Interest in graphene oxide (GO) due to its controllable and adjustable properties has been increasing, especially in the field of electronic and electrochemical charge storage devices. Hence, the modification of surface chemistry and structure of GO can be outlined as crucial for achieving the preferable properties. In this study, we have investigated the influence of 15 keV proton-beam irradiation on GO structure and surface chemistry. The results obtained by Raman spectroscopy, Fourier-transform infrared (FTIR) and X-ray photoelectron spectroscopy (XPS) were complemented with theoretical ones, obtained by using density functional theory (DFT), semi-empirical (SE) calculations and inelastic thermal spike (iTS) model. The FTIR and XPS results showed that proton irradiation partially reduces the GO with the preferential removal of the alkoxy and epoxy groups. Also, we identified a clear linear relation between the decresase of oxygen content and the decrease of ID/IG ratio i.e. increasing disorder of GO structure. The SE and DFT calculations highlighted a reduction of GO as a single- or multi-step process depending on the type of basal-plane or edge oxygen group. Dynamic SE calculations revealed that for kinetic energy of hydrogen below 1.5 eV the reduction is chemically driven, while at energies higher than 20 eV, the reduction of GO is a result of physical processes. iTS results showed that increase of temperature might contribute to reduction of GO via desorption of epoxy and alcoxy groups, as the least thermally stable groups (T ∼200 °C). The results of this work emphasize the capabilities ion beam irradiation for gradual modification of surface chemistry and structural properties of GO by providing more information about the mechanisms of hydrogen interaction with individual groups, interplay between defect creation, oxygen content and accompaning effects of ion energy loss processes.

由于其可控和可调的特性，人们对氧化石墨烯（GO）的兴趣一直在增加，特别是在电子和电化学电荷存储设备领域。因此，GO 的表面化学和结构的改性可以概括为实现优选性能的关键。在这项研究中，我们研究了 15 keV 质子束辐照对 GO 结构和表面化学的影响。通过使用密度泛函理论（DFT）、半经验（SE）计算和非弹性热尖峰获得的拉曼光谱、傅里叶变换红外（FTIR）和X射线光电子能谱（XPS）得到的结果与理论结果相辅相成(iTS) 模型。FTIR 和 XPS 结果表明，质子辐照部分还原了 GO，优先去除了烷氧基和环氧基团。此外，我们确定了氧含量的降低与 ID/IG 比率的降低之间存在明显的线性关系IEGO结构的无序性增加。SE 和 DFT 计算强调了 GO 的减少作为单步或多步过程，具体取决于基面或边缘氧基团的类型。动态 SE 计算表明，对于低于 1.5 eV 的氢动能，还原是化学驱动的，而在高于 20 eV 的能量下，GO 的还原是物理过程的结果。iTS 结果表明，温度升高可能有助于通过解吸环氧基和烷氧基还原 GO，因为这些基团是热稳定性最低的基团（T~200 °C）。这项工作的结果通过提供有关氢与单个基团相互作用机制的更多信息，强调了离子束辐照逐渐改变 GO 表面化学和结构特性的能力，