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1.
Dake Hu Tianqi Zhao Xiaofan Ping Husong Zheng Lei Xing Xiaozhi Liu Jingying Zheng Lifei Sun Lin Gu Chenggang Tao Dong Wang Liying Jiao 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2019,131(21):7051-7055
Two‐dimensional (2D) PtSe2 shows the most prominent layer‐dependent electrical properties among various 2D materials and high catalytic activity for hydrogen evolution reaction (HER), and therefore, it is an ideal material for exploring the structure–activity correlations in 2D systems. Here, starting with the synthesis of single‐crystalline 2D PtSe2 with a controlled number of layers and probing the HER catalytic activity of individual flakes in micro electrochemical cells, we investigated the layer‐dependent HER catalytic activity of 2D PtSe2 from both theoretical and experimental perspectives. We clearly demonstrated how the number of layers affects the number of active sites, the electronic structures, and electrical properties of 2D PtSe2 flakes and thus alters their catalytic performance for HER. Our results also highlight the importance of efficient electron transfer in achieving optimum activity for ultrathin electrocatalysts. Our studies greatly enrich our understanding of the structure–activity correlations for 2D catalysts and provide new insight for the design and synthesis of ultrathin catalysts with high activity. 相似文献
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An integrated shape morphing and topology optimization approach based on the deformable simplicial complex methodology is developed to address Stokes and Navier‐Stokes flow problems. The optimized geometry is interpreted by a set of piecewise linear curves embedded in a well‐formed triangular mesh, resulting in a physically well‐defined interface between fluid and impermeable regions. The shape evolution is realized by deforming the curves while maintaining a high‐quality mesh through adaption of the mesh near the structural boundary, rather than performing global remeshing. Topological changes are allowed through hole merging or splitting of islands. The finite element discretization used provides smooth and stable optimized boundaries for simple energy dissipation objectives. However, for more advanced problems, boundary oscillations are observed due to conflicts between the objective function and the minimum length scale imposed by the meshing algorithm. A surface regularization scheme is introduced to circumvent this issue, which is specifically tailored for the deformable simplicial complex approach. In contrast to other filter‐based regularization techniques, the scheme does not introduce additional control variables, and at the same time, it is based on a rigorous sensitivity analysis. Several numerical examples are presented to demonstrate the applicability of the approach. 相似文献
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Low-flow chromatography has a rich history of innovation but has yet to reach widespread implementation in bioanalytical applications. Improvements in pump technology, microfluidic connections, and nano-electrospray sources for MS have laid the groundwork for broader application, and innovation in this space has accelerated in recent years. This article reviews the instrumentation used for nano-flow LC, the types of columns employed, and strategies for multidimensionality of separations, which are key to the future state of the technique to the high-throughput needs of modern bioanalysis. An update of the current applications where nano-LC is widely used, such as proteomics and metabolomics, is discussed. But the trend toward biopharmaceutical development of increasingly complex, targeted, and potent therapeutics for the safe treatment of disease drives the need for ultimate selectivity and sensitivity of our analytical platforms for targeted quantitation in a regulated space. The selectivity needs are best addressed by mass spectrometric detection, especially at high resolutions, and exquisite sensitivity is provided by nano-electrospray ionization as the technology continues to evolve into an accessible, robust, and easy-to-use platform. 相似文献
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Jing He Mohan Yu Maofu Pang Yanqing Fan Zhe Lian Dr. Ying Wang Prof. Wenguang Wang Prof. Yajun Liu Prof. Hua Jiang 《Chemistry (Weinheim an der Bergstrasse, Germany)》2022,28(13):e202103832
Structural designs combining cycloparaphenylenes (CPPs) backbone with planar chiral [2.2]paracyclophane ([2.2]PCP) lead to optical-active chiral macrocycles with intriguing properties. X-ray crystal analysis revealed aesthetic necklace-shaped structures and size-dependent packages with long-range channels. The macrocycles exhibit unique photophysical properties with high fluorescence quantum yield of up to 82 %, and the fluorescent color varies with ring size. In addition, size-dependent chiroptical properties with moderately large CPL dissymmetry factor of 10−3 and CPL brightness in the range of 30–40 M−1 cm−1 were observed. 相似文献
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Jie‐Lian Han Ying Qin Cheng‐Wei Ju Dongbing Zhao 《Angewandte Chemie (International ed. in English)》2020,59(16):6555-6560
Organosilicon compounds have been extensively utilized both in industry and academia. Studies on the syntheses of diverse organosilanes is highly appealing. Through‐space metal/hydrogen shifts allow functionalization of C?H bonds at a remote site, which are otherwise difficult to achieve. However, until now, an aryl to alkyl 1,5‐palladium migration process seems to have not been presented. Reported herein is the remote olefination, arylation, and borylation of a methyl group on silicon to access diverse vinyl‐, benzyl‐, and borylsilanes, constituting a unique C(sp3)?H transformation based on a 1,5‐palladium migration process. 相似文献
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为了确定ZrO2和(ZrO2)0.97(Bi2O3)0.03的晶体结构和原子热振动各向同性温度因子B,对该粉末晶体进行X射线衍射实验,建立了晶体结构模型,进行晶体结构分析。首先,采用共沉淀法和高温固相烧结法制备了纳米氧化锆ZrO2和(ZrO2)0.97(Bi2O3)0.03粉末晶体,接着,使用X射线测试仪对两种样品进行了衍射实验(XRD),利用Rietveld 精修方法的 RIETAN-2000程序对所得实验结果进行了晶体结构分析,获得了晶体结构参量和原子热振动各向同性温度因子B。通过Maximum Entropy Method(MEM)解析得到了粉末晶体(ZrO2)x(Bi2O3)1-x(x=1.0,0.97)的等高电子密度分布可视化图谱。结果表明,(ZrO2)0.97(Bi2O3)0.03的晶胞体积比ZrO2的晶胞体积大分别为140.6850 Å3和140.5637Å3;ZrO2晶体的原子热振动各向同性温度因子B(Zr)、BO(1)、BO(2)和 B(Bi)分别为0.690、0.269、 0.178 和 0 Å2,(ZrO2)0.97(Bi2O3)0.03晶体的分别为0.460 、0.583 、0.121 和0.581 Å2。 确定了(ZrO2)0.97(Bi2O3)0.03的晶体结构属于单斜晶系,实现了等高电子密度分布三维(3D)和二维(2D)的可视化,进一步确定了晶体结构和原子位置。 相似文献
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