JP4134982B2 - Cold storage method, cold storage system, cold storage agent, and method of extracting cold - Google Patents
Cold storage method, cold storage system, cold storage agent, and method of extracting cold Download PDFInfo
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Description
本発明は、冷房などの空調設備や、食品等の冷却装置などに用いられる、蓄冷方法、蓄冷システム、蓄冷剤、および冷熱の取り出し方法に関する。 The present invention relates to a cold storage method, a cold storage system, a cold storage agent, and a method of extracting cold heat, which are used for air conditioning equipment such as cooling, and cooling devices for foods and the like.
この種の用途に使用される従来公知の蓄冷方法として以下のものがある。 Conventionally known cold storage methods used for this type of application include the following.
(1)冷水の温度差による蓄冷空調では、冷房用の冷水温度は5〜7℃であり、負荷の小さい時間に冷凍機により冷水を貯蔵タンク(蓄熱槽)に貯蔵する。冷水の比熱は1kcal/kgKであるため、利用温度差を7℃とすると、1kg冷水あたり7kcal/kgと単位重量当りの蓄冷量が少ないという欠点がある。 (1) In the cold storage air conditioning by the temperature difference of cold water, the cold water temperature for cooling is 5-7 degreeC, and cold water is stored in a storage tank (heat storage tank) with a refrigerator at the time of a small load. Since the specific heat of cold water is 1 kcal / kgK, there is a drawback that if the utilization temperature difference is 7 ° C., the amount of cold storage per unit weight is 7 kcal / kg per kg cold water.
(2)氷などの凝固・融解潜熱を用いた蓄冷氷の融解潜熱は、約80kcal/kgであるため、氷水の一部を氷にして蓄冷することで、蓄熱密度は冷水より高くできる。例えば、冷水中の氷の体積割合を20%とすると、氷の潜熱及び冷水の顕熱(温度差12℃の場合)を含めた蓄熱密度は、約28kcal/kgとなる。 (2) Since the latent heat of fusion of the cold storage ice using solidification / melting latent heat of ice or the like is about 80 kcal / kg, the heat storage density can be made higher than that of the cold water by storing a part of the ice water as ice. For example, if the volume ratio of ice in cold water is 20%, the heat storage density including the latent heat of ice and the sensible heat of cold water (temperature difference of 12 ° C.) is about 28 kcal / kg.
しかし、氷を生成させるためには、冷水を0℃以下に冷却しなければならず、冷水を5℃に冷却するよりも冷凍機の動力は大きくなるのが欠点である。 However, in order to generate ice, cold water must be cooled to 0 ° C. or lower, and the disadvantage is that the power of the refrigerator becomes larger than that of cooling cold water to 5 ° C.
(3)氷以外の固液相変化物質を用いた蓄冷水や氷以外の冷熱蓄熱材として利用可能な物質として、LiClO2・3H2OやNa2SO4・10H2O+NH4Clなどの無機水和塩類や気体水和物が知られている(非特許文献1、非特許文献2参照)。しかし、LiClO2・3H2OやNa2SO4・10H2O+NH4Clなどの無機水和塩類は、比較的潜熱量は大きいものの、調和融点(後述)を持たず、無水塩の濃度によって水和物が変化する。このため、冷却・加熱過程で相分離をおこし、所定の蓄熱量が得られなくなる問題が生ずる。 (3) Inorganic materials such as LiClO 2 .3H 2 O and Na 2 SO 4 .10H 2 O + NH 4 Cl that can be used as cold storage water using solid-liquid phase change materials other than ice and cold heat storage materials other than ice Hydrated salts and gaseous hydrates are known (see Non-Patent Document 1 and Non-Patent Document 2). However, inorganic hydrated salts such as LiClO 2 .3H 2 O and Na 2 SO 4 .10H 2 O + NH 4 Cl have a relatively large amount of latent heat but do not have a harmonic melting point (described later). Japanese products change. For this reason, there arises a problem that phase separation is performed in the cooling and heating process, and a predetermined heat storage amount cannot be obtained.
また、非特許文献1に記載されている気体水和物は、R11やR12などのオゾン破壊係数の大きい物質であったり、また、大気圧下では気体であるため、加圧された密閉容器や配管を用いる必要があり、蓄冷装置が高価なものとなる。
以上のように、今までに実用化あるいは提案されてきた蓄冷方法には、それぞれ問題点があった。本発明は、これらの課題を解決すべくなされたもので、蓄冷材に求められる蓄熱密度(潜熱量)が大きく、安定した熱特性を有し、経済性、安全性があり取り扱いが容易である包接水和物を用いた蓄冷方法、蓄冷システム、蓄熱剤、および冷熱の取り出し方法を提供することを目的とする。 As described above, the cold storage methods that have been put to practical use or proposed so far have problems. The present invention has been made to solve these problems, has a large heat storage density (latent heat amount) required for a cold storage material, has stable thermal characteristics, is economical, safe and easy to handle. An object is to provide a cold storage method using a clathrate hydrate, a cold storage system, a heat storage agent, and a method of extracting cold.
すなわち本発明は、
(1)包接水和物生成物質を含み、その濃度が調和融点を与える濃度未満に設定された水溶液を用意する工程と、この水溶液を冷却して包接水和物のスラリを生成し調和融点より低い温度で冷熱を蓄冷する工程とを有することを特徴とする蓄冷方法。
That is, the present invention
(1) A step of preparing an aqueous solution containing a clathrate hydrate-forming substance, the concentration of which is set to a concentration lower than a concentration that gives a harmonic melting point, and cooling the aqueous solution to produce a clathrate hydrate slurry to harmonize And a step of storing cold energy at a temperature lower than the melting point.
(2)前記水溶液が、融点降下剤を含むことを特徴とする(1)に記載の蓄冷方法。 (2) The cold storage method according to (1), wherein the aqueous solution contains a melting point depressant.
(3)前記包接水和物生成物質は、テトラ−n−ブチルアンモニウム塩、テトラiso−アミルアンモニウム塩、テトラ−n−ブチルフォスフォニウム塩、及びトリiso−アミルサルフォニウム塩の群から選択される一種又は二種以上であることを特徴とする(1)又は(2)に記載の蓄冷方法。 (3) The clathrate hydrate-forming substance is selected from the group consisting of tetra-n-butylammonium salt, tetraiso-amylammonium salt, tetra-n-butylphosphonium salt, and triiso-amylsulfonium salt. The cold storage method according to (1) or (2), wherein one or two or more types are selected.
(4)調和融点を与える濃度未満に設定された包接水和物生成物質の水溶液を収容する手段と、この収容手段に収容された水溶液を冷却して、包接水和物のスラリを生成し調和融点より低い温度で冷熱を蓄冷する手段とを備えることを特徴とする蓄冷システム。 (4) A means for containing an aqueous solution of clathrate hydrate-forming substance set to a concentration that gives a harmonic melting point and a slurry of clathrate hydrate are produced by cooling the aqueous solution contained in the containing means. And means for storing cold heat at a temperature lower than the harmonic melting point.
(5)調和融点を与える濃度未満に設定された包接水和物生成物質の水溶液を収容する手段と、この収容手段に収容された水溶液を冷却して、包接水和物のスラリを生成し調和融点より低い温度で冷熱を蓄冷する手段と、この包接水和物のスラリに蓄冷された冷熱を取り出す熱交換器を備えることを特徴とする蓄冷システム (5) A means for containing an aqueous solution of clathrate hydrate-forming substance set to a concentration that gives a harmonic melting point and a slurry of clathrate hydrate are produced by cooling the aqueous solution contained in the containing means. A cold storage system comprising: means for storing cold heat at a temperature lower than the harmonic melting point; and a heat exchanger for taking out the cold heat stored in the clathrate hydrate slurry.
(6)包接水和物生成物質を含む水溶液であって、その調和融点を与える濃度未満に設定されていて、調和融点より低い温度で冷却されることにより、冷熱を蓄冷した包接水和物のスラリを生成することを特徴とする蓄冷剤。 (6) An clathrate hydrate that is an aqueous solution containing a clathrate hydrate-forming substance, and is set at a concentration lower than its harmonic melting point and cooled at a temperature lower than the harmonic melting point , thereby storing cold heat. cold storage agent characterized and generating child slurry of the object.
(7)前記水溶液が、融点降下剤を含むことを特徴とする(6)に記載の蓄冷剤。 (7) The cold storage agent according to (6), wherein the aqueous solution contains a melting point depressant.
(8)前記包接水和物生成物質は、テトラ−n−ブチルアンモニウム塩、テトラiso−アミルアンモニウム塩、テトラ−n−ブチルフォスフォニウム塩、及びトリiso−アミルサルフォニウム塩の群から選択される一種又は二種以上であることを特徴とする(6)又は(7)に記載の蓄冷剤。 (8) The clathrate hydrate-forming substance is selected from the group consisting of tetra-n-butylammonium salt, tetraiso-amylammonium salt, tetra-n-butylphosphonium salt, and triiso-amylsulfonium salt. The regenerator according to (6) or (7), wherein the regenerator is one or more selected.
(9)包接水和物生成物質を含み、その濃度が調和融点を与える濃度未満に設定された水溶液を用意する工程と、この水溶液を冷却して包接水和物のスラリを生成し調和融点より低い温度で冷熱を蓄冷する工程と、この包接水和物のスラリに蓄冷された冷熱を熱交換により取り出す工程を有することを特徴とする冷熱の取り出し方法、である。 (9) A step of preparing an aqueous solution containing a clathrate hydrate-forming substance, the concentration of which is set to a concentration lower than a concentration that gives a harmonic melting point, and cooling the aqueous solution to generate a clathrate hydrate slurry to harmonize A method for extracting cold energy, comprising: a step of storing cold energy at a temperature lower than the melting point; and a step of extracting cold energy stored in the clathrate hydrate slurry by heat exchange.
本発明に係る蓄冷剤を用いれば、蓄熱密度が大きく、安定した熱特性を有する。また、従来は触媒として用いられており、容易に入手可能であり、経済的かつ安全である。特に、調和融点を与える上記水溶液濃度より低い濃度に設定した水溶液を用いると、所望の低い温度範囲で冷熱を蓄冷でき、その結果、低い温度で取出せる。そして、熱交換効率が高いので、熱交換器をコンパクトにでき、さらに、コストも安く、水和物スラリの輸送や貯蔵のハンドリングが容易となる。 If the cool storage agent which concerns on this invention is used, a heat storage density is large and it has the stable thermal characteristic. Moreover, it is conventionally used as a catalyst, is easily available, and is economical and safe. In particular, when an aqueous solution set to a concentration lower than the above aqueous solution concentration giving a harmonic melting point is used, cold energy can be stored in a desired low temperature range, and as a result, it can be taken out at a low temperature. Further, since the heat exchange efficiency is high, the heat exchanger can be made compact, the cost is low, and the transportation and storage handling of the hydrate slurry is facilitated.
さらに、水より融点の低い物質を混入させることによって、同じ塩を用いた水溶液で任意の融点を持つ蓄冷剤を作ることができるため、汎用性が高く、コスト安にもなる。 Further, by incorporating a substance having a melting point lower than that of water, a regenerator having an arbitrary melting point can be made with an aqueous solution using the same salt, so that the versatility is high and the cost is low.
本発明に係る包接水和物とは、水分子(ホスト分子)で構成された籠状の包接格子内に以下の様なゲスト分子が包み込まれて結晶化する化合物をいう。ゲスト分子として、テトラ−n−ブチルアンモニウム塩、テトラiso−アミルアンモニウム塩、テトラ−n−フォスフォニウム塩、トリiso−アミルサルフォニウム塩の例として、テトラ−n−ブチルアンモニウム塩としてフッ化テトラ−n−ブチルアンモニウム(n−C4H9)4NF),塩化テトラ−n−ブチルアンモニウム((n−C4H9)4NCl),臭化テトラ−n−ブチルアンモニウム((n−C4H9)4NBr)などがある。 The clathrate hydrate according to the present invention refers to a compound that crystallizes by encapsulating the following guest molecules in a cage-like clathrate composed of water molecules (host molecules). Examples of guest molecules include tetra-n-butylammonium salt, tetraiso-amylammonium salt, tetra-n-phosphonium salt, triiso-amylsulfonium salt, fluoride as tetra-n-butylammonium salt Tetra-n-butylammonium (n-C 4 H 9 ) 4 NF), tetra-n-butylammonium chloride ((n-C 4 H 9 ) 4 NCl), tetra-n-butylammonium bromide ((n- C 4 H 9 ) 4 NBr).
これらF,Cl,Brの代わりに酢酸(CH3CO2),重炭酸(HCO2),クロム酸(CrO4),タングステン酸(WO4),シュウ酸(C2O4),リン酸(HPO4)でもよい。その他の上記塩も同様である。 Instead of these F, Cl and Br, acetic acid (CH 3 CO 2 ), bicarbonate (HCO 2 ), chromic acid (CrO 4 ), tungstic acid (WO 4 ), oxalic acid (C 2 O 4 ), phosphoric acid ( HPO 4 ) may also be used. The same applies to the other salts.
以下、臭化テトラ−n−ブチルアンモニウム((n−C4H9)4NBr)を例にとり、本発明の蓄冷システムを説明する。水溶液濃度と融点の関係を図1に示す。また、包接水和物が生成、分解するときの反応式を式(1)に示す。 Hereinafter, the cold storage system of the present invention will be described by taking tetra-n-butylammonium bromide ((n-C 4 H 9 ) 4 NBr) as an example. The relationship between the aqueous solution concentration and the melting point is shown in FIG. The reaction formula when the clathrate hydrate is generated and decomposed is shown in Formula (1).
(n-C4H9)4NBr+n・H2O←→(n-C4H9)4NBr・n・H2O…式(1)
ここで、nは水和数で、その値はおよそ26で常に一定である。
(nC 4 H 9 ) 4 NBr + n · H 2 O ← → (nC 4 H 9 ) 4 NBr · n · H 2 O ... Formula (1)
Here, n is a hydration number, and its value is approximately 26 and is always constant.
図1に示されるように、この包接水和物生成物質を含む水溶液は、水溶液濃度約40wt%で融点が極大値、11.8℃である。この水溶液濃度の融点は調和融点と呼ばれ、ここでは水溶液中の濃度と包接水和物中の塩分濃度が等しい。 As shown in FIG. 1, the aqueous solution containing the clathrate hydrate-forming substance has an aqueous solution concentration of about 40 wt% and a melting point at a maximum value of 11.8 ° C. The melting point of this aqueous solution concentration is called the harmonic melting point, and here, the concentration in the aqueous solution is equal to the salinity concentration in the clathrate hydrate.
従って、調和融点を与える水溶液濃度(この例では常温における塩濃度が40wt%)に設定した水溶液を用いてこれを冷却すると、調和融点(11.8℃)で包接水和物が生成しはじめ、水溶液が全て包接水和物になるまでこの融点で一定になる。分解(融解)時も同様にこの融点一定で冷熱を放出する。なお、潜熱量は約46kcal/kgであり、利用上限温度を12℃とすると、水和物の体積割合が56%で蓄熱密度は26kcal/kgとなる。 Therefore, when an aqueous solution set to a concentration of an aqueous solution giving a harmonic melting point (in this example, the salt concentration at room temperature is 40 wt%) is cooled, clathrate hydrate begins to form at the harmonic melting point (11.8 ° C.). The melting point remains constant until the aqueous solution is all clathrate hydrate. Similarly, at the time of decomposition (melting), cold heat is released with this constant melting point. The latent heat amount is about 46 kcal / kg. If the upper limit temperature of use is 12 ° C., the volume ratio of hydrate is 56% and the heat storage density is 26 kcal / kg.
このようにこの蓄冷剤は、蓄熱密度が大きく、安定した熱特性を有する。また、従来は触媒として用いられているので容易に入手可能であり、経済的かつ安全である。 Thus, this cool storage agent has a large heat storage density and stable thermal characteristics. Further, since it is conventionally used as a catalyst, it can be easily obtained, and is economical and safe.
また、調和融点を与える上記水溶液濃度より低い濃度に設定した水溶液(例えば常温で27.2wt%の水溶液)を用いて冷却すると、約9.4℃で水和物が生成しはじめ、次第に水溶液中の塩分濃度が低下していき、それにつれて水和物の生成温度も低下していく。すなわち、図1の曲線に沿って包接水和物の生成温度も下がる。空調に適する15℃程度の水・空気を作るために水溶液を5℃まで冷却すると、水溶液中の塩分濃度は約17wt%になる。このとき、水溶液の43%が水和物になる。また蓄熱量は、およそ26kcal/kgとなる(水和物の比熱を0.53kcal/kgK,水溶液の比熱を0.96kcal/kgKとした)。また、包接水和物の潜熱を利用する場合には常温で濃度4%以上の濃度にする必要がある。
Further, when cooling with an aqueous solution set to a concentration lower than the above aqueous solution concentration giving a harmonic melting point (for example, an aqueous solution of 27.2 wt% at room temperature), a hydrate begins to be formed at about 9.4 ° C., and gradually in the aqueous solution. As the salt concentration of the hydrate decreases, the hydrate formation temperature also decreases. That is, the production temperature of clathrate hydrate also decreases along the curve of FIG. When the aqueous solution is cooled to 5 ° C. in order to produce water / air at about 15 ° C. suitable for air conditioning, the salt concentration in the aqueous solution becomes about 17 wt%. At this time, 43% of the aqueous solution becomes a hydrate. The heat storage amount is approximately 26 kcal / kg (the specific heat of the hydrate is 0.53 kcal / kgK and the specific heat of the aqueous solution is 0.96 kcal / kgK). Further, when utilizing the latent heat of clathrate hydrate, it is necessary to make the
このように、調和融点を与える上記水溶液濃度より低い濃度に設定した水溶液を用いると、更に以下の利点を備える。 Thus, when the aqueous solution set to a concentration lower than the concentration of the aqueous solution giving a harmonic melting point is used, the following advantages are further provided.
(1)融点(生成温度)が低温側に変化するため、低い温度の冷熱を蓄冷でき、その結果、所望の低い温度で取出することができる。 (1) Since the melting point (generation temperature) changes to the low temperature side, cold heat at a low temperature can be stored, and as a result, it can be taken out at a desired low temperature.
(2)融点(生成温度)が低温側に変化していくため、水和物と水又は空気と熱交換させる場合、その温度差がほぼ一定でしかも大きい。このため熱交換効率が高く、熱交換器をコンパクトとすることができる。即ち、熱交換器で20℃の水または空気を冷却して15℃とするに際し、図2のaに示す調和融点濃度の場合、水又は空気の出側(蓄冷剤の入り側)の蓄冷剤の温度が11.8℃であり、その温度差が3.8℃しかないが、図2のbに示す調和融点濃度より低い場合、例えば水又は空気の出側(蓄冷剤の入り側)の蓄冷剤の温度が5℃であり、その温度差を10℃とすることができる。 (2) Since the melting point (generation temperature) changes to the low temperature side, when heat exchange is performed with hydrate and water or air, the temperature difference is substantially constant and large. For this reason, heat exchange efficiency is high and a heat exchanger can be made compact. That is, when the water or air at 20 ° C. is cooled to 15 ° C. with a heat exchanger, the regenerator on the outlet side of water or air (on the side of the regenerator) in the case of the harmonic melting point concentration shown in FIG. The temperature is 11.8 ° C. and the temperature difference is only 3.8 ° C., but if it is lower than the harmonic melting point concentration shown in FIG. 2b, for example, water or air exit side (cold storage agent entrance side) The temperature of the cold storage agent is 5 ° C., and the temperature difference can be 10 ° C.
(3)ほぼ同じ利用上限温度で蓄熱密度が同じ場合、水溶液中の塩分濃度を低くできるため、その分低コストになる。 (3) When the heat storage density is the same at almost the same use upper limit temperature, the salinity concentration in the aqueous solution can be lowered, and the cost is reduced accordingly.
(4)ほぼ同じ利用上限温度で蓄熱密度が同じ場合、水和物の体積割合は小さくてすむため、水和物スラリの輸送や貯蔵のハンドリングが容易となる。顕熱分が大きくなる。即ち、蓄熱量は「潜熱」+「顕熱」で示されるが、蓄熱量を同じとした場合、調和融点より低い濃度の方が顕熱分が大きいため、水和物の体積割合が小さくてすむ。この試算を表1に示す。
次に本発明では、水溶液に水よりも凝固点の小さい物質を混入させて、包接水和物の生成温度(融点)を低下させることができる。臭化テトラ−n−ブチルアンモニウム((n−C4H9)4NBr)を例に取ると、その調和融点は、11.8℃であり、水溶液濃度と融点の関係は上述したように図1のようになる。 Next, in the present invention, a production temperature (melting point) of clathrate hydrate can be lowered by mixing a substance having a freezing point smaller than water in the aqueous solution. Taking tetra-n-butylammonium bromide ((n-C 4 H 9 ) 4 NBr) as an example, its harmonic melting point is 11.8 ° C., and the relationship between the aqueous solution concentration and the melting point is as shown above. It becomes like 1.
この水溶液に、エチレングリコール、プロピレングリコールなど融点降下剤(水よりも融点の低い物質)を混入させると、水溶液の融点は、この物質の混入量によって低下する。そこで、用途により利用温度幅を下げる必要がある場合、これら物質を適量混入させることにより、任意の融点を持つ蓄冷剤を作ることができる。 When a melting point depressant (a substance having a melting point lower than that of water) such as ethylene glycol or propylene glycol is mixed in this aqueous solution, the melting point of the aqueous solution is lowered depending on the amount of this substance. Therefore, when it is necessary to lower the use temperature range depending on the application, a regenerator having an arbitrary melting point can be made by mixing an appropriate amount of these substances.
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JP4736776B2 (en) * | 2005-12-14 | 2011-07-27 | Jfeエンジニアリング株式会社 | Coolant and cold insulation material |
JP4893036B2 (en) * | 2006-03-17 | 2012-03-07 | Jfeエンジニアリング株式会社 | Thermal storage agent and method for preparing thermal storage agent |
JP4752618B2 (en) * | 2006-05-30 | 2011-08-17 | パナソニック株式会社 | Heat storage system |
JP4840075B2 (en) * | 2006-10-19 | 2011-12-21 | Jfeエンジニアリング株式会社 | Coolant and cold insulation material |
JP5076554B2 (en) * | 2007-03-02 | 2012-11-21 | Jfeエンジニアリング株式会社 | Aqueous solution containing clathrate hydrate, clathrate hydrate and slurry thereof, method for producing clathrate hydrate slurry, and latent heat storage agent |
JP5157197B2 (en) * | 2007-03-02 | 2013-03-06 | Jfeエンジニアリング株式会社 | Aqueous solution, clathrate hydrate and slurry thereof, method for adjusting melting point of clathrate hydrate, method for increasing latent heat storage amount of slurry of clathrate hydrate, and method for producing clathrate hydrate or slurry thereof |
JP5056072B2 (en) * | 2007-03-02 | 2012-10-24 | Jfeエンジニアリング株式会社 | Tetra-n-butylammonium phosphate and method for producing latent heat storage medium |
AU2008222018A1 (en) | 2007-03-02 | 2008-09-12 | Jfe Engineering Corporation | Latent heat storage substance, clathrate hydrate or slurry thereof, method for producing clathrate hydrate or slurry thereof, and latent heat storage agent |
JP5003213B2 (en) | 2007-03-06 | 2012-08-15 | Jfeエンジニアリング株式会社 | Method to increase heat storage rate of heat storage agent, clathrate hydrate |
JP5125316B2 (en) * | 2007-08-24 | 2013-01-23 | Jfeエンジニアリング株式会社 | Raw material for clathrate hydrate production, method for producing clathrate hydrate or slurry thereof, and method for reducing pressure loss generated when cooling an aqueous solution for clathrate hydrate production |
JP5104160B2 (en) * | 2007-09-26 | 2012-12-19 | Jfeエンジニアリング株式会社 | Aqueous solution for producing clathrate hydrate, heat storage agent, clathrate hydrate or manufacturing method thereof, slurry storage method, and method for preparing aqueous solution for generating latent heat storage agent or main component thereof |
JP5104159B2 (en) * | 2007-09-26 | 2012-12-19 | Jfeエンジニアリング株式会社 | Aqueous solution for producing clathrate hydrate, heat storage agent, clathrate hydrate or manufacturing method thereof, slurry storage method, and method for preparing aqueous solution for generating latent heat storage agent or main component thereof |
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JP2010230228A (en) * | 2009-03-26 | 2010-10-14 | Jfe Engineering Corp | Hydrate forming method, heat storage method, and heat storage device |
WO2016075941A1 (en) * | 2014-11-14 | 2016-05-19 | 株式会社デンソー | Super-cooling release material and method for producing same |
JP6601145B2 (en) * | 2014-11-14 | 2019-11-06 | 株式会社デンソー | Subcool release substance and method for producing the same |
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