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81.
Due to the rigid structure of 1,3,5-triaza-7-phosphaadamantane (PTA), its 31P chemical shift solely depends on non-covalent interactions in which the molecule is involved. The maximum range of change caused by the most common of these, hydrogen bonding, is only 6 ppm, because the active site is one of the PTA nitrogen atoms. In contrast, when the PTA phosphorus atom is coordinated to a metal, the range of change exceeds 100 ppm. This feature can be used to support or reject specific structural models of organometallic transition metal complexes in solution by comparing the experimental and Density Functional Theory (DFT) calculated values of this 31P chemical shift. This approach has been tested on a variety of the metals of groups 8–12 and molecular structures. General recommendations for appropriate basis sets are reported. 相似文献
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本文针对坡莫合金椭圆形盘中的磁涡旋结构, 采用微磁学模拟与傅里叶分析相结合的技术研究了磁涡旋自旋波的本征激发模式. 通过沿样品短轴方向施加一面内方向的脉冲磁场, 观察到一系列方位角自旋波模式. 观察到的自旋波模式具有两重对称性, 可以通过C2群理论来进行类型的划分. 此外, 自旋波模式的频率随着方位角指标的变化而线性增加. 模拟结果显示样品的平均交换能量密度明显的高于平均静磁能量密度; 局域交换能量密度主要集中在涡核初始位置, 而局域静磁能量密度主要分布在长轴附近. 交换作用对受限于铁磁薄膜椭圆盘中的单个涡旋态的能量要起主导作用, 从而导致方位角自旋波模式频率随着方位角指标的增加而增加. 相似文献
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《中国化学快报》2020,31(7):1970-1973
The biogeochemical transformation of gold (Au), i.e. its dissolution and re-precipitation, is critical in supergene transport of Au and formation of Au granules. Besides biogenic reduction, the formation Au granules can also be driven by chemical processes. Previous studies have showed the formation of Au nanoparticles (AuNPs) from ionic Au(III) can be mediated by dissolved organic matter under sunlight. In this letter, we further demonstrated that these AuNPs can further slowly (in years) grow into visible Au granules. Different sized nano-flower and fractal dendrite-like branched gold structures (from tens of nanometres to over 100 μm) were observed in the Au granule sample. This growth of AuNPs into visible Au granules may play a critical role in the supergene mineralization and enrichment of secondary Au and drive the biogeochemical cycle of Au. 相似文献
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在生物体内到处都是由蛋白质、核酸和多糖等生物大分子构成的各种不同生物凝聚态物质,这些生物凝聚态物质形成不同的高级结构,执行不同的生物功能。获取这些生物凝聚态物质的高分辨结构是理解生命过程的重要途径。在离体环境中,获取高分辨结构的手段主要有X-射线晶体衍射、冷冻电镜和核磁共振等,而在活细胞内原位研究生物凝聚体的结构,核磁共振和化学交联质谱具有独特优势。本文总结了利用多种分析手段对生物凝聚态物质进行多层次结构表征的研究进展:包括简单纯化体系下的蛋白质分子机器,蛋白质纤维等;液-液相分离,大分子拥挤、限域等模拟细胞复杂环境下的生物大分子以及活细胞内生物大分子。 相似文献
87.
Dissolved organic matter is an important component of the global carbon cycle that allows the distribution of carbon and nutrients. Therefore, analysis of soil dissolved organic matter helps us to better understand climate change impacts as it is the most dynamic and reactive fraction in terrestrial ecosystems. Its characterization at the molecular level is still challenging due to complex mixtures of hundreds of compounds at low concentration levels in percolating water. This work presents simple methods, such as thermochemolysis– or derivatization–gas chromatography, as an alternative for the analysis of fatty acids in dissolved organic matter without any purification step. The variables of the protocols were examined to optimize the processing conditions for the C9–C18 range. As a proof of concept, fatty acid distributions of soil percolating water samples from a long-term field experiment were successfully assessed. The variability of dissolved organic acid distributions was pronounced through depth profile and soil treatment but no major change in composition was observed. However, although the optimization was done from C9 to C18, detection within the C6-C32 fatty acids range was performed for all samples. 相似文献
88.
Yantao Pang Anoop Thomas Kalaivanan Nagarajan Robrecht M. A. Vergauwe Kripa Joseph Bianca Patrahau Kuidong Wang Cyriaque Genet Thomas W. Ebbesen 《Angewandte Chemie (International ed. in English)》2020,59(26):10436-10440
It is well known that symmetry plays a key role in chemical reactivity. Here we explore its role in vibrational strong coupling (VSC) for a charge‐transfer (CT) complexation reaction. By studying the trimethylated‐benzene–I2 CT complex, we find that VSC induces large changes in the equilibrium constant KDA of the CT complex, reflecting modifications in the ΔG° value of the reaction. Furthermore, by tuning the microfluidic cavity modes to the different IR vibrations of the trimethylated benzene, ΔG° either increases or decreases depending only on the symmetry of the normal mode that is coupled. This result reveals the critical role of symmetry in VSC and, in turn, provides an explanation for why the magnitude of chemical changes induced by VSC are much greater than the Rabi splitting, that is, the energy perturbation caused by VSC. These findings further confirm that VSC is powerful and versatile tool for the molecular sciences. 相似文献
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