A Straightforward approach to multifunctional graphene

Graphene has been covalently functionalized through a one‐pot reductive pathway using graphite intercalation compounds (GICs), in particular KC8, with three different orthogonally protected derivatives of 4‐aminobenzylamine. This novel multifunctional platform exhibits excellent bulk functionalization homogeneity (Hbulk) and degree of addition while preserving the chemical functionalities of the organic addends through different protecting groups, namely: tert‐butyloxycarbonyl (Boc), benzyloxycarbonyl (Cbz) and phthalimide (Pht). We have employed (temperature‐dependent) statistical Raman spectroscopy (SRS), X‐ray photoelectron spectroscopy (XPS), magic angle spinning solid state 13C NMR (MAS‐NMR), and a characterization tool consisting of thermogravimetric analysis coupled with gas chromatography and mass spectrometry (TG‐GC‐MS) to unambiguously demonstrate the covalent binding and the chemical nature of the different molecular linkers. This work paves the way for the development of smart graphene‐based materials of great interest in biomedicine or electronics, to name a few, and will serve as a guide in the design of new 2D multifunctional materials

Tuning Conductivity and Spin Dynamics in Few-Layer Graphene via In Situ Potassium Exposure

Chemical modification such as intercalation or doping of novel materials is of great importance for exploratory material science and applications in various fields of physics and chemistry. Herein, the systematic intercalation of chemically exfoliated few-layer graphene with potassium is reported while monitoring the sample resistance using microwave conductivity. It is found that the conductivity of the samples increases by about an order of magnitude upon potassium exposure. The increased number of charge carriers deduced from the electron spin resonance (ESR) intensity also reflects this increment. The doped phases exhibit two asymmetric Dysonian lines in ESR, a usual sign of the presence of mobile charge carriers. The width of the broader component increases with the doping steps; however, the narrow components seem to have a constant line width

Solvent-driven electron trapping and mass transport in reduced graphites to access perfect graphene

Herein, we report on a significant discovery, namely, the quantitative discharging of reduced graphite forms, such as graphite intercalation compounds, graphenide dispersions and graphenides deposited on surfaces with the simple solvent benzonitrile. Because of its comparatively low reduction potential, benzonitrile is reduced during this process to the radical anion, which exhibits a red colour and serves as a reporter molecule for the quantitative determination of negative charges on the carbon sheets. Moreover, this discovery reveals a very fundamental physical–chemical phenomenon, namely a quantitative solvent reduction induced and electrostatically driven mass transport of K+ ions from the graphite intercalation compounds into the liquid. The simple treatment of dispersed graphenides suspended on silica substrates with benzonitrile leads to the clean conversion to graphene. This unprecedented procedure represents a rather mild, scalable and inexpensive method for graphene production surpassing previous wet-chemical approaches