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首页> 外文期刊>Chemistry: A European journal >Direct Measurement of Electron Transfer in Nanoscale Host-Guest Systems: Metallocenes in Carbon Nanotubes
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Direct Measurement of Electron Transfer in Nanoscale Host-Guest Systems: Metallocenes in Carbon Nanotubes

机译：纳米宿主系统中电子转移的直接测量：碳纳米管中的茂金属

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Electron-transfer processes play a significant role in host-guest interactions and determine physicochemical phenomena emerging at the nanoscale that can be harnessed in electronic or optical devices, as well as biochemical and catalytic systems. A novel method for qualifying and quantifying the electronic doping of single walled carbon nanotubes (SWNTs) using electrochemistry has been developed that establishes a direct link between these experimental measurements and ab initio DFT calculations. Metallocenes such as cobaltocene and methylated ferrocene derivatives were encapsulated inside SWNTs (1.4nm diameter) and cyclic voltammetry (CV) was performed on the resultant host-guest systems. The electron transfer between the guest molecules and the host SWNTs is measured as a function of shift in the redox potential (E-1/2) of Co-II/Co-I, Co-III/Co-II and Fe-III/Fe-II. Furthermore, the shift in E-1/2 is inversely proportional to the nanotube diameter. To quantify the amount of electron transfer from the guest molecules to the SWNTs, a novel method using coulometry was developed, allowing the mapping of the density of states and the Fermi level of the SWNTs. Correlated with theoretical calculations, coulometry provides an accurate indication of n/p-doping of the SWNTs.
机译：电子转移过程在宿主与客体的相互作用中起着重要作用，并确定了可在电子或光学设备以及生化和催化系统中利用的纳米级物理化学现象。已经开发出一种使用电化学方法对单壁碳纳米管（SWNT）的电子掺杂进行鉴定和定量的新方法，该方法在这些实验测量值和从头算DFT计算之间建立了直接联系。将茂金属如钴茂金属和甲基化的二茂铁衍生物封装在SWNT（直径为1.4nm）内，并在所得的主客体系统上进行循环伏安法（CV）。客体分子与主体SWNT之间的电子转移根据Co-II / Co-I，Co-III / Co-II和Fe-III /的氧化还原电势（E-1 / 2）的变化进行测量铁-II。此外，E-1 / 2的位移与纳米管直径成反比。为了量化电子从客体分子转移到单壁碳纳米管的数量，开发了一种使用库仑法的新方法，可以绘制单壁碳纳米管的态密度和费米能级。与理论计算相关，库仑法提供了SWNT的n / p掺杂的准确指示。

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