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調控金屬摻雜二氧化鈦電子傳輸層與鹼土金屬摻雜鈣鈦礦主動層之高效率太陽能電池

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Contents指導教授推薦書口試委員會審定書致謝 iii摘要 ivAbstract viContents viiiList of Tables xList of Figures xiChapter 1 Introduction 11.1 Perovskite solar cells 11.2 Hysteresis phenomena in perovskite solar cells 41.3 TiO2 electron transport layer for perovskite solar cell 71.4 Lead-free/reduced perovskite solar cel

l 111.5 Mixed-cation perovskite solar cell 151.6 Motivation 17Chapter 2 Experimental Section 192.1 Chemicals 192.2 Materials and sample preparation 202.2.1 Synthesis of methylammonium iodide 202.2.2 Preparation of Zn-doped TiO2 precursor solution 202.2.3 Synthesis of meso-Zn:TiO2 paste 212.2.4 Prepa

ration of perovskite precursor solution 222.2.5 Preparation of spiro-OMeTAD solution 222.3 Fabrication of perovskite solar cells 222.3.1 Fabrication of planar perovskite solar cells 222.3.2 Fabrication of mesoporous perovskite solar cells 232.4 Instruments 252.5 Characterization of Materials and Dev

ices 262.5.1 Photovoltaic performance of perovskite solar cell 262.5.2 Morphology observation 262.5.3 Optical property 272.5.4 Crystal structure 28Chapter 3 Results and Discussion 293.1 Enhanced short-circuit current density of perovskite solar cells using zinc-doped TiO2 as electron transport layer

293.2 Enhancing efficiency of perovskite solar cells using mesoscopic zinc-doped TiO2 as electron transport layer through band alignment 433.3 Enhancing perovskite solar cell performance and stability by doping alkaline earth metal in methylammonium lead halide 64Chapter 4 Conclusion 82Chapter 5 Re

commendation 84References 85Appendix 93List of TablesTable 1.1 Photovoltaic performance of PSCs with metal-doped TiO2 10Table 1.2 List of PCE and lead content of CH3NH3M1-xPbxX3 PSC 14Table 2.1 List of chemicals used in this study 19Table 2.2 List of instruments used in this study 25Table 3.1 Summar

y of conductivity of various Zn-doped TiO2 compact layers 33Table 3.2 Summary of measured fast decay time (τ1), slow decay time (τ2), and PL average decay (τavg) for CH3NH3PbI3-xClx/Zn-doped TiO2 37Table 3.3 Characteristics of PSCs with different Zn doping concentration in the TiO2 compact layer 39T

able 3.4 The theoretical and experimental atomic ratios of Zn/Zn+Ti in pristine TiO2 and various Zn-doped TiO2 41Table 3.5 The ratios of Zn/Zn+Ti in 5.0 mol% Zn-doped TiO2 thick film measured by EDS analysis 42Table 3.6 Photovoltaic performance of various PSCs based on different ETL 48Table 3.7 Summ

ary of decay time and PL average decay time for CH3NH3PbI3/meso-Zn:TiO2/dense TiO2/FTO 48Table 3.8 Summary of measured fast and slow decay time and PL average decay for the film of Ba2+-doped perovskite/TiO2/FTO 73Table 3.9 Characteristics of the pristine perovskite film and various alkaline earth m

etal-doped PSCs 74Table 3.10. The stoichiometric ratio of elements as determined by EDS for pristine perovskite and 3.0 mol% Ba-doped perovskite film 77List of FiguresFigure 1.1 The efficiency chart of PSCs by different research groups 2Figure 1.2 The typical structure of perovskite (e.g. CH3NH3PbX3

) 3Figure 1.3 Schematic diagrams of PSCs in (a) p-i-n and (b) n-i-p structure 4Figure 1.4 J-V curves of PSC (a) with and (b) without hysteresis 5Figure 1.5 Diffusion paths for (a) I vacancy, (b) CH3NH3 vacancy, (c) Pb vacancy, and (d) iodine interstitials 6Figure 1.6 Schematic diagram of energy leve

l of (a) p-i-n structure and (b) n-i-p structure PSC 7Figure 1.7 (a) I-V curves of non-doped TiO2 NPs and Co-doped TiO2 NPs and (b) corresponding J-V curves of PSCs. (c) Diagram of energy levels and (d) J-V curves of PSCs with Li-doped TiO2. (e) The cross-section SEM image and (f) J-V curves of PSCs

with Ta-doped TiO2 NR arrays 9Figure 1.8 (a) Simulated crystal structure of CH3NH3SnI3 and (b) J-V curve of CH3NH3SnI3 PSC. (c) J-V curves of FASnI3 PSC and (d) histogram of the solar cell reproducibility. (e) J-V curve of the CsSnI3 PSC and (f) EQE spectrum and integrated Jsc 12Figure 1.9 (a) J-V

curves and (b) EQE spectra of PSC with and without Al3+ doping. (c) Diffuse reflectance UV-Vis spectra for the CH3NH3PbI3, and CH3NH3Pb1-xBxI3, with B=Sn, Sr, Cd, Ca, and x=0.10. (d) J-V curves of Sr-doped PSCs with different doping concentration 13Figure 1.10 (a) UV-vis-NIR absorption and photolumi

nescence spectrum for the FAPbI3 single crystal . (b) Tauc plot and energy level of FAPbI3 single crystal. Thermal stability of perovskite film (c) without and (d) with Cs+ doping. (e) J-V curves of Rb+-doped PSCs 16Figure 1.11 Plot of tolerance factors versus octahedral factors of CH3NH3MI3 (M=Mg,

Ca, Sr and Ba) 18Figure 2.1 Flow chart of preparation of Zn-doped TiO2 precursor solution 21Figure 2.2 Schematic diagram of preparation of fabrication of mesoscopic PSC 24Figure 2.3 Photographs of KPFM measurement under wavelength-switchable LED light source illumination. (a) 470 nm, (b) 530 nm, (c)

656 nm, (d) 850 nm, and (e) white light 27Figure 3.1 Synchrotron X-ray spectra of (a) pristine TiO2 and various Zn-doped TiO2 and (b) magnified spectra 29Figure 3.2 (a) Absorption spectra and (b) the plot of (αhν)2 versus hν of pristine TiO2 and various Zn-doped TiO2 compact layer 31Figure 3.3 The

current density-electric field (J-E) curves of the various Zn-doped TiO2 compact layers and the inset is the schematic diagram of testing structure 32Figure 3.4 SEM images of (a) pristine TiO2 compact layer and various Zn-doped TiO2 compact layers, including (b) 1.0 mol% Zn-TiO2, (c) 3.0 mol% Zn-TiO

2, (d) 5.0 mol% Zn-TiO2, and (e) 7.0 mol% Zn-TiO2. (f) The RMS roughness distribution of various Zn-doped TiO2 compact layers are measured by AFM 34Figure 3.5 AFM images of (a) pristine TiO2 compact layer and various Zn-doped TiO2 compact layers, including (b) 1.0 mol% Zn-TiO2, (c) 3.0 mol% Zn-TiO2,

(d) 5.0 mol% Zn-TiO2, and (e) 7.0 mol% Zn-TiO2 35Figure 3.6 Photoluminescence spectra using (a) static and (b) time-resolved of CH3NH3PbI3-xClx/Zn-doped TiO2/FTO measured at room temperature 37Figure 3.7 (a) The schematic diagram of PSC structure. (b) J-V curves, (c) the plots of photovoltaic chara

cteristics, and (d) EQE spectra of the PSCs with different Zn-doped TiO2 compact layer 40Figure 3.8 EDS spectra at separated six positions of 5.0 mol% Zn-doped TiO2 film 42Figure 3.9 The SEM images showing the surface microstructure of (a) non-doped meso-TiO2 and various meso-Zn:TiO2, including (b)

1.0 mol%, (c) 3.0 mol%, (d) 5.0 mol%, and (e) 7.0 mol%. (f) The particle size distribution of the meso-TiO2 with different Zn doping level 44Figure 3.10 (a) XRD patterns, (b) UV-vis absorption spectra, and (c) Tauc plots of various meso-Zn:TiO2. (d) J-V curves of various PSCs based on different TiO2

-based ETL. (e) PL spectra and (f) transient TRPL plots of the device based on the following structure: CH3NH3PbI3/meso-Zn:TiO2/dense TiO2/FTO 47Figure 3.11 UPS spectra of the meso-TiO2 with different Zn doping level. (a) Secondary-electron cut-off, and (b) the valence-band region 50Figure 3.12 Sche

matic energy level diagram of various meso-Zn:TiO2 from UPS measurements 51Figure 3.13 2D GIWAXS patterns of CH3NH3PbI3/meso-TiO2/dense TiO2/FTO, where the meso-TiO2 is (a) without and (b) with 5.0 mol% Zn doping. (c) 1D patterns of out-of-plane line cut. The images of the contact angles of water on

(d) non-doped meso-TiO2 and (e) 5.0 mol% meso-Zn:TiO2 52Figure 3.14 Azimuthal intensity plots that corresponding to Figure 3.13(a) and 3.13(b) along the ring at q=10 nm-1, produced by the (110) plane of the CH3NH3PbI3 film 53Figure 3.15 AFM topographic image and cross-sectional measurement along th

e red line of two types of CH3NH3PbI3/meso-TiO2/dense TiO2/FTO films without (a) and with (b) 5.0 mol% Zn doping in meso-TiO2. The corresponding CPD images and cross-sectional analyses of CPD data under different wavelengths of light, including (c, d) 470 nm, (e, f) 530 nm, (g, h) 636 nm, (i, j) 850

nm, and (k, l) white light 55Figure 3.16 Bar charts of ΔCPD v.s. different wavelengths of light for CH3NH3PbI3/meso-TiO2/dense TiO2/FTO structure with non-doped meso-TiO2 and 5.0 mol% meso-Zn:TiO2 56Figure 3.17 (a) I-V curves of the device with the following structure: FTO/dense TiO2/meso-TiO2/Au w

ithout and with 5.0 mol% Zn doping. (b) I-V curves of ohmic region (I∝V) and (c) J-V2 curve of Child’s region (I∝V2) 58Figure 3.18 (a) Jsc and (b) Voc are dependent on light intensity of PSC without and with 5.0 mol% meso-Zn:TiO2 60Figure 3.19 (a) The schematic diagram and the (b) cross-section SEM

image of PSC with 5.0 mol% meso-Zn:TiO2 (scale bar = 500 nm). (c) J-V curves of PSCs without and with 5.0 mol% meso-Zn:TiO2 under reverse and forward scans. (d) PCE distribution and (e) EQE spectra of PSCs with either the pristine or 5.0 mol% meso-Zn:TiO2. (f) The J-V curve of champion device 62Figu

re 3.20 Long-term stability of PSCs with non-doped meso-TiO2¬ and 5.0 mol% meso-Zn:TiO2 under (a) ambient atmosphere (∼30% relative humidity, 25 oC) and (b) glovebox system (N2 with H2O