WO2003008500A1 - Materiau constitue d'un gel de polyurethanne, son procede de production et ses utilisations - Google Patents

Materiau constitue d'un gel de polyurethanne, son procede de production et ses utilisations Download PDF

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Publication number
WO2003008500A1
WO2003008500A1 PCT/DE2002/002605 DE0202605W WO03008500A1 WO 2003008500 A1 WO2003008500 A1 WO 2003008500A1 DE 0202605 W DE0202605 W DE 0202605W WO 03008500 A1 WO03008500 A1 WO 03008500A1
Authority
WO
WIPO (PCT)
Prior art keywords
phase change
gel
pcm
polyurethane
weight
Prior art date
Application number
PCT/DE2002/002605
Other languages
German (de)
English (en)
Inventor
Barbara Pause
Adolf Stender
Peter Gansen
Original Assignee
Otto Bock Healthcare Gmbh
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
Priority claimed from EP02010042A external-priority patent/EP1277801B1/fr
Application filed by Otto Bock Healthcare Gmbh filed Critical Otto Bock Healthcare Gmbh
Priority to DE10293140T priority Critical patent/DE10293140D2/de
Priority to US10/484,528 priority patent/US20040234726A1/en
Publication of WO2003008500A1 publication Critical patent/WO2003008500A1/fr

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Classifications

    • C—CHEMISTRY; METALLURGY
    • C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09K—MATERIALS FOR MISCELLANEOUS APPLICATIONS, NOT PROVIDED FOR ELSEWHERE
    • C09K5/00—Heat-transfer, heat-exchange or heat-storage materials, e.g. refrigerants; Materials for the production of heat or cold by chemical reactions other than by combustion
    • C09K5/02—Materials undergoing a change of physical state when used
    • C09K5/06—Materials undergoing a change of physical state when used the change of state being from liquid to solid or vice versa
    • C09K5/063—Materials absorbing or liberating heat during crystallisation; Heat storage materials
    • A—HUMAN NECESSITIES
    • A43—FOOTWEAR
    • A43B—CHARACTERISTIC FEATURES OF FOOTWEAR; PARTS OF FOOTWEAR
    • A43B17/00—Insoles for insertion, e.g. footbeds or inlays, for attachment to the shoe after the upper has been joined
    • A43B17/003—Insoles for insertion, e.g. footbeds or inlays, for attachment to the shoe after the upper has been joined characterised by the material
    • A—HUMAN NECESSITIES
    • A43—FOOTWEAR
    • A43B—CHARACTERISTIC FEATURES OF FOOTWEAR; PARTS OF FOOTWEAR
    • A43B17/00—Insoles for insertion, e.g. footbeds or inlays, for attachment to the shoe after the upper has been joined
    • A43B17/02—Insoles for insertion, e.g. footbeds or inlays, for attachment to the shoe after the upper has been joined wedge-like or resilient
    • A43B17/026—Insoles for insertion, e.g. footbeds or inlays, for attachment to the shoe after the upper has been joined wedge-like or resilient filled with a non-compressible fluid, e.g. gel, water
    • A—HUMAN NECESSITIES
    • A43—FOOTWEAR
    • A43B—CHARACTERISTIC FEATURES OF FOOTWEAR; PARTS OF FOOTWEAR
    • A43B7/00—Footwear with health or hygienic arrangements
    • A43B7/34—Footwear with health or hygienic arrangements with protection against heat or cold
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
    • C08K5/00—Use of organic ingredients
    • C08K5/0008—Organic ingredients according to more than one of the "one dot" groups of C08K5/01 - C08K5/59
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
    • C08K5/00—Use of organic ingredients
    • C08K5/01—Hydrocarbons
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
    • C08L75/00—Compositions of polyureas or polyurethanes; Compositions of derivatives of such polymers
    • C08L75/04—Polyurethanes
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L23/00—Details of semiconductor or other solid state devices
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L23/00—Details of semiconductor or other solid state devices
    • H01L23/34—Arrangements for cooling, heating, ventilating or temperature compensation ; Temperature sensing arrangements
    • H01L23/42—Fillings or auxiliary members in containers or encapsulations selected or arranged to facilitate heating or cooling
    • H01L23/427—Cooling by change of state, e.g. use of heat pipes
    • H01L23/4275—Cooling by change of state, e.g. use of heat pipes by melting or evaporation of solids
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08G—MACROMOLECULAR COMPOUNDS OBTAINED OTHERWISE THAN BY REACTIONS ONLY INVOLVING UNSATURATED CARBON-TO-CARBON BONDS
    • C08G2220/00—Compositions for preparing gels other than hydrogels, aerogels and xerogels
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08G—MACROMOLECULAR COMPOUNDS OBTAINED OTHERWISE THAN BY REACTIONS ONLY INVOLVING UNSATURATED CARBON-TO-CARBON BONDS
    • C08G2350/00—Acoustic or vibration damping material
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08G—MACROMOLECULAR COMPOUNDS OBTAINED OTHERWISE THAN BY REACTIONS ONLY INVOLVING UNSATURATED CARBON-TO-CARBON BONDS
    • C08G2410/00—Soles
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L2924/00—Indexing scheme for arrangements or methods for connecting or disconnecting semiconductor or solid-state bodies as covered by H01L24/00
    • H01L2924/0001—Technical content checked by a classifier
    • H01L2924/0002—Not covered by any one of groups H01L24/00, H01L24/00 and H01L2224/00

Definitions

  • the invention relates to a material made of a polyurethane gel with the finely distributed phase change materials contained therein, so-called “phase change materials” (PCM), a method for producing such materials and associated uses.
  • PCM phase change materials
  • phase change materials introduced or applied have the ability to change their state of matter within a certain (desired and adjustable) temperature range.
  • a phase transition from the solid to the liquid state occurs.
  • the PCM absorbs and stores a large amount of latent heat.
  • the temperature of the PCM remains almost constant throughout the process.
  • the PCM Before being used in functional textiles, the PCM is microencapsulated to prevent the molten PCM from leaking into the textile structure.
  • the amount of latent heat that is absorbed by a PCM during the phase transition is compared to the specific heat in an ordinary heating process.
  • the ice-water transition is used for comparison. When ice melts, it absorbs a latent heat of about 335 J / g. If the water is heated further, it absorbs a specific heat of only 4 J / g during a temperature increase of 1 ° C.
  • the absorption of latent heat during the phase transition from ice to water is therefore almost 100 times greater than the absorption of specific heat during the normal heating process outside the phase transition range.
  • PCMs In addition to the ice / water system, more than 500 natural and synthetic PCMs are known. These materials differ in their phase transition temperatures and their heat absorption capacities.
  • the crystalline alkanes are used either in technical purity of approx. 95% or in mixtures which are intended to cover certain phase transition temperature ranges.
  • the crystalline alkanes are non-toxic, non-corrosive and non-hygroscopic.
  • the thermal behavior of these PCMs remains stable even with continuous use.
  • Crystalline alkanes are by-products from the oil refinery and therefore cheap. They are pure, as are also available in mixtures defined according to the melting range.
  • PCMs microencapsulated crystalline alkanes
  • These microencapsulated PCMs are applied to the textiles by placing them in acrylic fibers or polyurethane foams and applying them to the fibers as a coating.
  • U.S. Patent 4,756,958 describes a fiber with integrated microcapsules filled with PCM.
  • the fiber has improved thermal properties in a predetermined temperature range.
  • Microencapsulation processes are very time-consuming and complicated, multi-stage processes. Microencapsulated PCMs are therefore very expensive.
  • Polyurethane gels are known, which among other things. are characterized by high deformability and can be used, for example, for seat cushions and upholstery. However, these polyurethane gels often cause an uncomfortable feeling of cold and poor air conditioning when in contact with the body.
  • the object of the invention is to improve the thermal behavior of polyurethane gels in the sense of a temperature-compensating behavior.
  • the invention provides a material made of a polyurethane gel, which contains finely divided phase change materials (PCMs).
  • phase change materials do not have to be encapsulated and still do not diffuse or agglomerate.
  • Finely divided PCMs emulsified or dispersed in the polyurethane gel remain stable over long periods of use.
  • the polyurethanes used for polyurethane gels are covalently cross-linked polyurethane matrices with high molecular weights.
  • the gel structure comes about through a suitable choice of the functionalities and molecular weights of the starting components.
  • the polyurethane gels used can contain additives and additives common in polyurethane chemistry.
  • the gel compositions used for the invention are preferably produced with raw materials having an isocyanate functionality and a functionality of the polyol component of at least 5.2, more preferably at least 6.5 and in particular of at least 7.5.
  • the polyol component for the preparation of the gel can consist of one or more polyols with a molecular weight between 1,000 and 1,200 and an OH number between 20 and 112, the product of the functionalities of the polyurethane-forming components being at least 5.2, as above indicated, and the isocyanate index is between 1 5 and 60.
  • Preferred isocyanates used for gel preparation are those of the formula Q (NCO) n, where n is 2 to 4 and Q is an aliphatic hydrocarbon radical with 8 to 18 carbon atoms, a cycloaliphatic hydrocarbon radical with 4 to 15 carbon atoms aromatic hydrocarbon radical having 6 to 15 C atoms or an araliphatic hydrocarbon radical having 8 to 15 C atoms.
  • the Isocyanates are used in pure form or in a conventional isocyanate modification such as urethanization, allphanatization or biuretization, as is known to the person skilled in the art.
  • PCMs phase change materials or phase change materials (PCMs) whose phase transition is in the desired temperature range and which can be incorporated in the gel production.
  • PCMs phase change materials
  • These can be paraffins or fats, for example. Crystalline alkanes are preferably used.
  • the melting points or melting ranges of the PCMs used are preferably between 20 and 45 ° C, more preferably between 34 and 39 ° C. In applications in which the material is supposed to provide a body temperature compensation, a phase transition area at medium human body temperature is ideal in order to be able to immediately absorb overheating - for example during sports.
  • the PCMs are preferably incorporated into the material in a weight fraction of up to 60% by weight, more preferably up to 40% by weight, based on the weight of the weight.
  • Fillers may also be contained in the material.
  • the person skilled in the art can select the fillers and the usable amounts of these fillers within the scope of what is generally known in polymer chemistry and in particular in polyurethane chemistry.
  • elastic hollow microspheres can also be provided as fillers, the shells preferably consisting of polymeric material, in particular polyolefin.
  • the elastic hollow microspheres can, if this is additionally desired, be expanded or expandable under processing conditions. Hollow microspheres are gas-filled (air-filled) microballoons, whereby the spherical shape is not important. Often one speaks of "microcellular material" or of microcells.
  • the hollow microspheres reduce the specific weight and influence the mechanical properties of the material. Up to 20, preferably up to 10 wt.% Microcells used. Suitable hollow microspheres, as well as other fillers, are commercially available.
  • Shoe insoles can preferably consist of the new material at least in some areas, for example in the area of the foot pressure points.
  • Soles, mattresses, seat covers and pillows can be provided with a textile cover.
  • the material according to the invention can be laminated directly onto textile materials.
  • the invention also includes a method for producing the new material.
  • the above-mentioned polyurethane components are preferably used. Suitable compositions for polyurethane gels are described, for example, in EP 057 838 and also EP 0 51 1 570.
  • the PCMs are added to the starting components or at the latest during gel formation. As a result, they are permanently integrated into the solid polyurethane structure that forms.
  • the material according to the invention can be produced particularly advantageously by emulsifying or dispersing the phase change material in a liquid PU component and then converting the PU components to the polyurethane gel.
  • the PCM can also be introduced into the finished polyurethane mixture before gel formation. Which procedure is chosen also depends on the desired distribution profile. Experts can use trials to determine the best way to incorporate the PCM.
  • phase change material preferably an alkane in the liquid state
  • the liquid PCM is initially under formation a liquid / liquid emulsion incorporated into the polyol component, which is then processed as usual.
  • the degree of fine distribution of the PCM in the emulsion depends, inter alia, on the intensity and duration with which the mixture is mixed, ie generally stirred. Suitable additives such as stabilizers and emulsifiers also influence the degree of fine distribution. The person skilled in the art can set this within certain limits and thereby influence the distribution of the PCM in the later material.
  • the emulsion can preferably be stabilized by adding an emulsion stabilizer.
  • an emulsion stabilizer for example, aerosils can be used for this.
  • liquid phase change material can be mixed with all components of the later gel material and stirred vigorously until gel formation begins. With the onset of gel formation, the mass is then generally poured into the shapes specified by the desired products.
  • solid, powdered PCMs could be incorporated into the gel or dispersed in the polyol component.
  • the processing is otherwise done in the usual way.
  • microencapsulated PCMs would also be possible within the gel material according to the invention, but only in a deteriorated embodiment, since the encapsulation fundamentally hinders the heat transfer, reduces the heat capacity and also makes the product more expensive overall.
  • Polyurethane gels have numerous advantageous properties that are already used in the prior art for many products. These well-known properties, such as good pressure distribution, high shock and shear force absorption, high elasticity and good resilience, are retained in the new phase change material. In addition to the properties of previously known polyurethane gels, the new material now has good air conditioning behavior, ie good heat regulation behavior.
  • Thermal conductivity of the PU gels of around 0.410 W / mK enables very good heat transfer between PCMs and the environment.
  • the structure of the polyurethane gel material allows a high loading with PCMs, for crystalline alkanes up to about 60% by weight based on the total weight of the material, preferably up to 40% by weight.
  • the polyurethane gel can contain other additives, in particular those which are already known for polyurethane gels, for example low-density particles.
  • a heat absorption capacity of about 140 kJ / m 2 can be achieved if crystalline alkanes with a latent heat capacity of about 200 J / g be used.
  • the heat storage capacity can be increased up to about 250 kJ / m 2 if the alkane PCM is used in a gel material with a specific weight of 31 50 g / m 2 .
  • the heat absorption capacity that can be achieved in this way far exceeds the capacity of conventional PU foams with microencapsulated PCMs, which is 20 to 40 kJ / m 2 .
  • Textiles coated with microencapsulated PCMs have latent heat absorption capacities of between 5 kJ / m 2 and 1 5 kJ / m 2 .
  • the PCM is supposed to absorb the excess heat given off by the foot and thus noticeably delay the temperature rise on the skin.
  • the delay in the rise in temperature leads to a later onset and, in addition, less sweating, which results in a significant improvement in thermophysiological comfort.
  • the combination of the excellent mechanical properties of the polyurethane gel materials and the thermal effect of the PCMs results in a significant improvement in comfort when using the insoles in a wide variety of shoe variants.
  • PCM-containing PU gel sole with 20% paraffin-PCM PCM-containing PU gel sole with 40% paraffin-PCM
  • the percentages relate to% by weight based on the total weight of the material.
  • paraffin PCM a commercially available paraffin mixture is, for example, Cera Ser® .
  • a calorimetric DSC measuring device With the help of a calorimetric DSC measuring device, the temperature ranges of latent heat absorption and release of the paraffin PCM contained in the insoles were determined and its heat storage capacity was determined.
  • MB microcells / hollow microspheres
  • the PU gel insoles used have different sizes and are therefore of different weights, among other things.
  • Table 3 contains the weights of the insoles used in the tests.
  • the latent heat storage capacity of the insoles was determined with reference to the sole weight.
  • the value in brackets refers to a uniform insole size that corresponds to shoe size 39/40.
  • the sole size was used in the wear tests.
  • Table 3 Weights of the insoles and latent heat storage capacity of the paraffin PCM contained in the soles
  • the tests consisted of a 30-minute run in a climatic chamber on the treadmill ergometer at a speed of about 8 km / h. During the tests, the ambient temperature was 21 ° C and the relative humidity 40%. For the tests, the respective sole pattern was placed in a normal sports shoe. In the tests, the test subjects wore cotton socks and normal sports clothing.
  • the temperature profile at a total of 4 skin measuring points (big toe, back of the foot, ankle and footbed) and at two points on the surface of the insole was continuously determined using a logging system.
  • the mean skin temperature was calculated from the temperature measurements at the four different skin measuring points.
  • the measurement results of the two sensors, which were located on the surface of the insole, were also averaged.
  • the increase in moisture in the microclimate was also determined.
  • Each sole pattern was tested twice and the test results obtained were averaged. The following were examined:
  • Fig. 1 Temperature development in the shoe microclimate
  • Fig. 2 Moisture development over 30 minutes.
  • Figure 2 shows that the heat absorption by the PCM leads to a significantly lower increase in moisture in the microclimate of the shoe. Overall, this leads to a significant increase in comfort when wearing the insoles according to the invention.
  • PCM-containing polyurethane gel can also improve the climate behavior of bicycle seats, chair cushions, car seats, wheelchair seats or mattresses, to name just a few examples.

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Organic Chemistry (AREA)
  • Physics & Mathematics (AREA)
  • Health & Medical Sciences (AREA)
  • Polymers & Plastics (AREA)
  • Medicinal Chemistry (AREA)
  • Materials Engineering (AREA)
  • Power Engineering (AREA)
  • Thermal Sciences (AREA)
  • Combustion & Propulsion (AREA)
  • Microelectronics & Electronic Packaging (AREA)
  • Computer Hardware Design (AREA)
  • Condensed Matter Physics & Semiconductors (AREA)
  • General Physics & Mathematics (AREA)
  • Wood Science & Technology (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Epidemiology (AREA)
  • General Health & Medical Sciences (AREA)
  • Public Health (AREA)
  • Polyurethanes Or Polyureas (AREA)
  • Compositions Of Macromolecular Compounds (AREA)
  • Footwear And Its Accessory, Manufacturing Method And Apparatuses (AREA)

Abstract

La présente invention concerne des matériaux à base de gel de polyuréthanne, comprenant des matières à changement de phase (PCM) finement dispersées dans lesdits matériaux, par exemple des hydrocarbures cristallins saturés. Ces matériaux permettent une régulation thermique au moyen d'une absorption de chaleur et d'un dégagement de chaleur dans la zone de transition de phase des PCM. L'utilisation de ce nouveau matériau dans des semelles de chaussure, des selles de vélo, des coussin de chaise et des articles similaires permet d'obtenir un meilleur confort.
PCT/DE2002/002605 2001-07-19 2002-07-17 Materiau constitue d'un gel de polyurethanne, son procede de production et ses utilisations WO2003008500A1 (fr)

Priority Applications (2)

Application Number Priority Date Filing Date Title
DE10293140T DE10293140D2 (de) 2001-07-19 2002-07-17 Werkstoff aus einem Polyurethan-Gel, Herstellungsverfahren und Verwendungen
US10/484,528 US20040234726A1 (en) 2001-07-19 2002-07-17 Material consisting of a polyurethane gel, production method and uses thereof

Applications Claiming Priority (4)

Application Number Priority Date Filing Date Title
US30664401P 2001-07-19 2001-07-19
US60/306,644 2001-07-19
EP02010042A EP1277801B1 (fr) 2001-07-19 2002-05-06 Matériau à base de gel de polyuréthanne, procédé de préparation et utilisations
EP02010042.6 2002-05-06

Publications (1)

Publication Number Publication Date
WO2003008500A1 true WO2003008500A1 (fr) 2003-01-30

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PCT/DE2002/002605 WO2003008500A1 (fr) 2001-07-19 2002-07-17 Materiau constitue d'un gel de polyurethanne, son procede de production et ses utilisations

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DE (1) DE10293140D2 (fr)
WO (1) WO2003008500A1 (fr)

Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US10687632B1 (en) 2016-04-03 2020-06-23 Soothsoft Innovations Worldwide, Inc. PCM containing liquid saturated foam device
CN113651634A (zh) * 2021-08-11 2021-11-16 吉林大学 一种防泄漏的复合储热材料的制备方法

Citations (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE2652255A1 (de) * 1975-11-17 1977-05-26 Nl Industries Inc Mittel und verfahren zum reinigen und abdichten der innenraeume von isolierten elektrischen einrichtungen
US4102716A (en) * 1976-05-11 1978-07-25 Minnesota Mining And Manufacturing Company Two-part reactive dielectric filler composition
EP0057839A1 (fr) * 1981-02-03 1982-08-18 Bayer Ag Gels sur la base d'une matrice de polyuréthane et de polyols de haut poids moléculaire, contenant, le cas échéant, des substances actives, un procédé pour leur fabrication ainsi que leur utilisation
US5713143A (en) * 1995-06-06 1998-02-03 Kendall Orthotics Orthotic system
US5939157A (en) * 1995-10-30 1999-08-17 Acushnet Company Conforming shoe construction using gels and method of making the same
WO2002034809A1 (fr) * 2000-10-27 2002-05-02 Atofina Composition isolante a base de gel elastomere polyurethane et son utilisation

Patent Citations (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE2652255A1 (de) * 1975-11-17 1977-05-26 Nl Industries Inc Mittel und verfahren zum reinigen und abdichten der innenraeume von isolierten elektrischen einrichtungen
US4102716A (en) * 1976-05-11 1978-07-25 Minnesota Mining And Manufacturing Company Two-part reactive dielectric filler composition
EP0057839A1 (fr) * 1981-02-03 1982-08-18 Bayer Ag Gels sur la base d'une matrice de polyuréthane et de polyols de haut poids moléculaire, contenant, le cas échéant, des substances actives, un procédé pour leur fabrication ainsi que leur utilisation
US5713143A (en) * 1995-06-06 1998-02-03 Kendall Orthotics Orthotic system
US5939157A (en) * 1995-10-30 1999-08-17 Acushnet Company Conforming shoe construction using gels and method of making the same
WO2002034809A1 (fr) * 2000-10-27 2002-05-02 Atofina Composition isolante a base de gel elastomere polyurethane et son utilisation

Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US10687632B1 (en) 2016-04-03 2020-06-23 Soothsoft Innovations Worldwide, Inc. PCM containing liquid saturated foam device
CN113651634A (zh) * 2021-08-11 2021-11-16 吉林大学 一种防泄漏的复合储热材料的制备方法

Also Published As

Publication number Publication date
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