Latest ArticlesPhotodynamic therapy (PDT) has garnered significant attention as a promising approach to cancer therapy, harnessing the combined benefits of localized light treatment and the accompanying host immune response. In this study, we engineered an immuno-enhanced PDT nanoplatform, denoted as HM@p-MOF (hybrid membrane@porphyrin-metal organic framework). The core porphyrin-MOF was cloaked with a hybrid membrane derived from B16F10 cancer cells and NK cells, resulting in enhanced stability. In both in vitro and in vivo experiments, our finding demonstrated that the hybrid membrane conferred dual targeting capabilities to the nanoplatform, leveraging the unique properties of the B16F10 membrane and NK membrane to augment immunogenic cell death (ICD) induced by photodynamic effects. Additionally, in conjunction with the immunomodulatory functions of the NK cell membrane, we observed an expansion of in situ immune infiltration leading to a systemic immune response. The HM@p-MOF nanoplatform exhibited the capacity to not only inhibit the growth of mouse melanoma but also suppress metastasis. This innovative HM@p-MOF nanoplatform present a viable strategy to enhance phototherapeutic efficacy for both localized and metastatic tumors. It provides a direction for the fabrication of biomimetic nanomedicines possessing immuno-modulatory function.
Carbon dots (CDs), as a solid-state phosphor, have great potential for application in a new solid-state lighting device—laser diode (LD). For high efficiency LD devices, both high photoluminescence quantum yield (PLQY) and high photothermal stability of CDs are essential. Herein, yellow CDs@ZIF-8 composites with high structural stability were prepared by encapsulating CDs in zeolitic imidazolate framework-8 (ZIF-8) through electrostatic adsorption between CDs and ZIF-8, in which CDs with amino groups on the surface were used as luminescent feeders and ZIF-8 was used as a protective layer matrix. The as-prepared CDs@ZIF-8 not only possess a high PLQY of up to 81.17%, but also maintain a high fluorescence intensity of 100% and 80% under long-term illumination (60 min) and high temperature (478 K), respectively. The hydrogen bonding between CDs and ZIF-8 in the encapsulated structure can enhance the degree of electron cloud delocalization, which can improve the PLQY of CDs@ZIF-8. Meanwhile, CDs@ZIF-8 has high photothermal stability due to the binding effect of ZIF-8 on CDs and high thermal stability of ZIF-8. The white LD device, fabricated from CDs@ZIF-8 as a phosphor in combination with 450 nm blue LD, has a color coordinate of (0.37, 0.33), a color temperature of 3762 K, and a high color rendering index of 86. This study provides a new strategy for the construction of solid-state phosphors with high PLQY and high photothermal performance.
As a hydrolase, chymotrypsin (CHT) is involved in many physiological activities, and its abnormal activity is closely related to diabetes, pancreatic fibrosis, chronic pancreatitis and pancreatic cancer. In this work, an innovative long-wavelength emission fluorescent probe TCF-CHT was designed and synthesized for the high specificity detection of CHT, which utilized TCF-OH and a mimetic peptide substrate 4-bromobutyryl as chromogenic group and recognition group, respectively. TCF-CHT exhibited excellent selectivity and eye-catching sensitivity (8.91 ng/mL) towards CHT, "off-on" long-wavelength emission at 670 nm and large Stokes shift (140 nm). Furthermore, the successful fulfillment and perfect performance in imaging endogenous CHT in complex organisms (P815 cells, HepG2 cells, zebrafish and tumor-bearing mice) verified its potential as a powerful tool for the recognition of CHT in complicated biological environments.
The first example of sono-photocatalytic bond formation was reported. With both visible light and ultrasound wave as the energy, various 3-aminoquinoxalin-2(1H)-ones were efficiently obtained with good functional group tolerance in the absence of any additive or external photocatalyst. Compared with the conventional photocatalysis, sono-photocatalysis not only dramatically improved the reaction rates and yields, but also reduced energy consumption.
Solid polymer electrolytes (SPEs) are considered to be one of the most promising systems applied in all-solid-state lithium metal batteries (ASSLMBs) on account of their chemical and electrochemical robustness, mechanical stability, cost-effective and scalable manufacturing techniques. Lately, significant endeavors have been directed towards mitigating the formation of the Li dendrite in SPE-based ASSLMBs, while research on the inactive lithium in the forms of the solid-electrolyte interface has been rarely reported. Herein, a bi-functional GaI3 additive is developed for in-situ generating Li3Ga alloy for suppressing Li dendrite growth, as well as I3− in recovering dead lithium. Relying on the density functional theory (DFT) results, the Li atom prefers to deposit on the Li3Ga surface and then guide uniform Li deposition, while the I3 species features a relatively lower lowest unoccupied molecular orbital (LUMO) energy level (-2.12 eV), meaning a higher electron affinity, which is beneficial for reviving inactive lithium to counterbalance the loss of lithium. As a result, in comparison to cells employing pure PEGDME-based electrolytes, the Li-Li symmetric cells utilizing GaI3-containing solid-state electrolyte exhibited a cycling life nearly 30 times longer at a current density/capacity of 0.2 mA/cm2, 0.2 mAh/cm2. The full batteries of LFP//1%GaI3-SPE//40 µm Li delivered a noteworthy capacity retention of 82% after 1300 cycles at a rate of 1 C.
Molecular-based ferroelastics with dielectric switching properties are highly desirable for their applications on microelectronic dielectric switches, sensors, data storage, and so on. However, the current reports mostly focus on organic-inorganic hybrids containing toxic heavy metal atoms, and the relatively low phase transition temperature limits their application. In this paper, low-toxic organic salt ferroelastic enantiomers (R/S)-4-fluoro-1-azabicyclo[3.2.1]octonium chloride [(R/S)-F-321] were designed and synthesized under the introducing chirality strategy. They undergo a 432F422-type ferroelastic phase transition with a high Curie temperature (Tc) of 470 K, simultaneously exhibiting excellent dielectric switching characteristics. In addition to the ordered-disordered movement of cations, the significant displacement of anions is also responsible for such high Tc and large dielectric switching ratios, which is very rare in molecular-based switching materials. This work enriches the development of molecular ferroelastic switching materials and gives inspiration for the exploration of environmentally friendly high Tc organic salt ferroelastics with prominent switching performances.
Using hydrogen-bonded organic frameworks (HOFs) as photosensitizers to perform photocatalytic oxidation reactions under green and mild conditions is still a challenge for the application of HOFs materials. This study presents a novel approach that exploits HOFs to enhance the efficiency of photocatalytic oxidation for achieving visible light catalytic oxidation of styrene and its derivatives in the aqueous environment. By using 1,3,6,8-tetrakis(p-benzoic acid)pyrene (H4TBAPy) as the monomer, a pyrene-based hydrogen-bonded organic framework (PFC-1) with a microporous structure was successfully prepared. Compared with monomer H4TBAPy, due to the exciton effect and the interlayer confinement of HOFs, the singlet oxygen (1O2) production efficiency is significantly improved, which has great potential in photocatalytic oxidation reactions. Subsequently, the practicality of PFC-1 as a photocatalyst was studied, and the photocatalytic oxidation of styrene and its derivatives in aqueous solution was achieved under visible light with high catalytic efficiency, indicating that PFC-1 has significant potential to promote photocatalytic oxidation reactions under mild conditions. The utilization of HOFs as photosensitizers in this straightforward approach enables the attainment of green photocatalytic oxidation, hence expanding the potential applications of HOFs materials within the realm of photocatalysis.
Post-synthetic modifications (PSM) have drawn great attention as a vigoroso tool to tune or enhance the performance of metal-organic frameworks (MOFs). However, the current PSM method usually have to sacrifice the porosity of MOFs to enrich their functionality, such as pore space partition (PSP) and post-synthetic elimination and insertion (PSE&I), causing a trade-off in this aspect. To address this issue, we herein propose a new PSM strategy of using the size-matching ligands as the bolts to lock MOFs’ pores, which could be anchored onto open metal sites (OMSs) after guest loading through a stepwise manipulation. As a result, the loaded cargoes undergo a controlled releasing process with respect to different bolt ligands. Our proposed strategy provides a promising way to balance the functionality and porosity of MOFs.
An oxidative annulation of 2-arylidene-1,3-indanediones with Meldrum's acid has been developed for the divergent syntheses of spirolactones with a spirocenter located at the γ-position with respect to the carbonyl group. This heteroannulation protocol tolerates various functional groups and delivers moderate-to-good product yields. Interestingly, the reaction outcomes are exclusively controlled by the reaction oxidant/medium. This annulation strategy can also be executed in the flow system with decent product yields. Control experiments revealed that the reaction proceeds via a radical tandem annulation pathway.
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