Latest ArticlesCancer persists as a major global health challenge, marked by high recurrence rates in aggressive malignancies such as melanoma. While immunotherapy has emerged as a promising approach, its clinical benefits are often limited by tumor immune escape mechanisms and an immunosuppressive tumor microenvironment (TME). These hurdles have driven the exploration of integrated approaches, with photothermal-immunotherapy gaining significant traction. In this study, we developed a multifunctional nanoadjuvant (MICN@PI) engineered with an acid-responsive calcium carbonate core, a hypoxia-alleviating MnO2 component, a polydopamine shell for photothermal ablation, and co-loaded immunomodulators (imiquimod and indoximod). The MnO2 in the nanoadjuvant catalytically converted the overexpressed H2O2 in the TME into O2. Concurrently, the combined action of imiquimod and indoximod orchestrated a potent adaptive immune response. Upon near-infrared laser irradiation, MICN@PI achieved significant tumor ablation, inhibited recurrence, and prolonged survival in a murine melanoma model, offering a safe and effective synergistic photothermal-immunotherapy strategy for cancer treatment.
Transition metal sulfides (TMSs) are primitive composition of biocatalysts that are active for molecular hydrogen production. The development of non-precious TMSs with appropriate spatial ordering has great potentials to contribute high-level hydrogen generation. Herein, super-hybrid transition metal sulfide nanoarrays of NiS nanoparticle/WS2 nanosheet/Ni3S4 nanoparticle (Super-NiS/WS2/Ni3S4) with high spatial ordering and abundant plane- and edge-type WS2NiS and WS2Ni3S4 heterointerfaces were elaborately constructed though manipulating the sequential dissociation of phosphotungstic acid (PW12) as W precursor and nickel foam as Ni precursor in one pot. When evaluated for the electrocatalytic hydrogen evolution reaction (HER), the Super-NiS/WS2/Ni3S4 only required overpotentials of 57, 95, and 151 mV to drive HER in alkaline, acid, and neutral media, respectively, and presented favorable reaction kinetics and test stability. The theoretical and experimental results verify the adsorption and dissociation of water molecules are preferential on WS2-plane-related heterointerfaces. The Gibbs free energy (ΔGH*) analysis indicated the WS2-plane-NiS interface is thermodynamically optimal for HER. Moreover, the collaborations of the abundant plane- and edge-type active interfaces, the open nanosheet-based vertical array, and the phosphorus doping in Super-NiS/WS2/Ni3S4 strengthen mass transport and electron transfer in electrocatalysis. The polyoxometalates-based synthetic strategy will inspire the new vision for the rational design and construction of advanced functional materials.
The trithiocyanurate, (H2C3N3S3)-, exhibits a strong optical anisotropy but has a small HOMO-LUMO gap, limiting its application to the higher energy wavelength ranges. Herein, by applying an amino substitution strategy, we report that 2-amino-4,6-dimercapto-S-triazine, (H3C3N4S2)-, generates a series new compound: A2(H2C3N4S2)2•H2O (NH4, Ⅰ; K−Cs, Ⅱ−Ⅳ). Compound Ⅰ crystallizes in P21/n, while compounds Ⅱ–Ⅳ crystallize in P1. Their experimental optical band gaps (Eg) range from 3.52 eV to 3.65 eV, corresponding to a blue shift of 30~60 nm compared to those of the trithiocyanuric containing systems. Moreover, the birefringence of all compounds ranges from 0.440 to 0.510, indicating strong anisotropy. Notably, compound Ⅰ (Eg = 3.65 eV,
Garnet-type ceramic Li7La3Zr2O12 (LLZO) stands out as a potential solid-state electrolyte, offering a promising alternative to conventional flammable liquid electrolytes. However, its large interfacial resistance with electrodes remains a significant challenge. In this research, we have successfully in-situ fabricated polymeric interface layers on both cathode and anode sides with LLZO. By tuning the gel-polymer interphase via fluoroethylene carbonate (FEC), known as FGPE, we have established a rapid Li+ transport channel by enhancing the solid-solid interfacial contact. This FGPE layer exhibits exceptional ionic conductivity of 1.38 mS/cm and a high Li-ion transference number of 0.64. Furthermore, FGPE effectively mitigates concentration polarization under high currents, thereby enabling a higher capacity output. In comparison to gel-polymer interphases with dimethyl carbonate (DMC) as the solvent (referred to as GPE), the Li|FGPE|Li symmetrical cell has demonstrated superior stability in plating/strapping performance over 800 h at a current density of 0.1 mA/cm2. Moreover, the Li|FGPE|LLZO|FGPE|LiFePO4 cell has exhibited commendable rate capability and has maintained a high capacity retention of 98.94% at 0.5 C after 200 cycles. This study underscores an innovative approach in advancing in field of solid-state batteries, anticipated to be broadly applicable to other solid-state batteries by facilitating an abundance of robust solid-solid interfacial contacts.
Trapping and manipulating microscopic particles (micron or nano) in a liquid environment are of great significance for research and applications in nanoscience, engineering, and biomedicine. Although optical tweezers, magnetic tweezers, acoustic tweezers, etc. have been successfully developed, it is still challenging to separate, select, and manipulate micron and submicron particles with comparable morphologies and sizes in trace amounts of liquids with high viscosity and extremely tiny concentrations. Herein, an electric tweezer with measurable force was introduced in an environmental transmission electron microscope (ETEM) for trapping a single submicron particle in high viscosity liquids. The critical voltages for trapping SiO2 and TiO2 spheres were determined to be 75 V and 25 V, respectively, due to their dielectric characteristics. As a result, although TiO2 particles exhibited a similar size and morphology, they were able to be successfully separated from a mixed suspension of SiO2 and TiO2. Moreover, by applying a reasonable bias voltage to the electric tweezer and customizing the size and shape of the tweezer tip, individual 500, 750, and 1000 nm TiO2 spheres could be easily trapped from the corresponding TiO2 suspension. The displacements of atomic force microscope (AFM) cantilevers indicated that the forces to trapped a single particle gradually increased with the diameter of the particles. Additionally, the electric tweezer could precisely manipulate a single particle, and stack a specific structure on the top of the electric tweezer. When the electric tweezer was combined with an optical microscope, it could successfully transfer a 5 µm SiO2 sphere to a HeLa cell. Precisely trapping and manipulating micron and submicron particles is the foundation for fabricating microdevices to achieve specific functions, and it also show great potential for use in biological applications.
Electrocatalytic carbon dioxide reduction reaction (eCO2RR) holds great promise in producing value-added chemicals, and achieving carbon neutrality. However, the efficiency of eCO2RR is often hindered by the sluggish oxygen evolution reaction (OER) at the anode. Thereby, various strategies have been developed to boost anode reaction, aiming to realize economic viability and reduce energy consumption in an eCO2RR electrolyzer. To give a comprehensive overview of anode engineering for optimizing eCO2RR, this review summarizes and discusses the cutting-edge anodic design strategies from recent research progress. They mainly include the direct substitution of OER to the value-added oxidation reaction of other small molecules, the introduction of photo/bio-assistance anodes, and the construction of metal-CO2 batteries. Furthermore, the emerging challenges and a forward-looking perspective on anode development by coupling renewable energy, sewage treatment and eCO2RR are also proposed.
In order to cope with harsh situations without an external power supply, developing high-performance aqueous zinc batteries (AZBs) with chemically self-charging as a self-powered system is of great practical significance. Herein, we present the synthesis of a new porous organic polymer with hexaazatriphenylene hexacarboxylic acid trianhydride (HHAT) and 2,6-diaminoanthraquinone (DAAQ) units (HTAQ). Due to its π-conjugated aromatic structure with abundant redox-active centers and limited solubility in electrolytes, the constructed flexible and coin-type AZBs based on HTAQ cathodes display a superior volume energy density (8.7 mWh/cm3) and a higher energy density (104 Wh/kg), respectively, and excellent cycle life, where both Zn2+ and H+ ions participate in the cathode reaction. Impressively, the electric energy exhausted flexible Zn//HTAQ AZB can be chemically self-recharged by exposing the discharged HTAQ cathode to air, ascribing to the spontaneous redox reaction between O2 and the discharged HTAQ cathode. The exhausted flexible Zn//HTAQ AZB after air-charging for 30 h, can present a high discharge capacity of 294 mAh/g at 0.5 A/g, a higher self-charging cycle stability (15 cycles), a high-rate capability, and work well at hybrid modes (chemical or/and galvanostatic charging). Our work opens a new route to construct high-performance self-powered systems based on AZBs.
The regulation of guest molecules on the self-assembly system of tetracarboxylic acid derivative (H4BDETP) at the liquid/solid interface was studied by scanning tunneling microscopy (STM) and density functional theory (DFT) calculations. Coronene (COR) guest molecules induced H4BDETP to transform from linear assembly structure to diversified nanoporous structures in which COR could be captured. And the regulation of pyridine guest molecules (DPE, BPYB, TYPY) on the mono-component assembly structure of H4BDETP was achieved by forming O–H···N hydrogen bonds with H4BDETP. The introduction of both COR and pyridine derivatives could destroy the hydrogen-bonded dimers of H4BDETP, and new O–H···O hydrogen bonds were formed between H4BDETP molecules. In addition, H4BDETP/pyridine co-assembly structures depended on the central bridging units and the number of pyridine groups in pyridine derivatives. Furthermore, H4BDETP/TYPY structure underwent structural transformation induced by COR and multi-component assembly structures with thermodynamic stability were constructed.
The surficial inherent properties of TiO2 like exposed facet and crystalline state are vital for their surface reactions. However, efficiently controlling the specific crystal structure and the exposed crystal surface still faces big challenge. Here, the controlled solid phase transition of amorphous TiO2 to crystalline phase with exposed crystal facet (001) is achieved by photo-assisted atomic layer deposition (ALD) Pt process. Significantly, the obtained Pt/TiO2 film via photo-assisted treatment exhibits high sensing performance to NO and HF, and shows a lower optimized working temperature. The enhanced sensing performance is attributed to the metal-support strong interaction under oxidative atmosphere (O-SMSI). The facet effects leading to the unique distribution of charges at the interface combined with the catalytic effects result in the high sensing performance. This work provides a novel phase transition engineering strategy for regulating TiO2 from amorphous to crystalline phase, and the controllable synthesis of high Pt monatomic loading on TiO2 via ALD, which are critical for the accurate synthesis of efficient sensing and catalytic nanomaterials.
The emerging anode-free lithium metal battery (AFLMB) is very promising for the next-generation electrochemical energy storage technology due to its remarkable high-energy density. However, the current development of AFLMB is seriously hampered by the low Coulombic efficiency and limited lifespan caused mainly by the uncontrolled dendritic lithium growth and significant volume change during Li plating/stripping on the traditional current collector. Here, we report the design of a “breathable” three-dimensional (3D) lithium host with MnO2 nanoflake array for long-lifespan AFLMB. Specifically, a dense MnO2 nanoflake array stretchably grown on carbon cloth by an easy solution dipping method is constructed as a 3D current collector for AFLMBs. Both experimental and theoretical studies underlined that the Li2O/Mn nanoflake arrays produced spontaneously upon the initial lithiation can effectively guide uniform lithium nucleation and growth. Moreover, this unique 3D hierarchical structure expands/shrinks along with the lithium plating/stripping, accommodating the large volume expansion/shrinkage over the subsequent charge/discharge processes. As such, a dendrite-free lithium structure was achieved even at a high capacity of 10 mAh/cm2. More importantly, the as-constructed AFLMB with this current collector exhibits impressive cycling stability with 64% capacity retained after 200 cycles. This study offers new insights into constructing highly efficient 3D protective layers for metal anodes toward the practical feasibility of anode-free batteries.
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