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排序方式: 共有220条查询结果,搜索用时 15 毫秒
91.
Dr. Benjamin C. M. Martindale Georgina A. M. Hutton Prof. Christine A. Caputo Sebastian Prantl Dr. Robert Godin Prof. James R. Durrant Dr. Erwin Reisner 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2017,129(23):6559-6563
Single-source precursor syntheses have been devised for the preparation of structurally similar graphitic carbon dots (CDs), with (g-N-CD) and without (g-CD) core nitrogen doping for artificial photosynthesis. An order of magnitude improvement has been realized in the rate of solar (AM1.5G) H2 evolution using g-N-CD (7950 μmolH2 (gCD)−1 h−1) compared to undoped CDs. All graphitized CDs show significantly enhanced light absorption compared to amorphous CDs (a-CD) yet undoped g-CD display limited photosensitizer ability due to low extraction of photogenerated charges. Transient absorption spectroscopy showed that nitrogen doping in g-N-CD increases the efficiency of hole scavenging by the electron donor and thereby significantly extends the lifetime of the photogenerated electrons. Thus, nitrogen doping allows the high absorption coefficient of graphitic CDs to be translated into high charge extraction for efficient photocatalysis. 相似文献
92.
Yoo SD Boston JR El-Jaroudi A Li CC Durrant JD Kovacyk K Shaiman S 《The Journal of the Acoustical Society of America》2007,122(2):1138-1149
The role of transient speech components on speech intelligibility was investigated. Speech was decomposed into two components--quasi-steady-state (QSS) and transient--using a set of time-varying filters whose center frequencies and bandwidths were controlled to identify the strongest formant components in speech. The relative energy and intelligibility of the QSS and transient components were compared to original speech. Most of the speech energy was in the QSS component, but this component had low intelligibility. The transient component had much lower energy but was almost as intelligible as the original speech, suggesting that the transient component included speech elements important to speech perception. A modified version of speech was produced by amplifying the transient component and recombining it with the original speech. The intelligibility of the modified speech in background noise was compared to that of the original speech, using a psychoacoustic procedure based on the modified rhyme protocol. Word recognition rates for the modified speech were significantly higher at low signal-to-noise ratios (SNRs), with minimal effect on intelligibility at higher SNRs. These results suggest that amplification of transient information may improve the intelligibility of speech in noise and that this improvement is more effective in severe noise conditions. 相似文献
93.
D. L. Damcott J. M. Cookson R. D. Carter JR. J. R. Martin M. Atzmon G. S. Was 《辐射效应与固体损伤》2013,168(4):383-392
Abstract A technique is developed which addresses the problem of irradiation assisted stress corrosion cracking of stainless steels in light water reactors using high energy protons to induce grain boundary segregation. These results represent the first grain boundary segregation measurements in bulk produced by proton irradiation of stainless steel. The technique allows the study of grain boundary composition with negligible sample activation, short irradiation time, rapid sample turnaround and at minimal cost. Scanning Auger electron microscopy is used to obtain grain boundary composition measurements of irradiated and unirradiated samples of ultra high purity (UHP) type 304L stainless steel and UHP type 304L steels with the additions of phosphorus (UHP + P) and sulphur (UHP + S). Results show that irradiation of all three alloys causes significant Ni segregation to the grain boundary and Cr and Fe away from it. Irradiation of the UHP + P alloy also results in segregation of P at the grain boundary from 5.3 to 8.7 at %, over 80 times the bulk value. No radiation-induced grain boundary segregation of S was measured in the UHP + S alloy. Results also indicate that the presence of P or S may enhance radiation-induced segregation of major alloying elements at the boundary. Comparison of irradiated and unirradiated regions of the UHP + P alloy indicate that while a prior thermal treatment segregates P to the grain boundary to 5.3 at %, the major element concentrations at the grain boundary are completely different from those under irradiation. 相似文献
94.
Pendlebury SR Barroso M Cowan AJ Sivula K Tang J Grätzel M Klug D Durrant JR 《Chemical communications (Cambridge, England)》2011,47(2):716-718
Transient absorption spectroscopy on the μs-s time scale is used to monitor the yield and decay dynamics of photogenerated holes in nanocrystalline hematite photoanodes. In the absence of a positive applied bias, these holes are observed to undergo rapid electron-hole recombination. The application of a positive bias results in the generation of long-lived (3 ± 1 s lifetime) photoholes. 相似文献
95.
O. EL AKRAMINE W. A. LESTER JR X. KROKIDIS C. A. TAFT T. C. GUIMARAES A. C. PAVAO 《Molecular physics》2013,111(1-2):277-285
The chemisorption of CO on a Cr (110) surface is investigated using the quantum Monte Carlo method in the diffusion Monte Carlo (DMC) variant and a model Cr2CO cluster. The present results are consistent with the earlier ab initio HF study with this model that showed the tilted/near-parallel orientation as energetically favoured over the perpendicular arrangement. The DMC energy difference between the two orientations is larger (1.9 eV) than that computed in the previous study. The distribution and reorganization of electrons during CO adsorption on the model surface are analysed using the topological electron localization function method that yields electron populations, charge transfer and clear insight on the chemical bonding that occurs with CO adsorption and dissociation on the model surface. 相似文献
96.
In this study, the aromatic-thiol π hydrogen bonding and phenylalanine-cysteine side chain interactions are characterized through both molecular orbital calculations on a C6H6-HSCH3 model complex and database analyses of 609 X-ray protein structures. The aromatic-thiol π hydrogen bonding interaction can achieve a stabilization energy of 2.60 kcal mol?1, and is stronger than the already documented aromatic-hydroxyl and aromatic-amino hydrogen bonds. However, the occurrence of the aromatic-thiol hydrogen bond is rather rare in proteins. This is because most of the thiol groups participate in the formation of either disulphide bonds or stronger S—H…O (or N) ‘normal’ hydrogen bonds in a protein environment. Interactions between the side chains of phenylalanine and cysteine residues are characterized as the phenyl(Phe)(HSCH2-)(Cys) interaction. The bonding energy for such interactions is approximately 3.71 kcal mol-1 and is achieved in a geometric arrangement with an optimal phenyl(Phe)-(HS-)(Cys) π-type hydrogen bonding interaction. The interaction is very sensitive to the orientation of the two lone electron pairs on the sulphur atom relative to the π electron cloud of the phenyl ring. Accordingly, the interaction configurations that can accomplish a significant bonding energy exist only within a narrow configurational space. The database analysis of 609 experimental X-ray protein structures demonstrates that only 268 of the 1620 cysteine residues involve such phenylalanine-cysteine side chain interactions. Most of these interactions occur in the form of π (aromatic)-lone pair(sulphur) attractions, and correspond to a bonding energy less than 1.5 kcal mol?1. A few were identified as the aromatic-thiol hydrogen bond with a bonding energy of 2.0–3.6 kcal mol?1. 相似文献
97.
Applied Biochemistry and Biotechnology - The present work examines the production of ethanol via direct fermentation of pure celluloses and lignocellulosic wastes by two soil fungi isolated under... 相似文献
98.
This paper presents a method of obtaining the complete asymptoticsolution of boundary value problems of the form
for x [0,1] where b(x) is strictly positive andfor small and positive. Physically, the problem arises in determiningthe steady-state concentration of a substance in a chemicalflow reactor. A "two-variable" expansion procedure is used. 相似文献
99.
Aitala EM Amato S Anjos JC Appel JA Ashery D Banerjee S Bediaga I Blaylock G Bracker SB Burchat PR Burnstein RA Carter T Carvalho HS Copty NK Costa I Cremaldi LM Darling C Denisenko K Fernandez A Gagnon P Gerzon S Gobel C Gounder K Halling AM Herrera G Hurvits G James C Kasper PA Kwan S Langs DC Leslie J Lundberg B MayTal-Beck S Meadows B de Mello Neto JR Milburn RH de Miranda JM Napier A Nguyen A d'Oliveira AB O'Shaughnessy K Peng KC Perera LP Purohit MV Quinn B Radeztsky S Rafatian A 《Physical review letters》1996,77(12):2384-2387
100.
Abstract— The effects of u.v.-irradiation at 254 nm upon lyophilized ribonuclease, lysozyme, insulin, and chymotrypsinogen have been investigated by electron spin resonance (ESR). enzymatic assay, and labeling of free radical sites with tritiated hydrogen sulfide (HST). The ESR signal of the irradiated protein diminishes on exposure to HST, and tritium becomes covalently bound to carbon. The distribution of tritium among the amino acids of each protein. studied as an indicator of the carbon free radical distribution, differs markedly from those observed previously to result from exposure to gamma radiation, electrical discharge. or hydrogen atoms. However, the earlier observation that the tritium distribution is influenced by protein conformation holds true as well for u.v.-irradiation. Moreover, the distributions of tritium among the amino acids of u.v.-irradiated proteins indicate a broad scattering of free radicals. Tyrosine and phenylalanine, residues that absorb light energy in the region of the wavelength employed, are not particularly important as radical carriers. Thus, for ribonuclease, these residues incorporated 3.8 and 1.5 per cent of the total tritium, but they absorb 51 and 12 per cent of the light, respectively. These results, together with the observed low recoveries of methionine, an amino acid that does not absorb at 254 nm, add weight to the concept that a migration of energy ensues after the initial absorption of light energy and that photolytic damage may thus be due to destruction of amino acids other than those initially absorbing the u.v.-radiation. 相似文献