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DDC: 500 × Subject: synthesis ×

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Now showing 1 - 4 of 4
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    Universal emulsion stabilization from the arrested adsorption of rough particles at liquid-liquid interfaces
    ([London] : Nature Publishing Group UK, 2017) Zanini, Michele; Marschelke, Claudia; Anachkov, Svetoslav E.; Marini, Emanuele; Synytska, Alla; Isa, Lucio
    Surface heterogeneities, including roughness, significantly affect the adsorption, motion and interactions of particles at fluid interfaces. However, a systematic experimental study, linking surface roughness to particle wettability at a microscopic level, is currently missing. Here we synthesize a library of all-silica microparticles with uniform surface chemistry, but tuneable surface roughness and study their spontaneous adsorption at oil-water interfaces. We demonstrate that surface roughness strongly pins the particles' contact lines and arrests their adsorption in long-lived metastable positions, and we directly measure the roughness-induced interface deformations around isolated particles. Pinning imparts tremendous contact angle hysteresis, which can practically invert the particle wettability for sufficient roughness, irrespective of their chemical nature. As a unique consequence, the same rough particles stabilize both water-in-oil and oil-in-water emulsions depending on the phase they are initially dispersed in. These results both shed light on fundamental phenomena concerning particle adsorption at fluid interfaces and indicate future design rules for particle-based emulsifiers.
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    Highly active and efficient catalysts for alkoxycarbonylation of alkenes
    ([London] : Nature Publishing Group UK, 2017) Dong, Kaiwu; Fang, Xianjie; Gülak, Samet; Franke, Robert; Spannenberg, Anke; Neumann, Helfried; Jackstell, Ralf; Beller, Matthias
    Carbonylation reactions of alkenes constitute the most important industrial processes in homogeneous catalysis. Despite the tremendous progress in this transformation, the development of advanced catalyst systems to improve their activity and widen the range of feedstocks continues to be essential for new practical applications. Herein a palladium catalyst based on 1,2-bis((tert-butyl(pyridin-2-yl)phosphanyl)methyl)benzene L3 (py t bpx) is rationally designed and synthesized. Application of this system allows a general alkoxycarbonylation of sterically hindered and demanding olefins including all kinds of tetra-, tri-and 1,1-disubstituted alkenes as well as natural products and pharmaceuticals to the desired esters in excellent yield. Industrially relevant bulk ethylene is functionalized with high activity (TON: >1,425,000; TOF: 44,000 h-1 for initial 18 h) and selectivity (>99%). Given its generality and efficiency, we expect this catalytic system to immediately impact both the chemical industry and research laboratories by providing a practical synthetic tool for the transformation of nearly any alkene into a versatile ester product.
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    Synthesis of a molecularly defined single-active site heterogeneous catalyst for selective oxidation of N-heterocycles
    ([London] : Nature Publishing Group UK, 2018) Zhang, Yujing; Pang, Shaofeng; Wei, Zhihong; Jiao, Haijun; Dai, Xingchao; Wang, Hongli; Shi, Feng
    Generally, a homogeneous catalyst exhibits good activity and defined active sites but it is difficult to recycle. Meanwhile, a heterogeneous catalyst can easily be reused but its active site is difficult to reveal. It is interesting to bridge the gap between homogeneous and heterogeneous catalysis via controllable construction of a heterogeneous catalyst containing defined active sites. Here, we report that a molecularly defined, single-active site heterogeneous catalyst has been designed and prepared via the oxidative polymerization of maleimide derivatives. These polymaleimide derivatives can be active catalysts for the selective oxidation of heterocyclic compounds to quinoline and indole via the recycling of -C=O and -C-OH groups, which was confirmed by tracing the reaction with GC-MS using maleimide as the catalyst and by FT-IR analysis with polymaleimide as the catalyst. These results might promote the development of heterogeneous catalysts with molecularly defined single active sites exhibiting a comparable activity to homogeneous catalysts.
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    Investigating potential transferability of place-based research in land system science
    (Bristol : IOP Publishing, 2016) Václavík, Tomáš; Langerwisch, Fanny; Cotter, Marc; Fick, Johanna; Häuser, Inga; Hotes, Stefan; Kamp, Johannes; Settele, Josef; Spangenberg, Joachim H.; Seppelt, Ralf
    Much of our knowledge about land use and ecosystem services in interrelated social-ecological systems is derived from place-based research. While local and regional case studies provide valuable insights, it is often unclear how relevant this research is beyond the study areas. Drawing generalized conclusions about practical solutions to land management from local observations and formulating hypotheses applicable to other places in the world requires that we identify patterns of land systems that are similar to those represented by the case study. Here, we utilize the previously developed concept of land system archetypes to investigate potential transferability of research from twelve regional projects implemented in a large joint research framework that focus on issues of sustainable land management across four continents. For each project, we characterize its project archetype, i.e. the unique land system based on a synthesis of more than 30 datasets of land-use intensity, environmental conditions and socioeconomic indicators. We estimate the transferability potential of project research by calculating the statistical similarity of locations across the world to the project archetype, assuming higher transferability potentials in locations with similar land system characteristics. Results show that areas with high transferability potentials are typically clustered around project sites but for some case studies can be found in regions that are geographically distant, especially when values of considered variables are close to the global mean or where the project archetype is driven by large-scale environmental or socioeconomic conditions. Using specific examples from the local case studies, we highlight the merit of our approach and discuss the differences between local realities and information captured in global datasets. The proposed method provides a blueprint for large research programs to assess potential transferability of place-based studies to other geographical areas and to indicate possible gaps in research efforts.