Spectrophotometric Analysis and Optimization of 2D Gold Nanosheet Formation.
Spectrophotometric Analysis and Optimization of 2D Gold Nanosheet Formation.
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DOI：
10.1021/acs.jpcc.2c07582
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发表时间：
2023-02-16
影响因子：
3.7
通讯作者：
Evans, Stephen D.
中科院分区：
文献类型：
--
作者：
Fox, Joseph;Newham, George;Bushby, Richard J.;Valleley, Elizabeth M. A.;Coletta, Patricia Louise;Evans, Stephen D.
独立式二维金纳米片 (AuNS) 提供从计算到生物传感和医疗保健的广泛潜在应用。然而，此类应用需要改进对材料生长的控制。我们最近报道了仅~0.47 nm（两个原子）厚的AuNS的合成，其表现出非常高的催化活性。该合成是一锅、无籽程序，其中氯金酸在甲基橙 (MO) 存在下被柠檬酸钠还原。在本研究中，我们使用分光光度分析和 TEM 成像来探测 AuNS 的形成并优化程序。之前，我们认为 MO 充当限制剂，引导金的二维生长。在这里，我们提供了首次报道的 HAuCl4 和 MO 反应的分析。我们发现 MO 被快速氧化生成 4-重氮苯磺酸，这表明 HAuCl4、MO 和其他反应产物之间复杂的相互作用导致 AuNS 的形成。时间分辨研究表明，合成时间可以从 12 小时以上显着缩短至 2-3 小时。将反应温度从 20°C 降低至 4°C，AuNS 产率提高了 16 倍，并且优化后材料的催化活性与之前获得的相匹配。我们对 AuNS 形成机制的阐明为进一步改进和调整合成开辟了途径，增强了超薄 AuNS 的潜在应用。
Free-standing, 2D gold nanosheets (AuNS) offer broad potential applications from computing to biosensing and healthcare. Such applications, however, require improved control of material growth. We recently reported the synthesis of AuNS only ∼0.47 nm (two atoms) thick, which exhibited very high catalytic activity. The synthesis is a one-pot, seedless procedure in which chloroauric acid is reduced by sodium citrate in the presence of methyl orange (MO). In this study, we use spectrophotometric analysis and TEM imaging to probe AuNS formation and optimize the procedure. Previously, we suggested that MO acted as the confining agent, directing two-dimensional growth of the gold. Here, we provide the first reported analysis of the HAuCl4 and MO reaction. We show that MO is rapidly oxidized to give 4-diazobenzenesulfonic acid, indicating that a complex interplay between HAuCl4, MO, and other reaction products leads to AuNS formation. Time-resolved studies indicate that synthesis time can be significantly reduced from over 12 to 2–3 h. Decreasing the reaction temperature from 20 to 4 °C improved AuNS yield by 16-fold, and the catalytic activity of the optimized material matches that obtained previously. Our elucidation of AuNS formation mechanisms has opened avenues to further improve and tune the synthesis, enhancing the potential applications of ultrathin AuNS.
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