RESUMEN
OBJECTIVE: We developed and validated a clinical-radiomics model for preoperative prediction of the short-term efficacy of initial drug-eluting beads transarterial chemoembolization (D-TACE) treatment in patients with hepatocellular carcinoma (HCC). METHODS: In this retrospective cohort study of 113 patients with intermediate and advanced HCC, 5343 features were extracted based on three sequences of the arterial phase (AP), diffusion-weighted imaging, and T2-weighted images based on contrast-enhanced magnetic resonance imaging, and minimum redundancy maximum correlation and least absolute shrinkage and selection operator (LASSO) regression were applied for feature selection and model construction. Multifactor logistic regression was used to build a clinical-imaging model based on clinical factors and a clinical-radiomics model. The area under the curve (AUC) and calibration curves were used to assess model performance, and the clinical value of the model was analyzed using decision curve analysis. The relationship between the actual and predicted short-term efficacy of the combined model and progression-free survival (PFS) was evaluated using Kaplan-Meier survival curves and log-rank tests. RESULTS: A total of 34 radiomics features were selected by LASSO, and the clinical-radiomics model had the best predictive performance (AUC = 0.902 and AUC = 0.845 for the training and testing sets, respectively), and the model based on AP had the best predictive performance among the four radiomics models (AUC = 0.89 for the training set and AUC = 0.85 for the testing set); the multifactorial logistic regression results showed that microsphere type (p = 0.042) and AP Rad-score (p = 0.01) were associated with short-term efficacy. In addition, a difference in PFS was observed in patients with HCC with different short-term efficacies predicted by the combined model. Moreover, prognosis was better in the objective versus non-objective response group. CONCLUSIONS: The combined clinical-radiomics model is an effective predictor of the short-term efficacy of initial D-TACE in patients with HCC, contributing to clinical and economic benefits for patients.
Asunto(s)
Carcinoma Hepatocelular , Quimioembolización Terapéutica , Medios de Contraste , Neoplasias Hepáticas , Imagen por Resonancia Magnética , Humanos , Carcinoma Hepatocelular/diagnóstico por imagen , Carcinoma Hepatocelular/terapia , Neoplasias Hepáticas/diagnóstico por imagen , Neoplasias Hepáticas/terapia , Quimioembolización Terapéutica/métodos , Femenino , Masculino , Estudios Retrospectivos , Persona de Mediana Edad , Imagen por Resonancia Magnética/métodos , Anciano , Resultado del Tratamiento , Valor Predictivo de las Pruebas , Adulto , Estudios de Cohortes , RadiómicaRESUMEN
PURPOSE: To develop thrombus radiomics models based on dual-energy CT (DECT) for predicting etiologic cause of stroke. METHODS: We retrospectively enrolled patients with occlusion of the middle cerebral artery who underwent computed tomography (NCCT) and DECT angiography (DECTA). 70 keV virtual monoenergetic images (simulate conventional 120kVp CTA images) and iodine overlay maps (IOM) were reconstructed for analysis. Five logistic regression radiomics models for predicting cardioembolism (CE) were built based on the features extracted from NCCT, CTA and IOM images. From these, the best one was selected to integrate with clinical information for further construction of the combined model. The performance of the different models was evaluated and compared using ROC curve analysis, clinical decision curves (DCA), calibration curves and Delong test. RESULTS: Among all the radiomic models, model NCCT+IOM performed the best, with AUC = 0.95 significantly higher than model NCCT, model CTA, model IOM and model NCCT+CTA in the training set (AUC = 0.88, 0.78, 0.90,0.87, respectively, P < 0.05), and AUC = 0.92 in the testing set, significantly higher than model CTA (AUC = 0.71, P < 0.05). Smoking and NIHSS score were independent predictors of CE (P < 0.05). The combined model performed similarly to the model NCCT+IOM, with no statistically significant difference in AUC either in the training or test sets. (0.96 vs. 0.95; 0.94 vs. 0.92, both P > 0.05). CONCLUSION: Radiomics models constructed based on NCCT and IOM images can effectively determine the source of thrombus in stroke without relying on clinical information.
RESUMEN
Well-orchestrated carbon nanostructure with superb stable framework and high surface accessibility is crucial for zinc-ion hybrid capacitors (ZIHCs). Herein, a hydrogen-bonded micelle self-assembly strategy is proposed for morphology-controllable synthesis of conjugated microporous polymers (CMPs) derived carbon to boost zinc ion storage capability. In the strategy, F127 micellar assembly through intermolecular hydrogen bonds serves as structure-directed agents, directing CMPs' oligomers grow into nanospherical assembly. The nanospherical carbon frameworks derived from CMPs (CNS-2) have shown maximized surface accessibility due to their plentiful tunable porosity and hierarchical porous structure with abundant mesoporous interconnected channels, and superb stability originating from CMPs' robust framework, thus the CNS-2-based ZIHCs exhibit ultrahigh energy density of 163 Wh kg-1 and ultralong lifespan with 93 % capacity retention after 200, 000 cycles at 20 A g-1. Charged ion storage efficiency also lies in dual-ion alternate uptake of Zn2+ and CF3SO3- as well as chemical redox of Zn2+ with carbonyl/pyridine motifs forming O-Zn-N bonds. Maximized surface accessibility and dual-ion storage mechanism ensure excellent electrochemical performance. Thus, the hydrogen-bond-guide micelle self-assembly strategy has provided a facile way to design nanoarchitectures of CMPs derived carbon for advanced cathodes of ZIHCs.
RESUMEN
The direct construction of metal-free catalysts on conductive substrates for electrocatalytic organic hydrogenation reactions is significant but still unexplored. Here, learning from the homogeneous molecular catalysts, an organic molecular mimetic metal-free heterogeneous catalyst is designed and constructed in situ on a graphite flake electrode via a mild electrochemical oxidationâreduction relay strategy. The as-prepared -COOH- and -OH-functionalized metal-free catalyst exhibits an electrocatalytic alkyne semihydrogenation performance with a 72% Faradaic efficiency, 99% selectivity and 96% yield of the alkene product, which is comparable to that of noble metal catalysts. The removal of these oxygen-containing groups leads to negligible activity. The experimental and calculation results reveal that the origin of the high activity can be assigned to the -COOH and -OH groups on graphite. A flow electrolytic cell delivers ten grams of hydrogenated products with 81% Faradaic efficiency. This metal-free catalyst is also suitable for gas-phase acetylene semihydrogenation and other electrocatalytic hydrogenation reactions.
RESUMEN
Recently, aqueous Zn-X (X=S, Se, Te, I2, Br2) batteries (ZXBs) have attracted extensive attention in large-scale energy storage techniques due to their ultrahigh theoretical capacity and environmental friendliness. To date, despite tremendous research efforts, achieving high energy density in ZXBs remains challenging and requires a synergy of multiple factors including cathode materials, reaction mechanisms, electrodes and electrolytes. In this review, we comprehensively summarize the various reaction conversion mechanism of zinc-sulfur (Zn-S) batteries, zinc-selenium (Zn-Se) batteries, zinc-tellurium (Zn-Te) batteries, zinc-iodine (Zn-I2) batteries, and zinc-bromine (Zn-Br2) batteries, along with recent important progress in the design and electrolyte of advanced cathode (S, Se, Te, I2, Br2) materials. Additionally, we investigate the fundamental questions of ZXBs and highlight the correlation between electrolyte design and battery performance. This review will stimulate an in-deep understanding of ZXBs and guide the design of conversion batteries.
RESUMEN
In this paper, we study the problem of 3D object segmentation from raw point clouds. Unlike existing methods which usually require a large amount of human annotations for full supervision, we propose the first unsupervised method, called OGC, to simultaneously identify multiple 3D objects in a single forward pass, without needing any type of human annotations. The key to our approach is to fully leverage the dynamic motion patterns over sequential point clouds as supervision signals to automatically discover rigid objects. Our method consists of three major components, 1) the object segmentation network to directly estimate multi-object masks from a single point cloud frame,2)the auxiliary self-supervised scene flow estimator,and 3)our core object geometry consistency component. By carefully designing a series of loss functions, we effectively take into account the multi-object rigid consistency and the object shape invariance in both temporal and spatial scales. This allows our method to truly discover the object geometry even in the absence of annotations. We extensively evaluate our method on five datasets, demonstrating the superior performance for object part instance segmentation and general object segmentation in both indoor and the challenging outdoor scenarios. Our code and data are available at https://github.com/vLAR-group/OGC.
RESUMEN
Capacitive carbon cathodes deliver great potential for zinc-ion hybrid capacitors (ZHCs) due to their resource abundance and structural versatility. However, the dimension mismatch between the micropores of carbons and hydrated Zn2+ ions often results in unsatisfactory charge storage capability. Here well-arranged heterodiatomic carbon superstructures are reported with compatible pore dimensions for activating Zn2+ ions, initiated by the supramolecular self-assembly of 1,3,5-triazine-2,4,6-triamine and cyanuric acid via in-plane hydrogen-bonds and out-of-plane π-π interactions. Flower-shaped carbon superstructures expose more surface-active motifs, continuous charge-transport routes, and more importantly, well-developed pores. The primary subnanopores of 0.82 nm are size-exclusively accessible for solvated Zn2+ ions (0.86 nm) to maximize spatial charge storage, while rich mesopores (1-3 nm) allow for high-kinetics ion migration with a low activation energy. Such favorable superstructure cathodes contribute to all-round performance improvement for ZHCs, including high energy density (158 Wh kg-1), fast-charging ability (50 A g-1), and excellent cyclic lifespan (100 000 cycles). An anion-cation hybrid charge storage mechanism is elucidated for superstructure cathode, which entails alternate physical uptake of Zn2+/CF3SO3 - at electroactive pores and bipedal chemical binding of Zn2+ to electronegative carbonyl/pyridine motifs. This work expands the design landscape of carbon superstructures for advanced energy storage.
RESUMEN
Zinc-organic batteries (ZOBs) are receiving widespread attention as up-and-coming energy-storage systems due to their sustainability, operational safety and low cost. Charge carrier is one of the critical factors affecting the redox kinetics and electrochemical performances of ZOBs. Compared with conventional large-sized and sluggish Zn2+ storage, non-metallic charge carriers with small hydrated size and light weight show accelerated interfacial dehydration and fast reaction kinetics, enabling superior electrochemical metrics for ZOBs. Thus, it is valuable and ongoing works to build better ZOBs with non-metallic ion storage. In this review, versatile non-metallic cationic (H+, NH4 +) and anionic (Cl-, OH-, CF3SO3 -, SO4 2-) charge carriers of ZOBs are first categorized with a brief comparison of their respective physicochemical properties and chemical interactions with redox-active organic materials. Furthermore, this work highlights the implementation effectiveness of non-metallic ions in ZOBs, giving insights into the impact of ion types on the metrics (capacity, rate capability, operation voltage, and cycle life) of organic cathodes. Finally, the challenges and perspectives of non-metal-ion-based ZOBs are outlined to guild the future development of next-generation energy communities.
RESUMEN
Background: Disorders associated with cognitive impairment impose a significant burden on both families and society. Previous studies have indicated that gait characteristics under dual-task as reliable markers of early cognitive impairment. Therefore, digital gait detection has great potential for future cognitive screening. However, research on digital biomarkers based on smart devices to identify cognitive impairment remains limited. The aim of this study is to explore digital gait biomarkers by utilizing intelligent wearable devices for discriminating mild cognitive impairment and dementia. Methods: This study included 122 subjects (age: 74.7 ± 7.7 years) diagnosed with normal cognition (NC, n = 38), mild cognitive impairment (MCI, n = 42), or dementia (n = 42). All subjects underwent comprehensive neuropsychological assessments and cranial Magnetic Resonance Imaging (MRI). Gait parameters were collected using validated wearable devices in both single-task and dual-task (DT). We analyzed the ability of gait variables to predict MCI and dementia, and examined the correlations between specific DT-gait parameters and sub-cognitive functions as well as hippocampal atrophy. Results: Our results demonstrated that dual-task could significantly improve the ability to predict cognitive impairment based on gait parameters such as gait speed (GS) and stride length (SL). Additionally, we discovered that turn velocity (TV and DT-TV) can be a valuable novel digital marker for predicting MCI and dementia, for identifying MCI (DT-TV: AUC = 0.801, sensitivity 0.738, specificity 0.842), and dementia (DT-TV: AUC = 0.923, sensitivity 0.857, specificity 0.842). The correlation analysis and linear regression analysis revealed a robust association between DT-TV and memory function, as well as the hippocampus atrophy. Conclusion: This study presents a novel finding that DT-TV could accurately identify varying degrees of cognitive impairment. DT-TV is strongly correlated with memory function and hippocampus shrinkage, suggests that it can accurately reflect changes in cognitive function. Therefore, DT-TV could serve as a novel and effective digital biomarker for discriminating cognitive impairment.
RESUMEN
Dendrite growth and parasitic reactions of a Zn metal anode in aqueous media hinder the development of up-and-coming Zn-ion batteries. Optimizing the crystal growth after Zn nucleation is promising to enable stable cyclic performance of the anode, but directly regulating specific crystal plane growth for homogenized Zn electrodeposition remains highly challenging. Herein, a perfluoropolymer (Nafion) is introduced into an aqueous electrolyte to activate a thermodynamically ultrastable Zn/electrolyte interface for long-term Zn-ion batteries. The low adsorption energy (-2.09 eV) of Nafion molecules on Zn metal ensures the in situ formation of a Nafion-nanofilm during the first charge process. This ultrathin artificial solid electrolyte interface with zincophilic -SO3- groups guides the directional Zn2+ electrodeposition along the (002) crystal surface even at high current density, yielding a dendrite-free Zn anode. The synergic Zn/electrolyte interphase electrochemistry contributes an average coulombic efficiency of 99.71% after 4500 cycles for ZnâCu cells, and ZnâZn cells achieve an ultralong lifespan of over 7000 h at 5 mA cm-2. Besides, ZnâMnO2 cells operate well over 3000 cycles. Even at -40 °C, ZnâZn cells achieve stable Zn2+ plating/stripping for 1200 h.
RESUMEN
Background: The old adults have high incidence of cognitive impairment, especially in patients with cerebral small vessel disease (CSVD). Cognitive impairment is not easy to be detected in such populations. We aimed to develop clinical prediction models for different degrees of cognitive impairments in elderly CSVD patients based on conventional imaging and clinical data to determine the better indicators for assessing cognitive function in the CSVD elderly. Methods: 210 CSVD patients were screened out by the evaluation of Magnetic Resonance Imaging (MRI). Then, participants were divided into the following three groups according to the cognitive assessment results: control, mild cognitive impairment (MCI), and dementia groups. Clinical data were collected from all patients, including demographic data, biochemical indicators, carotid ultrasound, transcranial Doppler (TCD) indicators, and linear measurement parameters based on MRI. Results: Our results showed that the brain atrophy and vascular lesions developed progressive worsening with increased degree of cognitive impairment. Crouse score and Interuncal distance/Bitemporal distance (IUD/BTD) were independent risk factors for MCI in CSVD patients, and independent risk factors for dementia in CSVD were Crouse Score, the pulsatility index of the middle cerebral artery (MCAPI), IUD/BTD, and Sylvian fissure ratio (SFR). Overall, the parameters with high performance were the IUD/BTD (OR 2.28; 95% CI 1.26-4.10) and SFR (OR 3.28; 95% CI 1.54-6.91), and the AUC (area under the curve) in distinguishing between CSVD older adults with MCI and with dementia was 0.675 and 0.724, respectively. Linear brain measurement parameters had larger observed effect than other indexes to identify cognitive impairments in CSVD patients. Conclusion: This study shows that IUD/BTD and SFR are good predictors of cognitive impairments in CSVD elderly. Linear brain measurement showed a good predictive power for identifying MCI and dementia in elderly subjects with CSVD. Linear brain measurement could be a more suitable and novel method for screening cognitive impairment in aged CSVD patients in primary healthcare facilities, and worth further promotion among the rural population.
RESUMEN
Bipolar organics fuse the merits of n/p-type redox reactions for better Zn-organic batteries (ZOBs), but face the capacity plafond due to low density of active units and single-electron reactions. Here we report multielectron redox-bipolar tetranitroporphyrin (TNP) with quadruple two-electron-accepting n-type nitro motifs and dual-electron-donating p-type amine moieties towards high-capacity-voltage ZOBs. TNP cathode initiates high-kinetics, hybrid anion-cation 10e- charge storage involving four nitro sites coordinating with Zn2+ ions at low potential and two amine species coupling with SO4 2- ions at high potential. Consequently, Zn||TNP battery harvests high capacity (338â mAh g-1), boosted average voltage (1.08â V), and outstanding energy density (365â Wh kg-1 TNP). Moreover, the extended π-conjugated TNP macrocycle achieves anti-dissolution in electrolytes, prolonging the battery life to 50,000â cycles at 10â A g-1 with 71.6 % capacity retention. This work expands the chemical landscape of multielectron redox-bipolar organics for state-of-the-art ZOBs.
RESUMEN
Most navigation aids for visually impaired individuals require users to pay close attention and actively understand the instructions or feedback of guidance, which impose considerable cognitive loads in long-term usage. To tackle the issue, this study proposes a cognitive burden-free electronic travel aid for individuals with visual impairments. Utilizing human instinctive compliance in response to external force, we introduce the "Aerial Guide Dog", a helium balloon aerostat drone designed for indoor guidance, which leverages gentle tugs in real time for directional guidance, ensuring a seamless and intuitive guiding experience. The introduced Aerial Guide Dog has been evaluated in terms of directional guidance and path following in the pilot study, focusing on assessing its accuracy in orientation and the overall performance in navigation. Preliminary results show that the Aerial Guide Dog, utilizing Ultra-Wideband (UWB) spatial positioning and Measurement Unit (IMU) angle sensors, consistently maintained minimal deviation from the targeting direction and designated path, while imposing negligible cognitive burdens on users while completing the guidance tasks.
Asunto(s)
Aeronaves , Animales de Servicio , Animales , Perros , Humanos , Proyectos Piloto , Electrónica , CogniciónRESUMEN
Compared with Zn2+ storage, non-metallic charge carrier with small hydrated size and light weight shows fast dehydration and diffusion kinetics for Zn-organic batteries. Here we first report NH4 + /H+ co-storage in self-assembled organic superstructures (OSs) by intermolecular interactions of p-benzoquinone (BQ) and 2, 6-diaminoanthraquinone (DQ) polymer through H-bonding and π-π stacking. BQ-DQ OSs exhibit exposed quadruple-active carbonyl motifs and super electron delocalization routes, which are redox-exclusively coupled with high-kinetics NH4 + /H+ but exclude sluggish and rigid Zn2+ ions. A unique 4e- NH4 + /H+ co-coordination mechanism is unravelled, giving BQ-DQ cathode high capacity (299â mAh g-1 at 1â A g-1 ), large-current tolerance (100â A g-1 ) and ultralong life (50,000 cycles). This strategy further boosts the capacity to 358â mAh g-1 by modulating redox-active building units, giving new insights into ultra-fast and stable NH4 + /H+ storage in organic materials for better Zn batteries.
RESUMEN
BACKGROUND: How brain neural activity changes at multiple time points throughout the day and the neural mechanisms underlying time-dependent modulation of vigilance are less clear. PURPOSE: To explore the effect of circadian rhythms and homeostasis on brain neural activity and the potential neural basis of time-dependent modulation of vigilance. STUDY TYPE: Prospective. SUBJECTS: A total of 30 healthy participants (22-27 years old). FIELD STRENGTH/SEQUENCE: A 3.0 T, T1-weighted imaging, echo-planar functional MRI (fMRI). ASSESSMENT: Six resting-state fMRI (rs-fMRI) scanning sessions were performed at fixed times (9:00 h, 13:00 h, 17:00 h, 21:00 h, 1:00 h, and 5:00 h) to investigate fractional amplitude of low-frequency fluctuation (fALFF) and regional homogeneity (ReHo) diurnal variation. The fALFF/ReHo and the result of the psychomotor vigilance task were used to assess local neural activity and vigilance. STATISTICAL TESTS: One-way repeated measures analysis of variance (ANOVA) was used to assess changes in vigilance (P < 0.05) and neural activity in the whole brain (P < 0.001 at the voxel level and P < 0.01 at the cluster level, Gaussian random field [GRF] corrected). Correlation analysis was used to examine the relationship between neural activity and vigilance at all-time points of the day. RESULTS: The fALFF/ReHo in the thalamus and some perceptual cortices tended to increase from 9:00 h to 13:00 h and from 21:00 h to 5:00 h, whereas the key nodes of the default mode network (DMN) tended to decrease from 21:00 h to 5:00 h. The vigilance tended to decrease from 21:00 h to 5:00 h. The fALFF/ReHo in the thalamus and some perceptual cortices was negatively correlated with vigilance at all-time points of the day, whereas the fALFF/ReHo in the key nodes of the DMN was positively correlated with vigilance. DATA CONCLUSION: Neural activities in the thalamus and some perceptual cortices show similar trends throughout the day, whereas the key nodes of the DMN show roughly opposite trends. Notably, diurnal variation of the neural activity in these brain regions may be an adaptive or compensatory response to changes in vigilance. EVIDENCE LEVEL: 1. TECHNICAL EFFICACY: 1.
Asunto(s)
Encéfalo , Imagen por Resonancia Magnética , Humanos , Adulto Joven , Adulto , Imagen por Resonancia Magnética/métodos , Estudios Prospectivos , Mapeo Encefálico/métodos , HomeostasisRESUMEN
Understanding the self-stacking interactions in precursors can facilitate the preparation of high-performance carbon materials and promote the commercial application of zinc ion hybrid capacitors (ZIHCs). Here, a π-conjugated molecule mediated pyrolysis strategy is presented to prepare carbon materials. Taking intermolecular force simulation (reduced density gradient plots) as a guide, the relationship between the self-stacking interactions in π-conjugated molecules and the structural parameters of carbon materials can be extrapolated. The resultant self-doped hierarchical porous carbons (NHPCs) derived from 1, 8, 4, 5-naphthalenetetracarboxdiimide with suitable self-stacking interactions empower the highest specific surface areas (2038 m2/g) and surface opening macropores. The NHPCs-based ZIHCs deliver a high capacity of 220 mAh/g, a high energy density of 149.5 Wh kg-1 and a super-stable cycle lifespan with 93.2 % capacity retention after 200, 000 cycles. The excellent electrochemical performance roots in the superior hierarchical porous structure with surface opening macropores, which guarantees the structural stability of carbon cathodes upon repeated rounds. Meanwhile, the heteroatom doping further relieves the kinetics concern of Zn2+ uptake/removal to enhance O-Zn-N binding particularly at high discharge currents. Besides, the proton-assisted Zn2+ dual-ion storage mechanism plays an essential role in the energy storage process. This work demonstrates a facile synthesis method and advances the fundamental understanding of its dual-ion storage mechanism.
RESUMEN
With the continuous in-depth study of the interaction mechanism between viruses and hosts, the virus has become a promising tool in cancer treatment. In fact, many oncolytic viruses with selectivity and effectiveness have been used in cancer therapy. Human enterovirus is one of the most convenient sources to generate oncolytic viruses, however, the high seroprevalence of some enteroviruses limits its application which urges to exploit more oncolytic enteroviruses. In this study, coxsackievirus B5/Faulkner (CV-B5/F) was screened for its potential oncolytic effect against non-small cell lung cancers (NSCLCs) through inducing apoptosis and autophagy. For refractory NSCLCs, DNA-dependent protein kinase (DNA-PK) or ataxia telangiectasia mutated protein (ATM) inhibitors can synergize with CV-B5/F to promote refractory cell death. Here, we showed that viral infection triggered endoplasmic reticulum (ER) stress-related pro-apoptosis and autophagy signals, whereas repair for double-stranded DNA breaks (DSBs) contributed to cell survival which can be antagonized by inhibitor-induced cell death, manifesting exacerbated DSBs, apoptosis, and autophagy. Mechanistically, PERK pathway was activated by the combination of CV-B5/F and inhibitor, and the irreversible ER stress-induced exacerbated cell death. Furthermore, the degradation of activated STING by ERphagy promoted viral replication. Meanwhile, no treatment-related deaths due to CV-B5/F and/or inhibitors occurred. Conclusively, our study identifies an oncolytic CV-B5/F and the synergistic effects of inhibitors of DNA-PK or ATM, which is a potential therapy for NSCLCs.
Asunto(s)
Carcinoma de Pulmón de Células no Pequeñas , Neoplasias Pulmonares , Virus Oncolíticos , Humanos , Carcinoma de Pulmón de Células no Pequeñas/genética , Carcinoma de Pulmón de Células no Pequeñas/terapia , Estudios Seroepidemiológicos , Neoplasias Pulmonares/genética , Neoplasias Pulmonares/terapia , Apoptosis/genética , Virus Oncolíticos/genética , ADNRESUMEN
Designing zincophilic and stable carbon nanostructures is critical for Zn-ion storage with superior capacitive activity and durability. Here, we report solvent-guided Lewis acid-base self-assembly to customize heterodiatomic carbon nanotubes, triggered by the reaction between iron chloride and α,α'-dichloro-p-xylene. In this strategy, modulating the solvent-precursor interaction through the optimization of solvent formula stimulates differential thermodynamic solubilization, growth kinetics, and self-assembly behaviors of Lewis polymeric chains, thereby accurately tailoring carbon nanoarchitectures to evoke superior Zn-ion storage. Featured with open hollow interiors and porous tubular topologies, the solvent-optimized carbon nanotubes allow low ion-migration barriers to deeply access the built-in zincophilic sites by high-kinetics physical Zn2+/CF3SO3- adsorption and robust chemical Zn2+ redox with pyridine/carbonyl motifs, which maximizes the spatial capacitive charge storage density. Thus, as-designed heterodiatomic carbon nanotube cathodes provide all-round improvement in Zn-ion storage, including a high energy density (140 W h kg-1), a large current activity (100 A g-1), and an exceptional long-term cyclability (100,000 cycles at 50 A g-1). This study provides appealing insights into the solvent-mediated Lewis pair self-assembly design of nanostructured carbons toward advanced Zn-ion energy storage.
RESUMEN
Organic small molecules as high-capacity cathodes for Zn-organic batteries have inspired numerous interests, but are trapped by their easy-dissolution in electrolytes. Here we knit ultrastable lock-and-key hydrogen-bonding networks between 2, 7-dinitropyrene-4, 5, 9, 10-tetraone (DNPT) and NH4 + charge carrier. DNPT with octuple-active carbonyl/nitro centers (H-bond acceptor) are redox-exclusively accessible for flexible tetrahedral NH4 + ions (H-bond donator) but exclude larger and rigid Zn2+ , due to a lower activation energy (0.14 vs. 0.31â eV). NH4 + coordinated H-bonding chemistry conquers the stability barrier of DNPT in electrolyte, and gives fast diffusion kinetics of non-metallic charge carrier. A stable two-step 4e- NH4 + coordination with DNPT cathode harvests a high capacity (320â mAh g-1 ), a high-rate capability (50â A g-1 ) and an ultralong life (60,000 cycles). This finding points to a new paradigm for H-bond stabilized organic small molecules to design advanced zinc batteries.
RESUMEN
This study addresses the challenges faced by individuals with upper limb disadvantages in operating power wheelchair joysticks by utilizing the extended Function-Behavior-Structure (FBS) model to identify design requirements for an alternative wheelchair control system. A gaze-controlled wheelchair system is proposed based on design requirements from the extended FBS model and prioritized using the MosCow method. This innovative system relies on the user's natural gaze and comprises three levels: perception, decision making, and execution. The perception layer senses and acquires information from the environment, including user eye movements and driving context. The decision-making layer processes this information to determine the user's intended direction, while the execution layer controls the wheelchair's movement accordingly. The system's effectiveness was validated through indoor field testing, with an average driving drift of less than 20 cm for participates. Additionally, the user experience scale revealed overall positive user experiences and perceptions of the system's usability, ease of use, and satisfaction.