TW201533937A - Flexible thermoelectric material film and manufacturing method thereof - Google Patents
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- 239000000463 material Substances 0.000 title claims abstract description 58
- 238000004519 manufacturing process Methods 0.000 title claims abstract description 23
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Abstract
Description
本發明係為一種熱電材料膜及其製造方法，尤指一種能自由彎曲的可撓式熱電材料膜。 The invention relates to a thermoelectric material film and a manufacturing method thereof, in particular to a flexible thermoelectric material film which can be freely bent.
近年來，隨著環保意識的提升，各種能減少碳排放量的發電方式漸漸受到各界的重視，其中，面對核能或火力發電在能量轉換時，無法轉換為電能的能量有極大部分轉變為熱能，並以廢熱的形式逸散，因此，能夠將這些發電廢熱的熱能轉換成電能的熱電材料成為一個最好的選擇。然而，理想的熱電材料必須具備有優良的導電係數(σ)及較低的導熱係數(κ)，而熱電轉換效率公式T中，ZT為熱電優質係數，S為西貝克(Seebeck)係數，而T為絕對溫度；其中，熱電優質係數(ZT)其值越大則熱電能量轉換效率越高。 In recent years, with the improvement of environmental awareness, various power generation methods that can reduce carbon emissions have gradually received attention from all walks of life. Among them, in the face of nuclear energy or thermal power generation, the energy that cannot be converted into electric energy is greatly converted into heat energy. And it is dissipated in the form of waste heat. Therefore, it is the best choice to be able to convert these thermal energy of waste heat from power generation into electrical energy. However, an ideal thermoelectric material must have an excellent conductivity (σ) and a low thermal conductivity (κ), while the thermoelectric conversion efficiency formula In T, ZT is the thermoelectric quality coefficient, S is the Seebeck coefficient, and T is the absolute temperature; among them, the higher the thermoelectric quality coefficient (ZT), the higher the thermoelectric energy conversion efficiency.
然而，要達到同時具有優良導電係數(σ)及低導熱係數(κ)，由無機材料所製成的熱電材料無非為最合適的選擇。有鑑於無機材料所製成的無機熱電材料雖具有較好的熱電優質係數(ZT)，相對的卻不具任意形變或彎折的方便性，使得其安裝位置、方便性及用途受到極大的限制。為了解決此問題，以有機材料製成的有機熱電材料因應而生，但現有的有機熱電材料仍存在著熱電優質係數(ZT)無法提升的瓶頸，係因相較於無機熱電材 料，有機熱電材料因其材質而無法擁有相對優良的導電係數(σ)；然而，現有針對有機熱電材料皆採用提升導電係數(σ)的方法來提高其整體的熱電優質係數(ZT)，但若如此，必會伴隨著西貝克(Seebeck)係數(S)大幅下降及導熱係數(κ)大幅提升，使得整體熱電優質係數(ZT)增加困難。 However, in order to achieve both excellent electrical conductivity (σ) and low thermal conductivity (κ), thermoelectric materials made of inorganic materials are no more suitable choices. In view of the fact that the inorganic thermoelectric material made of inorganic material has a good thermoelectric quality coefficient (ZT), the relative convenience of bending or bending is not limited, so that the installation position, convenience and use thereof are greatly limited. In order to solve this problem, organic thermoelectric materials made of organic materials are produced in response, but the existing organic thermoelectric materials still have a bottleneck that cannot be improved by the thermoelectric quality coefficient (ZT), which is due to the comparison of inorganic thermoelectric materials. Materials, organic thermoelectric materials cannot have a relatively good conductivity (σ) due to their materials; however, existing organic thermoelectric materials use a method of increasing the conductivity (σ) to improve the overall thermoelectric coefficient (ZT), but If so, it will be accompanied by a significant drop in the Seebeck coefficient (S) and a significant increase in the thermal conductivity (κ), making it difficult to increase the overall thermoelectric quality factor (ZT).
另外，傳統的無機熱電材料或有機熱電材料，為提高其導電係數(σ)，製造方法中常常需要用到昂貴的金屬元素，造成製程繁瑣，且其成本因金屬價格而提高，但又無法得到優良的熱電優質係數(ZT)。 In addition, in order to increase the conductivity (σ) of conventional inorganic thermoelectric materials or organic thermoelectric materials, expensive metal elements are often used in the manufacturing method, which causes cumbersome processes, and the cost thereof is increased due to the price of metal, but it is not available. Excellent thermoelectric quality factor (ZT).
因此，本發明提供了一種嶄新的可撓式熱電材料膜及其製造方法，不僅具有多領域的用途及優良的形變能力，更大幅提昇了相對於現今有機熱電材料無法提升的熱電優質係數(ZT)，此外，其製造方法相較於傳統，更具有簡單且成本低廉的優點。 Therefore, the present invention provides a novel flexible thermoelectric material film and a manufacturing method thereof, which not only have multi-field applications and excellent deformation ability, but also greatly improve the thermoelectric quality coefficient (ZT) which cannot be improved compared to the current organic thermoelectric materials. In addition, its manufacturing method is simpler and less expensive than conventional ones.
如先前技術所述，為同時解決以往無機熱電材料應用領域及安裝位置的限制及其無優良形變曲折能力，和現今有機熱電材料其熱電優質係數(ZT)無法有效提升的問題，本發明提供了一種可撓式熱電材料膜及其製造方法，包括：一有機高分子有機高分子基底膜，而該有機高分子基底膜具有至少一親水性(Hydrophilic)官能基；以及一多孔碳材料，混於該有機高分子基底膜中。其製造方法則包括：(a)將中孔洞碳材料與具有親水性(Hydrophilic)官能基之高分子有機溶液混和，得到其混合溶液；(b)將混合溶液經由超音波震盪直到中孔洞碳材料顆粒懸浮(Suspension)；(c)倒入培養皿中實施以一溫度成膜。 As described in the prior art, in order to simultaneously solve the limitation of the application field and installation position of the conventional inorganic thermoelectric material and its excellent deformation and tortuosity, and the problem that the thermoelectric quality coefficient (ZT) of the organic thermoelectric material cannot be effectively improved, the present invention provides A flexible thermoelectric material film and a manufacturing method thereof, comprising: an organic polymer organic polymer base film, wherein the organic polymer base film has at least one hydrophilic (Hydrophilic) functional group; and a porous carbon material, mixed In the organic polymer base film. The manufacturing method comprises the following steps: (a) mixing the medium pore carbon material with a polymer organic solution having a hydrophilic (Hydrophilic) functional group to obtain a mixed solution thereof; (b) oscillating the mixed solution via ultrasonic waves until the medium pore carbon material Suspension; (c) Pour into a Petri dish to form a film at a temperature.
該有機高分子基底膜為整個可撓式熱電材料的主體，係因絕大多數的有機高分子材料具有優良的柔軟性、可形變性、可成膜性及絕緣性，而其中，又以全氟磺化聚合物(Nafion)溶液所製成的有機高分子基底膜最佳，係因其內富含水通道結構(Water Channel)，其通道內面滿佈該至少一親水性(Hydrophilic)官能基，在全氟磺化聚合物(Nafion)薄膜中，此官能基為磺酸基(Sulfonyl hydroxide)，使該有機高分子基底膜具有極為強大的吸水能力，同時使之成為具有質子給體(Proton donor)能力的材料，此外，在其他有機高分子材質中，該至少一親水性(Hydrophilic)官能基可為醯胺基(Amide group)、胺基(Amino group)或其他具有作為質子給體(Proton donor)能力之官能基。 The organic polymer base film is the main body of the entire flexible thermoelectric material, because most of the organic polymer materials have excellent flexibility, deformability, film formability and insulation, and The organic polymer base film made of the fluorosulfonated polymer (Nafion) solution is optimal because it is rich in water channel structure, and the inner surface of the channel is filled with the at least one hydrophilic (Hydrophilic) function. In the perfluorosulfonated polymer (Nafion) film, the functional group is a Sulfonyl hydroxide, so that the organic polymer base film has an extremely strong water absorption capacity, and at the same time, it has a proton donor ( Proton donor material, in addition, in other organic polymer materials, the at least one hydrophilic (Hydrophilic) functional group may be an Amide group, an Amino group or the like as a proton donor. (Proton donor) The functional group of the ability.
基於以上特性，使得僅會出現在液體中的索雷特(Soret)效應得以轉移到固體的有機高分子材料上體現，相較於一般固體材料僅有西貝克(Seebeck)效應，本發明運用此原理產生的電壓較一般的固體材料能提高數千倍；此外，在該有機高分子基底膜中均勻混入的該多孔碳材料，具有高導電係數(σ)及低導熱係數(κ)的特性，可以使熱電轉換效率公式T中，σ/κ的比值上升，再加上伴隨著因索雷特(Soret)效應，使得其熱電優質係數(ZT)大幅的增加，而該多孔碳材料可為中孔碳材料、奈米碳管或活性碳，其中，又以中孔碳材料CMK-1、CMK-3、CMK-8和CMK-9中的CMK-3為最佳材料。以往的有機熱電材料其熱電優質係數(ZT)僅有0.25左右，本發明之熱電優質係數(ZT)可提高至0.847，近乎三倍於現有的有機熱電材料，可謂熱電轉換效率提升的一大突破。 Based on the above characteristics, the Soret effect which only occurs in the liquid is transferred to the solid organic polymer material, and the present invention uses the Seebeck effect as compared with the general solid material. The voltage generated by the principle can be increased by several thousand times compared with a general solid material; in addition, the porous carbon material uniformly mixed in the organic polymer base film has high conductivity (σ) and low thermal conductivity (κ). Thermoelectric conversion efficiency formula In T, the ratio of σ/κ increases, and with the Soret effect, the thermoelectric quality coefficient (ZT) is greatly increased, and the porous carbon material can be mesoporous carbon material, nano Carbon tube or activated carbon, wherein CMK-3 in mesoporous carbon materials CMK-1, CMK-3, CMK-8 and CMK-9 is the best material. In the past, the thermoelectric quality coefficient (ZT) of organic thermoelectric materials is only about 0.25, and the thermoelectric quality coefficient (ZT) of the present invention can be increased to 0.847, which is nearly three times that of the existing organic thermoelectric materials, which is a breakthrough in the improvement of thermoelectric conversion efficiency. .
若欲製造該可撓式熱電材料膜，首先，為使該多孔碳材料得 以均勻混和在其中，先將含有該至少一親水性(Hydrophilic)官能基之該有機高分子基底膜之原料，為有機高分子樹脂，以乙醇、丙醇或丙酮等常見有機溶劑調和成重量百分比濃度5~20%的溶液，再將該多孔碳材料混入之後，得到該多孔碳材料在其中佔重量百分比濃度5~30%的一混合溶液，但由於該混合溶液為非均勻混合溶液，因此，該多孔碳材料之顆粒在該混合溶液中分佈不均，會導致該可撓式熱電材料膜品質不佳，因此，需對該混合溶液施以超音波震盪(Sonicate)的方式，直到該多孔碳材料懸浮(Suspension)於該混合溶液；最後，將該均勻混合的該混合溶液倒入培養皿中，實施以攝氏溫度50~60度，直到其成膜，進而得到該可撓式熱電材料膜；此製造方法相較於傳統的製程簡單，且易於實施，更重要的是，此製程並不需要使用到任何昂貴的金屬元素，便可以得到擁有優良熱電優質係數(ZT)的熱電材料。 If the flexible thermoelectric material film is to be manufactured, first, in order to make the porous carbon material In order to uniformly mix therein, the raw material of the organic polymer base film containing the at least one hydrophilic (Hydrophilic) functional group is an organic polymer resin, and is blended into a weight percentage by a common organic solvent such as ethanol, propanol or acetone. a solution having a concentration of 5 to 20%, and then mixing the porous carbon material to obtain a mixed solution in which the porous carbon material accounts for 5 to 30% by weight, but since the mixed solution is a non-uniform mixed solution, The uneven distribution of the particles of the porous carbon material in the mixed solution may result in poor quality of the flexible thermoelectric material film. Therefore, the mixed solution is subjected to ultrasonic sonication until the porous carbon Suspension of the material in the mixed solution; finally, the uniformly mixed solution is poured into a petri dish, and is carried out at a temperature of 50 to 60 degrees Celsius until the film is formed, thereby obtaining the flexible thermoelectric material film; This manufacturing method is simpler than the conventional process, and is easy to implement. More importantly, this process does not require the use of any expensive metal elements. Excellent quality pyroelectric coefficient (ZT) of the thermoelectric material.
100‧‧‧可撓式熱電材料膜 100‧‧‧Flexible thermoelectric material film
101‧‧‧有機高分子基底膜 101‧‧‧Organic polymer base film
102‧‧‧多孔碳材料 102‧‧‧Porous carbon material
(a)‧‧‧將中孔洞碳材料與具有親水性(Hydrophilic)官能基之高分子有機溶液混和，得到其混合溶液 (a) ‧‧‧ Mixing the medium-hole carbon material with a polymer organic solution having a hydrophilic (Hydrophilic) functional group to obtain a mixed solution
(b)‧‧‧將混合溶液經由超音波震盪直到中孔洞碳材料顆粒懸浮(Suspension) (b) ‧ ‧ The mixed solution is oscillated via ultrasonic waves until the medium carbon hole particles are suspended (Suspension)
(c)‧‧‧倒入培養皿中實施以一溫度成膜 (c) ‧‧‧Pour into a petri dish to form a film at a temperature
圖1係本發明可撓式熱電材料膜之示意圖。 BRIEF DESCRIPTION OF THE DRAWINGS Figure 1 is a schematic illustration of a flexible thermoelectric material film of the present invention.
圖2係本發明多孔碳材料之示意圖。 Figure 2 is a schematic illustration of a porous carbon material of the present invention.
圖3係本發明製造方法之流程圖。 Figure 3 is a flow chart of the manufacturing method of the present invention.
請參閱圖1，圖1係本發明可撓式熱電材料膜之示意圖。如圖1所示，其中，可撓式熱電材料膜100以有機高分子基底膜101均勻包覆多孔碳材料102所組成，有機高分子基底膜101之材料為具有至少一親水性(Hydrophilic)官能基的有機高分子材料，本實施例為全氟磺化聚合物(Nafion)，有機高分子基底膜101內之水通道(Water channel)中富含有大量的 磺酸基(Sulfonyl hydroxide)，使其成為良好的質子給體(Proton donor)，令僅有在電解質溶液中才會出現的索雷特(Soret)效應得以體現在固體材料中，使其產生的電壓較以往的有機高分子熱電材料能提高數千倍。 Please refer to FIG. 1. FIG. 1 is a schematic view of a flexible thermoelectric material film of the present invention. As shown in FIG. 1 , the flexible thermoelectric material film 100 is composed of an organic polymer base film 101 uniformly coated with a porous carbon material 102. The material of the organic polymer base film 101 has at least one hydrophilic function. The organic polymer material of the base, in this embodiment is a perfluorosulfonated polymer (Nafion), and the water channel in the organic polymer base film 101 is rich in a large amount. Sulfonyl hydroxide makes it a good Proton donor, so that the Soret effect that only occurs in the electrolyte solution is reflected in the solid material. The voltage can be increased by several thousand times compared with the conventional organic polymer thermoelectric materials.
請參閱圖2，圖2係本發明多孔碳材料之示意圖。如圖2所示，多孔碳材料可為中孔碳材料、奈米碳管及活性碳或其混和物，而本實施例中的多孔碳材料102為中孔碳材料的CMK-3，具有極高的比表面積(1500m2/g)、比孔隙體積(1.3cm3/g)和均勻的孔隙度(2nm)，使可撓式熱電材料膜100其σ/κ的比值以及西貝克(Seebeck)係數(S)有極大幅度的提升；詳見表1，樣本Nf/PCx中，x代表CMK-3參雜在全氟磺化聚合物(Nafion)中的重量百分比濃度，在僅是添加了重量百分比3%的CMK-3後，其西貝克係數便從重量百分比為0%時的偵測不到，飆升至-34026μV/K，再者，添加重量百分比7%的CMK-3時，可在克氏溫度300度下得到可撓式熱電材料膜最高的熱電優質係數(ZT)0.847。 Please refer to FIG. 2, which is a schematic view of the porous carbon material of the present invention. As shown in FIG. 2, the porous carbon material may be a mesoporous carbon material, a carbon nanotube, and an activated carbon or a mixture thereof, and the porous carbon material 102 in this embodiment is a mesoporous carbon material of CMK-3 having a pole. High specific surface area (1500 m 2 /g), specific pore volume (1.3 cm 3 /g) and uniform porosity (2 nm), the ratio of σ/κ of the flexible thermoelectric material film 100 and Seebeck The coefficient (S) has a very large increase; see Table 1, in the sample Nf/PC x , x represents the weight percent concentration of CMK-3 doped in the perfluorosulfonated polymer (Nafion), only added After 3% by weight of CMK-3, the Westbeck coefficient is undetectable from 0% by weight, soaring to -34026μV/K, and further, when adding 7% by weight of CMK-3, The highest thermoelectric quality coefficient (ZT) of 0.847 is obtained for a flexible thermoelectric material film at a temperature of 300 °C.
請參閱圖3，圖3係本發明製造方法之流程圖。如圖3所示，首先，在步驟(a)中，將中孔碳材料CMK-3加入重量百分比濃度為20%的全氟磺化聚合物(Nafion)溶液中，調製成重量百分比濃度為7%的非均勻混合溶液，而全氟磺化聚合物(Nafion)溶液係以全氟磺化聚合物(Nafion)樹脂為溶質，丙醇為溶劑所調製而成之溶液，此時，該中孔碳材料CMK-3因無法溶解於全氟磺化聚合物(Nafion)溶液中，會在混合溶液中不均勻分佈，因此，以步驟(b)，對混合溶液以超音波震盪(Sonicate)的方式處理，利用液體震動傳導使其中不均勻分佈的CMK-3顆粒得以均勻懸浮(Suspension)在混和溶液中，最後以步驟(c)，將超音波震盪(Sonicate)處理後的混合溶液倒入培養皿 中，置於攝氏50度的環境下直至成膜。 Please refer to FIG. 3. FIG. 3 is a flow chart of the manufacturing method of the present invention. As shown in FIG. 3, first, in the step (a), the mesoporous carbon material CMK-3 is added to a 20% by weight solution of a perfluorosulfonated polymer (Nafion) to prepare a concentration of 7 by weight. % non-uniform mixed solution, and the perfluorosulfonated polymer (Nafion) solution is a solution prepared by using a perfluorosulfonated polymer (Nafion) resin as a solute and a propanol as a solvent. The carbon material CMK-3 cannot be dissolved in the perfluorosulfonated polymer (Nafion) solution and will be unevenly distributed in the mixed solution. Therefore, in step (b), the mixed solution is ultrasonically oscillated (Sonicate). Processing, using liquid vibration conduction, uniformly dispersing CMK-3 particles therein in a mixed solution, and finally, in step (c), pouring the ultrasonic solution (Sonicate) mixed solution into the culture dish. Medium, placed in an environment of 50 degrees Celsius until film formation.
100‧‧‧可撓式熱電材料膜 100‧‧‧Flexible thermoelectric material film
101‧‧‧有機高分子基底膜 101‧‧‧Organic polymer base film
102‧‧‧多孔碳材料 102‧‧‧Porous carbon material
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