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    National Tsing Hua University Institutional Repository > 工學院  > 化學工程學系 > 博碩士論文  >  高效率大面積串聯式高分子太陽能電池與鈣鈦礦太陽能電池之研究


    Please use this identifier to cite or link to this item: http://nthur.lib.nthu.edu.tw/dspace/handle/987654321/86984


    Title: 高效率大面積串聯式高分子太陽能電池與鈣鈦礦太陽能電池之研究
    Authors: 葉柏男
    Yeh, Po Nan
    Description: GH029632528
    博士
    化學工程學系
    Date: 2015
    Keywords: 高分子太陽能電池 鈣鈦礦太陽能電池 串聯式高分子太陽能電池
    polymer solar cell perovskite solar cell tandem polymer solar cell
    Abstract: 本論文以提高高分子及鈣鈦礦太陽能電池效率為主旨,主要可分成三部份。前兩部份為反式串聯式高分子太陽能電池中間層PEDOT:PSS成膜性的研究,並有效改善大面積元件的效率。第三部份為利用溶劑退火方式來製作高效率鈣鈦礦太陽能電池,並從中了解含浸法中不同CH3NH3I (MAI)濃渡下,鈣鈦礦的成長機制。
    在第五章中,我們提出蒸鍍超薄金屬層(Au and Ag)在活性層P3HT:ICBA與PEDOT:PSS之間,改善PEDOT在疏水性活性層上的成膜性。其中超薄金屬層Ag能使元件的效率增加,但Au會使元件效率下降,因為Au會使活性層的ionized potential 從4.54 eV減小到4.14 eV,導致電洞會累積在活性層與PEDOT:PSS的界面上,不利電洞傳遞。我們製作反式串聯式高分子太陽能電池,活性層由P3HT:ICBA和PTB7:PC71BM所組成,中間層為PEDOT:PSS/ZnO nanoparticle。在小面積的元件上,當加入了超薄金屬層Ag,效率可從7.06 %提升到7.81 %,而超薄金屬層Au的元件,其效率下降到 6.4 %;在當元件面積增加1 cm2時,加入了Ag的中間層其效率為6.11 %,相較於以PEDOT/ZnO np當中間層的元件(2.12 %),元件效率提升了2.78倍。
    在第六章中,我們利用醇類來處理活性層(P3HT:ICBA)的表面,使表面親水性增加,讓PEDOT:PSS在活性層上的成膜性得到改善。在元件面積為0.02 cm2下,用 1-hexanol處理過的反式串聯式高分子太陽能電池,其效率可以從7.06 %提升到8.10 %。在大面積1 cm2時,P3HT:ICBA表面經過1-hexanol處理過的元件效率仍維持7.00 %,遠高於沒有處理的元件2.18 %。此外,相較於先前引進超薄金屬層Ag的方法,醇類處理的方法更為簡單且能降低製作成本及縮短製程時間。
    在第七章中,我們提出溶劑退火的方式來改變PbI2薄膜的形態並製作成鈣鈦礦元件,我們發現利用溶劑退火的方式會增加PbI2的結晶,使薄膜產生較大較深的孔洞。在濃度為10 mg/mL的MAI中進行含浸時,因為MAI會快速和表面的PbI2反應形成CH3NH3PbI3,阻礙了MAI擴散至PbI2的內部;PbI2薄膜沒有溶劑退火的處理時,其元件效率只有1.08 %,當元件經過5分鐘以上的溶劑退火處理後,元件效率最高效率可達16.07 %,這結果說明了PbI2表面的孔洞大小和深度是影響元件效率的主要因素。當PbI2薄膜含浸在低濃度MAI(6 mg/mL)時,PbI2薄膜表面並不會快速生成CH3NH3PbI3,使得MAI有時間能擴散到PbI2薄膜的內部;因此,沒有溶劑退火的元件其效率為13.37 %,與溶劑退火的元件其效率為14.3 %,兩者差異不大,這說明了PbI2薄膜表面的孔洞大小就不在是影響元件效率的主要因素。
    The object of this thesis is to enhancement of the device performances of tandem polymer and perovskite solar cells, and the contents are divided into three topics. In the first two sections, we study on the film formation quality of aqueous hole-transport interlayer on hydrophobic active layer in the inverted tandem polymer solar cells, leading to significantly elevated performance for the large area devices. In the last section, we obtain high performance of perovskite solar cell by solvent annealing of the PbI2 film, and realize the growth mechanism of perovskite with dipping in various concentrations of CH3NH3I (MAI).
    In chapter 5, we propose the deposition of ultra-thin silver or gold layer (in subnano-scale) between bottom subcell and the hole-transport sublayer in the interlayer (IL), poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS), in the inverted tandem polymer solar cell (t-PSC) for improving the wettability of aqueous hole-transport interlayer on hydrophobic active layer. The ultra-thin sliver layer can improve device performance, but the ultra-thin gold layer induces a significant decrease of ionized potential from 4.54 eV to 4.14 eV leading to an accumulation of holes at (regioregular poly(3-hexylthiophene) (P3HT) side in the interface of P3HT/PEDOT:PSS, which decreases the device performance. In the inverted t-PSCs (small-area, 0.02 cm2) composed of the bottom subcell P3HT: indene-C60-bisadduct (ICBA)), the top subcell (thieno[3,4-b]thiophene/benzodithiophene (PTB7) with [6,6]-phenyl C71-butyric acid methyl ester (PC71BM)) and the IL, PEDOT:PSS/ZnO nanoparticles, the power conversion efficiency (PCE) is improved from 7.06 % (without any ultra-thin metal layer) to 7.81 % with 0.5 nm Ag layer but decreases to 6.4 % with 1nm Au layer. As enlarging the active area to 1 cm2, the PCE of 0.5 nm Ag device is still over 6 % (6.11 %) much higher than that without Ag layer (2.19 %) by a factor of 2.78.
    In chapter 6, we treat the active layer (P3HT:ICBA) surface by alcohols for hydrophiles leading to high-quality film of the next spin-coated PEDOT:PSS layer. For the small-area (0.02 cm2) inverted t-PSC, the PCE can be enhanced from 7.06 % to 8.10 % by 1-hexanol treatment. As enlarging the active area to about 1 cm2, the device with 1-hexanol treatment still performs 7.00 % high PCE, which is much better than that without any treatment (2.19 %). In addition, the main advancement of this work is the use of low cost material (1-hexanol) and low cost fabrication process (spin coating) as compared to depositing 0.5 nm Ag layer on active layer, in which the high cost material (silver) and high cost deposition process (vacuum thermal deposition) are used.
    In chapter 7, we demonstrate that treatment of the PbI2 films with solvent annealing can change the surface morphology with large and deeper porous due to increasing PbI2 crystallinity. For PbI2 film dipped into 10 mg/mL CH3NH3I (MAI) solution, crystals of CH3NH3PbI3 are quickly formed on the surface of PbI2 and inhibit MAI to further penetrate into the PbI2 film. Therefore, PbI2 film with large and deep porous surface can form more crystals of CH3NHPbI3. The PCE of the device with solvent annealing treatment for over 5 min is enhanced from 1.08 % to 16.07 %. For PbI2 film dipped into low concentration 6 mg/mL CH3NH3I (MAI) solution, crystals of CH3NH3PbI3 form slowly on PbI2 surface, which provide the MAI enough time going through surface to inside PbI2 film. Thus, the PCE of solvent annealed treatment device (14.3 %) is similar to that without treatment (13.37 %), demonstrating that the factor of the PbI2 morphology can be minimized.
    URI: http://nthur.lib.nthu.edu.tw/dspace/handle/987654321/86984
    Source: http://thesis.nthu.edu.tw/cgi-bin/gs/hugsweb.cgi?o=dnthucdr&i=sGH029632528.id
    Appears in Collections:[化學工程學系] 博碩士論文

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