聚（3,4-乙烯二氧噻吩）納米結(jié)構(gòu)及碳納米粒子熱電材料的制備及其性能研究
發(fā)布時(shí)間：2018-08-14 15:16
【摘要】：隨著能源短缺和資源利用率低等問(wèn)題的日益突出,作為可以實(shí)現(xiàn)熱能和電能直接相互轉(zhuǎn)化的熱電材料受到了廣泛的關(guān)注。有機(jī)導(dǎo)電聚合物以及高性能的碳納米粒子已經(jīng)成為熱電材料研究的重點(diǎn)對(duì)象。本論文主要研究了后處理對(duì)納米結(jié)構(gòu)導(dǎo)電聚合物熱電性能的影響以及利用碳納米粒子為原料制備高性能的熱電材料。主要內(nèi)容包括以下幾點(diǎn):1.以3,4-乙烯二氧噻吩(EDOT)為原料,利用水相表面活性劑法和反相膠束法制備了聚(3,4-乙烯二氧噻吩)(PEDOT)納米棒,并研究其熱電性能;然后利用不同濃度的硫酸對(duì)反相膠束法制備出的PEDOT納米棒進(jìn)行浸泡處理,接著用一定質(zhì)量分?jǐn)?shù)的亞硫酸鈉溶液對(duì)硫酸浸泡處理過(guò)的PEDOT納米棒進(jìn)行不同時(shí)間的化學(xué)還原。研究發(fā)現(xiàn):后處理有效地調(diào)節(jié)了PEDOT納米棒的氧化水平和摻雜水平,并且改善了分子鏈的規(guī)整度和極化狀態(tài),從而實(shí)現(xiàn)了PEDOT納米棒熱電性能的顯著提升。2.以氧化石墨烯和酸化單壁碳納米管為原料,通過(guò)化學(xué)還原的方法制備雜化氣凝膠材料,并測(cè)試不同原料配比下氣凝膠材料的孔隙率和各項(xiàng)熱電參數(shù)。研究發(fā)現(xiàn):氣凝膠的特殊網(wǎng)絡(luò)結(jié)構(gòu)為電子的傳輸提供了多重路徑,從而提高了電導(dǎo)率;豐富的界面使氣凝膠展現(xiàn)了更好的能量過(guò)濾效應(yīng),從而提高了Seebeck系數(shù);超高的孔隙率有效地抑制了聲子的傳輸,使得氣凝膠材料具有極低的熱導(dǎo)率;綜上使得氣凝膠熱電材料具有較高的熱電優(yōu)值。另外,氣凝膠對(duì)不同的有機(jī)溶劑具有較高的吸收效率,且對(duì)低沸點(diǎn)有機(jī)溶劑表現(xiàn)出較好的循環(huán)使用性,多次循環(huán)使用后吸收效率沒(méi)有出現(xiàn)明顯降低。3.通過(guò)對(duì)單壁碳納米管進(jìn)行酸化處理,在其表面引入羧酸基團(tuán);然后利用水合肼作為還原劑,以硫代鉬酸銨作為MoS2納米粒子的前驅(qū)體,經(jīng)過(guò)有效的還原得到了性能穩(wěn)定的MoS2/a-SWCNT N-型熱電材料。由于有效地對(duì)單壁碳納米管的表面修飾和摻雜,使單壁碳納米管的導(dǎo)電類型由空穴導(dǎo)電變?yōu)殡娮訉?dǎo)電,即由P型半導(dǎo)體轉(zhuǎn)變?yōu)镹型半導(dǎo)體。同時(shí),MoS2/a-SWCNT N-型熱電材料具有較高的性能穩(wěn)定性,且在空氣中,材料的熱電性能幾乎不會(huì)隨時(shí)間的延長(zhǎng)而出現(xiàn)衰減。
[Abstract]:With the shortage of energy and the low utilization of resources, the thermoelectric materials, which can realize the direct conversion of heat energy and electricity energy, have been paid more and more attention. Organic conductive polymers and high-performance carbon nanoparticles have become the focus of thermoelectric materials. In this paper, the effect of post-treatment on the thermoelectric properties of nanostructured conductive polymers and the preparation of high performance thermoelectric materials using carbon nanoparticles as raw materials were studied. The main content includes the following points: 1. ) (PEDOT) nanorods were prepared by using aqueous surfactant method and reverse micellar method from 3O4-ethylenedioxythiophene (EDOT). The thermoelectric properties of the nanorods were studied. Then the PEDOT nanorods prepared by reverse micellar method were soaked with different concentrations of sulfuric acid, and then the PEDOT nanorods soaked in sulfuric acid were chemically reduced for different time with sodium sulfite solution of a certain mass fraction. It is found that the oxidation level and doping level of PEDOT nanorods are adjusted effectively by the post-treatment, and the molecular chain regularity and polarization state are improved, so that the thermoelectric properties of PEDOT nanorods can be improved significantly. 2. Hybrid aerogel materials were prepared by chemical reduction from graphene oxide and acidified single-walled carbon nanotubes. The porosity and thermoelectric parameters of aerogel materials with different ratios were measured. It is found that the special network structure of aerogels provides multiple paths for electron transmission, which improves the conductivity of aerogels, and the rich interface makes aerogels exhibit better energy filtering effect, thus increasing the Seebeck coefficient. The high porosity effectively inhibits the phonon transport and makes the aerogel material have a very low thermal conductivity. In summary, the aerogel thermoelectric material has a higher thermoelectric value. In addition, aerogels have higher absorption efficiency for different organic solvents, and better recycling performance for low boiling point organic solvents. The absorption efficiency of aerogels does not decrease significantly after repeated recycling. Carboxylic groups were introduced on the surface of single-walled carbon nanotubes by acidification, and then hydrazine hydrate was used as reducing agent and ammonium thiomolybdate as precursor of MoS2 nanoparticles. A stable MoS2/a-SWCNT N-type thermoelectric material was obtained by effective reduction. Due to the effective surface modification and doping of single walled carbon nanotubes, the conduction type of single walled carbon nanotubes is changed from hole conduction to electron conduction, that is, from P type semiconductor to N type semiconductor. At the same time, MoS _ 2 / a-SWCNT N- type thermoelectric materials have high performance stability, and in air, the thermoelectric properties of the materials almost do not decay with the prolongation of time.
【學(xué)位授予單位】：青島科技大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2017
【分類號(hào)】：TB383.1;TB34
本文編號(hào)：2183270
[Abstract]:With the shortage of energy and the low utilization of resources, the thermoelectric materials, which can realize the direct conversion of heat energy and electricity energy, have been paid more and more attention. Organic conductive polymers and high-performance carbon nanoparticles have become the focus of thermoelectric materials. In this paper, the effect of post-treatment on the thermoelectric properties of nanostructured conductive polymers and the preparation of high performance thermoelectric materials using carbon nanoparticles as raw materials were studied. The main content includes the following points: 1. ) (PEDOT) nanorods were prepared by using aqueous surfactant method and reverse micellar method from 3O4-ethylenedioxythiophene (EDOT). The thermoelectric properties of the nanorods were studied. Then the PEDOT nanorods prepared by reverse micellar method were soaked with different concentrations of sulfuric acid, and then the PEDOT nanorods soaked in sulfuric acid were chemically reduced for different time with sodium sulfite solution of a certain mass fraction. It is found that the oxidation level and doping level of PEDOT nanorods are adjusted effectively by the post-treatment, and the molecular chain regularity and polarization state are improved, so that the thermoelectric properties of PEDOT nanorods can be improved significantly. 2. Hybrid aerogel materials were prepared by chemical reduction from graphene oxide and acidified single-walled carbon nanotubes. The porosity and thermoelectric parameters of aerogel materials with different ratios were measured. It is found that the special network structure of aerogels provides multiple paths for electron transmission, which improves the conductivity of aerogels, and the rich interface makes aerogels exhibit better energy filtering effect, thus increasing the Seebeck coefficient. The high porosity effectively inhibits the phonon transport and makes the aerogel material have a very low thermal conductivity. In summary, the aerogel thermoelectric material has a higher thermoelectric value. In addition, aerogels have higher absorption efficiency for different organic solvents, and better recycling performance for low boiling point organic solvents. The absorption efficiency of aerogels does not decrease significantly after repeated recycling. Carboxylic groups were introduced on the surface of single-walled carbon nanotubes by acidification, and then hydrazine hydrate was used as reducing agent and ammonium thiomolybdate as precursor of MoS2 nanoparticles. A stable MoS2/a-SWCNT N-type thermoelectric material was obtained by effective reduction. Due to the effective surface modification and doping of single walled carbon nanotubes, the conduction type of single walled carbon nanotubes is changed from hole conduction to electron conduction, that is, from P type semiconductor to N type semiconductor. At the same time, MoS _ 2 / a-SWCNT N- type thermoelectric materials have high performance stability, and in air, the thermoelectric properties of the materials almost do not decay with the prolongation of time.
【學(xué)位授予單位】：青島科技大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2017
【分類號(hào)】：TB383.1;TB34
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