A coarse-grained model for the mechanical behavior of graphene oxide

Published on Jun 1, 2017in Carbon8.821
· DOI :10.1016/J.CARBON.2017.02.061
Zhaoxu Meng13
Estimated H-index: 13
(NU: Northwestern University),
Rafael A. Soler-Crespo8
Estimated H-index: 8
(NU: Northwestern University)
+ 4 AuthorsSinan Keten34
Estimated H-index: 34
(NU: Northwestern University)
Sources
Abstract
Abstract Graphene oxide (GO) shows promise as a nanocomposite building block due to its exceptional mechanical properties. While atomistic simulations have become central to investigating its mechanical properties, the method remains prohibitively expensive for large deformations and mesoscale failure mechanisms. To overcome this, we establish a coarse-grained (CG) model that captures key mechanical and interfacial properties, and the non-homogeneous effect of oxidation in GO sheets. The CG model consists of three types of CG beads, representing groups of pristine sp2 carbon atoms, and hydroxyl and epoxide functionalized regions. The CG force field is parameterized based on density functional-based tight binding simulations on three extreme cases. It accurately quantifies deterioration of tensile modulus and strength at the expense of improving interlayer adhesion with increasing oxidation of varying chemical compositions. We demonstrate the applicability of the model to study mesoscale phenomena by reproducing different force vs. indentation curves in silico, corroborating recent experimental observations on how chemistry near contact point influences properties. Finally, we apply the model to measure the fracture toughness of pristine graphene and GO. The critical stress intensity factor ( K c ) of graphene is found to be the highest, and epoxide-rich GO also possesses higher K c compared to hydroxyl-rich GO.
📖 Papers frequently viewed together
23.9k Citations
200841.84Science
4 Authors (Changgu Lee, ..., James Hone)
13.9k Citations
20158.82Carbon
5 Authors (Changhong Cao, ..., Tobin Filleter)
100 Citations
References64
Newest
#1Zhaoxu Meng (NU: Northwestern University)H-Index: 13
#2Miguel A. Bessa (NU: Northwestern University)H-Index: 15
Last. Sinan KetenH-Index: 34
view all 5 authors...
Predicting the macroscopic fracture energy of highly cross-linked glassy polymers from atomistic simulations is challenging due to the size of the process zone being large in these systems. Here, we present a scale-bridging approach that links atomistic molecular dynamics simulations to macroscopic fracture properties on the basis of a continuum fracture mechanics model for two different epoxy materials. Our approach reveals that the fracture energy of epoxy resins strongly depends on the functi...
40 CitationsSource
#1Rafael A. Soler-Crespo (NU: Northwestern University)H-Index: 8
#2Wei Gao (NU: Northwestern University)H-Index: 16
Last. Horacio D. Espinosa (NU: Northwestern University)H-Index: 75
view all 7 authors...
The mechanical properties of graphene oxide (GO) are of great importance for applications in materials engineering. Previous mechanochemical studies of GO typically focused on the influence of the degree of oxidation on the mechanical behavior. In this study, using density functional-based tight binding simulations, validated using density functional theory simulations, we reveal that the deformation and failure of GO are strongly dependent on the relative concentrations of epoxide (−O−) and hyd...
47 CitationsSource
#1Wenjie Xia (NU: Northwestern University)H-Index: 20
#2Jake Song (NU: Northwestern University)H-Index: 8
Last. Sinan Keten (NU: Northwestern University)H-Index: 34
view all 5 authors...
Polymers reinforced with multi-layer graphene (MLG) phases are promising candidates for new materials with high modulus, strength and toughness. Drawing inspiration from nacre's layered “brick and mortar” structure, here we propose molecular scale design strategies to improve the mechanical performance of MLG–polymer layer-by-layer nanocomposites. We present a coarse-grained molecular dynamics (CG-MD) study of interfacial failure mechanisms of MLG domains embedded in a poly(methyl methacrylate) ...
28 CitationsSource
#1Wenjie Xia (NU: Northwestern University)H-Index: 20
#2Luis Ruiz (NU: Northwestern University)H-Index: 9
Last. Sinan Keten (NU: Northwestern University)H-Index: 34
view all 4 authors...
Multi-layer graphene assemblies (MLGs) or fibers with a staggered architecture exhibit high toughness and failure strain that surpass those of the constituent single sheets. However, how the architectural parameters such as the sheet overlap length affect these mechanical properties remains unknown due in part to the limitations of mechanical continuum models. By exploring the mechanics of MLG assemblies under tensile deformation using our established coarse-grained molecular modeling framework,...
40 CitationsSource
#1Xiaoding Wei (NU: Northwestern University)H-Index: 24
#2Zhaoxu Meng (NU: Northwestern University)H-Index: 13
Last. Horacio D. Espinosa (NU: Northwestern University)H-Index: 75
view all 9 authors...
Understanding the deformation mechanisms in multilayer graphene (MLG), an attractive material used in nanodevices as well as in the reinforcement of nanocomposites, is critical yet challenging due to difficulties in experimental characterization and the spatiotemporal limitations of atomistic modeling. In this study, we combine nanomechanical experiments with coarse-grained molecular dynamics (CG-MD) simulations to elucidate the mechanisms of deformation and failure of MLG sheets. Elastic proper...
64 CitationsSource
#1Chen Shao (NU: Northwestern University)H-Index: 6
#2Sinan Keten (NU: Northwestern University)H-Index: 34
Layered assemblies of polymers and graphene derivatives employ nacre’s tested strategy of intercalating soft organic layers with hard crystalline domains. These layered systems commonly display elastic properties that exceed simple mixture rule predictions, but the molecular origins of this phenomenon are not well understood. Here we address this issue by quantifying the elastic behavior of nanoconfined polymer layers on a model layered graphene-polymer nanocomposite. Using a novel, validated co...
25 CitationsSource
#1Changhong CaoH-Index: 11
#2Matthew DalyH-Index: 11
Last. Yu SunH-Index: 67
view all 7 authors...
Graphene oxide (GO) is a layered material comprised of hierarchical features which possess vastly differing characteristic dimensions. GO nanosheets represent the critical hierarchical structure which bridges the length-scale of monolayer and bulk material architectures. In this study, the strength and fracture behavior of GO nanosheets were examined. Under uniaxial loading, the tensile strength of the nanosheets was measured to be as high as 12 ± 4 GPa, which approaches the intrinsic strength o...
35 CitationsSource
#1Xiaoding Wei (NU: Northwestern University)H-Index: 24
#2Lily Mao (NU: Northwestern University)H-Index: 6
Last. Horacio D. Espinosa (NU: Northwestern University)H-Index: 75
view all 7 authors...
The ability to bias chemical reaction pathways is a fundamental goal for chemists and material scientists to produce innovative materials. Recently, two-dimensional materials have emerged as potential platforms for exploring novel mechanically activated chemical reactions. Here we report a mechanochemical phenomenon in graphene oxide membranes, covalent epoxide-to-ether functional group transformations that deviate from epoxide ring-opening reactions, discovered through nanomechanical experiment...
69 CitationsSource
#1David D. Hsu (NU: Northwestern University)H-Index: 10
#2Wenjie Xia (NU: Northwestern University)H-Index: 20
Last. Sinan Keten (NU: Northwestern University)H-Index: 34
view all 4 authors...
We present a systematic, two-bead per monomer coarse-graining strategy allowing for the prediction of the thermomechanical behavior of polystyrene. Analytical bonded potentials optimized to match atomistic bonded distributions for different stereochemistries emulate local structure. Alternatively, the backbone torsional potential is leveraged to match the chain stiffness in a direct approach. Nonbonded potentials using a temperature-dependent density correction term demonstrate transferability o...
44 CitationsSource
#1Luis Ruiz (NU: Northwestern University)H-Index: 9
#2Wenjie Xia (NU: Northwestern University)H-Index: 20
Last. Sinan Keten (NU: Northwestern University)H-Index: 34
view all 4 authors...
Abstract Graphene is the strongest and highest weight-to-surface ratio material known, rendering it an excellent building block for nanocomposites. Multi-layer graphene (MLG) assemblies have intriguing mechanical properties distinct from the monolayer that remain poorly understood due to spatiotemporal limitations of experimental observations and atomistic modeling. To address this issue, here we establish a coarse-grained molecular dynamics (CG-MD) model of graphene using a strain energy conser...
97 CitationsSource
Cited By33
Newest
#1Yang Wang (USTB: University of Science and Technology Beijing)H-Index: 1
#2Kangmin Niu (USTB: University of Science and Technology Beijing)H-Index: 7
Last. Ying Wu (USTB: University of Science and Technology Beijing)H-Index: 3
view all 3 authors...
Abstract null null Multiscale modeling strategy development of graphene and its composites is of critical importance in engineering and technological applications. In this work, we systematically developed a chirality preserved coarse-grained graphene model and the corresponding potential, TersoffCG(16-1). The robustness of this potential is verified through structural and mechanical characterization analysis comparison between coarse-grained and all-atomistic models. The Lennard-Jones potential...
Source
#1Farzin Najafi (U of T: University of Toronto)H-Index: 3
#2Guorui Wang (U of T: University of Toronto)H-Index: 3
Last. Chandra Veer Singh (U of T: University of Toronto)H-Index: 36
view all 8 authors...
Abstract null null Under cyclic loading, while graphene can suffer from catastrophic brittle fatigue failure, graphene oxide (GO) can be engineered to improve fatigue response and possibly ductile failure. Herein, we study the fatigue response of atomically thin GO using atomistic simulations complemented by atomic force microscopy-based experiments. Analysis of the damage and failure mechanisms demonstrated a notable role of functionalization degree and ratio on the fatigue resistance of GO. In...
Source
#1Ren Sixi (Beijing University of Technology)
#2Qingsheng Yang (Beijing University of Technology)
Last. Junjun Shang (Beijing University of Technology)
view all 3 authors...
Source
#1Sihan Liu (HUST: Huazhong University of Science and Technology)H-Index: 1
#2Ke Duan (HUST: Huazhong University of Science and Technology)H-Index: 11
Last. Yujin Hu (HUST: Huazhong University of Science and Technology)H-Index: 26
view all 5 authors...
Abstract Graphene-based structures have found widespread applications in the fabrication of superior composite materials, conductors and sensors owing to their excellent properties. Molecular dynamics (MD) simulation is often used to gain an in-depth understanding of the mechanical behaviors of those structures. However, MD simulation of mesoscale graphene structures faces great challenges due to its limited model size or high computation cost. In this work, we proposed a multilayer coarse-grain...
1 CitationsSource
#1Radhika Wazalwar (IISc: Indian Institute of Science)H-Index: 1
#2Megha Sahu (IISc: Indian Institute of Science)H-Index: 4
Last. Ashok M. Raichur (IISc: Indian Institute of Science)H-Index: 38
view all 3 authors...
High-performance epoxy composites find application in the aerospace industry. Although epoxy is a high-performance polymer, its fracture toughness is compromised due to its highly cross-linked nature. Nanomaterials such as carbon nanotubes (CNTs), graphene derivatives, and inorganic 2-dimensional (2D) nanomaterials are being explored to improve epoxy composites' mechanical properties. Graphene is one of the most popular 2D nano-reinforcing agents for epoxy composites. Following graphene discover...
Source
#1Yangchao Liao (NDSU: North Dakota State University)H-Index: 1
#2Zhaofan Li (NDSU: North Dakota State University)H-Index: 3
Last. Wenjie Xia (NDSU: North Dakota State University)H-Index: 20
view all 4 authors...
Abstract Understanding the complex structural behaviors of crumpled graphene at a fundamental level is of critical importance in various engineering and technological applications. Here, we present a coarse-grained molecular dynamics (CG-MD) study for investigating structural behaviors of graphene sheets having varying sizes (or masses) during the crumpling process. The simulation results reveal that larger size graphene sheets at the initial two-dimension (2D) state tends to become more self-ad...
4 CitationsSource
#1Sadeq Hooshmand Zaferani (University of Adelaide)H-Index: 6
#2Reza Ghomashchi (University of Adelaide)H-Index: 24
Last. Daryoosh Vashaee (NCSU: North Carolina State University)H-Index: 51
view all 3 authors...
We examine the role of graphene nanoplates (GNPs) in the critical properties of thermoelectric GNP nanocomposites. After a detailed analysis of the thermoelectric, microstructural, and mechanical c...
Source
#1Shaoheng Li (UGA: University of Georgia)
#2Ning Liu (UGA: University of Georgia)H-Index: 6
Last. Xianqiao Wang (UGA: University of Georgia)H-Index: 20
view all 6 authors...
We develop a generic coarse-grained potential for a general group of 2D materials to study the mechanical performance of 2D materials-based cellular kirigami structures for understanding of the relation between the mechanical properties and structure pattern as well as the material component. By patterning the structure lattice cell, the mechanical properties of 2D materials-based structures show a very wide range from almost zero to those of the pristine 2D materials by orders of magnitude. Mor...
Source
#1Tianjiao Li (NU: Northwestern University)H-Index: 2
#2Zhaoxu Meng (Clemson University)H-Index: 13
Last. Sinan Keten (NU: Northwestern University)H-Index: 34
view all 3 authors...
Abstract Graphene oxide (GO) is a promising building block for nanocomposites due to its excellent mechanical properties and tunable interfacial interactions with polymers. While experiments have shown that GO sheets consist of graphitic regions clustering into patches and oxidized regions constituting the remaining areas, the role that these heterogeneous patches play on interfacial and mechanical properties of GO reinforced nanocomposites have not yet been investigated. To address this issue a...
8 CitationsSource
#1Christopher D. Williams (University of Manchester)H-Index: 9
#2Martin LísalH-Index: 26
Obtaining stable aqueous dispersions of graphene-based materials is a major obstacle in the development and widespread use of graphene in nanotechnology. The efficacy of atomistic simulations in obtaining a molecular-level insight into aggregation and exfoliation of graphene / graphene oxide (GO) is hindered by length and time scale limitations. In this work, we developed coarse-grained (CG) models of graphene/GO sheets, compatible with the polarizable Martini water model, using molecular dynami...
4 CitationsSource