Khandelwal Mahima, Kumar Anil
Department of Chemistry, Indian Institute of Technology Roorkee, Roorkee-247667, India.
Dalton Trans. 2016 Mar 28;45(12):5180-95. doi: 10.1039/c5dt04880j.
The present paper reports the one-pot synthesis of N-doped graphene-Ag nanocomposites (N-GrAg) involving the in situ generation of Ag nanoparticles (NPs). The simultaneous reduction of GO and Ag(+) to produce N-GrAg has been achieved under mild reaction conditions using an environmentally benign reducing agent, glycine, in aqueous medium without adding any external stabilizer. XRD and SAED analyses revealed the presence of Ag in the fcc structure. HRTEM analysis shows a 'd' spacing of 0.236 nm corresponding to the highest intensity (111) reflection of Ag which matches the fcc structure. The N-doping of graphene and its uniform decoration by Ag NPs (with an av. dia. of 17.5 nm) having a relatively low surface atomic % of Ag (0.309) are evidenced by TEM and XPS analyses. Raman spectroscopy has also revealed that the decoration of N-Gr with Ag NPs resulted in the enhancement of the D and G bands by about 365%. The presence of Ag in N-GrAg prevents the folding of the graphene sheet as was revealed by TEM analysis. The supramolecular interactions of Ag with different moieties of N in N-GrAg were evidenced by IR, (13)C NMR and XPS analyses, which resulted in the enhancement of its surface area and electrical conductivity as compared to that of N-Gr. The presence of Ag NPs on N-Gr increased the current response in cyclic voltammetry by more than seven fold as compared to that of N-Gr. These nanocomposites exhibited a fairly high SERS activity for 4-aminothiophenol, employed as the probe molecule, and allowed its detection at a 50 nM concentration even for the fairly small sized Ag NPs used in the present work.
本文报道了一种一锅法合成氮掺杂石墨烯-银纳米复合材料(N-GrAg)的方法,该方法涉及原位生成银纳米颗粒(NPs)。在温和的反应条件下,使用环境友好型还原剂甘氨酸,在水介质中不添加任何外部稳定剂,实现了氧化石墨烯(GO)和Ag(+)的同时还原以制备N-GrAg。X射线衍射(XRD)和选区电子衍射(SAED)分析表明存在面心立方(fcc)结构的银。高分辨透射电子显微镜(HRTEM)分析显示,对应于银的最高强度(111)反射的“d”间距为0.236 nm,与fcc结构相符。透射电子显微镜(TEM)和X射线光电子能谱(XPS)分析证明了石墨烯的氮掺杂及其被平均直径为17.5 nm且银表面原子百分比相对较低(0.309)的银纳米颗粒均匀修饰。拉曼光谱还表明,用银纳米颗粒修饰N-Gr导致D带和G带增强了约365%。TEM分析表明,N-GrAg中银的存在可防止石墨烯片层折叠。红外光谱(IR)、碳-13核磁共振((13)C NMR)和XPS分析证明了银与N-GrAg中氮的不同部分之间存在超分子相互作用,与N-Gr相比,这导致其表面积和电导率增加。与N-Gr相比,N-Gr上银纳米颗粒的存在使循环伏安法中的电流响应增加了七倍以上。这些纳米复合材料对用作探针分子的4-氨基硫酚表现出相当高的表面增强拉曼散射(SERS)活性,即使对于本工作中使用的相当小尺寸的银纳米颗粒,也能在50 nM浓度下检测到它。