Chemical and Biomolecular Engineering - Research Publications

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    Revisiting cell-particle association in vitro: A quantitative method to compare particle performance.
    Faria, M ; Noi, KF ; Dai, Q ; Björnmalm, M ; Johnston, ST ; Kempe, K ; Caruso, F ; Crampin, EJ (Elsevier, 2019-08-10)
    Nanoengineering has the potential to revolutionize medicine by designing drug delivery systems that are both efficacious and highly selective. Determination of the affinity between cell lines and nanoparticles is thus of central importance, both to enable comparison of particles and to facilitate prediction of in vivo response. Attempts to compare particle performance can be dominated by experimental artifacts (including settling effects) or variability in experimental protocol. Instead, qualitative methods are generally used, limiting the reusability of many studies. Herein, we introduce a mathematical model-based approach to quantify the affinity between a cell-particle pairing, independent of the aforementioned confounding artifacts. The analysis presented can serve as a quantitative metric of the stealth, fouling, and targeting performance of nanoengineered particles in vitro. We validate this approach using a newly created in vitro dataset, consisting of seven different disulfide-stabilized poly(methacrylic acid) particles ranging from ~100 to 1000 nm in diameter that were incubated with three different cell lines (HeLa, THP-1, and RAW 264.7). We further expanded this dataset through the inclusion of previously published data and use it to determine which of five mathematical models best describe cell-particle association. We subsequently use this model to perform a quantitative comparison of cell-particle association for cell-particle pairings in our dataset. This analysis reveals a more complex cell-particle association relationship than a simplistic interpretation of the data, which erroneously assigns high affinity for all cell lines examined to large particles. Finally, we provide an online tool (http://bionano.xyz/estimator), which allows other researchers to easily apply this modeling approach to their experimental results.
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    Minimum information reporting in bio-nano experimental literature
    Faria, M ; Bjornmalm, M ; Thurecht, KJ ; Kent, SJ ; Parton, RG ; Kavallaris, M ; Johnston, APR ; Gooding, JJ ; Corrie, SR ; Boyd, BJ ; Thordarson, P ; Whittaker, AK ; Stevens, MM ; Prestidge, CA ; Porter, CJH ; Parak, WJ ; Davis, TP ; Crampin, EJ ; Caruso, F (NATURE PUBLISHING GROUP, 2018-09)
    Studying the interactions between nanoengineered materials and biological systems plays a vital role in the development of biological applications of nanotechnology and the improvement of our fundamental understanding of the bio-nano interface. A significant barrier to progress in this multidisciplinary area is the variability of published literature with regards to characterizations performed and experimental details reported. Here, we suggest a 'minimum information standard' for experimental literature investigating bio-nano interactions. This standard consists of specific components to be reported, divided into three categories: material characterization, biological characterization and details of experimental protocols. Our intention is for these proposed standards to improve reproducibility, increase quantitative comparisons of bio-nano materials, and facilitate meta analyses and in silico modelling.
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    Rust-Mediated Continuous Assembly of Metal-Phenolic Networks
    Rahim, MA ; Bjoernmalm, M ; Bertleff-Zieschang, N ; Besford, Q ; Mettu, S ; Suma, T ; Faria, M ; Caruso, F (WILEY-V C H VERLAG GMBH, 2017-06-13)
    The use of natural compounds for preparing hybrid molecular films-such as surface coatings made from metal-phenolic networks (MPNs)-is of interest in areas ranging from catalysis and separations to biomedicine. However, to date, the film growth of MPNs has been observed to proceed in discrete steps (≈10 nm per step) where the coordination-driven interfacial assembly ceases beyond a finite time (≈1 min). Here, it is demonstrated that the assembly process for MPNs can be modulated from discrete to continuous by utilizing solid-state reactants (i.e., rusted iron objects). Gallic acid etches iron from rust and produces chelate complexes in solution that continuously assemble at the interface of solid substrates dispersed in the system. The result is stable, continuous growth of MPN films. The presented double dynamic process-that is, etching and self-assembly-provides new insights into the chemistry of MPN assembly while enabling control over the MPN film thickness by simply varying the reaction time.
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    Controlling the Growth of Metal-Organic Frameworks Using Different Gravitational Forces
    Richardson, JJ ; Liang, K ; Lisi, F ; Bjoernmalm, M ; Faria, M ; Guo, J ; Falcaro, P (WILEY-V C H VERLAG GMBH, 2016-09-01)
    Control over Metal‐organic framework (MOF) size and morphology is interesting for both fundamental and applied science. Gravitational force (g) is generally acknowledged as an interesting parameter for controlling crystal size; however, a dedicated study on the effect of g on MOF synthesis is missing. Here, we investigate the effect of varied g (< 1, 1, 20, 50, and 100) during the crystallization of different MOFs [ZIF‐8, Tb2(BDC)3 and HKUST‐1] in solution. The obtained MOFs were investigated using dynamic light scattering (DLS), X‐ray scattering (SAXS and WAXS), and scanning electron and optical microscopy (SEM and OM, respectively). When compared with standard g (g = 1), high g (g = 20) gave rise to the formation of smaller MOF crystals, while low g (g < 1) led to larger crystals likely due to facet‐oriented crystal fusion. This demonstrates that gravity and g‐force can be used to rationally control the size of different MOFs by increasing or decreasing convection (mass transfer) and sedimentation.
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    Advancing Research Using Action Cameras
    Bjornmalm, M ; Faria, M ; Caruso, F (AMER CHEMICAL SOC, 2016-12-13)
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    Nanoengineering Particles through Template Assembly
    Bjoernmalm, M ; Cui, J ; Berdeff-Zieschang, N ; Song, D ; Faria, M ; Rahim, MA ; Caruso, F (AMER CHEMICAL SOC, 2017-01-10)
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    Increasing the Impact of Materials in and beyond Bio-Nano Science
    Bjornmalm, M ; Faria, M ; Caruso, F (AMER CHEMICAL SOC, 2016-10-19)
    This is an exciting time for the field of bio-nano science: enormous progress has been made in recent years, especially in academic research, and materials developed and studied in this area are poised to make a substantial impact in real-world applications. Herein, we discuss ways to leverage the strengths of the field, current limitations, and valuable lessons learned from neighboring fields that can be adopted to accelerate scientific discovery and translational research in bio-nano science. We identify and discuss five interconnected topics: (i) the advantages of cumulative research; (ii) the necessity of aligning projects with research priorities; (iii) the value of transparent science; (iv) the opportunities presented by "dark data"; and (v) the importance of establishing bio-nano standards.
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    Metal-Phenolic Supramolecular Gelation
    Rahim, MA ; Bjornmalm, M ; Suma, T ; Faria, M ; Ju, Y ; Kempe, K ; Muellner, M ; Ejima, H ; Stickland, AD ; Caruso, F (WILEY-V C H VERLAG GMBH, 2016-10-24)
    Materials assembled by coordination interactions between naturally abundant polyphenols and metals are of interest for a wide range of applications, including crystallization, catalysis, and drug delivery. Such an interest has led to the development of thin films with tunable, dynamic properties, however, creating bulk materials remains a challenge. Reported here is a class of metallogels formed by direct gelation between inexpensive, naturally abundant tannic acid and group(IV) metal ions. The metallogels exhibit diverse properties, including self-healing and transparency, and can be doped with various materials by in situ co-gelation. The robustness and flexibility, combined with the ease, low cost, and scalability of the coordination-driven assembly process make these metallogels potential candidates for chemical, biomedical, and environmental applications.
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    Dynamic Flow Impacts Cell-Particle Interactions: Sedimentation and Particle Shape Effects
    Bjornmalm, M ; Faria, M ; Chen, X ; Cui, J ; Caruso, F (AMER CHEMICAL SOC, 2016-10-25)
    The interaction of engineered particles with biological systems determines their performance in biomedical applications. Although standard static cell cultures remain the norm for in vitro studies, modern models mimicking aspects of the dynamic in vivo environment have been developed. Herein, we investigate fundamental cell-particle interactions under dynamic flow conditions using a simple and self-contained device together with standard multiwell cell culture plates. We engineer two particle systems and evaluate their cell interactions under dynamic flow, and we compare the results to standard static cell cultures. We find substantial differences between static and dynamic flow conditions and attribute these to particle shape and sedimentation effects. These results demonstrate how standard static assays can be complemented by dynamic flow assays for a more comprehensive understanding of fundamental cell-particle interactions.
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    A Framework to Account for Sedimentation and Diffusion in Particle-Cell Interactions
    Cui, J ; Faria, M ; Bjornmalm, M ; Ju, Y ; Suma, T ; Gunawan, ST ; Richardson, JJ ; Heidar, H ; Bals, S ; Crampin, EJ ; Caruso, F (AMER CHEMICAL SOC, 2016-11-29)
    In vitro experiments provide a solid basis for understanding the interactions between particles and biological systems. An important confounding variable for these studies is the difference between the amount of particles administered and that which reaches the surface of cells. Here, we engineer a hydrogel-based nanoparticle system and combine in situ characterization techniques, 3D-printed cell cultures, and computational modeling to evaluate and study particle-cell interactions of advanced particle systems. The framework presented demonstrates how sedimentation and diffusion can explain differences in particle-cell association, and provides a means to account for these effects. Finally, using in silico modeling, we predict the proportion of particles that reaches the cell surface using common experimental conditions for a wide range of inorganic and organic micro- and nanoparticles. This work can assist in the understanding and control of sedimentation and diffusion when investigating cellular interactions of engineered particles.