Electrochemical Cutting in Weak Aqueous Electrolytes: The Strategy for Efficient and Controllable Preparation of Graphene Quantum Dots.

The controllable and efficient electrochemical preparation of highly crystalline graphene quantum dots (GQDs) in an aqueous system is still challenging. Here, we developed a weak electrolyte-based (typically an ammonia solution) electrochemical method to enhance the oxidation and cutting process and therefore achieve a high yield of GQDs. The yield of GQDs (3-8 nm) is 28%, approximately 28 times higher than the yield of GQDs prepared by other strong electrolytes. The whole preparation process can be accomplished within 2 h because of the effective free radical oxidation process and the suppressed intercalation-induced exfoliation in weakly ionized aqueous electrolytes. The GQDs also showed excellent crystallinity which is obviously better than the crystallinity of GQDs obtained via bottom-up approaches. Moreover, amino-functionalization of GQDs can be realized by manipulating the electrolyte concentration. We further demonstrate that the proposed method can also be expanded to other weak electrolytes (such as HF and H2S) and different anode precursor materials (such as graphene/graphite papers, carbon fibers, and carbon nanotubes).

2D-Topology-Seeded Graphitization for Highly Thermally Conductive Carbon Fibers.

Highly thermally conductive carbon fibers (CFs) have become an important material to meet the increasing demand for efficient heat dissipation. To date, high thermal conductivity has been only achieved in specific pitch-based CFs with high crystallinity. However, obtaining high graphitic crystallinity and high thermal conductivity beyond pitch-CFs remains a grand challenge. Here, a 2D-topology-seeded graphitization method is presented to mediate the topological incompatibility in graphitization by seeding 2D graphene oxide (GO) sheets into the polyacrylonitrile (PAN) precursor. Strong mechanical strength and high thermal conductivity up to 850 W m- 1 K-1 are simultaneously realized, which are one order of magnitude higher in conductivity than commercial PAN-based CFs. The self-oxidation and seeded graphitization effect generate large crystallite size and high orientation to far exceed those of conventional CFs. Topologically seeded graphitization, verified in experiments and simulations, allows conversion of the non-graphitizable into graphitizable materials by incorporating 2D seeds. This method extends the preparation of highly thermally conductive CFs, which has great potential for lightweight thermal-management materials.

A polyimide-pyrolyzed carbon waste approach for the scalable and controlled electrochemical preparation of size-tunable graphene.

Carbon materials are widely used in numerous fields, thus changing our lives. With the increasing consumption of carbon-based products, the disposal of consequent wastes has become a challenge due to their inert nature, which is hard to degrade, burn, or melt. Here, a recyclable strategy is proposed to deal with the explosive growth of carbon wastes. Through a fast and clean electrochemical method, carbon wastes are converted into functional building blocks of high value, such as graphene and graphene quantum dots (GQDs). For typical polyimide-pyrolyzed carbon (PPC), we establish the relationship between the chemical structure of raw materials and the characteristics of graphene products, including size and yield. The size-tunable graphene ranging from 3 nm to tens of micrometers is prepared by tuning the sp3/sp2 carbon ratio of PPC from 0.5 to 0 at adjustable temperatures (800 °C-2800 °C). Significantly, PPC with a bicontinuous structure (comprising sp2 and sp3) was efficiently cut into GQDs in 2 h with a high yield of 98%. Our protocol offers great potential for the scale-up preparations and applications of GQDs. Besides, we demonstrate that the GQDs performed well as dispersants to disperse hydrophobic carbon nanotubes (0.6 mg mL-1) in water and improved the gravimetric capacitance of graphene-based supercapacitors by 79.4% with 3% GQDs added as nano-fillers.

Electrochemical Strategy for Flexible and Highly Conductive Carbon Films: The Role of 3-Dimensional Graphene/Graphite Aggregates.

Conductive carbon films with good flexibility are ever-increasingly desired for electronics. Previous efforts relying on graphene films to achieve this required special treatment to create wrinkles in the lamellar stacking sheet structure. Here, films with a wrinkled structure were facilely fabricated from electrochemically derived 3-dimiensional (3D) graphene/graphite aggregates, exhibiting excellent flexibility and high conductivity. The resulting films are very flexible that can bear 1000 times fold without breakage. A high conductivity up to 100 000 S m-1 can be achieved after a relatively low temperature annealing (1000 °C) owing to its low content of defect and large size of graphene/graphite aggregates. Based on these properties, an electrothermal heater assembled from these composite films supplies a high saturated temperature (423 °C) at low working voltages (4 V). These superior properties, together with the advantage of environmental friendliness and facile and large-scale fabrication, endow the composite films with great potential applications in flexible electronics.

Green and Mild Oxidation: An Efficient Strategy toward Water-Dispersible Graphene.

Scalable fabrication of water-dispersible graphene (W-Gr) is highly desirable yet technically challenging for most practical applications of graphene. Herein, a green and mild oxidation strategy to prepare bulk W-Gr (dispersion, slurry, and powder) with high yield was proposed by fully exploiting structure defects of thermally reduced graphene oxide (TRGO) and oxidizing radicals generated from hydrogen peroxide (H2O2). Owing to the increased carboxyl group from the mild oxidation process, the obtained W-Gr can be redispersed in low-boiling solvents with a reasonable concentration. Benefiting from the modified surface chemistry, macroscopic samples processed from the W-Gr show good hydrophilicity (water contact angle of 55.7°) and excellent biocompatibility, which is expected to be an alternative biomaterial for bone, vessel, and skin regeneration. In addition, the green and mild oxidation strategy is also proven to be effective for dispersing other carbon nanomaterials in a water system.