Chemical and Biomolecular Engineering - Research Publications

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    Metal-Phenolic-Mediated Assembly of Functional Small Molecules into Nanoparticles: Assembly and Bioapplications
    Chen, J ; Cortez-Jugo, C ; Kim, C-J ; Lin, Z ; Wang, T ; De Rose, R ; Xu, W ; Wang, Z ; Gu, Y ; Caruso, F (WILEY-V C H VERLAG GMBH, 2024-03-18)
    Small molecules, including therapeutic drugs and tracer molecules, play a vital role in biological processing, disease treatment and diagnosis, and have inspired various nanobiotechnology approaches to realize their biological function, particularly in drug delivery. Desirable features of a delivery system for functional small molecules (FSMs) include high biocompatibility, high loading capacity, and simple manufacturing processes, without the need for chemical modification of the FSM itself. Herein, we report a simple and versatile approach, based on metal-phenolic-mediated assembly, for assembling FSMs into nanoparticles (i.e., FSM-MPN NPs) under aqueous and ambient conditions. We demonstrate loading of anticancer drugs, latency reversal agents, and fluorophores at up to ~80 % that is mostly facilitated by π and hydrophobic interactions between the FSM and nanoparticle components. Secondary nanoparticle engineering involving coating with a polyphenol-antibody thin film or sequential co-loading of multiple FSMs enables cancer cell targeting and combination delivery, respectively. Incorporating fluorophores into FSM-MPN NPs enables the visualization of biodistribution at different time points, revealing that most of these NPs are retained in the kidney and heart 24 h post intravenous administration. This work provides a viable pathway for the rational design of small molecule nanoparticle delivery platforms for diverse biological applications.
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    Application of mechanistic modelling in membrane and fiber chromatography for purification of biotherapeutics - A review
    Qu, Y ; Baker, I ; Black, J ; Fabri, L ; Gras, SL ; Lenhoff, AM ; Kentish, SE (ELSEVIER, 2024-02-08)
    Mechanistic modelling is a simulation tool which has been effectively applied in downstream bioprocessing to model resin chromatography. Membrane and fiber chromatography are newer approaches that offer higher rates of mass transfer and consequently higher flow rates and reduced processing times. This review describes the key considerations in the development of mechanistic models for these unit operations. Mass transfer is less complex than in resin columns, but internal housing volumes can make modelling difficult, particularly for laboratory-scale devices. Flow paths are often non-linear and the dead volume is often a larger fraction of the overall volume, which may require more complex hydrodynamic models to capture residence time distributions accurately. In this respect, the combination of computational fluid dynamics with appropriate protein binding models is emerging as an ideal approach.
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    Controlling the Supramolecular Architecture Enables High Lithium Cationic Conductivity and High Electrochemical Stability for Solid Polymer Electrolytes
    Xie, K ; Fu, Q ; Chen, F ; Zhu, H ; Wang, X ; Huang, G ; Zhan, H ; Liang, Q ; Doherty, CM ; Wang, D ; Qiao, GG ; Li, D (WILEY-V C H VERLAG GMBH, 2024-01-01)
    Solid polymer electrolytes (SPEs) are long sought after for versatile applications due to their low cost, light weight, flexibility, ease of scale‐up, and low interfacial impedance. However, obtaining SPEs with high Li+ conductivity (σ+) and high voltage stability to avoid concentrated polarization and premature capacity loss has proven challenging. Here a stretchable dry‐SPE is reported with a semi‐interpenetrating, supermolecular architecture consisting of a cross‐linked polyethylene oxide (PEO) tetra‐network and an alternating copolymer poly(ethylene oxide‐alt‐butylene terephthalate). Such a unique supermolecular architecture suppresses the formation of Li+/PEO intermolecular complex and enhances the oxidation stability of PEO‐based electrolyte, thus maintaining high chain segmental motion even with high salt loading (up to 50 wt%) and achieving a wide electrochemical stability window of 5.3 V. These merits enable the simultaneous accomplishment of high ionic conductivity and high Li+ transference number (t+) to enhance the energy efficiency of energy storage device, and electrochemical stability.
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    Engineering poly(ethylene glycol) particles for targeted drug delivery
    Li, S ; Ma, Y ; Cui, J ; Caruso, F ; Ju, Y (ROYAL SOC CHEMISTRY, 2024-02-29)
    Poly(ethylene glycol) (PEG) is considered to be the "gold standard" among the stealth polymers employed for drug delivery. Using PEG to modify or engineer particles has thus gained increasing interest because of the ability to prolong blood circulation time and reduce nonspecific biodistribution of particles in vivo, owing to the low fouling and stealth properties of PEG. In addition, endowing PEG-based particles with targeting and drug-loading properties is essential to achieve enhanced drug accumulation at target sites in vivo. In this feature article, we focus on recent work on the synthesis of PEG particles, in which PEG is the main component in the particles. We highlight different synthesis methods used to generate PEG particles, the influence of the physiochemical properties of PEG particles on their stealth and targeting properties, and the application of PEG particles in targeted drug delivery.
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    Surface analysis insight note: Differentiation methods applicable to noisy data for determination of sp2-versus sp3-hybridization of carbon allotropes and AES signal strengths
    Fairley, N ; Compagnini, G ; Scardaci, V ; Baltrus, J ; Roberts, A ; Barlow, A ; Cumpson, P ; Baltrusaitis, J (WILEY, 2023-03)
    The derivatives of the spectra are commonly used for quantification in Auger Electron Spectroscopy (AES) spectra, while the derivative of the KLL C Auger line has proven to be valuable in obtaining a measure of the relative proportions of sp2‐ and sp3‐hybridization using the D‐parameter in both AES and X‐ray Photoelectron Spectroscopy (XPS). Differentiation of X‐ray Photoelectron Spectroscopy (XPS) and Auger Electron Spectroscopy (AES) spectra by numerical means is presented and illustrated for polymeric, such as PEEK and Nylon, as well as for graphitic materials including highly ordered pyrolytic graphite and graphene oxide. The most commonly available Savitzky–Golay method is explained mathematically and developed through the case of constructing a 5‐point quadratic polynomial convolution kernel suitable for differentiating spectra of adequate signal to noise. The concept of differentiation of spectra where signal to noise is less than adequate is also developed. Two alternative strategies to Savitzky–Golay differentiation are presented, which fit curves to data that allow derivatives to be obtained where Savitzky–Golay would otherwise fail. These alternative methods involve constructing a parametric curve that fits data over the entire energy interval of interest. Derivatives of spectra are then obtained by differentiating these parametric curves directly. A comparison of results for different materials for which specific sp2‐ vs sp3‐hybridized carbon proportions are of interest is used to emphasize the importance of characterizing methods used to differentiate spectra and understanding the characteristics of instrumentation used to measure spectra. The case for using Principal Component Analysis noise reduction with C KLL spectra is made for spectra collected from a heterogeneous graphene oxide sample.
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    Atomically Thin Synaptic Devices for Optoelectronic Neuromorphic Vision
    Ahmed, T ; Jannat, A ; Krishnamurthi, V ; Aung, T ; Mazumder, A ; Zavabeti, A ; Syed, N ; Daeneke, T ; Ou, JZ ; AI-Hourani, A ; Walia, S (Wiley, 2023)
    Imaging sensors with inbuilt processing capability are expected to form the backbone of low-latency and highly energy efficient artificial vision systems. A range of emerging atomically thin materials provide opportunities to exploit their electrical and optical properties for human vision and brain inspired functions. This work reports atomically thin nanosheets of β-In2S3 which exhibit inherent persistent photoconductivity (PPC) under ultraviolet and visible wavelengths. This PPC effect enables β-In2S3-based optoelectronic devices to optically mimic the dynamics of biological synapses. Based on the material characterizations, the PPC effect is attributed to the intrinsic defects in the synthesized β-In2S3 nanosheet. Furthermore, the feasibility of adopting these atomically thin synaptic devices for optoelectronic neuromorphic hardware is demonstrated by implementing a convolutional neural network for image classification. As such, the demonstrated atomically thin nanosheets and optoelectronic synaptic devices provide a platform for scaling up complex vision-sensory neural networks, which can find many promising applications for multispectral imaging and neuromorphic computation.
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    Particle Engineering via Supramolecular Assembly of Macroscopic Hydrophobic Building Blocks
    Kim, C ; Goudeli, E ; Ercole, F ; Ju, Y ; Gu, Y ; Xu, W ; Quinn, JF ; Caruso, F (Wiley, 2024-01-22)
    Abstract Tailoring the hydrophobicity of supramolecular assembly building blocks enables the fabrication of well‐defined functional materials. However, the selection of building blocks used in the assembly of metal–phenolic networks (MPNs), an emerging supramolecular assembly platform for particle engineering, has been essentially limited to hydrophilic molecules. Herein, we synthesized and applied biscatechol‐functionalized hydrophobic polymers (poly(methyl acrylate) (PMA) and poly(butyl acrylate) (PBA)) as building blocks to engineer MPN particle systems (particles and capsules). Our method allowed control over the shell thickness (e.g., between 10 and 21 nm), stiffness (e.g., from 10 to 126 mN m−1), and permeability (e.g., 28–72 % capsules were permeable to 500 kDa fluorescein isothiocyanate‐dextran) of the MPN capsules by selection of the hydrophobic polymer building blocks (PMA or PBA) and by controlling the polymer concentration in the MPN assembly solution (0.25–2.0 mM) without additional/engineered assembly processes. Molecular dynamics simulations provided insights into the structural states of the hydrophobic building blocks during assembly and mechanism of film formation. Furthermore, the hydrophobic MPNs facilitated the preparation of fluorescent‐labeled and bioactive capsules through postfunctionalization and also particle–cell association engineering by controlling the hydrophobicity of the building blocks. Engineering MPN particle systems via building block hydrophobicity is expected to expand their use.
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    Composite nanofibrous membranes with two-dimensional ZIF-L and PVDF-HFP for CO2 separation
    Kim, S ; Hou, J ; Choudhury, NR ; Kentish, SE (ELSEVIER SCIENCE SA, 2024-01-15)
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