Preparation of Graphene Oxide/Cellulose Composites with Microcrystalline Cellulose Acid Hydrolysis Using the Waste Acids Generated by the Hummers Method of Graphene Oxide Synthesis

The Hummers method is the most commonly used method to prepare graphene oxide (GO). However, many waste acids remain in the raw reaction mixture after the completion of this reaction. The aim of this study was to reuse these waste acids efficiently. In this study, microcrystalline cellulose (MCC) was directly dissolved in the mixture after the high-temperature reaction of the Hummers method. The residual acid was used to hydrolyze MCC, and the graphene oxide/microcrystalline cellulose (GO/MCC) composites were prepared, while the acid was reused. The effects of MCC addition (0.5 g, 1.0 g, and 1.5 g in 20 mL) on the properties of the composites were discussed. The structure, composition, thermal stability, and hydrophobicity of GO/MCC composites were characterized and tested by SEM, XRD, FTIR, TG, and contact angle tests. The results showed that MCC could be acid hydrolyzed into micron and nano-scale cellulose by using the strong acidity of waste liquid after GO preparation, and it interacted with the prepared GO to form GO/MCC composites. When the addition amount of MCC was 1 g, the thermal stability of the composite was the highest due to the interaction between acid-hydrolyzed MCC and GO sheets. At the same time, the hydrophobic property of the GO/MCC composite is better than that of the GO film. The freeze-dried GO/MCC composites are more easily dispersed in water and have stronger stability.

Effect of long-term ageing on graphene oxide: structure and thermal decomposition

After long-term ageing, the structure of graphene oxide prepared by the modified Hummers method changed. Because of the desorption of oxygen-containing functional groups, the C/O ratio of graphene oxide increased from 1.96 to 2.76. However, the average interlayer distance decreased from 0.660 to 0.567 nm. The content of -CH- and -CH 2 - decreased; however, the type of oxygen-containing functional groups did not change. Moreover, I D / I G increased from 0.87 to 0.92, indicating that the defect density decreased because of desorbing oxygen functional groups after ageing. When the temperature exceeded 60°C, CO 2 produced by decomposing graphene oxide was detected. The thermal decomposition changed after ageing. The decomposition peak temperature decreased from 216°C to 195°C. The CO 2 amount produced remained almost unchanged; however, the amount of CO, SO 2 and H 2 O decreased. After ageing, the apparent activation energy of graphene oxide decreased from 150 to 134 kJ mol −1 .

Oxidation Modification of Fuorinated Graphite and Its Reaction Mechanism

In this paper, Hummers method was used to oxidize fluorinated graphite in order to study the modification mechanism. The chemical composition and microstructure of the products before and after the reaction were characterized and analyzed. Oxidized fluorinated graphite (OFG) obtained by oxidation has a thin layered structure and different oxygen content. The main mechanism of KMnO4 modification is that MnO3+ with Lewis acid property can catalyze the activation of the fluorocarbon bond, which breaks to form F ion. At the same time, the unsaturated carbon bond is oxidized, resulting in the increase of carbon oxygen bond content and the generation of some OFG nano fragments. With the increase in KMnO4 dosage, the fluorocarbon bond will be gradually catalyzed to react according to its activity while the unsaturated carbon bond is oxidized, finally there are still some isolated fluorocarbon bonds with weak activity.

3D Graphene Oxide Hydrogel Derived from Waste Toner as Adsorbent

Waste toner powders are considered as hazardous materials to human and living things, and should be properly recycled by many effective ways due to their fine particle sizes and complex components. In this paper, waste toner powders were used as raw materials to successfully synthesize three dimensions (3D) graphene oxide (GO) hydrogel by means of a one-pot chemical transformation based on the improved Hummers’ method. The obtained 3D GO hydrogel has porous structure and abundant oxygen-containing functional groups because of the inherent 3D solid structure of waste toner powder and the strong oxidation process of the improved Hummers’ method. Interestingly, the as-prepared 3D GO hydrogel with excellent adsorptive property could quickly remove Pb(II) ions (100 mg/L, removal efficiency of 96% and removal capacity of 144 mg/g) and methylene blue (50 mg/L, removal efficiency of 97% and removal capacity of 48 mg/g) from water, respectively. The preparation process of 3D GO hydrogel was simple and easy to operate, and the output can be moderately mass produced, thus it would provide a new and effective disposal way for the recycling and reusing of waste toner.

Graphene Oxide as a Substrate for Biosensors: Synthesis and Characterization

Graphene oxide (GO) is an oxidized nanosheets of graphite with a 2D planar structure. GO could be readily complexed with bio-entities as it possesses many oxygen-containing functionalities on its surface. The preparation process is fast, easy, and cost-effective. It was prepared using modified Hummers’ method in acidic solution as a primary solvent and potassium permanganate as an oxidizing agent. Afterwards, it was successfully characterized by FTIR, UV-visible spectroscopy, as well as XRD and Raman spectroscopy, and finally, SEM analysis. It was observed that the formed GO is mainly composed of carbon and oxygen elements rich in oxygen functional groups. Furthermore, the existence of (001) plane in XRD interprets the complete oxidation of graphite with d-spacing 9 Å. Moreover, Raman spectroscopy displayed the sp3 carbon hybridization, besides, the ID/IG ratio is found to be 0.84, which confirms the disorder between graphene oxide layers. The SEM images also pointed out that graphene oxide sheets were regularly stacked together as flake-like structures. Accordingly, the richness of oxygen-containing functionalities was confirmed. Hence, it is appropriate to be used as a base transducer for biosensing applications.

Self-Photoluminescence of Unzipped Multi-Walled Carbon Nanotubes

Unzipping of carbon nanotubes (CNTs) has been widely explored to obtain new nanocarbon structures with promising properties. In this work, we report that unzipping of CNTs according to the well-established modified Hummers method produces unzipped CNTs (uCNTs) that exhibit self-photoluminescence that depends on the diameter of pristine CNTs. The uCNTs were characterized using FTIR spectroscopy, XRD, XPS, and Raman spectroscopy indicating that unzipping is accompanied by the introduction of defects and oxygen-containing functional groups. The morphology of CNTs and uCNTs was determined by TEM showing longitude unzipping of CNTs. Our study shows that increasing the diameter of pristine CNTs results in decreasing the edge etching effect and decreasing the functionality of uCNTs. Based on the UV-Vis spectra, the band gap of uCNTs was calculated using the Kubelka–Munk function. The band gap of uCNTs increased with decreasing diameter of pristine CNTs. The uCNTs exhibited photoluminescence with a good emission in the visible light region. The uCNTs with the largest band gap and the highest oxygen content had the strongest fluorescence intensity. Moreover, different metal ions produced different degrees of fluorescence quenching for uCNT-15, which verified the self-photoluminescence of uCNTs.

Tunable Synthesis of Predominant Semi-Ionic and Covalent Fluorine Bonding States on a Graphene Surface

In this study, fluorinated graphene (FG) was synthesized via a hydrothermal reaction. Graphene oxides (GOs) with different oxygen bonding states and oxygen contents (GO(F), GO(P), and GO(HU)) were used as starting materials. GO(F) and GO(P) are commercial-type GOs from Grapheneall. GO(HU) was prepared using a modified Hummers method. The synthesized FGs from GO(F), GO(P), and GO(HU) are denoted as FG(F), FG(P), and FG(HU), respectively. The F atoms were bound to the graphene surface with predominantly semi-ionic or covalent bonding depending on the GO oxygen state. FG(F) and FG(HU) exhibited less extensive fluorination than FG(P) despite the same or higher oxygen contents compared with that in FG(P). This difference was attributed to the difference in the C=O content of GOs because the C=O bonds in GO primarily produce covalent C–F bonds. Thus, FG(F) and FG(HU) mainly exhibited semi-ionic C–F bonds. The doped F atoms were used to tune the electronic properties and surface chemistry of graphene. The fluorination reaction also improved the extent of reduction of GO.