Continuous crystalline graphene papers with gigapascal strength by intercalation modulated plasticization

Abstract

Graphene has an extremely high in-plane strength yet considerable out-of-plane softness. High crystalline order of graphene assemblies is desired to utilize their in-plane properties, however, challenged by the easy formation of chaotic wrinkles for the intrinsic softness. Here, we find an intercalation modulated plasticization phenomenon, present a continuous plasticization stretching method to regulate spontaneous wrinkles of graphene sheets into crystalline orders, and fabricate continuous graphene papers with a high Hermans' order of 0.93. The crystalline graphene paper exhibits superior mechanical (tensile strength of 1.1 GPa, stiffness of 62.8 GPa) and conductive properties (electrical conductivity of 1.1 × 10 5 S m −1 , thermal conductivity of 109.11 W m −1 K −1). We extend the ultrastrong graphene papers to the realistic laminated composites and achieve high strength combining with attractive conductive and electromagnetic shielding performance. The intercalation modulated plasticity is revealed as a vital state of graphene assemblies, contributing to their industrial processing as metals and plastics.

3D Lamellar-Structured Graphene Aerogels for Thermal Interface Composites with High Through-Plane Thermal Conductivity and Fracture Toughness

“…2 c, d). These results prove that the increase in the GO dosage results in increases in graphene crystallinity as well as decreases in graphene sheet curvature [ 48 , 49 ].

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Highly Crystalline Graphene Fibers with Superior Strength and Conductivities by Plasticization Spinning

“…We calculated the sheet orientation degree of these rGFs by azimuthal scanning of (002) plane in wide angle X-ray scattering patterns (WAXS; Figure 3g-j). [10,24,25] The orientation degree of rGF is improved gradually from 0.64 of nascent rGF to 0.86 of rGF with SR of 32% (Figure 3k). The structural regulation also compacts graphene sheets in fibers with an enhanced density from 1.32 to 1.75 g cm −3 (Figure 3k).…”

“…[22,23] Different interlayer distance guided elastic-plastic transformation for GOFs corresponds with and confirms our recently reported intercalation modulated plasticization. [24] Based on the established deformable tension-shear (DTS) chain model, we rationalized the plasticization with the concept of self-healable interlayer links (van der Waals attraction, π-π interaction, and hydrogen bonding). The failure and reconstruction of interlayer links in balance contribute to the plastic strain like the dislocation gliding in metal.…”

Hydroplastic Micromolding of 2D Sheets

“…The molded GOPs, i.e., the dried GOPs after molding and solvent removal, became stronger but more brittle with no notable changes in the overall elongation and performance compared with the original casting GOPs (Figure S8, Supporting Information). [ 13 ] Microscopic sheet slippage was observed by fracture morphology analysis using a scanning electron microscope (SEM) (Figure 2c–f). Fractures occurred around the outer perimeter of the neck at an angle of ≈45° with a tensile axis by shear deformation (Figure 2e), accompanied by delamination and buckling of GO sheets.…”

“…Random wrinkles were eliminated in graphene fibers and papers and their overall performances improved by stretching plastic lamellate solids. [ 13 ] Although these efforts indicate the potential for a plastic state in solvated 2D sheets, high‐precision plastic manufacturing similar to that applied to metals and polymers has not been achieved yet.…”