作為高開路電壓的反式錫鈣鈦礦太陽能電池之WO3電洞傳遞層的研究

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研究生：	朱奇祐 Chi-Yu Chu
論文名稱：	作為高開路電壓的反式錫鈣鈦礦太陽能電池之WO3電洞傳遞層的研究
指導教授：	吳春桂 Chun-Guey Wu
口試委員:
學位類別：	碩士 Master
系所名稱：	理學院 - 化學學系 Department of Chemistry
論文出版年：	2022
畢業學年度：	110
語文別：	中文
論文頁數：	134
中文關鍵詞：	錫鈣鈦礦、太陽能電池
外文關鍵詞：	tin perovskite, solar cells
相關次數：	點閱：9 下載：0
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反式錫鈣鈦礦太陽能電池中錫鈣鈦礦層(Tin Perovskite簡稱TPsk)是沉積在電洞傳遞層(Hole transport layer簡稱HTL)上，HTL的品質將會影響TPsk的沉積與品質。本研究以熱蒸鍍的方式製備WO3作為反式錫鈣鈦礦太陽能電池的HTL，WO3的價帶能(-5.33 eV)與本實驗所使用TPsk (FA0.98EDA0.01SnI3，價帶能為-5.57 eV)之能量差比PEDOT:PSS的價帶能(-5.15 eV)與TPsk之能量差小，因此以WO3為HTL時，電洞在元件內傳輸時的能量損失較少，所組裝元件有較大的開路電壓(Open circuit voltage，Voc)及光電轉換效率(Power conversion efficiency，PCE)，以WO3及PEDOT:PSS膜作為HTL所組裝元件的Voc分別為0.59 V和0.53 V，最高PCE則分別為9.44%及8.93%。WO3膜為HTL所組裝的元件在手套箱中經2520小時仍可維持原效率的84% ，而PEDOT:PSS膜為HTL所組裝的元件在相同保存條件下經2520小時僅維持原效率67%。而元件的熱穩定性測試中，WO3膜為HTL所組裝的元件在手套箱中加熱60C經2小時仍可維持原效率的72%，而PEDOT:PSS膜為HTL所組裝的元件在相同測試條件下僅維持原效率58%。WO3膜可經UV/O3後處理提高膜與TPsk前驅溶液的相容性，使沉積其上的TPsk品質變好，由SEM表面形貌圖可看見沉積在WO3的錫鈣鈦礦膜顆粒較大且平整。時間解析螢光光譜也顯示TPsk沉積在WO3膜上的載子生命週期比沉積在PEDOT:PSS上短，意味著WO3膜比PEDOT:PSS能更快速的將電洞由TPsk萃取出來並傳遞至陽極。

In inverted tin perovskite solar cells (referred as TPSCs), the tin perovskite layer (referred as TPsk) is deposited on top of the hole transport layer (referred as HTL). Therefore the quality of the HTL will be effected by the deposition methods and the quality of the resulting TPsk layer. In this study, WO3 prepared by thermal evaporation was used as an HTL for inverted tin perovskite solar cells. The valence band energy of WO3 (-5.33 eV) closer (compared to the generally used PEDOT:PSS with a valence band energy of -5.15 eV) to that of TPsk (FA0.98EDA0.01SnI3 with the valence band energy of -5.57 eV) used in this experiment. Therefor WO3 can be a better HTL than PEDOT:PSS. The Voc and PCE of TPSCs based on WO3 and PEDOT:PSS HTLs are 0.59 V and 0.53 V, 9.44% and 8.93% respectively. Without packing, the TPSC based on WO3 HTL can maintain 84% of the original efficiency after 2520 hours in the glove box, while that assembled with PEDOT:PSS HTL 33% of the original efficiency lost under the same test conditions. When the cells were heated at 60oC in a glove box, the TPSCs assembled with WO3 HTL can maintain 72% of the original efficiency after heating for 2 hours, while the TPSC based on PEDOT:PSS HTL can only maintain 58% of the original efficiency. SEM surface topography revealed that the tin perovskite grains deposited on WO3 are larger and flatter compared to those coated on top of PEDOT:PSS. Time-resolved photoluminescence spectroscopy also shows that the carrier lifetime of TPsk deposited on WO3 film is shorter than that deposited on PEDOT:PSS meaning that WO3 film can extract holes from TPsk and transfer to the anode more quickly than PEDOT:PSS.

目錄
摘要
謝誌    XI
目錄    XII
圖目錄    XVIII
表目錄    XXIV
第1章    緒論    1
1-1、    前言    1
1-2、    鈣鈦礦太陽能電池    2
1-2-1.    反式元件架構的工作原理    3
1-2-2.    電洞傳遞層(HTL)應用於反式錫鈣鈦礦太陽能電池需具備的條件    4
1-2-3.    無機電洞傳遞材料的優點    5
1-2-4.    無機電洞傳遞層應用於鈣鈦礦太陽能電池相關文獻    6
1-3、    錫鈣鈦礦太陽能的研究歷程    6
1-3-1.    第一個以MASnI3作為吸收層的錫鈣鈦礦太陽能電池研究    7
1-3-2.    第一個以CsSnI3作為吸收層的錫鈣鈦礦太陽能電池研究    9
1-3-3.    第一個以FASnI3作為吸收層並以SnF2作為添加劑的錫鈣鈦礦太陽能電池研究    10
1-3-4.    目前文獻中錫鈣鈦礦太陽能電池的最高光電轉換效率    13
1-3-5.    目前文獻中無機電洞傳遞層所組裝錫鈣鈦礦太陽能電池的最高光電轉換效率    15
1-4、    製備錫鈣鈦礦膜的方法    17
1-4-1.    以一步合成法製備錫鈣鈦礦膜    17
1-4-2.    以兩步合成法製備錫鈣鈦礦膜    18
1-4-3.    以一步反溶劑法製備錫鈣鈦礦膜    19
1-5、    不同的電洞傳遞層組裝成反式鈣鈦礦太陽能電池    20
1-5-1.    尖晶石結構作為反式鉛鈣鈦礦太陽能電池之電洞傳遞層    21
1-5-2.    MoO3作為反式鉛鈣鈦礦太陽能電池之電洞傳遞層    21
1-5-3.    NiOx作為反式錫鈣鈦礦太陽能電池之電洞傳遞層    23
1-6、    不同方式製備WO3膜    23
1-6-1.    以Nanocrystals製備WO3膜作為電洞傳遞層並應用於反式鉛鈣鈦礦太陽能電池    23
1-6-2.    以Sol-gel法製備WO3膜作為電洞傳遞層並應用於一般式鉛銫鈣鈦礦太陽能電池    24
1-6-3.    WO3的結構與其性質    25
1-7、    實驗動機    27
第2章    實驗方法    28
2-1、    實驗藥品與儀器    28
2-1-1.    藥品    28
2-1-2.    儀器設備    30
2-2、    反式錫鈣鈦礦太陽能電池組裝步驟    31
2-2-1.    前置作業    31
2-2-2.    元件組裝步驟    32
2-3、    儀器原理及樣品製備    37
2-3-1.    太陽光模擬器的原理及光電轉換效率、暗電流與遲滯現象的量測(Solar Simulator, Enlitech SS-F5)    37
2-3-2.    太陽能電池外部量子效率量測系統(Incident Photon to Current Conversion Efficiency (IPCE), QE-S3011)    39
2-3-3.    X-ray繞射光譜儀(X-Ray Diffractometer, BRUKER D8 Discover)    40
2-3-4.    紫外光/可見光/近紅外光吸收光譜儀(Ultraviolet–visible-NIR spectroscopy, HITACHI U-4100)    41
2-3-5.    光致螢光光譜儀(Photoluminescence Spectrometer, Uni think UniRAM)    42
2-3-6.    場發射掃描式電子顯微鏡(Field Emission Scanning Electron Microscope, NOVA Nano SEM-230)    43
2-3-7.    UPS紫外光電子能譜儀(Ultraviolet photoelectron spectroscopy, Thermo VG-Scientific/Sigma Probe)    44
2-3-8.    XPS光電子能譜儀(X-ray photoelectron spectroscopy, Thermo VG-Scientific/Sigma Probe)    45
2-3-9.    接觸角量測儀(Contact angle, Grandhand Ctag01)    46
3-3-10.    空間電荷限制電流的原理及量測(Space Charge-Limited Current, SCLC)    47
第3章    結果與討論    50
3-1、    錫鈣鈦礦層的製備條件優化    50
3-1-1.    篩選錫鈣鈦礦前驅液的濃度製備成膜所組裝之元件的光伏表現    50
3-1-2.    篩選錫鈣鈦礦前驅液中SnI2 :有機鹵化物之比例製備成膜所組裝之元件的光伏表現    52
3-1-3.    錫鈣鈦礦前驅液旋轉塗佈時不同的轉速所組裝之元件的光伏表現    54
3-1-4.    篩選不同比例的混溶劑配製錫鈣鈦礦前驅溶液    55
3-1-5.    篩選錫鈣鈦礦前驅膜的加熱溫度    57
3-2、    WO3電洞傳遞層的製備條件篩選    59
3-2-1.    篩選WO3電洞傳遞層之厚度    59
3-2-2.    WO3膜的修飾    60
3-3、    錫鈣鈦礦層之優化    70
3-3-1.    細篩滴入反溶劑的時機點    70
3-4、    不同電洞傳遞層所組裝之元件的IPCE值及遲滯因子    74
3-5、    不同電洞傳遞層所組裝之元件手套箱中的長時間穩定性
3-6、    不同電洞傳遞層所組裝之元件大氣下的長時間穩定性    78
3-7、    不同電洞傳遞層所組裝之元件的熱穩定性    79
3-8、    不同電洞傳遞層的SEM表面形貌    80
3-9、    沉積在不同電洞傳遞層上之錫鈣鈦礦膜的SEM表面形貌及剖面圖    81
3-10、    沉積在不同電洞傳遞層上之錫鈣鈦礦膜的XRD圖    83
3-11、    PEDOT:PSS膜及WO3膜的UV-Vis穿透光譜    84
3-12、    不同電洞傳遞層之前置軌域能階    86
3-13、    不同電洞傳遞層上沉積錫鈣鈦礦的XPS能譜圖    88
3-14、    沉積在不同電洞傳遞層上之錫鈣鈦礦膜的PL及TRPL光譜    90
3-15、    錫鈣鈦礦前驅溶液與PEDOT:PSS膜及WO3膜的相容性    91
3-16、    不同電洞傳遞層所組裝之反式錫鈣鈦礦太陽能電池之穩態電流密度及效率輸出之影響    93
3-17、    不同電洞傳遞層所組裝之反式錫鈣鈦礦太陽能電池之暗電流的影響    94
3-18、    不同電洞傳遞層之電洞遷移率及沉積在不同電洞傳遞層上錫鈣鈦礦層之缺陷密度    96
第4章    結論    100
參考文獻    101









                                

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