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1.
Dr. Haiyuan Zou Gang Zhao Hao Dai Dr. Hongliang Dong Wen Luo Prof. Lei Wang Prof. Zhouguang Lu Prof. Yi Luo Dr. Guozhen Zhang Prof. Lele Duan 《Angewandte Chemie (International ed. in English)》2023,62(6):e202217220
Fine-tuning electronic structures of single-atom catalysts (SACs) plays a crucial role in harnessing their catalytic activities, yet challenges remain at a molecular scale in a controlled fashion. By tailoring the structure of graphdiyne (GDY) with electron-withdrawing/-donating groups, we show herein the electronic perturbation of Cu single-atom CO2 reduction catalysts in a molecular way. The elaborately introduced functional groups (−F, −H and −OMe) can regulate the valance state of Cuδ+, which is found to be directly scaled with the selectivity of the electrochemical CO2-to-CH4 conversion. An optimum CH4 Faradaic efficiency of 72.3 % was achieved over the Cu SAC on the F-substituted GDY. In situ spectroscopic studies and theoretical calculations revealed that the positive Cuδ+ centers adjusted by the electron-withdrawing group decrease the pKa of adsorbed H2O, promoting the hydrogenation of intermediates toward the CH4 production. Our strategy paves the way for precise electronic perturbation of SACs toward efficient electrocatalysis. 相似文献
2.
设Xi是无穷维复Banach空间, L(Xj,Xi)是Xj到Xi上的有界线性算子全体.考虑 n × n 上三角算子矩阵T=(Tij)1≤j≤n, 其中Tij L(Xj,Xi),1≤j≤n; Tij=0, i>j.本文研究了T的单值扩张性, 通过考察集合S(T)={λ∈C}: T在点λ没有SVEP},证明了S(T)在i=1 ? nS(Ti)中退化,进而给出等式S(T)=i=1 ? n S(Ti)成立的条件. 同时, 考察了T的单值扩张性扰动,得到了S(T)保持对角稳定时Ti所需的条件并予以证明, 同时举例说明这些条件的合理性.最后, 给出单值扩张性关于谱σ(T)和局部谱σT (x)的应用, 得到了谱扰动和局部谱扰动不变的新条件. 相似文献
3.
Mehmet Çevik 《International Journal of Non》2005,40(6):901-923
Non-linear coupled vertical and torsional vibrations of suspension bridges are investigated. Method of Multiple Scales, a perturbation technique, is applied to the equations to find approximate analytical solutions. The equations are not discretized as usually done, rather the perturbation method is applied directly to the partial differential equations. Free and forced vibrations with damping are investigated in detail. Amplitude and phase modulation equations are obtained. The dependence of non-linear frequency on amplitude is described. Steady-state solutions are analyzed. Frequency-response equation is derived and the jump phenomenon in the frequency-response curves resulting from non-linearity is considered. Effects of initial amplitude and phase values, amplitude of excitation, and damping coefficient on modal amplitudes, are determined. 相似文献
4.
J.C. Umavathi 《International Journal of Non》2005,40(1):91-101
The problem of combined free and forced convective magnetohydrodynamic flow in a vertical channel is analysed by taking into account the effect of viscous and ohmic dissipations. The channel walls are maintained at equal or at different constant temperatures. The velocity field and the temperature field are obtained analytically by perturbation series method and numerically by finite difference technique. The results are presented for various values of the Brinkman number and the ratio of Grashof number to the Reynolds number for both equal and different wall temperatures. Nusselt number at the walls is determined. It is found that the viscous dissipation enhances the flow reversal in the case of downward flow while it counters the flow in the case of upward flow. It is also found that the analytical and numerical solutions agree very well for small values of ε. 相似文献
5.
This paper concerns the quadratically-damped Mathieu equation:
6.
Angelo Luongo 《Nonlinear dynamics》1996,10(4):317-331
Two perturbation methods for nonlinear autonomous discrete-time dynamical systems are presented. They generalize the classical Lindstedt-Poincaré and multiple scale perturbation methods that are valid for continuous-time systems. The Lindstedt-Poincaré method allows determination of the periodic or almost-periodic orbits of the nonlinear system (limit cycles), while the multiple scale method also permits analysis of the transient state and the stability of the limit cycles. An application to the discrete Van der Pol equation is also presented, for which the asymptotic solution is shown to be in excellent agreement with the exact (numerical) solution. It is demonstrated that, when the sampling step tends to zero the asymptotic transient and steady-state discrete-time solutions correctly tend to the asymptotic continuous-time solutions. 相似文献
7.
We consider singular perturbation problems depending on a parameter ε?0 such that for ε>0 the solution uε belongs to a Sobolev space on a domain , but the limit u0 is not a distribution on . A very simple model problem, solvable by Fourier transform allows us to study the complexification process of uε as . The limit holds in the topology of a space of analytical functionals. To cite this article: C.A. De Souza, É. Sanchez-Palencia, C. R. Mecanique 332 (2004). 相似文献
8.
本文对中心带轴匀速旋转圆盘在均布压力作用下的受力及变形问题进行了摄动分析,得到了受载条件为J^2/JH<<1时,圆盘应力及形变的渐近解。其形变渐近解为Whitaker函数形式比较表明,渐近解与Chebyshev数值解有较好的一致性。 相似文献
9.
10.
《Physics letters. A》2019,383(19):2339-2345