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1.
Guanidine‐Based Polymer Brushes Grafted onto Silica Nanoparticles as Efficient Artificial Phosphodiesterases
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Claudia Savelli Riccardo Salvio 《Chemistry (Weinheim an der Bergstrasse, Germany)》2015,21(15):5856-5863
Polymer brushes grafted to the surface of silica nanoparticles were fabricated by atom‐transfer radical polymerization (ATRP) and investigated as catalysts in the cleavage of phosphodiesters. The surfaces of silica nanoparticles were functionalized with an ATRP initiator. Surface‐initiated ATRP reactions, in varying proportions, of a methacrylate moiety functionalized with a phenylguanidine moiety and an inert hydrophilic methacrylate species afforded hybrid nanoparticles that were characterized with potentiometric titrations, thermogravimetric analysis, and SEM. The activity of the hybrid nanoparticles was tested in the transesterification of the RNA model compound 2‐hydroxypropyl para‐nitrophenylphosphate (HPNP) and diribonucleoside monophosphates. A high catalytic efficiency and a remarkable effective molarity, thus overcoming the effective molarities previously observed for comparable systems, indicate the existence of an effective cooperation of the guanidine/guanidinium units and a high level of preorganization in the nanostructure. The investigated system also exhibits a marked and unprecedented selectivity for the diribonucleoside sequence CpA. The results presented open up the way for a novel and straightforward strategy for the preparation of supramolecular catalysts. 相似文献
2.
R. Pizzoferrato L. Lagonigro T. Ziller A. Di Carlo R. Paolesse F. Mandoj A. Ricci C. Lo Sterzo 《Chemical physics》2004,300(1-3):217-225
We study the infrared emission at 1.54 μm of an organolanthanide complex, Er(III)-tetraphenylporphyrin [Er(TPP)acac], both as a result of direct optical excitation and via energy transfer from host π-conjugate polymers of type poly(arylene–ethynylene) [PAE]. In the first case, the emission of the neat complex is characterized in inert transparent materials and a value of the quantum yield at 1.54 μm φIR=4×10−4 is measured. Then, fluorescence resonance transfer is investigated in blends of Er(TPP)acac with PAEs by monitoring the quenching of the polymer fluorescence along with the enhancement of both the visible emission of the ligand and the near-infrared band of Er3+. These different procedures allow a detailed analysis of the transfer efficiency within a specific implementation of the Förster model for polymeric donors. The experimental values of the critical radius R0, ranging from 1.3 to 2.5 nm for the different blends, are in good agreement with theory for a wide interval of the physical and spectroscopic parameters. This suggests that other mechanisms for excitation transfer do not play a significant role in these materials. 相似文献
3.
Some nickel, copper, and silver salts or complexes are efficient catalysts for the oxidation of benzylic ethers with oxygen in 1,2-dimethoxyethane. Salts of the weakly coordinating anion trifluoroacetate are particularly efficient, approaching (and, in some cases, improving) the yields obtained with cobalt(II) chloride, the best catalyst so far reported. 相似文献
4.
D. Guidotti J. G. Wilman A. J. Ricci 《Applied Physics A: Materials Science & Processing》1992,54(6):570-573
An instrument is described that can be used to monitor, with unprecedented sensitivity, changes in the optical reflectivity due to crystailine damage incurred during ion implantation. It is shown that at the shot-noise limit, changes in the optical reflectivity of silicon as small as 5·10–7 can be measured in a 10 Hz bandwidth with a signal-to-noise ratio of 100, corresponding to an extrapolated uniform implantation dose of 5·108 cm–2 for 11B+ at 50 keV in silicon. 相似文献
5.
Riccardo Rosso André M. Sonnet Epifanio G. Virga 《Continuum Mechanics and Thermodynamics》2002,14(1):127-136
kinks created in a biological membrane by the interaction with a movable bead. We arrive at the evolution equations for both the
bead and the membrane, whence we conclude that the force exerted on the bead by a fixed membrane points in the direction along
which the curvature of the membrane is more concentrated. This is the first step towards understanding the basic mechanism
behind the dynamics of protein aggregation which takes place on biological membranes.
Received November 6, 2001 / Published online February 4, 2002 相似文献
6.
7.
J. Walz S. B. Ross C. Zimmermann L. Ricci M. Prevedelli T. W. Hänsch 《Hyperfine Interactions》1996,100(1):133-144
Experiments with electrons and ions in a combined trap are reported. The unique capability to confine particles with opposite charge and very different mass simultaneously in the same spatial region makes the combined trap a promising device for future synthesis of antihydrogen. 相似文献
8.
P. Boccaccio L. Vannucci R.A. Ricci G. Vannini R. Dona I. Massa J.P. Coffin P. Fintz G. Guillaume F. Jundt F. Rami P. Wagner 《The European Physical Journal A - Hadrons and Nuclei》1998,1(4):399-406
We studied the sequential binary decay of the systems 32S+45Sc, 76Ge, 89Y, 59Co, 63Cu and 19F+63Cu induced by collisions at ≃6 MeV·A. The two stages of the process have reaction-times compatible with the dynamics of different mechanisms. The study of the
excitation energy partition shows that the reaction mechanism of the first step has influence on the de-excitation of the
primary fragments producing two decay components which have different time scale.
Received: 25 March 1997 / Revised version: 2 December 1997 相似文献
9.
Riccardo De Arcangelis 《Annali dell'Universita di Ferrara》1989,35(1):135-145
Summary Letf: (x, z)∈R
n×Rn→f(x, z)∈[0, +∞] be measurable inx and convex inz.
It is proved, by an example, that even iff verifies a condition as|z|
p≤f(x, z)≤Λ(a(x)+|z|q) with 1<p<q,a∈L
loc
s
(R
n),s>1, the functional
that isL
1(Ω)-lower semicontinuous onW
1,1(Ω), does not agree onW
1,1(Ω) with its relaxed functional in the topologyL
1(Ω) given by inf
Riassunto Siaf: (x, z)∈R n×Rn→f(x, z)∈[0, +∞] misurabile inx e convessa inz. Si mostra con un esempio che anche sef verifica una condizione del tipo|z| p≤f(x, z)≤Λ(a(x)+|z|q) con 1<p<q,a∈L loc s (R n),s>1, il funzionale , che èL 1(Ω)-semicontinuo inferiormente suW 1,1(Ω), non coincide suW 1,1(Ω) con il suo funzionale rilassato nella topologiaL 1(Ω) definito da inf相似文献
10.
Sandro Faetti Leone Fronzoni Paolo Grigolini Riccardo Mannella 《Journal of statistical physics》1988,52(3-4):951-978
It is shown that the Fokker-Planck operator can be derived via a projection-perturbation approach, using the repartition of a more detailed operator into a perturbation
1 and an unperturbed part
0. The standard Fokker-Planck structure is recovered at the second order in
1, whereas the perturbation terms of higher order are shown to provoke the breakdown of this structure. To get rid of these higher order terms, a key approximation, local linearization (LL), is made. In general, to evaluate at the second order in
1 the exact expression of the diffusion coefficient which simulates the influence of a Gaussian noise with a finite correlation time, a resummation up to infinite order in must be carried out, leading to what other authors call the best Fokker-Planck approximation (BFPA). It is shown that, due to the role of terms of higher order in
1, the BFPA leads to predictions on the equilibrium distributions that are reliable only up to the first order in t. The LL, on the contrary, in addition to making the influence of terms of higher order in
1 vanish, results in a simple analytical expression for the term of second order that is formally coincident with the complete resummation over all the orders in t provided by the Fox theory. The corresponding diffusion coefficient in turn is shown to lead in the limiting case to exact results for the steady-state distributions. Therefore, over the whole range 0 the LL turns out to be an approximation much more accurate than the global linearization proposed by other authors for the same purpose of making the terms of higher order in
1 vanish. In the short- region the LL leads to results virtually coincident with those of the BFPA. In the large- region the LL is a more accurate approximation than the BFPA itself. These theoretical arguments are supported by the results of both analog and digital simulation. 相似文献