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排序方式: 共有52条查询结果,搜索用时 421 毫秒
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Price SW Speed JD Kannan P Russell AE 《Journal of the American Chemical Society》2011,133(48):19448-19458
The underpotential deposition (upd) of a Cu shell on a non-Pt nanoparticle core followed by galvanic displacement of the Cu template shell to form core-shell electrocatalyst materials is one means by which the Pt-based mass activity targets required for commercialization of PEM fuel cells may be reached. In situ EXAFS measurements were conducted at both the Au L(3) and the Cu K absorption edges during deposition of Cu onto a carbon-supported Au electrocatalyst to study the initial stages of formation of such a core-shell electrocatalyst. The Au L(3) EXAFS data obtained in 0.5 mol dm(-3) H(2)SO(4) show that the shape of the Au core is potential dependent, from a flattened to a round spherical shape as the Cu upd potential is approached. Following the addition of 2 mmol dm(-3) Cu, the structure was also measured as a function of the applied potential. At +0.2 V vs Hg/Hg(2)SO(4), the Cu(2+) species was found to be a hydrated octahedron. As the potential was made more negative, single-crystal studies predict an ordered bilayer of sulfate anions and partially discharged Cu ions, followed by a complete/uniform layer of Cu atoms. In contrast, the model obtained by fitting the Au L(3) and Cu K EXAFS data corresponds first to partially discharged Cu ions deposited at the defect sites in the outer shell of the Au nanoparticles at -0.42 V, followed by the growth of clusters of Cu atoms at -0.51 V. The absence of a uniform/complete Cu shell, even at the most negative potentials investigated, has implications for the structure, and the activity and/or stability, of the core-shell catalyst that would be subsequently formed following galvanic displacement of the Cu shell. 相似文献
4.
The following modification of a general state space discrete-time Markov chain is considered: certain transitions are supposed “forbidden” and the chain evolves until there is such a transition. At this instant the value of the chain is “replaced” according to a given rule, and, starting from the new value, the chain evolves normally until there is a forbidden transition again; the cycle is then repeated. The relationship of this modified process to the original one is studied in general terms, with particular emphasis being given to invariant measures. Examples are given which illustrate the results obtained. 相似文献
5.
A new, vectorial approach to fast correlation attacks on binary memoryless combiners is proposed. Instead of individual input sequences or their linear combinations, the new attack is targeting subsets of input sequences as a whole thus exploiting the full correlation between the chosen subset and the output sequence. In particular, the set of all the input sequences can be chosen as the target. The attack is based on a novel iterative probabilistic algorithm which is also applicable to general memoryless combiners over finite fields or finite rings. To illustrate the effectiveness of the introduced approach, experimental results obtained for random balanced combining functions are presentedMost of this work was done while he was with Rome CryptoDesign Center, Gemplus, Italy 相似文献
6.
The motion of a holonomic scleronomic non-conservative mechanicalsystem with minimal dissipation is considered. As applicationsof the theory several problems are studied in detail. 相似文献
7.
Jonathan Guild Michael J. Morris Craig C. Robertson Alexander W.H. Speed 《Tetrahedron letters》2019,60(39):151079
The reaction of phenyl acetylide anion with aryl isocyanates followed by quenching with water is shown to produce pyrrolopyrrole (iso-DPP) derivatives in addition to the isomeric cyclopentadienone imines previously reported. If the reaction is quenched with dilute HCl, 5-ylidenepyrrol-2(5H)-ones, formed by a Meyer-Schuster rearrangement, can be isolated instead. A possible mechanism for this reaction is suggested. 相似文献
8.
Speed S Vicente R Aravena D Ruiz E Roubeau O Teat SJ El Fallah MS 《Inorganic chemistry》2012,51(12):6842-6850
The syntheses, structural characterization, and magnetic behavior of two new hexanuclear copper(II) complexes derived from R-phosphonic acids and 1,3-bis(dimethylamino)-2-propanol (Hbdmap) with formulas [Cu(6)(μ-bdmap)(3)(μ(3)-Ph-PO(3))(2)(μ(3)-O···H···μ(3)-O)(ClO(4))(2)(H(2)O)]·5H(2)O (1) and [Cu(6)(μ-bdmap)(3)(μ(3)-t-Bu-PO(3))(2)(μ(3)-O···H···μ(3)-O)(μ(1,3)-dca)(dca)(H(2)O)]·6H(2)O (2) (Ph-H(2)PO(3) = phenylphosphonic acid, t-Bu-H(2)PO(3) = tert-butylphosphonic acid, dca = dicyanamide) are reported. Compounds 1 and 2 are hexanuclear 3.111 R-phosphonate(2-)/1,3-bis(dimethylamino)-2-propanolato(1-) cages including in the center the [μ(3)-O···H···μ(3)-O](3-) unit. The temperature dependence of the magnetic properties of 1 and 2 clearly indicates an overall strong antiferromagnetic coupling confirmed by DFT calculations. 相似文献
9.
A Mukherjee M Dasgupta DJ Hinde CR Morton AC Berriman RD Butt JO Newton H Timmers 《Pramana》2001,57(1):195-198
Fusion cross-sections for the 7Li + 12C reaction have been measured at energies above the Coulomb barrier by the direct detection of evaporation residues. The heavy
evaporation residues with energies below 3 MeV could not be separated out from the α-particles in the spectrum and hence their
contribution was estimated using statistical model calculations. The present work indicates that suppression of fusion cross-sections
due to the breakup of 7Li may not be significant for 7Li + 12C reaction at energies around the barrier. 相似文献
10.
The alternating step generator is a well-known keystream generator consisting of two stop/go clocked LFSRs, LFSR1 and LFSR2, whose clocks are controlled by another LFSR, LFSR3, which is clocked regularly. A probabilistic analysis of this generator is conducted which shows that the posterior probabilites of individual bits of the first derivatives of the regularly clocked LFSR1 and LFSR2 sequences, when conditioned on a given segment of the first derivative of the keystream sequence, can be computed efficiently in a number of probabilistic models of interest. The expected values of these probabilities, for a random keystream sequence, are derived by an approximate theoretical analysis and are also verified by systematic computer experiments. It is pointed out that these posterior probabilities can be enhanced in a resynchronization scenario and thus used for a low-complexity fast correlation attack on the two LFSRs. More generally, it is argued that even without resynchronization these probabilities may be significantly different from one half for fast correlation attacks based on iterative decoding algorithms to be successful, although with incresead complexity. A related method for computing the posterior probabilities of individual bits of the LFSR3 sequence, when conditioned on both the keystream sequence and the LFSR1 and LFSR2 sequences, is also developed. As these posterior probabilities are much more different from one half, they can be used for a low-complexity fast correlation attack on LFSR3, provided that the initial states of LFSR1 and LFSR2 are previously reconstructed. 相似文献