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1.
Kamila B. Muchowska Dominic J. Pascoe Stefan Borsley Ivan V. Smolyar Ioulia K. Mati Catherine Adam Gary S. Nichol Kenneth B. Ling Scott L. Cockroft 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(34):14710-14716
Interactions between carbonyl groups are prevalent in protein structures. Earlier investigations identified dominant electrostatic dipolar interactions, while others implicated lone pair n→π* orbital delocalisation. Here these observations are reconciled. A combined experimental and computational approach confirmed the dominance of electrostatic interactions in a new series of synthetic molecular balances, while also highlighting the distance-dependent observation of inductive polarisation manifested by n→π* orbital delocalisation. Computational fiSAPT energy decomposition and natural bonding orbital analyses correlated with experimental data to reveal the contexts in which short-range inductive polarisation augment electrostatic dipolar interactions. Thus, we provide a framework for reconciling the context dependency of the dominance of electrostatic interactions and the occurrence of n→π* orbital delocalisation in C=O⋅⋅⋅C=O interactions. 相似文献
2.
Mark Prendergast Cormac Breen Aibhin Bray Fiona Faulkner Brian Carroll Dominic Quinn 《International Journal of Mathematical Education in Science & Technology》2018,49(8):1203-1218
Many studies over the past 30 years have highlighted the important role of students’ beliefs for successful problem-solving in mathematics. Given the recent emphasis afforded to problem-solving on the reformed Irish secondary school mathematics curriculum, the main aim of this study was to identify Irish students’ (n = 975) beliefs about the field. A quantitative measure of these beliefs was attained through the use of the Indiana Mathematical Belief Scale, an existing 30-item (five-scale) self-report questionnaire. A statistical analysis of the data revealed that students who were further through their secondary education had a stronger belief that not all problems could be solved by applying routine procedures. In contrast, the same students held less positive beliefs than their younger counterparts that they could solve time-consuming problems and that conceptual understanding was important. The analysis also indicated that gender had a significant impact on three of the five belief scales. 相似文献
3.
Torsten Roth Vladislav Vasilenko Callum G. M. Benson Hubert Wadepohl Dominic S. Wright Lutz H. Gade 《Chemical science》2015,6(4):2506-2510
A simple, “click” synthetic approach to a new type of hybrid phosph(III)azane/NHC system is described. The presence of the phosphazane P2N2 ring unit, with P atoms flanking the NCN fragment and with this ring perpendicular to the binding site of the NHC, provides unique opportunities for modifying the electronic and steric character of these carbenes. 相似文献
4.
Dominic Brenner Andreas Dellnitz Wilhelm Rödder 《The Journal of mathematical sociology》2017,41(2):84-103
To detect and study cohesive subgroups of actors is a main objective in social network analysis. What are the respective relations inside such groups and what separates them from the outside. Entropy-based analysis of network structures is an up-and-coming approach. It turns out to be a powerful instrument to detect certain forms of cohesive subgroups and to compress them to superactors without loss of information about their embeddedness in the net: Compressing strongly connected subgroups leaves the whole net’s and the (super-)actors’ information theoretical indices unchanged; i.e., such compression is information-invariant. The actual article relates on the reduction of networks with hundreds of actors. All entropy-based calculations are realized in an expert system shell. 相似文献
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Dominic Aboagye Dr. Ridha Djellabi Prof. Francesc Medina Dr. Sandra Contreras 《Angewandte Chemie (International ed. in English)》2023,62(36):e202301909
Photocatalytic biomass conversion into high-value chemicals and fuels is considered one of the hottest ongoing research and industrial topics toward sustainable development. In short, this process can cleave Cβ−O/Cα−Cβ bonds in lignin to aromatic platform chemicals, and further conversion of the polysaccharides to other platform chemicals and H2. From the chemistry point of view, the optimization of the unique cooperative interplay of radical oxidation species (which are activated via molecular oxygen species, ROSs) and substrate-derived radical intermediates by appropriate control of their type and/or yield is key to the selective production of desired products. Technically, several challenges have been raised that face successful real-world applications. This review aims to discuss the recently reported mechanistic pathways toward selective biomass conversion through the optimization of ROSs behavior and materials/system design. On top of that, through a SWOT analysis, we critically discussed this technology from both chemistry and technological viewpoints to help the scientists and engineers bridge the gap between lab-scale and large-scale production. 相似文献
7.
Annalena Gärtner Matthäus Marek Dr. Merle Arrowsmith Dr. Dominic Auerhammer Krzysztof Radacki Dr. Dominic Prieschl Dr. Rian D. Dewhurst Prof. Dr. Holger Braunschweig 《Chemistry (Weinheim an der Bergstrasse, Germany)》2021,27(37):9694-9699
Cyclic alkyl(amino)carbene-stabilized (cyano)hydroboryl anions were synthesized by deprotonation of (cyano)dihydroborane precursors. While they display boron-centered nucleophilic reactivity towards organohalides, generating fully unsymmetrically substituted cyano(hydro)organoboranes, they show cyano-nitrogen-centered nucleophilic reactivity towards haloboranes, resulting in the formation of hitherto unknown linear 2-aza-1,4-diborabutatrienes. 相似文献
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Asymmetric Rhodium‐Catalyzed Addition of Thiols to Allenes: Synthesis of Branched Allylic Thioethers and Sulfones 下载免费PDF全文
Adrian B. Pritzius Prof. Dr. Bernhard Breit 《Angewandte Chemie (International ed. in English)》2015,54(10):3121-3125
A highly regio‐ and enantioselective hydrothiolation of terminal allenes, a reaction which fulfills the criteria of atom economy, is reported. Applying two chiral rhodium catalyst systems, a wide variety of thiols and allenes could be coupled. Oxidation gave access to the corresponding allylic sulfones in essentially enantiomerically pure form. The reaction tolerates a variety of functional groups and labeling experiments gave first insights into the reaction mechanism of this new methodology. 相似文献
10.
Mono‐, di‐ and trimethylated homologues of isoprenoid tetraether lipid cores in archaea and environmental samples: mass spectrometric identification and significance 下载免费PDF全文
Chris Knappy Daniela Barillà James Chong Dominic Hodgson Hugh Morgan Muhammad Suleman Christine Tan Peng Yao Brendan Keely 《Journal of mass spectrometry : JMS》2015,50(12):1420-1432
Higher homologues of widely reported C86 isoprenoid diglycerol tetraether lipid cores, containing 0–6 cyclopentyl rings, have been identified in (hyper)thermophilic archaea, representing up to 21% of total tetraether lipids in the cells. Liquid chromatography‐tandem mass spectrometry confirms that the additional carbon atoms in the C87‐88 homologues are located in the etherified chains. Structures identified include dialkyl and monoalkyl (‘H‐shaped’) tetraethers containing C40‐42 or C81‐82 hydrocarbons, respectively, many representing novel compounds. Gas chromatography‐mass spectrometric analysis of hydrocarbons released from the lipid cores by ether cleavage suggests that the C40 chains are biphytanes and the C41 chains 13‐methylbiphytanes. Multiple isomers, having different chain combinations, were recognised among the dialkyl lipids. Methylated tetraethers are produced by Methanothermobacter thermautotrophicus in varying proportions depending on growth conditions, suggesting that methylation may be an adaptive mechanism to regulate cellular function. The detection of methylated lipids in Pyrobaculum sp. AQ1.S2 and Sulfolobus acidocaldarius represents the first reported occurrences in Crenarchaeota. Soils and aquatic sediments from geographically distinct mesotemperate environments that were screened for homologues contained monomethylated tetraethers, with di‐ and trimethylated structures being detected occasionally. The structural diversity and range of occurrences of the C87‐89 tetraethers highlight their potential as complementary biomarkers for archaea in natural environments. Copyright © 2015 John Wiley & Sons, Ltd. 相似文献