合成用於反式錫鈣鈦礦太陽能電池之兩性介面修飾材料之D-A type共軛高分子

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陳玟諭(Wun-Yu Chen) 查詢紙本館藏

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合成用於反式錫鈣鈦礦太陽能電池之兩性介面修飾材料之D-A type共軛高分子
(Synthesis of D-A type conjugated polymers used as amphiphilic interfacial modification materials for inverted perovskite solar cells)

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至系統瀏覽論文 (2026-8-23以後開放)

摘要(中)

錫鈣鈦礦太陽能電池(Tin Perovskite solar cells，簡稱TPSCs)中錫鈣鈦礦吸收層因具理想的能隙(∼1.4 eV)和較低的毒性而有巨大的前景，TPSCs之最高光電轉換效率(Power conversion efficiency, PCE)已達15%以上。但錫鈣鈦礦因Sn2+容易氧化及快速結晶，導致穩定性差及薄膜品質不佳，另外還有載子傳遞層與錫鈣鈦礦層的介面相容性不好等問題。許多學者透過在錫鈣鈦礦前驅液中加入添加劑抑制Sn2+的氧化，而對介面相容性的問題則較少研究。本研究以已發表的PDTON結構為基礎，以具有電洞傳輸能力的isopropyl-triphenylamine (i-pr-TPA)做為Acceptor，並將原先以TPA結構搭配一條親水鏈之Donor改為同樣具電洞傳輸能力的cyclopentadithiophene (CPDT)搭配兩條親水的烷基胺側鏈，合成出兩性高分子PTSN。PTSN的好處有三: 一為CPDT結構中具有電洞萃取能力之噻吩，能有效地將電洞從錫鈣鈦礦層中萃取出來。二為CPDT相較於TPA，結構中可再增加一條親水烷基胺鏈，以更好的修飾電洞傳遞層(HTL) Cu-SnCo2O4 (Cu-SCO)的表面及HOMO能階，來更加匹配錫鈣鈦礦的價帶，且路易斯鹼烷胺基可鈍化錫鈣鈦礦表面的缺陷。三為結構中同時具親、疏水基團，可增加與錫鈣鈦礦前驅液的相容性。兩個高分子(PTSN與PDTON)的熱裂解溫度皆大於200℃。UV-Vis吸收光譜顯示在相同濃度下，PTSN溶液及膜的光吸收度皆較PDTON小，可使更多光子到達錫鈣鈦礦吸光層。在Donor結構中含兩條親水鏈之高分子PTSN膜的錫鈣鈦礦前驅液接觸角較在PDTON膜上小，顯示與親水性之錫鈣鈦礦前驅液的相容性大。Cu-SCO/PTSN膜的價帶(-5.53 eV)比Cu-SCO/PDTON膜的價帶(-5.49 eV)更接近錫鈣鈦礦的價帶(-5.74 eV)，電洞在傳遞時的能量損失較少。FTIR光譜顯示PTSN+SnI2及PTSN+Cu-SCO的amine C-N stretching與thiophene C-S stretching皆比純PTSN的波數藍位移，代表胺基上氮的孤對電子與噻吩上硫的孤對電子，都能與Cu-SCO膜及錫鈣鈦礦配位未飽和之Sn2+作用。PL及TRPL數據顯示錫鈣鈦礦沉積在經PTSN修飾的Cu-SCO上的螢光強度比沉積在Cu-SCO/PDTON或Cu-SCO HTLs上弱且載子生命週期也較短，表示Cu-SCO/PTSN HTL能最有效的將錫鈣鈦礦中的電洞萃取出來。將高分子PTSN做為錫鈣鈦礦層與HTL間之介面修飾層所組裝之反式TPSCs的PCE可達9.30% (而以Cu-SCO/PDTON及Cu-SCO為HTL的元件效率分別為8.06%及7.91%)。

摘要(英)

The absorbers of Tin Perovskite solar cells (TPSCs) have great prospects due to their ideal energy gap (∼1.4 eV) and low toxicity. The power conversion efficiency (PCE) has achieved a significantly value of 15%. However, the tin perovskite absorber is susceptible to Sn2+ oxidation and rapid crystallization, leading to problems such as poor stability, and poor film quality. Moreover, the cell may have poor interfacial compatibility between carrier transporting layer and tin perovskite layer. Lots of researches focus on adding additives to the tin perovskite precursor solution to inhibit the oxidation of Sn2+, but less studies focus on the issue of interfacial compatibility. In this study, we used a published polymer PDTON as a base, using the same isopropyl-triphenylamine (i-pr-TPA) with hole transport ability as the Acceptor. The hole-transporting moiety cyclopentadithiophene (CPDT) with two hydrophilic alkylamine side chains was used (instead of TPA on PDTON) as a donor to prepared a new bipolar polymer PTSN. There are three advantages of PTSN: First, it uses the hole-extracting thiophene in the CPDT structure to extract effectively the holes from the tin perovskite layer. The second is that compared to TPA, CPDT has two hydrophilic alkylamine chain can better modify the surface and HOMO energy of the hole transport layer (HTL) Cu-SnCo2O4 (Cu-SCO) to match better the valence band of the tin perovskite and the Lewis base amine group can passivate the defects of the tin perovskite film. The third is that PTSN has both hydrophilic and hydrophobic groups, which can increase the affinity between the tin perovskite precursor and PTSN. The thermal decomposition temperatures of both polymers are greater than 200°C. UV-Vis absorption spectra show that at the same concentration, the light absorption of the PTSN solution and film is smaller than those of PDTON, allowing more photons to reach the tin perovskite absorber. Contact angle of the tin perovskite precursor solution on PTSN film is smaller than that on the PDTON film, indicating that the compatibility with tin perovskite precursor solution is better. Moreover, the valence band edge (-5.53) of the Cu-SCO/PTSN film better matched with the valence band (-5.74 eV) of the tin perovskite than that (-5.49) of Cu-SCO/PDTON film therefore the energy loss of hole transporting is less. FTIR spectra show that the C-N stretching of amine and C-S stretching of thiophene of PTSN+SnI2 and PTSN+Cu-SCO both blue-shifted compared to pure PTSN, indicating that the lone pairs of nitrogen on the amine group and sulfur on thiophene could interact with the coordinated unsaturated Sn2+ of Cu-SCO film and tin perovskite surface. PL and TRPL data show that the fluorescence intensity of tin perovskite deposited on PTSN-modified Cu-SCO is weaker than that deposited on Cu-SCO/PDTON and Cu-SCO HTLs, and the carrier lifetime is also shorter, indicating that Cu- SCO/PTSN HTL can most effectively extract the holes from tin perovskite. The PCE of inverted TPSCs using polymer PTSN as the interface modification layer can reach 9.30% (compared to 8.06% for using PDTON as a interface modificate agent and 7.91% for cell coithout interface modification agent).

關鍵字(中)

★ 錫鈣鈦礦太陽能電池
★ 兩性介面修飾
★ 高分子

關鍵字(英)

論文目次

摘要 v
Abstract vii
Graphical Abstract ix
謝誌 x
目錄 xi
圖目錄 xv
表目錄 xxi
第一章、緒論 1
1-1、前言 1
1-2、太陽能電池種類 1
1-3、鈣鈦礦太陽能電池PSC的元件架構及工作機制 4
1-4、反式鈣鈦礦太陽能電池的兩性介面修飾材料 6
1-4-1、反式錫鈣鈦礦層與電洞傳遞層之兩性介面修飾材料所需具備之性質 6
1-4-2、使用兩性高分子PFN衍生物作為鉛鈣鈦礦層與載子傳遞層之介面修飾材料 7
1-4-3、使用P3CT-BN作為一般式鉛鈣鈦礦層與電洞傳遞層之兩性介面修飾材料 13
1-4-4、使用PTFTS作為反式鉛鈣鈦礦層與電洞傳遞層之兩性介面修飾材料 16
1-4-5、使用CPE-K作為反式鉛鈣鈦礦層與電洞傳遞層之兩性介面修飾材料 19
1-4-6、兩性高分子PDTON應用於鈣鈦礦太陽能電池之電洞傳遞層或電極緩衝層 22
1-4-7、使用有機兩性小分子TEA作為鉛鈣鈦礦層與電洞傳遞層之介面修飾材料 24
1-5、研究動機 28
第二章、實驗部分 30
2-1、實驗藥品 30
2-2、產物與中間產物之結構及簡稱 33
2-3、實驗步驟 36
2-3-1、兩性介面修飾材料的合成(polymer 1) 36
2-3-1-1、TBP-CPDT (Donor 1)的合成，如圖2-3-1-1所示 37
2-3-1-2、DiBpin-i-pr-TPA (Acceptor 1)的合成，如圖2-3-1-2所示 39
2-3-1-3、高分子中間體PTSBr的合成，如圖2-3-1-3所示 41
2-3-1-4、高分子PTSN的合成，如圖2-3-1-4所示 42
2-3-2、兩性介面修飾材料的合成(polymer 2) 44
2-3-2-1、Br-TON (Donor 2)的合成，如圖2-3-2-1所示 45
2-3-2-2、高分子PDTON的合成，如圖2-3-2-2所示 48
2-4、儀器分析及樣品製備 49
2-4-1、核磁共振光譜儀(Nuclear Magnetic Resonance Spectrometer, NMR) 49
2-4-2、聚焦微波化學反應系統(CEM) 50
2-4-3、紫外光/可見光/近紅外光分光光譜儀(UV/ Vis Sepectrometer) 51
2-4-4、電化學測量(Electrochemical Measurement System) 52
2-4-5、傅立葉轉換紅外光光譜儀(Fourier transform infrared spectrometer) 54
2-4-6、熱重分析(Thermogravimetric Analysis) 56
2-4-7、接觸角量測儀(Contact angle meter) 57
2-4-8、凝膠滲透層析儀(Gel Permeation Chromatography, GPC) 58
2-4-9、高分子溶解度的測量 61
2-4-10、反式錫鈣鈦礦太陽能電池元件的組裝及測試 61
第三章、結果與討論 62
3-1、高分子中間體PTSBr與高分子PTSN的結構鑑定 62
3-1-1、PTSBr與PTSN的1H NMR 62
3-1-2、PTSN的13C NMR 65
3-1-3、PTSN及PDTON的MALDI-TOF Mass圖譜 67
3-2、高分子PTSBr及PDTON的合成步驟探討 69
3-3、高分子PTSN及PDTON的溶解度比較 73
3-4、PTSN作為介面修飾層塗佈在Cu-SCO上的EDS圖 75
3-5、高分子PTSN及PDTON的熱穩定性質 76
3-6、高分子PTSN及PDTON個別DA單體的差異性比較 77
3-6-1、PTSN之DA單體的UV-Vis吸收光譜圖及Tauc plot圖 77
3-6-2、PTSN之DA單體的電化學循環伏安圖及前置軌域能階 78
3-6-3、PTSN與PDTON之個別DA單元的差異性 80
3-7、高分子PTSN及PDTON溶液及膜在相同濃度下之UV-Vis吸收光譜圖的吸收度比較 84
3-8、高分子PTSN及PDTON鍍在Cu-SCO上膜的UV-Vis吸收光譜圖及Tauc plot圖 86
3-9、高分子PTSN及PDTON鍍在Cu-SCO上膜的UPS能譜圖及前置軌域能階 87
3-10、高分子PTSN及PDTON的水接觸角及錫鈣鈦礦前驅溶液接觸角 90
3-11、介面修飾層塗佈在Cu-SCO上膜的SEM表面形貌圖及AFM圖 91
3-12、錫鈣鈦礦沉積在介面修飾層PTSN及PDTON上的SEM表面形貌圖 93
3-13、錫鈣鈦礦沉積在PTSN或PDTON膜上的PL及TRPL圖 94
3-14、PTSN及PDTON的電洞遷移率及缺陷密度 95
3-15、PTSN及PDTON與Cu-SCO及錫鈣鈦礦之作用 100
3-16、PTSN及PDTON作為錫鈣鈦礦層及電洞傳遞層之介面修飾層所組裝之反式錫鈣鈦礦太陽能電池的光伏表現 106
第四章、結論 108
參考文獻 110
附錄 114

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指導教授

吳春桂(Chun-Guey Wu)

審核日期

2024-8-21

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