Journal
ACS NANO
Volume 7, Issue 2, Pages 1769-1778Publisher
AMER CHEMICAL SOC
DOI: 10.1021/nn305919p
Keywords
carbon nanotube; electrochemistry; dispersion; deposition; purification; functionalization
Categories
Funding
- LSI Logic Corporation, USA
- EPSRC [EP/G007314/1]
- Engineering and Physical Sciences Research Council [EP/G007314/1] Funding Source: researchfish
- EPSRC [EP/G007314/1] Funding Source: UKRI
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The dissolution of single-walled carbon nanotubes (SWCNTs) remains a fundamental challenge, reliant on aggressive chemistry or ultrasonication and lengthy ultracentrifugation. In contrast, simple nonaqueous electrochemical reduction leads to spontaneous dissolution of individualized SWCNTs from raw, un-processed powders. The intrinsic electrochemical stability and conductivity of these nanomaterials allow their electrochemical dissolution from a pure SWCNT cathode to form solutions of individually separate and distinct (i.e., discrete) nanotube anions with varying charge density. The integrity of the SWCNT sp(2) framework during the charge/discharge process is demonstrated by optical spectroscopy data. Other than a reversible change in redox/solvation state, there is no obvious chemical functionalization of the structure, suggesting an analogy to conventional atomic electrochemical dissolution. The heterogeneity of as-synthesized SWCNT samples leads to the sequential dissolution of distinct fractions overtime, with fine control over the electrochemical potential. Initial preferential dissolution of defective nanotubes and carbonaceous debris provides a simple, nondestructive means to purify raw materials without recourse to the usual, damaging, competitive oxidation reactions. Neutral SWCNTs can be recovered either by electroplating at an anode or by reaction with a suitable electrophile.
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