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Title Page 2

ABSTRACT 5

Contents 6

Ⅰ. INTRODUCTION 11

1.1. Emerging perovskite solar cells with overcoming their structural instability 11

1.2. Instability of the perovskite precursors 11

1.3. The integrated strategy to regulate perovskite precursors and films 12

Ⅱ. EXPERIMENTAL 14

2.1. Materials 14

2.2. The preparation of perovskite solutions 14

2.3. The preparation of anodized nickel oxide (A-NiO) 14

2.4. Device fabrication 15

2.5. Characterization of perovskite film and devices 16

2.5.1. Note 1 16

2.5.2. Note 2 17

2.5.3. Note 3 17

2.5.4. Note 4 17

2.5.5. Note 5 18

2.5.6. Note 6 18

Ⅲ. RESULTS AND DISCUSSION 19

3.1. Characterization of perovskite films and precursors 19

3.2. Stabilization of 3-MBA in perovskite precursor 21

3.3. Film properties of 3-MBA-treated perovskite films 25

3.4. Photovoltaic performance 27

3.5. Stability test of perovskite films and devices 28

Ⅳ. CONCLUSION 30

Reference 71

요약문 77

List of Tables 8

Table 1. Integration of peaks corresponding organic cation for 10d-aged precursors, which is from the ¹H-NMR spectra 66

Table 2. Integration of peaks corresponding organic cation for 20d-aged precursors, which is from the ¹H-NMR spectra 66

Table 3. Integration of peaks corresponding organic cation for 35d-aged precursors, which is from the ¹H-NMR spectra 67

Table 4. Integration of peaks corresponding organic cation for 55d-aged precursors, which is from the ¹H-NMR spectra 67

Table 5. I : Pb atomic ratio estimated by atomic ratio XPS spectra from individual 4 films 68

Table 6. Average roughness values from the AFM images for control and 3-MBA films 68

Table 7. Parameters of TRPL spectra 69

Table 8. The Statistics of photovoltaic parameters of the highest performing PSCs (17 devices) 69

Table 9. Nyquist fitting parameters of the control and target PSCs 70

List of Figures 9

Figure 1. Schematic illustration of the major organic and iodide ion degradation mechanisms in perovskite precursor 31

Figure 2. Chemical interaction within perovskite films and characterization of pH evolution 32

Figure 3. pH variation on adding PbI₂ in 3-MBA with molar ratio of 1:1. DMF/DMSO 4:1 solvent (matrix solvent)... 33

Figure 4. ¹H-NMR spectra of FAI, 3-MBA and FAI+3-MBA mixtures (DMSO-d₆), The molecule structure of 3-... 34

Figure 5. ¹H-NMR spectra of FAI, BA and FAI+BA mixtures (DMSO-d₆), The molecule structure of BA, in which... 35

Figure 6. Stabilized 3-MBA-treated perovskite precursor and films 36

Figure 7. ¹H-NMR spectra of control perovskite precursors, 3-MBA- and BA-treated precursors tracked for 0d,... 37

Figure 8. ¹H-NMR spectra representing the generation of large organic cations (MEV⁺ (2.77 ppm) and DMFA⁺... 38

Figure 9. The FTIR spectra for the FAI with 3-MBA and BA.3-MBA and BA-treated FAI showed lower shift... 39

Figure 10. UV-vis absorption spectra of control, 3-MBA, and BA-treated films annealing for 93h. Corresponding... 40

Figure 11. XRD patterns of BA treated perovskite films using aged precursor for 0d, 20d, 35d, and 55d,... 41

Figure 12. Top-view SEM images of control, 3-MBA, and BA-treated perovskite films using aged precursor for... 42

Figure 13. UV-vis absorption spectra of control, 3-MBA, and BA-treated films using aged precursor for 0d, 35d,... 43

Figure 14. Proposed thiol to disulfide exchanged reaction of 3-MBA 44

Figure 15. Photographs of vials for inspection of iodine generation in the pure FAI, and FAI+BA, and FAI+3-... 45

Figure 16. UV-vis absorption spectra of pure FAI, BA-, and 3-MBA-treated FAI solution with aging time... 46

Figure 17. Normalized PL spectra for fresh and aged BA-treated film (55d) and fresh and aged 3-MBA-treated film (55d) 47

Figure 18. Film properties for the modified perovskite films 48

Figure 19. Top-view SEM images and corresponding cross-sectional SEM images. The size distribution of the grams 49

Figure 20. XRD patterns for the 3-MBA+PbI₂ with and without annealing process 50

Figure 21. Atomic force microscopy (AFM) images of the perovskite films with and without 3-MBA treatment 51

Figure 22. The kelvin probe force microscopy (KPFM) results for the with and without 3-MBA treatment 52

Figure 23. Ultraviolet photoelectron spectroscopy to estimate the band structure of the perovskite film with and... 53

Figure 24. Energy-level scheme for the control and 3-MBA treated films 54

Figure 25. Dark J-V curves with the SCLC measurement based on the electron only devices... 55

Figure 26. Photovoltaic characteristics for the control and target devices 56

Figure 27. J¹/²-V curves and fitted plots to estimate electron mobility based on the Mott-Gurney law[이미지참조] 57

Figure 28. J-V curves for the control and 3-MBA-treated PSCs. Hyteresis index is calculated from (PCEreverse-...[이미지참조] 58

Figure 29. Histograms of Photovoltaic parameter (Voc, JSC, FF, and PCE) distributions (17 devices)[이미지참조] 59

Figure 30. Stabilized PCE and photocurrent measured at fixed biases of maximum power point. The external... 60

Figure 31. J-V curves for the control and 3-MBA-treated PSCs with bandgap of 1.54 eV perovskite film. Bandgap... 61

Figure 32. Stability test of perovskite films and PSCs 62

Figure 33. Evolution of XRD patterns for control and 3-MBA-treated perovskite films stored in harsh humid 63

Figure 34. Variation of average PCE statistics for PSCs using aged precursor (~140d) with and without 3-MBA 64

Figure 35. Evolution test of Voc, Jsc, FF for the PSCs using aged precursor based on strorage time with and without...[이미지참조] 65

초록보기

 결함이 적은 고품질 페로브스카이트 층은 고효율 태양전지를 발전시키는데 중요합니다. 그러나 몇 가지 문제 중, 특히 유기 양이온 및 요오드화 이온과 같은 주요 불안정성을 남기는 페로브스카이트 잉크는 재현성을 갖춘 지속 가능한 페로브스카이트 태양전지에 대한 여러 가지 과제를 제기합니다. 여기서는 페로브스카이트 전구체를 우선적으로 안정화하기 위한 주요 사항을 해결합니다. 우리의 전략은 포름아미디늄 이온과의 강화된 수소 결합이 탈양성자화된 메틸아민과의 비가역적 반응을 상당히 억제시키는 것에 중점을 두고 있으며, 이러한 문제를 해결하기 위해 우리는 첨가제로 3-메르캅토벤조산 (3-MBA)을 도입하는 전략을 고안했습니다. 결과적으로, 페로브스카이트 잉크는 최대 140 일 동안 초기 효율의 96% 이상을 유지했습니다. 마찬가지로 중요한 것은 페로브스카이트 층에서 생성된다수의 결함이 3-MBA 의 배위 시스템에 의해 패시베이션된다는 것입니다. 따라서 우리는 페로브스카이트 전구체 잉크와 필름을 모두 관리하기 위한 통합된 전략을 강조합니다. 3-MBA 첨가제가 포함된 반구조 페로브스카이트 태양전지는 24.31%의 인상적인 효율을 나타내며 30 ± 5%의 상대습도에 노출된 후에도 초기 효율의 96% 이상을 유지합니다.

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