Template‐Assisted Formation of High‐Quality α‐Phase HC(NH2)2PbI3 Perovskite Solar Cells

Formamidinium (FA) lead halide (α‐FAPbI3) perovskites are promising materials for photovoltaic applications because of their excellent light harvesting capability (absorption edge 840 nm) and long carrier diffusion length. However, it is extremely difficult to prepare a pure α‐FAPbI3 phase because of its easy transformation into a nondesirable δ‐FAPbI3 phase. In the present study, a “perovskite” template (MAPbI3‐FAI‐PbI2‐DMSO) structure is used to avoid and suppress the formation of δ‐FAPbI3 phases. The perovskite structure is formed via postdeposition involving the treatment of colloidal MAI‐PbI2‐DMSO film with FAI before annealing. In situ X‐ray diffraction in vacuum shows no detectable δ‐FAPbI3 phase during the whole synthesis process when the sample is annealed from 100 to 180 °C. This method is found to reduce defects at grain boundaries and enhance the film quality as determined by means of photoluminescence mapping and Kelvin probe force microscopy. The perovskite solar cells (PSCs) fabricated by this method demonstrate a much‐enhanced short‐circuit current density (  Jsc) of 24.99 mA cm−2 and a power conversion efficiency (PCE) of 21.24%, which is the highest efficiency reported for pure FAPbI3, with great stability under 800 h of thermal ageing and 500 h of light soaking in nitrogen.

[1]  Jihuai Wu,et al.  Regulation of Interfacial Charge Transfer and Recombination for Efficient Planar Perovskite Solar Cells , 2020, Solar RRL.

[2]  R. Heeren,et al.  Understanding Detrimental and Beneficial Grain Boundary Effects in Halide Perovskites , 2018, Advanced materials.

[3]  T. Hayat,et al.  A Bi-functional additive for linking PI2 and decreasing defects in organo-halide perovskites , 2018 .

[4]  A. Jen,et al.  Intensive Exposure of Functional Rings of a Polymeric Hole‐Transporting Material Enables Efficient Perovskite Solar Cells , 2018, Advanced materials.

[5]  Yang Yang,et al.  2D perovskite stabilized phase-pure formamidinium perovskite solar cells , 2018, Nature Communications.

[6]  Zefeng Chen,et al.  Abnormal Synergetic Effect of Organic and Halide Ions on the Stability and Optoelectronic Properties of a Mixed Perovskite via In Situ Characterizations , 2018, Advanced materials.

[7]  Yongli Gao,et al.  Argon Plasma Treatment to Tune Perovskite Surface Composition for High Efficiency Solar Cells and Fast Photodetectors , 2018, Advanced materials.

[8]  Yongfang Li,et al.  Interfacial engineering via inserting functionalized water-soluble fullerene derivative interlayers for enhancing the performance of perovskite solar cells , 2018 .

[9]  S. Zakeeruddin,et al.  Formation of Stable Mixed Guanidinium-Methylammonium Phases with Exceptionally Long Carrier Lifetimes for High-Efficiency Lead Iodide-Based Perovskite Photovoltaics. , 2018, Journal of the American Chemical Society.

[10]  C. Ratcliffe,et al.  Methylammonium Cation Dynamics in Methylammonium Lead Halide Perovskites: A Solid-State NMR Perspective. , 2018, The journal of physical chemistry. A.

[11]  P. Fang,et al.  Passivated Perovskite Crystallization via g‐C3N4 for High‐Performance Solar Cells , 2018 .

[12]  Seonhee Lee,et al.  Universal Approach toward Hysteresis-Free Perovskite Solar Cell via Defect Engineering. , 2018, Journal of the American Chemical Society.

[13]  Y. Hao,et al.  Intermediate Phase Intermolecular Exchange Triggered Defect Elimination in CH3NH3PbI3 toward Room-Temperature Fabrication of Efficient Perovskite Solar Cells. , 2017, ACS applied materials & interfaces.

[14]  T. Hayat,et al.  Enhancing the crystallinity of HC(NH2)2PbI3 film by incorporating methylammonium halide intermediate for efficient and stable perovskite solar cells , 2017 .

[15]  Yongzhen Wu,et al.  Vertical recrystallization for highly efficient and stable formamidinium-based inverted-structure perovskite solar cells , 2017 .

[16]  K. Wong,et al.  Crystallinity Preservation and Ion Migration Suppression through Dual Ion Exchange Strategy for Stable Mixed Perovskite Solar Cells , 2017 .

[17]  Chunhui Huang,et al.  Mixed‐Organic‐Cation Tin Iodide for Lead‐Free Perovskite Solar Cells with an Efficiency of 8.12% , 2017, Advanced science.

[18]  M. Grätzel,et al.  Cation Dynamics in Mixed-Cation (MA)x(FA)1-xPbI3 Hybrid Perovskites from Solid-State NMR. , 2017, Journal of the American Chemical Society.

[19]  Bo Chen,et al.  Defect passivation in hybrid perovskite solar cells using quaternary ammonium halide anions and cations , 2017, Nature Energy.

[20]  G. Cui,et al.  Methylammonium-Mediated Evolution of Mixed-Organic-Cation Perovskite Thin Films: A Dynamic Composition-Tuning Process. , 2017, Angewandte Chemie.

[21]  Yasutaka Nagaoka,et al.  Synthesis of formamidinium lead halide perovskite nanocrystals through solid–liquid–solid cation exchange , 2017 .

[22]  Ying Liu,et al.  Pressure-Induced Polymorphic, Optical, and Electronic Transitions of Formamidinium Lead Iodide Perovskite. , 2017, The journal of physical chemistry letters.

[23]  M. Grätzel,et al.  Morphology Engineering: A Route to Highly Reproducible and High Efficiency Perovskite Solar Cells. , 2017, ChemSusChem.

[24]  Abdullah M. Asiri,et al.  Optimization of Stable Quasi-Cubic FAxMA1–xPbI3 Perovskite Structure for Solar Cells with Efficiency beyond 20% , 2017 .

[25]  Dongsheng Xu,et al.  Quantitative Doping of Chlorine in Formamidinium Lead Trihalide (FAPbI3−xClx) for Planar Heterojunction Perovskite Solar Cells , 2017 .

[26]  Qingsong Shan,et al.  50‐Fold EQE Improvement up to 6.27% of Solution‐Processed All‐Inorganic Perovskite CsPbBr3 QLEDs via Surface Ligand Density Control , 2017, Advanced materials.

[27]  S. Shaheen,et al.  Thermal engineering of FAPbI3 perovskite material via radiative thermal annealing and in situ XRD , 2017, Nature Communications.

[28]  J. Ball,et al.  Defects in perovskite-halides and their effects in solar cells , 2016, Nature Energy.

[29]  Yixin Zhao,et al.  Ion-Exchange-Induced 2D-3D Conversion of HMA1-x FAx PbI3 Cl Perovskite into a High-Quality MA1-x FAx PbI3 Perovskite. , 2016, Angewandte Chemie.

[30]  Haiying Zheng,et al.  Effective and reproducible method for preparing low defects perovskite film toward highly photoelectric properties with large fill factor by shaping capping layer , 2016 .

[31]  A. Herzing,et al.  Film morphology evolution during solvent vapor annealing of highly efficient small molecule donor/acceptor blends. , 2016, Journal of materials chemistry. A.

[32]  Yan Yao,et al.  Interaction of Organic Cation with Water Molecule in Perovskite MAPbI3: From Dynamic Orientational Disorder to Hydrogen Bonding , 2016 .

[33]  J. Teuscher,et al.  Unreacted PbI2 as a Double-Edged Sword for Enhancing the Performance of Perovskite Solar Cells. , 2016, Journal of the American Chemical Society.

[34]  Dong Hoe Kim,et al.  Facile fabrication of large-grain CH3NH3PbI3−xBrx films for high-efficiency solar cells via CH3NH3Br-selective Ostwald ripening , 2016, Nature Communications.

[35]  Ruixia Yang,et al.  Hysteresis‐Suppressed High‐Efficiency Flexible Perovskite Solar Cells Using Solid‐State Ionic‐Liquids for Effective Electron Transport , 2016, Advanced materials.

[36]  S. Pang,et al.  Exceptional Morphology-Preserving Evolution of Formamidinium Lead Triiodide Perovskite Thin Films via Organic-Cation Displacement. , 2016, Journal of the American Chemical Society.

[37]  G. Cui,et al.  The fabrication of formamidinium lead iodide perovskite thin films via organic cation exchange. , 2016, Chemical communications.

[38]  Xin Guo,et al.  Identification and characterization of the intermediate phase in hybrid organic-inorganic MAPbI3 perovskite. , 2016, Dalton transactions.

[39]  M. Green,et al.  Mobile Ion Induced Slow Carrier Dynamics in Organic-Inorganic Perovskite CH₃NH₃PbBr₃. , 2016, ACS applied materials & interfaces.

[40]  S. Meloni,et al.  Ionic polarization-induced current–voltage hysteresis in CH3NH3PbX3 perovskite solar cells , 2016, Nature Communications.

[41]  Jinsong Huang,et al.  Advances in Perovskite Solar Cells , 2016, Advanced science.

[42]  J. Berry,et al.  Stabilizing Perovskite Structures by Tuning Tolerance Factor: Formation of Formamidinium and Cesium Lead Iodide Solid-State Alloys , 2016 .

[43]  Jinsong Huang,et al.  Stabilized Wide Bandgap MAPbBrxI3–x Perovskite by Enhanced Grain Size and Improved Crystallinity , 2015, Advanced science.

[44]  Zhiqun Lin,et al.  Graphene‐Containing Nanomaterials for Lithium‐Ion Batteries , 2015 .

[45]  Yongzhen Wu,et al.  High‐Quality Mixed‐Organic‐Cation Perovskites from a Phase‐Pure Non‐stoichiometric Intermediate (FAI)1−x‐PbI2 for Solar Cells , 2015, Advanced materials.

[46]  Ziquan Guo,et al.  Defects dynamics during ageing cycles of InGaN blue light-emitting diodes revealed by evolution of external quantum efficiency--current dependence. , 2015, Optics express.

[47]  Sang Il Seok,et al.  High-performance photovoltaic perovskite layers fabricated through intramolecular exchange , 2015, Science.

[48]  Suneth C. Watthage,et al.  Impact of Processing Temperature and Composition on the Formation of Methylammonium Lead Iodide Perovskites , 2015 .

[49]  Jianbin Xu,et al.  Hybrid halide perovskite solar cell precursors: colloidal chemistry and coordination engineering behind device processing for high efficiency. , 2015, Journal of the American Chemical Society.

[50]  N. Zhao,et al.  HPbI3: A New Precursor Compound for Highly Efficient Solution‐Processed Perovskite Solar Cells , 2015 .

[51]  Sergei Tretiak,et al.  High-efficiency solution-processed perovskite solar cells with millimeter-scale grains , 2015, Science.

[52]  Young Chan Kim,et al.  Compositional engineering of perovskite materials for high-performance solar cells , 2015, Nature.

[53]  Anthony K. Cheetham,et al.  Solid-state principles applied to organic–inorganic perovskites: new tricks for an old dog , 2014 .

[54]  Sang Il Seok,et al.  Solvent engineering for high-performance inorganic-organic hybrid perovskite solar cells. , 2014, Nature materials.

[55]  Xinhong Zhou,et al.  One-step, solution-processed formamidinium lead trihalide (FAPbI(3-x)Cl(x)) for mesoscopic perovskite-polymer solar cells. , 2014, Physical chemistry chemical physics : PCCP.

[56]  M. Johnston,et al.  Formamidinium lead trihalide: a broadly tunable perovskite for efficient planar heterojunction solar cells , 2014 .

[57]  Laura M. Herz,et al.  Electron-Hole Diffusion Lengths Exceeding 1 Micrometer in an Organometal Trihalide Perovskite Absorber , 2013, Science.

[58]  R. Bube Trap Density Determination by Space‐Charge‐Limited Currents , 1962 .