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41.
Enzymatic Desymmetrising Redox Reactions for the Asymmetric Synthesis of Biaryl Atropisomers 下载免费PDF全文
Samantha Staniland Bo Yuan Nelson Giménez‐Agulló Dr. Tommaso Marcelli Dr. Simon C. Willies Dr. Damian M. Grainger Prof. Nicholas J. Turner Prof. Jonathan Clayden 《Chemistry (Weinheim an der Bergstrasse, Germany)》2014,20(41):13084-13088
Atropisomeric biaryls carrying ortho‐hydroxymethyl and formyl groups were made enantioselectively by desymmetrisation of dialdehyde or diol substrates. The oxidation of the symmetrical diol substrates was achieved using a variant of galactose oxidase (GOase), and the reduction of the dialdehydes using a panel of ketoreductases. Either M or P enantiomers of the products could be formed, with absolute configurations assigned by time‐dependent DFT calculations of circular dichroism spectra. The differing selectivities observed with different biaryl structures offer an insight into the detailed structure of the active site of the GOase enzyme. 相似文献
42.
Javier Mateos Francesco Rigodanza Alberto Vega‐Pealoza Andrea Sartorel Mirco Natali Tommaso Bortolato Giorgio Pelosi Xavier Company Marcella Bonchio Luca Dell'Amico 《Angewandte Chemie (International ed. in English)》2020,59(3):1302-1312
Twelve naphthochromenone photocatalysts (PCs) were synthesized on gram scale. They absorb across the UV/Vis range and feature an extremely wide redox window (up to 3.22 eV) that is accessible using simple visible light irradiation sources (CFL or LED). Their excited‐state redox potentials, PC*/PC.? (up to 1.65 V) and PC.+/PC* (up to ?1.77 V vs. SCE), are such that these novel PCs can engage in both oxidative and reductive quenching mechanisms with strong thermodynamic requirements. The potential of these bimodal PCs was benchmarked in synthetically relevant photocatalytic processes with extreme thermodynamic requirements. Their ability to efficiently catalyze mechanistically opposite oxidative/reductive photoreactions is a unique feature of these organic photocatalysts, thus representing a decisive advance towards generality, sustainability, and cost efficiency in photocatalysis. 相似文献
43.
Maurizi Enrici Tommaso Mertens Anne Sinnaeve Mario Tchuindjang Jérôme Tchoufang 《Journal of Thermal Analysis and Calorimetry》2020,141(3):1075-1089
Journal of Thermal Analysis and Calorimetry - In this work, a complex graphitic high-speed steel (Gr-HSS) obtained from a spin-casting process that allows high cooling rates during solidification... 相似文献
44.
L. F. Rojas M. Bina G. Cerchiari M. A. Escobedo-Sánchez F. Ferri F. Scheffold 《The European physical journal. Special topics》2011,199(1):167-180
We show that the spectral speckle intensity correlation (SSIC) technique can be profitably exploited to recover the path length
distribution of photons scattered in a random turbid medium. We applied SSIC to the study of Teflon slabs of different thicknesses
and were able to recover, via the use of the photon diffusion approximation theory, the characteristic transport mean free
path ℓ∗ and absorption length s
a
of the medium. These results were compared and validated by means of complementary measurements performed on the same samples
with standard pulsed laser time of flight techniques. 相似文献
45.
46.
The interplay of geometric randomness and strong quantum fluctuations is an exciting topic in quantum many-body physics, leading to the emergence of novel quantum phases in strongly correlated electron systems. Recent investigations have focused on the case of homogeneous site and bond dilution in the quantum antiferromagnet on the square lattice, reporting a classical geometric percolation transition between magnetic order and disorder. In this study we show how inhomogeneous bond dilution leads to percolative quantum phase transitions, which we have studied extensively by quantum Monte Carlo simulations. Quantum percolation introduces a new class of two-dimensional spin liquids, characterized by an infinite percolating network with vanishing antiferromagnetic order parameter. 相似文献
47.
Making use of exact results and quantum Monte Carlo data for the entanglement of formation, we show that the ground state of anisotropic two-dimensional S=1/2 antiferromagnets in a uniform field takes the classical-like form of a product state for a particular value and orientation of the field, at which the purely quantum correlations due to entanglement disappear. Analytical expressions for the energy and the form of such states are given, and a novel type of exactly solvable two-dimensional quantum models is therefore singled out. Moreover, we show that the field-induced quantum phase transition present in the models is unambiguously characterized by a cusp minimum in the pairwise-to-global entanglement ratio R, marking the quantum-critical enhancement of multipartite entanglement. 相似文献
48.
The field-induced antiferromagnetic ordering in systems of weakly coupled S = 1/2 dimers at zero temperature can be described as a Bose-Einstein condensation of triplet quasiparticles (singlet quasiholes) in the ground state. For the case of a Heisenberg bilayer, it is here shown how the above picture is altered in the presence of site dilution of the magnetic lattice. Geometric randomness leads to quantum localization of the quasiparticles or quasiholes and to an extended Bose-glass phase in a realistic disordered model. This localization phenomenon drives the system towards a quantum-disordered phase well before the classical geometric percolation threshold is reached. 相似文献
49.
We study the thermodynamics of the spin-S two-dimensional quantum Heisenberg antiferromagnet on the square lattice with nearest (J1) and next-nearest (J2) neighbor couplings in its collinear phase (J(2)/J(1)>0.5), using the pure-quantum self-consistent harmonic approximation. Our results show the persistence of a finite-temperature Ising phase transition for every value of the spin, provided that the ratio J(2)/J(1) is greater than a critical value corresponding to the onset of collinear long-range order at zero temperature. We also calculate the spin and temperature dependence of the collinear susceptibility and correlation length, and we discuss our results in light of the experiments on Li2VOSiO4 and related compounds. 相似文献
50.