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1.
Small ; : e2400774, 2024 Apr 15.
Artigo em Inglês | MEDLINE | ID: mdl-38616778

RESUMO

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.

2.
J Magn Reson Imaging ; 59(1): 211-222, 2024 01.
Artigo em Inglês | MEDLINE | ID: mdl-37078514

RESUMO

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.


Assuntos
Encéfalo , Imageamento por Ressonância Magnética , Humanos , Adulto Jovem , Adulto , Imageamento por Ressonância Magnética/métodos , Estudos Prospectivos , Mapeamento Encefálico/métodos , Homeostase
3.
Sensors (Basel) ; 24(1)2024 Jan 04.
Artigo em Inglês | MEDLINE | ID: mdl-38203159

RESUMO

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.


Assuntos
Aeronaves , Animais de Trabalho , Animais , Cães , Humanos , Projetos Piloto , Eletrônica , Cognição
4.
Angew Chem Int Ed Engl ; 63(3): e202316835, 2024 Jan 15.
Artigo em Inglês | MEDLINE | ID: mdl-38010854

RESUMO

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 (299 mAh g-1 at 1 A g-1 ), large-current tolerance (100 A g-1 ) and ultralong life (50,000 cycles). This strategy further boosts the capacity to 358 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.

5.
Angew Chem Int Ed Engl ; 63(16): e202401049, 2024 Apr 15.
Artigo em Inglês | MEDLINE | ID: mdl-38372434

RESUMO

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 (338 mAh g-1), boosted average voltage (1.08 V), and outstanding energy density (365 Wh kg-1 TNP). Moreover, the extended π-conjugated TNP macrocycle achieves anti-dissolution in electrolytes, prolonging the battery life to 50,000 cycles at 10 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.

6.
Neuroradiology ; 65(5): 923-931, 2023 May.
Artigo em Inglês | MEDLINE | ID: mdl-36892613

RESUMO

PURPOSE: To explore the static and dynamic characteristics of intrinsic brain activity (IBA) in subcortical ischemic vascular disease (SIVD) patients with or without cognitive impairment. METHODS: In total, 90 participants were recruited, including 32 SIVD patients with cognitive impairment (SIVD-CI, N = 32), 26 SIVD patients with no cognitive impairment (SIVD-NCI, N = 26), and 32 healthy controls (HC, N = 32) matched for age, gender, and education. All subjects underwent resting-state functional magnetic resonance imaging (rs-fMRI) scanning and neuropsychological tests. Amplitude of low-frequency fluctuation (ALFF) was calculated to reflect static alterations of regional IBA. Sliding window analysis was conducted in order to explore the dynamic characteristics. RESULTS: Both SIVD-CI and SIVD-NCI group showed significantly decreased ALFF in left angular gyrus (ANG), whereas SIVD-CI group showed increased ALFF in right superior frontal gyrus (SFG), compared with HCs. Furthermore, SIVD-CI group showed significantly decreased ALFF dynamics (dALFF) in right precuneus (PreCu) and left dorsal anterior cingulate cortex (dACC), compared with HC and SIVD-NCI groups (Gaussian random field-corrected, voxel-level P < 0.001, cluster-level P < 0.05). No dynamic changes were detected between SIVD-NCI group and HC group. The mean ALFF value in left ANG of SIVD-CI group was correlated with the score of delayed memory scale. CONCLUSION: ANG may be a vulnerable brain region in SIVD patients. Temporal dynamic analysis could serve as a sensitive and promising method to investigate IBA alterations in SIVD patients.


Assuntos
Imageamento por Ressonância Magnética , Doenças Vasculares , Humanos , Imageamento por Ressonância Magnética/métodos , Encéfalo/diagnóstico por imagem , Mapeamento Encefálico/métodos , Giro do Cíngulo
7.
Sensors (Basel) ; 23(12)2023 Jun 14.
Artigo em Inglês | MEDLINE | ID: mdl-37420738

RESUMO

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.


Assuntos
Cadeiras de Rodas , Humanos , Movimentos Oculares , Extremidade Superior , Sensação , Desenho de Equipamento
8.
Angew Chem Int Ed Engl ; 62(38): e202309446, 2023 Sep 18.
Artigo em Inglês | MEDLINE | ID: mdl-37507839

RESUMO

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. 0.31 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 (320 mAh g-1 ), a high-rate capability (50 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.

9.
Angew Chem Int Ed Engl ; 62(13): e202219136, 2023 Mar 20.
Artigo em Inglês | MEDLINE | ID: mdl-36695445

RESUMO

With fast (de)coordination kinetics, the smallest and the lightest proton stands out as the most ideal charge carrier for aqueous Zn-organic batteries (ZOBs). Hydrogen-bonding networks with rapid Grotthuss proton conduction is particularly suitable for organic cathodes, yet not reported. We report the supramolecular self-assembly of cyanuric acid and 1,3,5-triazine-2,4,6-triamine into organic superstructures through in-plane H-bonds and out-of-plane π-π interaction. The supramolecular superstructures exhibit highly stable lock-and-key H-bonding networks with an ultralow activation energy for protonation (0.09 eV vs. 0.25 eV of zincification). Then, high-kinetics H+ coordination is prior to Zn2+ into protophilic C=O sites via a two-step nine-electron reaction. The assembled ZOBs show high-rate capability (135 mAh g-1 at 150 A g-1 ), high energy density (267 Wh kg-1 cathode ) and ultra-long life (50 000 cycles at 10 A g-1 ), becoming the state-of-the-art ZOBs in comprehensive performances.

10.
Angew Chem Int Ed Engl ; 61(35): e202208821, 2022 Aug 26.
Artigo em Inglês | MEDLINE | ID: mdl-35781762

RESUMO

Highly active and stable cathodes are critical for aqueous Zn-organic batteries with high capacity, fast redox kinetics, and long life. We herein report para-, meta-, and ortho-dinitrobenzene (p-, m-, and o-DB) containing two successive two-electron processes, as cathode materials to boost the battery performance. Theoretical and experimental studies reveal that nitro constitutional isomerism is key to zincophilic activity and redox kinetics. p-DB hosted in carbon nanoflower harvests a high capacity of 402 mAh g-1 and a superior stability up to 25 000 cycles at 5 A g-1 , giving a Zn-organic battery with a high energy density of 230 Wh kg-1 . An anionic co-insertion charge storage mechanism is proposed, entailing a two-step (de)coordination of Zn(CF3 SO3 )+ with nitro oxygen. Besides, dinitrobenzene can be electrochemically optimized by side group regulation via implanting electron-withdrawing motifs. This work opens a new window to design multielectron nitroaromatics for Zn-organic batteries.

11.
Artigo em Inglês | MEDLINE | ID: mdl-38843053

RESUMO

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.

12.
Adv Sci (Weinh) ; 11(19): e2310319, 2024 May.
Artigo em Inglês | MEDLINE | ID: mdl-38477446

RESUMO

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.

13.
Chem Sci ; 15(12): 4322-4330, 2024 Mar 20.
Artigo em Inglês | MEDLINE | ID: mdl-38516081

RESUMO

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 Zn‖Cu cells, and Zn‖Zn cells achieve an ultralong lifespan of over 7000 h at 5 mA cm-2. Besides, Zn‖MnO2 cells operate well over 3000 cycles. Even at -40 °C, Zn‖Zn cells achieve stable Zn2+ plating/stripping for 1200 h.

14.
ChemSusChem ; : e202400886, 2024 Jun 20.
Artigo em Inglês | MEDLINE | ID: mdl-38899510

RESUMO

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.

15.
Front Neurol ; 15: 1297076, 2024.
Artigo em Inglês | MEDLINE | ID: mdl-38318441

RESUMO

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.

16.
J Colloid Interface Sci ; 658: 856-864, 2024 Mar 15.
Artigo em Inglês | MEDLINE | ID: mdl-38157610

RESUMO

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.

17.
Front Aging Neurosci ; 16: 1304265, 2024.
Artigo em Inglês | MEDLINE | ID: mdl-38476660

RESUMO

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.

18.
ACS Appl Mater Interfaces ; 15(29): 35380-35390, 2023 Jul 26.
Artigo em Inglês | MEDLINE | ID: mdl-37440355

RESUMO

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.

19.
Huan Jing Ke Xue ; 44(2): 889-899, 2023 Feb 08.
Artigo em Zh | MEDLINE | ID: mdl-36775612

RESUMO

In order to clarify effect of magnetic biocarriers on the performance of MBBR at low temperatures, the microbial diversity, community structure, functional characteristics, and nitrogen metabolism of biofilm in the reaction system were investigated. The results indicated that MBBR with magnetic biocarriers had a better pollutant removal efficiency, with the average removal rates of NH4+-N and TN being 16.2% and 12.1% higher than those in the control group (commercial biocarriers), respectively. Illumina high-throughput sequencing analysis showed that higher diversity and richness of the bacterial community was established in the biofilm of magnetic biocarriers. There were obvious differences in microbial community structure of biofilm between the two biocarrier duos to bacterial magnetic susceptibility. The relative abundances of nitrifying bacteria (e.g., Nitrosomonas and Nitrospira) and denitrifying bacteria (e.g., Sphaerotilus and Zoogloea) were increased in the magnetic biocarriers. Functional prediction analysis with PICRUSt2 showed that the microorganism of magnetic biocarriers had a better total gene function expression level, which was significantly more increased than commercial biocarriers in gene-representing signal transduction mechanisms and intracellular trafficking, secretion, and vesicular transport. Furthermore, most of the abundances of nitrogen metabolism genes were raised in the biofilm of magnetic biocarriers (e.g., genes amo and hao, were responsible for nitrification, and genes nap and nor, which were responsible for denitrification). Magnetic biocarriers increased biofilm potential for denitrification at low temperatures. Our results explained the difference in performance between the two reactors from microbiology and provided the theoretical basis for magnetic biocarrier-enhanced performances of MBBR at low temperatures.


Assuntos
Biofilmes , Microbiota , Temperatura , Reatores Biológicos/microbiologia , Nitrogênio/análise , Nitrificação , Bactérias/genética , Bactérias/metabolismo , Fenômenos Magnéticos , Desnitrificação
20.
Nat Commun ; 14(1): 3057, 2023 May 26.
Artigo em Inglês | MEDLINE | ID: mdl-37236928

RESUMO

Cyclohexanone oxime, an important nylon-6 precursor, is conventionally synthesized through cyclohexanone-hydroxylamine (NH2OH) and cyclohexanone ammoxidation methodologies. These strategies require complicated procedures, high temperatures, noble metal catalysts, and toxic SO2 or H2O2 usage. Here, we report a one-step electrochemical strategy to synthesize cyclohexanone oxime from nitrite (NO2-) and cyclohexanone under ambient conditions using a low-cost Cu-S catalyst, avoiding complex procedures, noble metal catalysts and H2SO4/H2O2 usage. This strategy produces 92% yield and 99% selectivity of cyclohexanone oxime, comparable to the industrial route. The reaction undergoes a NO2- → NH2OH→oxime reaction pathway. This electrocatalytic strategy is suitable for the production of other oximes, highlighting the methodology universality. The amplified electrolysis experiment and techno-economic analysis confirm its practical potential. This study opens a mild, economical, and sustainable way for the alternative production of cyclohexanone oxime.

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