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Register a new userSize-selected polyynes synthesized by submerged arc discharge in water
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Added by
Carlo Spartaco Casari
Publication date
2019
fields
Physics
and research's language is
English
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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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In recent years there has been a growing interest in sp-carbon chains as possible novel nanostructures. An example of sp-carbon chains are the so-called polyynes, characterized by the alternation of single and triple bonds that can be synthesized by pulsed laser ablation in liquid (PLAL) of a graphite target. In this work, by exploiting different solvents in the PLAL process, e.g. water, acetonitrile, methanol, ethanol, and isopropanol, we systematically investigate the solvent role in polyyne formation and stability. The presence of methyland cyano-groups in the solutions influences the termination of polyynes, allowing to detect, in addition to hydrogen-capped polyynes up to HC22H, methyl-capped polyynes up to 18 carbon atoms (i.e. HCnCH3) and cyanopolyynes up to HC12CN. The assignment of each species was done by UV-Vis spectroscopy and supported by density functional theory simulations of vibronic spectra. In addition, surface-enhanced Raman spectroscopy allowed to observe differences, due to different terminations (hydrogen, methyl-and cyano group), in the shape and positions of the characteristic Raman bands of the size-selected polyynes. The evolution in time of each polyyne has been investigated evaluating the chromatographic peak area, and the effect of size, terminations and solvents on polyynes stability has been individuated.
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