Markus J. Buehler

Quantifying the deformation of biological tissues under mechanical loading is crucial to understand its biomechanical response in physiological conditions and important for designing materials and treatments for biomedical applications. However, strain measurements for biological tissues subjected to large deformations and humid environments are challenging for conventional methods due to several limitations such as strain range, boundary conditions, surface bonding and biocompatibility. Here… Show more

Quantifying the deformation of biological tissues under mechanical loading is crucial to understand its biomechanical response in physiological conditions and important for designing materials and treatments for biomedical applications. However, strain measurements for biological tissues subjected to large deformations and humid environments are challenging for conventional methods due to several limitations such as strain range, boundary conditions, surface bonding and biocompatibility. Here we propose the use of silk solutions and printing to synthesize prototype strain gauges for large strain measurements in biological tissues. The study shows that silk-based strain gauges can be stretched up to 1300% without failure, which is more than two orders of magnitude larger than conventional strain gauges, and the mechanics can be tuned by adjusting ion content. We demonstrate that the printing approach can accurately provide well bonded fluorescent features on the silk membranes using designs which can accurately measure strain in the membrane. The results show that these new strain gauges measure large deformations in the materials by eliminating the effects of sliding from the boundaries, making the measurements more accurate than direct outputs from tensile machines. Show less

We report a new ultrathin filtration membrane prepared from silk nanofibrils (SNFs), directly exfoliated from natural Bombyx mori silk fibers to retain structure and physical properties. These membranes can be prepared with a thickness down to 40 nm with a narrow distribution of pore sizes ranging from 8 to 12 nm. Typically, 40 nm thick membranes prepared from SNFs have pure water fluxes of 13 000 L h–1 m–2 bar–1, more than 1000 times higher than most commercial ultrathin filtration membranes… Show more

We report a new ultrathin filtration membrane prepared from silk nanofibrils (SNFs), directly exfoliated from natural Bombyx mori silk fibers to retain structure and physical properties. These membranes can be prepared with a thickness down to 40 nm with a narrow distribution of pore sizes ranging from 8 to 12 nm. Typically, 40 nm thick membranes prepared from SNFs have pure water fluxes of 13 000 L h–1 m–2 bar–1, more than 1000 times higher than most commercial ultrathin filtration membranes and comparable with the highest water flux reported previously. The commercial membranes are commonly prepared from polysulfone, poly(ether sulfone), and polyamide. The SNF-based ultrathin membranes exhibit efficient separation for dyes, proteins, and colloids of nanoparticles with at least a 64% rejection of Rhodamine B. This broad-spectrum filtration membrane would have potential utility in applications such as wastewater treatment, nanotechnology, food industry, and life sciences in part due to the protein-based membrane polymer (silk), combined with the robust mechanical and separation performance features. Show less

In recent years, continuum and atomistic modeling of cementitious materials has provided significant advances towards studying the durability of civil infrastructure. An important frontier to understanding structure-property relationships is the “mesoscale”, which represents the bridge between underlying (e.g. molecular) processes and bulk macroscale behavior. This review highlights examples of a mesoscale approach within biological materials and emphasizes their applicability to the study and… Show more

In recent years, continuum and atomistic modeling of cementitious materials has provided significant advances towards studying the durability of civil infrastructure. An important frontier to understanding structure-property relationships is the “mesoscale”, which represents the bridge between underlying (e.g. molecular) processes and bulk macroscale behavior. This review highlights examples of a mesoscale approach within biological materials and emphasizes their applicability to the study and design of sustainable cement-based materials at multiple length scales. We propose a methodology focused on the coupling of computation and experiment for furthering our understanding of the microstructural properties that control the durability of hardened cement paste. Show less

We apply the mathematical framework of category theory to articulate the precise relation between the structure and mechanics of a nanoscale system in a macroscopic domain. We maintain the chosen molecular mechanical properties from the nanoscale to the continuum scale. Therein we demonstrate a procedure to 'protoype a model', as category theory enables us to maintain certain information across disparate fields of study, distinct scales, or physical realizations. This process fits naturally… Show more

We apply the mathematical framework of category theory to articulate the precise relation between the structure and mechanics of a nanoscale system in a macroscopic domain. We maintain the chosen molecular mechanical properties from the nanoscale to the continuum scale. Therein we demonstrate a procedure to 'protoype a model', as category theory enables us to maintain certain information across disparate fields of study, distinct scales, or physical realizations. This process fits naturally with prototyping, as a prototype is not a complete product but rather a reduction to test a subset of properties. To illustrate this point, we use large-scale multi-material printing to examine the scaling of the elastic modulus of 2D carbon allotropes at the macroscale and validate our printed model using experimental testing. The resulting hand-held materials can be examined more readily, and yield insights beyond those available in the original digital representations. We demonstrate this concept by twisting the material, a test beyond the scope of the original model. The method developed can be extended to other methods of additive manufacturing. Show less

Scalable computational modelling tools are required to guide the rational design of complex hierarchical materials with predictable functions. Here, we utilize mesoscopic modelling, integrated with genetic block copolymer synthesis and bioinspired spinning process, to demonstrate de novo materials design that incorporates chemistry, processing and material characterization. We find that intermediate hydrophobic/hydrophilic block ratios observed in natural spider silks and longer chain lengths… Show more

Scalable computational modelling tools are required to guide the rational design of complex hierarchical materials with predictable functions. Here, we utilize mesoscopic modelling, integrated with genetic block copolymer synthesis and bioinspired spinning process, to demonstrate de novo materials design that incorporates chemistry, processing and material characterization. We find that intermediate hydrophobic/hydrophilic block ratios observed in natural spider silks and longer chain lengths lead to outstanding silk fibre formation. This design by nature is based on the optimal combination of protein solubility, self-assembled aggregate size and polymer network topology. The original homogeneous network structure becomes heterogeneous after spinning, enhancing the anisotropic network connectivity along the shear flow direction. Extending beyond the classical polymer theory, with insights from the percolation network model, we illustrate the direct proportionality between network conductance and fibre Young's modulus. This integrated approach provides a general path towards de novo functional network materials with enhanced mechanical properties and beyond (optical, electrical or thermal) as we have experimentally verified. Show less

Defect tolerance, the capacity of a material to maintain strength even under the presence of cracks or flaws, is one of the essential demands in the design of composite materials, as manufacturing induced defects, or those generated during operation, can lead to catastrophic failure and dramatically reduce the mechanical performance. In this paper, we combine computational modeling and advanced multimaterial 3D printing to examine the mechanics of several different classes of defect-tolerant… Show more

Defect tolerance, the capacity of a material to maintain strength even under the presence of cracks or flaws, is one of the essential demands in the design of composite materials, as manufacturing induced defects, or those generated during operation, can lead to catastrophic failure and dramatically reduce the mechanical performance. In this paper, we combine computational modeling and advanced multimaterial 3D printing to examine the mechanics of several different classes of defect-tolerant bioinspired hierarchical composites, built from two base materials with contrasting mechanical properties (stiff and soft). We find that in contrast to the brittle base constituents of the composites, the existence of a hierarchical architecture leads to superior defect-tolerant properties. We show that composites with more hierarchical levels dramatically improve the defect tolerance of the material. We also examine the effect of adding both self-similar and dissimilar hierarchical levels to the materials architecture, and show that the geometries with multiple hierarchical levels can retain a significant portion of their fracture strength in the presence of either large edge cracklike flaws or multiple small distributed defects in the material. We compare the stress distributions in materials with different numbers of hierarchies in both simulation and experiment and find a more uniform stress distribution in the uncracked region of materials with higher hierarchy levels. These results provide micromechanical insights into the origin of the higher defect tolerance observed in simulation and experiment. Show less

Recently emerging ultrathin two-dimensional carbon materials provide potentially game-changing membranes for water filtration. Here we discover a changed water behavior at the nanoscale that is significantly distinct from its bulk state as water flows through two-dimensional carbon allotropes. We find that water exhibits a very high viscosity due to the cooperativity of water molecules that enhances the nonbonded H-bond interactions with the dense lattice of carbon structures, which renders… Show more

Recently emerging ultrathin two-dimensional carbon materials provide potentially game-changing membranes for water filtration. Here we discover a changed water behavior at the nanoscale that is significantly distinct from its bulk state as water flows through two-dimensional carbon allotropes. We find that water exhibits a very high viscosity due to the cooperativity of water molecules that enhances the nonbonded H-bond interactions with the dense lattice of carbon structures, which renders flow significantly more viscous, with a resistance that is inversely proportional to the sixth power of the characteristic length of the nanopores. This is in contrast to a constant value as assumed in conventional knowledge. Our findings reveal how water molecules behave drastically different from their bulk state under extreme nanoconfinement conditions. These insights enable us to incorporate the size analysis of particles in variant untreated water into membrane design and propose the design of more efficient devices with higher filtration throughput and greater mechanical resilience. Show less

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