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Shedding light on the soft and efficient free radical induced reduction of graphene oxide: hidden mechanisms and energetics

机译：脱落浅浅，高效的自由基诱导石墨烯氧化物的减少：隐藏机制和能量学

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摘要

Reduction of graphene oxide (GO) in aqueous dispersions by strongly reducing free radicals has recently been identified to be a very powerful approach, because functional groups are removed softly but efficiently, and non-volatile impurities as well as defects are largely avoided. However, the reaction mechanisms remained somewhat speculative. Recently we showed that GO can be efficiently reduced in water by indirect photoreduction mediated by (CH3)(2)C-center dot(OH) radicals generated via the reaction of triplet acetone with isopropanol. Those radicals efficiently defunctionalize oxo-groups of GO forming the carbon lattice without generating additional defects. In this comprehensive study we shed more light on the reaction mechanism of reduction of GO by H-center dot, CO2 center dot, (CH3)(2)C-center dot(OH) and (CH3CH)-H-center dot(OH) by combining pulsed radiolysis and determine its overall energetics via quantum-chemical calculations. In time-dependent experiments mechanistic insights have been obtained and unknown intermediates have been discovered. Moreover, different reduction mechanisms, such as radical addition, electron-transfer, concerted water elimination and HCO3- elimination are identified. Here we show that all mechanisms lead to sp(2)-carbon formation and therefore high quality graphene by reductive defunctionalization.
机译：通过牢固地减少自由基将石墨烯氧化物（GO）的氧化石墨烯（GO）的降低是一种非常强大的方法，因为官能团被轻轻地除去，而且有效地除去，并且在很大程度上避免了非挥发性杂质以及缺陷。然而，反应机制保持有些投机。最近，我们表明，通过由三联丙酮与异丙醇的反应产生的（CH3）（2）C中心点（OH）基团介导的间接照相，可以在水中有效地降低水中。那些自由基有效地透明氧代官能化的氧代组形成碳晶格而不产生额外的缺陷。在这项综合研究中，我们在H中心点，CO2中心点，（2）C中心点（OH）和（CH3CH）-H中心点（OH）和（CH3CH） - 中心点（OH）和（CH3CH）-H中心点（OH ）通过将脉冲放射性分解并通过量子化学计算确定其整体能量。在时间依赖的实验中，已经获得了机械洞察，并且已发现未知的中间体。此外，鉴定了不同的减少机制，例如自由基添加，电子转移，齐齐的水消除和HCO3消除。在这里，我们表明所有机制都会导致SP（2） - 通过还原抗核化化的碳碳和因此高质量的石墨烯。

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  • 来源
    《RSC Advances》 |2016年第73期|共11页
  • 作者

    Kahnt A.; Flyunt R.; Naumov S.; Knolle W.; Eigler S.; Hermann R.; Abel B.;

  • 作者单位

    Univ Erlangen Nurnberg Chair Phys Chem 1 Dept Chem &

    Pharm Egerlandstr 3 D-91058 Erlangen Germany;

    Leibniz Inst Surface Modificat IOM Dept Chem Permoserstr 15 D-04303 Leipzig Germany;

    Leibniz Inst Surface Modificat IOM Dept Chem Permoserstr 15 D-04303 Leipzig Germany;

    Leibniz Inst Surface Modificat IOM Dept Chem Permoserstr 15 D-04303 Leipzig Germany;

    Univ Erlangen Nurnberg Inst Adv Mat &

    Proc ZMP Dept Chem &

    Pharm Henkestr 42 D-91054 Erlangen Germany;

    Univ Leipzig Wilhelm Ostwald Inst Phys &

    Theoret Chem Linne Str 2 D-04103 Leipzig Germany;

    Leibniz Inst Surface Modificat IOM Dept Chem Permoserstr 15 D-04303 Leipzig Germany;

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  • 正文语种 eng
  • 中图分类 化学;
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