A new solution-processable fabrication protocol using a soluble tetrabenzoporphyrin (BP) precursor and bis(dimethylphenylsilylmethyl)[60]fullerene (SIMEF) created three-layered p-i-n photovoltaic devices, in which the i-layer possesses a well-defined bulk heterojunction structure in which columnar BP crystals grow vertically from the bottom p-layer. The device showed a power conversion efficiency of 5.2% (V(OC) = 0.75 V; J(SC) = 10.5 mA/cm(2); FF = 0.65).
Despite tremendous progress in optoelectronic devices using lead perovskite (CH3NH3(+)PbI3(-)), there has been a paucity of mechanistic information on how photoactive micron-sized crystals of lead perovskite grow from a mixture of a layered crystal of lead(II) iodide and methylammonium iodide mediated by a polar solvent, DMSO or DMF. We report here that the whole process of the lead perovskite synthesis consists of a series of equilibria driven by reversible solvent participation involving a polymeric strip of plumbate(II) oligomer as a key intermediate. A significant finding includes quick decomposition of perovskite crystal upon exposure to DMSO or DMF at room temperature, where the solvent molecules act as a base to remove acidic ammonium iodide from the perovskite crystal. This observation accounts for the difficulty in controlling perovskite solar cell fabrication. Overall, the polar solvent is indispensible first to degrade a 2-D sheet of crystals of lead(II) iodide into 1-D fibrous intermediates and then to promote Oswald ripening of perovskite crystals. The detailed chemical information provided here will help to rationalize the photovoltaic device studies that have so far remained empirical and to open a new venue to a developing field of microscale lead perovskite devices, as illustrated by fabrication of photovoltaic devices and photodetectors.
Polar liquid crystalline materials can be used in optical and electronic applications, and recent interest has turned to formation strategies that exploit the shape of polar molecules and their interactions to direct molecular alignment. For example, banana-shaped molecules align their molecular bent within smectic layers, whereas conical molecules should form polar columnar assemblies. However, the flatness of the conical molecules used until now and their ability to flip have limited the success of this approach to making polar liquid crystalline materials. Here we show that the attachment of five aromatic groups to one pentagon of a C(60) fullerene molecule yields deeply conical molecules that stack into polar columnar assemblies. The stacking is driven by attractive interactions between the spherical fullerene moiety and the hollow cone formed by the five aromatic side groups of a neighbouring molecule in the same column. This packing pattern is maintained when we extend the aromatic groups by attaching flexible aliphatic chains, which yields compounds with thermotropic and lyotropic liquid crystalline properties. In contrast, the previously reported fullerene-containing liquid crystals all exhibit thermotropic properties only, and none of them contains the fullerene moiety as a functional part of its mesogen units. Our design strategy should be applicable to other molecules and yield a range of new polar liquid crystalline materials.
Contents 1. Introduction 3016 2. Multiple Addition of the Organocopper Reagents to [60]Fullerene 3017 2.1. Penta-Additions of Aryl Groups 3017 2.1.1. The Reaction, Its Synthetic Scope, and the Utility of the Products 3017 2.1.2. Penta(hydroxyphenyl)[60]fullerenes 3020 2.1.3. Penta(mercaptophenyl)[60]fullerenes 3020 2.2. Penta-Additions of Alkyl Groups 3021 2.2.1. Penta(methyl)[60]fullerenes 3021 2.2.2. Penta(silylmethyl)[60]fullerenes 3022 2.3. Additions of Functionalized Organocopper Reagents 3023 2.3.1. Synthesis Using Organocopper Reagents with Mg/I Exchange 3023 2.3.2. Organocopper Reagents from the Reformatsky Reagent 3023 2.3.3. Addition of 2-Tetrahydrofuranyl Groups by C-H Bond Activation 3024 2.4. Octa-and Deca-Additions 3024 2.5. Additions to [60]Fullerene Derivatives 3026 3. Tri-Addition of the Organocopper Reagents to [70]Fullerene 3026 4. Concluding Remarks 3027 5. Acknowledgments 3027 6. References 3027
[structure: see text] Depending on the exact length of the tube, the chemical structure of finite-length armchair [n,n] single-wall carbon nanotube (n = 5 and 6) falls into three different classes that may be referred to as Kekulé, incomplete Clar, and complete Clar networks. The C-C bond lengths, nucleus-independent chemical shift analysis, and orbital energies suggest that the chemical reactivities of the finite-length tube change periodically as the tube length is elongated by one-by-one layering of cyclic carbon array.
Transparent carbon electrodes, carbon nanotubes, and graphene were used as the bottom electrode in flexible inverted perovskite solar cells. Their photovoltaic performance and mechanical resilience were compared and analyzed using various techniques. Whereas a conventional inverted perovskite solar cells using indium tin oxide showed a power conversion efficiency of 17.8%, the carbon nanotube- and graphene-based cells showed efficiencies of 12.8% and 14.2%, respectively. An established MoO doping was used for carbon electrode-based devices. The difference in the photovoltaic performance between the carbon nanotube- and graphene-based cells was due to the difference in morphology and transmittance. Raman spectroscopy, and cyclic flexural testing revealed that the graphene-based cells were more susceptible to strain than the carbon nanotube-based cells, though the difference was marginal. Overall, despite higher performance, the transfer step for graphene has lower reproducibility. Thus, the development of better graphene transfer methods would help maximize the current capacity of graphene-based cells.
In this work, both anode and cathode interfaces of p‐i‐n CH3NH3PbI3 perovskite solar cells (PVSCs) are simultaneously modified to achieve large open‐circuit voltage (Voc) and fill factor (FF) for high performance semitransparent PVSCs (ST‐PVSCs). At the anode, modified NiO serves as an efficient hole transport layer with appropriate surface property to promote the formation of smooth perovskite film with high coverage. At the cathode, a fullerene bisadduct, C60(CH2)(Ind), with a shallow lowest unoccupied molecular orbital level, is introduced to replace the commonly used phenyl‐C61‐butyric acid methyl ester (PCBM) as an alternative electron transport layer in PVSCs for better energy level matching with the conduction band of the perovskite layer. Therefore, the Voc, FF and power conversion efficiency (PCE) of the PVSCs increase from 1.05 V, 0.74 and 16.2% to 1.13 V, 0.80 and 18.1% when the PCBM is replaced by C60(CH2)(Ind). With the advantages of high Voc and FF, ST‐PVSCs are also fabricated using an ultrathin transparent Ag as cathode, showing an encouraging PCEs of 12.6% with corresponding average visible transmittance (AVT) over 20%. These are the highest PCEs reported for ST‐PVSCs with similar AVTs paving the way for using ST‐PVSCs as power generating windows.
PSS as an electron-blocking layer on SWNTs in perovskite SCs due to superior wettability, whereas MoO3 is not compatible owing to energy level mismatching. Diluted HNO3 (35 v/v%)-doped SWNT-based device produced the highest PCE of 6.32% among SWNT-based perovskite SCs, which is 70% of an indium tin oxide (ITO)-based device (9.05%). Its flexible application showed a PCE of 5.38% on polyethylene terephthalate (PET) substrate.
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