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Morphology Control of Photoactive Layer for Highly Efficient Perovskite solar cells

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Cross-sectional TEM images of devices with (a) MAPbI3 and (b) CsMAPbI3. perovskite films as light absorbers. The inset images show the corresponding deformation (twisting, crumpling, bending) of the rectangular AgNW electrode foil adhered to the PDMS thin film.

Introduction

In this perspective, this thesis investigates the morphological control of the photoactive layer for high-efficiency perovskite solar cells. In Chapter 6, a simple and effective new process for high-efficiency p-i-n planar heterojunction structure of perovskite solar cells (PeSCs) using the compact seed perovskite layer (CSPL) is described in Chapter 6.

Figure 1. 2. 12% conversion efficiency arrived in land from the sun cover the demand of energy in 2050
Figure 1. 2. 12% conversion efficiency arrived in land from the sun cover the demand of energy in 2050

Background theory and device physics for perovskite Solar Cells

  • Properties of perovskite materials
  • Working principle of perovskite solar cells
  • Crystallization process of perovskite films
  • Figures of merit of thin film solar cells

Similarly, using PbCl2 as one of the perovskite precursors for the "one step" method also produced a uniform perovskite film in the same way. For universal characterization of solar cells manufactured anywhere in the world, the standard air mass, AM1.5G, is widely used on the solar simulator.

Figure 2. 2. Basic device structure of perovskite solar cells
Figure 2. 2. Basic device structure of perovskite solar cells

Mixed solvents for the Optimization of Morphology in Solution-processed,

  • Research background
  • Experimental details
  • Results and discussion
  • Conclusion

Although the film of DMF had relatively smaller voids and almost completely covered the PEDOT:PSS layer, there were uneven crystal domains with small (~100 nm) and large (200-300 nm) grain sizes (Figure 3.2b). In contrast, the film from the solvent mixture had uniform crystal domains with smaller grain sizes (~100 nm) (Figure 3. 2c). We calculated the internal quantum efficiency (IQE) of the devices from the EQE and measured reflectance (Figure 3.5b).

8 shows high-resolution transmission electron microscopy (HR-TEM) cross-sectional images of the devices prepared from different solvents. The device from GBL exhibited the thickest perovskite film with a large variation in film thickness (37 ± 18 nm) (Figure 3. 8a), while the devices from DMF and mixed solvents exhibited relatively thin and flat perovskite films (DMF: 32 ± 13 ) nm and mixed solvent: 30 ± 11 nm) (Figure 3. 8b and 3. 8c).

Figure 3. 1. (a) Device structure. (b) Energy band diagram of p-i-n structure PeSCs.
Figure 3. 1. (a) Device structure. (b) Energy band diagram of p-i-n structure PeSCs.

Cesium-Doped Methylammonium lead Iodide Perovskite Light Absorber for

Research background

XPbI3 as electron donor and [6,6]-phenyl-C60 butyric acid methyl ester (PCBM) as electron acceptor. The cation (A) in ABX3 perovskites generally includes alkylammonium or alkali metal cations (eg, methylammonium, formamidinium, cesium, etc.). The identity of the A cation greatly influences the band gap and electronic properties of the perovskites through its influence on the crystal structure.28, 41 Since MAPbI3 perovskite is a well-known light absorber with a low band gap of 1.5 eV and high extinction coefficient in PeSCs, 3, 20 , 26 we replace a fraction of the MA ions with Cs to optimize the optical and electrical properties of the material while maintaining the basic properties of MAPbI3 (Figure 4. 1a).

To prepare MAPbI3 absorbent films, a precursor solution consisting of equimolar amounts of methylammonium iodide (MAI) and lead iodide (PbI2) was first dissolved in a mixed solvent of dimethylformamide (DMF) and γ-butyrolactone (GBL) (DMF:GBL) = 97: 3 vol.%) and stirred at 60 °C for 24 h in a nitrogen-filled glove box. The CsXMA1-XPbI3 precursor solutions were prepared using the same procedure in which a fraction of MAI was replaced by CsI.

Experimental details

Results and discussion

Optical bandgap of CsXMA1-XPbI3 perovskite with different Cs ratio obtained from transformed Kubelka-Munk spectra. The transformed Kubelka-Munk spectra from the UV-vis absorption results clearly showed changes in the optical band gap of CsXMA1-XPbI3 perovskite with different Cs ratio (Fig. 4. . 2b). The ED(VB)-EA(LUMO) of the perovskite/PCBM HSC is about 1.1 eV, indicating that the VOC values ​​can be improved by Cs doping. a) J-V characteristics and (b) EQE of CsXMA1-XPbI3 perovskite devices with different Cs ratio.

5b, we compared the EQE curves of devices using CsXMA1-XPbI3 perovskites with different Cs ratio. 10 shows cross-sectional transmission electron microscopy (TEM) images of optimized MAPbI3 and CsXMA1-XPbI3 perovskite devices.

Figure 4. 2. (a) UV-vis absorption and (b) transformed Kuberka-Munk spectra of CsXMA1-XPbI3 perovskite  films with different Cs ratio
Figure 4. 2. (a) UV-vis absorption and (b) transformed Kuberka-Munk spectra of CsXMA1-XPbI3 perovskite films with different Cs ratio

Conclusion

Research background

Here, we demonstrate planar heterojunction ternary p-i-n PeSC halides prepared via a low-temperature solution processing route. Previous literature has shown that high-efficiency devices prepared from precursor solutions containing binary mixtures of Cl- and I- ions yield films with negligible Cl- content after the film is dried and annealed, since most of the Cl- evaporates as CH3NH3Cl (MACl). during the baking step. Despite the low concentration of Cl- in the finished film, this halide is closely involved in the formation of the perovskite film.

The processing used in this study conveniently involves the incorporation of PbBr2 into binary MAPbI3-xClx precursor solutions and similar device processing as used in binary perovskite materials, while the proportions of the three halides can be easily controlled to modulate and optimize film properties. Since the final Cl content in the film remains small, we refer to ternary halide perovskite as CH3NH3PbI3-y-xBryClx.

Experimental details

Briefly, the optical absorption of each layer within the device was calculated using the transfer matrix method.[38] Then, the parasitic absorption, i.e. the absorption absorbed by the buffer layers and electrodes, was subtracted from the experimentally measured absorption of the fully structured device to determine the absorption of the active layer only. Finally, the relationship between the EQE and the absorption spectrum of the active layer was used to calculate the IQE spectrum of the devices.

Results and discussion

XRD diffraction patterns for MAPbI2.9-xBr0.1Clx ternary halide perovskite films deposited on glass substrates. The MAPbI2.9-xBr0.1Clx condition yielded a homogeneous and pinhole-free morphology, which most completely covered the hole transport layer compared to other ratios (y in the MAPbI3-y-xBryClx system. In particular, the EV of MAPbI2. 9- xBr0.1Clx was found to be 0.1 eV larger than the binary.

2b, the homogeneous and defect-free crystal domains of MAPbI2.9-xBr0.1Clx led to higher overall JSC values. The VOC of MAPbI2.9-xBr0.1Clx devices is particularly reproducible with a deviation of less than 10% compared to the MAPbI3-xClx.

Table 5. 1. Optical band gaps of MAPbI 3-y-x Br y Cl x  (y = 0, 0.1, 0.3, 0.5, 1) perovskite films with different Br ratios  derived from Tauc plots
Table 5. 1. Optical band gaps of MAPbI 3-y-x Br y Cl x (y = 0, 0.1, 0.3, 0.5, 1) perovskite films with different Br ratios derived from Tauc plots

Conclusion

The introduction of perovskite seed layer for high performance perovskite solar

  • Research background
  • Experimental details
  • Results and discussion
  • Conclusion

Cross-sectional SEM images directly display the perovskite seed layer which can be a core point to make a high crystalline perovskite film. On the PTAA (control) substrate, PbI2 seed layer and MAPbBrxI3-x perovskite seed layer were respectively deposited. XPS recording spectrum of PTAA control, PbI2 seed layer and CSPL films after washing with DMF solvent.

The presence of the seed layer was confirmed by XPS measurement even after washing with DMF solvent. The 2D-GIWAXS patterns of the perovskite layer have a similar peak position and shape compared to the control perovskite film at and (310).

Figure 6. 1. Energy band diagram of perovskite solar cells.
Figure 6. 1. Energy band diagram of perovskite solar cells.

Ultrathin, Lightweight and Flexible Perovskite Solar Cells with an Excellent

Research background

Thus, they developed AgNW-based flexible PSC devices with an amorphous metal oxide protective layer on both sides of the AgNW layer; their device achieved the energy conversion efficiency (PCE) of Kim et al. Therefore, a method that allows manipulation of the surface morphology of AgNW networks is needed to efficiently prevent silver halide formation while improving device efficiency. The orthogonal orientation of the AgNWs effectively prevents the formation of silver halide during the fabrication of the PSC device due to the smooth surface morphology, resulting in a higher device efficiency of 15.18% for the orthogonal AgNW electrodes on glass substrates compared to those (10.3%) of electrodes with random AgNWs.

On top of the hole transport layer, the MAI precursor solutions were centrifuged at 3000 rpm for 30 s, and the PbI2 solution was spin coated at 5000 rpm for 30 s. Thin metal apertures (13.0 mm2) were attached to each cell before measuring the J–V characteristics.

Results and discussion

Figure 1e shows a cross-sectional scanning electron microscopy (SEM) image of our PSC with orthogonal AgNW electrodes. To verify the smooth surface morphology of the rectangular AgNW electrodes, the surface of the PEDOT:PSS (AI4083) layer deposited on the PH1000/orthogonal and random AgNW electrodes was analyzed (Figure 7.6). These topological results indicate that AgNW/PH1000 orthogonal electrodes can prevent the formation of AgI more effectively than AgNW random electrodes.

J–V hysteresis characteristics of a PSC with ITO, orthogonal AgNW, and random AgNW electrode measured with forward and reverse bias. Comparison of the device performance of our PSC with orthogonal AgNW arrays and those of other AgNW-based PSC devices.

Figure 7. 2. Dark-field optical micrograph of a random AgNW network. The fast Fourier transform (FFT) image  of the optical micrograph (inset) shows a blurred circular pattern, reflecting the randomness of the corresponding  surface geometric structure
Figure 7. 2. Dark-field optical micrograph of a random AgNW network. The fast Fourier transform (FFT) image of the optical micrograph (inset) shows a blurred circular pattern, reflecting the randomness of the corresponding surface geometric structure

Conclusion

Summary

학위를 시작하기 전의 새로운 시작에 대한 설렘과 두려움은 아득히 먼 기억으로, 그때의 열정도 사라지는 동안, 제 곁에서 지켜봐 주시고 동기를 부여해 주시고 '나무 심기'의 씨앗을 심도록 지켜봐 주세요. new passion 이 글을 통해 저에게 변함없는 힘을 주시는 많은 분들께 감사의 마음을 전하고 싶습니다. 하지만 교수님의 인내와 격려 덕분에 좋은 결과를 얻을 수 있었습니다. 많은 교수님들이 제가 논문을 개발하는 데 도움을 주셨습니다.

먼저, 석사과정 동안 연구방법과 기본자세를 가르쳐주신 박혁규 교수님, 논문심사 과정에서 많은 조언을 해주신 석상일 교수님, 그리고 가르침을 주신 송명훈 교수님. LG디스플레이 프로젝트를 함께 진행하면서 새로운 도전과 방향에 어떻게 접근하는지 알아보세요. 또한, 태양전지를 활용한 응용연구를 수행할 수 있도록 도와주신 고현협 교수님, 센터장 김동석 박사님에게도 감사의 말씀을 전하고 싶습니다. 연구에 막힐 때마다 늘 적절한 조언과 도움을 줬던 한국에너지기술연구원 조임현 연구원. . 연구실에 처음 왔을 때와는 달랐던 효성, 마피아가 아닌 진짜 학자의 길을 잘 보여주신 김성범 교수님, 저의 영어를 이해하고 설명해주신 브라이트 명보 교수님 쉽게 물어보고 실험해볼게 많았는데 너무 짧았습니다. 떠나신 이정훈 교수님, 그리고 지난 2년 동안 저를 많이 괴롭혔지만 잘 받아주신 기환 선생님, 많은 성과를 거둘 수 있어서 행운이라고 생각합니다.

Gambar

Figure 1. 1. Solar cells convert light energy into electrical energy by photovoltaic effect
Figure 2. 9. An example of external quantum efficiency and integrated JSC of solar cell
Figure 3. 2. (a-c) SEM top-view. (d-f) AFM topography images of CH3NH3PbI3 perovskite films from  different solvents
Figure 3. 3. (a) UV-vis absorption spectra. (b) XRD patterns of CH3NH3PbI3 perovskite films from different  solvents
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