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首页> 外文期刊>The journal of physical chemistry, C. Nanomaterials and interfaces >Resolving Detonation Nanodiamond Size Evolution and Morphology at Sub-Microsecond Timescales during High-Explosive Detonations
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Resolving Detonation Nanodiamond Size Evolution and Morphology at Sub-Microsecond Timescales during High-Explosive Detonations

机译：在高爆炸爆炸期间解决亚微秒时间尺寸的爆炸纳米胺大小演化与形态

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Characterization of the initial morphology of detonation nanodiamond (DND) has been the focus of many research studies that aim to develop a fundamental under-standing of carbon condensation under extreme conditions. Identifying the pathways of DND formation has the potential for significant impact on many of the controlled synthesis of nanoscale carbon with a tailored functionality; currently, a wide range of possible (and conflicting) mechanisms of nucleation and growth have been proposed, and further research is essential. Building a comprehensive understanding of DND formation is challenging because it requires in situ characterization on the sub-microsecond (sub-mu s) timescale during a high-explosive detonation. In this study, time-resolved small-angle X-ray scattering (TR-SAXS) is used to reveal the early-stage DND morphology from <0.1 to 6 mu s after the detonation front passes through the X-ray beam path. We address the ambiguity of models previously reported for the analysis of small-angle scattering from DND by comparing (i) in situ, TR-SAXS recorded during early-stage particulate formation and (ii) ex situ SAXS and transmission electron microscopy (TEM) measurements of products recovered from detonation of the same high explosive within a carefully designed ice chamber. The SAXS from both late-time (>1 mu s) in situ and recovered DND exhibits consistent features in the I(q) curve. Such a close similarity allows a high-fidelity SAXS model derived from the ex situ SAXS and TEM measurements to be applied to the in situ data, which yields new insight into the early-stage (<1 mu s) morphology of DND. Our analysis indicates that the size distribution of DND particles is observed within 0.1 /is postdetonation, which indicates that carbon is condensed within the reaction zone. Between 0.1 and 0.3 mu s, the mean size of the diamond particles increases slightly toward 4 nm, and evidence of surface texture is observed. Based on TEM imaging, this surface texture consists of hemispherical protrusions that extend similar to 1 nm from the surface. Beyond 0.3 mu s, neither the mean size of the diamond core nor the surface texture changes significantly for several microseconds after the detonation. Combined with thermochemical simulations, these results indicate that during detonation of composition B, carbon is condensed into nanoscale diamond much faster than that previously reported in other studies. Furthermore, the surface texture of the DND is shown to arise during condensation rather than via subsequent graphitization.
机译：爆炸纳米金刚胺（DND）的初始形态的表征是许多研究研究的焦点，旨在在极端条件下在极端条件下发展碳凝结的基本潜伏。鉴定DND形成的途径具有对许多对纳米碳碳的许多对纳米碳碳的途径产生重大影响的可能性;目前，已经提出了各种可能的（和矛盾）的成核和生长机制，进一步研究至关重要。建立对DND形成的全面了解是具有挑战性的，因为它需要在高爆炸爆炸期间对亚微秒（子MU S）时间尺度的原位表征。在该研究中，时间分辨的小角X射线散射（TR-SAX）用于在爆炸前沿通过X射线束路径之后从<0.1至6μs中揭示早期DND形态。我们通过比较（i）原位，在早期颗粒形成期间的原位，TR-SAXS和透射电子显微镜（TEM）以原位，TR-SAX来解决从DND的小角度散射分析的模型的模型的模特的模拟。在精心设计的冰室内从爆炸中回收的产品的测量。来自后期（>1μs）的淋巴原位和恢复的DND在I（Q）曲线中表现出一致的特征。这种近似相似性允许从EX原位SAXS和TEM测量导出的高保真萨克斯模型以应用于原位数据，这产生了进入DND的早期（<1μs）形态的新洞察。我们的分析表明，在0.1 /是后，观察到DND颗粒的尺寸分布，这表明碳在反应区内凝结。在0.1和0.3μs之间，金刚石颗粒的平均尺寸略微增加到4nm，并且观察到表面纹理的证据。基于TEM成像，该表面纹理由半球形突起组成，该半球形突起从表面延伸到1nm。超过0.3亩，钻石核心的平均尺寸和表面纹理在爆炸后几微秒的变化显着变化。结合热化学模拟，这些结果表明，在组合物B的爆炸期间，碳浓缩成纳米级金刚石，比以前在其他研究中报道的纳米级钻石。此外，DND的表面纹理被示出在冷凝期间出现在冷凝期间而不是通过后续的石墨化。

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