enrdf_load_stackoverflow) 1972-06-06
DE2059559B2 (de) 1975-03-13

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