The exceptional thermal conductivity of graphene is expected to endow polymer composites with ultrahigh thermal conductivities, which can be even similar to those of some metals such as stainless steel and aluminum alloy. The thermal conductivities of composites prepared by dispersing multilayer graphene (MLG) in epoxy matrix increase only by an order of magnitude over the pure epoxy. However, the improvement has been limited since the large interfacial thermal resistance exists between graphene and the surrounding epoxy. We have reported an extraordinary increase in thermal conductivity of the MLG/epoxy composites through the fabrication of the vertically aligned and densely packed MLG in the epoxy matrix. The ultrahigh thermal conductivity of 33.54 W/(m K) has been achieved in the aligned MLG/epoxy composite (AG/E). The thermal conductivity of AG/E exhibits a positive temperature response related to the aligned structure while increasing the temperature from 40 °C to 90 °C.

A facile and high-yield approach to the preparation of few-layer graphene (FLG) by electrochemical intercalation exfoliation (EIE) of expanded graphite in sulfuric acid electrolyte is reported. Stage-1 H2SO4-graphite intercalation compound is used as a key intermediate in EIE to realize the efficient exfoliation. The yield of the FLG sheets (<7 layers) with large lateral sizes (tens of microns) is more than 75% relative to the total amount of starting expanded graphite. A low degree of oxygen functionalization existing in the prepared FLG flakes enables them to disperse effectively, which contributes to the film-forming characteristics of the FLG flakes. These electrochemically exfoliated FLG flakes are integrated into several kinds of macroscopic graphene structures. Flexible and freestanding graphene papers made of the FLG flakes retain excellent conductivity (≈24,500 S m(-1)). Three-dimensional (3D) graphene foams with light weight are fabricated from the FLG flakes by the use of Ni foams as self-sacrifice templates. Furthermore, 3D graphene/Ni foams without any binders, which are used as supercapacitor electrodes in aqueous electrolyte, provide the specific capacitance of 113.2 F g(-1) at a current density of 0.5 A g(-1), retaining 90% capacitance after 1000 cycles.

Mass production of reduced graphene oxide and graphene nanoplatelets has recently been achieved. However, a great challenge still remains in realizing large-quantity and high-quality production of large-size thin few-layer graphene (FLG). Here, we create a novel route to solve the issue by employing one-time-only interlayer catalytic exfoliation (ICE) of salt-intercalated graphite. The typical FLG with a large lateral size of tens of microns and a thickness less than 2 nm have been obtained by a mild and durative ICE. The high-quality graphene layers preserve intact basal crystal planes owing to avoidance of the degradation reaction during both intercalation and ICE. Furthermore, we reveal that the high-quality FLG ensures a remarkable lithium-storage stability (>1,000 cycles) and a large reversible specific capacity (>600 mAh g−1). This simple and scalable technique acquiring high-quality FLG offers considerable potential for future realistic applications.