Process for producing monolithic film of integrated highly oriented halogenated graphene sheets or molecules

A process for producing an integrated layer of highly oriented, essentially parallel halogenated graphene sheets or molecules, said process comprising:

• (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, wherein said graphene oxide sheets or graphene oxide molecules contain an oxygen amount higher than 5% by weight;
• (b) dispensing and depositing a layer of said graphene oxide dispersion or graphene oxide gel onto a surface of a supporting substrate under a shear stress condition, wherein said dispensing and depositing procedure includes shear-induced thinning of said graphene oxide dispersion or gel and shear-induced orientation of graphene oxide sheets or molecules, to form a wet layer of graphene oxide on said supporting substrate;
• and
• (c) either (i) introducing a halogenating agent into said wet layer of graphene oxide and effecting a chemical reaction between said halogenating agent and said graphene oxide sheets or molecules to form a wet layer of halogenated graphene and removing said fluid medium from said wet layer of halogenated graphene to form the integrated layer of oriented halogenated graphene sheets or molecules, or (ii) removing said fluid medium from the wet layer of graphene oxide to form a dried layer of graphene oxide and introducing a halogenating agent into said dried layer of graphene oxide and effecting a chemical reaction between said halogenating agent and said graphene oxide sheets or molecules, to form the integrated layer of oriented halogenated graphene sheets or molecules;
• wherein said integrated layer of oriented halogenated graphene sheets or molecules formed by either (i) or (ii) has a chemical formula of C6ZxOy, wherein Z is a halogen element selected from F, Cl, Br, I, or a combination thereof, x=0.01 to 6.0, y=0 to 5.0, and x+y≦6.0;
• and said integrated layer of oriented halogenated graphene sheets or molecules has an inter-planar spacing d002 of 0.35 nm to 1.2 nm as determined by X-ray diffraction.