State Key Laboratory and Institute of Elemento-Organic Chemistry, Nankai University, 300071, Tianjin, China.
J Mass Spectrom. 2012 Apr;47(4):523-8. doi: 10.1002/jms.2985.
The distributions of positive carbon cluster ions produced by laser ablation of graphene (G) and graphene oxide (GO) are found to be quite different. Under a typical experimental condition, narrow distributions of even-numbered clusters from C60+ to C162+ were observed for G, and broad distributions including even-numbered clusters from C100+ to C400+ and odd-numbered clusters from C189+ to C395+ were observed for GO. The threshold of laser energy for G is lower than that of GO. Further results of collision-activated dissociation mass spectrometry indicate that the cluster ions generated from G are structurally similar but are different with those generated from GO or nanodiamonds. It is proposed that the experimentally observed difference can be attributed to the different mechanisms behind the process. A top-down mechanism including both direct transformation of G to fullerene and fragmentation of large-sized fullerenes is suggested for the generation of carbon cluster cations in the process of laser ablation of G. For GO, the experimental results are close to those of nanodiamonds and other materials reported previously and can be explained by the generally accepted bottom-up mechanism.
通过激光烧蚀石墨烯(G)和氧化石墨烯(GO)产生的正碳簇离子的分布被发现有很大的不同。在典型的实验条件下,对于 G,观察到了从 C60+ 到 C162+ 的偶数碳簇的窄分布,而对于 GO,则观察到了包括从 C100+ 到 C400+ 的偶数碳簇和从 C189+ 到 C395+ 的奇数碳簇的宽分布。G 的激光能量阈值低于 GO。进一步的碰撞激活解离质谱结果表明,从 G 产生的团簇离子在结构上相似,但与从 GO 或纳米金刚石产生的团簇离子不同。据推测,实验观察到的差异可以归因于过程背后的不同机制。提出了一种自上而下的机制,包括 G 到富勒烯的直接转化和大尺寸富勒烯的碎裂,用于激光烧蚀 G 过程中碳簇阳离子的产生。对于 GO,实验结果与先前报道的纳米金刚石和其他材料的结果接近,可以用普遍接受的自下而上的机制来解释。