發(fā)布時(shí)間：2018-06-01 09:19

  本文選題：熱電材料 + 共軛聚合物�。� 參考：《深圳大學(xué)》2017年碩士論文

【摘要】：熱電材料又稱溫差材料,由于熱電材料可實(shí)現(xiàn)熱能與電能直接轉(zhuǎn)換,作為一種新型可持續(xù)發(fā)展的清潔能源材料而逐漸受到人們的關(guān)注。盡管無機(jī)熱電材料經(jīng)過了多年的發(fā)展,相關(guān)研究已經(jīng)相對(duì)成熟,但是近年來,由于有機(jī)熱電材料具有無毒、易制備、柔性、高的塞貝克系數(shù)及低熱導(dǎo)率等優(yōu)點(diǎn),逐漸受到學(xué)者們的青睞。本文主要針對(duì)具有D-A結(jié)構(gòu)的高分子熱電材料展開研究,以強(qiáng)受體噻唑?yàn)榛A(chǔ)單元,通過引入芴、噻吩及咔唑單元作為給體,系統(tǒng)探究噻唑類聚合物結(jié)構(gòu)(烷基側(cè)鏈和分子骨架)與熱電性能之間的關(guān)系。選取其中具有高塞貝克系數(shù)的F8BT與單壁碳納米管(SWCNT)進(jìn)行復(fù)合,以期進(jìn)一步提高復(fù)合材料的熱電性能。通過對(duì)D-A型噻唑類聚合物熱電性能的系統(tǒng)研究,我們發(fā)現(xiàn)可以通過調(diào)整烷基側(cè)鏈長度、減小帶隙、引入導(dǎo)電性好的給體及和導(dǎo)電性較好的SWCNT進(jìn)行復(fù)合來提高熱電性能。其具體內(nèi)容如下:1.合成具有D-A結(jié)構(gòu)的芴-噻唑類聚合物(F6BT,F8BT及F12BT),在不改變帶隙前提下,探究烷基側(cè)鏈對(duì)熱電性能的影響。結(jié)果表明烷基側(cè)鏈越短,分子堆積越明顯,越有助于電子傳輸。因此F6BT擁有較好的熱電性能,其電導(dǎo)率最高可達(dá)1.52 S/cm(22°C),功率因子為1.65μW m~(-1) K~(-2)。變溫條件下,伴隨溫度的逐漸升高,分子間運(yùn)動(dòng)加劇,進(jìn)而分子有序排列降低,分子間π-π堆積效應(yīng)逐漸減弱,致使載流子遷移率減小,電導(dǎo)率下降,相反其賽貝克系數(shù)升高。2.在第1部分基礎(chǔ)之上,選取容易制備且原料便宜的F8BT為引入噻吩單元,使聚合物帶隙變窄,探究帶隙變化對(duì)噻唑類聚合物熱電性能影響。發(fā)現(xiàn)帶隙變窄,電導(dǎo)率升高,塞貝克系數(shù)降低,但仍具有較高賽貝克系數(shù),約為45μV/K。在不改變帶隙的條件下,將給體換成導(dǎo)電性較好的咔唑單元,探究給體對(duì)熱電性能的影響,發(fā)現(xiàn)咔唑單元的引入可以進(jìn)一步提高材料的導(dǎo)電性,并且在90°C條件下,C8TBT的塞貝克系數(shù)可達(dá)335μV/K,功率因子可以達(dá)到13μW m~(-1) K~(-2)。3.在第2部分的基礎(chǔ)之上,選取具有高塞貝克系數(shù)且容易制備的F8BT與導(dǎo)電性較好的SWCNT進(jìn)行復(fù)合制備復(fù)合熱電材料。發(fā)現(xiàn)加入SWCNT之后,復(fù)合材料電導(dǎo)率顯著提高。伴隨SWCNT質(zhì)量分?jǐn)?shù)的增加,電導(dǎo)率呈先增加后降低的趨勢,然而SWCNT的含量對(duì)復(fù)合材料的塞貝克系數(shù)影響較小。當(dāng)SWCNT質(zhì)量分?jǐn)?shù)為50%時(shí),F8BT-Fe Cl3/SWCNT復(fù)合材料電導(dǎo)率可達(dá)1625 S/cm,功率因子為33.4μW m~(-1) K~(-2)。該研究表明,通過將F8BT與SWCNT復(fù)合,可以兼具SWCNT高的導(dǎo)電性與F8BT高的賽貝克系數(shù),獲得更優(yōu)良的熱電性能。
[Abstract]:Thermoelectric materials, also called thermoelectric materials, have been paid more and more attention as a new kind of clean energy materials for sustainable development, because thermoelectric materials can realize the direct conversion of thermal energy and electric energy. Although inorganic thermoelectric materials have been developed for many years, the related research has been relatively mature, but in recent years, due to the advantages of non-toxic, easy to prepare, flexible, high Seebeck coefficient and low thermal conductivity, organic thermoelectric materials have many advantages, such as non-toxic, easy preparation, high Seebeck coefficient and low thermal conductivity. Gradually attracted the favor of scholars. In this paper, the high molecular thermoelectric materials with D-A structure were studied. Based on the strong receptor thiazole, fluorene, thiophene and carbazole units were introduced as donors. The relationship between the structure of thiazole polymers (alkyl side chain and molecular skeleton) and thermoelectric properties was systematically investigated. In order to further improve the thermoelectric properties of the composites, F8BT with high Seebeck coefficient and SWCNT with single wall carbon nanotubes were selected. Through the systematic study of the thermoelectric properties of D-A thiazole polymers, we find that the thermoelectric properties can be improved by adjusting the length of alkyl side chain, reducing the band gap, introducing a donor with good conductivity and compounding with SWCNT with good conductivity. The details are as follows: 1. Fluorene thiazole polymers (F _ 6BTN, F _ 8BT and F _ 12BTN) with D-A structure were synthesized. The influence of alkyl side chain on thermoelectric properties was investigated without changing the band gap. The results show that the shorter the alkyl side chain, the more obvious the molecular stacking is, and the more favorable the electron transport is. Therefore, F6BT has good thermoelectric properties, its conductivity is up to 1.52 S/cm(22 擄C ~ (-1), and its power factor is 1.65 渭 W / m ~ (-1) K ~ (2 +). Under the condition of changing temperature, the intermolecular motion intensifies with the increase of temperature, and then the ordered arrangement of molecules decreases, and the 蟺-蟺 stacking effect weakens gradually, which results in the decrease of carrier mobility and the decrease of conductivity. On the contrary, the Seebeck coefficient increases by .2. On the basis of the first part, F8BT, which is easy to be prepared and cheap as raw material, is selected as the thiophene unit to narrow the band gap of the polymer. The influence of the band gap on the thermoelectric properties of thiazole polymers is investigated. It is found that the band gap becomes narrower, the conductivity increases, and the Seebeck coefficient decreases, but still has a higher Seebeck coefficient, which is about 45 渭 V / K / L. Under the condition that the band gap is not changed, the donor is replaced by carbazole unit with good electrical conductivity, and the effect of donor on thermoelectric property is explored. It is found that the introduction of carbazole unit can further improve the conductivity of the material. At 90 擄C, the Seebeck coefficient of C8TBT can reach 335 渭 V / K, and the power factor can reach 13 渭 W / m ~ (-1). On the basis of the second part, the composite thermoelectric materials were prepared by using F8BT with high Seebeck coefficient and SWCNT with good conductivity. It was found that the conductivity of the composites increased significantly after the addition of SWCNT. With the increase of mass fraction of SWCNT, the conductivity increased first and then decreased. However, the content of SWCNT had little effect on Seebeck coefficient of composites. When the mass fraction of SWCNT is 50, the conductivity of F8BT-Fe Cl3/SWCNT composites can reach 1625 S / cm, and the power factor is 33.4 渭 W / m ~ (-1) K ~ (2 +). The results show that by combining F8BT with SWCNT, the better thermoelectric properties can be obtained by combining the high conductivity of SWCNT with the high Seebeck coefficient of F8BT.
【學(xué)位授予單位】：深圳大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2017
【分類號(hào)】：TB34

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