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11.
12.
Michiel Janssen Prof. Dirk E. De Vos 《Chemistry (Weinheim an der Bergstrasse, Germany)》2019,25(45):10724-10734
The practical application of Shilov-type Pt catalysis to the selective hydroxylation of terminal aliphatic C−H bonds remains a formidable challenge, due to difficulties in replacing PtIV with a more economically viable oxidant, particularly O2. We report the potential of employing FeCl2 as a suitable redox mediator to overcome the kinetic hurdles related to the direct use of O2 in the Pt reoxidation. For the selective conversion of butyric acid to γ-hydroxybutyric acid (GHB), a significantly enhanced catalyst activity and stability (turnover numbers (TON)>30) were achieved under 20 bar O2 in comparison to current state-of-the-art systems (TON<10). In this regard, essential reaction parameters affecting the overall activity were identified, along with specific additives to attain catalyst stability at longer reaction times. Notably, deactivation by reduction to Pt0 was prevented by the addition of monodentate pyridine derivatives, such as 2-fluoropyridine, but also by introducing varying partial pressures of N2 in the gaseous atmosphere. Finally, stability tests revealed the involvement of PtII and FeCl2 in catalyzing the non-selective overoxidation of GHB. Accordingly, in situ esterification with boric acid proved to be a suitable strategy to maintain enhanced selectivities at much higher conversions (TON>60). Altogether, a useful catalytic system for the selective hydroxylation of primary aliphatic C−H bonds with O2 is presented. 相似文献
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15.
V. De Sabbata C. Sivaram H.-H. v. Borzeszkowski H.-J. Treder 《Annalen der Physik》1991,503(7):497-502
It is shown that in gravitational theories with torsion one is led to commutation rules corresponding to Landau-Peierls type uncertainty relations. 相似文献
16.
D. De Salvador A. Coati E. Napolitani M. Berti A.V. Drigo M.S. Carroll J.C. Sturm J. Stangl G. Bauer L. Lazzarini 《Applied Physics A: Materials Science & Processing》2002,75(6):667-672
In this work we investigate the diffusion and precipitation of supersaturated substitutional carbon in 200-nm-thick SiGeC
layers buried under a silicon cap layer of 40 nm. The samples were annealed in either inert (N2) or oxidizing (O2) ambient at 850 °C for times ranging from 2 to 10 h. The silicon self-interstitial (I) flux coming from the surface under
oxidation enhances the C diffusion with respect to the N2-annealed samples. In the early stages of the oxidation process, the loss of C from the SiGeC layer by diffusion across the
layer/cap interface dominates. This phenomenon saturates after an initial period (2–4 h), which depends on the C concentration.
This saturation is due to the formation and growth of C-containing precipitates that are promoted by the I injection and act
as a sink for mobile C atoms. The influence of carbon concentration on the competition between precipitation and diffusion
is discussed.
Received: 19 October 2001 / Accepted: 19 December 2001 / Published online: 20 March 2002 / Published online: 20 March 2002 相似文献
17.
T. Temesvári C. De Dominicis I.R. Pimentel 《The European Physical Journal B - Condensed Matter and Complex Systems》2002,25(3):361-372
Symmetry considerations and a direct, Hubbard-Stratonovich type, derivation are used to construct a replica field-theory relevant
to the study of the spin glass transition of short range models in a magnetic field. A mean-field treatment reveals that two
different types of transitions exist, whenever the replica number n is kept larger than zero. The Sherrington-Kirkpatrick critical point in zero magnetic field between the paramagnet and replica
magnet (a replica symmetric phase with a nonzero spin glass order parameter) separates from the de Almeida-Thouless line,
along which replica symmetry breaking occurs. We argue that for studying the de Almeida-Thouless transition around the upper
critical dimension d = 6, it is necessary to use the generic cubic model with all the three bare masses and eight cubic couplings. The critical
role n may play is also emphasized. To make perturbative calculations feasible, a new representation of the cubic interaction is
introduced. To illustrate the method, we compute the masses in one-loop order. Some technical details and a list of vertex
rules are presented to help future renormalisation-group calculations.
Received 9 October 2001 相似文献
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19.
M. Castagnino R. Id Betan R. Laura 《International Journal of Theoretical Physics》2003,42(10):2423-2439
By extending the notion of mixed states to functionals acting on the space of observables with diagonal singularity we obtain a well-defined complex spectral decomposition of the time evolution for a quantum decaying system. In this formalism, generalized Gamow states are obtained with well-defined physical properties. 相似文献
20.
Zuo LIU Zhen De WU 《数学学报(英文版)》2005,21(5):997-1000
Let κ be non-negative integer. The unoriented bordism classes, which can be represented as [RP(ξ^κ)] where ξ^κ is a k-plane bundle, form an ideal of the unoriented bordism ring MO.. A group of generators of this ideal expressed by a base of MO. and a necessary and sufficient condition for a bordism class to belong to this ideal are given. 相似文献