pH-Responsive Micellar Nanoparticles for the Delivery of a Self-Amplifying ROS-Activatable Prodrug.

The objective of this study is to enhance the therapeutic efficacy of the anticancer drug, camptothecin (CPT) via a nanoparticle (NP) formulation using a novel amphiphilic biopolymer. We have designed a dimeric prodrug of CPT with the ability to self-amplify and respond to reactive oxygen species (ROS). For this, we incorporated the intracellular ROS generator cinnamaldehyde into a ROS-cleavable thioacetal (TA) linker to obtain the dimeric prodrug of CPT (DCPT(TA)). For its efficient NP delivery, a pH-responsive block copolymer of acetalated dextran and poly(2-ethyl-2-oxazoline) (AcDex-b-PEOz) was synthesized. The amphiphilic feature of the block copolymer enables its self-assembly into micellar NPs and results in high prodrug loading capacity and a rapid release of the prodrug under acidic conditions. Upon cellular uptake by HeLa cells, DCPT(TA)-loaded micellar NPs induce intracellular ROS generation, resulting in accelerated prodrug activation and enhanced cytotoxicity. These results indicate that this system holds significant potential as an effective prodrug delivery strategy in anticancer treatment.

Light-Switchable Biocatalytic Covalent-Organic Framework Nanomotors for Aqueous Contaminants Removal.

Self-propelled nanomotors represent a promising class of adaptable and versatile technologies with broad applications in the realms of biomedicine and environmental remediation. Herein, we report a biocatalytic nanomotor based on a covalent-organic framework (COF) that demonstrates intelligent and switchable motion triggered by a blue-to-red light switch. Consequently, when exposed to blue light, the nanomotor significantly enhances the removal of contaminants in aqueous solutions due to its elevated mobility. Conversely, it effectively deactivates its motion and contaminant removal upon exposure to red light. This study explores the heterogeneous assembly strategy of the COF-based nanomotor and its light-controlled propulsion performance and provides a novel strategy for the regulation of movement, offering valuable insights for the design and practical applications of nanomotors.

Metal-Organic Frameworks as a Versatile Materials Platform for Unlocking New Potentials in Biocatalysis.

Biocatalysts immobilization with nanomaterials has promoted the development of biocatalysis significantly and made it an indispensable part of catalysis industries nowadays. Metal-organic frameworks (MOFs), constructed from organic linkers and metal ions or clusters, have raised significant interests for biocatalysts immobilization in recent years. The diversity of building units, molecular-scale tunability, and modular synthetic routes of MOFs greatly expand its ability as the host to integrate with biocatalysts. In this review, the general synthetic strategies of MOFs with biocatalysts are first summarized. Then, the recent progress of MOFs as a versatile host for a series of biocatalysts, including natural enzymes, nanozymes, and organism-based biocatalysts, followed by the introduction of MOFs themselves as biocatalysts, is discussed. Furthermore, the stimuli-responsive properties of MOFs themselves or the additional functionalization of protein, polymer, and peptide within/on MOF that enable the biocatalysts with the controllable and tunable behavior are also summarized, which could unlock new potentials in biocatalysis. Finally, a perspective of the upcoming challenges, potential impacts, and future directions of biocatalytic MOFs is provided.