水中埋弧放电合成尺寸选择性多炔化合物
Size-selected polyynes synthesized by submerged arc discharge in water
摘要：
多炔化合物是由一系列交替的单键和三键组成的有限长度的直链sp-碳链，具有吸引人的光学和电子性质。液相埋弧放电是一种简单、低成本、可规模化生产多炔化合物的方法，目前主要在有机溶剂中进行。在这项工作中，我们详细研究了SAD在水中作为一种廉价和无毒的溶剂生产多炔。研究了工艺参数如电流（10-25 A）和电压（20-25 V）在生产产率中的作用以及多炔稳定性。通过高效液相色谱（HPLC）结合紫外-可见吸收光谱和密度泛函理论（DFT）计算对氢封端的多炔（CnH 2：n=6-16）进行了鉴定。通过表面增强拉曼光谱（SERS）分析了通过HPLC分离的尺寸选择的多炔。形成过程进行了监测原位SERS使用浸没光纤拉曼探针和采用银纳米粒子直接在溶液中产生的SAD。
英文摘要：
Polyynes are linear sp-carbon chains of finite length consisting in a sequence of alternated single and triple bonds and displaying appealing optical and electronic properties. A simple, low cost and scalable production technique for polyynes is the submerged arc discharge (SAD) in liquid, which so far, has been mainly exploited in organic solvents. In this work, we investigated in detail SAD in water as a cheap and non-toxic solvent for the production of polyynes. The role of process parameters such as current (10-25 A) and voltage (20-25 V) in the production yield have been investigated, as well as polyynes stability. Polyynes terminated by hydrogen (CnH2: n=6-16) were identified by High-Performance Liquid Chromatography (HPLC) coupled with UV-Visible absorption spectroscopy and with the support of density functional theory (DFT) calculations. Size-selected polyynes separated by HPLC were analyzed by surface enhanced Raman spectroscopy (SERS). The formation process was monitored by in situ SERS using an immersed fiber-optic Raman probe and employing Ag nanoparticles directly produced in the solution by SAD.
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