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Hydroxyl groups on the surface of cellulose nanocrystals (CNC) are modified by chemical methods, CNC and the modified CNC are used as fillers to prepare PHB/cellulose nanocomposites. The absorption peak of carbonyl group of the modified CNC (CNC-CL and CNC-LA) appears in the FT-IR spectra, which proves that the modifications are successful. Thermal stability of CNC-CL and CNC-LA is better than that of pure CNC. Pure CNC is beneficial to the nucleation of PHB, while CNC-CL and CNC-LA inhibit the nucleation of PHB. The spherulite size of PHB and its nanocomposites increases linearly over time, and the maximum growth rate of PHB spherulite exists at 90 °C. Rheological analysis shows that viscous deformation plays the dominant role in PHB, PHBC and PHBC-CL samples, while the elastic deformation is dominant in PHBC-LA. According to the rheological data, the dispersion of CNC-CL and CNC-LA in PHB is better than that of CNC. This work demonstrates the impact of modified CNC on the crystallization and viscoelastic properties of PHB. Moreover, the interface enhancement effect of modified CNC on PHB/CNC nanomaterials is revealed from the crystallization and rheology perspectives.
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BACKGROUND: Precise glioma segmentation from multi-parametric magnetic resonance (MR) images is essential for brain glioma diagnosis. However, due to the indistinct boundaries between tumor sub-regions and the heterogeneous appearances of gliomas in volumetric MR scans, designing a reliable and automated glioma segmentation method is still challenging. Although existing 3D Transformer-based or convolution-based segmentation networks have obtained promising results via multi-modal feature fusion strategies or contextual learning methods, they widely lack the capability of hierarchical interactions between different modalities and cannot effectively learn comprehensive feature representations related to all glioma sub-regions. PURPOSE: To overcome these problems, in this paper, we propose a 3D hierarchical cross-modality interaction network (HCMINet) using Transformers and convolutions for accurate multi-modal glioma segmentation, which leverages an effective hierarchical cross-modality interaction strategy to sufficiently learn modality-specific and modality-shared knowledge correlated to glioma sub-region segmentation from multi-parametric MR images. METHODS: In the HCMINet, we first design a hierarchical cross-modality interaction Transformer (HCMITrans) encoder to hierarchically encode and fuse heterogeneous multi-modal features by Transformer-based intra-modal embeddings and inter-modal interactions in multiple encoding stages, which effectively captures complex cross-modality correlations while modeling global contexts. Then, we collaborate an HCMITrans encoder with a modality-shared convolutional encoder to construct the dual-encoder architecture in the encoding stage, which can learn the abundant contextual information from global and local perspectives. Finally, in the decoding stage, we present a progressive hybrid context fusion (PHCF) decoder to progressively fuse local and global features extracted by the dual-encoder architecture, which utilizes the local-global context fusion (LGCF) module to efficiently alleviate the contextual discrepancy among the decoding features. RESULTS: Extensive experiments are conducted on two public and competitive glioma benchmark datasets, including the BraTS2020 dataset with 494 patients and the BraTS2021 dataset with 1251 patients. Results show that our proposed method outperforms existing Transformer-based and CNN-based methods using other multi-modal fusion strategies in our experiments. Specifically, the proposed HCMINet achieves state-of-the-art mean DSC values of 85.33% and 91.09% on the BraTS2020 online validation dataset and the BraTS2021 local testing dataset, respectively. CONCLUSIONS: Our proposed method can accurately and automatically segment glioma regions from multi-parametric MR images, which is beneficial for the quantitative analysis of brain gliomas and helpful for reducing the annotation burden of neuroradiologists.
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Combining the merits of the dendrite-free formation of a Mg anode and the fast kinetics of Li ions, the Mg-Li hybrid ion batteries (MLIBs) are considered an ideal energy storage system. However, the lack of advanced cathode materials limits their further practical application. Herein, we report a dual strategy of morphology optimization and interlayer expansion for the construction of hierarchical flower-like VS2 architecture coated by N-doped amorphous carbon layers. This tailored hierarchical flower-like structure coupled with homogeneous N-doped amorphous carbon layers cooperatively provide more active sites and buffer volume changes, thus realizing the enhancement of capacity and structural stability. Moreover, the enlarged interlayer spacing caused by the cointercalation of polyvinylpyrrolidone and ammonium ions can effectively promote the charge transfer rate and facilitate the rapid ion diffusion, as further demonstrated by electrochemical results and theoretical calculations. These features endow the hierarchical flower-like VS2 cathode with superior specific energy density (644.4 Wh kg-1, average voltage of 1.2 V vs Mg2+/Mg) and excellent rate capability (181.1 mAh g-1 at 2000 mA g-1). Systematic ex situ characterization measurements are employed to reveal the ion storage mechanism, which confirms that Li+ storage plays a leading role in the capacity contribution of MLIBs. Our strategy is in favor of providing useful insights to design and construct MLIBs with high energy density and excellent rate performance.
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Next Point-of-Interest (POI) recommendation aims to predict the next POI for users from their historical activities. Existing methods typically rely on location-level POI check-in trajectories to explore user sequential transition patterns, which suffer from the severe check-in data sparsity issue. However, taking into account region-level and category-level POI sequences can help address this issue. Moreover, collaborative information between different granularities of POI sequences is not well utilized, which can facilitate mutual enhancement and benefit to augment user preference learning. To address these challenges, we propose multi-granularity contrastive learning (MGCL) for next POI recommendation, which utilizes multi-granularity representation and contrastive learning to improve the next POI recommendation performance. Specifically, location-level POI graph, category-level, and region-level sequences are first constructed. Then, we use graph convolutional networks on POI graph to extract cross-user sequential transition patterns. Furthermore, self-attention networks are used to learn individual user sequential transition patterns for each granularity level. To capture the collaborative signals between multi-granularity, we apply the contrastive learning approach. Finally, we jointly train the recommendation and contrastive learning tasks. Extensive experiments demonstrate that MGCL is more effective than state-of-the-art methods.
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PURPOSE: The purpose was to evaluate the clinical outcomes of a dedicated venous stent with the tripartite composite segments for the treatment of iliofemoral venous obstruction (IVO) in a mixed cohort of nonthrombotic iliac vein lesion (NIVL) and post-thrombotic syndrome (PTS) over a period of 12 months. METHODS: The Grency Trial is a prospective, multicenter, single-arm, open-label, pivotal study, which was conducted at 18 large tertiary hospitals in China from August 2019 to October 2020. A total of 133 hospitalized patients were screened and 110 patients with clinical, etiology, anatomical, and pathophysiology clinical class (CEAP) clinical grade C>3 and iliac vein stenosis >50% or occlusion, including 72 patients with NIVL and 38 patients with PTS, were implanted with Grency venous stents. Primary endpoint was stent patency at 12 months follow-up, and secondary outcomes were technical success; improvement in venous clinical severity score (VCSS) at 3, 6, and 12 month follow-up; and rates of clinical adverse events. RESULTS: Among 110 patients who were implanted with Grency venous stents, 107 patients completed the 12 month follow-up. All 129 stents were successfully implanted in 110 limbs. Twelve-month primary patency rate was 94.39% [95% confidence interval [CI]=88.19%-97.91%] overall, and 100% [94.94%-100%] and 83.33% [67.19%-93.63%] in the NIVL and PTS subgroups, respectively. Venous clinical severity score after iliac vein stenting improved significantly up to 12 months follow-up. There were 3 early major adverse events (1 intracerebral hemorrhage and 2 stent thrombosis events related to anticoagulation therapy), and 7 late major adverse events (1 cardiovascular death, 1 intracranial hemorrhage with uncontrolled hypertension, and 5 in-stent restenosis cases without stent fractures or migration). CONCLUSIONS: The Grency venous stent system appeared excellent preliminary safe and effective for IVO treatment. Further large-scale studies with longer-term follow-up are needed to evaluate long-term patency and durability of stent. CLINICAL IMPACT: The design of venous stents for iliofemoral venous obstruction (IVO) must address engineering challenges distinct from those encountered in arterial stenting. The Grency venous stent, a nitinol self-expanding stent specifically tailored for IVO, features a composite structure designed to meet the stent requirements of various iliac vein segments. The Grency Trial is a prospective, multicenter, single-arm, open-label pivotal study aimed at evaluating the efficacy and safety of the Grency stent system. Following a 12-month follow-up period, the Grency venous stent system has demonstrated both safety and efficacy in treating iliofemoral venous outflow obstruction.
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Based on Sima and Lu's system of the family Magnoliaceae, the genus Lirianthe Spach s. l. includes approximately 25 species, each with exceptional landscaping and horticultural or medical worth. Many of these plants are considered rare and are protected due to their endangered status. The limited knowledge of species within this genus and the absence of research on its chloroplast genome have greatly impeded studies on the relationship between its evolution and systematics. In this study, the chloroplast genomes of eight species from the genus Lirianthe were sequenced and analyzed, and their phylogenetic relationships with other genera of the family Magnoliaceae were also elucidated. The results showed that the chloroplast genome sizes of the eight Lirianthe species ranged from 159,548 to 159,833 bp. The genomes consisted of a large single-copy region, a small single-copy region, and a pair of inverted repeat sequences. The GC content was very similar across species. Gene annotation revealed that the chloroplast genomes contained 85 protein-coding genes, 37 tRNA genes, and 8 rRNA genes, totaling 130 genes. Codon usage analysis indicated that codon usage was highly conserved among the eight Lirianthe species. Repeat sequence analysis identified 42-49 microsatellite sequences, 16-18 tandem repeats, and 50 dispersed repeats, with microsatellite sequences being predominantly single-nucleotide repeats. DNA polymorphism analysis revealed 10 highly variable regions located in the large single-copy and small single-copy regions, among which rpl32-trnL, petA-psbJ, and trnH-psbA were the recommended candidate DNA barcodes for the genus Lirianthe species. The inverted repeat boundary regions show little variation between species and are generally conserved. The result of phylogenetic analysis confirmed that the genus Lirianthe s. l. is a monophyletic taxon and the most affinal to the genera, Talauma and Dugandiodendron, in Sima and Lu's system and revealed that the genus Lirianthe s. s. is paraphyletic and the genus Talauma s. l. polyphyletic in Xia's system, while Magnolia subsection Gwillimia is paraphyletic and subsection Blumiana polyphyletic in Figlar and Nooteboom's system. Morphological studies found noticeable differences between Lirianthe species in aspects including leaf indumentum, stipule scars, floral orientation, tepal number, tepal texture, and fruit dehiscence. In summary, this study elucidated the chloroplast genome evolution within Lirianthe and laid a foundation for further systematic and taxonomic research on this genus.
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Genome, Chloroplast , Magnolia , Phylogeny , Molecular Sequence Annotation , Plants/geneticsABSTRACT
Direct photocatalytic methane oxidation into value-added products provides a promising strategy for methane utilization. However, the inefficient generation of reactive oxygen species (ROS) partly limits the activation of CH4. Herein, it is reported that Pd and VOδ co-modified TiO2 enables direct and selective methane oxidation into liquid oxygenates in the presence of O2 and H2. Due to the extra ROS production from the in situ formed H2O2, a highly improved yield rate of 5014 µmol g-1 h-1 for liquid oxygenates with a selectivity of 89.3% is achieved over the optimized Pd0.5V0.2-TiO2 catalyst at ambient temperature, which is much better than those (2682 µmol g-1 h-1, 77.8%) without H2. Detailed investigations also demonstrate the synergistic effect between Pd and VOδ species for enhancing the charge carrier separation and transfer, as well as improving the catalytic activity for O2 reduction and H2O2 production.
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To investigate the relationship between selenium (Se) based multi-element combined exposure and cognitive function in rural elderly individuals, a cross-sectional study was conducted. The study involved 416 older adults aged 60 and above, residing in four different areas of Enshi county, China, with varying soil Se levels. Inductively coupled plasma mass spectrometry (ICP-MS) was employed to measure the concentrations of Se, copper (Cu), iron (Fe), zinc (Zn), calcium (Ca), magnesium (Mg), cadmium (Cd), arsenic (As), and lead (Pb) in whole blood. Nine standard cognitive tests were applied to assess cognitive function. Analysis of the least absolute shrinkage and selection operator regression (LASSO), covariance (ANCOVA), and generalized linear model (GLM) were utilized to investigate the relationship between element exposure and cognitive function. The results of LASSO revealed that Se, Cu, Fe, Zn, Ca, and Pb were independently identified to be associated with cognition. Both ANCOVA and GLM demonstrated that Se and Ca were correlated with cognitive function. The multi-element model showed higher composite Z scores of 0.32 (95% CI: 0.09 to 0.55) for log-transformed Se (P = 0.007), 0.75 (95% CI: 0.01 to 1.49) for log-transformed Cu (P = 0.048), and a lower score of - 0.67 (95% CI: - 1.26 to - 0.08) for log-transformed Ca (P = 0.025). Furthermore, there was evidence that Se could counteract the negative impact of Ca on cognitive function (P for interaction = 0.031). Our findings suggested that higher levels of Se and Cu were associated with better cognitive function in the elderly and Se can counteract the cognitive damage caused by Ca.
Subject(s)
Selenium , Trace Elements , Humans , Aged , Cross-Sectional Studies , Lead , Zinc , Copper , CognitionABSTRACT
PURPOSE: To report the outcomes of the IN-DEPT trial assessing the feasibility, preliminary safety data, and 12-month outcomes of a new drug-coated balloon (DCB) product for peripheral artery disease (PAD) in Chinese patients. MATERIALS AND METHODS: This is a prospective, multicenter, single-arm clinical trial. A total of 160 patients with superficial femoral artery (SFA) and/or proximal popliteal artery lesions were treated with a new paclitaxel-coated DCB. The preliminary effectiveness end point was 12-month primary patency. The primary safety end point was freedom from device- and procedure-related mortality over 30 days and freedom from major target limb amputation and clinically driven target lesion revascularization (CD-TLR) within 12 months after the index procedure. RESULTS: In total, 160 patients presented with 162 target lesions. A total of 139 lesions (85.8%) were treated with 1 DCB, whereas the other 23 lesions (14.2%) were treated with 2 devices. The device success rate was 100%. A total of 135 subjects reached the preliminary effectiveness end point, with a 12-month primary patency rate of 84.4%. There was no 30-day device- or procedure-related death or unplanned major target limb amputation at 12 months. Five CD-TLRs (3.1%) occurred during the 12-month follow-up period. CONCLUSIONS: Results from the IN-DEPT SFA trial showed satisfactory feasibility and safety of the new DCB over 12 months in Chinese patients with PAD and femoropopliteal de novo lesions, including both stenoses and total occlusions.
Subject(s)
Angioplasty, Balloon , Cardiovascular Agents , Peripheral Arterial Disease , Humans , Femoral Artery/diagnostic imaging , Femoral Artery/pathology , Prospective Studies , Angioplasty, Balloon/adverse effects , Coated Materials, Biocompatible , Time Factors , Cardiovascular Agents/adverse effects , Popliteal Artery/diagnostic imaging , Peripheral Arterial Disease/diagnostic imaging , Peripheral Arterial Disease/therapy , Peripheral Arterial Disease/pathology , Vascular Patency , Treatment OutcomeABSTRACT
Nanotransfer printing of colloidal nanoparticles is a promising technique for the fabrication of functional materials and devices. However, patterning nonplanar nanostructures pose a challenge due to weak adhesion from the extremely small nanostructure-substrate contact area. Here, the study proposes a thermal-assisted nonplanar nanostructure transfer printing (NP-NTP) strategy for multiscale patterning of polystyrene (PS) nanospheres. The printing efficiency is significantly improved from ≈3.1% at low temperatures to ≈97.2% under the glass transition temperature of PS. Additionally, the arrangement of PS nanospheres transitioned from disorder to long-range order. The mechanism of printing efficiency enhancement is the drastic drop of Young's modulus of nanospheres, giving rise to an increased contact area, self-adhesive effect, and inter-particle necking. To demonstrate the versatility of the NP-NTP strategy, it is combined with the intaglio transfer printing technique, and multiple patterns are created at both micro and macro scales at a 4-inch scale with a resolution of ≈2757 pixels per inch (PPI). Furthermore, a multi-modal anti-counterfeiting concept based on structural patterns at hierarchical length scales is proposed, providing a new paradigm of imparting multiscale nanostructure patterning into macroscale functional devices.
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BACKGROUND: With the rising prevalence of severe obesity, bariatric surgery has emerged as a crucial treatment option. As the number of surgeries performed worldwide increases, there has been growing interest in the impact of bariatric surgery on cancer incidence. While several studies have examined this relationship, the topic remains controversial. OBJECTIVES: We conducted this systematic review of cohort studies with meta-analysis to evaluate the effect of bariatric surgery versus nonsurgical treatment on overall cancer incidence. However, the effects may vary when focusing on specific cancer types, surgical procedures, or gender, so we conducted additional subgroup analyses. SETTING: A meta-analysis. University hospital. METHODS: The Cochrane, Embase, PubMed, and Web of Science databases were searched for studies from 1 January 2000 to 1 December 2022. Meta-analysis was conducted to evaluate the pooled effect and further implemented subgroup analysis stratified by cancer type, operation type, and sex. RESULTS: All cohort studies were included in this meta-analysis from 18,216 studies. The overall cancer incidence demonstrated a significant decrease in the group with bariatric surgery (odds ratios [OR] = .56, P = .000, 95% CI .46 to .68). In subgroup analysis, similar decrease effect was found in 9 cancers. Furthermore, the incidence of cancer decreased significantly in male (OR = .66, P = .001, 95% CI .51 to .85) and female patients (OR = .63, P = .000, 95% CI .57 to .69) and patients undergoing gastric bypass (OR = .46, P = .000, 95% CI .33 to .63) or sleeve gastrectomy (OR = .44, P = .001, 95% CI .27 to .70). CONCLUSIONS: In the overall analysis, bariatric surgery could reduce the incidence of cancer significantly. Further large-scale well-matched studies are needed to verify the protective effect of bariatric surgery on cancer incidence.
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Bariatric Surgery , Neoplasms , Obesity, Morbid , Humans , Bariatric Surgery/adverse effects , Bariatric Surgery/statistics & numerical data , Incidence , Neoplasms/epidemiology , Neoplasms/surgery , Obesity, Morbid/surgery , Obesity, Morbid/epidemiology , Obesity, Morbid/complications , Male , Female , Cohort StudiesABSTRACT
Gaze estimation, as a technique that reflects individual attention, can be used for disability assistance and assisting physicians in diagnosing diseases such as autism spectrum disorder (ASD), Parkinson's disease, and attention deficit hyperactivity disorder (ADHD). Various techniques have been proposed for gaze estimation and achieved high resolution. Among these approaches, electrooculography (EOG)-based gaze estimation, as an economical and effective method, offers a promising solution for practical applications. OBJECTIVE: In this paper, we systematically investigated the possible EOG electrode locations which are spatially distributed around the orbital cavity. Afterward, quantities of informative features to characterize physiological information of eye movement from the temporal-spectral domain are extracted from the seven differential channels. METHODS AND PROCEDURES: To select the optimum channels and relevant features, and eliminate irrelevant information, a heuristical search algorithm (i.e., forward stepwise strategy) is applied. Subsequently, a comparative analysis of the impacts of electrode placement and feature contributions on gaze estimation is evaluated via 6 classic models with 18 subjects. RESULTS: Experimental results showed that the promising performance was achieved both in the Mean Absolute Error (MAE) and Root Mean Square Error (RMSE) within a wide gaze that ranges from -50° to +50°. The MAE and RMSE can be improved to 2.80° and 3.74° ultimately, while only using 10 features extracted from 2 channels. Compared with the prevailing EOG-based techniques, the performance improvement of MAE and RMSE range from 0.70° to 5.48° and 0.66° to 5.42°, respectively. CONCLUSION: We proposed a robust EOG-based gaze estimation approach by systematically investigating the optimal channel/feature combination. The experimental results indicated not only the superiority of the proposed approach but also its potential for clinical application. Clinical and translational impact statement: Accurate gaze estimation is a key step for assisting disabilities and accurate diagnosis of various diseases including ASD, Parkinson's disease, and ADHD. The proposed approach can accurately estimate the points of gaze via EOG signals, and thus has the potential for various related medical applications.
Subject(s)
Autism Spectrum Disorder , Parkinson Disease , Humans , Electrooculography/methods , Autism Spectrum Disorder/diagnosis , Parkinson Disease/diagnosis , Eye Movements , ElectrodesABSTRACT
Gaze estimation based on electrooculograms (EOGs) has been widely explored. However, the inter-subject variability of EOGs still leaves a significant challenge for practical applications. It contributes to performance degradation when handling inter-subject issues. In this paper, an unsupervised transfer learning approach with an adaptive reweighting and resampling (ARR) strategy to fully consider individual variability is proposed for EOG-based gaze angle estimation. It allows quantifying domain shifts by leveraging the source-target similarities, reweighting and resampling the source data to retain relevant instances and disregard irrelevant instances during adaptation. Specifically, our proposed methodology first assesses the domain shifts via decomposing transformation matrices, which are estimated between the training subjects (denoted as multi-source domains) and the test subject (denoted as target domain). Then, the multi-domain shifts are assigned as weighted indicators to resample the multi-source domains for model training. Comparative experiments with several prevailing transfer learning methods including CORrelation ALignment (CORAL), Geodesic Flow Kernel (GFK), Joint Distribution Adaptation (JDA), Transfer component analysis (TCA), and Balanced distribution adaption (BDA) using two different normalization processes were conducted on a realistic scenario across 18 subjects. Experimental results demonstrate that the ARR strategy can significantly improve performance (mean absolute error (MAE) reduction: 7.0%, root mean square error (RMSE) reduction: 6.3%), outperforming the prevailing methods. Besides, the impacts of data diversity and data size on ARR strategy are further investigated. It exhibits that data size is more important than data diversity for EOG-based gaze angle estimation, and also presents the benefits of the ARR strategy for dealing with practical scenarios.
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OBJECTIVE: The value of tumor deposits (TDs) in the prognosis and staging of gastric cancer (GC) is still under debate. This study aims to evaluate the prognostic value of TDs and the best ways to incorporate TDs in the TNM classification of GC. METHODS: Patients (n = 3460) undergoing curative gastrectomy for GC in the West China Hospital from 2005 to 2017 were retrospectively reviewed and divided into two groups according to the TD status (positive vs. negative). Later, clinicopathological features and overall survival (OS) between the two groups were compared. Thereafter, the associations between the presence of TD and other clinicopathological factors were evaluated through logistic regression. In addition, univariate and multivariate Cox regression were conducted for determining prognostic factors. The possibility of selection bias was reduced through conducting the 1:1 propensity score matching (PSM) analysis. The modified classification systems proposed previously that incorporated TDs into the TNM staging system were assessed. RESULTS: There were 10.5% of patients (362/3460) diagnosed with TDs. TDs were significantly related to unfavorable factors such as advanced T stage and N stage and independently associated with poor prognosis. The 5-year OS of patients with TDs was significantly lower than that of patients without TDs (31.0% vs. 60.9%, P < 0.001), whereas higher than that of patients with peritoneal metastasis (31.0% vs. 5.0%, P < 0.001). In patients receiving chemotherapy, the 5-year OS of patients with TDs was also significantly lower than that of patients without TDs (42.0% vs. 50.9%, P = 0.026). Moreover, the system incorporating TDs in the TNM classification as metastatic lymph nodes outperformed others. CONCLUSIONS: TDs are related to the aggressive characteristics and are an independent prognostic factor for GC. Incorporating TDs in the TNM classification as the metastatic lymph nodes increases the accuracy in predicting prognosis.
Subject(s)
Stomach Neoplasms , Humans , Stomach Neoplasms/pathology , Retrospective Studies , Propensity Score , Extranodal Extension/pathology , Clinical Relevance , Prognosis , Neoplasm Staging , GastrectomyABSTRACT
Drug resistance remains the greatest challenge in improving outcomes for cancer patients who receive chemotherapy and targeted therapy. Surmounting evidence suggests that a subpopulation of cancer cells could escape intense selective drug treatment by entering a drug-tolerant state without genetic variations. These drug-tolerant cells (DTCs) are characterized with a slow proliferation rate and a reversible phenotype. They reside in the tumor region and may serve as a reservoir for resistant phenotypes. The survival of DTCs is regulated by epigenetic modifications, transcriptional regulation, mRNA translation remodeling, metabolic changes, antiapoptosis, interactions with the tumor microenvironment, and activation of signaling pathways. Thus, targeting the regulators of DTCs opens a new avenue for the treatment of therapy-resistant tumors. In this review, we first provide an overview of common characteristics of DTCs and the regulating networks in DTCs development. We also discuss the potential therapeutic opportunities to target DTCs. Last, we discuss the current challenges and prospects of the DTC-targeting approach to overcome acquired drug resistance. Reviewing the latest developments in DTC research could be essential in discovering of methods to eliminate DTCs, which may represent a novel therapeutic strategy for preventing drug resistance in the future.
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Although MXene catalysts etched from precursor MAX have greatly improved the hydrogen storage performance of magnesium hydride (MgH2), the use of dangerous and polluting etchers (such as hydrofluoric acid) and the direct removal of potentially catalytically active A-layer substances (such as Al) present certain limitations. Here, solid-solution MAX phase TiVAlC catalyst without etching treatment has been directly introduced into MgH2 system to improve the hydrogen storage performance. The optimal MgH2-10 wt% TiVAlC can release about 6.00 wt% hydrogen at 300 °C within 378 s and absorb about 4.82 wt% hydrogen at 175 °C within 900 s. After 50 isothermal hydrogen ab/desorption cycles, the excellent cyclic stability and capacity retention (6.4 wt%, 99.6%) can be found for MgH2-10 wt% TiVAlC. The superb catalytic activity of TiVAlC catalyst can be explained by abundant electron transfer at external interfaces with MgH2/Mg, which can be further enhanced by impurity phase Ti3AlC2 due to strong H affinity brought from abundant electron transfer at internal interfaces (Ti3AlC2/TiVAlC). The influence of impurity phase which is common in MAX phase on the overall activity of catalysts has been firstly studied here, providing a unique method for designing composite catalyst to improve hydrogen storage performance of MgH2.
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Organic memory has attracted tremendous attention for next-generation electronic elements for the molecules' striking ease of structural design. However, due to them being hardly controllable and their low ion transport, it is always essential and challenge to effectively control their random migration, pathway, and duration. There are very few effective strategies, and specific platforms with a view to molecules with specific coordination-groups-regulating ions have been rarely reported. In this work, as a generalized rational design strategy, the well-known tetracyanoquinodimethane (TCNQ) is introduced with multiple coordination groups and small plane structure into a stable polymers framework to modulate Ag migration and then achieve high-performance devices with ideal productivity, low operation voltage and power, stable switching cycles, and state retention. Raman mapping demonstrates that the migrated Ag can specially coordinate with the embedded TCNQ molecules. Notably, the TCNQ molecule distribution can be modulated inside the polymer framework and regulate the memristive behaviors through controlling the formed Ag conductive filaments (CFs) as demonstrated by Raman mapping, in situ conductive atomic force microscopy (C-AFM), X-ray diffraction (XRD) and depth-profiling X-ray photoelectron spectroscopy (XPS). Thus the controllable molecule-mediated Ag movements show its potential in rationally designing high-performance devices and versatile functions and is enlightening in constructing memristors with molecule-mediated ion movements.
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V-based sulfides are considered as potential cathode materials for Mg2+/Li+ hybrid ion batteries (MLIBs) due to their high theoretical specific capacities, unique crystal structure, and flexible valence adjustability. However, the formation of irreversible polysulfides, poor cycling performance, and severe structural collapse at high current densities impede their further development. Herein, VS4 microspheres with various controllable nanoarchitectures were successfully constructed via a facile solvothermal method by adjusting the amount of hydrochloric acid and were used as cathode materials for MLIBs. The VS4 microsphere self-assembled by bundles of paralleled-nanorods and some intersected-nanorods (VS4@NC-5) exhibits an outstanding initial discharge capacity of 805.4 mAh g-1 at 50 mA g-1 that is maintained at 259.1 mAh g-1 after 70 cycles. Moreover, the VS4@NC-5 cathode can deliver a superior rate capability (146.1 mAh g-1 at 2000 mA g-1) and ultralong cycling life (134.5 mAh g-1 at 2000 mA g-1 after 2000 cycles). The extraordinary electrochemical performance of VS4@NC-5 could be attributed to its special multi-hierarchical microsphere structure and the formation of N-doped carbon layers and V-C bonds, resulting in unobstructed ion diffusion channels, multidimensional electron transfer pathways, and enhancements of electrical conductivity and structure stability. Furthermore, the electrochemical reaction mechanism and phase conversion behavior of the VS4@NC-5 cathode at various states are investigated by a series of ex situ characterization methods. The VS4 well-designed through morphological engineering in this work can pave a way to explore more sulfides with high-rate performance and long cycling stability for energy storage devices.
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Proton exchange membrane water electrolysers and alkaline exchange membrane water electrolysers for hydrogen production suffer from sluggish kinetics and the limited durability of the electrocatalyst toward oxygen evolution reaction (OER). Herein, a rutile Ru0.75 Mn0.25 O2-δ solid solution oxide featured with a hierarchical porous structure has been developed as an efficient OER electrocatalyst in both acidic and alkaline electrolyte. Specifically, compared with commercial RuO2 , the catalyst displays a superior reaction kinetics with small Tafel slope of 54.6â mV dec-1 in 0.5â M H2 SO4 , thus allowing a low overpotential of 237 and 327â mV to achieve the current density of 10 and 100â mA cm-2 , respectively, which is attributed to the enhanced electrochemically active surface area from the porous structure and the increased intrinsic activity owing to the regulated Ru>4+ proportion with Mn incorporation. Additionally, the sacrificial dissolution of Mn relieves the leaching of active Ru species, leading to the extended OER durability. Besides, the Ru0.75 Mn0.25 O2-δ catalyst also shows a highly improved OER performance in alkaline electrolyte, rendering it a versatile catalyst for water splitting.
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Introduction: Melanoma is a common and aggressive type of skin cancer with rising incidence rate globally. Gender is one of the determining factors, and overall males have a higher risk of developing melanoma as well as worse prognosis. Emerging evidence show that GPR68, a G protein-coupled receptor that is sensitive to acid and mechanical stimulations for cellular microenvironment, plays an important role in tumor biology. However, whether GPR68 is involved in gender-dependent regulation of tumor growth is unclear. Methods: We established a syngeneic melanoma model in Gpr68-deficient mice and investigated tumor growth in males and females. The GPR68 activation-induced cellular responses of melanocytes, including intracellular calcium dynamics, proliferation and migration were measured. The landscape of tumor-infiltrating immune cells were analyzed by flow cytometry and the expression various cytokines were checked by qRT-PCR. Results: GPR68 is required for melanoma growth in males but dispensable in females. GPR68 is expressed and functional in B16-F10 melanocytes, but the activity of the receptor does not directly contribute to proliferation and migration of the cells. GPR68 inhibits infiltration of CD45+ lymphocytes, CD8+ T cells and NK cells in melanoma in male mice, but has no apparent effect in females. Furthermore, GPR68 functionally inhibits the expression of IFNγ in the tumor infiltrating CD8+ T cells and NK cells as well as the inflammatory cytokine expression in the spleen in male mice but not in females. Our results show the gender-dependent modulatory effect of GPR68 on tumor-infiltrating immune cells and their tumor-killing capacity. Discussion: GPR68 is sensor for acid and mechanical stimulations, which are two important factors in the microenvironment associated with tumor growth and metastasis. Our results suggest a prominent role of the receptor molecules in tumor biology in a gender-dependent manner. Since GPCRs are more feasible to develop small molecule drugs compared to transcription factors, our study demonstrates the potential of GPR68 as a novel druggable therapeutic target for melanoma in male patients.