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Flexible Perovskite Hybrid Solar Cells Through Organic FLEXIBLE PEROVSKITE HYBRID SOLAR CELLS THROUGH ORGANIC SALT TREATED CONDUCTING POLYMER AS THE TRANSPARENT ELECTRODE A Thesis Presented to The Department of Polymer Engineering of the University of Akron In Partial Fulfillment of the Requirements for the Degree Master of Science Zixu Huang April 2018 i FLEXIBLE PEROVSKITE HYBRID SOLAR CELLS THROUGH ORGANIC SALT TREATED CONDUCTING POLYMER AS THE TRANSPARENT ELECTRODE Zixu Huang Thesis Approved: Accepted: _________________________ ________________________ Advisor Dean of College Dr. Xiong Gong Dr. Eric J. Amis _________________________ _________________________ Faculty Reader Dean of the Graduate School Dr. Ruel McKenzie Dr. Chand K. Midha _________________________ _________________________ Department Chair Date Dr. Sadhan C. Jana ii FLEXIBLE PEROVSKITE HYBRID SOLAR CELLS THROUGH ORGANIC SALT TREATED CONDUCTING POLYMER AS THE TRANSPARENT ELECTRODE Zixu Huang Thesis Approved: Accepted: _________________________ _________________________ Advisor Department Chair Dr. Xiong Gong Dr. Sadhan C. Jana _________________________ _________________________ Committee Member Dean of College Dr. Ruel McKenzie Dr. Eric J. Amis _________________________ _________________________ Committee Member Dean of the Graduate School Dr. Jiahua Zhu Dr. Chand K. Midha _________________________ Date iii ABSTRACT Organic-inorganic hybrid perovskite solar cells (PSCs) have been widely researched due to its low fabrication cost and impressive power conversion efficiency (PCE) in the past 9 years. However, most of the PSCs are developed on transparent conductive oxides (TCOs) like indium tin oxide (ITO), which fabrication process requires energy- consuming high-temperature sintering process. In addition, the high rigidity and brittleness of the ITO electrode also impede the PSCs to be fabricated on flexible substrates like poly(ethylene terephthalate)(PET) film through solution processes. In this study, we corroborated a facile routine to utilize highly electrically conductive and highly transparent poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate) (PEDOT:PSS) thin films as the transparent electrode of the PSCs. To circumvent the problem of low electrical conductivity of the thin films prepared from the pristine PEDOT:PSS solution, organic salt formamidinium iodide (FAI) was used as the treating reagent to boost the conductivity of the thin films from 0.3 S/cm to about 1,600 S/cm. The increment of the conductivity was achieved by the partial removal of the PSS segments and the phase segregation of PEDOT and PSS. As a result, a PCE of 13.36% was obtained for the devices fabricated on FAI-PEDOT:PSS/glass substrate and a PCE of 8.86% for that developed on FAI-PEDOT:PSS/PET substrate This thesis provides a facile way to fabricate flexible and efficient perovskite hybrid solar cells. iv ACKNOWLEDGMENTS First and foremost, I’d like to take this opportunity to show my sincere gratitude to my advisor Dr. Xiong Gong for his insightful guidance and invaluable suggestions in my studies and research project ever since I joined this group in 2016. I also acknowledge him for his constructive supervision on my way to achieve scientific goals which has laid a solid foundation for becoming an open-minded scientist in my long-term career. In addition, I am grateful to my committee, Dr. Ruel McKenzie, and Dr. Jiahua Zhu for their attendance and fruitful discussion for my research proposal and defense. Special thanks to Mr. Tianyu Meng for ESR measurement and Mr. Tao Zhu for the fabrication and characterization of the flexible quantum dot photodetectors, and other group members for their suggestions and assistance. I also would like to express my greatest appreciation to my parents for everything they have offered me as well as their unconditional love and support. Last but not the least, I take this chance to express my gratitude to all of the faculty members in the Department of Polymer Engineering and my classmates for their generous support. v TABLE OF CONTENTS ABSTRACT ............................................................................................................... iv ACKNOWLEDGEMENTS ........................................................................................ v LIST OF FIGURES ................................................................................................. viii LIST OF SCHEMES................................................................................................... x LIST OF TABLES ..................................................................................................... xi CHAPTER 1. INTRODUCTION ................................................................................. 1 1.1 Solar energy and history of solar cells .................................................................. 1 1.2 Crystal structure and history of organic-inorganic perovskite hybrid solar cells . 2 1.3 Fundamental physics of perovskite hybrid solar cells .......................................... 4 1.4 Characterization of perovskite solar cells ............................................................. 5 1.4.1 J V characteristics .............................................................................................. 5 1.4.2 External quantum efficiency (EQE) ................................................................... 6 1.5 TCO-free perovskite solar cells with PEDOT:PSS as transparent electrode. ....... 7 1.5.1 Organic acid treated PEDOT:PSS as transparent electrode. .............................. 7 1.5.2 Silver mesh and PEDOT:PSS hybrid transparent electrode. ............................. 9 1.5.3 Roll-to-roll (R2R) printed flexible perovskite solar cells based on silver nanowire/PH1000 electrode. ..................................................................................... 11 1.6. Poly(3,4-ethylenedioxythiophene): poly(styrene sulfonate) (PEDOT:PSS) ..... 12 1.6.1 Overview of PEDOT:PSS ................................................................................ 12 vi 1.6.2 Structure and conformation of PEDOT:PSS .................................................... 13 1.6.3 Methods to improve the electrical conductivity of PEDOT:PSS ..................... 14 CHAPTER 2. HIGHLY ELECTRICALLY CONDUCTIVE PEDOT:PSS TREATED BY ORGANIC SALT ....................................................................................................... 15 2.1 Introduction ......................................................................................................... 15 2.2 Experimental section ........................................................................................... 16 2.3 Results and Discussion ....................................................................................... 17 CHAPTER 3. TRANSPARENT CONDUCTIVE OXIDE-FREE PEROVSKITE HYBRID SOLAR CELLS WITH ORGANIC SALT TREATED PEDOT:PSS AS TRANSPARENT ELECTRODE...................................................................................... 25 3.1 Introduction ......................................................................................................... 25 3.2 Experimental Section .......................................................................................... 26 3.3 Results and discussion ........................................................................................ 28 CHAPTER 4. CONCLUSION ................................................................................... 34 CHAPTER 5. FUTURE PLAN .................................................................................. 36 vii LIST OF FIGURES Figure Page + Figure 1.1 (a) The crystal lattice of CH3NH3PbI3 perovskite, cation A is CH3NH3 , cation 2+ - B is Pb , anion X is I . (b) unit cell of CH3NH3PbI3 perovskite. Reproduced from Ref. 1 with permission. Copyright © 2014 Elsevier Ltd. .............................................................. 2 Figure 1.2 The device configuration of the perovskite hybrid solar cells (a) Meso- superstructured (MS) PSCs. (b) Planar heterojunction (PHJ) PSCs. .................................. 4 Figure 1.3 The J V characteristics of a perovskite solar cell under illumination. The fill factor (FF) is defined as the ratio of the blue area determined by the maximum power point (mpp) over the green area defined by short circuit current density (JSC) and open circuit voltage. (VOC). .................................................................................................................... 6 Figure 1.4 The external quantum efficiency (EQE) of the organic-inorganic hybrid perovskite solar cells. .......................................................................................................... 7 Figure 1.5. (a) The J V characteristics of the flexible perovskite solar cells fabricated on glass and PET substrates. (b) Photo of a device fabricated on PET substrate. Ref. 6 with permission. Copyright © 2015 American Chemical Society. ............................................. 9 Figure 1.6 (a)The device configuration of the flexible perovskite solar cell (PET/Ag mesh/PH1000/PEDOT:PSS/Perovskite/PCBM/Al). (b)The J V characteristics of the flexible solar cell measured in the dark and under illumination. Ref. 7 with permission. Copyright © 2016 Macmillan Publishers Limited. ........................................................... 10 Figure 1.7 (a)The working mechanism of the roll-to-roll (R2R) printing machine, the inset is a photo of the slot die head for printing ink feeding. (b) SEM image of the cross-sectional view of the printed flexible
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