Chemical and Biomedical Engineering - Research Publications

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    Engineering of Nebulized Metal-Phenolic Capsules for Controlled Pulmonary Deposition
    Ju, Y ; Cortez-Jugo, C ; Chen, J ; Wang, T-Y ; Mitchell, AJ ; Tsantikos, E ; Bertleff-Zieschang, N ; Lin, Y-W ; Song, J ; Cheng, Y ; Mettu, S ; Rahim, MA ; Pan, S ; Yun, G ; Hibbs, ML ; Yeo, LY ; Hagemeyer, CE ; Caruso, F (John Wiley & Sons, 2020-03-18)
    Particle-based pulmonary delivery has great potential for delivering inhalable therapeutics for local or systemic applications. The design of particles with enhanced aerodynamic properties can improve lung distribution and deposition, and hence the efficacy of encapsulated inhaled drugs. This study describes the nanoengineering and nebulization of metal–phenolic capsules as pulmonary carriers of small molecule drugs and macromolecular drugs in lung cell lines, a human lung model, and mice. Tuning the aerodynamic diameter by increasing the capsule shell thickness (from ≈100 to 200 nm in increments of ≈50 nm) through repeated film deposition on a sacrificial template allows precise control of capsule deposition in a human lung model, corresponding to a shift from the alveolar region to the bronchi as aerodynamic diameter increases. The capsules are biocompatible and biodegradable, as assessed following intratracheal administration in mice, showing >85% of the capsules in the lung after 20 h, but <4% remaining after 30 days without causing lung inflammation or toxicity. Single-cell analysis from lung digests using mass cytometry shows association primarily with alveolar macrophages, with >90% of capsules remaining nonassociated with cells. The amenability to nebulization, capacity for loading, tunable aerodynamic properties, high biocompatibility, and biodegradability make these capsules attractive for controlled pulmonary delivery.
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    Modular Assembly of Host-Guest Metal-Phenolic Networks Using Macrocyclic Building Blocks
    Pan, S ; Guo, R ; Bertleff-Zieschang, N ; Li, S ; Besford, QA ; Zhong, Q-Z ; Yun, G ; Zhang, Y ; Cavalieri, F ; Ju, Y ; Goudeli, E ; Richardson, JJ ; Caruso, F (Wiley, 2020-01-02)
    The manipulation of interfacial properties has broad implications for the development of high‐performance coatings. Metal–phenolic networks (MPNs) are an emerging class of responsive, adherent materials. Herein, host–guest chemistry is integrated with MPNs to modulate their surface chemistry and interfacial properties. Macrocyclic cyclodextrins (host) are conjugated to catechol or galloyl groups and subsequently used as components for the assembly of functional MPNs. The assembled cyclodextrin‐based MPNs are highly permeable (even to high molecular weight polymers: 250–500 kDa), yet they specifically and noncovalently interact with various functional guests (including small molecules, polymers, and carbon nanomaterials), allowing for modular and reversible control over interfacial properties. Specifically, by using either hydrophobic or hydrophilic guest molecules, the wettability of the MPNs can be readily tuned between superrepellency (>150°) and superwetting (ca. 0°).