Ultrahigh Loading Copper Single Atom Catalyst for Palladium-free Wacker Oxidation

Wacker oxidation is an industry-adopted process to transform olefins into value-added epoxides and carbonyls. However, traditional Wacker oxidation involves the use of homogeneous palladium and copper catalysts for the olefin addition and reductive elimination. Here, we demonstrated an ultrahigh loading Cu single atom catalyst(14% Cu, mass fraction) for the palladium-free Wacker oxidation of 4-vinylanisole into the corresponding ketone with N-methylhydroxylamine hydrochloride as an additive under mild conditions. Mechanistic studies by ¹⁸O and deuterium isotope labelling revealed a hydrogen shift mechanism in this palladium-free process using N-methylhydroxylamine hydrochloride as the oxygen source. The reaction scope can be further extended to Kucherov oxidation. Our study paves the way to replace noble metal catalysts in the traditional homogeneous processes with single atom catalysts.     

Lagrangian for the t–J Model Constructed from the Generators of the Supersymmetric Hubbard Algebra

In order to describe the dynamics of the t–J model, two different families of first-order Lagrangians in terms of the generators of the Hubbard algebra are found. Such families correspond to different dynamical second-class constrained systems. The quantization is carried out by using the path-integral formalism. In this context the introduction of proper ghost fields is needed to render the model renormalizable. In each case the standard Feynman diagrammatics is obtained and the renormalized physical quantities are computed and analyzed. In the first case a nonperturbative large-N expansion is considered with the purpose of studying the generalized Hubbard model describing N-fold-degenerate correlated bands. In this case the 1/N correction to the renormalized boson propagator is computed. In the second case the perturbative Lagrangian formalism is developed and it is shown how propagators and vertices can be renormalized to each order. In particular, the renormalized ferromagnetic magnon propagator coming from our formalism is studied in details. As an example the thermal softening of the magnon frequency is computed. The antiferromagnetic case is also analyzed, and the results are confronted with previous one obtained by means of the spin-polaron theories.     

SPECTRUM-PRESERVING ELEMENTARY OPERATORS ON B（X）

1.IntroductionLetXbeaninfinitedimensionalcomplexBanachspaceandB(X)theBanachalgebraofallboundedlinearoperatorsonX.ForTEB(X),a(T),asusual,willdenotethespectrumofT.Let4bealinearmapfromB(X)intoitself.4isspectrum-preservingifa(di(T))=a(T)forallTEB(X);4isspectrum-compressingifa(4(T))ga(T)forallTEB(X).Itisclearthatif4isunital(i.e.,ac(I)=I),thenacisspectrum-preserving(spectrum-compressing)ifandonlyif4preservesinvertibilityinbothdirections(preservesinvertibility),i.e.,4(T)isinvertibleifando…     

Spectra and Transport in Almost Periodic Dimers

We study spectral properties of discrete Schrödinger operators with potentials obtained via dimerization of a class of aperiodic sequences. It is shown that both the nature of the autocorrelation measure of a regular sequence and the presence of generic (full probability) singular continuous spectrum in the hull of primitive and palindromic (four block substitution) potentials are robust under dimerization. Generic results also hold for circle potentials. We illustrate these results with numerical studies of the quantum mean square displacement as a function of time. The numerical techniques provide a very fast algorithm for the time evolution of wave packets.     

Wavelet Collocation Methods for a First Kind Boundary Integral Equation in Acoustic Scattering

In this paper we consider a wavelet algorithm for the piecewise constant collocation method applied to the boundary element solution of a first kind integral equation arising in acoustic scattering. The conventional stiffness matrix is transformed into the corresponding matrix with respect to wavelet bases, and it is approximated by a compressed matrix. Finally, the stiffness matrix is multiplied by diagonal preconditioners such that the resulting matrix of the system of linear equations is well conditioned and sparse. Using this matrix, the boundary integral equation can be solved effectively.     

Rank 2 Ample Vector Bundles on Some Smooth Rational Surfaces

Several classification results for ample vector bundles of rank 2 on Hirzebruch surfaces, and on Del Pezzo surfaces, are obtained. In particular, we classify rank 2 ample vector bundles with _c2 less than seven on Hirzebruch surfaces, and with _c2 less than four on Del Pezzo surfaces.     

An Improved Gradient Projection-based Decomposition Technique for Support Vector Machines

In this paper we propose some improvements to a recent decomposition technique for the large quadratic program arising in training support vector machines. As standard decomposition approaches, the technique we consider is based on the idea to optimize, at each iteration, a subset of the variables through the solution of a quadratic programming subproblem. The innovative features of this approach consist in using a very effective gradient projection method for the inner subproblems and a special rule for selecting the variables to be optimized at each step. These features allow to obtain promising performance by decomposing the problem into few large subproblems instead of many small subproblems as usually done by other decomposition schemes. We improve this technique by introducing a new inner solver and a simple strategy for reducing the computational cost of each iteration. We evaluate the effectiveness of these improvements by solving large-scale benchmark problems and by comparison with a widely used decomposition package.     

Well-Posedness by Perturbations of Variational Problems

In this paper, we consider the extension of the notion of well-posedness by perturbations, introduced by Zolezzi for optimization problems, to other related variational problems like inclusion problems and fixed-point problems. Then, we study the conditions under which there is equivalence of the well-posedness in the above sense between different problems. Relations with the so-called diagonal well-posedness are also given. Finally, an application to staircase iteration methods is presented.