Building Carbon Bridges on and between Fullerenes in Helium Nanodroplets.
Building Carbon Bridges on and between Fullerenes in Helium Nanodroplets.
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DOI：
10.1021/acs.jpclett.6b00462
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发表时间：
2016-04-21
期刊：
影响因子：
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通讯作者：
Scheier P
中科院分区：
文献类型：
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作者：
Krasnokutski SA;Kuhn M;Kaiser A;Mauracher A;Renzler M;Bohme DK;Scheier P
我们报道了在极冷的环境中富勒烯与C原子的连续相遇的观察结果。在0.37 K的氦液滴中掺杂C60分子和来自一种新的纯C原子源的C原子进行了实验。非常高分辨率的质谱显示形成的卡宾类型C60（C：）n与n高达6。还观察到C吸附原子形成已知的哑铃C60=C=C60的桥式键合。通过密度泛函理论计算，阐明了C60（C：）n物种的卡宾特征及其结构。在水杂质的存在下，并在单独的实验中与添加H2的质谱也显示的加合物C60 Cn（H2O）n和C60 Cn（H2）n的形成可能是通过H-OH和H-H键插入，分别和哑铃的非反应性。因此，形成卡宾C60（C：）n的C吸附原子可以赋予原始C60更高的化学反应活性。
We report the observation of sequential encounters of fullerenes with C atoms in an extremely cold environment. Experiments were performed with helium droplets at 0.37 K doped with C60 molecules and C atoms derived from a novel, pure source of C atoms. Very high-resolution mass spectra revealed the formation of carbenes of the type C60(C:)n with n up to 6. Bridge-type bonding of the C adatoms to form the known dumbbell C60=C=C60 also was observed. Density functional theory calculations were performed that elucidated the carbene character of the C60(C:)n species and their structures. Mass spectra taken in the presence of water impurities and in separate experiments with added H2 also revealed the formation of the adducts C60Cn(H2O)n and C60Cn(H2)n probably by H–OH and H–H bond insertion, respectively, and nonreactivity for the dumbell. So C adatoms that form carbenes C60(C:)n can endow pristine C60 with a higher chemical reactivity.