Jae-Yup Kim

Completely Transparent Conducting Oxide-Free and Flexible Dye-Sensitized Solar Cells Fabricated on Plastic Substrates

To achieve commercialization and widespread application of next-generation photovoltaics, it is important to develop flexible and cost-effective devices. Given this, the elimination of expensive transparent conducting oxides (TCO) and replacement of conventional glass substrates with flexible plastic substrates presents a viable strategy to realize extremely low-cost photovoltaics with a potentially wide applicability. To this end, we report a completely TCO-free and flexible dye-sensitized solar cell (DSSC) fabricated on a plastic substrate using a unique transfer method and back-contact architecture. By adopting unique transfer techniques, the working and counter electrodes were fabricated by transferring high-temperature-annealed TiO2 and Pt/carbon films, respectively, onto flexible plastic substrates without any exfoliation. The fabricated working electrode with the conventional counter electrode exhibited a record efficiency for flexible DSSCs of 8.10%, despite its TCO-free structure. In addition, the completely TCO-free and flexible DSSC exhibited a remarkable efficiency of 7.27%. Furthermore, by using an organic hole-transporting material (spiro-MeOTAD) with the same transfer method, solid-state flexible TCO-free DSSCs were also successfully fabricated, yielding a promising efficiency of 3.36%.

Novel D-π-A Organic Dyes with Thieno[3,2-b]thiophene-3,4-ethylenedioxythiophene Unit as a π-Bridge for Highly Efficient Dye-Sensitized Solar Cells with Long-Term Stability

This paper reports on new D-π-A organic dyes for application in dye-sensitized solar cells (DSSCs), which were developed by incorporating thieno[3,2-b]thiophene-thiophene (M9) and thieno[3,2-b]thiophene-EDOT (M10) as π-bridges. These dyes exhibited relatively small highest occupied molecular orbital (HOMO)-lowest unoccupied molecular orbital (LUMO) energy gaps in spite of the short π-conjugation lengths, resulting in broad spectral responses. As photosensitizers in DSSCs, M10 showed a broader spectral response than M9, leading to a greater short-circuit photocurrent (Jsc). In addition, M10 exhibited higher open-circuit voltage (Voc) compared to M9, because of the greater electron lifetime of the photoanode. The impedance analysis revealed that the greater electron lifetime of the photoanode with M10 was attributed to the lower electron recombination rate caused by the blocking effect of the bulky EDOT unit. As a result, M10 showed much higher conversion efficiency (η = 7.00%) than M9 (η = 5.67%) under one sun condition (AM 1.5 G, 100 mW/cm(2)). This conversion efficiency was comparable to that of the conventional Ru-based dye N719 (η = 7.24%) under the same condition. In addition, M10 exhibited a remarkable long-term stability, i.e., 95% of the initial conversion efficiency was maintained after light soaking for 45 days (1080 h).

Highly ordered and vertically oriented TiO2/Al2O3 nanotube electrodes for application in dye-sensitized solar cells

The surface of long TiO2 nanotube (NT) electrodes in dye-sensitized solar cells (DSSCs) was modified without post-annealing by using atomic layer deposition (ALD) for the enhancement of photovoltage. Vertically oriented TiO2 NT electrodes with highly ordered and crack-free surface structures over large areas were prepared by a two-step anodization method. The prepared TiO2 NTs had a pore size of 80 nm, and a length of 23 μm. Onto these TiO2 NTs, an Al2O3 shell of a precisely controlled thickness was deposited by ALD. The conformally coated shell layer was confirmed by high-resolution transmission electron microscopy, energy-dispersive x-ray spectroscopy, and x-ray photoelectron spectroscopy. The open-circuit voltage (V(oc)) of the DSSCs was gradually enhanced as the thickness of the Al2O3 shell of the TiO2/Al2O3 NT electrodes was increased, which resulted from the enhanced electron lifetime. The enhanced electron lifetime caused by the energy barrier effect of the shell layer was measured quantitatively by the open-circuit voltage decay technique. As a result, 1- and 2-cycle-coated samples showed enhanced conversion efficiencies compared to the bare sample.

Rapid Dye Adsorption via Surface Modification of TiO2 Photoanodes for Dye-Sensitized Solar Cells

A facile method for increasing the reaction rate of dye adsorption, which is the most time-consuming step in the production of dye-sensitized solar cells (DSSCs), was developed. Treatment of a TiO2 photoanode with aqueous nitric acid solution (pH 1) remarkably reduced the reaction time required to anchor a carboxylate anion of the dye onto the TiO2 nanoparticle surface. After optimization of the reaction conditions, the dye adsorption process became 18 times faster than that of the conventional adsorption method. We studied the influence of the nitric acid treatment on the properties of TiO2 nanostructures, binding modes of the dye, and adsorption kinetics, and found that the reaction rate improved via the synergistic effects of the following: (1) electrostatic attraction between the positively charged TiO2 surface and ruthenium anion increases the collision frequency between the adsorbent and the anchoring group of the dye; (2) the weak anchoring affinity of NO3(-) in nitric acid with metal oxides enables the rapid coordination of an anionic dye with the metal oxide; and (3) sufficient acidity of the nitric acid solution effectively increases the positive charge density on the TiO2 surface without degrading or transforming the TiO2 nanostructure. These results demonstrate the developed method is effective for reducing the overall fabrication time without sacrificing the performance and long-term stability of DSSCs.

Tailoring of Energy Levels in D- π -A Organic Dyes via Fluorination of Acceptor Units for Efficient Dye-Sensitized Solar Cells

A molecular design is presented for tailoring the energy levels in D-π-A organic dyes through fluorination of their acceptor units, which is aimed at achieving efficient dye-sensitized solar cells (DSSCs). This is achieved by exploiting the chemical structure of common D-π-A organic dyes and incorporating one or two fluorine atoms at the ortho-positions of the cyanoacetic acid as additional acceptor units. As the number of incorporated fluorine atoms increases, the LUMO energy level of the organic dye is gradually lowered due to the electron-withdrawing effect of fluorine, which ultimately results in a gradual reduction of the HOMO-LUMO energy gap and an improvement in the spectral response. Systematic investigation of the effects of incorporating fluorine on the photovoltaic properties of DSSCs reveals an upshift in the conduction-band potential of the TiO2 electrode during impedance analysis; however, the incorporation of fluorine also results in an increased electron recombination rate, leading to a decrease in the open-circuit voltage (Voc). Despite this limitation, the conversion efficiency is gradually enhanced as the number of incorporated fluorine atoms is increased, which is attributed to the highly improved spectral response and photocurrent.