Dong Hoe Kim

Highly efficient and bending durable perovskite solar cells: toward a wearable power source

Perovskite solar cells are promising candidates for realizing an efficient, flexible, and lightweight energy supply system for wearable electronic devices. For flexible perovskite solar cells, achieving high power conversion efficiency (PCE) while using a low-temperature technology for the fabrication of a compact charge collection layer is a critical issue. Herein, we report on a flexible perovskite solar cell exhibiting 12.2% PCE as a result of the employment of an annealing-free, 20 nm thick, amorphous, compact TiOx layer deposited by atomic layer deposition. The excellent performance of the cell was attributed to fast electron transport, verified by time-resolved photoluminescence and impedance studies. The PCE remained the same down to 0.4 sun illumination, as well as to a 45° tilt to incident light. Mechanical bending of the devices worsened device performance by only 7% when a bending radius of 1 mm was used. The devices maintained 95% of the initial PCE after 1000 bending cycles for a bending radius of 10 mm. Degradation of the device performance by the bending was the result of crack formation from the transparent conducting oxide layer, demonstrating the potential of the low-temperature-processed TiOx layer to achieve more efficient and bendable perovskite solar cells, which becomes closer to a practical wearable power source.

Facile fabrication of large-grain CH3NH3PbI3-xBrx films for high-efficiency solar cells via CH3NH3Br-selective Ostwald ripening

Organometallic halide perovskite solar cells (PSCs) have shown great promise as a low-cost, high-efficiency photovoltaic technology. Structural and electro-optical properties of the perovskite absorber layer are most critical to device operation characteristics. Here we present a facile fabrication of high-efficiency PSCs based on compact, large-grain, pinhole-free CH3NH3PbI3−xBrx (MAPbI3−xBrx) thin films with high reproducibility. A simple methylammonium bromide (MABr) treatment via spin-coating with a proper MABr concentration converts MAPbI3 thin films with different initial film qualities (for example, grain size and pinholes) to high-quality MAPbI3−xBrx thin films following an Ostwald ripening process, which is strongly affected by MABr concentration and is ineffective when replacing MABr with methylammonium iodide. A higher MABr concentration enhances I–Br anion exchange reaction, yielding poorer device performance. This MABr-selective Ostwald ripening process improves cell efficiency but also enhances device stability and thus represents a simple, promising strategy for further improving PSC performance with higher reproducibility and reliability.

Retarding charge recombination in perovskite solar cells using ultrathin MgO-coated TiO2 nanoparticulate films

MgO-coated TiO2 nanoparticle (NP)-based electron collecting layers were fabricated to prevent charge recombination at the methylamine lead iodide/TiO2 interface in perovskite solar cells. The open circuit voltage (Voc) and fill factor (ff) of perovskite solar cells based on MgO-coated TiO2 charge collectors were 0.89 V and 71.2%, respectively. These values were 4.7% and 6.1% higher than the pure TiO2 based perovskite solar cells. Transient photovoltage decay data exhibited recombination times for MgO-coated TiO2 NP-based perovskite solar cells about three times longer than those of TiO2 NP based solar cells. The longer recombination time was responsible for enhancing the Voc and ff of MgO-coated TiO2 NP-based perovskite solar cells. By employing a MgO nanolayer, we observed that the power conversion efficiency (PCE) was increased from 11.4% to 12.7%, demonstrating that MgO ultrathin nanolayers are able to efficiently retard charge recombination in perovskite solar cells.

Niobium Doping Effects on TiO2 Mesoscopic Electron Transport Layer-Based Perovskite Solar Cells.

Perovskite solar cells (PSCs) are the most promising candidates as next-generation solar energy conversion systems. To design a highly efficient PSC, understanding electronic properties of mesoporous metal oxides is essential. Herein, we explore the effect of Nb doping of TiO2 on electronic structure and photovoltaic properties of PSCs. Light Nb doping (0.5 and 1.0 at %) increased the optical band gap slightly, but heavy doping (5.0 at %) distinctively decreased it. The relative Fermi level position of the conduction band is similar for the lightly Nb-doped TiO2 (NTO) and the undoped TiO2 whereas that of the heavy doped NTO decreased by as much as ∼0.3 eV. The lightly doped NTO-based PSCs exhibit 10 % higher efficiency than PSCs based on undoped TiO2 (from 12.2 % to 13.4 %) and 52 % higher than the PSCs utilizing heavy doped NTO (from 8.8 % to 13.4 %), which is attributed to fast electron injection/transport and preserved electron lifetime, verified by transient photocurrent decay and impedance studies.

Crystallographically preferred oriented TiO2 nanotube arrays for efficient photovoltaic energy conversion

We describe the fabrication of crystallographically preferred oriented TiO2 anatase nanotube arrays (p-NTAs) and the characterization of their photovoltaic properties. The preferred orientation to the (004) plane of the TiO2 nanotube array (NTA) was carefully controlled by adjusting the water content in the anodizing electrolyte; ∼2 wt% of water yielded a p-NTA, whereas other contents of water yielded randomly oriented NTAs (r-NTAs). A structural analysis using X-ray diffraction and a high-resolution transmission electron microscope revealed that the p-NTA showed a preferred orientation along the [001] direction of the anatase crystal structure. When the NTAs were employed to dye-sensitized solar cells (DSSCs) as photoelectrodes, the p-NTA showed a similar electron lifetime to the r-NTA, which was an order of magnitude higher than that for a TiO2 nanoparticle (NP) film. Moreover, the p-NTA exhibited faster electron transport than the NP film, and even faster than the r-NTA. These properties resulted in a longer electron diffusion length of the p-NTA, compared to the r-NTA and NP film, thereby improving the charge collection property of the photoelectrode. The p-NTA exhibited superior photovoltaic energy conversion performance in the DSSC system, and showed a higher thickness for the optimal photovoltaic performance compared to the NP film, which were attributed to the excellent charge collection properties. Our results address that the crystallographic orientation of NTAs improves their charge transport properties, which can be applied to various optoelectronics, especially to solar-driven energy conversion devices.

Extrinsic ion migration in perovskite solar cells

The migration of intrinsic ions (e.g., MA+, Pb2+, I−) in organic–inorganic hybrid perovskites has received significant attention with respect to the critical roles of these ions in the hysteresis and degradation in perovskite solar cells (PSCs). Here, we demonstrate that extrinsic ions (e.g., Li+, H+, Na+), when used in the contact layers in PSCs, can migrate across the perovskite layer and strongly impact PSC operation. In a TiO2/perovskite/spiro-OMeTAD-based PSC, Li+-ion migration from spiro-OMeTAD to the perovskite and TiO2 layer is illustrated by time-of-flight secondary-ion mass spectrometry. The movement of Li+ ions in PSCs plays an important role in modulating the solar cell performance, tuning TiO2 carrier-extraction properties, and affecting hysteresis in PSCs. The influence of Li+-ion migration was investigated using time-resolved photoluminescence, Kelvin probe force microscopy, and external quantum efficiency spectra. Other extrinsic ions such as H+ and Na+ also show a clear impact on the performance and hysteresis in PSCs. Understanding the impacts of extrinsic ions in perovskite-based devices could lead to new material and device designs to further advance perovskite technology for various applications.

BaSnO3 perovskite nanoparticles for high efficiency dye-sensitized solar cells.

The synthesis of highly crystalline perovskite BaSnO3 nanoparticles for use as photoanode materials in dye-sensitized solar cells (DSSCs) is reported, and the photovoltaic properties of DSSCs based on BaSnO3 nanoparticles (BaSnO3 cells) are demonstrated. The resulting DSSCs exhibit remarkably rapid charge collection and a DSSC fabricated with a BaSnO3 film thickness of 43 µm leads to a high energy conversion efficiency of 5.2 %, which is one of the highest reported for ternary oxide-based DSSCs. More importantly, the BaSnO3 cells show superior charge collection in nanoparticle films compared to TiO2 cells and could offer a breakthrough in the efficiencies of DSSCs.

300% Enhancement of Carrier Mobility in Uniaxial-Oriented Perovskite Films Formed by Topotactic-Oriented Attachment

Organic-inorganic perovskites with intriguing optical and electrical properties have attracted significant research interests due to their excellent performance in optoelectronic devices. Recent efforts on preparing uniform and large-grain polycrystalline perovskite films have led to enhanced carrier lifetime up to several microseconds. However, the mobility and trap densities of polycrystalline perovskite films are still significantly behind their single-crystal counterparts. Here, a facile topotactic-oriented attachment (TOA) process to grow highly oriented perovskite films, featuring strong uniaxial-crystallographic texture, micrometer-grain morphology, high crystallinity, low trap density (≈4 × 1014 cm-3 ), and unprecedented 9 GHz charge-carrier mobility (71 cm2 V-1 s-1 ), is demonstrated. TOA-perovskite-based n-i-p planar solar cells show minimal discrepancies between stabilized efficiency (19.0%) and reverse-scan efficiency (19.7%). The TOA process is also applicable for growing other state-of-the-art perovskite alloys, including triple-cation and mixed-halide perovskites.

Selective dissolution of halide perovskites as a step towards recycling solar cells

Most research on perovskite solar cells has focused on improving power-conversion efficiency and stability. However, if one could refurbish perovskite solar cells, their stability might not be a critical issue. From the perspective of cost effectiveness, if failed, perovskite solar cells could be collected and recycled; reuse of their gold electrodes and transparent conducting glasses could reduce the price per watt of perovskite photovoltaic modules. Herein, we present a simple and effective method for removing the perovskite layer and reusing the mesoporous TiO2-coated transparent conducting glass substrate via selective dissolution. We find that the perovskite layer can be easily decomposed in polar aprotic solvents because of the reaction between polar aprotic solvents and Pb2+ cations. After 10 cycles of recycling, a mesoporous TiO2-coated transparent conducting glass substrate-based perovskite solar cell still shows a constant power-conversion efficiency, thereby demonstrating the possibility of recycling perovskite solar cells.

1-D structured flexible supercapacitor electrodes with prominent electronic/ionic transport capabilities.

A highly efficient 1-D flexible supercapacitor with a stainless steel mesh (SSM) substrate is demonstrated. Indium tin oxide (ITO) nanowires are prepared on the surface of the stainless steel fiber (SSF), and MnO2 shell layers are coated onto the ITO/SSM electrode by means of electrodeposition. The ITO NWs, which grow radially on the SSF, are single-crystalline and conductive enough for use as a current collector for MnO2-based supercapacitors. A flake-shaped, nanoporous, and uniform MnO2 shell layer with a thickness of ~130 nm and an average crystallite size of ~2 nm is obtained by electrodeposition at a constant voltage. The effect of the electrode geometry on the supercapacitor properties was investigated using electrochemical impedance spectroscopy, cyclic voltammetry, and a galvanostatic charge/discharge study. The electrodes with ITO NWs exhibit higher specific capacitance levels and good rate capability owing to the superior electronic/ionic transport capabilities resulting from the open pore structure. Moreover, the use of a porous mesh substrate (SSM) increases the specific capacitance to 667 F g(-1) at 5 mV s(-1). In addition, the electrode with ITO NWs and the SSM shows very stable cycle performance (no decrease in the specific capacitance after 5000 cycles).