Since Gratzel and co-workers developed a new type of solar cell based on the nanocrystalline $TiO_2$ electrode, dye-sensitized solar cells (DSSCs) have attracted considerable attention on account of their high solar energy-to-conversion efficiencies (11%), their easy manufacturing process with low cost production compared to conventional p-n junction solar cells. The mechanism of DSSC is based on the injection of electrons from the photoexcited dye into the conduction band of nanocrystalline $TiO_2$. The oxidized dye is reduced by the hole injection process from either the hole counter or electrolyte. Thus, the electronic structures, such as HOMO, LUMO, and HOMO-LUMO gap, of dye molecule in DSSC are deeply related to the electron transfer by photoexcitation and redox potential. To date, high performance and good stability of DSSC based on Ru-dyes as a photosensitizer had been widely addressed in the literatures. DSSC with Ru-bipyridyl complexes (N3 and N719), and the black ruthenium dye have achieved power conversion efficiencies up to 11.2% and 10.4%, respectively. However, the Ru-dyes are facing the problem of manufacturing costs and environmental issues. In order to obtain even cheaper photosensitizers for DSSC, metal-free organic photosensitizers are strongly desired. Metal-free organic dyes offer superior molar extinction coefficients, low cost, and a diversity of molecular structures, compared to conventional Ru-dyes. Recently, novel photosensitizers such as coumarin, merocyanine, cyanine, indoline, hemicyanine, triphenylamine, dialkylaniline, bis(dimethylfluorenyl)-aminophenyl, phenothiazine, tetrahydroquinoline, and carbazole based dyes have achieved solar-to-electrical power conversion efficiencies up to 5-9%. On the other hand, organic dye molecules have large ${\pi}$-conjugated planner structures which would bring out strong molecular stacking in their solid-state and poor solubility in their media. It was well known that the molecular stacking of organic dyes could reduce the electron transfer pathway in opto-electronic devices, significantly. In this paper, we have studied on synthesis and characterization of dendritic organic dyes with different number of electron acceptor/anchoring moieties in the end of dendrimer. The photovoltaic performances and the incident photon-to-current (IPCE) of these dyes were measured to evaluate the effects of the dendritic strucuture on the open-circuit voltage and the short-circuit current.
Kim, MyeongSeok;Cheon, Jong Hun;Jung, DaeYoung;Kim, JaeHong
한국신재생에너지학회:학술대회논문집
/
2011.05a
/
pp.117.2-117.2
/
2011
Since Gratzel and co-workers developed a new type of solar cell based on the nanocrystalline TiO2 electrode, dye-sensitized solar cells (DSSCs) have attracted considerable attention on account of their high solar energy-to-conversion efficiencies (11%), their easy manufacturing process with low cost production compared to conventional p-n junction solar cells. The mechanism of DSSC is based on the injection of electrons from the photoexcited dye into the conduction band of nanocrystalline TiO2. The oxidized dye is reduced by the hole injection process from either the hole counter or electrolyte. Thus, the electronic structures, such as HOMO, LUMO, and HOMO-LUMO gap, of dye molecule in DSSC are deeply related to the electron transfer by photoexcitation and redox potential. To date, high performance and good stability of DSSC based on Ru-dyes as a photosensitizer had been widely addressed in the literatures. DSSC with Ru-bipyridyl complexes (N3 and N719), and the black ruthenium dye have achieved power conversion efficiencies up to 11.2% and 10.4%, respectively. However, the Ru-dyes are facing the problem of manufacturing costs and environmental issues. In order to obtain even cheaper photosensitizers for DSSC, metal-free organic photosensitizers are strongly desired. Metal-free organic dyes offer superior molar extinction coefficients, low cost, and a diversity of molecular structures, compared to conventional Ru-dyes. Recently, novel photosensitizers such as coumarin, merocyanine, cyanine, indoline, hemicyanine, triphenylamine, dialkylaniline, bis(dimethylfluorenyl)-aminophenyl, phenothiazine, tetrahydroquinoline, and carbazole based dyes have achieved solar-to-electrical power conversion efficiencies up to 5-9%. On the other hand, organic dye molecules have large ${\pi}$-conjugated planner structures which would bring out strong molecular stacking in their solid-state and poor solubility in their media. It was well known that the molecular stacking of organic dyes could reduce the electron transfer pathway in opto-electronic devices, significantly. In this paper, we have studied on synthesis and characterization of dendritic organic dyes with different number of electron acceptor/anchoring moieties in the end of dendrimer. The photovoltaic performances and the incident photon-to-current (IPCE) of these dyes were measured to evaluate the effects of the dendritic strucuture on the open-circuit voltage and the short-circuit current.
Kim, Taeyoon;Kwon, Yongju;Kang, Choonghyun;Kim, Jongyoung;Shin, Hyun Suk;Kwon, Soonchul;Cha, Sung Min
Journal of Wetlands Research
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v.20
no.3
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pp.263-271
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2018
In this study, we analyzed the removal efficiency of ammonia nitrogen and phosphate dependant on the column depths using various absorbents such as zeolite silica sand, and activated carbon through the column test. In addition, we analyzed electrochemical adsorption behaviors of ammonia nitrogen and phosphate through the quantum mechanical calculation based on density functional theory calculation. Experimental results represent the removal efficiency of ammonia nitrogen and phosphate are zeolite > activated carbon > silica sand, and activated carbon > zeolite > silica sand, respectively. Zeolite shows high adsorption property for ammonia nitrogen over 90%, regardless of the column depth, while activated carbon exhibits high adsorption property for both ammonia nitrogen and phosphate as the column depth for filter media increases. Theoretical findings using DFT calculation for the adsorption behaviors of adsorbents (activated carbon and silica sand) and nutrients ($PO_4{^{3-}}$, $NH_4{^{+}}$) show that activated carbon represented narrower HOMO-LUMO band gap with high adsorption energy, and even more favorable environment for electron adsorption than silica sand, which leads to the effective removal of nutrients.
Within the framework of the density functional theory combined with the method of non-equilibrium Green's functions (DFT + NEGF), the features of electron transport in fullerene nanojunctions, which are «core-shell» nanoobjects made of a combination of fullerenes of different diameters C20, C80, C180, placed between gold electrodes (in a nanogap), are studied. Their transmission spectra, the density of state, current-voltage characteristics and differential conductivity are determined. It was shown that in the energy range of -0.45-0.45 eV in the transmission spectrum of the "Au-C180-Au" nanojunction appears a HOMO-LUMO gap with a width of 0.9 eV; when small-sized fullerenes C20, C80 are intercalation into the cavity C180 the gap disappears, and a series of resonant structures are observed on their spectra. It has been established that distinct Coulomb steps appear on the current-voltage characteristics of the "Au-C180-Au" nanojunction, but on the current-voltage characteristics "Au-C80@C180-Au", "Au-(C20@C80)@C180-Au" these step structures are blurred due to a decrease in Coulomb energy. An increase in the number of Coulomb features on the dI/dV spectra of core-shell fullerene nanojunctions was revealed in comparison with nanojunctions based on fullerene C60, which makes it possible to create high-speed single-electron devices on their basis. Models of single-electron transistors (SET) based on fullerene nanojunctions "Au-C180-Au", "Au-C80@C180-Au" and "Au-(C20@C80)@C180-Au" are considered. Their charge stability diagrams are analyzed and it is shown that SET based on C80@C180-, (C20@C80)@C180- nanojunctions is output from the Coulomb blockade mode with the lowest drain-to-source voltage.
A new donor-accepter-donor-accepter-donor (D-A-D-A-D) type 2,1,3-benzothiadiazole-thiophene-based acceptor unit 2,5-di(4-(5-bromo-4-octylthiophen-2-yl)-2,1,3-benzothiadiazol-7-yl)thiophene ($DTBTTBr_2$) was synthesized. Copolymerized with fluorene and indeno[1,2-b]fluorene electron-rich moieties, two alternating narrow band gap (NBG) copolymers PF-DTBTT and PIF-DTBTT were prepared. And two copolymers exhibit broad and strong absorption in the range of 300-700 nm with optical band gap of about 1.75 eV. The highest occupied molecular orbital (HOMO) energy levels vary between -5.43 and -5.52 eV and the lowest unoccupied molecular orbital (LUMO) energy levels range from -3.64 to -3.77 eV. Potential applications of the copolymers as electron donor material and $PC_{71}BM$ ([6,6]-phenyl-$C_{71}$ butyric acid methyl ester) as electron acceptors were investigated for photovoltaic solar cells (PSCs). Photovoltaic performances based on the blend of PF-DTBTT/$PC_{71}BM$ (w:w; 1:2) and PIF-DTBTT/$PC_{71}BM$ (w:w; 1:2) with devices configuration as ITO/PEDOT: PSS/blend/Ca/Al, show an incident photon-to-current conversion efficiency (IPCE) of 2.34% and 2.56% with the open circuit voltage ($V_{oc}$) of 0.87 V and 0.90 V, short circuit current density ($J_{sc}$) of $6.02mA/cm^2$ and $6.12mA/cm^2$ under an AM1.5 simulator ($100mA/cm^2$). The photocurrent responses exhibit the onset wavelength extending up to 720 nm. These results indicate that the resulted narrow band gap copolymers are viable electron donor materials for polymer solar cells.
A quantum-chemical investigation on the conformations and electronic properties of bis[2-{2-methoxy-4,6-di(t-butyl)phenyl}ethenyl]benzenes (MBPBs) as building block for ${\pi}$-conjugate polymer are performed in order to display the effects of t-butyl and methoxy group substitution and of kink(ortho and meta) linkage. The conjugation length of the polymers can be controlled by substituents and kink linkages of backbone. Structures for the molecules, o-, m-, and p-MBPBs as well as unsubstituted o-, m-, and p-DSBs were fully optimized by using semiempirical AM1, PM3 methods, and ab initio HF method with 3-21G(d) basis set. The potential energy curves with respect to the change of single torsion angle are obtained by using semiempirical methods and ab initio HF/3-21G(d) basis set. The curves are similar shape in the molecules with respect to the position of vinylene groups. It is shown that the conformations of the molecules are compromised between the steric repulsion interaction and the degree of the conjugation. Electronic properties of the molecules were obtained by applying the optimized structures and geometries to the ZINDO/S method. ZINDO/S analysis performed on the geometries obtained by AM1 method and HF/3-21G(d) level is reported. The absorption wavelength on the geometries obtained by AM1 method is much longer than that by HF/3-21G(d) level. The absorption wavelength of MBPBs are red shifted with comparison to that of corresponding DSBs in the same torsion angle because of electron donating substituents. The absorption wavelength of isomers with kink(orth and meta) linkage is shorter than that of para linkage.
Nguyen, Thanh Nhan;Nguyen, Hoang Phuc;Kim, Tae-Ho;Lee, Soo Wohn
Korean Journal of Materials Research
/
v.28
no.1
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pp.68-74
/
2018
Cobalt-incorporated zeolitic imidazolate framework ZIF-8 was synthesized by a simple one-pot synthesis method at room temperature. Powder X-ray diffraction patterns and energy dispersive X-ray spectrum confirmed the formation of the bimetallic Co/Zn-ZIF structure. UV-Vis diffuse reflectance spectra revealed that the bimetallic ZIF had a lower HOMO-LUMO gap compared with ZIF-8 due to the charge transfer process from organic ligands to cobalt centers. A hydrolytic stability test showed that Co/Zn-ZIF is very robust in aqueous solution - the most important criterion for any material to be applied in photodegradation. The photocatalytic efficiency of the synthesized samples was investigated over the Indigo Carmine (IC) dye degradation under solar simulated irradiation. Cobalt incorporated ZIF-8 exhibited high efficiency over a wide range of pH and initial concentration. The degradation followed through three distinct stages: a slow initial stage, followed by an accelerated stage and completed with a decelerated stage. Moreover, the photocatalytic performance of the synthesized samples was highly improved in alkaline environment rather than in acidic or neutral environments, which may have been because in high pH medium, the increased concentration of hydroxyl ion facilitated the formation of hydroxyl radicals, a reactive species responsible for the breaking of the Indigo Carmine structure. Thus, Co/Zn-ZIF is a promising and green material for solving the environmental pollution caused by textile industries.
In this article, we have designed and synthesized a novel donor-${\pi}$-acceptor (D-${\pi}$-A) type porphyrin-based sensitizer (denoted UI-5), in which a carboxyl anchoring group and a 9,9-dimethyl fluorene were introduced at the meso-positions of porphyrin ring via phenylethynyl and ethynyl bridging units, respectively. Long alkoxy chains in ortho-positions of the phenyls were supposed to reduce the degree of dye aggregation, which tends to affect electron injection yield in a photovoltaic cell. The cyclic voltammetry was employed to determine the band gap of UI-5 to be 1.41 eV based on the HOMO and LUMO energy levels, which were estimated by the onset oxidation and reduction potentials. The incident monochromatic photon-to-current conversion efficiency of the UI-5 DSSC assembled with double-layer (20 nm-sized $TiO_2$/400 nm-sized $TiO_2$) film electrodes appeared lower upon overall ranges of the excitation wavelengths, but exhibited a higher value over the NIR ranges (${\lambda}$ = 650-700 nm) compared to the common reference sensitizer N719. The UI-5-sensitized cell yielded a relatively poor device performance with an overall conversion efficiency of 0.74% with a short circuit photocurrent density of $3.05mA/cm^2$, an open circuit voltage of 0.54 mV and a fill factor of 0.44 under the standard global air mass (AM 1.5) solar conditions. However, our report about the synthesis and the photovoltaic characteristics of a porphyrin-based sensitizer in a D-${\pi}$-A structure demonstrated a significant complex relationship between the sensitizer structure and the cell performance.
In this paper, for the first time, the electroanalytical study of Triethylenediamine, TEDA was done on a typically graphene modified carbon paste electrode (Gr/CPE) in pH=10.5 of phosphate buffer solutions (PBS). The surface morphology of the bare and modified electrodes was characterized by scanning electron microscopy (SEM), electrochemical impedance spectroscopy (EIS) and cyclic voltammetry (CV). The electro-oxidation of TEDA was investigated at the surface of modified electrode. The results revealed that the oxidation peak current of TEDA at the surface of Gr/CPE is 2.70 times than that shown at bare-CPE. A linear calibration plot was observed in the range of 1.0 to 202.0 ppm. In this way, the detection limit was found to be 0.18 ppm. The method was then successfully applied to determination of TEDA in aqueous samples obtained from two kinds of activated carbon from the masks of war. On the other hand, density functional theory (DFT) method at B3LYP/6-311++G** level of theory and a conductor-like Polarizable Continuum Model (CPCM) was used to calculate the $pK_a$ values of TEDA. The energies of lowest unoccupied molecular orbital ($E_{LUMO}$) and highest occupied molecular orbital ($E_{HOMO}$), gap energy (${\Delta}E$) and some thermodynamic parameters such as Gibbs free energy of TEDA and its conjugate acid ($HT^+$) were calculated. The results of calculated $pK_a$ were found to be in good agreement with the experimental values.
Shin, Woong;Park, Jeong Bae;Park, Sang Jun;Jo, Mi Young;Suh, Hongsuk;Kim, Joo Hyun
Applied Chemistry for Engineering
/
v.22
no.1
/
pp.15-20
/
2011
Poly[2,3-dimethyl-5,8-dithiophene-2-yl-quinoxaline-alt-9,9-dihexyl-9H-fluorene] (PFTQT) and poly[2,3-dimethyl-5,8-dithiophen-2-yl-quinoxaline-alt-10-hexyl-10H-phenothiazine (PPTTQT) based on 2,3-dimethyl-5,8-dithiophen-2-yl-quinoxaline weresynthesized by Suzuki coupling reaction. All polymers were soluble in common organic solvents such as chloroform, chlorobenzene, o-dichlorobenzene, tetrahydrofuran (THF) and toluene. The maximum absorption wavelength and band gap of PFTQT were 440 nm and 2.30 eV, and PPTTQT were 445 nm and 2.23 eV, respectively. The HOMO and LUMO energy level of PFTQT were -6.05 and -3.75 eV, and PPTTQT were -5,89 and -3.66 eV, respectively. The organic photovoltaic devices based on the blend of polymer and PCBM (1 : 2 by weight ratio) were fabricated. Efficiencies of devices were 0.24% (PFTQT) and 0.16% (PPTTQT), respectively. The short circuit current density ($J_{sc}$), fill factor (FF), and open circuit voltage ($V_{oc}$) of the device with PFTQT were $0.97mA/cm^2$, 29% and 0.86 V, and the device based on PPTTQT were $0.80mA/cm^2$, 28% and 0.71 V, 31% and 0.71 V, respectively, under air mass (AM) 1.5 G and 1 sun condition ($100mA/cm^2$).
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