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111.
Dielectric measurements on a nematic room temperature mixture and the mixture with 20% aerosil were carried out. Addition of aerosil results in a small increase of the clearing temperature and in increasing relaxation frequency for the reorientation around the short molecular axis. The results are interpreted as orientation effect of the nematic sample at the fractal aerosil. 相似文献
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Peptide synthesis in aqueous environments: the role of extreme conditions and pyrite mineral surfaces on formation and hydrolysis of peptides 总被引:1,自引:0,他引:1
Schreiner E Nair NN Wittekindt C Marx D 《Journal of the American Chemical Society》2011,133(21):8216-8226
A comprehensive study of free energy landscapes and mechanisms of COS-mediated polymerization of glycine via N-carboxy anhydrides (NCAs, "Leuchs anhydrides") and peptide hydrolysis at the water-pyrite interface at extreme thermodynamic conditions is presented. Particular emphasis is set on the catalytic effects of the mineral surface including the putative role of the ubiquitous sulfur vacancy defects. It is found that the mere presence of a surface is able to change the free energetics of the elementary reaction steps. This effect can be understood in terms of a reduction of entropic contributions to the reactant state by immobilizing the reactants and/or screening them from bulk water in a purely geometric ("steric") sense. Additionally, the pyrite directly participates chemically in some of the reaction steps, thus changing the reaction mechanism qualitatively compared to the situation in bulk water. First, the adsorption of reactants on the surface can preform a product-like structure due to immobilizing and scaffolding them appropriately. Second, pyrite can act as a proton acceptor, thus replacing water in this role. Third, sulfur vacancies are found to increase the reactivity of the surface. The finding that the presence of pyrite speeds up the rate-determining step in the formation of peptides with respect to the situation in bulk solvent while stabilizing the produced peptide against hydrolysis is of particular interest to the hypothesis of prebiotic peptide formation at hydrothermal aqueous conditions. Apart from these implications, the generality of the studied organic reactions are of immediate relevance to many fields such as (bio)geochemistry, biomineralization, and environmental chemistry. 相似文献
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Chukwuemeka Okolie Yasmeen F. Belhseine Yimeng Lyu Dr. Matthew M. Yung Dr. Mark H. Engelhard Dr. Libor Kovarik Dr. Eli Stavitski Dr. Carsten Sievers 《Angewandte Chemie (International ed. in English)》2017,56(44):13876-13881
The conversion of methane into alcohols under moderate reaction conditions is a promising technology for converting stranded methane reserves into liquids that can be transported in pipelines and upgraded to value‐added chemicals. We demonstrate that a catalyst consisting of small nickel oxide clusters supported on ceria–zirconia (NiO/CZ) can convert methane to methanol and ethanol in a single, steady‐state process at 723 K using O2 as an abundantly available oxidant. The presence of steam is required to obtain alcohols rather than CO2 as the product of catalytic combustion. The unusual activity of this catalyst is attributed to the synergy between the small Lewis acidic NiO clusters and the redox‐active CZ support, which also stabilizes the small NiO clusters. 相似文献
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Werner Damm Carsten Ihlemann Viorica Sofronie-Stokkermans 《Mathematics in Computer Science》2011,5(4):469-497
This paper identifies an industrially relevant class of linear hybrid automata (LHA) called reasonable LHA for which parametric verification of convex safety properties with exhaustive entry states can be verified in polynomial
time and time-bounded reachability can be decided in nondeterministic polynomial time for non-parametric verification and
in exponential time for parametric verification. Properties with exhaustive entry states are restricted to runs originating
in a (specified) inner envelope of some mode-invariant. Deciding whether an LHA is reasonable is shown to be decidable in
polynomial time. 相似文献
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