Atherosclerosis is driven by metabolic dysregulation, particularly aberrant cholesterol accumulation and impaired nitric oxide (NO) signaling. However, most therapeutic strategies address these abnormalities separately, while biomaterials capable of translating pathological metabolic dysregulation into localized biochemical regulation remain limited. Herein, we report MMCoac@ChOx/HRP, a macrophage membrane-camouflaged coacervate microreactor formed via liquid–liquid phase separation (LLPS). The microreactor features a macromolecularly crowded core self-assembled from poly(diallyldimethylammonium chloride) and sulfobutylether-β-cyclodextrin, which enables cholesterol recognition and enrichment of cholesterol oxidase (ChOx) and horseradish peroxidase (HRP). These co-encapsulated enzymes achieve high enrichment efficiencies of 87.5 and 92.1%, respectively, to drive cholesterol oxidation and subsequent NO generation. In simulated body fluid, MMCoac@ChOx/HRP depleted cholesterol levels from 5.0 to 2.9 ± 0.4 mM and generated 12.1 ± 0.8 μM NO within 12 h. In vitro, it significantly attenuated macrophage foam cell formation and promoted endothelial repair. Furthermore, following systemic administration in ApoE–/– mice, MMCoac@ChOx/HRP preferentially accumulated in atherosclerotic aortic plaques, enhanced in situ NO generation, and reduced aortic plaque burden from 27.4 ± 4.5 to 8.2 ± 3.0%. Overall, this study demonstrates a localized metabolic intervention strategy driven by an LLPS-based microreactor. This versatile biomaterial platform effectively modulates the plaque microenvironment, holding great potential for therapeutic interventions against metabolic syndrome.
Insufficient Li+ transport kinetics and poor interfacial stability hinder the practical application of polyethylene oxide (PEO)-based solid-state electrolytes (SSEs) in all-solid-state lithium metal batteries. In this work, we propose iodine-induced charge transfer of a covalent organic framework (COF) as an effective strategy to achieve fast ion transport and a stable SSE/Li interface. First, the electron-deficient COF skeleton in the I2/COF charge-transfer complex anchors TFSI- anions through enhanced electrostatic interactions, thereby promoting the dissociation of lithium salt to release free Li+. Second, the electron deficiency of COF strengthens its dipole–dipole interactions with PEO, leading to suppressed PEO crystallization and enhanced COF/PEO compatibility. Third, the electron-deficient COF tailors the Li+ coordination environment via weakening the affinity of PEO and COF toward Li+. Consequently, the I2/COF charge-transfer complex accelerates Li+ transport kinetics in PEO-based composite SSEs. Furthermore, the confinement effect of COF toward I2 via charge transfer effectively inhibits the aggressive lithium anode corrosion by I2, resulting in the controlled growth of a stable, robust, and conductive solid electrolyte interface (SEI) rich in LiF and LiI. Thus, the I2/COF charge-transfer complex enables excellent rate capability and cycling stability of the resulting COF/PEO-based composite SSE, maintaining a capacity retention of 88.58% after 1000 cycles at 2 C. This work offers a promising strategy for designing COF/PEO-based composite SSEs for next-generation all-solid-state lithium metal batteries.
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