Chemical and Biomolecular Engineering - Research Publications

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    Hydrodynamic Cavitation: A Novel Non-Thermal Liquid Food Processing Technology
    Sun, X ; You, W ; Wu, Y ; Tao, Y ; Yoon, JY ; Zhang, X ; Xuan, X (FRONTIERS MEDIA SA, 2022-03-04)
    Hydrodynamic cavitation (HC), as a novel non-thermal processing technology, has recently shown unique effects on the properties of various liquid foods. The extreme conditions of pressure at ~500 bar, local hotspots with ~5,000 K, and oxidation created by HC can help obtain characteristic products with high quality and special taste. Moreover, compared with other emerging non-thermal approaches, the feature of the HC phenomenon and its generation mechanism helps determine that HC is more suitable for industrial-scale processing. This mini-review summarizes the current knowledge of the recent advances in HC-based liquid food processing. The principle of HC is briefly introduced. The effectiveness of HC on the various physical (e.g., particle size, viscosity, temperature, and stability), chemical (nutrition loss), and biological characteristics (microorganism inactivation) of various liquid foods are evaluated. Finally, several recommendations for future research on the HC technique are provided.
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    Fermentation and Storage Characteristics of "Fuji" Apple Juice Using Lactobacillus acidophilus, Lactobacillus casei and Lactobacillus plantarum: Microbial Growth, Metabolism of Bioactives and in vitro Bioactivities
    Yang, J ; Sun, Y ; Gao, T ; Wu, Y ; Sun, H ; Zhu, Q ; Liu, C ; Zhou, C ; Han, Y ; Tao, Y (FRONTIERS MEDIA SA, 2022-02-09)
    Fruit juices have been widely used as the substrates for probiotic delivery in non-dairy products. In this study, three lactic acid bacteria (LAB) strains, including Lactobacillus acidophilus, Lactobacillus casei and Lactobacillus plantarum, were selected to ferment apple juice. During 72-h of fermentation, these LAB strains grew well in the apple juice with significant increases in viable cell counts (from 7.5 log CFU/mL to 8.3 log CFU/mL) and lactic acid content (from 0 to 4.2 g/L), and a reduction of pH value (from 5.5 to around 3.8). In addition, the antioxidant and antibacterial capacities of fermented apple juice in vitro were significantly improved through the phenolic and organic acid metabolisms. After storage at 4°C for 30 days, the total amino acid content of fermented apple juice was significantly increased, although the viable cell counts and total phenolic content were decreased (p < 0.05). Furthermore, the stored fermented apple juices still possessed antibacterial and in vitro antioxidant activities. Overall, all the selected LAB strains could be suitable for apple juice fermentation and can effectively improve their biological activities.
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    Influence of protein corona on the interaction of glycogen-siRNA constructs with ex vivo human blood immune cells.
    Wojnilowicz, M ; Laznickova, P ; Ju, Y ; Ang, C-S ; Tidu, F ; Bendickova, K ; Forte, G ; Plebanski, M ; Caruso, F ; Cavalieri, F ; Fric, J (Elsevier BV, 2022-09)
    Glycogen-nucleic acid constructs i.e., glycoplexes are emerging promising platforms for the alteration of gene expression and transcription. Understanding the interaction of glycoplexes with human blood components, such as serum proteins and peripheral blood mononuclear cells (PBMCs), is important to overcome immune cell activation and control biodistribution upon administration of the glycoplexes in vivo. Herein, we investigated the interactions of polyethylene glycol (PEG)ylated and non-PEGylated glycoplexes carrying siRNA molecules with PBMCs isolated from the blood of healthy donors. We found that both types of glycoplexes were non-toxic and were primarily phagocytosed by monocytes without triggering a pro-inflammatory interleukin 6 cytokine production. Furthermore, we investigated the role of the protein corona on controlling the internalization efficiency in immune cells - we found that the adsorption of serum proteins, in particular haptoglobin, alpha-1-antitrypsin and apolipoprotein A-II, onto the non-PEGylated glycoplexes, significantly reduced the uptake of the glycoplexes by PBMCs. Moreover, the non-PEGylated glycoplexes were efficient in the nuclear factor kappa-light-chain-enhancer of activated B cells (NF-κB) knockdown in monocytic THP-1 cell line. This study provides an insight into the rational design of glycogen-based nanocarriers for the safe delivery of siRNA without eliciting unwanted immune cell activation and efficient siRNA activity upon its delivery.
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    Engineering Programmable DNA Particles and Capsules Using Catechol-Functionalized DNA Block Copolymers
    Kim, CJ ; Ercole, F ; Goudeli, E ; Bhangu, SK ; Chen, J ; Faria, M ; Quinn, JF ; Caruso, F (American Chemical Society (ACS), 2022-08-23)
    DNA block copolymer (DBC) assemblies have attracted attention because of their tunable properties (e.g., programmability, high biocompatibility, efficient cellular uptake, and stability against enzymatic degradation); however, controlling the size of DNA block copolymer assemblies and preparing well-defined DNA-functionalized particle systems are challenging. Herein, we report the preparation of DBC-based particles and capsules with different sizes (i.e., from approximately 0.15 to 3.2 μm) and a narrow size distribution (i.e., polydispersity index <0.2) through the assembly of catechol-functionalized DBC, DNA-b-poly(methyl methacrylate-co-2-methacryloylethyl dihydrocaffeate, with metal ions (e.g., FeIII). This assembly process largely exploits the coordination bonding of the metal ions and phenolic (i.e., catechol) groups, forming metal-phenolic networks (MPNs). The DBC-FeIIIMPN capsules formed are stable under acidic, metal-chelating, and surfactant solutions because of the coexistence of metal coordination, hydrogen bonding, and hydrophobic interactions. The molecular recognition properties of the DNA strands enable tailorable interactions with small molecules and nanoparticles and are used to tune the permeability of the assembled capsules (>40% permeability decrease for 2000 kDa fluorescein isothiocyanate dextran compared with untreated capsules). The DBC-FeIIIMPN particles show efficient cellular uptake and endosomal escape capability, allowing the efficient delivery of small-interfering RNA for gene silencing (89% downregulation). The reported approach provides the rational design of a range of DNA-functionalized particles, which can potentially be applied in materials science and biomedical applications.
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    Next-generation enhanced-efficiency fertilizers for sustained food security
    Lam, SK ; Wille, U ; Hu, H-W ; Caruso, F ; Mumford, K ; Liang, X ; Pan, B ; Malcolm, B ; Roessner, U ; Suter, H ; Stevens, G ; Walker, C ; Tang, C ; He, J-Z ; Chen, D (NATURE PORTFOLIO, 2022-07-21)
    Nitrogen losses in agricultural systems can be reduced through enhanced-efficiency fertilizers (EEFs), which control the physicochemical release from fertilizers and biological nitrogen transformations in soils. The adoption of EEFs by farmers requires evidence of consistent performance across soils, crops and climates, paired with information on the economic advantages. Here we show that the benefits of EEFs due to avoided social costs of nitrogen pollution considerably outweigh their costs—and must be incorporated in fertilizer policies. We outline new approaches to the design of EEFs using enzyme inhibitors with modifiable chemical structures and engineered, biodegradable coatings that respond to plant rhizosphere signalling molecules.
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    Anti-PEG Antibodies Boosted in Humans by SARS-CoV-2 Lipid Nanoparticle mRNA Vaccine
    Ju, Y ; Lee, WS ; Pilkington, EH ; Kelly, HG ; Li, S ; Selva, KJ ; Wragg, KM ; Subbarao, K ; Nguyen, THO ; Rowntree, LC ; Allen, LF ; Bond, K ; Williamson, DA ; Truong, NP ; Plebanski, M ; Kedzierska, K ; Mahanty, S ; Chung, AW ; Caruso, F ; Wheatley, AK ; Juno, JA ; Kent, SJ (AMER CHEMICAL SOC, 2022-06-27)
    Humans commonly have low level antibodies to poly(ethylene) glycol (PEG) due to environmental exposure. Lipid nanoparticle (LNP) mRNA vaccines for SARS-CoV-2 contain small amounts of PEG, but it is not known whether PEG antibodies are enhanced by vaccination and what their impact is on particle-immune cell interactions in human blood. We studied plasma from 130 adults receiving either the BNT162b2 (Pfizer-BioNTech) or mRNA-1273 (Moderna) mRNA vaccines or no SARS-CoV-2 vaccine for PEG-specific antibodies. Anti-PEG IgG was commonly detected prior to vaccination and was significantly boosted a mean of 13.1-fold (range 1.0-70.9) following mRNA-1273 vaccination and a mean of 1.78-fold (range 0.68-16.6) following BNT162b2 vaccination. Anti-PEG IgM increased 68.5-fold (range 0.9-377.1) and 2.64-fold (0.76-12.84) following mRNA-1273 and BNT162b2 vaccination, respectively. The rise in PEG-specific antibodies following mRNA-1273 vaccination was associated with a significant increase in the association of clinically relevant PEGylated LNPs with blood phagocytes ex vivo. PEG antibodies did not impact the SARS-CoV-2 specific neutralizing antibody response to vaccination. However, the elevated levels of vaccine-induced anti-PEG antibodies correlated with increased systemic reactogenicity following two doses of vaccination. We conclude that PEG-specific antibodies can be boosted by LNP mRNA vaccination and that the rise in PEG-specific antibodies is associated with systemic reactogenicity and an increase of PEG particle-leukocyte association in human blood. The longer-term clinical impact of the increase in PEG-specific antibodies induced by lipid nanoparticle mRNA vaccines should be monitored. It may be useful to identify suitable alternatives to PEG for developing next-generation LNP vaccines to overcome PEG immunogenicity in the future.
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    Role of Molecular Interactions in Supramolecular Polypeptide-Polyphenol Networks for Engineering Functional Materials
    Han, Y ; Lafleur, RPM ; Zhou, J ; Xu, W ; Lin, Z ; Richardson, JJ ; Caruso, F (AMER CHEMICAL SOC, 2022-07-01)
    Supramolecular assembly affords the development of a wide range of polypeptide-based biomaterials for drug delivery and nanomedicine. However, there remains a need to develop a platform for the rapid synthesis and study of diverse polypeptide-based materials without the need for employing complex chemistries. Herein, we develop a versatile strategy for creating polypeptide-based materials using polyphenols that display multiple synergistic cross-linking interactions with different polypeptide side groups. We evaluated the diverse interactions operating within these polypeptide-polyphenol networks via binding affinity, thermodynamics, and molecular docking studies and found that positively charged polypeptides (Ka of ∼2 × 104 M-1) and polyproline (Ka of ∼2 × 106 M-1) exhibited stronger interactions with polyphenols than other amino acids (Ka of ∼2 × 103 M-1). Free-standing particles (capsules) were obtained from different homopolypeptides using a template-mediated strategy. The properties of the capsules varied with the homopolypeptide used, for example, positively charged polypeptides produced thicker shell walls (120 nm) with reduced permeability and involved multiple interactions (i.e., electrostatic and hydrogen), whereas uncharged polypeptides generated thinner (10 nm) and more permeable shell walls due to the dominant hydrophobic interactions. Polyarginine imparted cell penetration and endosomal escape properties to the polyarginine-tannic acid capsules, enabling enhanced delivery of the drug doxorubicin (2.5 times higher intracellular fluorescence after 24 h) and a corresponding higher cell death in vitro when compared with polyproline-tannic acid capsules. The ability to readily complex polyphenols with different types of polypeptides highlights that a wide range of functional materials can be generated for various applications.
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    Exploiting Supramolecular Dynamics in Metal–Phenolic Networks to Generate Metal–Oxide and Metal–Carbon Networks
    Pan, S ; Goudeli, E ; Chen, J ; Lin, Z ; Zhong, Q ; Zhang, W ; Yu, H ; Guo, R ; Richardson, JJ ; Caruso, F (Wiley, 2021-06-21)
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    Protein precoating modulates biomolecular coronas and nanocapsule-immune cell interactions in human blood
    Li, S ; Ju, Y ; Zhou, J ; Faria, M ; Ang, C-S ; Mitchell, AJ ; Zhong, Q-Z ; Zheng, T ; Kent, SJ ; Caruso, F (ROYAL SOC CHEMISTRY, 2022-06-09)
    The biomolecular corona that forms on particles upon contact with blood plays a key role in the fate and utility of nanomedicines. Recent studies have shown that precoating nanoparticles with serum proteins can improve the biocompatibility and stealth properties of nanoparticles. However, it is not fully clear how precoating influences biomolecular corona formation and downstream biological responses. Herein, we systematically examine three precoating strategies by coating bovine serum albumin (single protein), fetal bovine serum (FBS, mixed proteins without immunoglobulins), or bovine serum (mixed proteins) on three nanoparticle systems, namely supramolecular template nanoparticles, metal-phenolic network (MPN)-coated template (core-shell) nanoparticles, and MPN nanocapsules (obtained after template removal). The effect of protein precoating on biomolecular corona compositions and particle-immune cell interactions in human blood was characterized. In the absence of a pre-coating, the MPN nanocapsules displayed lower leukocyte association, which correlated to the lower amount (by 2-3 fold) of adsorbed proteins and substantially fewer immunoglobulins (more than 100 times) in the biomolecular corona relative to the template and core-shell nanoparticles. Among the three coating strategies, FBS precoating demonstrated the most significant reduction in leukocyte association (up to 97% of all three nanoparticles). A correlation analysis highlights that immunoglobulins and apolipoproteins may regulate leukocyte recognition. This study demonstrates the impact of different precoating strategies on nanoparticle-immune cell association and the role of immunoglobulins in bio-nano interactions.
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    Cover Image, Volume 8, Issue 2
    Kattel, G ; Reeves, J ; Western, A ; Zhang, W ; Jing, W ; McGowan, S ; Cuo, L ; Scales, P ; Dowling, K ; He, Q ; Wang, L ; Capon, S ; Pan, Z ; Cui, J ; Zhang, L ; Xiao, L ; Liu, C ; Zhang, K ; Gao, C ; Tian, Z ; Liu, Y (Wiley, 2021-03)