▎ 摘　　要

NOVELTY - Producing (p1) highly oriented graphene film comprises: (a) preparing graphene oxide dispersion having graphene oxide sheets dispersed in fluid medium or graphene oxide gel having graphene oxide molecules dissolved in medium; (b) dispensing and depositing dispersion or gel onto substrate to form first layer of graphene oxide; (c) partially or completely removing fluid medium to form first dried layer of graphene oxide; (d) preparing second dried layer of graphene oxide; (e) stacking first dried layer with second dried layer or multiple sheets of dried graphene oxide; and (f) heat treating. USE - The processes are useful for producing a highly oriented graphene film or bulk highly oriented graphene film, that is used in thermal management device (all claimed) comprising a heat dissipation film used in a smart phone, tablet computer, flat-panel TV display, or other microelectronic or communications device. ADVANTAGE - The process produces highly oriented graphene film (no greater than 100 mu m in thickness) or unitary graphene film having: an electrical conductivity greater than 5000 S/cm, preferably 12000 S/cm, a thermal conductivity greater than 800 W/mK, preferably greater than 1500 W/mK, a physical density greater than 1.9 g/cm3, preferably greater than 2.1 g/cm3, a tensile strength greater than 80 MPa, preferably greater than 120 mPa, and/or an elastic modulus greater than 60 GPa, preferably 120 GPa; an inter-graphene spacing less than 0.337 nm and a mosaic spread value less than 1, degree of graphitization no less than 80% and/or a mosaic spread value less than 0.4 or degree of graphitization no less than 90% and/or a mosaic spread value no greater than 0.4 (all claimed); length or width greater than the original graphite crystallites; and great cohesion power (self-bonding, self-polymerizing and self-crosslinking capability). The process: involves lower heat treatment temperatures and lower pressures; is simple hence, more reliable, faster, less energy-intensive, and highly scalable; produces a bulk graphene oxide-derived highly oriented graphene film on a continuous roll-to-roll basis and, hence cost-effective; provides highly oriented graphene film that is an integrated graphene entity, is not a simple aggregate or stack of multiple discrete graphite flakes or discrete platelets of graphene/ graphene oxide/reduced graphite oxide, and does not contain any discernible or discrete flake/platelet derived from the original graphite oxide sheets; and does not exhibits limitation on the number layers that can be stacked and then chemically linked together to become a single integrated entity (not just an aggregate discrete graphene sheets). The graphene oxide sheets are adhered into an integrated graphene entity, without using any externally added linker or binder molecules or polymers. DETAILED DESCRIPTION - Producing (p1) a highly oriented graphene film with a thickness no greater than 0.1 mm, comprises: (a) preparing either a graphene oxide dispersion having graphene oxide sheets dispersed in a fluid medium or a graphene oxide gel having graphene oxide molecules dissolved in a fluid medium, where the graphene oxide sheets or graphene oxide molecules contain higher than 5 wt.% oxygen; (b) dispensing and depositing the graphene oxide dispersion or graphene oxide gel onto a surface of a supporting substrate to form a first layer of graphene oxide, where the step of dispensing and depositing procedure includes subjecting the graphene oxide dispersion or graphene oxide gel to an orientation-inducing stress; (c) partially or completely removing the fluid medium from the first layer of graphene oxide to form a first dried layer of graphene oxide having a layer thickness less than 200 mu m and having an inter-plane spacing (d002) of 0.4-1.2 nm as determined by X-ray diffraction and no less than 5 wt.% oxygen; (d) preparing at least a second dried layer of graphene oxide by repeating steps (b) and (c) at least one time or preparing multiple sheets of dried graphene oxide by slicing the first dried layer of graphene oxide; (e) stacking either first dried layer of graphene oxide with second dried layer of graphene oxide or multiple sheets of dried graphene oxide under an optional first compressive stress to form a mass of multiple layers of graphene oxide; and (f) heat treating the mass of multiple layers of graphene oxide under an optional second compressive stress to produce the highly oriented graphene film at a first heat treatment temperature higher than 100 degrees C to an extent that an inter-plane spacing (d002) is decreased to a value less than 0.4 nm and the oxygen content is decreased to less than 5 wt.%, where step (f) occurs before, during, or after step (e). INDEPENDENT CLAIMS are also included for: (1) producing (p2) a highly oriented graphene film with a thickness no greater than 0.1 mm; (2) producing (p3) a highly oriented graphene film with a thickness no greater than 0.1 mm; and (3) the highly oriented graphene film or bulk highly oriented graphene film produced by a processes.