Xing Lixiang, Xiahou Yujiao, Zhang Peina, Du Wei, Xia Haibing
State Key Laboratory of Crystal Materials , Shandong University , Jinan 250100 , P. R. China.
School of Environment and Material Engineering , Yantai University , Yantai 264005 , Shandong , China.
ACS Appl Mater Interfaces. 2019 May 15;11(19):17637-17646. doi: 10.1021/acsami.9b02052. Epub 2019 Apr 30.
In this work, we reported the synthesis of monodisperse, quasispherical Ag nanoparticles (NPs) with sizes of 40-300 nm by using ascorbic acid reduction of a silver-ammonia complex onto preformed, 23 nm Ag-NP seeds in the aqueous solution with an optimal pH of about 9.6 at room temperature. The as-prepared Ag NPs with such a large size span (from 40 to 300 nm) and high quality by one-pot seeded growth method are reported for the first time to the best of our knowledge. It is found that the key in the present seed-mediated growth method is to introduce a proper amount of ammonia water for the formation of a stable complex with a silver precursor (silver-ammonia complex) while maintaining the pH value of the growth solution simultaneously. By using rhodamine 6G molecules as probes, the surface-enhanced Raman scattering (SERS) activities of the as-prepared Ag NPs in ethanol solution are highly dependent on the sizes of Ag NPs at the fixed 633 nm laser and at the fixed particle number, which show a volcano-like curve. Moreover, 125 nm Ag NPs bear the largest SERS activity among them. Furthermore, Ag NPs with narrow distributions in shape and size (say, less than 10%) can achieve the uniformity and reproducibility of their SERS signals in solution; their relative standard deviations can be as low as 5% in space and temporal scale.
在本工作中,我们报道了通过在室温下于最佳pH约为9.6的水溶液中,利用抗坏血酸将银氨络合物还原到预先形成的23 nm银纳米颗粒(NP)种子上,合成尺寸为40 - 300 nm的单分散、准球形银纳米颗粒(NPs)。据我们所知,首次报道了通过一锅法种子生长法制备出如此大尺寸跨度(从40到300 nm)且高质量的银纳米颗粒。研究发现,当前种子介导生长法的关键在于引入适量氨水以形成与银前驱体的稳定络合物(银氨络合物),同时保持生长溶液的pH值。以罗丹明6G分子为探针,在固定633 nm激光和固定颗粒数条件下,所制备的银纳米颗粒在乙醇溶液中的表面增强拉曼散射(SERS)活性高度依赖于银纳米颗粒的尺寸,呈现出类似火山的曲线。此外,125 nm的银纳米颗粒在其中具有最大的SERS活性。此外,形状和尺寸分布狭窄(例如小于10%)的银纳米颗粒在溶液中能够实现其SERS信号的均匀性和可重复性;在空间和时间尺度上,它们的相对标准偏差可低至5%。