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利用原位X射线散射深入了解CdSe纳米片的形成机制

Insights into the Formation Mechanism of CdSe Nanoplatelets Using in Situ X-ray Scattering.

作者信息

Castro Nicolo, Bouet Cécile, Ithurria Sandrine, Lequeux Nicolas, Constantin Doru, Levitz Pierre, Pontoni Diego, Abécassis Benjamin

机构信息

Laboratoire de Physique des Solides , CNRS, Univ. Paris-Sud, Université Paris-Saclay , 91405 Orsay Cedex , France.

Laboratoire de Physique et d'Etude des Matériaux, ESPCI-Paris, PSL Research University , Sorbonne Université, CNRS , 10 rue Vauquelin 75005 , Paris , France.

出版信息

Nano Lett. 2019 Sep 11;19(9):6466-6474. doi: 10.1021/acs.nanolett.9b02687. Epub 2019 Aug 27.

Abstract

Two-dimensional ultrathin CdSe nanoplatelets have attracted a large interest due to their optical properties but their formation mechanism is not well understood. Several different mechanisms have been proposed: confined growth in a surfactant mesophase acting as a template, anisotropic ripening of small seeds into 2D nanoplatelets, or continuous anisotropic growth of a limited number of nuclei. However, quantitative in situ data that could validate or disprove these formation scenarios are lacking. We use synchrotron-based small-angle and wide-angle X-ray scattering to probe the formation mechanism of CdSe nanoplatelets synthesized using a heating-up method. We prove the absence of a molecular mesophase in the reactive medium at the onset of nanoplatelet formation ruling out a templating effect. We also show that our data are inconsistent with the anisotropic ripening of small seeds whereas the evolution of the SAXS patterns during the reaction is consistent with the continuous lateral growth of nanoplatelets fed by reactive monomers. Finally, we show that when the final temperature of the synthesis is lowered, nanoplatelets with larger lateral dimensions form. We reveal that they bend in solution during their growth to yield nanoscrolls.

摘要

二维超薄硒化镉纳米片因其光学性质而备受关注,但其形成机制尚未完全明确。目前已提出了几种不同的机制:在作为模板的表面活性剂中间相中受限生长、小晶种向二维纳米片的各向异性熟化,或有限数量晶核的连续各向异性生长。然而,缺乏能够验证或反驳这些形成过程的定量原位数据。我们利用基于同步加速器的小角和广角X射线散射来探究采用升温法合成的硒化镉纳米片的形成机制。我们证明在纳米片形成开始时反应介质中不存在分子中间相,排除了模板效应。我们还表明,我们的数据与小晶种的各向异性熟化不一致,而反应过程中SAXS图案的演变与由反应性单体提供的纳米片的连续横向生长一致。最后,我们表明当合成的最终温度降低时,会形成横向尺寸更大的纳米片。我们发现它们在生长过程中在溶液中弯曲形成纳米卷轴。

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