Biomimetic Metal–Organic Framework Composite-Mediated Cascade Catalysis for Synergistic Bacteria Killing

Abstract

Encapsulating nanoparticles/biomolecules into metal–organic freamworks (MOFs) has proven to be highly effective in creating new functions during their applications. However, it is highly desirable yet remains challenging to achieve the synergy of specific functions between the MOF host and guest species. Herein, inspired by the natural multienzyme system, a novel MOF composite biomimetic structure based on the coencapsulation of glucose oxidase (GOx) and l-arginine (l-Arg) into Cu-MOFs (CuBDC) with Fenton-like catalytic activity is designed for achieving the synergistic antibacterial effect. Once activated by GOx-catalyzed glucose oxidation, a large amount of oxygen radicals, toxic ONOO–, and NO are rapidly produced over this well-designed l-Arg/GOx@CuBDC through a double-cascade reaction. Thanks to the synergy of highly reactive species, outstanding antibacterial effects (bacterial inactivation ≥97%) are observed at very low doses (38 μg mL–1 for Escherichia coli and 3.8 μg mL–1 for Staphylococcus aureus). In addition, the in vivo experiment in mice demonstrated that the as-prepared l-Arg/GOx@CuBDC has good biocompatibility, indicating its good potential in practical applications. Such a biomimetic multienzyme system proposes a new design idea for highly efficient antibiosis as well as even therapy for tumors.

Enzyme Mimics for Engineered Biomimetic Cascade Nanoreactors: Mechanism, Applications, and Prospects

“…In vivo wound healing 2DMOF/GOx GOx and POD [25] Antibacterial application MIL@GOx-MIL NRs GOx and POD [143] Synergistic bacteria killing l-Arg/GOx@CuBDC GOx and POD [144] Against Inflammation Fe/N-HCNs SOD, POD, CAT, and OXD [72] Bacterial killing MoS 2 /rGO VHS POD, CAT, and OXD [145] Bacterial killing Dex-IONP-GOx GOx and POD [146] Antioxidation ROS scavenging V 2 O 5 @pDA SOD, CAT, and GPx [147] Cytoprotection Mn 3 O 4 nanozyme SOD, CAT, and GPx [148] Preventing oxidative damage Mn 3 O 4 SOD, CAT, and GPx [30] Brain injury triM nanozyme HRP and CAT [136a]…”

“…[72] Moreover, biomimetic cascade nanoreactors using MOF-based nanozymes have been employed as antibacterial agents. [25,143,144] Using a two-step procedure, Li et al used MOF and GOx to construct a cascade MOF/ enzyme hybrid nanoreactor (MIL@GOx-MIL NRs) as a novel antibacterial agent. MIL shells loaded with GOx can catalyze the formation of gluconic acid, leading to a decrease in pH to around 4 resulting in MIL@GOx-MIL with enhanced cascade catalytic activity.…”

“…[ 72 ] Moreover, biomimetic cascade nanoreactors using MOF‐based nanozymes have been employed as antibacterial agents. [ 25,143,144 ] Using a two‐step procedure, Li et al. used MOF and GOx to construct a cascade MOF/enzyme hybrid nanoreactor (MIL@GOx‐MIL NRs) as a novel antibacterial agent.…”

“…Moreover, the double‐cascade reaction system could significantly enhance enzymatic cascade catalysis and could improve the applicability and durability of the antibacterial nanomaterials. [ 144 ] Using a one‐step microwave‐assisted hydrothermal strategy, the group of Chen have developed a dispersed and uniform defect‐rich molybdenum disulfide/rGO vertical heterostructure (VHS) (MoS 2 /rGO VHS) material, featuring rough surface and abundant Mo and S vacancies. The MoS 2 /rGO VHS exhibited excellent defect and irradiation dual‐enhanced enzyme‐like catalytic activity (including OXD‐, POD‐, and CAT‐like activity), and exhibited excellent potential for killing bacteria.…”

Controllable Nitric Oxide‐Delivering Platforms for Biomedical Applications

“…A large number of oxygen radicals, toxic ONOO − , and NO are rapidly produced through a double cascade reaction, showing the antibacterial effects of the synergy of highly reactive species. [ 144] Arg NIR stimulates ICG to produce ROS, causing catalysis of l-Arg to release NO gas.…”