From understanding the roles of tetraoctylammonium bromide in the two-phase Brust-Schiffrin method to tuning the size of gold nanoclusters.,Nanoscale

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From understanding the roles of tetraoctylammonium bromide in the two-phase Brust-Schiffrin method to tuning the size of gold nanoclusters.
Nanoscale ( IF 5.8 ) Pub Date : 2020-08-31 , DOI: 10.1039/d0nr04439c
Xinyue Dou ₁ , Xiangyu Wang , Shuyu Qian , Naiwei Liu , Xun Yuan

Affiliation

The two-phase Brust–Schiffrin (B–S) method has been widely used for synthesizing small-sized Au nanoparticles (NPs) of size 2–6 nm, as well as Au nanoclusters (NCs) of size <2 nm. However, size tuning of Au NCs at the atomic level by this method is challenging probably due to a lack of in-depth understanding of its mechanism. Herein, we report the identification of two roles of tetraoctylammonium bromide (TOAB) in the two-phase B–S method: TOAB not only transfers Au(III) precursors but also transfers the reducing agent NaBH₄ from the aqueous to the organic phase. On this basis, we developed a novel two-phase synthetic strategy by decoupling the roles of the TOAB: (1) using the hydrophobic selenolate ligand to transfer Au(III) precursors from the aqueous to the organic phase via the formation of selenolate–Au(I) complexes and (2) deploying a small amount of TOAB as “shuttles” to transfer NaBH₄ into the organic phase for controlled reduction of selenolate–Au(I) complexes in organic phase. Using this strategy, size tuning of Au NCs at the atomic level could be achieved by simply varying the amount of TOAB. The high yields of Au NCs (≥76%) together with the short synthetic time (≤3 h) and size-tuning capability further illustrate the attractiveness of this synthetic strategy. These advantages also present the classical B–S method with greater strength and flexibility towards NC synthesis.

中文翻译：

从理解四辛基溴化铵在两相Brust-Schiffrin方法中的作用到调整金纳米簇的大小。

两阶段的Brust-Schiffrin（BS）方法已广泛用于合成大小为2-6 nm的小尺寸Au纳米粒子（NPs）以及大小为<2 nm的Au纳米团簇（NCs）。但是，由于缺乏对其机理的深入了解，通过这种方法在原子水平上对Au NCs的尺寸调节具有挑战性。在这里，我们报告了在四相溴化乙锭方法中溴化四辛基铵（TOAB）的两个作用的鉴定：TOAB不仅将Au（III）前体转移，还将还原剂NaBH ₄从水相转移到有机相。在此基础上，我们通过解偶联TOAB的作用，开发了一种新颖的两相合成策略：（1）使用疏水性硒酸酯配体转移Au（III））通过形成硒酸酯-Au（I）配合物而从水相到有机相的前体；（2）部署少量TOAB作为“穿梭”，将NaBH ₄转移到有机相中，以控制还原硒酸酯-Au（I）有机相中的络合物。使用此策略，可以通过简单地改变TOAB的量来实现原子级Au NCs的尺寸调节。Au NCs的高收率（≥76％）以及较短的合成时间（≤3h）和尺寸调节能力进一步说明了这种合成策略的吸引力。这些优点还展示了经典的BS方法，具有更高的强度和灵活性，可用于NC合成。

更新日期：2020-10-08

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