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Formation of hydrogen-capped polyynes by laser ablation of C_(60) particles suspended in solution

机译:通过激光烧蚀悬浮在溶液中的C_(60)颗粒形成氢封端聚炔

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摘要

Laser ablation of C_(60) particles suspended in hexane or methanol solution has been studied using a Nd:YAG laser (266, 355, 532, and 1064 nm). Insoluble product analysis by Raman spectroscopy showed that C_(60) particles transformed to graphite-like ones. On the other hand, soluble product analysis by HPLC coupled with UV absorption spectroscopy and GC/MS demonstrated that linear hydrogen-capped polyynes (C_nH_2: n=8, 10, 12) were formed. The dominant C_nH_2 polyyne was C_8H_2 in all cases. The relative abundance of polyynes decreased with increasing wavelength of the Nd:YAG laser, except for 266-nm irradiation in hexane, where the relative abundance of polyynes at 355 nm was greater than that at 266 nm. It was therefore concluded that photochemical processes are more important than thermal ones for the formation of polyynes. The relative abundance of polyynes in hexane was greater than that in methanol. The dependence of relative abundance of polyynes on the particles concentration, laser irradiation time, and laser power was measured in order to obtain information on formation mechanism of polyynes. These results and reported laser photochemical processes of C_(60) molecules in the gas phase suggested that C_2 radicals produced from C_(60) are polymerized and hydrogenated to form C_8H_2 and much smaller amounts of C_(10)H_2 and C_(12)H_2.
机译:使用 Nd:YAG 激光(266、355、532 和 1064 nm)研究了悬浮在己烷或甲醇溶液中的 C_(60) 颗粒的激光烧蚀。拉曼光谱的不溶产物分析表明,C_(60)颗粒转化为石墨状颗粒。另一方面,HPLC结合紫外吸收光谱和GC/MS对可溶性产物的分析表明,形成了线性氢封端聚炔(C_nH_2:n=8,10,12)。在所有情况下,C_nH_2聚炔的优势均C_8H_2。聚炔的相对丰度随着Nd:YAG激光波长的增加而降低,但己烷的266 nm辐照除外,其中355 nm处的聚炔相对丰度大于266 nm处的相对丰度。因此得出的结论是,光化学过程比热化学过程对多炔的形成更重要。己烷中多炔的相对丰度大于甲醇中的相对丰度。测量了多炔相对丰度对颗粒浓度、激光照射时间和激光功率的依赖性,以获得多炔的形成机理。这些结果和报道的气相中C_(60)分子的激光光化学过程表明,由C_(60)产生的C_2自由基被聚合和氢化,形成C_8H_2和少量的C_(10)H_2和C_(12)H_2。

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