鈣鈦礦電池之覆晶封裝開發與失效機制;The development of flip-chip package perovskite solar cells and failure mechanism

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题名:	鈣鈦礦電池之覆晶封裝開發與失效機制;The development of flip-chip package perovskite solar cells and failure mechanism
作者:	黃俊凱;Huang, Chun-Kai
贡献者:	化學工程與材料工程學系
关键词:	鈣鈦礦電池;覆晶封裝;鈍化層;氮化矽薄膜;可靠度測試;perovskite solar cell;flip-chip package;passivation layer;Si nitride thin film;reliability test
日期:	2021-06-02
上传时间:	2021-12-07 11:10:32 (UTC+8)
出版者:	國立中央大學
摘要:	在高光電轉換效率且可以製作成軟性元件的優勢下，鈣鈦礦電池從2009年起被廣泛的研究。然而，吸光層中的不穩定的銨鹽與碘離子造成鈣鈦礦電池在高濕度環境下穩定性不佳。除了改質吸光層與結構，封裝結構也可以有效改善鈣鈦礦電池的穩定度。儘管三明治玻璃夾層搭配有機材料的封裝結構可以通過濕熱測試，過大的封裝體體積將減少薄膜電池單位體積產生的功率。因此表面沉積氧化物或氮化物薄膜達到阻水氣氧氣的封裝結構受到各方學者注意。原子沉積(ALD)氧化鋁薄膜是最有效的封裝方式，但是受限於電池面積與過度耗時的缺點而不宜商業化。在第四章節，為解決鈣鈦礦電池的封裝問題，我們決定開發鈣鈦礦電池的覆晶封裝。表面鈍化的製程中，熱累積的效應會明顯影響電池的效率。因此以電漿輔助化學氣相沉積(PECVD)的氮化矽薄膜作為主要抗水氧層，並搭配有機材料、低溫(< 90℃)錫鉍銦焊料與圖案化基板，完成鈣鈦礦電池的覆晶封裝。分析可靠度測試的結果，意外發現純水環境中的封裝電池保有90.2 %的起始效率，高於氮氣環境中的79 % (570 小時)。我們認為封裝的鈣鈦礦電池承受的風險(risk index)與環境中的氧氣/濕度比例有關，而不是水氣與氧氣的含量。在第五章，我們分析不同殘留應力([Si-H]/[Si-N])的氮化矽薄膜在氮氣、氧氣與水氣環境下的失效機制。從傅立葉轉換紅外光譜(FTIR)，我們發現氮化矽薄膜的Si-H鍵氧化受到Si-N鍵的保護。從電子顯微鏡(SEM)的結果發現，殘留的拉伸應力會增加氣體擴散進入氮化物-金屬的介面。在氧氣/水氣複合環境中，氧氣將作為「環境緩衝」的腳色與水氣競爭表面吸附，而降低氮化矽薄膜的氧化程度。然而，氧氣作為環境緩衝層的能力隨著環境氧氣濃度上升而失效，甚至因為擴散促使薄膜與基板分層。我們發現氮化矽的氧化程度與不僅與薄膜本質([Si-H]/[Si-N])相關，甚至須考慮環境的氧氣/濕度比例。藉由以上分析，本研究提出氮化矽薄膜在氧氣與水氣環境下的失效機制。最終，綜合氧化與分層的結果進一步提出氮化矽薄膜在氧氣/水氣混和環境中的失效機制。;Perovskite solar cells were well study since 2009 since the high power conversion efficiency (PCE) and capable of making flexible device. However, unstable alkylammonium salts and iodine ions in the absorption layer lead to the perovskite solar cells low reliability in high humidity ambient. Except the modification of absorption layer or the design structure of perovskite solar cells, the package process can also effectively improve the stability. Despite the common glass-glass sandwich structure with organic sealing can pass the damp heat test, the over-size package will reduce the power per unit volume of thin film solar cell. Therefore, the package structure with nitride/oxide surface passivation film blocking the oxygen and humidity was studied. The Al oxide deposited by ALD was the most effective process, however, the less process-area and time-consuming shortcoming making it hard to commercialize. In order to solve the packing issue mention above, we develop the flip-chip package process of the perovskite solar cells in the Chapter 4. The flip –chip package process was developed with PECVD Si nitride film with chemical materials, low temperature (< 90 ℃) Sn-Bi-In solders and pattern glass substrate. From the reliability test, we surprising finds packaged solar cells remain 90.2 % in the DI-water ambient, however, it only remains 79 % in the N2 ambient (570 hours). We consider not the amount but the ratio of oxygen/humidity in the ambient related with risk index of the packaged perovskite solar cell. In the chapter 5, we analyzed the failure mechanism of different residual stress Si nitride film in the N2, O2 and H2O ambient, which depends on [Si-H]/[Si-N]. From the Fourier-transform infrared spectroscopy (FTIR), we finds the Si-H bonds were passivated by the Si-N bonds. From the Scanning Electron Microscope (SEM), the residual stress enhanced the gas diffusion into the nitride-metal interface. In the oxygen/humidity hybrid ambient, the oxygen was consider as the ambient buffer to decrease the oxidation by conducting the surface competitive adsorption. However, the oxygen acted as ambient buffer was vanished since increasing of oxygen, the delamination happened as well. We finds the Si nitride oxidation depends not only the intrinsic property ([Si-H]/[Si-N]) but also oxygen/humidity of ambient. According to the analysis above, this study illustrated the delamination mechanism of Si nitride film under O2 and H2O ambient. Finally, after understanding the oxidation and delamination, we recognized the delamination of Si nitride film in the oxygen/humidity hybrid ambient.
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