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91.
Avinash Chettri Jan-Hendrik Kruse Keshav Kumar Jha Lara Dröge Dr. Iuliia Romanenko Dr. Christof Neumann Dr. Stephan Kupfer Prof. Dr. Andrey Turchanin Prof. Dr. Sven Rau Prof. Dr. Felix H. Schacher Prof. Dr. Benjamin Dietzek 《Chemistry (Weinheim an der Bergstrasse, Germany)》2021,27(68):17049-17058
Recently, porous photocatalytically active block copolymer membranes were introduced, based on heterogenized molecular catalysts. Here, we report the integration of the photosensitizer, i. e., the light absorbing unit in an intermolecular photocatalytic system into block copolymer membranes in a covalent manner. We study the resulting structure and evaluate the orientational mobility of the photosensitizer as integral part of the photocatalytic system in such membranes. To this end we utilize transient absorption anisotropy, highlighting the temporal reorientation of the transition dipole moment probed in a femtosecond pump-probe experiment. Our findings indicate that the photosensitizer is rigidly bound to the polymer membrane and shows a large heterogeneity of absolute anisotropy values as a function of location probed within the matrix. This reflects the sample inhomogeneity arising from different protonation states of the photosensitizer and different intermolecular interactions of the photosensitizers within the block copolymer membrane scaffold. 相似文献
92.
Alexandra Mavridi-Printezi Arianna Menichetti Moreno Guernelli Prof. Dr. Marco Montalti 《Chemistry (Weinheim an der Bergstrasse, Germany)》2021,27(66):16309-16319
Melanin-like nanomaterials have found application in a large variety of high economic and social impact fields as medicine, energy conversion and storage, photothermal catalysis and environmental remediation. These materials have been used mostly for their optical and electronic properties, but also for their high biocompatibility and simplicity and versatility of preparation. Beside this, their chemistry is complex and it yields structures with different molecular weight and composition ranging from oligomers, to polymers as well as nanoparticles (NP). The comprehension of the correlation of the different compositions and morphologies to the optical properties of melanin is still incomplete and challenging, even if it is fundamental also from a technological point of view. In this minireview we focus on scientific papers, mostly recent ones, that indeed examine the link between composition and structural feature and photophysical and photochemical properties proposing this approach as a general one for future research. 相似文献
93.
Chinmoy Biswas Prof. Venugopal Rao Soma Dr. Prabhakar Chetti Dr. Sai Santosh Kumar Raavi 《Chemphyschem》2021,22(24):2562-2572
An all-inclusive investigation of the ultrafast excited state relaxation dynamics of a triphenylmethane derivative molecule, New Fuchsine (NF), using a combined approach of density functional theory (DFT), femtosecond transient absorption spectroscopy (fs-TAS), and photoluminescence spectroscopy is presented in this work. The DFT calculations confirmed the formation of twisted molecular structure in the excited state of NF in ethanol solution with bond rotation of ≈86°. TAS measurements of NF solution exhibited ultrafast ground state-recovery pathway via a conical intersection confirming an ultrafast structural reorientation. On the contrary, TAS measurements of NF thin-film exhibited a longer excited-state lifetime suggesting a hindered molecular twisted state formed as an intermediate step. Photophysical kinetic models are proposed to globally fit the fs-TAS data establishing the twisted intramolecular charge transfer (TICT) state mediated ground state recovery for NF in solution and thin film, respectively. Temperature-dependent photoluminescence study of NF film provided a clear insight into the effect of rotational motion of phenyl rings in NF molecules over the TICT mediated emission. 相似文献
94.
Jazer Jose H. Togonon Eugene A. Esparcia Jr. Prof. Julie Anne D. del Rosario Prof. Joey D. Ocon 《ChemistryOpen》2021,10(4):471-476
Biodegradable primary batteries, also known as transient batteries, are essential to realize autonomous biodegradable electronic devices with high performance and advanced functionality. In this work, magnesium, copper, iron, and zinc – metals that exist as trace elements in the human body – were tested as materials for biomedical transient electronic devices. Different full cell combinations of Mg and X (where X = Cu, Fe, and Zn and the anodized form of the metals) with phosphate buffered saline (PBS) as electrolyte were studied. To form the cathodes, metal foils were anodized galvanostatically at a current density of 2.0 mA cm−2 for 30 mins. Electrochemical measurements were then conducted for each electrode combination to evaluate full cell battery performance. Results showed that the Mg−Cuanodized chemistry has the highest power density at 0.99 mW/cm2. Nominal operating voltages of 1.26 V for the first 0.50 h and 0.63 V for the next 3.7 h were observed for Mg−Cuanodized which was discharged at a current density of 0.70 mA cm−2. Among the materials tested, Mg−Cuanodized exhibited the best discharge performance with an average specific capacity of 2.94 mAh cm−2, which is comparable to previous reports on transient batteries. 相似文献
95.
《化学:亚洲杂志》2017,12(20):2749-2762
A novel class of β‐functionalized push–pull zinc opp ‐dibenzoporphyrins were designed, synthesized, and utilized as sensitizers for dye‐sensitized solar cells. Spectral, electrochemical, and computational studies were systematically performed to evaluate their spectral coverage, redox behavior, and electronic structures. These porphyrins displayed much broader spectral coverage and more facile oxidation upon extension of the π conjugation. Free‐energy calculations and femtosecond transient absorption studies (charge injection rate in the range of 1011 s−1) suggested efficient charge injection from the excited singlet state of the porphyrin to the conduction band of TiO2. The power conversion efficiency (η ) of YH3 bearing acrylic acid linkers (η =5.9 %) was close to that of the best ruthenium dye N719 (η =7.4 %) under similar conditions. The superior photovoltaic performance of YH3 was attributed to its higher light‐harvesting ability and more favorable electron injection and collection, as supported by electrochemical impedance spectral studies. This work demonstrates the exceptional potential of benzoporphyrins as sensitizers for dye‐sensitized solar cells. 相似文献
96.
《Angewandte Chemie (International ed. in English)》2017,56(20):5471-5474
We present a proof of concept that ultrafast dynamics combined with photochemical stability information of molecular photocatalysts can be acquired by electrospray ionization mass spectrometry combined with time‐resolved femtosecond laser spectroscopy in an ion trap. This pump‐probe “fragmentation action spectroscopy” gives straightforward access to information that usually requires high purity compounds and great experimental efforts. Results of gas‐phase studies on the electronic dynamics of two supramolecular photocatalysts compare well to previous findings in solution and give further evidence for a directed electron transfer, a key process for photocatalytic hydrogen generation. 相似文献
97.
98.
《Arabian Journal of Chemistry》2023,16(4):104589
PurposeThe purpose of the current framework is to scrutinize the two-dimensional flow and heat transfer of Casson nanofluid over cylinder/plate along with impacts of thermophoresis and Brownian motion effects. Also, the effects of exponential thermal sink/source, bioconvection, and motile microorganisms are taken.Methodology/ApproachThe resulting non-linear equations (PDEs) are reformed into nonlinear ODEs by using appropriate similarity variables. The resultant non-linear (ODEs) were numerically evaluated by the use of the Bvp4c package in the mathematical solver MATLAB.FindingsThe numerical and graphical illustration regarding outcomes represents the performance of flow-involved physical parameters on velocity, temperature, concentration, and microorganism profiles. Additionally, the skin friction coefficient, local Nusselt number, local Sherwood number, and local microorganism density number are computed numerically for the current presented system. We noted that the velocity profile diminishes for the rising estimations of magnetic and mixed convection parameters. The Prandtl number corresponds with the declining performance of the temperature profile observed. The enhancement in the values of the Solutal Biot number and Brownian motion parameter increased in the concentration profile.OriginalityIn specific, this framework focuses on the rising heat transfer of Casson nanofluid with bioconvection by using a shooting mathematical model. The novel approach of the presented study is the use of motile microorganisms with exponential thermal sink/source in a Casson nano-fluid through a cylinder/plate. A presented study performed first time in the author’s opinion. Understanding the flow characteristics and behaviors of these nanofluids is crucial for the scientific community in the developing subject of nanofluids. 相似文献
99.
100.
G. G. Fedoruk 《Journal of Applied Spectroscopy》2002,69(2):161-182
The application of transient nutations in EPR spectroscopy of condensed media is considered. The main methods of formation and observation of transient nutations are presented. The laws governing this phenomenon in twolevel and multilevel spin systems and also in inhomogeneous broadening of EPR lines are described. Recent advances in the use of transient nutations to separate overlapping spectra, identify quantum numbers and quantum transitions, investigate the kinetics of photoinduced paramagnetic centers, and determine relaxation times for a wide range of crystalline and disordered media are presented. 相似文献