Graphene oxide is highly desired for printing electronics, catalysis, energy storage, separation membranes, biomedicine, and composites. However, the present synthesis methods depend on the reactions of graphite with mixed strong oxidants, which suffer from explosion risk, serious environmental pollution, and long-reaction time up to hundreds of hours. Here, we report a scalable, safe and green method to synthesize graphene oxide with a high yield based on water electrolytic oxidation of graphite. The graphite lattice is fully oxidized within a few seconds in our electrochemical oxidation reaction, and the graphene oxide obtained is similar to those achieved by the present methods. We also discuss the synthesis mechanism and demonstrate continuous and controlled synthesis of graphene oxide and its use for transparent conductive films, strong papers, and ultra-light elastic aerogels.
Ultrathin, lightweight, high‐strength, and thermally conductive electromagnetic interference (EMI) shielding materials with high shielding effectiveness (SE) are highly desired for next‐generation portable and wearable electronics. Pristine graphene (PG) has a great potential to meet all the above requirements, but the poor processability of PG nanosheets hinders its applications. Here, efficient synthesis of highly aligned laminated PG films and nacre‐like PG/polymer composites with a superhigh PG loading up to 90 wt% by a scanning centrifugal casting method is reported. Due to the PG‐nanosheets‐alignment‐induced high electrical conductivity and multiple internal reflections, such films show superhigh EMI SE comparable to the reported best synthetic material, MXene films, at an ultralow thickness. An EMI SE of 93 dB is obtained for the PG film at a thickness of ≈100 µm, and 63 dB is achieved for the PG/polyimide composite film at a thickness of ≈60 µm. Furthermore, such PG‐nanosheets‐based films show much higher mechanical strength (up to 145 MPa) and thermal conductivity (up to 190 W m−1 K−1) than those of their MXene counterparts. These excellent comprehensive properties, along with ease of mass production, pave the way for practical applications of PG nanosheets in EMI shielding.
It is crucial to align two-dimensional nanosheets to form a highly compact layered structure for many applications, such as electronics, optoelectronics, thermal management, energy storage, separation membranes, and composites. Here we show that continuous centrifugal casting is a universal, scalable and efficient method to produce highly aligned and compact two-dimensional nanosheets films with record performances. The synthesis mechanism, structure control and property dependence of alignment and compaction of the films are discussed. Significantly, 10-μm-thick graphene oxide films can be synthesized within 1 min, and scalable synthesis of meter-scale films is demonstrated. The reduced graphene oxide films show super-high strength (~660 MPa) and conductivity (~650 S cm−1). The reduced graphene oxide/carbon nanotube hybrid-film-based all-solid-state flexible supercapacitors exhibit ultrahigh volumetric capacitance (407 F cm−3) and energy density (~10 mWh cm−3) comparable to that of thin-film lithium batteries. We also demonstrate the production of highly anisotropic graphene nanocomposites as well as aligned, compact films and vertical heterostructures of various nanosheets.
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