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61.
Yinwu Li Jiahao Liu Dr. Xiao Huang Prof. Dr. Ling-Bo Qu Prof. Dr. Cunyuan Zhao Prof. Dr. Robert Langer Prof. Dr. Zhuofeng Ke 《Chemistry (Weinheim an der Bergstrasse, Germany)》2019,25(60):13785-13798
As a new type of bifunctional catalyst, the Lewis acid transition-metal (LA-TM) catalysts have been widely applied for hydrogen activation. This study presents a mechanistic framework to understand the LA-TM-catalyzed H2 activation through DFT studies. The mer(trans)-homolytic cleavage, the fac(cis)-homolytic cleavage, the synergetic heterolytic cleavage, and the dissociative heterolytic cleavage should be taken as general mechanisms for the field of LA-TM catalysis. Four typical LA-TM catalysts, the Z-type κ4-L3B-Rh complex tri(azaindolyl)borane-Rh, the X-type κ3-L2B-Co complex bis-phosphino-boryl (PBP)-Co, the η2-BC-type κ3-L2B-Pd complex diphosphine-borane (DPB)-Pd, and the Z-type κ2-LB-Pt complex (boryl)iminomethane (BIM)-Pt are selected as representative models to systematically illustrate their mechanistic features and explore the influencing factors on mechanistic variations. Our results indicate that the tri(azaindolyl)borane-Rh catalyst favors the synergetic heterolytic mechanism; the PBP-Co catalyst prefers the mer(trans)-homolytic mechanism; the DPB-Pd catalyst operates through the fac(cis)-homolytic mechanism, whereas the BIM-Pt catalyst tends to undergo the dissociative heterolytic mechanism. The mechanistic variations are determined by the coordination geometry, the LA-TM bonding nature, the electronic structure of the TM center, and the flexibility or steric effect of the LA ligands. The presented mechanistic framework should provide helpful guidelines for LA-TM catalyst design and reaction developments. 相似文献
62.
Experimental Mechanics - Identification of impact force is essential for various engineering applications, such as performance evaluation, design optimisation, noise suppression, and vibration... 相似文献
63.
Jie Li Prof. Dr. Shuanglin Qu Prof. Dr. Wanxiang Zhao 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(6):2380-2384
A rhodium-catalyzed remote C(sp3)−H borylation of silyl enol ethers (SEEs, E/Z mixtures) by alkene isomerization and hydroboration is reported. The reaction exhibits mild reaction conditions and excellent functional-group tolerance. This method is compatible with an array of SEEs, including linear and branched SEEs derived from aldehydes and ketones, and provides direct access to a broad range of structurally diverse 1,n-borylethers in excellent regioselectivities and good yields. These compounds are precursors to various valuable chemicals, such as 1,n-diols and aminoalcohols. 相似文献
64.
Dr. Yang Li Dr. Xinghua Guo Dr. Xiaofeng Li Dr. Meicheng Zhang Dr. Zhimin Jia Prof. Yun Deng Prof. Yin Tian Prof. Shoujian Li Prof. Lijian Ma 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(10):4197-4204
We report the first example of 2D covalent organic framework nanosheets (Redox-COF1) for the selective reduction and in situ loading of valence-variable, redox-sensitive and long-lived radionuclides (abbreviated as VRL nuclides). Compared with sorbents based on chemical adsorption and physical adsorption, the redox adsorption mechanism of Redox-COF1 can effectively reduce the impact of functional group protonation under the usual high-acidity conditions in chemisorption, and raise the adsorption efficiency from the monotonous capture by pores in physisorption. The adsorption selectivity for UO22+ reaches up to unprecedented ca. 97 % at pH 3, more than for any analogous adsorbing material. 相似文献
65.
66.
We fabricate Sm-doped Ca3Co4O9+δ(CCO)bulk materials in magnetic field during both processes of chemical synthesis and cold pressing.The structure and electrical performance of the samples are investigated.With the increasing Sm concentration,the electrical conductivity 1/ρ decreases and the Seebeck coefficientαincreases.As a result,the power factor(PF=α^2/ρ)is raised slightly.After applying magnetic field,the extent of texture,grain size and density of all the bulk materials are improved obviously,thereby an enhanced electrical conductivity can be gained.Additionally,the degeneracy of Co^4+ state in the CoO2 layer of CCO is also increased as the magnetic field is used in the preparing process,which results in an enhancedα.The Ca2.85Sm0.15Co4O9+δ prepared in magnetic field shows the largest power factor(0.20 mW·m^-1·K^-2 at 1073 K). 相似文献
67.
68.
We presented a microfabrication process for optical volume vortex grating inside glass by femtosecond laser pulses. The self-trapped filament of femtosecond laser pulses can induce hundreds μm-long region refractive-index changes in glass. We realized the restructured optical vortex beams using a collimated He–Ne laser beam. The maximum first-order diffraction efficiency was about 19.6%. The volume vortex grating structure fabricated in glass is polarization dependent. 相似文献
69.
We apply functional separation of variables within the approach of the group foliation method to the nonlinear wave equation with variable speed and external force: utt=A(x)(Dx(u)ux)+B(x)Q(u), Ax≠0. A classification of these equations admitting functionally separable solutions is performed and the resulting solutions are obtained in explicit form in many cases. 相似文献
70.
The forward current-voltage (I-V) characteristics of polycrystalline CoSi2/n-Si(100) Schottky contacts have been measured in a wide temperature range. At low temperatures (≤200K), a plateau-like section is observed in the I-V characteristics around 10-4A·cm-2. The current in the small bias region significantly exceeds that expected by the model based on thermionic emission (TE) and a Gaussian distribution of Schottky barrier height (SBH). Such a double threshold behaviour can be explained by the barrier height inhomogeneity, i.e. at low temperatures the current through some patches with low SBH dominates at small bias region. With increasing bias voltage, the Ohmic effect becomes important and the current through the whole junction area exceeds the patch current, thus resulting in a plateau-like section in the I-V curves at moderate bias. For the polycrystalline CoSi2/Si contacts studied in this paper, the apparent ideality factor of the patch current is much larger than that calculated from the TE model taking the pinch-off effect into account. This suggests that the current flowing through these patches is of the tunnelling type, rather than the thermionic emission type. The experimental I-V characteristics can be fitted reasonably well in the whole temperature region using the model based on tunnelling and pinch-off. 相似文献