Resolving Single-layer Nanosheets as Short-lived Intermediates in the Solution Synthesis of FeS,ACS Materials Letters

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Resolving Single-layer Nanosheets as Short-lived Intermediates in the Solution Synthesis of FeS
ACS Materials Letters ( IF 9.6 ) Pub Date : 2021-04-27 , DOI: 10.1021/acsmaterialslett.1c00193
Michelle L. Beauvais ₁ , Peter J. Chupas ₁ , Daniel O’Nolan ₁ , John B. Parise _{1,

2} , Karena W. Chapman ₁

Affiliation

Short-lived reaction intermediates play a critical role in mediating material synthesis. Such short-lived species often elude characterization because of the mismatch between the time scale of measurements capable of describing them and their lifetimes. Thus, we have limited ability to probe, understand, and control the mechanism for material synthesis. Here we demonstrate a new approach to in situ X-ray pair distribution function (PDF) measurements of dynamic nanomaterials structure that yields an unprecedented combination of reaction time resolution and sensitivity. Reaction time is resolved spatially as a function of position along a flow path. By applying this approach to the well-studied aqueous reaction leading to FeS, mackinawite, we identify a novel metastable intermediate, FeS_layer, that forms in the first second of the reaction and which can be described as individual FeS nanosheets. Recognizing these nanosheets as synthons in the reaction opens up the possibility to deliberately redirect this assembly of the nanosheet toward different phases, including novel heterostructures.

中文翻译：

在 FeS 溶液合成中将单层纳米片解析为短寿命中间体

短寿命反应中间体在介导材料合成中起着关键作用。由于能够描述它们的测量时间尺度与其寿命之间的不匹配，这种短命物种通常无法表征。因此，我们探测、理解和控制材料合成机制的能力有限。在这里，我们展示了一种对动态纳米材料结构进行原位X 射线对分布函数 (PDF) 测量的新方法，该方法产生了前所未有的反应时间分辨率和灵敏度组合。反应时间在空间上被解析为沿流动路径的位置的函数。通过将这种方法应用于导致 FeS、mackinawite 的经过充分研究的水性反应，我们确定了一种新的亚稳态中间体 FeS_层，它在反应的第一秒形成，可以描述为单独的 FeS 纳米片。将这些纳米片识别为反应中的合成子开辟了将纳米片的这种组装重新定向到不同相（包括新型异质结构）的可能性。

更新日期：2021-06-07

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