The potential of Lu(3)N@C(80) and its analogues as electron acceptors in the areas of photovoltaics and artificial photosynthesis is tremendous. To this date, their electron-donating properties have never been explored, despite the facile oxidations that they reveal when compared to those of C(60). Herein, we report on the synthesis and physicochemical studies of a covalently linked Lu(3)N@C(80)-perylenebisimide (PDI) conjugate, in which PDI acts as the light harvester and the electron acceptor. Most important is the unambiguous evidence--in terms of spectroscopy and kinetics--that corroborates a photoinduced electron transfer evolving from the ground state of Lu(3)N@C(80) to the singlet excited state of PDI. In stark contrast, the photoreactivity of a C(60)-PDI conjugate is exclusively governed by a cascade of energy-transfer processes. Also, the electron-donating property of the Lu(3)N@C(80) moiety was confirmed through constructing and testing a bilayer heterojunction solar cell device with a PDI and Lu(3)N@C(80) derivative as electron acceptor and electron donor, respectively. In particular, a positive photovoltage of 0.46 V and a negative short circuit current density of 0.38 mA are observed with PDI/Ca as anode and ITO/Lu(3)N@C(80) as cathode. Although the devices were not optimized, the sign of the V(OC) and the flow direction of J(SC) clearly underline the unique oxidative role of Lu(3)N@C(80) within electron donor-acceptor conjugates toward the construction of novel optoelectronic devices. 相似文献
This study investigates the effect of high intensity focused ultrasound (HIFU) to muscle tissue transfected with a luciferase reporter gene under the control of a CMV-promoter. HIFU was applied to the transfected muscle tissue using a dual HIFU system. In a first group four different intensities (802 W/cm2, 1401 W/cm2, 2117 W/cm2, 3067 W/cm2) of continuous HIFU were applied 20 s every other week for four times. In a second group two different intensities (802 W/cm2, 1401 W/cm2) were applied 20 s every fourth day for 20 times. The luciferase activity was determined by bioluminescence imaging. The effect of HIFU to the muscle tissue was assessed by T1-weighted ± Gd-DTPA, T2-weighted and a diffusion-weighted STEAM sequence obtained on a 1.5-T GE-MRI scanner. Histology of the treated tissue was done at the end. In the first group the photon emission was at 3067.6 W/cm2 1.28 × 107 ± 3.1 × 106 photon/s (5.5 ± 1.2-fold), of 2157.9 W/cm2 8.1 ± 2.7 × 106 photon/s (3.2 ± 1.1-fold), of 1401.9 W/cm2 9.3 ± 1.3 × 106 photon/s (4.9 ± 0.4-fold) and of 802.0 W/cm2 8.6x ± 1.2 × 106 photon/s (4.5 ± 0.6-fold) compared to baseline. In the second group the photon emission was at 1401.9 W/cm2 and 802.0 W/cm2 14.1 ± 3.6 × 106 photon/s (6.1 ± 1.5-fold), respectively, 5.1 ± 4.7 × 106 photon/s (6.5 ± 2.0-fold). HIFU can enhance the luciferase activity controlled by a CMV-promoter. 相似文献
A new model for the excess Gibbs energy of aqueous solutions of polyelectrolytes is presented and applied for the correlation of the activity of water in aqueous solutions of polyelectrolytes without as well as with an added (single) salt. The model considers the phenomenon of counterion condensation, i.e., the partial dissociation of highly charged polyelectrolytes in water. Three parameters (a binary interaction parameter between polymer segments, the equilibrium constant of the dissociation reaction and a parameter which accounts for the polymer configuration) were fitted to the experimental results. The model allows for a reliable correlation of experimental results for the osmotic coefficient of aqueous solutions of a single polyelectrolyte (without as well as with an added salt). 相似文献
A combination of PFG-NMR imaging and velocity encoding methods was applied to investigate the dynamic behavior of a bed of poppy seeds subjected to air flow, representing a model setup for fluidized bed reactors. The particle motion is described both from a statistical point of view, by determining propagators and dispersion coefficients representing an average over the whole bed volume, as well as combined with spatial resolution by generating velocity maps. Velocity images of different horizontal slices in the bed confirm the notion of a toroidal particle flow pattern inside the shallow granular bed. Despite the need of considerable averaging due to the random motion of the relatively few particles in the bed, quantitative velocity images and statistical information about the random particle motion can be obtained from monitoring the fluid component in the seeds by conventional spin-echo techniques. 相似文献
The single‐step syngas‐to‐dimethyl ether (STD) process entails economic and technical advantages over the current industrial two‐step process. Pd/ZnO‐based catalysts have recently emerged as interesting alternatives to currently used Cu/ZnO/Al2O3 catalysts, but the nature of the active site(s), the reaction mechanism, and the role of Pd and ZnO in the solid catalyst are not well established. Now, Zn‐stabilized Pd colloids with a size of 2 nm served as the key building blocks for the methanol active component in bifunctional Pd/ZnO‐γ‐Al2O3 catalysts. The catalysts were characterized by combining high‐pressure operando X‐ray absorption spectroscopy and DFT calculations. The enhanced stability, longevity, and high dimethyl ether selectivity observed makes Pd/ZnO‐γ‐Al2O3 an effective alternative system for the STD process compared to Cu/ZnO/γ‐Al2O3. 相似文献
Single molecule spectroscopy was applied to study the optical properties of native and refolded peridinin-chlorophyll-protein (PCP) complexes. The native system is a trimer with six chlorophyll a (Chl a) molecules, while the refolded one contains two Chl a and resembles structurally and spectroscopically the PCP monomer. The fluorescence emission of single PCP complexes strongly broadens with increasing excitation power. Simultaneously, the distribution of fluorescence maximum frequencies is also broadened. These spectral changes are attributed to photoinduced conformational changes of the protein that influence the fluorescence of embedded chromophores. Comparison of fluorescence intensities measured for PCP complexes in two different solvents indicates that the native PCP trimers are preserved in EDTA Tris buffer, while in PVA polymer matrix only monomers are stable. 相似文献
Chlorine‐functionalized TEMPO‐capped polystyrenes were investigated using the matrix‐assisted laser desorption/ionization time‐of‐flight (MALDI‐TOF) technique. Amine‐ and acrylate‐functionalized agents and bifunctional TEMPO‐capped polystyrene were also analyzed to demonstrate the applicability of this method. Using this technique allowed to analyze the conversion of the chlorine function to an acrylate function, which was previously difficult to detect with other methods.
MALDI‐TOF mass spectrum of a polystyrene described in this article, as obtained with DHB as the matrix. 相似文献