GB2569637A - Electronic device - Google Patents

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Publication number
GB2569637A
GB2569637A GB1721676.3A GB201721676A GB2569637A GB 2569637 A GB2569637 A GB 2569637A GB 201721676 A GB201721676 A GB 201721676A GB 2569637 A GB2569637 A GB 2569637A
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GB
United Kingdom
Prior art keywords
electronic device
layer
thermoelectric
metal foil
electrically insulating
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.)
Withdrawn
Application number
GB1721676.3A
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GB201721676D0 (en
Inventor
Fletcher Thomas
O'Regan Bryan
King Simon
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.)
Sumitomo Chemical Co Ltd
Original Assignee
Sumitomo Chemical Co Ltd
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.)
Filing date
Publication date
Application filed by Sumitomo Chemical Co Ltd filed Critical Sumitomo Chemical Co Ltd
Priority to GB1721676.3A priority Critical patent/GB2569637A/en
Publication of GB201721676D0 publication Critical patent/GB201721676D0/en
Publication of GB2569637A publication Critical patent/GB2569637A/en
Withdrawn legal-status Critical Current

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Classifications

    • H—ELECTRICITY
    • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10N—ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10N10/00—Thermoelectric devices comprising a junction of dissimilar materials, i.e. devices exhibiting Seebeck or Peltier effects
    • H10N10/10—Thermoelectric devices comprising a junction of dissimilar materials, i.e. devices exhibiting Seebeck or Peltier effects operating with only the Peltier or Seebeck effects
    • H10N10/17—Thermoelectric devices comprising a junction of dissimilar materials, i.e. devices exhibiting Seebeck or Peltier effects operating with only the Peltier or Seebeck effects characterised by the structure or configuration of the cell or thermocouple forming the device
    • H—ELECTRICITY
    • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
    • H10K77/00—Constructional details of devices covered by this subclass and not covered by groups H10K10/80, H10K30/80, H10K50/80 or H10K59/80
    • H10K77/10—Substrates, e.g. flexible substrates
    • H10K77/111—Flexible substrates
    • 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
    • Y02E10/00—Energy generation through renewable energy sources
    • Y02E10/50—Photovoltaic [PV] energy
    • Y02E10/549—Organic PV cells

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  • Insulated Metal Substrates For Printed Circuits (AREA)

Abstract

A bilayer substrate 101 of a flexible electronic device has an electrically insulating polymer layer 101B (may be a thermosetting polymer, photoresist or epoxy) in contact with a thicker un-patterned metal foil layer 101A (may be aluminium or steel). The polymer layer 101B is between the metal foil layer 101A and a first electrode 103. The electronic device may be a thermoelectric device having n-type 105n and p–type 105p thermoelectric legs as thermoelectric couples between the first electrode 103 and a second electrode 107, which may be patterned. The polymer layer 101B may be deposited on the metal foil layer 101A as a solution and cured. The thermoelectric legs may be printed into wells defined by a patterned insulating layer 109 formed over the first electrode 103. The bilayer substrate may be used with a heat sink in other heat generating devices, such as organic LEDs, TFTs or batteries.

Description

Electronic Device
Field of the Invention
The invention relates to electronic devices, particularly thermoelectric devices.
Background
Thermoelectric devices, operating by the Peltier Effect, are known.
WO 03/007391 discloses a flexible thermoelectric module having a pair of flexible substrates.
WO 2012/140652 discloses a thermoelectric module having an anodised aluminium substrate.
WO 2015/071635 discloses a flexible electronic substrate of a metal layer having a ceramic layer of an oxide of the metal.
It is an object of the invention to provide a substrate suitable for use with flexible electronic devices.
It is a further object of the invention to provide a substrate for high efficiency thermoelectric devices.
Summary of the Invention
The present inventors have found that a bilayer of a metal foil layer and a thin dielectric layer can be used as a high thermal conductivity substrate for electronic devices.
Accordingly, in a first aspect the invention provides a flexible electronic device comprising a first electrode on a first substrate wherein the first substrate comprises an unpatterned metal foil layer and an insulating layer comprising a polymer in contact with the metal foil layer and between the metal foil layer and the first electrode, wherein the insulating layer is thinner than the metal foil layer.
In a second aspect the invention provides a method of forming an electronic device according to the first aspect, the method comprising: formation of the insulating layer comprising the step of depositing a polymer on the metal foil from a solution; and forming the first electrode on the insulating layer
In a third aspect the invention provides use of a bilayer comprising an unpatterned metal foil layer and an insulating layer comprising an insulating polymer in contact with the metal foil layer as a substrate for an electronic device, wherein the electronic device is provided on the insulating layer.
Description of the Drawings
The invention will now be described in more detail with reference to the Figures, in which:
Figure 1 is a schematic illustration of a thermoelectric device according to an embodiment;
Figure 2 schematically illustrates part of a thermoelectric array of a thermoelectric device according to an embodiment; and
Figure 3 is a graph of voltage vs applied temperature gradient for a thermoelectric generator according to an embodiment.
Detailed Description of the Invention
Figure 1, which is not drawn to any scale, schematically illustrates a thermoelectric device according to an embodiment.
A thermoelectric couple is provided between a first flexible substrate 101 and a second flexible substrate 111.
The thermoelectric couple comprises a first electrode 103, a second electrode 107, and a p-type thermoelectric leg 105p and an n-type thermoelectric leg 105n between the first and second electrodes. Each of the first and second electrodes may consist of a single conductive layer or may comprise two or more layers.
First substrate 101 has a metal foil layer 101A and electrically insulating polymer layer 10IB in contact with the metal foil layer. The metal foil layer is unpatterned, i.e. it is a continuous layer extending across the surface area of the electrically insulating polymer layer. Suitably, the electrically insulating layer is unpatterned. Flexible substrate 101 carries first electrode 103. Electrically insulating polymer layer 101B is between metal foil layer 101A and first electrode 103. Preferably, electrically insulating polymer layer 101B is the only layer between the metal foil layer 101A and the first electrode 103.
The electrically insulating polymer layer 10IB has a thickness sufficient to electrically insulate metal foil layer 101A from the first electrode 103, preferably a thickness of at least 1 micron.
The electrically insulating polymer layer has lower thermal conductivity than metal foil layer 101A and is therefore preferably thinner than the metal foil layer. Optionally, the electrically insulating polymer layer 101B has a thickness of less than about 20 microns. Optionally, metal foil layer 101A has a thickness in the range of about 20-100 microns.
Metal foil layer may 101A be a layer of any metal or metal alloy capable of forming a flexible layer, such as a layer of aluminium or steel, preferably a layer of aluminium.
Electrically insulating polymer layer 101B preferably has a thermal conductivity in the range of 0.1-10 W/m.K, optionally 0.1-5 W/m.K.
The thickness of the thermocouple(s) of the thermoelectric device is preferably in the range of about 50-500 microns, optionally 50-200 microns.
The p-type and n-type thermoelectric leg each have a thermal conductivity lower than that of the metal foil and preferably lower than that of the insulating polymer layer.
The active materials of the thermoelectric legs may be inorganic, organic or a combination thereof. Exemplary active materials of thermoelectric legs are described in
J. Mater. Chem. C, 2015, 3, 10362 and Chem. Soc. Rev., 2016, 45, 6147-6164, the contents of which are incorporated herein by reference.
The thermoelectric device preferably has a bend radius of 30 mm or less, optionally 20 mm or less. The bend radius may be at least 5 mm or at least 10 mm.
The electrically insulating polymer layer may consist of an electrically insulating polymer or may comprise one or more further materials.
The polymer of the electrically insulating polymer layer is preferably a thermosetting polymer, optionally a photoresist. The polymer may be an epoxy polymer. Preferably, the electrically insulating layer is formed by depositing the polymer dissolved in one or more solvents, along with any other components of the layer dissolved or dispersed in the solvent or solvents, onto the metal foil layer followed by evaporation of the solvent or solvents and curing of the polymer. Curing may be by heat and / or UV treatment. The concentration of the polymer in a solution or dispersion containing the polymer may be selected according to the required thickness of the electrically insulating polymer layer.
In embodiments, second substrate 111 may comprise a metal foil layer and an electrically insulating polymer layer as described with reference to the first substrate 101 wherein second electrode 107 is separated from the metal foil layer of the second substrate by the electrically insulating polymer layer of the second substrate.
In embodiments, second substrate 111 is different from first substrate 101. Optionally in these embodiments, second substrate 111 consists of a single electrically insulating polymer layer.
Preferably, the thermoelectric device comprises an array of electrically connected thermoelectric couples as illustrated in Figure 2. For simplicity, only two thermoelectric couples are illustrated in Figure 2 however it will be appreciated that a larger number may be connected in an array. The thermoelectric couples may be connected to one another in series, parallel or a combination thereof. The first and second electrodes may each form a pattern of a plurality of conducting pads connecting the thermoelectric couples. The first and second electrodes are each preferably in the form of a patterned layer defining a plurality of conductive pads. The first and second electrodes may each independently consist of a single conductive layer or two or more conductive layers. The or each conductive layer may consist of a single conductive material or may comprise two or more materials. Conductive materials for forming the conductive layers are preferably selected from metals and conductive metal compounds, for example conductive metal oxides. Exemplary metals are copper, aluminium and gold. The first and second electrodes optionally each independently have a thickness in the range of about 1-10 microns.
The thermoelectric device may comprise a patterned insulating structure 109 between the thermoelectric legs. The patterned insulating structure may comprise one or more layers. Preferably, the patterned insulating structure is a single patterned insulating polymer layer. The patterned insulating polymer layer may be a patterned layer of positive or negative photoresist.
The thermoelectric device may be formed by forming a patterned first electrode 103 on layer 101A of the first substrate; forming a patterned insulating structure defining wells over the patterned first electrode; depositing material for forming the n-type and p-type thermoelectric legs into the wells; and providing a patterned second electrode and second substrate over the thermoelectric legs.
In embodiments, the patterned second electrode may be deposited onto the thermoelectric legs by any suitable technique such as sputtering or evaporation, followed by application of a second substrate over the second electrode.
In embodiments, a second substrate carrying a patterned second electrode formed thereon may be applied over the thermoelectric legs to complete the device.
In other embodiments, the patterned first electrode may be supported on a substrate which is not a substrate comprising layers 101A and 10IB as described herein, for example a substrate consisting of a single insulating polymer layer, and wherein the substrate comprising layers 101A and 101B is formed over the second electrodes.
The materials for forming the n-type and p-type thermoelectric legs may be deposited into the wells by any suitable technique including thermal evaporation, sputtering and deposition of an ink comprising the material or materials for forming the thermoelectric legs dissolved or dispersed in one or more solvents. Ink deposition is preferred.
Suitable techniques for depositing an ink are coating or printing methods including, without limitation,, roll-coating, spray coating, doctor blade coating, slit coating, inkjet printing, screen printing, dispense printing, gravure printing and flexographic printing. Dispense printing is particularly preferred. In dispense printing, each thermoelectric leg is formed by depositing a continuous flow of ink from a nozzle positioned above the first electrode.
A semiconductor material may be deposited in n-doped or p-doped form or may be deposited with an n-dopant or p-dopant followed by ίη-situ doping of the semiconductor.
Ink formulations may consist of an n-doped or p-doped semiconductor, or precursors thereof, dissolved or dispersed in one or more solvents or may comprise one or more further materials. Preferably, ink formulations as described herein further comprise a polymeric binder. The binder may make layers formed from the formulation more resilient and less likely to crack than films in which no binder is present.
The substrate may be heated during deposition of the ink. The temperature of the substrate may be selected so as to control rate of evaporation of the solvents from the ink, for example to avoid non-uniform evaporation.
In operation as a thermoelectric generator, the first or second substrate is brought into contact with a surface having a temperature higher than the environmental temperature. Pads of the first or second electrode are electrically connected to a load.
In operation as a thermoelectric cooler, the first or second substrate is brought into contact with a surface to be cooled and a voltage is applied to the device.
The polymeric binder may be a conjugated or non-conjugated polymer. The polymeric binder may be a crosslinked polymer, for example a crosslinked epoxy. The polymeric binder may be a thermoplastic or thermosetting polymer. The polymeric binder may be deposited in polymeric form followed by crosslinking. A monomer may be deposited followed by polymerisation to form the polymer binder, optionally a crosslinked polymeric binder.
The substrate of a metal foil layer and an insulating polymer layer has been described herein with reference to thermoelectric devices however it will be appreciated that this substrate may be used as the substrate for other electronic devices, particularly devices which generate heat including, without limitation, flexible organic devices such as organic light-emitting devices, organic thin film transistors and organic batteries. When used to remove heat from a heat-generating device supported on the insulating polymer layer of the substrate, a heat sink may be applied to the opposing metal foil surface of the substrate.
Examples
Insulating layer
Properties of selected materials are set out in Table 1 in which X is a ratio of the temperature difference across the thermoelectric material of a thermoelectric device to the temperature difference applied to the device assuming the thermoelectric material is 50 micron thick and has thermal conductivity 0.45 W/m.K:
v_^7*>nQfBn-Q| Lti applied
As set out in Table 1, a combination of a thin insulating polymer and an aluminium foil gives both flexibility and a high X ratio.
Table 1
Substrate Thermal Conductivity (W/m.K) Thickness (micron) X Notes
PEN1 0.45 125 0.167 Poor thermal performance
Thermosilicone on polyimide2 1.05 150 0.259 Poor thermal performance
Flexible Ceramic3 2.7 40 0.789 Hard and brittle, requires specialised handling
Spin on glass (1) on aluminium foil (2) 1) i+ 2) 237* 1)6 2)40 0.900 Requires high temperature processing
SU8 (1) on aluminium foil (2) 1) 0.45 2) 237* 1)6 2) 40 0.804 Low temperature processing, solvent resistant
+ Estimated thermal conductivity based on thermal conductivity of glass *CRC Handbook of Physics and Chemistry, 67th Edition, D-185 'Teijin Dupont Teonex Q65HA 2Aavid Kunze KU-KC15 3Enrg-Inc E-Strate, https://www.enrg-inc.com/
Creative Materials 122-07(SP)
Device Example 1
A first substrate of aluminium foil and thermosetting polymer was formed using a carrier substrate to aid fabrication. The carrier substrate consisted of a 1.1mm square glass plate (355x355mm) laminated with a double-sided adhesive gel film (Gel-Pak, DGL Film x4).
Aluminium foil was cut from a roll to the carrier substrate size and laminated to the gel film. A 6 micron layer of the negative photoresist SU-8 3025 (available from MicroChem) was spin coated onto the Al foil to form the insulating polymer layer. To achieve the 6 micron layer thickness the SU-8 3025 was diluted with cyclopentanone to a ratio of 3:1 (SU-8 3025 : Cyclopentanone). Before spin coating, the surface of the Al foil was wetted with propylene glycol methyl ether acetate (PGMEA) for uniform coating.
A volume of ~40ml of the diluted SU-8 solution was dispensed at lOOOrpm for 30s with an initial ramp acceleration of 400 rpm/s followed with a bake at 95°C for 20 minutes. The SU-8 layer was crosslinked by exposing it to UV light from a super-high-pressure mercury lamp (total energy of 210 mJ) followed by baking at 130°C for 5 minutes and at 150°C for 1 hour.
Metal electrodes were deposited by evaporation, sputtering or lamination of a metal foil onto the polymer layer and patterned via photolithography. A 60 micron thick photoresist bank layer was then applied to form open wells via photolithography above the patterned electrode.
Thermoelectric legs were deposited into the wells by dispense printing Heraeus Clevios ™ PH 1000 for the p-type legs and an ink containing PCBM fullerene and N-DMBI (disclosed \r\Adv. Mater. 2014, 26, 4268 -4272, the contents of which are incorporated herein by reference) for the p-type legs and a top metal electrode was evaporated through a shadow mask, and are then encapsulated with a second substrate of the same type as the first substrate. The device was heated to activate N-DMBI for n-doping of PCBM.
The assembled device was tested by clamping it between temperature controlled aluminium blocks. The temperature of each side of the assembly was adjusted to generate several temperature gradients, and the thermovoltage produced by the Seebeck Effect of the thermoelectric material was measured.
Comparative Device 1
For the purpose of comparison, devices were prepared according to the Device Example except that the substrate was polyethylene naphthalate (PEN).
With reference to Figure 3, the generated thermovoltage is much higher for Device Example 1 than for Comparative Device 1, which is attributed to a higher temperature gradient across the thermoelectric legs of Device Example 1 as compared to Comparative Device 1.
Although the present invention has been described in terms of specific exemplary embodiments, it will be appreciated that various modifications, alterations and/or combinations of features disclosed herein will be apparent to those skilled in the art without departing from the scope of the invention as set forth in the following claims.

Claims (19)

1. A flexible electronic device comprising a first electrode on a first substrate wherein the first substrate comprises an unpatterned metal foil layer and an electrically insulating layer comprising an electrically insulating polymer in contact with the metal foil layer and between the metal foil layer and the first electrode, wherein the electrically insulating layer is thinner than the metal foil layer.
2. A flexible electronic device according to claim 1 wherein the electrically insulating layer consists of the electrically insulating polymer.
3. A flexible electronic device according to claim 1 or 2 wherein the electrically insulating polymer is a cured thermosetting polymer.
4. A flexible electronic device according to any one of the preceding claims wherein the electrically insulating polymer is an epoxy.
5. A flexible electronic device according to any one of the preceding claims wherein the electrically insulating layer has a thickness of less than 20 microns.
6. A flexible electronic device according to any one of the preceding claims wherein the metal foil layer has a thickness of at least 20 microns.
7. A flexible electronic device according to any one of the preceding claims wherein the metal foil is aluminium foil.
8. A flexible electronic device according to any one of the preceding claims wherein the electronic device is a thermoelectric device.
9. A flexible electronic device according to claim 8 wherein the thermoelectric device comprises a plurality of thermoelectric couples comprising n-type and p-type thermoelectric legs between the first electrode and a second electrode wherein the first electrode and second electrode are patterned electrodes.
10. A flexible electronic device according to claim 9 wherein the thermoelectric legs are separated from one another by a patterned electrically insulating layer defining wells containing the thermoelectric legs.
11. A flexible electronic device according to any of claims 8-10 wherein the plurality of thermoelectric couples are provided between the first substrate and a second substrate.
12. A flexible electronic device according to any one of claims 8-11 wherein the n-type and p-type thermoelectric legs comprise an n-doped and a p-doped organic semiconductor respectively.
13. A flexible electronic device according to claim 12 wherein the second substrate comprises a second metal foil layer and a second electrically insulating layer between the second electrodes and the second metal foil layer.
14. A flexible electronic device according to any one of claims 8-13 wherein the thermoelectric device has a thickness of no more than 1 mm.
15. A method of forming an electronic device according to any one of the preceding claims, the method comprising: formation of the electrically insulating layer comprising the step of depositing an electrically insulating polymer on the metal foil from a solution; and forming the first electrode on the electrically insulating layer
16. A method according to claim 15 wherein formation of the insulating layer further comprises curing of the deposited electrically insulating polymer.
17. A method according to claim 15 or 16 further comprising the step of patterning the first electrode.
18. A method according to any one of claims 15-17 wherein the electronic device is a thermoelectric device and wherein thermoelectric legs of the thermoelectric device are printed into wells defined by a patterned insulating layer formed over the first electrodes.
19. Use of a bilayer comprising an unpatterned metal foil layer and an insulating layer comprising an insulating polymer in contact with the metal foil layer as a substrate for an electronic device, wherein the electronic device is provided on the insulating layer.
GB1721676.3A 2017-12-21 2017-12-21 Electronic device Withdrawn GB2569637A (en)

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Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2023283188A1 (en) * 2021-07-05 2023-01-12 Soft-Tex International, Inc. Bedding systems based on localized climate control, and related methods

Citations (7)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US6274803B1 (en) * 1999-08-10 2001-08-14 Matsushita Electric Works, Ltd. Thermoelectric module with improved heat-transfer efficiency and method of manufacturing the same
EP2109161A1 (en) * 2008-04-11 2009-10-14 Xerox Corporation Thin-film transistors
KR20100096345A (en) * 2009-02-24 2010-09-02 연세대학교 산학협력단 A thermoelectric device for a tactile sensor and an electrical power generator, and methods of its fabrication
WO2012140652A1 (en) * 2011-04-11 2012-10-18 Lamos Inc. Anodized aluminum substrate
WO2012155099A1 (en) * 2011-05-12 2012-11-15 Universal Display Corporation Flexible lighting devices
US20140174496A1 (en) * 2012-12-21 2014-06-26 Georgia Tech Research Corporation Hybrid generator using thermoelectric generation and piezoelectric generation
WO2015071635A1 (en) * 2013-11-15 2015-05-21 Cambridge Nanotherm Limited Flexible electronic substrate

Patent Citations (7)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US6274803B1 (en) * 1999-08-10 2001-08-14 Matsushita Electric Works, Ltd. Thermoelectric module with improved heat-transfer efficiency and method of manufacturing the same
EP2109161A1 (en) * 2008-04-11 2009-10-14 Xerox Corporation Thin-film transistors
KR20100096345A (en) * 2009-02-24 2010-09-02 연세대학교 산학협력단 A thermoelectric device for a tactile sensor and an electrical power generator, and methods of its fabrication
WO2012140652A1 (en) * 2011-04-11 2012-10-18 Lamos Inc. Anodized aluminum substrate
WO2012155099A1 (en) * 2011-05-12 2012-11-15 Universal Display Corporation Flexible lighting devices
US20140174496A1 (en) * 2012-12-21 2014-06-26 Georgia Tech Research Corporation Hybrid generator using thermoelectric generation and piezoelectric generation
WO2015071635A1 (en) * 2013-11-15 2015-05-21 Cambridge Nanotherm Limited Flexible electronic substrate

Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2023283188A1 (en) * 2021-07-05 2023-01-12 Soft-Tex International, Inc. Bedding systems based on localized climate control, and related methods

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