Reduced Graphene Oxides Modified Bi2Te3 Nanosheets for Rapid Photo-Thermoelectric Catalytic Therapy of Bacteria-Infected Wounds

Temperature variation-induced thermoelectric catalytic efficiency of thermoelectric material is simultaneously restricted by its electrical conductivity, Seebeck coefficient, and thermal conductivity. Herein, Bi₂Te₃ nanosheets are in situ grown on reduced graphene oxides (rGO) to generate an efficient photo-thermoelectric catalyst (rGO-Bi₂Te₃). This system exhibits phonon scattering effect and extra carrier transport channels induced by the formed heterointerface between rGO and Bi₂Te₃, which improves the power factor value and reduces thermal conductivity, thus enhancing the thermoelectric performance of 2.13 times than single Bi₂Te₃. The photo-thermoelectric catalysis of rGO-Bi₂Te₃ significantly improves the reactive oxygen species yields, resulting from the effective electron–hole separation caused by the unique thermoelectric field and heterointerfaces of rGO-Bi₂Te₃. Correspondingly, the electrospinning membranes containing rGO-Bi₂Te₃ nanosheets exhibit high antibacterial efficiency in vivo (99.35 ± 0.29%), accelerated tissue repair ability, and excellent biosafety. This study provides an insight into heterointerface design in photo-thermoelectric catalysis.     

Exploring a Stable and Dense 3D Lead Chloride Hybrid with Emission of Self-Trapped Excitons toward X-Ray Scintillation

The exceptional photophysical properties of 3D organic–inorganic lead halide hybrids (OILHs) endow their significant potential for usage in optoelectronics, which has sparked intense research on novel 3D OILHs and associated applications. However, constructing new 3D OILHs based on large organic cations suffers from tough challenges due to the limitation of the Goldschmidt tolerance factor rule, let alone further explorations of their practical applications. Herein, a brand-new 3D lead chloride hybrid, (1MPZ)Pb₄Cl₁₀·H₂O ( 1 , 1MPZ = 1-methylpiperazine) is reported, featuring a dense 3D lead chloride framework made of the corner-, edge-, and face-shared lead chloride polyhedra. 1 presents a broadband white light emission with a large Stokes shift and a nanosecond photoluminescence lifetime, which originates from radiative recombination of self-trapped excitons (STEs) induced by the highly distorted structure. Such a reabsorption-free and fast-decayed STEs emission coupling with the dense 3D architecture further enables 1 with effective X-ray scintillation with good sensitivity. Impressively, 1 also shows superior environmental and radiation stability. This study provides a new 3D OILH with appealing luminescence, not only expanding the 3D OILH family but also inspiring the exploitation of their optoelectronic applications.     

Unlocking the Capacity of Vanadium Oxide by Atomically Thin Graphene-Analogous V2O5·nH2O in Aqueous Zinc-Ion Batteries

Aqueous Zn-ion batteries (AZIBs) are promising due to their high theoretical energy density and intrinsic safety, and the natural abundance of Zn. Since low voltage is an intrinsic shortage of AZIBs, achieving super-high capacity of cathode materials is a vital way to realize high practical energy density, which however remains a huge challenge. Herein, the capacity increase of classical vanadium oxide cathode is predicted via designing atomic thickness of 2D structure to introduce abundant Zn²⁺ storage sites based on density functional theory (DFT) calculation; then graphene-analogous V₂O₅·nH₂O (GAVOH) with only few atomic layers is fabricated, realizing a record capacity of 714 mAh g⁻¹. Pseudocapacitive effect is unveiled to mainly contribute to the super-high capacity due to the highly exposed GAVOH external surface. In situ Raman and synchrotron X-ray techniques unambiguously uncover the Zn²⁺ storage mechanism. Carbon nanotubes (CNTs) are further introduced to design GAVOH-CNTs gel ink for large-scale cathode fabrication. The hybrid cathode demonstrates ultra-stable cycling and excellent rate capability and delivers a high energy density of 476 Wh kg⁻¹ at 76 W kg⁻¹; 228 Wh kg⁻¹ is still retained at high mass loading of 10.2 mg cm⁻². This work provides inspiration for breaking the capacity limit of cathode in AZIBs.     

Light-Responsive Programmable Shape-Memory Soft Actuator Based on Liquid Crystalline Polymer/Polyurethane Network

Liquid crystalline polymers (LCPs), especially liquid crystalline elastomers (LCEs) can generate ultrahigh shape change amplitude but has lower mechanical strength. Although some attempts have been tried to improve the mechanical performance of LCE, there are still limitations including complicated fabrication and high actuation temperature. Here, a versatile method is reported to fabricate light-driven actuator by covalently cross-linking polyurethane (PU) into LCP networks (PULCN). This new scheme is distinct from the previous interpenetrating network strategy, the hydrogen bonds and covalent bonds are used in this study to improve the miscibility of non-liquid-crystalline PU and LCP materials and enhance the stability of the composite system. This material not only possesses the shape memory properties of PU but shows shape-changing behavior of LCPs. With a shrinkage ratio of 20% at the phase transition temperature, the prepared materials reached a maximum mechanical strength of 20 MPa, higher than conventional LCP. Meanwhile, the resulting film shows diverse and programmable initial shapes by constructing crosslinking density gradient across the thickness of the film. By integration of PULCN with near-infrared light-responsive polydopamine, local and sequential light control is achieved. This study may provide a new route for the fabrication of programmable and mechanically robust light-driven soft actuator.     

High-Performing Quasi-2D Perovskite Photodetectors with Efficient Charge Transport Network Built from Vertically Orientated and Evenly Distributed 3D-Like Phases

Quasi-two-dimensional (Q-2D) perovskites are emerging as one of the most promising materials for photodetectors. However, a significant challenge to Q-2D perovskites for photodetection is their insufficient charge transport ability, which is mainly attributed to their hybrid low-dimensional n-phase structure. This study demonstrates that evenly-distributed 3D-like phases with vertical orientation throughout the film can greatly facilitate charge transport and suppress charge recombination, outperforming the prevalent phase structure with a vertical dimension gradient. Based on such a phase structure, a Q-2D Ruddlesden−Popper perovskite self-powered photodetector achieving a combination of exceptional figures-of-merit is realized, including a responsivity of 0.45 AW⁻¹, a peak specific detectivity of 2.3 × 10¹³ Jones, a 156 dB linear dynamic range, and a rise/fall time of 2.89 µs/1.93 µs. The desired phase structure is obtained by utilizing a double-hole transport layer (HTL), combining hydrophobic PTAA and hydrophilic PEDOT: PSS. Besides, the dependence of the hybrid low-dimensional phase structure is also identified on the surface energy of the buried HTL substrate. This study gives insight into the correlation between Q-2D perovskites’ phase structure and performance, providing a valuable design guide for Q-2D perovskite-based photodetectors.     

Phase-Separated Polyzwitterionic Hydrogels with Tunable Sponge-Like Structures for Stable Solar Steam Generation

Solar steam generation (SSG) through hydrogel-based evaporators has shown great promise for freshwater production. However, developing hydrogel-based evaporators with stable SSG performance in high-salinity brines remains challenging. Herein, phase-separated polyzwitterionic hydrogel-based evaporators are presented with sponge-like structures comprising interconnected pores for stable SSG performance, which are fabricated by photopolymerization of sulfobetaine methacrylate (SBMA) in water-dimethyl sulfoxide (DMSO) mixed solvents. It is shown that driven by competitive adsorption, the structures of the resulting poly(sulfobetaine methacrylate) (PSBMA) hydrogels can be readily tuned by the volume ratio of DMSO to achieve phase separation. The optimized phase-separated PSBMA hydrogels, combining the unique anti-polyelectrolyte effects of polyzwitterionic hydrogels, demonstrate a rapid water transport capability in brines. After introducing photothermal polypyrrole particles on the surface of the phase-separated PSBMA hydrogel evaporators, a stable water evaporation rate of ≈2.024 kg m⁻² h⁻¹ and high solar-to-vapor efficiency of ≈97.5% in a 3.5 wt.% brine are obtained under simulated solar light irradiation (1.0 kW m⁻²). Surprisingly, the evaporation rates remain stable even under high-intensity solar irradiation (2.0 kW m⁻²). It is anticipated that the polyzwitterionic hydrogel evaporators with sponge-like porous structures will contribute to developing SSG technology for high-salinity seawater applications.     

Macrophage Membrane-Coated Nanoparticles Sensitize Glioblastoma to Radiation by Suppressing Proneural–Mesenchymal Transformation in Glioma Stem Cells

Radiotherapy is identified as a crucial treatment for patients with glioblastoma, but recurrence is inevitable. The efficacy of radiotherapy is severely hampered partially due to the tumor evolution. Growing evidence suggests that proneural glioma stem cells can acquire mesenchymal features coupled with increased radioresistance. Thus, a better understanding of mechanisms underlying tumor subclonal evolution may develop new strategies. Herein, data highlighting a positive correlation between the accumulation of macrophage in the glioblastoma microenvironment after irradiation and mesenchymal transdifferentiation in glioblastoma are presented. Mechanistically, elevated production of inflammatory cytokines released by macrophages promotes mesenchymal transition in an NF-κB-dependent manner. Hence, rationally designed macrophage membrane-coated porous mesoporous silica nanoparticles (MMNs) in which therapeutic anti-NF-κB peptides are loaded for enhancing radiotherapy of glioblastoma are constructed. The combination of MMNs and fractionated irradiation results in the blockage of tumor evolution and therapy resistance in glioblastoma-bearing mice. Intriguingly, the macrophage invasion across the blood-brain barrier is inhibited competitively by MMNs, suggesting that these nanoparticles can fundamentally halt the evolution of radioresistant clones. Taken together, the biomimetic MMNs represent a promising strategy that prevents mesenchymal transition and improves therapeutic response to irradiation as well as overall survival in patients with glioblastoma.     

Catalytically Induced Robust Inorganic-Rich Cathode Electrolyte Interphase for 4.5 V Li||NCM622 Batteries

Tailoring inorganic components of cathode electrolyte interphase (CEI) and solid electrolyte interphase (SEI) is critical to improving the cycling performance of lithium metal batteries. However, it is challenging due to complicated electrolyte reactions on cathode/anode surfaces. Herein, the species and inorganic component content of the CEI/SEI is enriched with an objectively gradient distribution through employing pentafluorophenyl 4-nitrobenzenesulfonate (PFBNBS) as electrolyte additive guided by engineering bond order with functional groups. In addition, a catalytic effect of LiNi_0.6Mn_0.2Co_0.2O₂ (NCM622) cathode is proposed on the decomposition of PFBNBS. PFBNBS with lower highest occupied molecular orbital can be preferentially oxidized on the NCM622 surface with the help of the catalytic effect to induce an inorganic-rich CEI for superior electrochemical performance at high voltage. Moreover, PFBNBS can be reduced on the Li surface due to its lower lowest unoccupied molecular orbital , increasing inorganic moieties in SEI for inhibiting Li dendrite generation. Thus, 4.5 V Li||NCM622 batteries with such electrolyte can retain 70.4% of initial capacity after 500 cycles at 0.2 C, which is attributed to the protective effect of the excellent CEI on NCM622 and the inhibitory effect of its derived CEI/SEI on continuous electrolyte decomposition.     

Self-Mineralizing Dnazyme Hydrogel as a Multifaceted Bone Microenvironment Amendment for Promoting Osteogenesis in Osteoporosis

The accumulation of reactive oxygen species (ROS) and minimal osteogenic raw material in the osteoporotic bone microenvironment greatly inhibits the activity of osteoblasts. Herein, it is originally proposed to construct a biomatrix multifaceted bone microenvironment amendment -Mineralized zippered G4-Hemin DNAzyme hydrogel (MDH)-to improve osteoporotic osteogenic capacity and promote high-quality bone defect repair. The programmed design of the rolling circle amplified DNA hydrogel synthesis system allows the introduction of massive amounts of zippered G4-Hemin DNAzyme in MDH. The zippered G4-Hemin DNAzyme highly mimics the tight catalytic configuration of horseradish peroxidase and exerts excellent enzyme-like activity with considerable ROS molecule scavenging ability. In addition, the DNA amplification by-product pyrophosphate is ingeniously employed as a sufficient phosphorus source, thus constituting an autonomous mineralization system for waste reuse through the introduction of pyrophosphate hydrolase and calcium ions, which deposits in MDH as an osteogenic raw material and addresses the challenge of DNA hydrogel bio-application stability. The remarkable in vitro and in vivo outcomes demonstrate that MDH can effectively improve the oxidative stress status of osteoblasts, restore the balance of mitochondrial membrane potential, and reduce apoptosis, ultimately demonstrating superior osteogenic capacity.     

An Apoptotic Body-based Vehicle with Navigation for Photothermal-Immunotherapy by Precise Delivery and Tumor Microenvironment Regulation

Tumor precision therapy and preventing tumor recurrence and metastasis are the main challenges to tumor eradication. Herein, an apoptotic body-based vehicle with imaging navigation is developed for precise tumor delivery and photothermal-immunotherapy by IR820-conjugated apoptotic body loaded with R848 nanoparticles. The apoptotic body serves as ammunition stores as well as vehicle drive engines, while IR820 acts as a fluorescence imaging navigation and photothermal controlling system. The apoptotic body vehicle can deliver the ammunition to tumor and achieve deep penetration by macrophage-hitchhiking. Fluorescence imaging navigation opens a control window for photothermal treatment, followed by photothermal triggering of in situ vaccine formation. Further, CD47 antibody loaded hydrogel strengthens innate and adaptive immunity, simultaneously the polarization of macrophages regulates the immunosuppressive microenvironment to further promote the combined antitumor immunotherapy. With breast tumor (4T1)-bearing mice model, the apoptotic body vehicle performs excellent therapeutic efficacy for primary tumor, distant tumor, tumor metastasis, and recurrence prevention.