이동석 진공학회 초록
동석 이
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Abstract
Hybrid organic-inorganic perovskite solar cells recently have received much interest for next generation photovoltaic devices due to simple manufacturing process, low-cost, and high energy conversion efficiency. Relatively large bandgap of perovskite materials enables the fabrication of tandem solar cells with small bandgap Si or thin film solar cells. However, Si cell usually has random pyramid texture which makes it hard to form compact and crystalline perovskite layer on top of Si layer through conventional solution spin-coating technique. Electrodeposition method is scalable, low-cost process, and widely used way to form the various film regardless of substrate morphology.
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Investigation into the Advantages of Pure Perovskite Film without PbI 2 for High Performance Solar Cell OPEN
In CH 3 NH 3 PbI 3-based high efficiency perovskite solar cells (PSCs), tiny amount of PbI 2 impurity was often found with the perovskite crystal. However, for two-step solution process-based perovskite films, most of findings have been based on the films having different morphologies between with and without PbI 2. This was mainly due to the inferior morphology of pure perovskite film without PbI 2 , inevitably produced when the remaining PbI 2 forced to be converted to perovskite, so advantages of pure perovskite photoactive layer without PbI 2 impurity have been overlooked. In this work, we designed a printing-based two-step process, which could not only generate pure perovskite crystal without PbI 2 , but also provide uniform and full surface coverage perovskite film, of which nanoscale morphology was comparable to that prepared by conventional two-step solution process having residual PbI 2. Our results showed that, in two-step solution process-based PSC, pure perovskite had better photon absorption and longer carrier lifetime, leading to superior photocurrent generation with higher power conversion efficiency. Furthermore, this process was further applicable to prepare mixed phase pure perovskite crystal without PbI 2 impurity, and we showed that the additional merits such as extended absorption to longer wavelength, increased carrier lifetime and reduced carrier recombination could be secured. Recently, organometal trihalide perovskite materials having composition ABX 3 (e.g. A = Cs + , CH 3 NH 3 + (meth-ylammonium, MA), or HC(NH 2) 2 + (formamidinium, FA); B = Pb or Sn; X = I, Br or Cl) have been investigated extensively for use as light-absorbing material in solar cells because of their unique properties such as direct optical bandgap, broadband light absorption, bipolar transport, and long carrier diffusion length. Since the first report about perovskite solar cells (PSC) having 3.81% power conversion efficiency (PCE) by Kojima et al. in ref. 1, which triggered intensive research in the development of PSC, remarkable enhancement in power conversion efficiency (PCE) reaching 20% has been achieved during past several years 2–4. In conventional silicon-based p-n junction photovoltaic (PV) devices, the pure crystal structure in photoac-tive layer has been known to be advantageous to efficient charge transport and reduced exciton quenching for high efficiency solar cell. However, in MAPbI 3-based PSC showing high efficiency, tiny amount of residual PbI 2 impurity was often found with the perovskite crystal phase, even though the equimolar composition of organic (MAI) and inorganic (PbI 2) components was utilized to fully convert them to perovskite crystal 3,5–14. Therefore, various approaches have been reported to find out if perovskite crystal with PbI 2 impurity would be advantageous to the performance of PSC or not. However, in general, the crystalline structure and nanoscale morphology of perovskite photoactive layers are significantly influenced by their deposition methodology 15–22 , and therefore those reports should be individually interpreted depending on their growth mechanism. Chen el al. reported an approach to produce pure MAPbI 3 film by treating as-deposited PbI 2 film with MAI vapor for several hours, from which PbI 2 component could be reversibly regenerated when annealed at 150 °C 5,6. They showed that the regenerated PbI 2 from the pure MAPbI 3 crystal structure by annealing was helpful to pas-sivate grain boundary (GB) between crystal domains, consequently improving their device performances due to the reduced recombination 6. Similarly, Zhang et al. investigated the role of PbI 2 in their perovskite film, grown by spin-casting hydrohalide deficient PbI 2 ·xHI (x = 0.9~1) precursor under MA vapor atmosphere. Using their
A Novel Strategy for Scalable High-Efficiency Planar Perovskite Solar Cells with New Precursors and Cation Displacement Approach
Advanced materials (Deerfield Beach, Fla.), 2018
Methylammonium iodide (MAI) and lead iodide (PbI ) have been extensively employed as precursors for solution-processed MAPbI perovskite solar cells (PSCs). However, the MAPbI perovskite films directly deposited from the precursor solutions, usually suffer from poor surface coverage due to uncontrolled nucleation and crystal growth of the perovskite during the film formation, resulting in low photovoltaic conversion efficiency and poor reproducibility. Herein, propylammonium iodide and PbI are employed as precursors for solution deposition of propylammonium lead iodide (PAPbI ) perovskite film. It is found that the precursors have good film formability, enabling the deposition of a large-area and homogeneous PAPbI perovskite film by a scalable dip-coating technique. The dip-coated PAPbI film is then subjected to an organic-cation displacement reaction, resulting in MAPbI film with high surface coverage and crystallinity. With the MAPbI film as the light absorber, planar PSCs are fabr...
Fully Roll-to-Roll Processed Efficient Perovskite Solar Cells via Precise Control on the Morphology of PbI2:CsI Layer
Nano-Micro Letters, 2022
Perovskite solar cells (PSCs) have attracted tremendous attention as a promising alternative candidate for clean energy generation. Many attempts have been made with various deposition techniques to scale-up manufacturing. Slot-die coating is a robust and facile deposition technique that can be applied in large-area roll-to-roll (R2R) fabrication of thin film solar cells with the advantages of high material utilization, low cost and high throughput. Herein, we demonstrate the encouraging result of PSCs prepared by slot-die coating under ambient environment using a two-step sequential process whereby PbI2:CsI is slot-die coated first followed by a subsequent slot-die coating of organic cations containing solution. A porous PbI2:CsI film can promote the rapid and complete transformation into perovskite film. The crystallinity and morphology of perovskite films are significantly improved by optimizing nitrogen blowing and controlling substrate temperature. A power conversion efficiency...
Investigation into the Advantages of Pure Perovskite Film without PbI2 for High Performance Solar Cell
Scientific Reports, 2016
In CH3NH3PbI3-based high efficiency perovskite solar cells (PSCs), tiny amount of PbI2 impurity was often found with the perovskite crystal. However, for two-step solution process-based perovskite films, most of findings have been based on the films having different morphologies between with and without PbI2. This was mainly due to the inferior morphology of pure perovskite film without PbI2, inevitably produced when the remaining PbI2 forced to be converted to perovskite, so advantages of pure perovskite photoactive layer without PbI2 impurity have been overlooked. In this work, we designed a printing-based two-step process, which could not only generate pure perovskite crystal without PbI2, but also provide uniform and full surface coverage perovskite film, of which nanoscale morphology was comparable to that prepared by conventional two-step solution process having residual PbI2. Our results showed that, in two-step solution process-based PSC, pure perovskite had better photon ab...
E-MRS Spring Meeting 2015 Symposium C -Advanced inorganic materials and structures for photovoltaics Development of homogeneous perovskite films on flat substrates for planar heterojunction solar cells
CH 3 NH 3 PbI 3 layers have been prepared by two-step procedure (spin coating and dipping) on flat substrates under open-air conditions and high relative humidity. The films have been characterized by means of scanning electron microscopy, absorption coefficient and x-ray diffraction when varying spinning rate, washing procedure and dipping time. In particular a novel washing procedure has been developed to improve the film uniformity. Hole transport material free solar cells have been realized on flat substrates. The devices have been characterized by measuring the current density-voltage J(V) characteristics under AM1.5g illumination and the external quantum efficiency (EQE). Preliminary results are discussed.
Fabrication of Efficient Low-Bandgap Perovskite Solar Cells by Combining Formamidinium Tin Iodide with Methylammonium Lead Iodide
Journal of the American Chemical Society, 2016
Mixed tin (Sn)-lead (Pb) perovskites with high Sn content exhibit low bandgaps suitable for fabricating the bottom cell of perovskite-based tandem solar cells. In this work, we report on the fabrication of efficient mixed Sn-Pb perovskite solar cells using precursors combining formamidinium tin iodide (FASnI3) and methylammonium lead iodide (MAPbI3). The best-performing cell fabricated using a (FASnI3)0.6(MAPbI3)0.4 absorber with an absorption edge of ∼1.2 eV achieved a power conversion efficiency (PCE) of 15.08 (15.00)% with an open-circuit voltage of 0.795 (0.799) V, a short-circuit current density of 26.86(26.82) mA/cm(2), and a fill factor of 70.6(70.0)% when measured under forward (reverse) voltage scan. The average PCE of 50 cells we have fabricated is 14.39 ± 0.33%, indicating good reproducibility.
Novel inorganic-organic perovskites for solution processable photovoltaics
2014
We have fabricated semi-transparent perovskite solar cells with an efficiency of over 12%. This has enabled us to make 4-terminal hybrid tandem solar cells which comprise of a semi-transparent large bandgap (MA)PbI3 (MA = CH3NH3 ) perovskite solar cell stacked on top of a smaller bandgap CIGS or silicon solar cell, achieving efficiencies over 18% in the case of the CIGSperovskite tandem. As the reliability of the perovskite material remains the greatest technical risk in commercialization of perovskite photovoltaics, we have made several important discoveries regarding instabilities of the perovskite to electrical bias and illumination. In particular, we have found that perovskite solar cells in planar architectures typically exhibit hysteresis with voltage, and a decline in performance under steady-state conditions that can be reversed by forward biasing the device. These observations are consistent with electromigration of ions within the device during operation. We have also foun...
A hybrid physical–chemical deposition process at ultra-low temperatures for high-performance perovskite solar cells
J. Mater. Chem. A, 2015
The quality of a perovskite film will directly determine the performance and stability of the corresponding perovskite solar cell. High-quality and uniform CH 3 NH 3 PbI 3 films were synthesized by a new hybrid physical-chemical vapor deposition (HPCVD) process in a vacuum and isothermal environment. The reaction temperature can be accurately adjusted from 73 C to 100 C, with 73 C as the lowest reaction temperature for a vapor based approach. CH 3 NH 3 PbI 3 solar cells with high performance were fabricated at 82 C to achieve a high power conversion efficiency (PCE) up to 14.7%. The unsealed champion solar cell was tested for 31 days continuously, and its efficiency could maintain 12.1%, demonstrating high effectiveness of this HPCVD process.
Factor affecting the performance of perovskite solar cell for distinct MAPI layer thickness
INTERNATIONAL CONFERENCE ON MULTIFUNCTIONAL MATERIALS (ICMM-2019)
From an extensive study, we proposed a perovskite solar cell device structure (ITO/ZnO/CH 3 NH 3 PbI 3 /C 60 /Au) to demonstrate the carrier transport and optical characterization using a commercially available software package. We used a distinct thickness of CH 3 NH 3 PbI 3 active layer for the bandgap of 1.65 eV which delivers a power conversion efficiency (PCE) of 14.37% and external quantum efficiency about 82% respectively. Amongst the different thicknesses of perovskite layer, the 250 nm thick perovskite layer offers the highest open-circuit voltage of 0.807V, short-circuit current density (9.28mA/cm 2), and fill factor about 0.7677. It accounts for quite remarkable significant improvement depicted in absorbance profile, mainly 86% for 250 nm thickness of the perovskite MAPI layer. Simultaneously, an average of 94% observed in the absorbance profile in sweeping angle cases from 0 to 85 degrees.
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Novel Solvent-free Perovskite Deposition in Fabrication of Normal and Inverted Architectures of Perovskite Solar Cells
Scientific Reports, 2016
Using a two-step deposition technique to prepare perovskite (CH3NH3PbI3) for thin film solar cells based on ZrO2 and TiO2 mesostructures
RSC Advances, 2013
A two-step deposition technique is used for preparing CH 3 NH 3 PbI 3 perovskite solar cells. Using ZrO 2 and TiO 2 as a mesoporous layer, we obtain an efficiency of 10.8% and 9.5%, respectively, under 1000 W m 22 illumination. The ZrO 2 based solar cell shows higher photovoltage and longer electron lifetime than the TiO 2 based solar cell. Although highly efficient solar cells have already been commercialized based on silicon and compound semiconductors, the manufacturing processes are still relatively expensive in terms of both materials and techniques. On the other hand, efficient and low-cost organic and dye-sensitized solar cells (DSSCs) have been making good progress recently, 1-3 although their maximum performance still falls behind the inorganic thin-film counterparts. Thus, further improvement of the solar cell performance and stability is still required for practical applications. Lately, threedimensional hybrid perovskites, due to their unique electrical and optical properties, along with their enormous flexibility in construction of quantum confinement structures, 6,7 have been used in thin film solar cells, 8,9 with a highest efficiency of 12.3%, which affords a good alternative for solar energy utilization. Generally, there are four methods, including spin-coating, 12 vacuum vapor deposition, 13 two-step deposition technique (TSD), and patterning thin film 16 to prepare the hybrid perovskite film. 17 One-step spin-coating is the most widely method to prepare the solar cells, but it is difficult to control film properties including thickness, uniformity, and morphology. Additionally, for the organic part, the longer the organic chains, the more difficult to find a good solvent. For the inorganic part, solvent techniques always encounter some problems, because of
Synthesis of Hybrid Lead Iodide Perovskite Thin Film by Two-Step Method Modified with a Double Dipping Circle to Control Its Crystallization and Morphology to Improve Solar Cells’ Performance
Journal of Nanomaterials
Crystallization and morphology of perovskite film played an important role to obtain efficient performance of perovskite solar cells. This study is aimed at optimizing the fabrication of hybrid organic–inorganic lead iodide perovskite layer by a two-step method modified by a double dip coating process which enables to control the perovskite crystallization and morphology. The duration time of each circle for the step of dipping PbI2 film to methylammonium iodide solution was varied from 90 to 240 second. The obtained perovskite films were characterized by X-ray diffraction to evaluate the transformation of PbI2 reactant to the perovskite product and its crystallization, by scanning electron microscopy to observe its morphology. Then, the perovskite films were implemented in functional perovskite solar cell devices followed by current–voltage characterization. Results showed that the perovskite was formed via an equilibrium process which reached an optimum transformation of PbI2 to t...
Enhancing the performance and stability of MAPbI3 perovskite solar cells by inserting the ITO layer before the Ag electrode
NATIONAL CONFERENCE ON PHYSICS AND CHEMISTRY OF MATERIALS: NCPCM2020, 2021
Diffusion of silver(Ag) from the electrode in perovskite solar cell layers in presence of moisture is a serious issue in fabrication of stable halide perovskite-based solar cells (PSC). We witnessed a fast degradation of the fabricated planar p-in PSC having device structure as glass/ITO/PEDOT:PSS/MAPbI3/PCBM/Ag. This degradation is due to the presence of ambient moisture and reaction of Ag with perovskite to form silver iodide(AgI). The diffusion of Ag into the layers of PSC was easily noticeable after a few hours of device fabrication. Therefore, to suppress the fast diffusion of silver electrode into the perovskite absorber layer, a thin layer of ITO indium tin oxide(ITO) was incorporated in PSC, between the electron transport layer(ETL) and Ag electrode which modified the device configuration as glass/ITO/PEDOT:PSS/ MAPbI3/PCBM/ITO/Ag. It was observed that the performance and stability of the device with this ITO layer improved significantly compared to the device without ITO. Using intermediate ITO layer, improved the device power conversion efficiency (PCE, η) from 1% to 8%, with open-circuit voltage(Voc) = 0.86V, short-circuit current density(Jsc) = 19.11mAcm-2 , and fill factor(FF) = 0.49.
Synthesis and characterization of MAPbI3 thin film and its application in C-Si/perovskite tandem solar cell
Journal of Materials Science: Materials in Electronics, 2020
Silicon, polymer and dye sensitized have been increasing rapidly in thin film of solar cells. Recently, perovskite is proposed as alternative material in the fabrication of solar cells. In this study, methyl ammonium lead triiodide (MAPbI 3 , CH 3 NH 3 PbI 3) perovskite thin film was prepared by two-step process of spin coating. The preparation process of thin film is summarized by reaction between the methyl ammonium iodide (CH 3 NH 3 I) and lead iodide (PbI 2). The absorbent layer of the prepared perovskite solar cell is based on the MAPbI 3 (CH 3 NH 3 PbI 3) thin film. The conversion efficiency of p-n silicon solar cells can be improved by preparing tandem solar cells. The X-ray diffraction result of the MAPbI 3 perovskite film manifested that it is polycrystalline with tetragonal system having a crystallite size of about 40 nm. The absorption spectrum of perovskite film was recorded by Ultra Violet-Visible spectrophotometer. The energy band gap of the MAPbI 3 film calculated by Tauc's formula was ~ 1.51 eV. The field emission scanning electron microscope image of the MAPbI 3 film surface elucidated a cubic-like crystal structure and other irregular structures also. The atomic force microscope image and the distribution chart of the grains of the film displayed that the grain size was ~ 58.7 nm. The results demonstrated that the conversion efficiency for silicon, perovskite and tandem (silicon/perovskite) solar cells are 3%, 4.83% and 7.42%, respectively.
Highly Efficient 2D/3D Hybrid Perovskite Solar Cells via Low-Pressure Vapor-Assisted Solution Process
Advanced Materials, 2018
high carrier mobility. [2,3] A typical perovskite has a 3D lattice structure with a formula of ABX 3 where A + is composed of organic (CH 3 NH 3 + (MA +) or CH 3 (NH 2) 2 + (FA +)) or inorganic (cesium + (Cs +) or rubidium + (Rb +)) cation, B 2+ is the divalent metal (Pb 2+ or Sn 2+), and X − is the halide (Cl − , Br − , or I −). [2,4] To realize commercial applications, the long-term stability issues such as durability under humid, thermal, and light-soaking conditions should be further investigated and improved. [5] Most annoyingly, the perovskite thin film is quite sensitive to moisture and oxygen, resulting in degradation under atmosphere. The low formation energy of the perovskite structures tends to hydrolyze in the presence of moisture. [6] One of the methods to stabilize halide perovskite is to use the layered structure with 2D perovskites, the so-called Ruddlesden-Popper layered perovskites, where larger hydrophobic cation acts as a spacer to isolate the 3D MAPbI 3. [7-12] The general formula of Ruddlesden-Popper perovskites is defined as A′ 2 A n−1 B n X 3n+1 , where n is an integer between 1 and ∞ and A′ + is large-sized cation (typically ammonium-based cation such as phenyl ethylammonium (PEA), [10] polyethylenimine (PEI), [13] n-butylammine (BA), [14] cyclopropylamine (CA), [15] octadecylamine (OA), [16] or ammoniumvaleric The fabrication of multidimensional organometallic halide perovskite via a lowpressure vapor-assisted solution process is demonstrated for the first time. Phenyl ethyl-ammonium iodide (PEAI)-doped lead iodide (PbI 2) is first spincoated onto the substrate and subsequently reacts with methyl-ammonium iodide (MAI) vapor in a low-pressure heating oven. The doping ratio of PEAI in MAI-vapor-treated perovskite has significant impact on the crystalline structure, surface morphology, grain size, UV-vis absorption and photoluminescence spectra, and the resultant device performance. Multiple photoluminescence spectra are observed in the perovskite film starting with high PEAI/ PbI 2 ratio, which suggests the coexistence of low-dimensional perovskite (PEA 2 MA n−1 Pb n I 3n+1) with various values of n after vapor reaction. The dimensionality of the as-fabricated perovskite film reveals an evolution from 2D, hybrid 2D/3D to 3D structure when the doping level of PEAI/PbI 2 ratio varies from 2 to 0. Scanning electron microscopy images and Kelvin probe force microscopy mapping show that the PEAI-containing perovskite grain is presumably formed around the MAPbI 3 perovskite grain to benefit MAPbI 3 grain growth. The device employing perovskite with PEAI/PbI 2 = 0.05 achieves a champion power conversion efficiency of 19.10% with an open-circuit voltage of 1.08 V, a current density of 21.91 mA cm −2 , and a remarkable fill factor of 80.36%. Perovskite Solar Cells Organic-inorganic hybrid perovskite materials have attracted numerous attentions in solar energy conversion and various optoelectronic applications [1] due to their long carrier diffusion length, high absorption coefficients in the visible range, and The ORCID identification number(s) for the author(s) of this article can be found under
Bi and Sn Doping Improved the Structural, Optical and Photovoltaic Properties of MAPbI3-Based Perovskite Solar Cells
Materials
One of the most amazing photovoltaic technologies for the future is the organic–inorganic lead halide perovskite solar cell, which exhibits excellent power conversion efficiency (PCE) and can be produced using a straightforward solution technique. Toxic lead in perovskite can be replaced by non-toxic alkaline earth metal cations because they keep the charge balance in the material and some of them match the Goldschmidt rule’s tolerance factor. Therefore, thin films of MAPbI3, 1% Bi and 0%, 0.5%, 1% and 1.5% Sn co-doped MAPbI3 were deposited on FTO-glass substrates by sol-gel spin-coating technique. XRD confirmed the co-doping of Bi–Sn in MAPbI3. The 1% Bi and 1% Sn co-doped film had a large grain size. The optical properties were calculated by UV-Vis spectroscopy. The 1% Bi and 1% Sn co-doped film had small Eg, which make it a good material for perovskite solar cells. These films were made into perovskite solar cells. The pure MAPbI3 film-based solar cell had a current density (Jsc)...
Perovskite solar cells based on a perovskite film with improved film coverage
Synthetic Metals, 2020
Organic-inorganic halide perovskite solar cells have attracted considerable attention because of its high efficiency, low-cost fabrication, and flexibility. The film morphology has to be well controlled since the presence of pinholes in the perovskite films deteriorates the performance of the devices. Therefore, a variety of methods have been developed to realize high quality perovskite films and excellent device performance. In this work, hotcasting technique and additive engineering were investigated for obtaining a better film morphology. Optical microscopy, electron scanning microscopy and X-ray diffraction were used to monitor the morphology and the crystallinity of the perovskite films. We found that pinhole-free perovskite films cannot be obtained by the hotcasting technique alone. By using the hot-casting technique and incorporating the additive in the perovskite precursor, perovskite films with minimum pinholes were obtained when optimum hot-casting temperature and the amount of the additive were used. A reproducible average power conversion efficiency of 9.24 % was observed. The findings showed that the perovskite films depend not only on the usage of hot-casting technique but also through the incorporation of additives which can be used for other perovskite materials utilizing as solar cells.
Synthesis and characterization of one-step spin-coated organic perovskite (CH3NH3PbI3) thin films for photovoltaic applications
In the present work, we have synthesized methylammonium lead iodide(MAPbI 3)films in ambient air condition using a single step spin coating technique. X-Ray Diffraction (XRD) pattern revealed the formation of perovskite films along with an average grain size of 59.44 nm. Closely packed, uneven grain sizes can be observed in the pin hole free Field Emission Scanning Electron Microscopy (FESEM) image. The calculated value of band gap for MAPbI 3 was estimated as 1.581 eV using Tauc's relation. The current-voltage characteristic clearly indicates the ohmic nature of the thin films. The results indicate that the films can be further used for fabrication of low-costperovskite solar cells.
Fabrication and Characterization of a Perovskite-Type Solar Cell with a Substrate Size of 70 mm
A perovskite-type solar cell with a substrate size of 70 mm × 70 mm was fabricated by a simple spin-coating method using a mixed solution. The photovoltaic properties of the TiO2/CH3NH3PbI3-based photovoltaic devices were investigated by current density-voltage characteristic and incident photon to current conversion efficiency measurements. Their short-circuit current densities were almost constant over a large area. The photoconversion efficiency was influenced by the open-circuit voltage, which depended on the distance from the center of the cell.
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