Latest ArticlesOrganic scintillators, materials with the ability to exhibit luminescence when exposed to X-rays, have aroused increasing interest in recent years. However, the enhancement of radioluminescence and improving X-ray absorption of organic scintillators lie in the inherent dilemma, due to the waste of triplet excitons and weak X-ray absorption during scintillation. Here, we employ halogenated thermally activated delayed fluorescence materials to improve the triplet exciton utilization and X-ray absorption simultaneously, generating efficient scintillation with a low detection limit, which is one order of magnitude lower than the dosage for X-ray medical diagnostics. Through experimental study and theoretical calculation, we reveal the positive role of X-ray absorption, quantum yields of prompt fluorescence, and intersystem crossing in promoting the radioluminescence intensity. This finding offers an opportunity to design diverse types of organic scintillators and expands the applications of thermally activated delayed fluorescence.
Borrowing from natural mechanisms for material design can lead to functional mimicry and improvement. Inspired by graphite formation, a thermopressure coupling strategy under micropressure (<400 Pa) is applied to prepare carbon anodes. A thermopressure response is discovered based on the cellulose precursor. Here, homologous graphene quantum dot/hard carbon (GQD/HC) heterostructures are synthesized. Under 181.4 Pa and 1,200 °C, the product shows a capacity of 310 mAh g−1, while the capacity of the direct carbonization product is only 120 mAh g−1. Prominently, the GQD/HC heterostructure displays marked mechanical strength and flexibility. The experimental and theoretical results illustrate the ion and electron transfer, coordination environment, and electronic states in the GQD/HC heterostructure and elaborate on the origin of the enhanced performance. The thermopressure coupling under micropressure mimics graphite formation, but the heterostructure has better properties than traditional carbon materials. Additionally, micropressure injects new vitality into material research.
HfO2-based ferroelectrics have evoked considerable interest owing to the complementary metal–oxide semiconductor compatibility and robust ferroelectricity down to a few unit cells. However, the unique wake-up effect of HfO2-based ferroelectric films severely restricts the improvement of their performance. In particular, the domain structure is an important characteristic of ferroelectric materials, which still has not been well understood in HfO2-based ferroelectrics. In this work, a Hf0.5Zr0.5O2 ferroelectric thin film is grown on a typical Si substrate buffered with TiN electrode. The 90° domains of the Pca21 ferroelectric phase with head-to-tail and tail-to-tail structures can be observed by Cs-corrected scanning transmission electron microscope under their pristine condition. After waking up, the 180° domain is displayed in the ferroelectric phase. The remarkable differences in domain walls for 90° and 180° domains are characterized by qualitatively mapping the polarization distributions at the atomic scale. The domain wall changes from the of the Hf0.5Zr0.5O2 film to the [001] of the Hf0.5Zr0.5O2 film. This result provides fundamental information for understanding the domain structure of HfO2-based ferroelectrics.
Intelligent stimuli-responsive fluorescence materials are extremely pivotal for fabricating luminescent turn-on switching in solid-state photonic integration technology, but it remains a challenging objective for typical 3-dimensional (3D) perovskite nanocrystals. Herein, by fine-tuning the accumulation modes of metal halide components to dynamically control the carrier characteristics, a novel triple-mode photoluminescence (PL) switching was realized in 0D metal halide through stepwise single-crystal to single-crystal (SC-SC) transformation. Specifically, a family of 0D hybrid antimony halides was designed to exhibit three distinct types of PL performance including nonluminescent [Ph3EtP]2Sb2Cl8 (1), yellow-emissive [Ph3EtP]2SbCl5·EtOH (2), and red-emissive [Ph3EtP]2SbCl5 (3). Upon stimulus of ethanol, 1 was successfully converted to 2 through SC-SC transformation with enhanced PL quantum yield from ~0% to 91.50% acting as “turn-on” luminescent switching. Meanwhile, reversible SC-SC and luminescence transformation between 2 and 3 can be also achieved in the ethanol impregnation–heating process as luminescence vapochromism switching. As a consequence, a new triple-model turn-on and color-adjustable luminescent switching of off–onI–onII was realized in 0D hybrid halides. Simultaneously, wide advanced applications were also achieved in anti-counterfeiting, information security, and optical logic gates. This novel photon engineering strategy is expected to deepen the understanding of dynamic PL switching mechanism and guide development of new smart luminescence materials in cutting-edge optical switchable device.
The enzyme-mimicking catalytic activity of single-atom nanozymes has been widely used in tumor treatment. However, research on alleviating metabolic diseases, such as hyperglycemia, has not been reported. Herein, we found that the single-atom Ce-N4-C-(OH)2 (SACe-N4-C-(OH)2) nanozyme promoted glucose absorption in lysosomes, resulting in increased reactive oxygen species production in HepG2 cells. Furthermore, the SACe-N4-C-(OH)2 nanozyme initiated a cascade reaction involving superoxide dismutase-, oxidase-, catalase-, and peroxidase-like activity to overcome the limitations associated with the substrate and produce •OH, thus improving glucose intolerance and insulin resistance by increasing the phosphorylation of protein kinase B and glycogen synthase kinase 3β, and the expression of glycogen synthase, promoting glycogen synthesis to improve glucose intolerance and insulin resistance in high-fat diet-induced hyperglycemic mice. Altogether, these results demonstrated that the novel nanozyme SACe-N4-C-(OH)2 alleviated the effects of hyperglycemia without evident toxicity, demonstrating its excellent clinical application potential.
While conventional nanosystems can target infected lung tissue, they cannot achieve precise cellular targeting and enhanced therapy by modulating inflammation and microbiota for effective therapy. Here, we designed a nucleus-targeted nanosystem with adenosine triphosphate (ATP) and reactive oxygen species stimuli–response to treat pneumonia coinfected with bacteria and virus that is enhanced through inflammation and microbiota regulation. The nucleus-targeted biomimetic nanosystem was prepared through the combined bacteria–macrophage membrane and loaded hypericin and ATP-responsive dibenzyl oxalate (MMHP) subsequently. The MMHP despoiled the Mg2+ of intracellular cytoplasm in bacteria to achieve an effective bactericidal performance. Meanwhile, MMHP can target the cell nucleus and inhibit the H1N1 virus duplication by inhibiting the activity of nucleoprotein. MMHP possessed an immunomodulatory ability to reduce the inflammatory response and activate CD8+ T cells for assisted infection elimination. During the mice model, the MMHP effectively treated pneumonia coinfected with Staphylococcus aureus and H1N1 virus. Meanwhile, MMHP mediated the composition of gut microbiota to enhance the pneumonia therapy. Therefore, the dual stimuli-responsive MMHP possessed promising clinical translational potential to therapy infectious pneumonia.
It is well known that alcohol consumption leads to substantially increased free radical levels and health risks, which lacks effective treatment besides alcohol abstinence. Here, we compared different static magnetic field (SMF) settings and found that a downward quasi-uniform SMF of ~0.1 to 0.2 T could effectively alleviate alcohol-induced liver damage and lipid accumulation and improve hepatic function. SMFs of two different directions can reduce the inflammation, reactive oxygen species levels, and oxidative stress in the liver, while the downward SMF had more obvious effects. Moreover, we found that the upward direction SMF of ~0.1 to 0.2 T could inhibit DNA synthesis and regeneration in hepatocytes, which caused detrimental effects on the lifespan of "heavy drinking" mice. In contrast, the downward SMF prolongs survival of "heavy drinking" mice. On one hand, our study shows that ~0.1 to 0.2 T moderate quasi-uniform SMFs with a downward direction have great promises to be developed into a physical method to reduce alcohol-induced liver damage; on the other hand, although the internationally recognized upper limit for SMF public exposure is 0.4 T, people should also pay extra attention to SMF strength, direction, and inhomogeneity that could generate harmful effects on specific severe pathological conditions.
Traditional metal oxide semiconductor (MOS) gas sensors have limited applications in wearable devices owing to their inflexibility and high-power consumption by substantial heat loss. To overcome these limitations, we prepared doped Si/SiO2 flexible fibers by a thermal drawing method as substrates to fabricate MOS gas sensors. A methane (CH4) gas sensor was demonstrated by subsequently in situ synthesizing Co-doped ZnO nanorods on the fiber surface. The doped Si core acted as the heating source through Joule heating, which conducted heat to the sensing material with reduced heat loss; the SiO2 cladding was an insulating substrate. The gas sensor was integrated into a miner cloth as a wearable device, and the concentration change of CH4 was monitored in real time through different colored light-emitting diodes. Our study demonstrated the feasibility of using doped Si/SiO2 fibers as the substrates to fabricate wearable MOS gas sensors, where the sensors have substantial advantages over tradition sensors in flexibility, heat utilization, etc.
The stimulator of interferon genes (STING) protein is an important and promising innate immune target for tumor therapy. However, the instability of the agonists of STING and their tendency to cause systemic immune activation is a hurdle. The STING activator, cyclic di-adenosine monophosphate (CDA), produced by the modified Escherichia coli Nissle 1917, shows high antitumor activity and effectively reduces the systemic effects of the “off-target” caused by the activation of the STING pathway. In this study, we used synthetic biological approaches to optimize the translation levels of the diadenylate cyclase that catalyzes CDA synthesis in vitro. We developed 2 engineered strains, CIBT4523 and CIBT4712, for producing high levels of CDA while keeping their concentrations within a range that did not compromise the growth. Although CIBT4712 exhibited stronger induction of the STING pathway corresponding to in vitro CDA levels, it had lower antitumor activity than CIBT4523 in an allograft tumor model, which might be related to the stability of the surviving bacteria in the tumor tissue. CIBT4523 exhibited complete tumor regression, prolonged survival of mice, and rejection of rechallenged tumors, thus, offering new possibilities for more effective tumor therapy. We showed that the appropriate production of CDA in engineered bacterial strains is essential for balancing antitumor efficacy and self-toxicity.
Two-dimensional (2D) materials have gained lots of attention due to the potential applications. In this work, we propose that based on first-principles calculations, the (2 × 2) patterned PtTe2 monolayer with kagome lattice formed by the well-ordered Te vacancy (PtTe1.75) hosts large and tunable spin Hall conductivity (SHC) and excellent hydrogen evolution reaction (HER) activity. The unconventional nature relies on the A1 @ 1b band representation of the highest valence band without spin–orbit coupling (SOC). The large SHC comes from the Rashba SOC in the noncentrosymmetric structure induced by the Te vacancy. Even though it has a metallic SOC band structure, the ℤ2 invariant is well defined because of the existence of the direct bandgap and is computed to be nontrivial. The calculated SHC is as large as 1.25 × 103 (Ω cm)−1 at the Fermi level (EF). By tuning the chemical potential from EF − 0.3 to EF + 0.3 eV, it varies rapidly and monotonically from −1.2 × 103 to 3.1 . In addition, we also find that the Te vacancy in the patterned monolayer can induce excellent HER activity. Our results not only offer a new idea to search 2D materials with large SHC, i.e., by introducing inversion–symmetry breaking vacancies in large SOC systems, but also provide a feasible system with tunable SHC (by applying gate voltage) and excellent HER activity.