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Dynamics of colloidal particles can be controlled by the application of electric fields at micrometer-nanometer length scales. Here, an electric field-coupled microfluidic flow-focusing device is designed for investigating the effect of an externally applied alternating current (AC) electric field on the hydrodynamic assembly of cellulose nanofibrils (CNFs). We first discuss how the nanofibrils align parallel to the direction of the applied field without flow. Then, we apply an electric field during hydrodynamic assembly in the microfluidic channel and observe the effects on the mechanical properties of the assembled nanostructures. We further discuss the nanoscale orientational dynamics of the polydisperse and entangled fibrillar suspension of CNFs in the channel. It is shown that electric fields induced with the electrodes locally increase the degree of orientation. However, hydrodynamic alignment is demonstrated to be much more efficient than the electric field for aligning CNFs. The results are useful for understanding the development of the nanostructure when designing high-performance materials with microfluidics in the presence of external stimuli., QC 20210803

Personalized wound dressings provide enhanced healing for different wound types; however multicomponent wound dressings with discretely controllable delivery of different biologically active agents are yet to be developed. Here we report 3D-printed multicomponent biocomposite hydrogel wound dressings that have been selectively loaded with small molecules, metal nanoparticles, and proteins for independently controlled release at the wound site. Hydrogel wound dressings carrying antibacterial silver nanoparticles and vascular endothelial growth factor with predetermined release profiles were utilized to study the physiological response of the wound in a mouse model. Compared to controls, the application of dressings resulted in improvement in granulation tissue formation and differential levels of vascular density, dependent on the release profile of the growth factor. Our study demonstrates the versatility of the 3D-printed hydrogel dressings that can yield varied physiological responses in vivo and can further be adapted for personalized treatment of various wound types., QC 20210901

Hydrodynamic alignment of proteinaceous or polymeric nanofibrillar building blocks can be utilized for subsequent assembly into intricate three-dimensional macrostructures. The non-equilibrium structure of flowing nanofibrils relies on a complex balance between the imposed flow-field, colloidal interactions and Brownian motion. The understanding of the impact of non-equilibrium dynamics is not only weak, but is also required for structural control. Investigation of underlying dynamics imposed by the flow requiresin situdynamic characterization and is limited by the time-resolution of existing characterization methods, specifically on the nanoscale. Here, we present and demonstrate a flow-stop technique, using polarized optical microscopy (POM) to quantify the anisotropic orientation and diffusivity of nanofibrils in shear and extensional flows. Microscopy results are combined with small-angle X-ray scattering (SAXS) measurements to estimate the orientation of nanofibrils in motion and simultaneous structural changes in a loose network. Diffusivity of polydisperse systems is observed to act on multiple timescales, which is interpreted as an effect of apparent fibril lengths that also include nanoscale entanglements. The origin of the fastest diffusivity is correlated to the strength of velocity gradients, independent of type of deformation (shear or extension). Fibrils in extensional flow results in highly anisotropic systems enhancing interfibrillar contacts, which is evident through a slowing down of diffusive timescales. Our results strongly emphasize the need for careful design of fluidic microsystems for assembling fibrillar building blocks into high-performance macrostructures relying on improved understanding of nanoscale physics., QC 20200908

Many nanoscale biopolymer building blocks with defect-free molecular structure and exceptional mechanical properties have the potential to surpass the performance of existing fossil-based materials with respect to barrier properties, load-bearing substrates for advanced functionalities, as well as light-weight construction. Comprehension and control of performance variations of macroscopic biopolymer materials caused by humidity-driven structural changes at the nanoscale are imperative and challenging. A long-lasting challenge is the interaction with water molecules causing reversible changes in the intrinsic molecular structures that adversely affects the macroscale performance. Using in situ advanced X-ray and neutron scattering techniques, we reveal the structural rearrangements at the nanoscale in ultrathin nanocellulose films with humidity variations. These reversible rearrangements are then correlated with wettability that can be tuned. The results and methodology have general implications not only on the performance of cellulose-based materials but also for hierarchical materials fabricated with other organic and inorganic moisture-sensitive building blocks., QC 20200916

QC 20190918

QC 20190919

Polydisperse fiber networks are the basis of many natural and manufactured structures, ranging from high-performance biobased materials to components of living cells and tissues. The formation and behavior of such networks are given by fiber properties such as length and stiffness as well as the number density and fiber-fiber interactions. Studies of fiber network behavior, such as connectivity or rigidity thresholds, typically assume monodisperse fiber lengths and isotropic fiber orientation distributions, specifically for nano scale fibers, where the methods providing time-resolved measurements are limited. Using birefringence measurements in a microfluidic flow-focusing channel combined with a flow stop procedure, we here propose a methodology allowing investigations of length-dependent rotational dynamics of nanoscale polydisperse fiber suspensions, including the effects of initial nonisotropic orientation distributions. Transition from rotational mobility to rigidity at entanglement thresholds is specifically addressed for a number of nanocellulose suspensions, which are used as model nanofiber systems. The results show that the proposed method allows the characterization of the subtle interplay between Brownian diffusion and nanoparticle alignment on network dynamics., QC 20190318. QC 20191031

QC 20180718

QC 20190111

Nanoscale building blocks of many materials exhibit extraordinary mechanical properties due to their defect-free molecular structure. Translation of these high mechanical properties to macroscopic materials represents a difficult materials engineering challenge due to the necessity to organize these building blocks into multiscale patterns and mitigate defects emerging at larger scales. Cellulose nanofibrils (CNFs), the most abundant structural element in living systems, has impressively high strength and stiffness, but natural or artificial cellulose composites are 3-15 times weaker than the CNFs. Here, we report the flow-assisted organization of CNFs into macroscale fibers with nearly perfect unidirectional alignment. Efficient stress transfer from macroscale to individual CNF due to cross-linking and high degree of order enables their Young's modulus to reach up to 86 GPa and a tensile strength of 1.57 GPa, exceeding the mechanical properties of known natural or synthetic biopolymeric materials. The specific strength of our CNF fibers engineered at multiscale also exceeds that of metals, alloys, and glass fibers, enhancing the potential of sustainable lightweight high-performance materials with multiscale self-organization., QC 20180608

Successful assembly of suspended nanoscale rod-like particles depends on fundamental phenomena controlling rotational and translational diffusion. Despite the significant developments in fluidic fabrication of nanostructured materials, the ability to quantify the dynamics in processing systems remains challenging. Here we demonstrate an experimental method for characterization of the orientation dynamics of nanorod suspensions in assembly flows using orientation relaxation. This relaxation, measured by birefringence and obtained after rapidly stopping the flow, is deconvoluted with an inverse Laplace transform to extract a length distribution of aligned nanorods. The methodology is illustrated using nanocelluloses as model systems, where the coupling of rotational diffusion coefficients to particle size distributions as well as flow-induced orientation mechanisms are elucidated., QC 20180903

Mechanistic behavior and flow properties of cellulose nanofibers (CNFs) in aqueous systems can be described by the crowding factor and the concept of contact points, which are functions of the aspect ratio and concentration of CNF in the suspension. In this study, CNFs with a range of aspect ratio and surface charge density (380-1360 mu mol/g) were used to demonstrate this methodology. It was shown that the critical networking point of the CNF suspension, determined by rheological measurements, was consistent with the gel crowding factor, which was 16. Correlated to the crowding factor, both viscosity and modulus of the systems were found to decrease by increasing the charge density of CNF, which also affected the flocculation behavior. Interestingly, an anomalous rheological behavior was observed near the overlap concentration (0.05 wt %) of CNF, at which the crowding factor was below the gel crowding factor, and the storage modulus (G') decreased dramatically at a given frequency threshold. This behavior is discussed in relation to the breakup of the entangled flocs and network in the suspension. The analysis of the mechanistic behavior of CNF aqueous suspensions by the crowding factor provides useful insight for fabricating high-performance nanocellulose-based materials., QC 20180323

QC 20190205

We present the synthesis and applications of multifunctional hollow porous carbon spheres with well-ordered pore architecture and ability to encapsulate functional nanoparticles. In the present work, the applications of hollow mesoporous carbon capsules (HMCCs) are illustrated in two different contexts. In the first approach, the hollow capsule core is used to encapsulate silver nanoparticles to impart antimicrobial characteristics. It is shown that silver-loaded HMCCs (concentration ?100 μg/mL) inhibit the growth and multiplication of bacterial colonies of Escherichia coli (Gram-negative) and Staphylococcus aureus (Gram-positive) up to 96% and 83%, respectively. In the second part, the fabrication of hierarchical micro- and nanostructured superhydrophobic coatings of HMCCs (without encapsulation with silver nanoparticles) is evaluated for anti-bioadhesion properties. Studies of protein adsorption and microorganism and platelet adhesion have shown a significant reduction (up to 100%) for the HMCC-based superhydrophobic surfaces compared with the control surfaces. Therefore, this unique architecture of HMCCs and their coatings with the ability to encapsulate functional materials make them a promising candidate for a variety of applications., QC 20170630

QC 20190225

In this work, we mechanically perturb a liquid-in-liquid jet to manipulate the size and structure of the droplets formed from break-up of the jet. The induced break-up is relatively insensitive to fluctuations in the surrounding fluid flow. When the amplitude of perturbations is large and the interfacial tension of the liquid–liquid system is low, the size of the droplets can be precisely tuned by controlling the rate at which the liquid exits the tip of the dispensing nozzle through the frequency of perturbation. When applied to microfluidic devices with the appropriate geometry, our perturbation-induced droplet approach offers a strategy to manipulating droplet structures. We demonstrate that by varying the imposed perturbation frequency and phase lag, the structure of the multi-compartmental drops and the configuration of the resultant drops in the same flow condition can be manipulated. Moreover, after careful treatment of the wettability of the devices, we show that the structure of the droplets can be precisely controlled to change from single emulsion to double emulsion within the same device. The perturbation-induced droplet generation represents a new paradigm in the engineering of droplets, enhancing current droplet-based technologies for applications ranging from particle fabrication to confined micro-reactions., QC 20160404

In this work, we mechanically perturb a liquid-in-liquid jet to manipulate the size and structure of the droplets formed from break-up of the jet. The induced break-up is relatively insensitive to fluctuations in the surrounding fluid flow. When the amplitude of perturbations is large and the interfacial tension of the liquid-liquid system is low, the size of the droplets can be precisely tuned by controlling the rate at which the liquid exits the tip of the dispensing nozzle through the frequency of perturbation. When applied to microfluidic devices with the appropriate geometry, our perturbation-induced droplet approach offers a strategy to manipulating droplet structures. We demonstrate that by varying the imposed perturbation frequency and phase lag, the structure of the multi-compartmental drops and the configuration of the resultant drops in the same flow condition can be manipulated. Moreover, after careful treatment of the wettability of the devices, we show that the structure of the droplets can be precisely controlled to change from single emulsion to double emulsion within the same device. The perturbation-induced droplet generation represents a new paradigm in the engineering of droplets, enhancing current droplet-based technologies for applications ranging from particle fabrication to confined micro-reactions., QC 20180522

Microfluidics has proven to be an efficient tool for making fine and calibrated emulsion droplets. The parallelization of drop makers is required for producing large amounts. Here, we investigate the generation of emulsion drops along a series of shallowmicrochannels emerging in a deep one, in other words the step-emulsification process. The dynamics of a single drop maker is first characterized as a function of interfacial tension and viscosities of both phases. The characteristic time scale of drop formation, namely, the necking time that finally sets drop size, is shown to be principally governed by the outer phase viscosity to interfacial tension ratio with a minor correction linked to the viscosity ratio. The step emulsification process experiences a transition of fragmentation regime where both the necking time and drop size suddenly raise. This transition, that corresponds to a critical period of drop formation and thus defines a maximum production rate of small droplets, is observed to be ruled by the viscosity ratio of the two phases. When drops are produced along an array of microchannels with a cross flow of the continuous phase, a configuration comparable to a one-dimensional membrane having rectangular pores, a drop boundary layer develops along the drop generators. In the small drop regime, the local dynamics of drop formation is shown to be independent on the emulsion cross flow. Moreover, we note that the development of the drop boundary layer is even beneficial to homogenize drop size along the production line. On the other hand, in the large drop regime, drop collision can trigger fragmentation and thus lead to size polydispersity., QC 20180522

In this study, the effect of mixed convection flow in a lid-driven porous cavity using different nanoparticles, such as aluminum oxide (Al 2 O 3), copper (Cu), silver (Ag), and titanium dioxide (TiO 2), are investigated. The base fluid is considered as water. The transport equations are solved numerically by finite volume method on a co-located grid arrangement using quadratic upwind interpolation for convective kinematics (QUICK) scheme. A two-dimensional square cavity is considered for the present investigation whose horizontal walls are insulated. The cold left wall is moving up and hot right wall is moving down with equal velocities. The variations of temperature distribution, stream function, and Nusselt number (Nu) are analyzed at constant Grashof numbers (Gr), Richardson numbers (Ri), and Darcy numbers (Da) as 1 × 10 4, 100, and 0.1, respectively, for different nanoparticles. The present results are validated by favorable comparison with previously published literature. The predicted results clearly indicate that the presence of nanoparticles inside the porous media enhances the heat transfer significantly. It is observed from the numerical results that the average Nusselt numbers (Nu) were found to increase linearly with an increase in volume fraction (χ). For the given volume fraction, the average Nu is maximum for a silver-based nanoparticle., QC 20160415

The present work encloses the application of a Brinkman-extended Darcy model in a problem concerning mixed convection ina lid-driven porous cavity using nanofluids. The transport equations are solved numerically by the finite volume method on a co-located grid arrangement using the Quadratic Upstream Interpolation for Convective Kinematics (QUICK) scheme. The effects of governing parameters, namely, Grashof number (Gr), Darcy number (Da), and solid volume fraction $(\chi)$, on the streamlines and the isotherms are studied. The present results are validated by favorable comparisons with previously published results and are in good agreement with them. The present numerical results show that the addition of nanoparticles to a base fluid has produced an augmentation of the heat transfer coefficient and it is found to increase significantly with an increase of the particle volume concentration. It is observed from the results that at the higher value of the Grashof number (Gr = 104), the average Nusselt number increases with an increase in the Darcy number for a constant solid volume fraction. The detailed results are reported by means of streamlines, isotherms, and Nusselt numbers, QC 20160415