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Chemistry and Structure of Graphene Oxide via Direct Imaging
ACS Nano ( IF 15.8 ) Pub Date : 2016-07-19 00:00:00 , DOI: 10.1021/acsnano.6b02391
Shreya H. Dave , Chuncheng Gong 1 , Alex W. Robertson 1 , Jamie H. Warner 1 , Jeffrey C. Grossman
Affiliation  

Graphene oxide (GO) and reduced GO (rGO) are the only variants of graphene that can be manufactured at the kilogram scale, and yet the widely accepted model for their structure has largely relied on indirect evidence. Notably, existing high-resolution transmission electron microscopy (HRTEM) studies of graphene oxide report long-range order of sp2 lattice with isolated defect clusters. Here, we present HRTEM evidence of a different structural form of GO, where nanocrystalline regions of sp2 lattice are surrounded by regions of disorder. The presence of contaminants that adsorb to the surface of the material at room temperature normally prevents direct observation of the intrinsic atomic structure of this defective GO. To overcome this, we use an in situ heating holder within an aberration-corrected TEM (AC-TEM) to study the atomic structure of this nanocrystalline graphene oxide from room temperature to 700 °C. As the temperature increases to above 500 °C, the adsorbates detach from the GO and the underlying atomic structure is imaged to be small 2–4 nm crystalline domains within a polycrystalline GO film. By combining spectroscopic evidence with the AC-TEM data, we support the dynamic interpretation of the structural evolution of graphene oxide.

中文翻译:

化学氧化石墨烯的结构通过直接成像

氧化石墨烯(GO)和还原GO(rGO)是可以在千克规模上生产的石墨烯的唯一变体,然而,其结构广为接受的模型很大程度上依赖于间接证据。值得注意的是,现有的氧化石墨烯的高分辨率透射电子显微镜(HRTEM)研究报告了带有孤立缺陷簇的sp 2晶格的长程分布。在这里,我们介绍了GO的不同结构形式的HRTEM证据,其中sp 2晶格的纳米晶体区域被无序区域包围。在室温下吸附到材料表面的污染物的存在通常会阻止直接观察这种有缺陷的GO的固有原子结构。为了克服这个问题,我们使用了原位像差校正TEM(AC-TEM)中的加热支架,以研究这种纳米晶氧化石墨烯在室温至700°C范围内的原子结构。当温度升高到高于500°C时,被吸附物从GO分离,下面的原子结构被成像为多晶GO膜中2–4 nm的小晶畴。通过结合光谱证据与AC-TEM数据,我们支持对氧化石墨烯结构演变的动态解释。
更新日期:2016-07-19
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