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reference_paper.json

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+[{"abstract":"The morphology of PbI2 film plays a critical role in determining the quality of the resultant CH3NH3PbI3 film and power conversion efficiency of CH3NH3PbI3 perovskite solar cell. Here, we propose a solvent treatment method in the two-step sequential deposition process to control the morphology of PbI2 film, which leads to enhanced power conversion efficiency. Hole transport material free perovskite solar cell is chosen as a paradigm to demonstrate this idea. Solvent (isopropanol, chlorobenzene, or ethanol) treated PbI2 films exhibit dendrite-like or flake-like morphologies, which facilitate more complete conversion of PbI2 to CH3NH3PbI3 perovskite in ambient atmosphere with a relative high humidity. Therefore, enhanced performance is obtained with the solvent treated PbI2 films. Average power conversion efficiency has been improved from 9.42% in the traditional two-step sequential deposition to 11.22% in solar cells derived from ethanol treated PbI2 films.","classification":"psc","classification_value":0,"doi":"10.1016/j.jpowsour.2016.04.062","journal":"Journal of Power Sources","paragraphs":"Enhanced performance in hole transport material free perovskite solar cells via morphology control of PbI2 film by solvent treatmentThe morphology of PbI2 film plays a critical role in determining the quality of the resultant CH3NH3PbI3 film and power conversion efficiency of CH3NH3PbI3 perovskite solar cell. Here, we propose a solvent treatment method in the two-step sequential deposition process to control the morphology of PbI2 film, which leads to enhanced power conversion efficiency. Hole transport material free perovskite solar cell is chosen as a paradigm to demonstrate this idea. Solvent (isopropanol, chlorobenzene, or ethanol) treated PbI2 films exhibit dendrite-like or flake-like morphologies, which facilitate more complete conversion of PbI2 to CH3NH3PbI3 perovskite in ambient atmosphere with a relative high humidity. Therefore, enhanced performance is obtained with the solvent treated PbI2 films. Average power conversion efficiency has been improved from 9.42% in the traditional two-step sequential deposition to 11.22% in solar cells derived from ethanol treated PbI2 films.Organic-inorganic hybrid perovskites have been demonstrated to be an outstanding class of light harvest materials In this manuscript, we have proposed a solvent treatment method to modify the morphologies of PbI2 films in the two-step sequential deposition process, in order to ensure more complete conversion of PbI2 to CH3NH3PbI3 perovskite and better control of the morphologies of CH3NH3PbI3 films. The spin-coated wet PbI2 films are immediately treated with different solvent, i.e., isopropanol, chlorobenzene and ethanol, before the subsequently thermal drying process. Due to the low solubility of PbI2 in these solvent, PbI2 would quickly precipitate and crystallize, leading to a dendrite-like or flake-like morphologies with many nano-sized voids. The existence of voids in the PbI2 films facilitates the diffusion of CH3NH3I, and the nano-sized PbI2 crystal is easily converted into CH3NH3PbI3 perovskite. Thus high quality CH3NH3PbI3 films with controllable morphology and low amount of residual PbI2 are obtained. Hole transport material free perovskite solar cells fabricated on these CH3NH3PbI3 films prepared from solvent treated PbI2 films exhibit superior PCEs. Average PCE has been improved from 9.42% for the traditional two-step sequential deposition to 11.22% in solar cells derived from ethanol treated PbI2 films.1.0M PbI2 and 0.2M PbCl2 was dissolved into N,N-dimethylformamide (DMF) at 70°C under stirring overnight. a presents the schematic two-step sequential deposition process to prepare the CH3NH3PbI3 films without solvent treatment. At first, PbI2 precursor solution was spin-coated onto the mesoporous TiO2 film at 6000rpm for 20s. The obtained PbI2 films were directly dried at 100°C for 5min. Then to convert PbI2 film into perovskite, CH3NH3I isopropanol solution (7mgmL−1) was loaded onto the PbI2 film for 2min, and spun at 2000rpm for 20s. b presents the two-step sequential deposition process with solvent treatment. Immediately after the first-step spin-coating of the PbI2 films, a few drops of solvent, i.e., isopropanol (IPA), chlorobenzene (CB), or ethanol (ET), were dropped onto the wet PbI2 film, soaked for 10s and spun at 2000rpm, the solvent treated PbI2 film was dried at 100°C for 5min. The second-step spin-coating process is the same as the procedure in a. The as-prepared CH3NH3PbI3 films were further dried at 100°C for 15min.Solar cells were fabricated under ambient atmosphere with a relative high humidity, usually around 50%. FTO glass was ultrasonic cleaned with ethanol and acetone. A 0.15M solution of titanium diisopropoxide bis(acetylacetonate) in 1-butanol was spin-coated onto the FTO glass at 3000rpm for 30s, and dried at 150°C for 30min to form the compact TiO2 layer. A homemade P25 paste was prepared by ball milling 2.845g commercial P25 TiO2 particles, 1.423g ethyl cellulose, 11.538g terpineol and 63.222g ethanol together for 24h and was spin-coated onto the compact TiO2 layer at 3000rpm for 30s, and then annealed at 500°C for 30min to form the mesoporous TiO2 layer. The TiO2 films were further treated with 0.4M TiCl4 aqueous solution at 70°C for 30min, then sintered again at 500°C for 30min. The CH3NH3PbI3 perovskite film was prepared using two-step sequential deposition method as discussed in the previous context. Finally, a carbon paste was doctor-bladed onto the perovskite film and dried at 100°C to serve as a counter electrode.X-ray diffraction (XRD) measurements were carried out on a Bruker D8 focus X-ray diffractometer with Cu Kα radiation. Absorption of PbI2 films and CH3NH3PbI3 perovskite films were characterized by UV–vis spectrometer (Lambda 650S, PerkinElmer). SEM images were obtained using scanning electron microscopy (SEM, Sirion FEG, USA). J-V characteristics of the perovskite solar cells were measured on a CHI660C electrochemical workstation under AM 1.5 illumination (100mWcm−2). The applied bias voltage was from 1.0V to−0.1V for the reverse scan, and from−0.1V to 1.0V for the forward scan. The scan rate was 0.05Vs−1. Effective area of the solar cells was 0.10cm2. Incident photon to electron conversion efficiency (IPCE) was measured from 300nm to 800nm with a 300W xenon lamp.Solvent treatment is a commonly used method in one-step spin-coating process to obtain high quality perovskite films . This phenomenon is very similar to that observed in one-step spin-coating process with solvent treatment, thus can be used to control the morphologies of PbI2 films in the two-step sequential deposition process.  displays the photograph of PbI2 films both with solvent treatment and without solvent treatment. The spin-coated wet PbI2 film without solvent treatment shows a light yellow color. When dried at 100°C, solvent evaporates and the film turns to deep yellow color. In the solvent treatment process, when a few drops of solvent are dropped onto the wet PbI2 film, color of the film quickly turns to deep yellow, indicating the quick precipitation and crystallization of PbI2 particles, and stays unchanged in the subsequently drying process.Morphologies of dried PbI2 films and corresponding CH3NH3PbI3 films are studied using SEM, the obtained results are displayed in . PbI2 film without solvent treatment is compact and fully cover the underlying TiO2 layer, some nano-grain PbI2 particles are observed but their boundaries are very blurry, see a. When PbI2 film is exposed to CH3NH3I isopropanol solution, CH3NH3I molecular will diffuse and intercalate into PbI2 lattice forming CH3NH3PbI3 perovskite. Nano-cuboid CH3NH3PbI3 crystals are obtained in the two-step sequential deposition, see b-d. Nano-sized PbI2 particles with well defined boundaries are clearly seen in these solvent treated PbI2 films. In contrary to the compact PbI2 film without solvent treatment, a lot of voids are observed in these solvent treated PbI2 films. Nano-sized PbI2 particles together with the voids will facilitate easier diffusion and reaction of the CH3NH3I molecular with the PbI2 particles f–h. Nano-cuboid CH3NH3PbI3 is obtained again, which is same as the CH3NH3PbI3 film without solvent treatment. But the size of the CH3NH3PbI3 particles with solvent treatment is smaller than that without solvent treatment, which is due to the nano-sized PbI2 prepared from solvent treatment.XRD patterns of the PbI2 films are presented in supporting information . When solvent treated PbI2 films are dried at 100°C, their XRD patterns show only a characteristic PbI2 diffraction peak at ∼12.8° . A strong diffraction peak at ∼12.8° is clearly observed in CH3NH3PbI3 film prepared from PbI2 film without solvent treatment, which indicates a considerable amount of residual PbI2. The relative intensity of PbI2 diffraction peak decreases while relative intensity of the characteristic CH3NH3PbI3 diffraction peak at ∼14.1° increases in the CH3NH3PbI3 films prepared from solvent treated PbI2 films. This indicates that the amount of residual PbI2 decreases while the amount of CH3NH3PbI3 increases in these CH3NH3PbI3 films. As discussed in the previous context, the solvent treated PbI2 films exhibit a favorable morphology, which facilitates more complete conversion of PbI2 to CH3NH3PbI3 films. Our experiments are conducted in ambient atmosphere with a relative high humidity, the PbI2 cannot be completely converted to CH3NH3PbI3UV–vis absorption spectrum of PbI2 films are presented in supporting information . Characteristic absorption edge of PbI2 at ∼500nm is observed in all the PbI2 films, which is in agreement with XRD results. UV–vis absorption spectrum of CH3NH3PbI3 films are presented in . All the spectra exhibit a sharp absorption edge at ∼750nm, as can be seen in the inset picture of a shows typical J-V curves of hole transport material free CH3NH3PbI3 perovskite solar cells prepared from PbI2 films with different treatment process under standard AM1.5 illumination. Variation of open circuit voltage (Voc), short circuit current density (Jsc), fill factor (FF) and power conversion efficiency (PCE) are presented in . CH3NH3PbI3 perovskite solar cells prepared from PbI2 films without solvent treatment show an average Voc of 851mV, Jsc of 18.26mAcm−2, FF of 60.54%, and PCE of 9.42%. When PbI2 films are solvent treated, more complete conversion of PbI2 to CH3NH3PbI3 are observed as discussed in the previous context. The lowered residual PbI2 leads to larger Voc. Solar cells prepared from ethanol treated PbI2 films also show acceptable J-V hysteresis.  shows the J-V curve of the champion cell in PCE. In forward scan mode, the champion cell shows a Voc of 910mV, Jsc of 22.33mAcm−2, FF of 59.7%, corresponding to a PCE of 12.13%. In reverse scan mode, the champion cell gives a Voc of 866mV, Jsc of 21.65mAcm−2, FF of 59.7%, and PCE of 10.45%. The main difference between forward scan and reverse scan is in Voc and Jsc.To confirm the observed variation of Jsc in the CH3NH3PbI3 perovskite solar cells, see a and b, incident photon to current conversion efficiency (IPCE) are measured and presented in . CH3NH3PbI3 perovskite solar cells prepared from PbI2 films without solvent treatment show the lowest IPCE, and solar cells prepared from isopropanol and chlorobenzene treated PbI2 films show comparable IPCE, which are much higher than solar cells prepared from PbI2 films without solvent treatment. The ethanol treated solar cells show the highest IPCE. Therefore, the IPCE spectrum confirms the variation of Jsc in the solar cells with different treatment process.We report a solvent treatment process in the two-step sequential deposition process. The spin-coated wet PbI2 films are immediately treated with isopropanol, or chlorobenzene or ethanol, which induces fast precipitation and crystallization of PbI2 particles. Dendrite-like or flake-like PbI2 films with nano-sized PbI2 particles and a lot of voids are obtained. The voids in the solvent treated PbI2 films facilitate easier diffusion of CH3NH3I molecular. Nano-sized PbI2 particles can be more complete converted to CH3NH3PbI3 perovskite and ensure better control of the resultant morphologies of CH3NH3PbI3 films. Hole transport material free perovskite solar cells fabricated on CH3NH3PbI3 films prepared from solvent treated PbI2 films exhibit enhanced performance compared with that from PbI2 films without solvent treatment. Solar cells from ethanol treated PbI2 films show the best PCE of 11.22%. This method provides a new route to control the morphologies of CH3NH3PbI3 films, and can be used to further improve the efficiency of perovskite solar cells.Photographs of PbI2 films, XRD and UV–vis spectrum of PbI2 films, J-V curve of champion perovskite solar cell.Supplementary data related to this article can be found at ","press":"elsevier","title":"Enhanced performance in hole transport material free perovskite solar cells via morphology control of PbI2 film by solvent treatment"}]