Optimizing the mechanical properties of cellulose nanopaper through surface energy and critical length scale considerations

Published on Jun 16, 2017in Cellulose4.21
· DOI :10.1007/S10570-017-1367-X
Xin Qin7
Estimated H-index: 7
(NU: Northwestern University),
Shizhe Feng4
Estimated H-index: 4
(NU: Northwestern University)
+ 1 AuthorsSinan Keten34
Estimated H-index: 34
(NU: Northwestern University)
Cellulose nanopaper exhibits outstanding stiffness, strength, and toughness that originate from the exceptional properties of constituent cellulose nanocrystals (CNCs). However, it remains challenging to link the nanoscale properties of rod-like CNCs and their structural arrangements to the macroscale performance of nanopaper in a predictive manner. Here we address this need by establishing an atomistically informed coarse-grained model for CNCs via a strain energy conservation paradigm and simulating CNC nanopaper properties mesoscopically. We predict how the mechanical properties of CNC nanopaper with nacre-inspired brick-and-mortar structure depend on CNC overlap length and interfacial energy. We show that the modulus and strength both increase with increasing overlap length, but saturate at different critical length scales where a transition from non-covalent interfacial sliding to CNCs fracture is the key influencing mechanism. Maximum toughness is achieved when the interface and CNC failure are tuned to occur at the same time through balanced failure. We propose strategies for maximizing nanopaper mechanical performance by tuning interfacial interactions of constitutive CNCs through surface modifications that improve shear transfer capability. Our model generates broadly applicable insights into factors governing the performance of self-assembling paper materials made from 1D nanostructures.
📖 Papers frequently viewed together
38 Citations
23.9k Citations
#1Zhaoxu Meng (NU: Northwestern University)H-Index: 13
#2Rafael A. Soler-Crespo (NU: Northwestern University)H-Index: 8
Last. Sinan Keten (NU: Northwestern University)H-Index: 34
view all 7 authors...
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 mode...
33 CitationsSource
#1Djalal Trache ('ENS Paris': École Normale Supérieure)H-Index: 23
#2M. Hazwan Hussin (Universiti Sains Malaysia)H-Index: 20
Last. Vijay Kumar Thakur (Cranfield University)H-Index: 78
view all 4 authors...
Cellulose nanocrystals, a class of fascinating bio-based nanoscale materials, have received a tremendous amount of interest both in industry and academia owing to its unique structural features and impressive physicochemical properties such as biocompatibility, biodegradability, renewability, low density, adaptable surface chemistry, optical transparency, and improved mechanical properties. This nanomaterial is a promising candidate for applications in fields such as biomedical, pharmaceuticals,...
389 CitationsSource
#1Douglas M. Fox (AU: American University)H-Index: 17
#2Rebeca S. Rodriguez (AU: American University)H-Index: 1
Last. Jeffrey W. Gilman (NIST: National Institute of Standards and Technology)H-Index: 50
view all 8 authors...
Cellulose nanocrystals (CNCs) have great potential as sustainable reinforcing materials for polymers, but there are a number of obstacles to commercialization that must first be overcome. High levels of water absorption, low thermal stabilities, poor miscibility with nonpolar polymers, and irreversible aggregation of the dried CNCs are among the greatest challenges to producing cellulose nanocrystal–polymer nanocomposites. A simple, scalable technique to modify sulfated cellulose nanocrystals (N...
25 CitationsSource
#1Eleonora D'Elia (Imperial College London)H-Index: 8
#2Salvador Eslava (University of Bath)H-Index: 22
Last. Eduardo Saiz (Imperial College London)H-Index: 64
view all 5 authors...
Strong and tough natural composites such as bone, silk or nacre are often built from stiff blocks bound together using thin interfacial soft layers that can also provide sacrificial bonds for self-repair. Here we show that it is possible exploit this design in order to create self-healing structural composites by using thin supramolecular polymer interfaces between ceramic blocks. We have built model brick-and-mortar structures with ceramic contents above 95 vol% that exhibit strengths of the or...
30 CitationsSource
#1Zhaoqiang Song (USTC: University of Science and Technology of China)H-Index: 9
#2Yong Ni (USTC: University of Science and Technology of China)H-Index: 26
Last. Linghui He (USTC: University of Science and Technology of China)H-Index: 17
view all 5 authors...
Bioinspired discontinuous nanolaminate design becomes an efficient way to mitigate the strength-ductility tradeoff in brittle materials via arresting the crack at the interface followed by controllable interface failure. The analytical solution and numerical simulation based on the nonlinear shear-lag model indicates that propagation of the interface failure can be unstable or stable when the interfacial shear stress between laminae is uniform or highly localized, respectively. A dimensionless k...
29 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
#1Pei Huang (CAS: Chinese Academy of Sciences)H-Index: 4
#2Yang Zhao (CAS: Chinese Academy of Sciences)H-Index: 45
Last. Yong Huang (CAS: Chinese Academy of Sciences)H-Index: 31
view all 5 authors...
A facile method was developed to produce functionalized cellulose nanofibers in one step by ball milling. Through the synergy of mechanical and chemical actions, the produced cellulose nanofibers are ca. 20 nm wide and several micrometers long, with surface properties tailored by choice of modifying reagent. Modified by succinic anhydride, a cellulose nanofiber shows enhanced hydrophilicity, can be readily dispersed in water or DMSO, and gives a zeta potential of −38.7 mV due to carboxyl groups ...
51 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
#1Hong Dong (ARL: United States Army Research Laboratory)H-Index: 18
#2Yelena R. Sliozberg (ARL: United States Army Research Laboratory)H-Index: 12
Last. Alan W. Rudie (USFS: United States Forest Service)H-Index: 12
view all 9 authors...
Cellulose nanofibrils (CNFs) are a class of cellulosic nanomaterials with high aspect ratios that can be extracted from various natural sources. Their highly crystalline structures provide the nanofibrils with excellent mechanical and thermal properties. The main challenges of CNFs in nanocomposite applications are associated with their high hydrophilicity, which makes CNFs incompatible with hydrophobic polymers. In this study, highly transparent and toughened poly(methyl methacrylate) (PMMA) na...
42 CitationsSource
#1Xin Qin (NU: Northwestern University)H-Index: 7
#2Wenjie Xia (NU: Northwestern University)H-Index: 20
Last. Sinan Keten (NU: Northwestern University)H-Index: 34
view all 4 authors...
Cellulose nanocrystals (CNCs) exhibit impressive interfacial and mechanical properties that make them promising candidates to be used as fillers within nanocomposites. While glass-transition temperature (Tg) is a common metric for describing thermomechanical properties, its prediction is extremely difficult as it depends on filler surface chemistry, volume fraction, and size. Here, taking CNC-reinforced poly(methyl-methacrylate) (PMMA) nanocomposites as a relevant model system, we present a mult...
45 CitationsSource
Cited By17
#1Mehdi Shishehbor (Purdue University)H-Index: 8
#2Hyeyoung Son (Purdue University)H-Index: 1
Last. Pablo D. Zavattieri (Purdue University)H-Index: 37
view all 6 authors...
Abstract The mechanical properties of cellulose nanocrystal (CNC) films critically depend on many microstructural parameters such as fiber length distribution (FLD), fiber orientation distribution (FOD), and the strength of the interactions between the fibers. In this paper, we use our coarse-grained molecular model of CNC to study the effect of length and orientation distribution and attractions between CNCs on the mechanical properties of neat CNCs. The effect of misalignment of a 2D staggered...
1 CitationsSource
Cellulose is the most common biopolymer and widely used in our daily life. Due to its unique properties and biodegradability, it has been attracting increased attention in the recent years and various new applications of cellulose and its derivatives are constantly being found. The development of new materials with improved properties, however, is not always an easy task, and theoretical models and computer simulations can often help in this process. In this review, we give an overview of differ...
#1Upamanyu Ray (UMD: University of Maryland, College Park)H-Index: 9
#2Zhenqian Pang (UMD: University of Maryland, College Park)H-Index: 10
Last. Teng Li (UMD: University of Maryland, College Park)H-Index: 44
view all 3 authors...
Cellulose, the abundantly available and sustainable biopolymer, exhibits intrinsic mechanical properties superior to many high-performance structural materials. The exceptional mechanical properties of cellulose-based materials inherently hinge upon their bottom-up hierarchical material structure starting from cellulose molecular chains to large scale fibers. However, fully atomistic simulation of such materials at experimental sample dimension becomes computationally prohibitive for the explora...
1 CitationsSource
#1Qinghua Meng (CAS: Chinese Academy of Sciences)
#2Xinghua Shi (CAS: Chinese Academy of Sciences)H-Index: 35
Abstract Endowed with excellent mechanical properties, the cellulose nanopaper provides a promising design strategy for addressing the dilemma between strength and toughness of engineering materials. It is found that the anisotropic nanopaper with highly aligned nanofibers could achieve the highest mechanical properties. In this paper, we develop a multiscale tension-shear model that correlates both strength and toughness with microstructure to quantitatively understand the exceptional propertie...
#1Teng Li (UMD: University of Maryland, College Park)H-Index: 44
Abstract The ever-advancing modern world has been accompanied by rising grand challenges, from energy crisis, to environmental pollution, to access to clean water, and to curbing carbon emission. Never before has the world faced such a need for sound scientific knowledge and expertise, to better understand and tackle these rising global challenges. Natural and sustainable resources that are abundant on Earth hold great promise as solutions to these grand challenges. The EML Webinar on 29 July 20...
2 CitationsSource
#1Zhaofan Li (NDSU: North Dakota State University)H-Index: 3
#2Wenjie Xia (NDSU: North Dakota State University)H-Index: 20
Abstract Owing to the impressive mechanical properties and renewability, nanocellulose has been increasingly used for the development of lightweight materials in various applications. Here, we present a coarse-grained (CG) modeling study for investigations of mechanical performance of cellulose-based bulk material consisting of disordered cellulose nanocrystals (CNCs), forming a porous network microstructure. The simulation results reveal that increasing density and cohesive interaction between ...
7 CitationsSource
#1Chenxi Zhai (Cornell University)H-Index: 1
#1Chenxi Zhai (Cornell University)H-Index: 1
Last. Jingjie Yeo (Cornell University)H-Index: 16
view all 4 authors...
Materials chemistry is at the forefront of the global "Fourth Industrial Revolution", in part by establishing a "Materials 4.0" paradigm. A key aspect of this paradigm is developing methods to effectively integrate hardware, software, and biological systems. Towards this end, we must have intimate knowledge of the virtual space in materials design: materials omics (materiomics), materials informatics, computational modelling and simulations, artificial intelligence (AI), and big data. We focus o...
15 CitationsSource
#1Benjamin C. Marchi (NU: Northwestern University)H-Index: 1
#2Sinan Keten (NU: Northwestern University)H-Index: 34
Uniaxially arranged nanocomposite structures are common across biological materials. Through efficient structural ordering and hierarchies, these materials exhibit stiffnesses and strengths comparable to the better of their constituents. While much is known regarding the mechanical properties of materials with explicit stiff and compliant phases, substantially less is understood about neat (matrix-free) materials composed from high aspect ratio particles. A promising example of nanoparticle asse...
1 CitationsSource
#1Qinghua Meng (Xi'an Jiaotong University)H-Index: 7
#2Tiejun Wang (Xi'an Jiaotong University)H-Index: 35
34 CitationsSource
#1Majid G. RamezaniH-Index: 4
Cellulose nanocrystals (CNCs) is a promising biodegradable nanomaterial with outstanding physical, chemical, and mechanical properties for many applications. Although aligned CNCs can self-assemble into bundles, their mechanical performance is reduced by interfacial strength between CNCs and a twisted structure. In this paper, we employ developed coarse-grained (CG) molecular dynamic (MD) simulations to investigate the influence of twist and interface energy on the tensile performance of CNC bun...
11 CitationsSource