US3679945A - Electric quantity memory element - Google Patents

Electric quantity memory element Download PDF

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Publication number
US3679945A
US3679945A US72486A US3679945DA US3679945A US 3679945 A US3679945 A US 3679945A US 72486 A US72486 A US 72486A US 3679945D A US3679945D A US 3679945DA US 3679945 A US3679945 A US 3679945A
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Prior art keywords
electrode
memory element
metal
electrolyte
element according
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US72486A
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English (en)
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Satoshi Sekido
Tomohiko Arita
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Panasonic Holdings Corp
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Matsushita Electric Industrial Co Ltd
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    • G—PHYSICS
    • G11—INFORMATION STORAGE
    • G11C—STATIC STORES
    • G11C13/00—Digital stores characterised by the use of storage elements not covered by groups G11C11/00, G11C23/00, or G11C25/00
    • G11C13/0002—Digital stores characterised by the use of storage elements not covered by groups G11C11/00, G11C23/00, or G11C25/00 using resistive RAM [RRAM] elements
    • G11C13/0009—RRAM elements whose operation depends upon chemical change
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B82—NANOTECHNOLOGY
    • B82Y—SPECIFIC USES OR APPLICATIONS OF NANOSTRUCTURES; MEASUREMENT OR ANALYSIS OF NANOSTRUCTURES; MANUFACTURE OR TREATMENT OF NANOSTRUCTURES
    • B82Y10/00—Nanotechnology for information processing, storage or transmission, e.g. quantum computing or single electron logic
    • G—PHYSICS
    • G01—MEASURING; TESTING
    • G01R—MEASURING ELECTRIC VARIABLES; MEASURING MAGNETIC VARIABLES
    • G01R22/00—Arrangements for measuring time integral of electric power or current, e.g. electricity meters
    • G01R22/02—Arrangements for measuring time integral of electric power or current, e.g. electricity meters by electrolytic methods
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/42—Methods or arrangements for servicing or maintenance of secondary cells or secondary half-cells
    • H01M10/44—Methods for charging or discharging
    • H02J7/94—
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/10—Energy storage using batteries

Definitions

  • FIG. 1 A first figure.
  • FIG. 1 A first figure.
  • FIG. I7(b) TIME ELECTRIC QUANTITY MEMORY ELEMENT This invention relates to an electric quantity memory element comprising a first electrode made of a metal electrochemically dissolved or deposited in accordance with the Faradays laws, a second electrode made of a valve metal and an aqueous solution containing a water soluble salt the metal of the first electrode as an electrolyte.
  • the electric quantity memory element according to the present invention can be used to integrate and register the quantity of electric charge carried by a metal transferred from the first electrode to the second electrode by utilizing the current interruption phenomenon which takes place when the quantity of the metal of the first electrode, which has been deposited on the second electrode during the transfer of electric charges from the first electrode to the second electrode, is completely dissolved away by making a current to flow in the opposite direction. It is also used for the indication of a time interval, during which a constant current is made to flow, the alternating transfer of a constant quantity of an electric charge and the integration of the portion of a current above or below a predetermined value.
  • an apparatus comprising a first electrode of such a metal as silver electrochemically dissolved or deposited according to Faraday s laws, a second electrode of such an inactive metal as platinum and gold and an aqueous solution containing a water soluble salt of silver as an electrolyte or a solid electrolyte such as Agl, AgBr, Ag SI, Ag SBr, PbAg I KAg,l etc,
  • a first electrode of such a metal as silver electrochemically dissolved or deposited according to Faraday s laws
  • a second electrode of such an inactive metal as platinum and gold
  • an aqueous solution containing a water soluble salt of silver as an electrolyte or a solid electrolyte such as Agl, AgBr, Ag SI, Ag SBr, PbAg I KAg,l etc
  • the different kind of reaction as mentioned above means the electrolysis of water for electrolyte of an aqueous solution or the electrolysis of the solid electrolyte when it is used as the electrolyte.
  • reaction gases produced or other reaction products give rise to various problems.
  • the increase of a cell voltage should be held below 1.2 volts in the case of a liquid electrolyte and below 0.8 volt in the case of a solid electrolyte. Because of this limitation on the cell voltage, a large change of the cell voltage can not be expected when the deposited metal has been completely re-dissolved.
  • An object of the present invention is to provide a repeatedly usable memory element for storing a quantity of electricity, in which a valve metal such as tungsten and tantalum is used as the material of the second electrode to be plated with the metal electrochemically dissolved and deposited, and which can provide a large voltage change or effect a remarkable current interruption operation at the time of the complete dissolution of the deposited metal from the second electrode so as to be suitable for use as a means to produce an electric signal in response to the change of an electrical quantity.
  • a valve metal such as tungsten and tantalum
  • FIG. I shows the cell voltage (solid curve) and the cell current (dashed curve) versus the ratio of the electricity for the dissolution to that for the deposition of copper or gold, Graph (:1) being obtained by using molybdenum of titanium for the second electrode and Graph (b) being obtained by using tan talum for the second electrode;
  • FIG. 2 shows the ratio of the electricity for the dissolution to that for the deposition of the metal of the first electrode versus the number of cycles of the alternating transfer of the metal of the first electrode with the parameters of various materials sealing the second electrode;
  • FIG. 3 shows the limit of concentration of Cu or Ag ions (solid curve) and the lower limit of the electrolyte temperature (dashed curve) versus the hydrogen ion concentration of the electrolyte;
  • FIG. 4 shows the relation between the lower limit of the electrolyte temperature and the concentration of potassium sodium tartrate in the electrolyte
  • FIG. 5 shows the relation between the lower limit of the electrolyte temperature and the concentration of phosphoric acid in the electrolyte
  • FIG. 6 shows the relation between the lower limit of the electrolyte temperature and the concentration of methanol in the electrolyte
  • FIGS. 7 and 8 are schematic longitudinal sectional views showing the construction of preferred embodiments of the electrical quantity memory element according to the present invention.
  • FIG. 9 shows the performance of the electrical quantity memory element of FIG. 7
  • FIG. I0 is a block diagram showing a meter using the electrical quantity memory element according to the present invention.
  • FIGS. 11 and 12 are circuit diagrams showing other meters using the electrical quantity memory element according to the present invention.
  • FIG. 13 is a circuit diagram showing a battery charger using the electrical quantity memory element according to the invention.
  • FIGS. 14, I5 and I6 are schematic longitudinal sectional views showing other embodiments of the electrical quantity memory element according to the present invention.
  • FIG. 17a shows a circuit diagram employing the electrical quantity memory element according to the present invention for integrating electric signals above a threshold value
  • FIG. 17b shows a circuit diagram employing the electrical quantity memory element according to the present invention for integrating electric signals below a threshold value.
  • valve metals as tungsten, tantalum, titanium, niobium, molybdenum and aluminum is lower than (i.e., electronegative to) the dissolution or deposition potential of such metals as copper, silver and lead. Therefore, if these valve metals are used for the aforementioned second electrode, copper, etc., will be deposited on an oxide film formed on the second electrode. Therefore, it often occurs that copper or the like metal is deposited in a poor state.
  • valve metals As molybdenum, titanium, tungsten or tantalum for platinum or gold and such a metal as copper or lead for silver.
  • FIG. 1 shows typical examples of the manner of the change of a cell voltage and a cell current. With molybdenum and titanium, the deposition characteristics is superior, but the current remaining after the cell voltage has risen is relatively high as shown in graph (a) in FIG. 1.
  • valve metal electrode in the form of a wire 0.8 mm in diameter which was sealed with glass to leave its end portion of a length of 4 mm immersed in an aqueous solution containing 0.2 g/l of borax, was subjected to anodic oxidationv by using a platinum plate as the opposite electrode with a source voltage of 50 volts for 30 minutes, and then it was interposed between two plates of copper or silver for the electro-deposition of copper or silver.
  • an electrolyte having a composition of 350 g/l Cu( BF,,) 50 g/l HBF,, 5 g/l potassium sodium tartrate (Rochelle salt), 1 g/l p-phenol sulfonic acid and 50 g/l methanol was used.
  • an electrolyte having a composition of 90 g/l Ag;,(PO,) and 900 g/l H PO was used.
  • tungsten is most recommendable as it is of an excellent deposition nature and provides comparatively a low remaining current.
  • FIG. 2 shows the ratio between the dissolved and deposited quantities of copper or silver when the tungsten electrode is sealed in hard glass (a), ceramics (b) and polyvinyl chloride (c) versus the number of cycles of deposition and re-dissolution. As is seen, the reproducibility is most excellent when the electrode is sealed with hard glass.
  • the plots in this Figure are obtained with the same experimental conditions as for FIG. 1.
  • the coefficient of thermal expansion of hard glass is preferably close to that of tungsten, namely, about 38 X
  • the hard glass is preferably composed of 65 to 75 percent by weight of SiO 5 to 12 percent by weight of B 0 1 to 5 percent by weight of M 0 less than 0.5 percent by weight of Fe O 5 to 8 percent by weight of CaO, 0.5 to 2 percent by weight of MgO, less than 5 percent by weight of ZnO, 6 to 14 percent by weight of Na O and I to 6 percent by weight of K 0.
  • the usable temperature range of the electrolyte may be increased owing to the decrease of the freezing point and increase of the boiling point.
  • the current interruption characteristic is degradated with an increase of the concentration of Cu or Ag ions beyond a certain limit, although the reason why this occurs is not clear.
  • the limit is about mol/l in the case of Cu ions and about 60 mol/l in the case of Ag ions with the pH value of 2 of the electrolyte, with which it is thought that no insoluble oxide film is formed on the valve metal electrode.
  • the limit varies with the pH value of the electrolyte as shown in FIG.
  • FIG. 4 shows the effect of potassium sodium tartrate when the dissolved metal is copper.
  • FIG. 5 shows the effect of phosphoric acid when the dissolved metal is silver. These plots were obtained with the current density for the tungsten set to I00 mA/cm When the dissolved metal is copper, the lowering of the lower limit of the electrolyte temperature is not pronounced by the addition of potassium sodium tartrate.
  • FIG. 6 shows the effect of methanol when the dissolved metal is copper. The most effective content of added methanol is about 50 g/l.
  • the electrolyte contains 330 to 380 g/l of Cu(BF 20 to g/l of HBF,, 2 to 10 g/l of potassium sodium tartrate Rochelle salt) and 40 to 60 g/l of methanol when the dissolved metal is copper, while it contains 80 to g/l of Ag PO and 700 to 900 g/l of H PO when the dissolved metal is silver.
  • the current density should be lower than 200 mA/cm in the case of depositing copper and lower than mA/cm in the case of depositing silver on the tungsten electrode with an electrolyte of the above compositions. Otherwise, needle-like crystals become pronounced, resulting in reduced service life.
  • the electrolytic cell according to the present invention may have different numbers of electrodes for various uses.
  • FIG. 7 shows a preferred embodiment of the cell according to the present invention. It is of the two-electrode construction having a tungsten electrode I and a copper electrode 2.
  • the tungsten electrode is in the form of a wire of a diameter of 0.8 mm and is sealed with a glass mount 3 to leave its end portion of a length of 4 mm immersed in the electrolyte.
  • the coefficient of thermal expansion of the glass of the glass mount 3 is close to that of tungsten 38 X 10").
  • the copper electrode 2 is cylindrical. Its inner diameter is l 1 mm, its thickness 1 mm, and its height 12 mm.
  • Numeral 4 designates a lid of an electrolyte-resistant resin such as polyvinyl chloride, polystyrene, etc. It is screwed in or bonded to a cell 5 of the same material.
  • Numeral 6 designates a lead.
  • the copper electrode 2 may also serve as a cell as shown in FIG. 8. The relation between the quantity of electricity transferred and the distance between the electrodes (the inner diameter of the copper electrode) is most important in the cell construction.
  • FIG. 9 shows the relation between the quantity of electricity and the number of cycles which has been obtained with the construction shown in FIG. 7.
  • the element of the two-electrode construction described above is suitable for the storage and reading-out of a given quantity of electricity.
  • a given quantity of electricity has been stored into this cell by maintaining the tungsten electrode 1 negative, the cell voltage will be suddenly increased to interrupt the cell current if the same quantity of electricity is transferred in the opposite direction.
  • the storage of a given quantity of electricity is effected even if the cell current is not constant during the storing process, because the cell current is integrated through the storing process.
  • this element is suitable for use in a meter for commercial power supply, gas and water supplies, the battery charger controls, and various timers.
  • FIG. 10 shows a power supply meter using this element.
  • numeral 11 designates a sensor to convert the electric power or flow rate into the corresponding electric current.
  • the sensor 11 may be a Hall element for generating a voltage proportional to power or an electrochemical multiplier (solion multiplier) for generating a current proportional to power.
  • the pressure difference across a Venturi orifice or a Pitot tube is converted into the corresponding electric current by utilizing a piezoelectric effect, by means of an electrochemical transducer (solion" transducer) or by utilizing electroosmosis effect.
  • a current proportional to the supply current may be caused to pass through the electric quantity memory element 12 with the provision of a shunt resistor 14. This is possible because of a substantially constant supply voltage.
  • a predetermined quantity of the electrodeposition of a metal is prepared beforehand on one of the two elements connected in parallel with and in opposite polarities to each other and then the current is reversed to re-dissolve the deposited metal.
  • the cell voltage suddenly rises, whereupon one count of the counting is made, and at the same time the current is reversed again.
  • the two elements are connected in opposite polarities to each other, the same quantity of the deposited metal as beforehand deposited on one element is deposited on the other element when the previously deposited metal is completely re-dissolved.
  • the metering during that period may be effected.
  • meral I3 designates an amplifier, numeral 15 a resistor, numeral 16 a diode and numeral 17 a resistor of a high resistance.
  • the charging current can be controlled with the electric quantity control element according to the present invention. Since, if the quantity of electricity discharged in the element is stored, the voltage of the element suddenly rises when the charged quantity becomes equal to the dischargedquantity.
  • FIG. 13 An example of the circuit arrangement to this end is shown in FIG. 13.
  • numeral 21 designates the electric quantity memory element according to the present invention. During the discharging process of the battery 22 a current proportional to the load current passes through the element 21 to deposite copper or silver on the tungsten electrode.
  • the electric quantity memory element is applied to a timer, the setting of time ranging from one minute up to one year is possible by appropriately selecting the quantity of metal to be deposited and the value of the constant current.
  • FIG. 14 shows an example of three-electrode cell according to the present invention.
  • the three-electrode cell may have either a combination of two tungsten electrodes and one copper electrode or a combination of one tungsten electrode and two copper electrodes.
  • the cell having two tungsten electrodes as shown in FIG. 14 is suitable for use in the alternation of a constant quantity of electricity.
  • the illustrated embodiment comprises two tungsten electrodes 1 and l of the same size and shape and a copper electrode 2.
  • the tungsten electrodes 1 and l are sealed in the same manner as in the embodiment of FIG. 7.
  • the copper electrode 2 is cylindrical with an inner diameter of l 1 mm, a wall thickness of 1 mm and a height of [2 mm.
  • Lids 4 and 4 carrying the respective tungsten electrodes 1 and l are screwed into or bonded to the copper electrode 2 on opposite ends thereof. If the quantity of electricity involved is small, the copper electrode 2 may also serve as the cell shown in FIG. 15.
  • the cell having one tungsten electrode and two copper electrodes is suitable for use, for instance, in the integration of electric signals above or below a threshold value. It can also be used for the addition and subtraction of two signals.
  • FIG. I6 shows the construction of this cell. It comprises a tungsten electrode 1 and two copper electrodes 2 and 2'. The tungsten electrode 1 is sealed in the same manner as in the embodiment of FIGS. 7 and 14. It is substantially concentric with the copper electrodes 2 and 2'.
  • the copper electrodes 2 and 2' are cylindrical with an inner diameter of l 1 mm, a wall thickness of I mm and a height of 5 mm. They are spaced by a distance of at least 6 mm from each other.
  • the two copper electrodes 2 may be the anodes.
  • the copper electrode for a larger signal may be the anode and the copper electrode for a smaller signal may be the cathode.
  • the element is connected as shown in FIG. 170, while in the case of integrating signals below a threshold value it is connected as shown in FIG. 17b. A constant current equal to the threshold value is caused to flow through one of the copper electrodes.
  • the composition of the electrolyte should be suitably modified and the size of the tungsten electrode should be slightly increased.
  • a repeatedly usable memory element for storing a quantity of electricity comprising:
  • a first electrode made of a metal electrochemically dissolvable and depositable in accordance with Faradays law
  • a second electrode made of a metal selected from the group consisting of tungsten, molybdenum and titanium and having a quantity of the metal constituting said first electrode deposited thereon;
  • a repeatedly usable memory element according to claim I wherein said second electrode is sealed with hard glass having a coefficient of thermal expansion substantially equal to that of said metal constituting said second electrode leaving a portion of said second electrode naked, said portion of said second electrode being immersed in said liquid electrolyte.
  • a repeatedly usable memory element wherein said first electrode is made of copper and said electrolyte consists of an aqueous solution containing 330 to 380 g/l of Cu( 8H),, 20 to 60 g/l of HBF, and 2 to 10 g/l of potassium sodium tartrate.

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  • Crystallography & Structural Chemistry (AREA)
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US72486A 1969-09-20 1970-09-15 Electric quantity memory element Expired - Lifetime US3679945A (en)

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Cited By (10)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3768015A (en) * 1971-11-15 1973-10-23 Catalyst Research Corp Electrolytic timing cell
USRE28941E (en) * 1971-01-14 1976-08-24 Air Products And Chemicals, Inc. Electrolytic timer delay capsule
US4038586A (en) * 1972-09-20 1977-07-26 Matsushita Electric Industrial Co., Ltd. Coulomb memory element
US4332003A (en) * 1980-01-31 1982-05-25 Ford Motor Company Electrochemical analog transistor structure with two spaced solid electrochemical cells
US4435742A (en) 1980-01-31 1984-03-06 Ford Motor Company Electrochemical transistor structure with two spaced electrochemical cells
US20100092656A1 (en) * 2008-10-10 2010-04-15 Axon Technologies Corporation Printable ionic structure and method of formation
US20110062408A1 (en) * 2000-02-11 2011-03-17 Kozicki Michael N Programmable metallization cell structure including an integrated diode, device including the structure, and method of forming same
US20110194339A1 (en) * 2000-07-27 2011-08-11 Axon Technologies Corporation Microelectronic programmable device and methods of forming and programming the same
US8213218B2 (en) 2000-02-11 2012-07-03 Axon Technologies Corporation Optimized solid electrolyte for programmable metallization cell devices and structures
US8218350B2 (en) 2000-02-11 2012-07-10 Axon Technologies Corporation Programmable metallization cell structure including an integrated diode, device including the structure, and method of forming same

Citations (8)

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US2710369A (en) * 1952-09-29 1955-06-07 Mallory & Co Inc P R Electrolytic condenser
US3052830A (en) * 1959-02-16 1962-09-04 Ovitron Corp Electrical control device and process
US3158798A (en) * 1959-11-17 1964-11-24 William C Sauder Chemical memory cell
US3275901A (en) * 1963-03-14 1966-09-27 Gen Electric Sealed electrical assembly
US3423642A (en) * 1966-10-18 1969-01-21 Bissett Berman Corp Electrolytic cells with at least three electrodes
US3423648A (en) * 1966-01-10 1969-01-21 Bissett Berman Corp Electrolytic cell with electrically conductive masking surface
US3423643A (en) * 1966-05-31 1969-01-21 Bissett Berman Corp Electrolytic cell with electrolyte containing silver salt
US3512049A (en) * 1968-02-28 1970-05-12 Bergen Lab Inc Electrolytic timer

Patent Citations (8)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US2710369A (en) * 1952-09-29 1955-06-07 Mallory & Co Inc P R Electrolytic condenser
US3052830A (en) * 1959-02-16 1962-09-04 Ovitron Corp Electrical control device and process
US3158798A (en) * 1959-11-17 1964-11-24 William C Sauder Chemical memory cell
US3275901A (en) * 1963-03-14 1966-09-27 Gen Electric Sealed electrical assembly
US3423648A (en) * 1966-01-10 1969-01-21 Bissett Berman Corp Electrolytic cell with electrically conductive masking surface
US3423643A (en) * 1966-05-31 1969-01-21 Bissett Berman Corp Electrolytic cell with electrolyte containing silver salt
US3423642A (en) * 1966-10-18 1969-01-21 Bissett Berman Corp Electrolytic cells with at least three electrodes
US3512049A (en) * 1968-02-28 1970-05-12 Bergen Lab Inc Electrolytic timer

Cited By (11)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
USRE28941E (en) * 1971-01-14 1976-08-24 Air Products And Chemicals, Inc. Electrolytic timer delay capsule
US3768015A (en) * 1971-11-15 1973-10-23 Catalyst Research Corp Electrolytic timing cell
US4038586A (en) * 1972-09-20 1977-07-26 Matsushita Electric Industrial Co., Ltd. Coulomb memory element
US4332003A (en) * 1980-01-31 1982-05-25 Ford Motor Company Electrochemical analog transistor structure with two spaced solid electrochemical cells
US4435742A (en) 1980-01-31 1984-03-06 Ford Motor Company Electrochemical transistor structure with two spaced electrochemical cells
US20110062408A1 (en) * 2000-02-11 2011-03-17 Kozicki Michael N Programmable metallization cell structure including an integrated diode, device including the structure, and method of forming same
US8213218B2 (en) 2000-02-11 2012-07-03 Axon Technologies Corporation Optimized solid electrolyte for programmable metallization cell devices and structures
US8218350B2 (en) 2000-02-11 2012-07-10 Axon Technologies Corporation Programmable metallization cell structure including an integrated diode, device including the structure, and method of forming same
US20110194339A1 (en) * 2000-07-27 2011-08-11 Axon Technologies Corporation Microelectronic programmable device and methods of forming and programming the same
US8213217B2 (en) 2000-07-27 2012-07-03 Axon Technologies Corporation Microelectronic programmable device and methods of forming and programming the same
US20100092656A1 (en) * 2008-10-10 2010-04-15 Axon Technologies Corporation Printable ionic structure and method of formation

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