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1.
Adv Mater ; : e2404640, 2024 May 22.
Artigo em Inglês | MEDLINE | ID: mdl-38775475

RESUMO

Cathode materials of sodium-based batteries with high specific capacity and fast charge/discharge mode, as well as ultralong reversible cycles at wide applied temperatures, are essential for future development of advanced energy storage system. Developing transition metal selenides with intercalation features provides a new strategy for realizing the above cathode materials. Herein, we report a storage mechanism of sodium ion in hexagonal CuSe (h-CuSe) based on the DFT guidance. We reveal that the two-dimensional ion intercalation triggers localized redox reaction in the h-CuSe bulk phase, termed intercalation-induced localized conversion (ILC) mechanism, to stabilize the sodium storage structure by forming localized Cu7Se4 transition phase and adjusting the near-edge coordination state of the Cu sites to achieve high reversible capacity and ultra-long cycling life, while allowing rapid charge/discharge cycling over a wide temperature range. This article is protected by copyright. All rights reserved.

2.
Adv Mater ; : e2402245, 2024 Apr 14.
Artigo em Inglês | MEDLINE | ID: mdl-38615264

RESUMO

Zinc metal is an attractive anode material for rechargeable aqueous Zn-ion batteries (ZIBs). However, the dendrite growth, water-induced parasitic reactions, and freezing problem of aqueous electrolyte at low temperatures are the major roadblocks that hinder the widely commercialization of ZIBs. Herein, tetrahydrofuran (THF) is proposed as the electrolyte additive to improve the reversibility and stability of Zn anode. Theoretical calculation and experimental results reveal that the introduction of THF into the aqueous electrolyte can optimize the solvation structure which can effectively alleviate the H2O-induced side reactions and protect the Zn anode from corrosion. Moreover, THF can act as a hydrogen bond acceptor to interact with H2O, which can greatly reduce the activity of free H2O in electrolytes and improve the low-temperature electrochemical performance of Zn anode. As a result, the Zn anodes demonstrate high cyclic stability for 2800 h at 27 °C and over 4000 h at -10 °C at 1.0 mA cm-2 /1.0 mAh cm-2. The full cell exhibits excellent cyclic stability and rate capability at 27 and -10 °C. This work is expected to provide a new approach to regulate the aqueous electrolyte and Zn anode interface chemistry for highly stable and reversible Zn anodes.

3.
Nat Commun ; 15(1): 1634, 2024 Feb 23.
Artigo em Inglês | MEDLINE | ID: mdl-38395918

RESUMO

Lithium- and manganese-rich layered oxide cathode materials have attracted extensive interest because of their high energy density. However, the rapid capacity fading and serve voltage decay over cycling make the waste management and recycling of key components indispensable. Herein, we report a facile concentrated solar radiation strategy for the direct recycling of Lithium- and manganese-rich cathodes, which enables the recovery of capacity and effectively improves its electrochemical stability. The phase change from layered to spinel on the particle surface and metastable state structure of cycled material provides the precondition for photocatalytic reaction and thermal reconstruction during concentrated solar radiation processing. The inducement of partial inverse spinel phase is identified after concentrated solar radiation treatment, which strongly enhances the redox activity of transition metal cations and oxygen anion, and reversibility of lattice structure. This study sheds new light on the reparation of spent cathode materials and designing high-performance compositions to mitigate structural degradation.

4.
Adv Mater ; 36(16): e2312924, 2024 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-38180113

RESUMO

Zn metal, as one of the most promising anode materials for aqueous batteries, suffers from uncontrollable dendrite growth and water-induced parasitic reactions, which drastically compromise its cycle life and Coulombic efficiency (CE). Herein, a nonionic amphipathic additive Tween-20 (TW20) is proposed that bears both zincophilic and hydrophobic units. The zincophilic segment of TW20 preferentially adsorbs on the Zn anode, while the hydrophobic segment is exposed on the electrolyte side, forming an electrolyte-facing hydrophobic layer that shields the anode from active water molecules. Moreover, theoretical calculation and experimental results reveal that the TW20 additive can induce the preferential growth of (002) plane by adsorbing on other facets, enabling dendrite-free Zn anodes. Benefitting from these advantages, the stability and reversibility of Zn anodes are substantially improved, reflected by stable cycling for over 2500 h at 1.0 mA cm-2/1.0 mAh cm-2 and 500 h at 5 mA cm-2/5 mAh cm-2 as well as an average CE of 99.4% at 1.0 mA cm-2/1.0 mAh cm-2. The full cells paired with MnO2 demonstrate a long lifespan for more than 700 cycles at 500 mA g-1. This work is expected to provide a new approach to modulate Zn electrode interface chemistry for highly stable Zn anodes.

5.
Biomed Pharmacother ; 168: 115692, 2023 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-37844357

RESUMO

Hepatocytes, the predominant cellular constituents of the liver, exhibit the highest mitochondrial density within the human body. Remarkably, experimental insights from the latter part of the previous century involving extracellular injection of mitochondrial DNA (mtDNA) elucidated its potential to incite autoimmune disorders. Consequently, in instances of liver injury, the substantial release of mtDNA has the potential to trigger the activation of the innate immune response, thereby inducing sustained pathogenic consequences within the organism. This article provides a comprehensive retrospective analysis of recent literature pertaining to the impact of mtDNA release on various hepatic cell populations, elucidating its role and potential mechanisms in liver injury. The findings underscore the central role of mtDNA in modulating the immune system, primarily through the orchestration of a cytokine storm, further exacerbating the occurrence of liver injury.


Assuntos
DNA Mitocondrial , Fígado , Humanos , DNA Mitocondrial/genética , DNA Mitocondrial/metabolismo , Estudos Retrospectivos , Fígado/patologia , Hepatócitos/metabolismo , Mitocôndrias/fisiologia
6.
Small Methods ; 7(11): e2300662, 2023 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-37526329

RESUMO

Lithium-sulfur (Li-S) batteries are considered as one of the top competitors to go beyond Li-ion batteries. However, the shuttle effect triggered by soluble lithium polysulfides (LPSs) brings great troubles for understanding the solid-liquid-solid conversion process of the sulfur cathode. Herein, a new characterization technique is developed to deepen the understanding of such soluble LPSs shuttling, by integrating an electron-conductive interlayer. The voltage of the interlayer exhibits a voltage-adaptive effect to the cathode, indicating the true dependence of the open-circuit voltages on the LPSs instead of on the solid cathodes. Furthermore, a quantitative method can be introduced to monitor the shuttling LPSs by such interlayer design, and it shows great potential to be a new standard technique, providing direct comparison of the shuttle effect between different studies. The newly developed interlayer design paves an avenue to gain new insight into the reaction process and improve the performance of Li-S batteries.

7.
Angew Chem Int Ed Engl ; 62(35): e202307212, 2023 Aug 28.
Artigo em Inglês | MEDLINE | ID: mdl-37407432

RESUMO

Aqueous electrolytes typically suffer from poor electrochemical stability; however, eutectic aqueous solutions-25 wt.% LiCl and 62 wt.% H3 PO4 -cooled to -78 °C exhibit a significantly widened stability window. Integrated experimental and simulation results reveal that, upon cooling, Li+ ions become less hydrated and pair up with Cl- , ice-like water clusters form, and H⋅⋅⋅Cl- bonding strengthens. Surprisingly, this low-temperature solvation structure does not strengthen water molecules' O-H bond, bucking the conventional wisdom that increasing water's stability requires stiffening the O-H covalent bond. We propose a more general mechanism for water's low temperature inertness in the electrolyte: less favorable solvation of OH- and H+ , the byproducts of hydrogen and oxygen evolution reactions. To showcase this stability, we demonstrate an aqueous Li-ion battery using LiMn2 O4 cathode and CuSe anode with a high energy density of 109 Wh/kg. These results highlight the potential of aqueous batteries for polar and extraterrestrial missions.

8.
Adv Mater ; 35(41): e2304022, 2023 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-37358536

RESUMO

Electrochemical oxygen evolution reaction (OER) kinetics are heavily correlated with hybridization of the transition metal d-orbital and oxygen intermediate p-orbital, which dictates the barriers of intermediate adsorption/desorption on the active sites of catalysts. Herein, a strategy is developed involving strain engineering and coordination regulation to enhance the hybridization of Ni 3d and O 2p orbitals, and the as-synthesized Ni-2,6-naphthalenedicarboxylic acid metal-organic framework (DD-Ni-NDA) nanosheets deliver a low OER overpotential of 260 mV to reach 10 mA cm-2 . By integrating an alkaline anion exchange membrane electrolyzer and Pt/C electrode, 200 and 500 mA cm-2 current densities are reached with cell voltages of 1.6 and 2.1 V, respectively. When loaded on a BiVO4 photoanode, the nanosheet enables highly active solar-driven water oxygen. Structural characterizations together with theoretical calculations reveal that the spin state of the centre Ni atoms is regulated by the tensile strain and unsaturated coordination defects in DD-Ni-NDA, and such spin regulation facilitates spin-dependent charge transfer of the OER. Molecular orbital hybridization analysis reveals the mechanism of OH* and OOH* adsorption energy regulation by changes in the DD-Ni-NDA spin state, which provides a deeper understanding of the electronic structure design of catalysts for the OER.

9.
J Opt Soc Am A Opt Image Sci Vis ; 39(12): 2257-2270, 2022 Dec 01.
Artigo em Inglês | MEDLINE | ID: mdl-36520746

RESUMO

Infrared and visible image fusion aims to reconstruct fused images with comprehensive visual information by merging the complementary features of source images captured by different imaging sensors. This technology has been widely used in civil and military fields, such as urban security monitoring, remote sensing measurement, and battlefield reconnaissance. However, the existing methods still suffer from the preset fusion strategies that cannot be adjustable to different fusion demands and the loss of information during the feature propagation process, thereby leading to the poor generalization ability and limited fusion performance. Therefore, we propose an unsupervised end-to-end network with learnable fusion strategy for infrared and visible image fusion in this paper. The presented network mainly consists of three parts, including the feature extraction module, the fusion strategy module, and the image reconstruction module. First, in order to preserve more information during the process of feature propagation, dense connections and residual connections are applied to the feature extraction module and the image reconstruction module, respectively. Second, a new convolutional neural network is designed to adaptively learn the fusion strategy, which is able to enhance the generalization ability of our algorithm. Third, due to the lack of ground truth in fusion tasks, a loss function that consists of saliency loss and detail loss is exploited to guide the training direction and balance the retention of different types of information. Finally, the experimental results verify that the proposed algorithm delivers competitive performance when compared with several state-of-the-art algorithms in terms of both subjective and objective evaluations. Our codes are available at https://github.com/MinjieWan/Unsupervised-end-to-end-infrared-and-visible-image-fusion-network-using-learnable-fusion-strategy.


Assuntos
Algoritmos , Processamento de Imagem Assistida por Computador , Redes Neurais de Computação
10.
Front Psychol ; 13: 926301, 2022.
Artigo em Inglês | MEDLINE | ID: mdl-35910953

RESUMO

The increase in emotional consumption reflects the increased emotional appeal of people in modern life. As a place for people's daily life and consumption, the indoor environment has been regarded as a symbol of quality of life and esthetic taste. The purpose of this paper is to study how to analyze and study the color factor and space humanization in interior design based on emotional needs, and describe the neural network. This paper puts forward the problem of emotional needs, which is based on the neural network model, and then elaborates on its concept and related algorithms, and designs and analyzes the case design and analysis of the humanized design of interior color and space based on emotional needs. The experimental results show that in the evaluation of the emotional needs of indoor environment users, the emotional needs of users for the three levels are all above 3.00. Users have the highest emotional needs at the usage level, reaching 4.24. It shows that users pay more attention to the practical value of the indoor environment, and hope to obtain a pleasant emotional experience by meeting the needs of practical value.

11.
Front Psychol ; 13: 941196, 2022.
Artigo em Inglês | MEDLINE | ID: mdl-35967610

RESUMO

Sensation (the reflection of past experience in the mind) is the reflection of the brain on the individual attributes of objective things that directly act on the sense organs. Feeling is the most elementary cognitive process and the simplest psychological phenomenon. Vision is a kind of sense, and sense is produced by objective things acting on the sense organs. But at present, it is rare to analyze interior design exhibition from the perspective of visual psychology, an emerging science, as an interdisciplinary attempt, only in interior design research. Therefore, the study of sensory process should start from its external stimuli, in order to first understand how it acts on the sensory organs to produce sensory phenomena. This paper mainly studies the visual performance of psychological factors in interior design under the background of artificial intelligence. This paper proposes a K-means clustering algorithm and a localization algorithm fused with visual and inertial navigation. The distance thresholds corresponding to the SIFT feature descriptors of threshold T1, 128D, 96D, 64D, and 32D are 170, 160, 150, and 90, respectively. This verifies that the candidate image with the highest number of matching points is considered the best matching image.

12.
Adv Mater ; 34(5): e2106876, 2022 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-34648671

RESUMO

Potassium-ion batteries (KIBs) have attracted wide interest for energy storage because of the abundance of the electrode materials involved; however, their electrochemical performances are far behind what can be achieved from lithium-ion batteries (LIBs) or sodium-ion batteries (SIBs). Herein, key promising electrode and electrolyte materials for potassium-ion batteries are identified, the coupled electrochemical reactions in the cell are investigated, and the compatibility between different materials is demonstrated to play the most important role. K2 Mn[Fe(CN)6 ] cathode can deliver a high capacity of ≈125 mAh g-1 and exceptional cycling stability over 61 000 cycles (≈9 months) if the side reactions from the anode can be prevented. Graphite is a good anode material but is subjected to degradation in traditional carbonate electrolytes. New concentrated electrolytes are developed and evaluated. A stable KIB system is demonstrated by coupling a stable K2 Mn[Fe(CN)6 ] cathode, a prepotassiated graphite anode with a concentrated electrolyte to achieve a high energy density of ≈260 Wh kg-1 (based on the active mass of cathode and anode) and good cycling of over 1000 cycles.

13.
Adv Mater ; 33(49): e2105234, 2021 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-34623704

RESUMO

Iron ion batteries using Fe2+ as a charge carrier have yet to be widely explored, and they lack high-performing Fe2+ hosting cathode materials to couple with the iron metal anode. Here, it is demonstrated that VOPO4 ∙2H2 O can reversibly host Fe2+ with a high specific capacity of 100 mAh g-1 and stable cycling performance, where 68% of the initial capacity is retained over 800 cycles. In sharp contrast, VOPO4 ∙2H2 O's capacity of hosting Zn2+ fades precipitously over tens of cycles. VOPO4 ∙2H2 O stores Fe2+ with a unique mechanism, where upon contacting the electrolyte by the VOPO4 ∙2H2 O electrode, Fe2+ ions from the electrolyte get oxidized to Fe3+ ions that are inserted and trapped in the VOPO4 ∙2H2 O structure in an electroless redox reaction. The trapped Fe3+ ions, thus, bolt the layered structure of VOPO4 ∙2H2 O, which prevents it from dissolution into the electrolyte during (de)insertion of Fe2+ . The findings offer a new strategy to use a redox-active ion charge carrier to stabilize the layered electrode materials.

14.
Chem Commun (Camb) ; 57(77): 9918-9921, 2021 Sep 28.
Artigo em Inglês | MEDLINE | ID: mdl-34498654

RESUMO

We demonstrate a disposable aqueous primary battery chemistry that comprises environmentally benign materials of the sulfur cathode and Zn anode in a 1 M ZnCl2 aqueous electrolyte. The Zn-S battery shows a high energy density of 1083.3 Wh kg-1 for sulphur with a flat discharge voltage plateau around 0.7 V. When operating at a high mass loading of 8.3 mg cm-2 for sulfur in the cathode, the battery exhibits a very high areal capacity of 11.4 mA h cm-2 and areal energy of 7.7 mW h cm-2.

15.
Chem Commun (Camb) ; 57(82): 10703-10706, 2021 Oct 14.
Artigo em Inglês | MEDLINE | ID: mdl-34545386

RESUMO

Using elemental selenium as an electrode, the redox-active Cu2+/Cu+ ion is reversibly hosted via the sequential conversion reactions of Se → CuSe → Cu3Se2 → Cu2Se. The four-electron redox process from Se to Cu2Se produces a high initial specific capacity of 1233 mA h g-1 based on the mass of selenium alone or 472 mA h g-1 based on the mass of Cu2Se, the fully discharged product.

16.
ACS Appl Mater Interfaces ; 13(4): 5044-5051, 2021 Feb 03.
Artigo em Inglês | MEDLINE | ID: mdl-33464033

RESUMO

Metal-organic frameworks (MOFs) constructed with mixed ligands have shown great promise in the generation of materials with improved sorption, optical, and electronic properties. With an experimental, spectroscopic, and computational approach, herein, we investigated how the incorporation of different functionalized ligands within the structure of MIL-125-NH2 affects its performance in photocatalytic water reduction. We found that multiligand incorporation within the MOF structure has an impact on the light absorption spectrum and the electronic structure. These combined modifications improve the photocatalytic performance of MIL-125-NH2, thereby increasing the rate of hydrogen evolution reaction. Of the four nanoparticle/MOF photocatalytic systems tested, we showed that the Pt/MIL-125-NH2/(OH)2 system (Pt nanoparticle plus MIL-125-NH2 with amino and dihydroxyl functionalized ligands) outperforms its counterpart Pt/MIL-125-NH2 system, attributed to the enhanced p-π conjugation between the lone pairs of O atoms and their aromatic ligands resulting in a red-shifted absorption spectrum and greater spatial distribution of electron density.

17.
Angew Chem Int Ed Engl ; 59(49): 22007-22011, 2020 Dec 01.
Artigo em Inglês | MEDLINE | ID: mdl-32805079

RESUMO

A non-aqueous proton electrolyte is devised by dissolving H3 PO4 into acetonitrile. The electrolyte exhibits unique vibrational signatures from stimulated Raman spectroscopy. Such an electrolyte exhibits unique characteristics compared to aqueous acidic electrolytes: 1) higher (de)protonation potential for a lower desolvation energy of protons, 2) better cycling stability by dissolution suppression, and 3) higher Coulombic efficiency owing to the lack of oxygen evolution reaction. Two non-aqueous proton full cells exhibit better cycling stability, higher Coulombic efficiency, and less self-discharge compared to the aqueous counterpart.

18.
ACS Appl Mater Interfaces ; 12(8): 9201-9208, 2020 Feb 26.
Artigo em Inglês | MEDLINE | ID: mdl-32011119

RESUMO

Proton batteries are emerging as a promising solution for energy storage; however, their development has been hindered by the lack of suitable cathode materials. Herein, a hydrous Turnbull's blue analogue (TBA) of Ni[Fe(CN)6]2/3·4H2O has been investigated as a viable proton cathode. Particularly, it shows an extremely high rate performance up to 6000 C (390 A g-1) at room temperature and delivers good capacity values at a low temperature of -40 °C in an aqueous electrolyte. The excellent rate capability is also amenable to high mass loadings of 10 mg cm-2. Such fast and low-temperature rate behavior likely stems from the fast proton conduction that is afforded by the Grotthuss mechanism inside the TBA structure. Furthermore, advanced characterization, including in operando synchrotron X-ray diffraction (XRD), and X-ray absorption near-edge structure (XANES) were employed to understand the changes of crystal structures and the oxidation-states of metal elements of the electrodes.

19.
Angew Chem Int Ed Engl ; 58(36): 12640-12645, 2019 Sep 02.
Artigo em Inglês | MEDLINE | ID: mdl-31301101

RESUMO

The elemental sulfur electrode with Cu2+ as the charge carrier gives a four-electron sulfur electrode reaction through the sequential conversion of S↔CuS↔Cu2 S. The Cu-S redox-ion electrode delivers a high specific capacity of 3044 mAh g-1 based on the sulfur mass or 609 mAh g-1 based on the mass of Cu2 S, the completely discharged product, and displays an unprecedently high potential of sulfur/metal sulfide reduction at 0.5 V vs. SHE. The Cu-S electrode also exhibits an extremely low extent of polarization of 0.05 V and an outstanding cycle number of 1200 cycles retaining 72 % of the initial capacity at 12.5 A g-1 . The remarkable utility of this Cu-S cathode is further demonstrated in a hybrid cell that employs an Zn metal anode and an anion-exchange membrane as the separator, which yields an average cell discharge voltage of 1.15 V, the half-cell specific energy of 547 Wh kg-1 based on the mass of the Cu2 S/carbon composite cathode, and stable cycling over 110 cycles.

20.
J Am Chem Soc ; 141(15): 6338-6344, 2019 Apr 17.
Artigo em Inglês | MEDLINE | ID: mdl-30917652

RESUMO

Dual-ion batteries are known for anion storage in the cathode coupled to cation incorporation in the anode. We flip the sequence of the anion/cation-storage chemistries of the anode and the cathode in dual-ion batteries (DIBs) by allowing the anode to take in anions and a cation-deficient cathode to host cations, thus operating as a reverse dual-ion battery (RDIB). The anion-insertion anode is a nanocomposite having ferrocene encapsulated inside a microporous carbon, and the cathode is a Zn-insertion Prussian blue, Zn3[Fe(CN)6]2. This unique battery configuration benefits from the usage of a 30 m ZnCl2 "water-in-salt" electrolyte. This electrolyte minimizes the dissolution of ferrocene; it raises the cation-insertion potential in the cathode, and it depresses the anion-insertion potential in the anode, thus widening the full cell's voltage by 0.35 V compared with a dilute ZnCl2 electrolyte. RDIBs provide a configuration-based solution to exploit the practicality of cation-deficient cathode materials in aqueous electrolytes.

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