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• Dec@PLGA@aMM could enhance the tumor suppression through restoration of TSGs. • The Dec@PLGA@aMM group showed the higher CD4+ T cells and CD8+ T cells, indicating the enhanced immunotherapy. • The decitabine could enhance aPD-L1-mediated immunotherapy of HCC via epigenetic alteration. • This novel targeted PLGA NPs are aimed to treat HCC by decreasing DNA methylation and blocking PD-L1. DNA methyltransferase (DNMT) inhibitor represents the first clinical breakthrough via targeting aberrant cancer epigenomes. Demethylation drugs such as decitabine can restore tumor suppressor gene (TSG) expression and function to achieve anti-tumor effect. Despite DNMT inhibitors have shown significant efficacy for treating leukemia, their application in solid tumor such as HCC is limited due to short in vivo half-lives. In this study, the DNMT1 inhibitor decitabine was first loaded into the Polylactic-co-glycolic acid (PLGA) spherical nanoparticles (Dec@PLGA). The vesicle of PD-L1 antibody and macrophage membrane (aMM) was further coated onto the surface of Dec@PLGA to finally synthesize Dec@PLGA@aMM. Dec@PLGA@aMM was in uniformed spherical structure with hydrodynamic particle size of 95.7 ± 9.1 nm and surface zeta potential of −15.1 ± 3.3 mV. Dec@PLGA@aMM significantly increased the expression of both p14 and p16 in a concentration-dependent manner. Dec@PLGA@aMM could enhance the tumor suppression through restoration of TSGs, which were epigenetically silenced by DNA hypermethylation. The Dec@PLGA@aMM group showed significantly (P < 0.05) less tumor volume than PBS group, PLGA@MM group, aPD-L1 group, PLGA@aMM group, decitabine group, Dec + aPD-L1 group, and Dec@PLGA@MM group. The decitabine could enhance aPD-L1-mediated immunotherapy of HCC via epigenetic alteration. This novel targeted PLGA NPs are aimed to treat HCC by decreasing DNA methylation and blocking PD-L1, thus providing new ideas for effective treatments via epigenetic alteration for HCC patients clinically. [ABSTRACT FROM AUTHOR]

[Display omitted] • Ultra-firm homogeneous COF with ∼7 nm of tetragonal structure layers was prepared on the silicon nanoparticles surface. • The PMDA-NiPc@Si electrode shows only ∼44% of expansion rate, which is only 27.3% of that of the Si electrode. • The reversible capacity of 654 mAh g-1 with retention rate of 80.4% can still be maintained after 2000 cycles at 5 A g-1. • PMDA-NiPc@Si exhibits excellent Li+ conductivity after pre-lithiation, significantly improving initial coulombic efficiency. • The PMDA-NiPc@Si/NCM811 full battery can still preserve 175.8 mAh g-1 and 85.8% capacity retention after 100 cycles at 0.2 C. The enormous volume change of silicon (Si) leads to pulverization of Si electrodes and continuous growth of solid-electrolyte-interphase (SEI) layers on the Si surface, for which we report a new Si anode material (PMDA-NiPc@Si) with a homogeneous and tetragonal covalent organic frameworks (COFs) coating on the surface of nano-Si particles. COFs with tetragonal structures have higher stability than other structures, which helps to increase the long cycle life of the electrodes. The strong constraining buffering effect of the coating layer can fully inhibit and buffer the volume change of Si nanoparticles during charging-discharging, reduce the consumption of electrolytes and form a homogeneous, stable and robust, LiF- and LiN-rich SEI film, and ultimately improve the rate performance and long-cycle performance. The pre-lithiation of PMDA-NiPc@Si shows a superior lithium ion conductivity that can enhance the lithium ion transport kinetics of silicon electrodes and significantly improve the initial coulomb efficiency (ICE). PMDA-NiPc@Si exhibits excellent specific capacity and cycling performance, with a capacity retention rate of 93.8 % after 100 cycles, which is 2.7 times higher than that of nano-Si. It also offers a high reversible capacity of 654 mAh/g and a capacity retention rate of 80.4 % after 2000 cycles at 5 A/g. The assembled full battery with PMDA-NiPc@Si anode and NCM811 cathode displayed a specific capacity of 175.8 mAh/g with a retention rate of 85.8 % after 100 cycles at 0.2C. The PMDA-NiPc@Si electrode shows only about 44 % of the expansion rate (21.6 to 31.1 μm), which is only 27.3 % of that of the Si electrode. PMDA-NiPc@Si anodes show significantly enhanced electrochemical performance, which will provide novel ideas for the development of high-performance Li-ion batteries. [ABSTRACT FROM AUTHOR]

• Poly-dioxolane solid polymer electrolyte (PSiDOL) with network structure was in situ prepared. • The PSiDOL exhibit high thermal stability, superior ionic conductance, and outstanding electrolyte/electrode interfacial stability. • The PSiDOL-based cells show high safety and excellent cycling performance. Rechargeable batteries paired with polyether-based solid-state electrolytes is a promising system to solve the safety problem of lithium metal (Li-metal) batteries, and stable solid electrolyte interface (SEI) layer between electrolyte and anode is highly required for their long-term stability. Here we propose a novel thermal-stable polymerized 1,3-dioxolane electrolyte (PSiDOL), which is in situ formed via a multifunctional 1,3-bis(3-glycidoxypropyl) tetramethyl disiloxane crosslinker. This network structural PSiDOL not only achieves good flame retardancy, significantly increased operating temperature and improved oxidative stability, but also induces the formation of stable and robust SEI layer with rich Li x SiO y /LiF on the surface of Li-metal anode. Moreover, the three-dimensional polymer skeleton with abundant polar groups is beneficial to improve the ionic conductance and cationic transference number. As a result, the PSiDOL electrolyte enable ultralong-term (over 4000 h) reversible and stable lithium plating/stripping in Li symmetrical cell for lithium anode. In addition, the assembled full cells based on such electrolyte display desirable cycling stability at high temperature and high voltage with suppressed electrolyte degradation. This work affords a facile and practical approach to develop advanced electrolytes for solid-state Li-metal batteries with high safety and durability. [ABSTRACT FROM AUTHOR]