【摘要】：染料敏化太陽能電池(Dye-sensitized solar cell, DSSC)由于具有不錯(cuò)的能量轉(zhuǎn)化效率、制造成本低、環(huán)境友好等優(yōu)點(diǎn)，成為非常有吸引力的新一代太陽能電池。對(duì)電極是DSSC非常重要的組件之一，Pt是目前為止最常用的對(duì)電極材料。然而，Pt是貴金屬，且資源有限，使用Pt對(duì)電極大大增加了DSSC的成本。因此，開發(fā)不含Pt且具有較高效率的對(duì)電極材料代替?zhèn)鹘y(tǒng)Pt電極具有重要意義。由于CoS具有優(yōu)異的電催化性能、原材料豐富且成本低，，石墨烯具有卓越的導(dǎo)電性、快速的電荷遷移率、高的比表面積及良好的化學(xué)和熱穩(wěn)定性，在本文中，我們制備了硫化鈷-石墨烯復(fù)合對(duì)電極，并從以下幾個(gè)方面進(jìn)行了研究： (1)通過水熱法制備CoS粉體，與石墨烯混合，加入有機(jī)粘結(jié)劑CMC-Na形成均勻的漿料，采用刮刀法將漿料印刷到FTO玻璃基底上，通過控制漿料中CoS和石墨烯的比例，制備出不同配比的CoS-石墨烯復(fù)合對(duì)電極； (2)使用XRD、FSEM和EDS表征復(fù)合對(duì)電極的結(jié)構(gòu)和形貌，結(jié)果表明，水熱法制備的CoS粉體為六角結(jié)構(gòu)，尺寸約為500nm，大顆粒是由幾十納米的小顆粒聚集而成的。制備的復(fù)合對(duì)電極，CoS顆粒均勻的分布在對(duì)電極薄膜中，石墨烯為片層卷曲結(jié)構(gòu)，不同配比復(fù)合對(duì)電極薄膜的厚度都控制在13~15μm，且各元素在其中的分布較為均勻； (3)采用CV法測(cè)量復(fù)合對(duì)電極的電催化活性及長(zhǎng)期穩(wěn)定性，結(jié)果表明，CoS具有優(yōu)異的電催化活性，而石墨烯的電催化性能較差。當(dāng)在石墨烯中加入CoS后，復(fù)合對(duì)電極的電催化活性顯著提高，CoS-石墨烯復(fù)合對(duì)電極的電催化活性比Pt對(duì)電極高，長(zhǎng)期穩(wěn)定性與Pt一樣好； (4)采用I-V曲線和EIS表征DSSC的光電性能，結(jié)果表明，CoS和石墨烯具有很好的協(xié)同效應(yīng)，復(fù)合后，電荷轉(zhuǎn)移阻抗和Nernst擴(kuò)散阻抗均減小，硫化鈷-石墨烯復(fù)合對(duì)電極DSSC的能量轉(zhuǎn)化效率比硫化鈷和石墨烯單獨(dú)作為對(duì)電極時(shí)DSSC的能量轉(zhuǎn)化效率高； (5)研究CoS和石墨烯的最佳配比，隨著CoS比例的增加，短路電流和填充因子均呈現(xiàn)先增大后減小的趨勢(shì)。當(dāng)復(fù)合對(duì)電極中，CoS的質(zhì)量比為40%，石墨烯的質(zhì)量比為60%時(shí)，具有最佳的能量轉(zhuǎn)化效率，為6.31%，高于以CoS和石墨烯單獨(dú)作為DSSC對(duì)電極時(shí)的效率，分別為3.51%和4.26%，甚至高于以傳統(tǒng)Pt作為DSSC對(duì)電極的效率，為5.98%。
[Abstract]:Dye-sensitized solar cells (Dye-sensitized solar cell, DSSC) have become an attractive new generation of solar cells due to their good energy conversion efficiency, low manufacturing cost and environmental friendliness. Counter electrode is one of the most important components of DSSC. Pt is the most commonly used counter electrode material so far. However, Pt is a precious metal with limited resources. The use of Pt pair electrodes greatly increases the cost of DSSC. Therefore, it is of great significance to develop Pt free and efficient electrode materials instead of traditional Pt electrodes. Because of its excellent electrocatalytic properties, abundant raw materials and low cost, graphene has excellent electrical conductivity, fast charge mobility, high specific surface area and good chemical and thermal stability. Cobalt-graphene sulphide composite electrode was prepared and studied in the following aspects: (1) CoS powder was prepared by hydrothermal method, mixed with graphene, and organic binder CMC-Na was added to form uniform slurry. The slurry was printed on the FTO glass substrate by scraper method. By controlling the ratio of CoS and graphene in the slurry, the CoS- graphene composite counter electrode with different ratio was prepared. (2) XRD,FSEM and EDS were used to characterize the structure and morphology of the composite opposite electrode. The results showed that the CoS powder prepared by hydrothermal method was hexagonal structure with a size of about 500 nm, and the large particles were composed of dozens of nanometers and small particles. The CoS particles are uniformly distributed in the counter electrode film, and graphene is the crimp structure of the lamellar layer. The thickness of the composite counter electrode film is controlled at 1315 渭 m, and the distribution of the elements in the film is more uniform. (3) the electrocatalytic activity and long-term stability of composite electrode were measured by CV method. The results showed that CoS had excellent electrocatalytic activity, but graphene had poor electrocatalytic activity. When CoS was added into graphene, the electrocatalytic activity of the composite electrode increased significantly. The electrocatalytic activity of the CoS- graphene composite electrode was higher than that of the Pt electrode, and the long-term stability of the composite electrode was as good as that of Pt. (4) the photoelectric properties of DSSC were characterized by I-V curve and EIS. The results show that CoS and graphene have good synergistic effect, and the charge transfer impedance and Nernst diffusion impedance decrease after recombination. The energy conversion efficiency of cobalt sulphide / graphene composite to DSSC is higher than that of DSSC when cobalt sulphide and graphene are used as counter electrodes alone. (5) the optimum ratio of CoS and graphene is studied. With the increase of CoS ratio, the short-circuit current and filling factor increase first and then decrease. When the mass ratio of CoS and graphene is 40 and 60, the optimum energy conversion efficiency is 6.31, which is higher than that when CoS and graphene are used as DSSC pair electrodes alone. It was 3.51% and 4.26% respectively, which was even higher than that of traditional Pt as DSSC electrode, 5.98%.
【學(xué)位授予單位】：華中科技大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2014
【分類號(hào)】：TM914.4

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