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原子尺度下碳与第八族金属相互作用和键合的研究。

Investigation of the Interactions and Bonding between Carbon and Group VIII Metals at the Atomic Scale.

机构信息

Central Facility for Electron MicroscopyElectron Microscopy Group of Materials Science, Ulm University, Albert-Einstein-Allee 11, Ulm, D-89081, Germany.

Institute of Process Research and Development, School of Chemistry, University of Leeds, Leeds, LS2 9JT, United Kingdom.

出版信息

Small. 2016 Mar 23;12(12):1649-57. doi: 10.1002/smll.201502210. Epub 2016 Feb 5.

Abstract

The nature and dynamics of bonding between Fe, Ru, Os, and single-walled carbon nanotubes (SWNTs) is studied by aberration-corrected high-resolution transmission electron microscopy (AC-HRTEM). The metals catalyze a wide variety of different transformations ranging from ejection of carbon atoms from the nanotube sidewall to the formation of hollow carbon shells or metal carbide within the SWNT, depending on the nature of the metal. The electron beam of AC-HRTEM serves the dual purpose of providing energy to the specimen and simultaneously enabling imaging of chemical transformations. Careful control of the electron beam parameters, energy, flux, and dose allowed direct comparison between the metals, demonstrating that their chemical reactions with SWNTs are determined by a balance between the cohesive energy of the metal particles and the strength of the metal-carbon σ- or π-bonds. The pathways of transformations of a given metal can be drastically changed by applying different electron energies (80, 40, or 20 keV), thus demonstrating AC-HRTEM as a new tool to direct and study chemical reactions. The understanding of interactions and bonding between SWNT and metals revealed by AC-HRTEM at the atomic level has important implications for nanotube-based electronic devices and catalysis.

摘要

采用相衬校正高分辨透射电子显微镜(AC-HRTEM)研究了 Fe、Ru、Os 与单壁碳纳米管(SWNTs)之间的键合性质和动态。这些金属可以催化各种各样的不同转化,从从纳米管侧壁上逐出碳原子到在 SWNT 内形成中空碳壳或金属碳化物,这取决于金属的性质。AC-HRTEM 的电子束具有双重作用,既能为样品提供能量,又能同时实现化学转化的成像。通过仔细控制电子束参数、能量、通量和剂量,可以在金属之间进行直接比较,证明它们与 SWNTs 的化学反应取决于金属颗粒的内聚能与金属-碳 σ 或 π 键的强度之间的平衡。通过施加不同的电子能量(80、40 或 20 keV),可以彻底改变给定金属的转化途径,从而证明 AC-HRTEM 是一种用于指导和研究化学反应的新工具。AC-HRTEM 在原子水平上揭示的 SWNT 与金属之间的相互作用和键合对于基于纳米管的电子器件和催化具有重要意义。

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