Abstract

Pristine graphene is one of the strongest materials known in the world, and may play important roles in structural and functional materials. In order to utilize the extraordinary mechanical properties in practical engineering structures, graphene should be assembled into macroscopic structures such as graphene-based papers, fibers, foams, etc. However, the mechanical properties of graphene-based materials such as Young’s modulus and strength are 1–2 orders lower than those of pristine monolayer graphene. Many efforts have been made to unveil the multi-scale structure–property relations of graphene-based materials with hierarchical structures spanning the nanoscale to macroscale, and significant achievements have been obtained to improve the mechanical performance of graphene-based materials through composition and structure optimization across multi-scale. This review aims at summarizing the currently theoretical, simulation, and experimental efforts devoted to the multi-scale structure–property relation of graphene-based layer materials including defective monolayer graphene, nacre-like and laminar nanostructures of multilayer graphene, graphene-based papers, fibers, aerogels, and graphene/polymer composites. The mechanisms of mechanical property degradation across the multi-scale are discussed, based on which some multi-scale optimization strategies are presented to further improve the mechanical properties of graphene-based layer materials. We expect that this review can provide useful insights into the continuous improvement of mechanical properties of graphene-based layer materials.

Highlights

  • Graphene [1] has triggered great interest in two-dimensional (2D) materials in the past two decades

  • This review aims at summarizing the currently theoretical, simulation, and experimental efforts devoted to the multi-scale structure–property relation of graphene-based layer materials including defective monolayer graphene, nacre-like and laminar nanostructures of multilayer graphene, graphene-based papers, fibers, aerogels, and graphene/polymer composites

  • We primarily focus on the hierarchical structures as well as the related mechanical behaviors of graphene-based layer materials (GLMs), accompanied by a brief introduction of the fabricating methods resulting in such microstructures

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Summary

Introduction

Graphene [1] has triggered great interest in two-dimensional (2D) materials in the past two decades. The structure compaction and uniformity are two important parameters to influence the load-bearing properties of GLMs in experiments This is why GFs have superior mechanical properties, especially Young’s modulus and tensile strength, to that of GPs. the multi-scale mechanisms of mechanical property degradation from monolayer graphene to macroscopic graphene assemblies as well as the structure–property relations of GLMs are still unclear. Several strategies have been proposed to optimize the interface structures and properties to improve the overall mechanical properties of graphene nanocomposites including Young’s modulus, strength, and toughness [42,43] Other structures such as inverse nacre-like [44,45] or bicontinuous [46] laminar microstructures have been fabricated, which can simultaneously improve the strength and toughness of graphene nanocomposites.

Theoretical Models for Tension Behaviors of Monolayer Graphene
Method
Theoretical Models for Tensile Behaviors of Nacre-Like Structures
Theoretical Models for Bending Behaviors of Laminar Structure
Theoretical
Mechanical Behaviors of Monolayer Graphene
Bending Behaviors of Multilayer Graphene
In-Plane Mechanical Behaviors of Multilayer Graphene
Bending
In‐Plane Mechanical Behaviors of Multilayer Graphene
Structure–Property
Conformations of GO Macromolecules
12. Improving
Graphene Dispersed in Polymer Matrix
Polymer Infiltrated into Graphene Scaffold
Nacre-Like Graphene Nanocomposites
Multi-Scale Mechanical Property Optimization of GLMs
Findings
Conclusions and Perspectives
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