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31.
Mechanism of Back Electron Transfer in an Intermolecular Photoinduced Electron Transfer Reaction: Solvent as a Charge Mediator
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Sudhakar Narra Dr. Yoshifumi Nishimura Prof. Dr. Henryk A. Witek Prof. Dr. Shinsuke Shigeto 《Chemphyschem》2014,15(14):2945-2950
Back electron transfer (BET) is one of the important processes that govern the decay of generated ion pairs in intermolecular photoinduced electron transfer reactions. Unfortunately, a detailed mechanism of BET reactions remains largely unknown in spite of their importance for the development of molecular photovoltaic structures. Here, we examine the BET reaction of pyrene (Py) and 1,4‐dicyanobenzene (DCB) in acetonitrile (ACN) by using time‐resolved near‐ and mid‐IR spectroscopy. The Py dimer radical cation (Py2.+) and DCB radical anion (DCB.?) generated after photoexcitation of Py show asynchronous decay kinetics. To account for this observation, we propose a reaction mechanism that involves electron transfer from DCB.? to the solvent and charge recombination between the resulting ACN dimer anion and Py2.+. The unique role of ACN as a charge mediator revealed herein could have implications for strategies that retard charge recombination in dye‐sensitized solar cells. 相似文献
32.
Archana Chaudhary Nikita Sharma Meena Nagar Shaikh M. Mobin Pradeep Mathur Rakesh Bohra 《Journal of Sol-Gel Science and Technology》2014,70(3):464-472
Modification of [VO(OPri)3] with oximes in different molar ratios, yielded new class of vanadia precursors, [VO{OPri}3?n{L}n] {where, n = 1–3 and LH = C9H16C=NOH (1–3) and (CH3)2C=NOH (4–6)}.All the products are yellow in colour. (1) and (2) are liquid/viscous liquid, while others are solids. Molecular weight measurements of all these derivatives and the ESI-mass spectral studies of (1), (2), (3) and (5) indicate their monomeric nature. 1H and 13C{1H} NMR spectra suggest that the oximato moieties are monodentate in solution which was further confirmed by the 51V NMR signals, appeared in the region expected for tetra-coordinated oxo-vanadium atoms. On ageing, a disproportionation reaction occurs in (1) and some crystals appeared. Single crystal X-ray diffraction analyses of the crystals obtained from (1) as well as from (3) were found to be the same and indicate the presence of side-on {dihapto η 2-(N, O)} binding modes of the oximato ligands, leading to the formation of seven coordination environment around the vanadium atom. Thermogravimetric curve of (1) exhibits multi-step decomposition with the formation of V2O5 as the final product at ~850 °C. Sol–gel transformation of (3) yielded (a) VO2 sintered at 300 °C and (b) V2O5 at 600 °C. Similarly, sol–gel transformations of (1) and (2) yielded V2O5 (c) and (d) at 600 °C, respectively. Formation of monoclinic phase in (a) and orthorhombic phase in (b), (c) and (d) were confirmed by powder XRD patterns. 相似文献
33.
Archana Chaudhary Ram Gopal Meena Nagar Rakesh Bohra 《Journal of Sol-Gel Science and Technology》2014,69(1):102-106
Some oxime modified complexes of the type [Zr{OPri}4?n{L}n] {where, n = 1–4 and LH=(CH3)2C=NOH (1–4) and C9H16C=NOH (5–8)} have been synthesized by the reaction of [Zr(OPri)4·PriOH] with oximes, in anhydrous refluxing benzene. These synthesized complexes were characterized by elemental analyses, molecular weight measurements, ESI-mass, FT-IR and NMR (1H and 13C{1H}) spectral studies. The ESI-mass spectral studies indicate dimeric nature for [Zr{OPri}2{ONC(CH3)2}2] (2), [Zr{OPri}3{ONC10H16}] (5) and [Zr{OPri}{ONC10H16}3] (7) and monomeric nature for [Zr{ONC10H16}4] (8). Oximato ligands appear to bind the zirconium in side on manner in all the complexes. Thermogravimetric curves of (2) and (8) exhibit multi-step decomposition with the formation of ZrO2, under nitrogen atmosphere. Sol–gel transformations of precursors (5), (6), (7) and (8) in organic medium, yielded nano-sized tetragonal phase of zirconia samples (a), (b), (c) and (d), respectively, on sintering at ~600 °C. All these samples were characterized by Powder XRD patterns and EDX analyses. Surface morphologies of these samples were investigated by SEM images. 相似文献
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35.
The effect of injection on the flow of Oldroyd fluid in the inlet region of a channel has been investigated using the moment and energy integrals, taking into account the loss of energy due to viscous dissipation in the boundary layer. Analytical expression for boundary layer development has been presented. 相似文献
36.
The dc magnetization and ac susceptibility measurements on two dimensional layered manganite La1.2Ba1.8Mn2O7 samples reveal the occurrence of ferromagnetism above room temperature with ferromagnetic (FM) to paramagnetic (PM) transitions at 338 K. The bifurcation temperatures shown by the zero-field cooled (ZFC) and field cooled (FC) dc magnetization curves at high temperatures shift towards lower temperatures as the applied field is increased from 100 to 2500 Oe. The data are suggestive of a large magnetic anisotropy due to the strong competing ferromagnetic and antiferromagnetic interactions resulting in a spin-glass-like state. Ru doping is found to enhance the ferromagnetism and metallicity of the system in a remarkable way. The magnetoresistance (MR) values obtained are very high and about 40% even at 260 K for the undoped sample. 相似文献
37.
Mohsen Shenasa Sudhakar Sainkar David Lichtman 《Journal of Electron Spectroscopy and Related Phenomena》1986,40(4):329-337
X-ray photoelectron spectroscopy (XPS) of the Se 3d peak for Se in Se, SeO2, As2Se3, ZnSe, CdSe, CoSe, FeSe, CrSe, VSe2 and TiSe were studied. It was found that, firstly, in the case of As2Se3, ZnSe, CdSe, CoSe and CrSe, as the change in electronegativity of the anion increases, the change in the binding energy value of the Se 3d peak also increases and, secondly, in all of the Se compounds studied, the Se-Se bond in pure Se is stronger than the Se-x bond, where X = As, Zn, Cd, Co, Fe, Cr, V and Ti. 相似文献
38.
Padmanabhan Sudhakar 《Journal of polymer science. Part A, Polymer chemistry》2008,46(2):444-452
The newly synthesized 1‐TiCl (C3 symmetric) and 2‐TiCl (Cs symmetric) precatalysts in combination with MAO polymerized ethylene, cyclic olefins, and copolymerized ethylene/norbornene in good yields. The catalyst with C3 symmetry exhibits moderate catalytic activity and efficient norbornene incorporation for E/NBE copolymerization in the presence of MAO [activity = 360 kg polymer/(mol Ti h), ethylene 1 atm, NBE 5 mmol/mL, 10 min], affording poly(ethylene‐co‐NBE)s with high norbornene contents (42.0%) and the Cs symmetric catalyst showed an activity of 420 kg polymer/(mol Ti h), ethylene 1 atm, NBE 5 mmol/mL affording poly(ethylene‐co‐NBE)s with 33.0% norbornene content. The effect of monomer concentration at ambient temperature and constant Al/Ti ratio for the homo and copolymerization was studied in a detailed manner. We found that apart from the electronic environment around the metal center the steric environment provided by the symmetry of the catalyst systems has a considerable influence on the percentage of norbornene content of the copolymer obtained. We also found that with a given catalyst a variable clearly influencing the copolymer microstructure, hence also the copolymer properties, is the monomer concentration at a given feed ratio. © 2007 Wiley Periodicals, Inc. J Polym Sci Part A: Polym Chem 46: 444–452, 2008 相似文献
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40.
Treatment of tetrahydropyranyl ethers with cerium (III) chloride heptahydrate in methanol provides a simple, convenient and selective method for detetrahydropyranylation, and the parent alcohols are obtained in high yields. 相似文献