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921.
Nigel J. Brookes David C. Graham Gemma Christian Robert Stranger Brian F. Yates 《Journal of computational chemistry》2009,30(13):2146-2156
Electronic structure methods have been combined with the ONIOM approach to carry out a comprehensive study of the effect of ligand bulk on the activation of dinitrogen with three‐coordinate molybdenum complexes. Calculations were performed with both density functional and CCSD(T) methods. Our results show that not only is there expected destabilization of the intermediate on the pathway due to direct steric interactions of the bulky groups, but also there is significant electronic destabilization as the size of the ligand increases. This latter destabilization is due to the inability of the molecule to accommodate a rotated amide group bound to the molybdenum once the amide reaches a certain size. This destabilization also leads to a clear preference for the triplet intermediate (rather than the singlet intermediate) for bulky substituents which is in agreement with experiment. Overall, the calculated reaction profile for the bulky substituents shows a good correlation with the available experimental data. © 2009 Wiley Periodicals, Inc. J Comput Chem 2009 相似文献
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923.
H. Reiter Curt C. Christian H. Mitsch K. Sigmund H. G. Feichtinger I. Kolář 《Monatshefte für Mathematik》1986,102(2):175-178
924.
Ruth Müller Christian Wiencke Kai Bischof Bernd Krock 《Photochemistry and photobiology》2009,85(4):970-977
Phlorotannins have often been considered to act as UV-protective compounds in zoospores of brown algae. However, only the absorption characteristics of zoospores under UV exposure have been determined and no data are available on the actual content of phlorotannins or on temperature–UV interactions. Therefore, we determined the absorbance spectra and the phlorotannin contents in zoospore suspensions of three Arctic species ( Saccharina latissima , Laminaria digitata , Alaria esculenta ), and in the media surrounding zoospores after exposure to different radiation (400–700, 320–700, 295–700 nm) and temperature (2–18°C) conditions for 8 h. Absorption typical of phlorotannins with a maximum at 276 nm was monitored in zoospore suspensions as well as in the media surrounding zoospores, but the results depended strongly on radiation treatments and on zoospore densities. Surprisingly, the content of UV-absorbing phlorotannins subsequent to different exposures did not change in any of the three species. The observed exceptional absorption properties could, therefore, not be related to phlorotannin contents. These findings are discussed in light of a strong phlorotannin investment from sporophytes during spore release and a minor UV-protective role of phlorotannins for zoospores of Arctic kelp species. 相似文献
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A survey represented mainly by means of glasses of the borosilicate system shows the generally valid limits of the applicability of the crack growth model and the essential influence of the corrosion of glasses on fatigue. A close correlation between macroscopic crack growth and fatigue was affirmed for samples with fresh, slightly corroded cracks. If the state of corrosion of the samples is advanced, the influence of region 2 is reduced and the fatigue limit is increased. Processes of corrosion during the measurement influence the fatigue curve prevailingly in the range of great time-to-failure, in particular the slope in region 1. The results indicate the high complexity of the effective chemomechanical processes during the fatigue measurements. 相似文献