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首页> 外文期刊>Journal of the American Chemical Society >Modified Thermodynamics in Ionic Liquids for Controlled Electrocrystallization of Nanocubes, Nanowires, and Crystalline Thin Films of Silver-Tetracyanoquinodimethane
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Modified Thermodynamics in Ionic Liquids for Controlled Electrocrystallization of Nanocubes, Nanowires, and Crystalline Thin Films of Silver-Tetracyanoquinodimethane

机译：改进的离子液体中的热力学，用于控制四方银，四方银和喹啉银的纳米立方体，纳米线和结晶薄膜的电结晶

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摘要

Electrocrystallization of nanocubes, nanorods, nanowires, and crystalline thin films of silver-tetracyanoquinodimethane (AgTCNQ) onto glassy carbon, indium tin oxide, and platinum electrodes can be achieved from ionic liquids containing dissolved TCNQ and Ag(l) salts. In conventional molecular organic solvents, such as acetonitrile, the reduction of TCNQ and Ag~+ occurs at almost the same potential. In contrast, the different thermodynamics that apply to the room temperature ionic liquid, 1-n-butyl-3-methylimidazolium tetrafluoroborate (BMIMBF_4), give rise to a large potential separation in the two processes, which enables electrocrystallization of AgTCNQ to be undertaken via two distinctly different, potential-dependent mechanisms. Cyclic and microelectrode voltammetric, chronoamperometric, together with microscopic and spectroscopic techniques reveal that AgTCNQ nanostuctures of controlled morphology, size, density, and uniformity can be achieved by tuning the electrocrystallization parameters such as potential, stoichiometric ratio of Ag~+ and TCNQ, and their concentrations, time, and ionic liquid viscosity by altering the water content. In the potential range of -0.1 to 0.3 V vs Fc~(0/+) (Fc = ferrocene), electrocrystallization occurs when Ag is deposited at electrode defect sites via a progressive nucleation and 3-D growth mechanism followed by reaction with TCNQ to produce structures ranging from nanocubes to nanowires. At higher stoichiometric concentrations of Ag+ and more negative potentials (<-0.1 V vs Fc~(0/+)), extremely thin crystalline films could be obtained via overpotential deposition. Infrared and Raman spectroscopy, elemental analysis, together with X-ray diffraction and scanning electron microscopy all confirm the formation of highly pure AgTCNQ nanomaterials, which exhibit differences in morphology but not phase. The study highlights the capability of the electrocrystallization method to precisely control the morphology of nanomaterials, and also the unprecedented opportunities provided by using ionic liquids as the medium for preparation of technologically important metal-TCNQ charge transfer complexes.
机译：可以从包含溶解的TCNQ和Ag（l）盐的离子液体中，将纳米立方，纳米棒，纳米线和四氰基银二甲基银（AgTCNQ）的结晶薄膜电结晶到玻璃碳，铟锡氧化物和铂电极上。在常规的分子有机溶剂（如乙腈）中，TCNQ和Ag〜+的还原几乎在相同的电位下发生。相比之下，应用于室温离子液体1-正丁基-3-甲基咪唑四氟硼酸盐（BMIMBF_4）的不同热力学在两个过程中产生了较大的电势分离，这使得AgTCNQ的电结晶可以通过两种截然不同的，依赖电位的机制。循环和微电极伏安法，计时电流法以及显微和光谱学技术表明，通过调节电结晶参数（例如电势，Ag〜+和TCNQ的化学计量比）及其结构，可以控制形态，尺寸，密度和均匀性的AgTCNQ纳米结构浓度，时间和离子液体粘度（通过更改水含量）。在相对于Fc〜（0 / +）（Fc =二茂铁）的-0.1至0.3 V的电势范围内，当Ag通过逐步成核和3-D生长机制沉积在电极缺陷部位并随后与TCNQ反应生成Ag时，就会发生电结晶。产生从纳米立方体到纳米线的结构。在更高的化学计量浓度的Ag +和更多的负电位（<-0.1 V vs Fc〜（0 / +））下，可通过过电势沉积获得极薄的结晶膜。红外和拉曼光谱，元素分析以及X射线衍射和扫描电子显微镜都证实了高纯度AgTCNQ纳米材料的形成，该纳米材料表现出形态差异，但没有相差。这项研究强调了电结晶方法能够精确控制纳米材料形态的能力，并且强调了使用离子液体作为制备技术上重要的金属-TCNQ电荷转移络合物的介质所提供的前所未有的机会。

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  • 来源
    《Journal of the American Chemical Society》 |2009年第44期|16195-16205|共11页
  • 作者

    Chuan Zhao; Douglas R. MacFarlane; Alan M. Bond;

  • 作者单位

    School of Chemistry and ARC Special Research Centre for Green Chemistry, Monash University, Clayton, Victoria 3800, Australia;

    School of Chemistry and ARC Special Research Centre for Green Chemistry, Monash University, Clayton, Victoria 3800, Australia;

    School of Chemistry and ARC Special Research Centre for Green Chemistry, Monash University, Clayton, Victoria 3800, Australia;

  • 收录信息 美国《科学引文索引》(SCI);美国《工程索引》(EI);美国《生物学医学文摘》(MEDLINE);美国《化学文摘》(CA);
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  • 正文语种 eng
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