Perovskite Nanocrystals In Situ Encapsulated in TiO2 Microspheres for Stable CO2 Photoreduction in Water.

Photoreduction of carbon dioxide (CO2) into fuels presents a promising approach to mitigate global warming and energy crises. Halide perovskite nanocrystals (NCs) with prominent optoelectronic properties have triggered substantial attention as photocatalysts but are limited by the charge recombination and instability. Here, we develop stable CsPbBr3/titania microspheres (TMs) by in situ growth of CsPbBr3 NCs inside mesoporous TMs through solid-state sintering, which significantly improves the stability of perovskite NCs, making them applicable in water with efficient CO2 photoreduction performance. Notably, the CsPbBr3/TMs demonstrates a 6.73- and 9.23-fold increase in the rate of CH4 production compared to TMs and CsPbBr3, respectively. The internal electric field facilitates S-scheme charge transfer, enhancing the separation of electron-hole pairs, as evidenced by X-ray photoelectron spectroscopy and electron paramagnetic resonance analysis, which is pivotal for the selective photoreduction of CO2. These insights pave the way for the design of CsPbBr3-based photocatalysts with superior efficiency and stability.

Damage-Free Silica Coating for Colloidal Nanocrystals Through a Proactively Water-Generating Amidation Reaction at High Temperature.

Silica is a promising shell coating material for colloidal nanoparticles due to its excellent chemical inertness and optical transparency. To encapsulate high-quality colloidal nanocrystals with silica shells, the silane coupling hydrolysis is currently the most effective approach. However, this reaction requires water, which often adversely affects the intrinsic physicochemical properties of nanocrystals. Achieving a damage-free silica encapsulation process to nanocrystals by hydrolysis is a huge challenge. Here, a novel strategy is developed to coat colloidal nanocrystals with a denser silica shell via a proactively water-generating reaction at high temperature. In this work, water molecules are continuously and proactively released into the reaction system through the amidation reaction, followed by in situ hydrolysis of silane, completely avoiding the impacts of water on nanocrystals during the silica coating process. In this work, water sensitive perovskite nanocrystals (CsPbBr3 ) are selected as the typical colloidal nanocrystals for silica coating. Notably, this high-temperature in situ encapsulation technology greatly improves the optical properties of nanocrystals, and the silica shells exhibit a denser structure, providing nanocrystals with better protection. This method overcomes the challenge of the influence of water on nanocrystals during the hydrolysis process, and provides an important reference for the non-destructive encapsulation of colloidal nanocrystals.

Insights into the selectivity of a brain-penetrant CDK4/6 vs CDK1/2 inhibitor for glioblastoma used in multiple replica molecular dynamics simulations.

Cyclin dependent kinases (CDKs) play an important role in cell cycle regulation and their dysfunction is associated with many cancers. That is why CDKs have been attractive targets for the treatment of cancer. Glioblastoma is a cancer caused by the aberrant expression of CDK4/6, so exploring the mechanism of the selection of CDK4/6 toward inhibitors relative to the other family members CDK1/2 is essential. In this work, multiple replica molecular dynamics (MRMD) simulations, principal component analysis (PCA), free energy landscapes (FELs), molecular mechanics Poisson-Boltzmann/Generalized Born surface area (MM-PB/GBSA) and other methods were integrated to decipher the selectively binding mechanism of the inhibitor N1J to CDK4/6 and CDK1/2. Molecular electrostatic potential (MESP) analysis provides an explanation for the N1J selectivity. Residue-based free energy decomposition reveals that most of the hot residues are located at the same location of CDKs proteins, but the different types of residues in different proteins cause changes in binding energy, which is considered as a potential developmental direction to improve the selectivity of inhibitors to CDK4/6. These results provide insights into the source of inhibitor and CDK4/6 selectivity for the future development of more selective inhibitors.Communicated by Ramaswamy H. Sarma.

Interface defects repair of core/shell quantum dots through halide ion penetration.

The interface defects of core-shell colloidal quantum dots (QDs) affect their optoelectronic properties and charge transport characteristics. However, the limited available strategies pose challenges in the comprehensive control of these interface defects. Herein, we introduce a versatile strategy that effectively addresses both surface and interface defects in QDs through simple post-synthesis treatment. Through the combination of fine chemical etching methods and spectroscopic analysis, we have revealed that halogens can diffuse within the crystal structure at elevated temperatures, acting as "repairmen" to rectify oxidation and significantly reducing interface defects within the QDs. Under the guidance of this protocol, InP core/shell QDs were synthesized by a hydrofluoric acid-free method with a full width at half-maximum of 37.0 nm and an absolute quantum yield of 86%. To further underscore the generality of this strategy, we successfully applied it to CdSe core/shell QDs as well. These findings provide fundamental insights into interface defect engineering and contribute to the advancement of innovative solutions for semiconductor nanomaterials.

Molecular insights and optimization strategies for the competitive binding of engineered ACE2 proteins: a multiple replica molecular dynamics study.

The COVID-19 pandemic caused by severe acute respiratory syndrome coronavirus-2 (SARS-CoV-2) continues to spread globally, and rapid viral evolution and the emergence of new variants pose challenges to pandemic control. During infection, the spike protein of SARS-CoV-2 interacts with the human ACE2 protein via its receptor binding domain (RBD), and it is known that engineered forms of ACE2 can compete with wild-type (WT) ACE2 for binding to inhibit infection. Here, we conducted multiple replica molecular dynamics (MRMD) simulations to study the mechanisms of the engineered ACE2 variants 3N39 and 3N94 and provide directions for optimization. Our findings reveal that engineered ACE2 is notably more efficacious in systems that show weaker binding to WT ACE2 (i.e., WT and BA.1 RBD), but also faces immune escape as the virus evolves. Moreover, by modifying residue types near the binding interface, engineered ACE2 alters the electrostatic potential distribution and reconfigures the hydrogen bonding network, which results in modified binding to the RBD. However, this structural rearrangement does not occur in all RBD variants. In addition, we identified potentially engineerable beneficial residues and potentially engineerable detrimental residues in both ACE2 and RBD. Functional conservation can thus enable the optimization of these residues and improve the binding competitiveness of engineered ACE2, which therefore provides additional immune escape prevention. Finally, we conclude that these findings have implications for understanding the mechanisms responsible for engineered ACE2 and can help us to develop engineered ACE2 proteins that show superior performance.

Electroacupuncture combined with extracorporeal shock wave therapy improves pain symptoms and inflammatory factor levels in knee osteoarthritis patients.

Objective: To compare the clinical efficacy and safety of electroacupuncture combined with extracorporeal shock wave therapy (EESWT) and extracorporeal shock wave therapy (ESWT) in the treatment of knee osteoarthritis (KOA). Methods: A total of 135 KOA patients who received EESWT treatment were selected as the EESWT group, and 135 KOA patients who received extracorporeal shock wave therapy (ESWT) were selected as the ESWT group. The clinical efficacy, inflammatory factors in joint synovial fluid and adverse events during treatment were compared before and after treatment. Results: The clinical effective rate of patients in the EESWT group (89.63 %) after treatment was significantly higher than that of the ESWT group (74.81 %) (p < 0.01). The lysholm kness (LKSS) score and range of motion (ROM) of the patients in the EESWT group after treatment were higher than those of the ESWT group, while Lequesne index score, visual analogue scale (VAS) score and Western Ontario and McMaster Universities Arthritis Index (WOMAC) were lower than those of the ESWT group (p < 0.01). Compared with ESWT group, the changes in the expression levels of nitric oxide (NO), superoxide dismutase (SOD), interleukin 1ß (IL-1ß), tumor necrosis factor-α (TNF-α), matrix metalloproteinase-3 (MMP-3), and transforming growth factor ß1 (TGF-ß1) in the synovial fluid of the EESWT group after treatment were significantly greater than those of the ESWT group (p < 0.01). No significant difference in the incidence of adverse events between the EESWT group and the ESWT group (p > 0.05). Conclusion: EESWT significantly improves pain symptoms and inflammatory factor levels in KOA patients and is an optional KOA treatment option worthy of clinical attention.

Fluorine Passivation Inhibits "Particle Talking" Behaviors under Thermal and Electrical Conditions of Pure Blue Mixed Halide Perovskite Nanocrystals.

Owing to outstanding optoelectronic properties, lead halide perovskite nanocrystals (PNCs) are considered promising emitters for next-generation displays. However, the development of pure blue (460-470 nm) perovskite nanocrystal light-emitting diodes (PNC-LEDs), which correspond to the requirements of Rec. 2020 standard, lag far behind that of their green and red counterparts. Here, pure blue CsPb(Br/Cl)3 nanocrystals with remarkable optical performance are demonstrated by a facile fluorine passivation strategy. Prominently, the fluorine passivation on halide vacancies and strong bonding of Pb-F intensely enhance crystal structure stability and inhibit "particle talking" behaviors under both thermal and electrical conditions. Fluorine-based PNCs with high resistance of luminescence thermal quenching retain 70% of photoluminescent intensity when heated to 343 K, which can be attributed to the elevated activation energy for carrier trapping and unchanged grain size. Fluorine-based PNC-LEDs also exhibit stable pure blue electroluminescence (EL) emission with sevenfold promoted luminance and external quantum efficiencies (EQEs), where the suppression of ion migration is further evidenced by a lateral structure device with applied polarizing potential.

Nomogram to predict the incidence of new-onset heart failure after acute coronary syndrome among women.

Background: Although great progress has been made in caring for patients with acute coronary syndrome (ACS), the incidence of heart failure (HF) after discharge remains high after ACS. Aims: We aimed to investigate the risk predictors for new-onset HF and build a simple nomogram to optimize the clinical management of female patients. Methods: The clinical data of 319 female patients with ACS between January 1, 2021 and January 1, 2022, were obtained from the Zhejiang Provincial People's Hospital. Multivariate logistic regression analysis was carried out to build the prediction model among all participants and then verified by 10-fold cross-validation. The discrimination, calibration, and clinical usefulness of the prediction model were assessed using receiver operating characteristic curve, calibration curve, and decision curve analyses. Results: This study analyzed 15 potential independent risk predictors of new-onset HF in 319 female patients with ACS. The incidence of HF onset was 23.2%. The following 5 independent risk predictors were filtered out as most relevant for predicting 12-month HF onset: left ventricular ejection fraction ≤ 60.5%, high-density lipoprotein ≤ 1.055 mmol/L, human epididymal protein 4 > 69.6 pmol/L, creatinine > 71.95 µmol/L, and diagnosis of myocardial infarction (MI). Conclusion: Our nomogram, which used five easily obtained clinical variables, could be a useful tool to help identify female individuals with ACS who are at high risk of developing HF after discharge and facilitate communication between female patients and physicians.

Inverted semitransparent perovskite nanocrystal light-emitting diodes with a conjugated polymer as an electron transport layer.

Perovskite nanocrystals have attracted much attention due to their unique optical and electronic properties. Much progress has also been made in the development of light-emitting diodes based on perovskite nanocrystals in the past years. However, compared with the widely reported opaque perovskite nanocrystal light-emitting diodes, semitransparent perovskite nanocrystal light-emitting diodes are rarely studied, which affects the potential application of perovskite nanocrystals in the translucent display field in the future. Here, poly[(9,9-bis(3'-(N,N-dimethylamino)propyl)-2,7-fluorene)-alt-2,7-(9,9-dioctylfluorene)] (PFN), a conjugated polymer, was used as an electron transport layer to fabricate the inverted opaque and semitransparent perovskite light-emitting diodes. The maximum external quantum efficiency and luminance were improved from 0.13% and 1041 cd m-2 to 2.07% and 12 540 cd m-2, respectively, through device optimization in opaque light-emitting diodes. The corresponding semitransparent device also demonstrated high transmittance (average 61% from 380 to 780 nm) and high brightness of 1619 and 1643 cd m-2 for the bottom and top sides, respectively.

Association of Hemoglobin to Red Blood Cell Distribution Width-Standard Deviation (RDW-SD) Ratio and 3-Month Readmission in Elderly Chinese Patients with Heart Failure: A Retrospective Cohort Study.

Purpose: Hemoglobin (Hb) and red blood cell distribution width-standard deviation (RDW-SD) have clinical significance in the prognosis of heart failure (HF). Little is known regarding the prognostic value of the Hb/RDW-SD ratio in patients with HF. This study sought to investigate the association between Hb/RDW-SD ratio and HF 3-month readmission in Chinese elderly patients. Patients and Methods: The present study was a retrospective cohort study. A total of 1816 HF patients were extracted from the Chinese HF database. A generalized linear model was used to explore the association between Hb/RDW-SD and 3-month readmission in HF. The generalized additive model was used to explore the nonlinear relationship, and a two-piecewise linear regression model was used to find the inflection point. Subgroup analysis explored interactions and whether each subgroup was consistent with the primary outcome direction. Results: Result showed Hb/RDW-SD was negatively associated with HF 3-month readmission (OR = 0.70, 95% CI: 0.55 to 0.89, P = 0.0031). A non-linear relationship was detected between Hb/RDW-SD and HF 3-month readmission with two inflection points (1.78 and 2.17). Both Hb/RDW-SD < 1.78 and Hb/RDW-SD > 2.17 showed a significant correlation between them, with corresponding effect values of (OR = 0.38, 95% CI: 0.17 to 0.87, P = 0.0209) and (OR = 0.44, 95% CI: 0.27 to 0.71, P = 0.0007), respectively. Conclusion: Hb/RDW-SD is negatively associated with HF 3-month readmission. The relationship between Hb/RDW-SD and HF 3-month readmission is also non-linear. Both Hb/RDW-SD < 1.78 and Hb/RDW-SD > 2.17 were strong negatively associated with HF 3-month readmission.

Serum Human Epididymis Protein 4 as a Prognostic Predictor of New-Onset Heart Failure among Women after Acute Coronary Syndrome: A Single-Center Retrospective Study.

INTRODUCTION: Little is known about the prognostic factors among women with acute coronary syndrome (ACS), partly due to the small number of women included in heart failure (HF) clinical trials. Human epididymis protein 4 (HE4) has been proven to be a new biomarker for acute and chronic HF over the years. We hypothesize that HE4 could be a promising predictor. METHODS: This retrospective study analyzed data from Zhejiang Provincial People's Hospital. This study included 302 female patients with ACS between January 1, 2021, and December 1, 2021. The primary outcome was new-onset HF after ACS during the 12-month follow-up period. We used a logistic regression model to evaluate the association between serum HE4 levels and the incidence of HF. Serum HE4 levels were measured at baseline (within 24 h after admission). RESULTS: Of the 302 female patients, 70 (23.2%) developed new-onset HF within 12 months. Serum HE4 levels in patients with adverse events were significantly higher than those in patients without events (8.9 [7.3-11.5] pmol/dL versus 5.9 [5.0-6.8] pmol/dL, p < 0.001). The levels of HE4, troponin I peak, left ventricular ejection fraction (LVEF), and estimated glomerular filtration rate (eGFR) were validated as independent predictors, with HE4 being the best laboratory predictor (area under the curve, 0.863; 95% confidence interval, 0.817-0.909). Serum HE4 concentrations of >6.93 pmol/dL distinguished patients at risk of HF with 82.9% sensitivity and 78.0% specificity (maximum Youden index J, 0.609). Moreover, HE4 levels were associated with an increased risk of HF. DISCUSSION: We found a strong relationship between HE4 and the occurrence of HF after ACS among women, which might help identify patients at high risk of HF for whom close or intense management should be mandatory.

A Novel Strategy to Enhance the Photostability of InP/ZnSe/ZnS Quantum Dots with Zr Doping.

Plentiful research of InP semiconductor quantum dots (QDs) has been launched over the past few decades for their excellent photoluminescence properties and environmentally friendly characteristics in various applications. However, InP QDs show inferior photostability because they are extremely sensitive to the ambient environment. In this study, we propose a novel method to enhance the photostability of InP/ZnSe/ZnS QDs by doping zirconium into the ZnS layer. We certify that Zr can be oxidized to Zr oxides, which can prevent the QDs from suffering oxidation during light irradiation. The InP/ZnSe/ZnS:Zr QDs maintained 78% of the original photoluminescence quantum yields without significant photodegradation under the irradiation of LED light (450 nm, 3.0 W power intensity) for 14 h, while conventional InP/ZnSe/ZnS QDs dramatically decreased to 29%.

The role of TGR5 as an onco-immunological biomarker in tumor staging and prognosis by encompassing the tumor microenvironment.

The relationship between G protein-coupled bile acid receptor 1 (TGR5, GPBAR1) and, specifically, cancer has been studied in in vivo and in vitro experiments, but there is still a lack of pan-cancer analysis to understand the prognostic significance and functioning mechanism of TGR5 in different cancer-driving oncogenic processes. Here, we used Gene Expression Integration, Human Protein Atlas, and The Cancer Genome Atlas (TCGA) to perform a pan-cancer analysis of the role of TGR5 in all 33 tumors. In all TCGA tumors, the TGR5 gene expression has been assessed, and we found that the high TGR5 gene expression in most cancers is associated with poor prognosis of overall survival for cancers such as glioblastoma multiforme (p = 0.0048), kidney renal papillary cell carcinoma (p = 0.033), lower grade glioma (p = 0.0028), thymoma (p = 0.048), and uveal melanoma (p = 0.004), and then the lower expression of TGR5 was linked with poor prognosis in cervical squamous cell carcinoma and endocervical adenocarcinoma (p = 0.014), malignant mesothelioma (MESO) (p = 0.048), sarcoma (p = 0.018), and skin cutaneous melanoma (p = 0.0085). The TGR5 expression was linked with the immune infiltration level of the macrophage M2_TIDE and was also associated with DNA methylation in ovarian and breast cancers. The regulation of hormone secretion, Rap1 pathway, osteoclast differentiation, and bile acid pathway was involved in the functional mechanism of TGR5. Besides, gene expressions were different in different tumors detected by RT-PCR, and cell activity experiments have also found that TGR5 can increase the activity of renal cell carcinoma and reduce the activity of skin cancer and osteosarcoma cells. In this investigation, the aim was to assess the comprehensive overview of the oncogenic roles of TGR5 in all TCGA tumors using pan-analysis.