氧化还原态石墨烯：计算光谱学的新视角。

Oxidation states of graphene: insights from computational spectroscopy.

机构信息

Hefei National Laboratory for Physical Sciences at Microscale, University of Science and Technology of China, Hefei, Anhui 230026, China.

出版信息

J Chem Phys. 2009 Dec 28;131(24):244505. doi: 10.1063/1.3276339.

DOI:10.1063/1.3276339

PMID:20059077

Abstract

When it is oxidized, graphite can be easily exfoliated forming graphene oxide (GO). GO is a critical intermediate for massive production of graphene, and it is also an important material with various application potentials. With many different oxidation species randomly distributed on the basal plane, GO has a complicated nonstoichiometric atomic structure that is still not well understood in spite of intensive studies involving many experimental techniques. Controversies often exist in experimental data interpretation. We report here a first principles study on binding energy of carbon 1s orbital in GO. The calculated results can be well used to interpret experimental x-ray photoelectron spectroscopy (XPS) data and provide a unified spectral assignment. Based on the first principles understanding of XPS, a GO structure model containing new oxidation species epoxy pair and epoxy-hydroxy pair is proposed. Our results demonstrate that first principles computational spectroscopy provides a powerful means to investigate GO structure.

摘要

当石墨被氧化时，很容易剥落形成氧化石墨烯 (GO)。GO 是大规模生产石墨烯的关键中间体，也是具有各种应用潜力的重要材料。GO 基面上随机分布着许多不同的氧化物种，具有复杂的非化学计量原子结构，尽管涉及许多实验技术的研究很多，但仍未得到很好的理解。实验数据的解释往往存在争议。我们在此报告了对 GO 中碳 1s 轨道结合能的第一性原理研究。计算结果可以很好地用于解释实验 X 射线光电子能谱 (XPS)数据，并提供统一的光谱分配。基于对 XPS 的第一性原理理解，提出了一种含有新氧化物种环氧对和环氧-羟基对的 GO 结构模型。我们的结果表明，第一性原理计算光谱为研究 GO 结构提供了一种强大的手段。