Enhancing graphitic domains by thermally driven structural evolution in graphene oxide

Graphene oxide (GO) holds high potential for various applications due to its extraordinary properties as well as easy scalability and functionalization. Particularly, thermally driven structural evolution in GO might play a key role in enhancing and controlling its properties. Numerous experimental studies use this evolution to tailor GO and it was predicted through various theoretical studies. However, there is still a lack of direct experimental observation and these findings rely on modelling or indirect conclusions. Here, we present an extensive transmission electron microscopy study backed by structural and chemical analysis as a first direct observation of the thermally driven structural evolution. It is shown that graphitic domains dramatically increase including areas over 200 nm2. This change can be attributed to the thermally driven agglomeration of functional groups. In good agreement with previous theoretical predictions, this process is combined with a slight decomposition and composition changes in functional groups. Furthermore, the crucial role of this phenomenon for the room temperature stability of GO is confirmed and a so far unnoticed role of the environment on the agglomeration process is revealed.