Blue-Shifted and Broadened Fluorescence Enhancement by Visible and Mode-Selective Infrared Double Excitations.

Mode-selective vibrational excitations to modify the electronic states of fluorescein dianion in methanol solutions are carried out with a femtosecond visible pulse synchronized with a tunable high-power, narrow-band picosecond infrared (IR) pulse. In this work, simultaneous intensity enhancement, peak blueshift, and line width broadening of fluorescence are observed in the visible/IR double resonance experiments. Comprehensive investigations on the modulation mechanism with scanning the vibrational excitation frequencies, tuning the time delay between the two excitation pulses, theoretical calculations, and nonlinear and linear spectroscopic measurements suggest that the fluorescence intensity enhancement is caused by the increase of the Franck-Condon factor induced by the vibrational excitations at the electronic ground state. Various enhancement effects are observed as vibrations initially excited by the IR photons relax to populate the vibrational modes of lower frequencies. The peak blueshift and line width broadening are caused by both increasing the Franck-Condon factors among different subensembles because of IR pre-excitation and the long-lived processes induced by the initial IR excitation. The results demonstrate that the fluorescence from the visible/IR double resonance experiments is not a simple sum frequency effect, and vibrational relaxations can produce profound effects modifying luminescence.

Correction: Yu et al. Inhibiting Liver Autophagy and Promoting Hepatocyte Apoptosis by Schistosoma japonicum Infection. Trop. Med. Infect. Dis. 2024, 9, 42.

In the published publication [...].

Inhibiting Liver Autophagy and Promoting Hepatocyte Apoptosis by Schistosoma Japonicum Infection.

We established a mouse model of Schistosoma japonicum infection in order to study the effects of the infection on hepatocyte autophagy and apoptosis. We also stimulated HepG2 cells with soluble egg antigens (SEA) in vitro. At two, four, and six weeks post-infection, quantitative real-time PCR and Western blot (WB) were used to detect liver expression levels of autophagy and apoptosis-related proteins. HepG2 cells were treated with different concentrations of SEA. The changes in the levels of autophagy-related proteins and HepG2 cell apoptosis were detected. The Lc3b, Beclin1, Atg7, and Atg12 mRNA levels were significantly lower at four and six weeks after infection than those in the uninfected group. At four and six weeks following infection, the levels of Beclin1, LC3BII/I, Atg7, and p62 proteins were considerably lower than those in the uninfected group. The protein levels of pro-apoptotic Bax and cleaved caspase 3 and fibrosis-related proteins α-SMA and collagen 3 in the liver post-infection were significantly higher than those in uninfected mice. HepG2 cells stimulated with SEA showed decreased levels of Beclin1, p62, and Atg7 proteins and significantly increased apoptosis rates. The findings demonstrated that following infection with S. japonicum, mice's liver fibrosis worsened, hepatic autophagy was suppressed, and hepatocyte apoptosis was encouraged.

Staggered Assembly of a Dimeric Au13 Cluster: Impacts on Coupling of Geometric Isomerism.

The specific states of aggregation of metal atoms in sub-nanometer-sized gold clusters are related to the different quantum confinement volumes of electrons, leading to novel optical and electronic properties. These volumes can be tuned by changing the relative positions of the gold atoms to generate isomers. Studying the isomeric gold core and the electron coupling between the basic units is fundamentally important for nanoelectronic devices and luminescence; however, appropriate cases are lacking. In this study, the structure of the first staggered di-superatomic Au25 -S was solved using single-crystal X-ray diffraction. The optical properties of Au25 -S were studied by comparing with eclipsed Au25 -E. From Au25 -E to Au25 -S, changes in the electronic structures occurred, resulting in significantly different optical absorptions originating from the coupling between the two Au13 modules. Au25 -S shows a longer electron decay lifetime of 307.7 ps before populating the lowest triplet emissive state, compared to 1.29 ps for Au25 -E. The experimental and theoretical results show that variations in the geometric isomerism lead to distinct photophysical processes owing to isomerism-dependent electronic coupling. This study offers new insights into the connection between the geometric isomerism of nanosized building blocks and the optical properties of their assemblies, opening new possibilities for constructing function-specific nanomaterials.

CeO2 -Based Frustrated Lewis Pairs via Defective Engineering: Formation Theory, Site Characterization, and Small Molecule Activation.

Activation of small molecules is considered to be a central concern in the theoretical investigation of environment- and energy-related catalytic conversions. Sub-nanostructured frustrated Lewis pairs (FLPs) have been an emerging research hotspot in recent years due to their advantages in small molecule activation. Although the progress of catalytic applications of FLPs is increasingly reported, the fundamental theories related to the structural formation, site regulation, and catalytic mechanism of FLPs have not yet been fully developed. Given this, it is attempted to demonstrate the underlying theory of FLPs formation, corresponding regulation methods, and its activation mechanism on small molecules using CeO2 as the representative metal oxide. Specifically, this paper presents three fundamental principles for constructing FLPs on CeO2 surfaces, and feasible engineering methods for the regulation of FLPs sites are presented. Furthermore, cases where typical small molecules (e.g., hydrogen, carbon dioxide, methane oxygen, etc.) are activated over FLPs are analyzed. Meanwhile, corresponding future challenges for the development of FLPs-centered theory are presented. The insights presented in this paper may contribute to the theories of FLPs, which can potentially provide inspiration for the development of broader environment- and energy-related catalysis involving small molecule activation.

Strontium doped Fe-based porous carbon for highly efficient electrocatalytic ORR and MOR reactions.

The catalytic activity improvement of Fe-based active sites derived from metal organic frameworks toward oxygen reduction reaction (ORR) and methanol oxidation reaction (MOR) remains a major challenge. In this study, the growth of strontium decorated 2-methylimidazole zinc salt (Sr/ZIF-8) is prepared as a carrier to vapor deposited iron formation Sr doped Fe-based nitrogen-doped carbon framework (named as Sr/FeNC). After high-temperature pyrolysis and vapor deposition, strontium carbonate nanocrystals are evenly dispersed on the shrunk dodecahedron carbon frame and multitudinous Fe-based active catalytic sites are embedded in carbon skeleton. The optimal Sr/FeNC-2 catalyst demonstrates the outstanding ORR performance in terms of a half-wave potential of 0.851 V and an onset potential of 0.90 V, while Sr/FeNC-2 exhibits a high current density of 18.2 mA cm-2 and a lower Tafel slope of 21 mV dec-1 in MOR. The exceptional catalytic activity could be ascribed to the synergistic coupling effect of strontium compounds with Fe-based catalytic sites (Fe-Nx, Fe, and iron oxide). In particular, the formation of SrCO3 affects the bonding configuration of the iron species sites, leading to an optimization of the electronic structure within the multihole carbon matrix. The synthetic approach presents a prospective strategy for future endeavors in developing innovative and advanced bifunctional catalysts for ORR and MOR.

Transition metal phosphides: synthesis nanoarchitectonics, catalytic properties, and biomass conversion applications.

Developing inexpensive and efficient catalysts for biomass hydrogenation or hydrodeoxygenation (HDO) is essential for efficient energy conversion. Transition metal phosphides (TMPs), with the merits of abundant active sites, unique physicochemical properties, tunable component structures, and excellent catalytic activities, are recognized as promising biomass hydrogenation or HDO catalytic materials. Nevertheless, the biomass hydrogenation or HDO catalytic applications of TMPs are still limited by various complexities and inherent performance bottlenecks, and thus their future development and utilization remain to be systematically sorted out and further explored. This review summarizes the current popular strategies for the preparation of TMPs. Subsequently, based on the structural and electronic properties of TMPs, the catalytic activity origins of TMPs in biomass hydrogenation or HDO is elucidated. Additionally, the application of TMPs in efficient biomass hydrogenation or HDO catalysis, as well as highly targeted multiscale strategies to enhance the catalytic performance of TMPs, are comprehensively described. Finally, large-scale amplification synthesis, rational construction of TMP-based catalysts and in-depth study of the catalytic mechanism are also mentioned as challenges and future directions in this research field. Expectedly, this review can provide professional and targeted guidance for the rational design and practical application of TMPs biomass hydrogenation or HDO catalysts.

Development and comparison of parallel reaction monitoring and data-independent acquisition methods for quantitative analysis of hydrophilic compounds in white tea.

In the present work, parallel reaction monitoring (PRM) and data-independent acquisition (DIA) methods were developed for the accurate quantitation of amino acids, alkaloids nucleosides and nucleotides in tea. The quality peaks were significantly enhanced by optimizing the LC elution procedure, HCD voltage, MS resolution, and scanning event. Both methods were validated with good liner linearity (0.004-200 µg/mL), LODs (0.001-0.309 µg/mL for PRM and 0.001-0.564 µg/mL for DIA). Applied to white tea sample, the contents of these hydrophilic compounds were range from 34,655.39 to 70,586.14 mg/kg, and caffeine (32,529.02 mg/kg) and theanine (5483.46 mg/kg) were determined as the most abundant ones. Based on the quantitation data set, the white tea samples from Puer, Lincang and Xishuangbanna were clearly discriminated using multivariate data analysis. The results of the present works show that PRM and DIA have great potential in quantitative analysis of multiple hydrophilic compounds in food samples.

Patterns of physical and mental co-occurring developmental health among Chinese elderly: A multidimensional growth mixture model analysis.

Background: This study focuses on the heterogeneity, interaction, and imbalance in the concurrent development of physical and mental health trajectories among Chinese elderly. Methods: The data used in this study are from four waves of the China Health and Retirement Longitudinal Study (CHRLS) conducted between 2011 and 2018. A multidimensional growth mixture model (MGMM) was employed to analyze the patterns and characteristics of co-occurring physical and mental health development. Additionally, multinomial logistic regression analysis was conducted to systematically investigate the factors that predict the conjoint trajectories of physical and mental health. Results: The study findings reveal the presence of four distinct latent classes of conjoint trajectories for physical and mental health. These classes are categorized as follows: 'physical and mental health deteriorating', 'physical disease increasing & low mental vulnerability maintaining', 'low physical & mental vulnerability maintaining', and 'high physical disease increased & mental health moderate-stable'. Furthermore, demographic characteristics, socioeconomic status, family-society relations, health behaviors, and institutional factors were found to significantly predict these latent classes. Conclusion: The study emphasizes the diversity and complexity of physical and mental co-occurring developmental health issues in the elderly population in China. These findings have significant implications for the development of targeted intervention strategies that take into account the unique health changes experienced by older adults. Additionally, they can serve as evidence for the establishment of a comprehensive long-term care system.

Mortality prediction with adaptive feature importance recalibration for peritoneal dialysis patients.

The study aims to develop AICare, an interpretable mortality prediction model, using electronic medical records (EMR) from follow-up visits for end-stage renal disease (ESRD) patients. AICare includes a multichannel feature extraction module and an adaptive feature importance recalibration module. It integrates dynamic records and static features to perform personalized health context representation learning. The dataset encompasses 13,091 visits and demographic data of 656 peritoneal dialysis (PD) patients spanning 12 years. An additional public dataset of 4,789 visits from 1,363 hemodialysis (HD) patients is also considered. AICare outperforms traditional deep learning models in mortality prediction while retaining interpretability. It uncovers mortality-feature relationships and variations in feature importance and provides reference values. An AI-doctor interaction system is developed for visualizing patients' health trajectories and risk indicators.

Hollow Nanoreactors for Controlled Photocatalytic Behaviors: Fundamental Theory, Structure-Performance Relationship, and Catalytic Advantages.

Hollow nanoreactors (HoNRs) have regarded as an attractive catalytic material for photocatalysis due to their exceptional capabilities in enhancing light harvesting, facilitating charge separation and transfer, and optimizing surface reactions. Developing novel HoNRs offers new options to realize controllable catalytic behavior. However, the catalytic mechanism of photocatalysis occurring in HoNRs has not yet been fully revealed. Against this backdrop, this review elaborates on three aspects: 1) the fundamental theoretical insights of HoNRs-driven photocatalytic kinetics; 2) structure-performance relationship of HoNRs to photocatalysis; 3) catalytic advantages of HoNRs in photocatalytic applications. Specifically, the review focuses on the fundamental theories of HoNRs for photocatalysis and their structural advantages for strengthening light scattering, promoting charge separation and transfer, and facilitating surface reaction kinetics, and the relationship between key structural parameters of HoNRs and their photocatalytic performance is in-depth discussed. Also, future prospects and challenges are proposed. It is anticipated that this review paper will pave the way for forthcoming investigations in the realm of HoNRs for photocatalysis.

Optimizing internal control in public hospital supply chain: a game theory-based approach.

Objective: Our study aims to enhance the precision of internal control construction within public hospital supply chains and minimize the subjective bias influence. We have integrated the game theory combination weighting method into the design of internal control paths and based on this, developed a series of pioneering solutions. This innovative approach is anticipated to heighten the effectiveness and scientific rigor of the internal control design scheme within the supply chain. Method: Firstly, we utilized literature review and expert interviews to delve into the key factors of public hospital supply chain internal control, forming an index system for public hospital supply chain internal control that aligns with current informatization requirements. Subsequently, we incorporated the Game Theory Combination Weighting Method into this study. By means of the Analytic Hierarchy Process and the Entropy Weighting Method we determined the subjective and objective weights of each index and obtained their comprehensive weights through the Game Theory Combination Weighting Method. Then, based on the analysis results, we designed a series of internal control construction schemes and implemented these schemes at Weifang Maternal and Child Health Hospital between 2019 and 2023. Finally, using the Fuzzy Comprehensive Evaluation Method to assess and compare the actual effects before and after the implementation of the schemes, thereby validating the effectiveness of the Game Theory Combination Weighting Method in the design of the internal control path of public hospital supply chains. Results: The fuzzy comprehensive evaluation results for the years 2019 and 2023 demonstrated that after implementing our design schemes using the Game Theory Combination Weighting Method, the hospital's satisfaction in aspects such as plan-side control, purchase-side control, asset-side control, expenditure business control, and contract management control has significantly improved. Conclusion: Our research indicates that the Game Theory Combination Weighting Method is applicable to the path design of internal control links in public hospital supply chains. This method has effectively enhanced the targeted improvement of weak links within the construction of internal controls in the supply chain of public hospitals and is of great significance for improving the scientific nature of supply chain internal control management.

Analysis of Volatile Profile and Aromatic Characteristics of Raw Pu-erh Tea during Storage Based on GC-MS and Odor Activity Value.

Volatile constituents are critical to the flavor of tea, but their changes in raw Pu-erh tea (RAPT) during storage have not been clearly understood. This work aimed to investigate the volatile composition and their changes at various storage durations. The volatile profile of RAPT was determined using headspace solid-phase microextraction in combination gas chromatography-mass spectrometry. A total of 130 volatile compounds were identified in RAPT samples, and 64 of them were shared by all samples. The aroma attributes of RAPT over a storage period ranging from 0 to 10 years were assessed through the combination of odor activity value (OAV), aroma characteristic influence(ACI) value, and multivariate statistical analysis. The results revealed that RAPT exhibited a distinct floral and fruity aroma profile after storage for approximately 3-4 years. A notable shift in aroma was observed after 3-4 years of storage, indicating a significant turning point. Furthermore, the likely notable shift after 10 years of storage may signify the second turning point. According to the odor activity value (OAV ≥ 100), eight key volatile compounds were identified: linalool, α-terpineol, geraniol, trans-ß-ionone, α-ionone, (E,E)-2,4-heptadienal, 1-octanol, and octanal. Combining OAV (≥100) and ACI (≥1), five compounds, namely linalool, (E,E)-2,4-heptadienal, (Z)-3-hexen-1-ol, 2,6,10,10-tetramethyl-1-oxaspiro [4.5]dec-6-ene, and octanal, were identified as significant contributors to the aroma. The results offer a scientific foundation and valuable insights for understanding the volatile composition of RAPT and their changes during storage.

Reductive Amination of Levulinic Acid to Pyrrolidones: Key Step in Biomass Valorization towards Nitrogen-Containing Chemicals.

Nowadays, the field of biomass conversion is gradually moving towards an encouraging stage. The preparation of nitrogen-containing chemicals using various biomass resources instead of fossil resources do not only reduce carbon emissions, but also diversify the products of biomass conversion, thus increasing the economic competitiveness of biomass refining systems. Levulinic acid (LA) can be used as a promising intermediate in biomass conversion for further synthesis of pyrrolidone via reductive amination. However, there are still many critical issues to be solved. Particularly, the specific effects of catalysts on the performance of LA reductive amination have not been sufficiently revealed, and the potential impacts of key conditional factors have not been clearly elucidated. In view of this, this review attempts to provide theoretical insights through an in-depth interpretation of the above key issues. The contribution of catalysts to the reductive amination of LA as well as the catalyst structural preferences for improving catalytic performance are discussed. In addition, the role of key conditional factors is discussed. The insights presented in this review will contribute to the design of catalyst nanostructures and the rational configuration of green reaction conditions, which may provide inspiration to facilitate the nitrogen-related transformation of more biomass platform molecules.

Urolithin B alleviates Helicobacter pylori-induced inflammation and oxidative stress in mice.

BACKGROUND: Helicobacter pylori is one of the most common chronic bacterial infections. Active eradication of H. pylori infection is rare due to the fact that most infected patients are asymptomatic and the use of large amounts of antibiotics in eradication therapy leads to severe side effects. Urolithin B (UB) is an additional major intestinal metabolite of ellagic acid (EA), which has been shown to possess anti-inflammatory, antioxidant, and antiapoptotic biological activities. Preventing the incidence of H. pylori-related gastric disease and reducing the damage to the host by H. pylori is a current approach to control H. pylori infection. In this study, we explored the effect of UB on H. pylori infection. MATERIALS AND METHODS: The effects of UB on inflammation and oxidative stress induced by H. pylori in vivo and in vitro were investigated by qPCR, ELISA, HE staining, IHC staining, etc. RESULTS: UB reduced the adhesion and colonization of H. pylori and improved H. pylori-induced inflammation and oxidative stress in vivo and in vitro. Moreover, UB had better anti-inflammatory and antioxidant effects than clarithromycin (CLR) and metronidazole (MET). In addition to inhibiting the secretion of CagA, UB reduced tissue damage by H. pylori infection. CONCLUSIONS: UB was effective in improving damage caused by H. pylori.

Molecular Diffusion in Nanoreactors' Pore Channel System: Measurement Techniques, Structural Regulation, and Catalytic Effects.

Nanoreactors, as a new class of materials with highly enriched and ordered pore channel structures, can achieve special catalytic effects by precisely identifying and controlling the molecular diffusion behavior within the ordered pore channel system. Nanoreactors-driven molecular diffusion within the ordered pore channels can be highly dependent on the local microenvironment in the nanoreactors' pore channel system. Although the diffusion process of molecules within the ordered pore channels of nanoreactors is crucial for the regulation of catalytic behaviors, it has not yet been as clearly elucidated as it deserves to be in this study. In this review, fundamental theory and measurement techniques for molecular diffusion in the pore channel system of nanoreactors are presented, structural regulation strategies of pore channel parameters for controlling molecular diffusion are discussed, and the effects of molecular diffusion in the pore channel system on catalytic reactivity and selectivity are further analyzed. This article attempts to further develop the underlying theory of molecular diffusion within the theoretical framework of nanoreactor-driven catalysis, and the proposed perspectives may contribute to the rational design of advanced catalytic materials and the precise control of complex catalytic kinetics.

Methylene Blue-Loaded NanoMOFs: Accumulation in Chlamydia trachomatis Inclusions and Light/Dark Antibacterial Effects.

Metal-organic framework nanoparticles (nanoMOFs) are promising nanomaterials for biomedical applications. Some of them, including biodegradable porous iron carboxylates are proposed for encapsulation and delivery of antibiotics. Due to the high drug loading capacity and fast internalization kinetics, nanoMOFs are more beneficial for the treatment of intracellular bacterial infections compared to free antibacterial drugs, which poorly accumulate inside the cells because of the inability to cross membrane barriers or have low intracellular retention. However, nanoparticle internalization does not ensure their accumulation in the cell compartment that shelters a pathogen. This study shows the availability of MIL-100(Fe)-based MOF nanoparticles to co-localize with Chlamydia trachomatis, an obligate intracellular bacterium, in the infected RAW264.7 macrophages. Furthermore, nanoMOFs loaded with photosensitizer methylene blue (MB) exhibit complete photodynamic inactivation of C. trachomatis growth. Simultaneous infection and treatment of RAW264.7 cells with empty nanoMOFs resulted in a bacterial load reduction from 100 to 36% that indicates an intrinsic anti-chlamydial effect of this iron-containing nanomaterial. Thus, our findings suggest the use of iron-based nanoMOFs as a promising drug delivery platform, which contributes to antibacterial effect, for the treatment of chlamydial infections.

Ultrahigh-rate and ultralong-life aqueous batteries enabled by special pair-dancing proton transfer.

The design of Faradaic battery electrodes with high rate capability and long cycle life comparable to those of supercapacitors is a grand challenge. Here, we bridge this performance gap by taking advantage of a unique ultrafast proton conduction mechanism in vanadium oxide electrode, developing an aqueous battery with untrahigh rate capability up to 1000 C (400 A g-1) and extremely long life of 0.2 million cycles. The mechanism is elucidated by comprehensive experimental and theoretical results. Instead of slow individual Zn2+ transfer or Grotthuss chain transfer of confined H+, the ultrafast kinetics and excellent cyclic stability are enabled by rapid 3D proton transfer in vanadium oxide via the special pair dance switching between Eigen and Zundel configurations with little constraint and low energy barriers. This work provides insight into developing high-power and long-life electrochemical energy storage devices with nonmetal ion transfer through special pair dance topochemistry dictated by hydrogen bond.

Metal-Organic Framework-Based Nanomedicines for the Treatment of Intracellular Bacterial Infections.

Metal-organic frameworks (MOFs) are a highly versatile class of ordered porous materials, which hold great promise for different biomedical applications, including antibacterial therapy. In light of the antibacterial effects, these nanomaterials can be attractive for several reasons. First, MOFs exhibit a high loading capacity for numerous antibacterial drugs, including antibiotics, photosensitizers, and/or photothermal molecules. The inherent micro- or meso-porosity of MOF structures enables their use as nanocarriers for simultaneous encapsulation of multiple drugs resulting in a combined therapeutic effect. In addition to being encapsulated into an MOF's pores, antibacterial agents can sometimes be directly incorporated into an MOF skeleton as organic linkers. Next, MOFs contain coordinated metal ions in their structure. Incorporation of Fe2/3+, Cu2+, Zn2+, Co2+, and Ag+ can significantly increase the innate cytotoxicity of these materials for bacteria and cause a synergistic effect. Finally, abundance of functional groups enables modifying the external surface of MOF particles with stealth coating and ligand moieties for improved drug delivery. To date, there are a number of MOF-based nanomedicines available for the treatment of bacterial infections. This review is focused on biomedical consideration of MOF nano-formulations designed for the therapy of intracellular infections such as Staphylococcus aureus, Mycobacterium tuberculosis, and Chlamydia trachomatis. Increasing knowledge about the ability of MOF nanoparticles to accumulate in a pathogen intracellular niche in the host cells provides an excellent opportunity to use MOF-based nanomedicines for the eradication of persistent infections. Here, we discuss advantages and current limitations of MOFs, their clinical significance, and their prospects for the treatment of the mentioned infections.

Regional CO2 accounting and market layout of incinerator fly ash management in China.

The reduction of greenhouse gas (GHG) emissions from solid waste incinerator fly ash (IFA) management attracts growing interests since China's zero-waste plan and carbon peak/neutral goals. Herein, provincial GHG emissions from four demonstrated IFA reutilization technologies in China were estimated after analyzing IFA spatial-temporal distribution. Results indicate that technologies transition (landfilling-to-reutilization) could reduce GHG except for glassy slag production. IFA to cement option could potentially realize negative GHG emissions. Spatial GHG variation drivers in IFA management were recognized as provincial-different IFA composition and power emission factors. IFA management options were recommended provincially after weighting local development goals related to GHG reduction and economic benefits. Baseline scenario analysis shows that China's IFA industry would reach carbon peak in 2025 (5.02 Mt). 2030's GHG reduction potential (6.12 Mt) is equivalent to that of absorbed CO2 by 340 million trees annually. Overall, this research could contribute to illustrating future market layout complying with carbon peaking.