Physics and Chemistry of Nanostructures, Ghent University, B-9000 Ghent, Belgium.
ACS Nano. 2013 Feb 26;7(2):943-9. doi: 10.1021/nn3059168. Epub 2013 Jan 24.
Various literature studies show that increasing the concentration of free acid in the hot injection synthesis of colloidal nanocrystals raises the diameter of the resulting nanocrystals. We analyze this reaction chemistry/nanocrystal property relation by combining reaction simulations with an experimental study on a particular CdSe nanocrystal synthesis. We find that increasing the free acid concentration has the same effect on a real synthesis as raising the solute solubility in the simulations. Both lead to larger sizes and a deterioration of the size dispersion at constant reaction rate. Since free acids are used to coordinate the cation precursors in these syntheses, this leads to a meaningful link between a parameter in reaction simulations and the composition of an experimental reaction mixture. We thus explain the increase of the nanocrystal size with the acid concentration as resulting from an enhanced consumption of the solute by nanocrystal growth, which reduces the number of nanocrystals formed. This link between a simulation parameter and the composition of the reaction mixture provides a rational basis to further explore and understand reaction chemistry/nanocrystal property relations in the hot injection synthesis.
各种文献研究表明,增加胶体纳米晶体热注射合成中游离酸的浓度会提高所得纳米晶体的直径。我们通过将反应模拟与对特定 CdSe 纳米晶体合成的实验研究相结合,来分析这种反应化学/纳米晶体性质关系。我们发现,增加游离酸浓度对实际合成的影响与提高模拟中溶质溶解度的影响相同。这两种情况都会导致在恒定反应速率下尺寸更大,尺寸分布恶化。由于在这些合成中游离酸用于配位阳离子前体,因此这在反应模拟中的参数与实验反应混合物的组成之间建立了有意义的联系。因此,我们将纳米晶体尺寸随酸浓度的增加解释为纳米晶体生长消耗更多溶质,从而减少了形成的纳米晶体数量的结果。这种模拟参数与反应混合物组成之间的联系为进一步探索和理解热注射合成中的反应化学/纳米晶体性质关系提供了合理的基础。