Chemical and Biomolecular Engineering - Research Publications

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    Advanced Lipidomics in the Modern Meat Industry: Quality Traceability, Processing Requirement, and Health Concerns
    Li, C ; Ozturk-Kerimoglu, B ; He, L ; Zhang, M ; Pan, J ; Liu, Y ; Zhang, Y ; Huang, S ; Wu, Y ; Jin, G (FRONTIERS MEDIA SA, 2022-05-27)
    Over the latest decade, lipidomics has been extensively developed to give robust strength to the qualitative and quantitative information of lipid molecules derived from physiological animal tissues and edible muscle foods. The main lipidomics analytical platforms include mass spectrometry (MS) and nuclear magnetic resonance (NMR), where MS-based approaches [e.g., "shotgun lipidomics," ultra-performance liquid chromatography-tandem mass spectrometry (UPLC-MS/MS), matrix-assisted laser desorption and ionization time-of-flight mass spectrometry (MALDI-TOF-MS)] have been widely used due to their good sensitivity, high availability, and accuracy in identification/quantification of basal lipid profiles in complex biological point of view. However, each method has limitations for lipid-species [e.g., fatty acids, triglycerides (TGs), and phospholipids (PLs)] analysis, and necessitating the extension of effective chemometric-resolved modeling and novel bioinformatic strategies toward molecular insights into alterations in the metabolic pathway. This review summarized the latest research advances regarding the application of advanced lipidomics in muscle origin and meat processing. We concisely highlighted and presented how the biosynthesis and decomposition of muscle-derived lipid molecules can be tailored by intrinsic characteristics during meat production (i.e., muscle type, breed, feeding, and freshness). Meanwhile, the consequences of some crucial hurdle techniques from both thermal/non-thermal perspectives were also discussed, as well as the role of salting/fermentation behaviors in postmortem lipid biotransformation. Finally, we proposed the inter-relationship between potential/putative lipid biomarkers in representative physiological muscles and processed meats, their metabolism accessibility, general nutritional uptake, and potency on human health.
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    Material Optimization Engineering toward xLiFePO4·yLi3V2(PO4)3 Composites in Application-Oriented Li-Ion Batteries.
    Pi, Y ; Luo, G ; Wang, P ; Xu, W ; Yu, J ; Zhang, X ; Fu, Z ; Yang, X ; Wang, L ; Ding, Y ; Wang, F (MDPI AG, 2022-05-20)
    The development of LiFePO4 (LFP) in high-power energy storage devices is hampered by its slow Li-ion diffusion kinetics. Constructing the composite electrode materials with vanadium substitution is a scientific endeavor to boost LFP's power capacity. Herein, a series of xLiFePO4·yLi3V2(PO4)3 (xLFP·yLVP) composites were fabricated using a simple spray-drying approach. We propose that 5LFP·LVP is the optimal choice for Li-ion battery promotion, owning to its excellent Li-ion storage capacity (material energy density of 413.6 W·h·kg-1), strong machining capability (compacted density of 1.82 g·cm-3) and lower raw material cost consumption. Furthermore, the 5LFP·LVP||LTO Li-ion pouch cell also presents prominent energy storage capability. After 300 cycles of a constant current test at 400 mA, 75% of the initial capacity (379.1 mA·h) is achieved, with around 100% of Coulombic efficiency. A capacity retention of 60.3% is displayed for the 300th cycle when discharging at 1200 mA, with the capacity fading by 0.15% per cycle. This prototype provides a valid and scientific attempt to accelerate the development of xLFP·yLVP composites in application-oriented Li-ion batteries.
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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)