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61.
Dr. Guobin Wen Dr. Bohua Ren Dr. Moon G. Park Dr. Jie Yang Dr. Haozhen Dou Dr. Zhen Zhang Dr. Ya-Ping Deng Prof. Zhengyu Bai Prof. Lin Yang Prof. Jeff Gostick Prof. Gianluigi A. Botton Prof. Yongfeng Hu Prof. Zhongwei Chen 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(31):12960-12967
Simultaneously improving energy efficiency (EE) and material stability in electrochemical CO2 conversion remains an unsolved challenge. Among a series of ternary Sn-Ti-O electrocatalysts, 3D ordered mesoporous (3DOM) Sn0.3Ti0.7O2 achieves a trade-off between active-site exposure and structural stability, demonstrating up to 71.5 % half-cell EE over 200 hours, and a 94.5 % Faradaic efficiency for CO at an overpotential as low as 430 mV. DFT and X-ray absorption fine structure analyses reveal an electron density reconfiguration in the Sn-Ti-O system. A downshift of the orbital band center of Sn and a charge depletion of Ti collectively facilitate the dissociative adsorption of the desired intermediate COOH* for CO formation. It is also beneficial in maintaining a local alkaline environment to suppress H2 and formate formation, and in stabilizing oxygen atoms to prolong durability. These findings provide a new strategy in materials design for efficient CO2 conversion and beyond. 相似文献
62.
Raphael Bigler Kyle A. Mack Jeff Shen Paolo Tosatti Chong Han Stephan Bachmann Haiming Zhang Michelangelo Scalone Andreas Pfaltz Scott E. Denmark Stefan Hildbrand Francis Gosselin 《Angewandte Chemie (International ed. in English)》2020,59(7):2844-2849
Asymmetric hydrogenation has evolved as one of the most powerful tools to construct stereocenters. However, the asymmetric hydrogenation of unfunctionalized tetrasubstituted acyclic olefins remains the pinnacle of asymmetric synthesis and an unsolved challenge. We report herein the discovery of an iridium catalyst for the first, generally applicable, highly enantio‐ and diastereoselective hydrogenation of such olefins and the mechanistic insights of the reaction. The power of this chemistry is demonstrated by the successful hydrogenation of a wide variety of electronically and sterically diverse olefins in excellent yield and high enantio‐ and diastereoselectivity. 相似文献
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Jeff Kahn 《Proceedings of the American Mathematical Society》2002,130(2):371-378
For -regular, -vertex bipartite graphs with bipartition , a precise bound is given for the sum over independent sets of the quantity . (In other language, this is bounding the partition function for certain instances of the hard-core model.) This result is then extended to graded partially ordered sets, which in particular provides a simple proof of a well-known bound for Dedekind's Problem given by Kleitman and Markowsky in 1975.
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We exploit the approximate (broken) symmetries of time translation, time reversal, and Hamiltonian structure to obtain general scaling laws governing the process of pattern formation in weakly damped Faraday waves. Using explicit parameter symmetries we determine, for the case of two-frequency forcing, how the strength of observed three-wave interactions depends on the frequency ratio and on the relative phase of the two driving terms. These symmetry-based predictions are verified for numerically calculated coefficients, and help explain the results of recent experiments. 相似文献
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We present a model for a synthetic gene oscillator and consider the coupling of the oscillator to a periodic process that is intrinsic to the cell. We investigate the synchronization properties of the coupled system, and show how the oscillator can be constructed to yield a significant amplification of cellular oscillations. We reduce the driven oscillator equations to a normal form, and analytically determine the amplification as a function of the strength of the cellular oscillations. The ability to couple naturally occurring genetic oscillations to a synthetically designed network could lead to possible strategies for entraining and/or amplifying oscillations in cellular protein levels. 相似文献
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Erickson JK Caldwell RR Steinhardt PJ Armendariz-Picon C Mukhanov V 《Physical review letters》2002,88(12):121301
Quintessence, a time-varying energy component that may account for the accelerated expansion of the universe, can be characterized by its equation of state and sound speed. In this paper, we show that if the quintessence density is at least 1% of the critical density at the surface of last scattering the cosmic microwave background anisotropy can distinguish between models whose sound speed is near the speed of light versus near zero, which could be useful in distinguishing competing candidates for dark energy. 相似文献
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In hamiltonian lattice gauge theory, the fermion vacuum at lowest order in 1/g2 can be determined from degenerate perturbation theory plus mean field-spin wave techniques. Using compact QED as an example, we show that: (i) chiral symmetry is spontaneously broken; and (ii) . The pseudoscalar pseudoGoldstone particles—the “pions” of this abelian theory—correspond to antiferromagnetic spin wave excitations of the fermion vacuum. 相似文献