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1.
Small ; : e2400599, 2024 Jun 11.
Artigo em Inglês | MEDLINE | ID: mdl-38860549

RESUMO

Memristors are used in artificial neural networks owing to their exceptional integration capabilities and scalability. However, traditional memristors are hampered by limited resistance states and randomness, which curtails their application. The migration of metal ions critically influences the number of conductance states and the linearity of weight updates. Semi-metal filaments can provide subquantum conductance changes to the memristors due to the smaller single-atom conductance, such as Sb (≈0.01 G0 = 7.69 × 10-7 S). Here, a memristor featuring an active electrode composed of semi-metal Sb is introduced for the first time. This memristor demonstrates precise conductance control, a large on/off ratio, consistent switching, and prolonged retention exceeding 105 s. Density functional theory (DFT) calculations and characterization methods reveal the formation of Sb filaments during a set process. The interaction between Sb and O within the dielectric layer facilitates the Sb filaments' ability to preserve their morphology in the absence of electric fields.

2.
Small ; 20(2): e2304210, 2024 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-37626458

RESUMO

Due to their high designability, unique geometric and electronic structures, and surface coordination chemistry, atomically precise metal nanoclusters are an emerging class of functional nanomaterials at the forefront of materials research. However, the current research on metal nanoclusters is mainly fundamental, and their practical applications are still uncharted. The surface binding properties and redox activity of Au24 Pt(PET)18 (PET: phenylethanethiolate, SCH2 CH2 Ph) nanoclusters are herein harnessed as an high-efficiency electrocatalyst for the anchoring and rapid conversion of lithium polysulfides in lithium-sulfur batteries (LSBs). Au24 Pt(PET)18 @G composites are prepared by using the large specific surface area, high porosity, and conductive network of graphene (G) for the construction of battery separator that can inhibit polysulfide shuttle and accelerate electrochemical kinetics. Resultantly, the LSB using a Au24 Pt(PET)18 @G-based separator presents a high reversible specific capacity of 1535.4 mA h g-1 for the first cycle at 0.2 A g-1 and a rate capability of 887 mA h g-1 at 5 A g-1 . After 1000 cycles at 5 A g-1 , the capacity is 558.5 mA h g-1 . This study is a significant step toward the application of metal nanoclusters as optimal electrocatalysts for LSBs and other sustainable energy storage systems.

3.
Small ; 20(24): e2311180, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38174602

RESUMO

The practical application of the room-temperature sodium-sulfur (RT Na-S) batteries is currently limited by low reversible capacity and serious capacity decay due to the sluggish reaction kinetics and shuttle effect. It is necessary to design a suitable sulfur host integrated with electrocatalysts to realize effective chemisorption and catalysis of sodium polysulfides (NaPSs). Herein, under the guidance of theoretical calculation, the Mott-Schottky heterojunction with a built-in electric field composed of iron (Fe) and iron disulfide (FeS2) components anchored on a porous carbon matrix (Fe/FeS2-PC) is designed and prepared. The enhanced chemisorption effect of Fe, the fast electrocatalytic effect of FeS2, and the fast transfer effect of the built-in electric field within the Fe/FeS2 heterojunction in the cathode of RT Na-S batteries work together to effectively improve the electrochemical performance. As a result, the Fe/FeS2-PC@S cathode exhibits high reversible capacity (815 mAh g-1 after 150 cycles at 0.2 A g-1) and excellent stability (516 mAh g-1 after 600 cycles at 5 A g-1, with only 0.07% decay per cycle). The design of the Fe/FeS2 heterojunction electrocatalyst provides a new strategy for the development of highly stable RT Na-S batteries.

4.
Small ; 19(16): e2206083, 2023 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-36683234

RESUMO

The notorious shuttle effect and sluggish conversion of polysulfides seriously hinder the practical application of Lithium-sulfur (Li-S) batteries. In this study, a novel architecture of MoS2 /MoO3 heterostructure uniformly distributed on carbon nanotubes (MoS2 /MoO3 @CNT) is designed and introduced into Li-S batteries via decorating commercial separator to regulate the redox reactions of polysulfides. Systematic experiments and theoretical calculations showed that the heterostructure not only provides sufficient surface affinity to capture polysulfides and acts as an active catalyst to promote the conversion of polysulfides, but also the highly conductive CNT enables rapid electron/ion migration. As a result, Li-S batteries with the MoS2 /MoO3 @CNT-PP separator deliver an impressive reversible capacity (1015 mAh g-1 at 0.2 A g-1 after 100 cycles), excellent rate capacity (873 mAh g-1 at 5 A g-1 ), and low self-discharge capacity loss (94.6% capacity retention after 7 days of standing). Moreover, even at an elevated temperature of 70 °C, it still exhibits high-capacity retention (800 mAh g-1 at 1 A g-1 after 100 cycles). Encouragingly, when the sulfur load is increased to 8.7 mg cm-2 , the high reversible areal capacity of 6.61 mAh cm-2 can be stably maintained after 100 cycles, indicating a high potential for practical application.

5.
Small ; 18(50): e2205158, 2022 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-36310150

RESUMO

Although lithium-sulfur batteries (LSBs) promise high theoretical energy density and potential cost effectiveness, their applications are severely impeded by the shuttling and sluggish redox kinetics of lithium polysulfides (LiPSs). In this context, a Co9 S8 @MoS2 heterostructure is sophisticatedly designed as an efficient catalytic host to boost the sulfur reduction reaction/evolution reaction (SRR/SER) kinetics and suppresses the LiPSs shuttling in LSBs. The results indicate that the electronic structure is manipulated in the Co9 S8 @MoS2 heterostructure, where the built-in electric fields (BIEFs) within the heterointerfaces enable the sufficient adsorption sites to accelerate the ionic diffusion/charge transfer kinetics for LiPSs redox, thus enhancing the sulfur conversion. By tuning the electronic structure, the metal d-band of Co9 S8 @MoS2 heterostructure plays an important role in adsorbing and catalyzing the conversion of LiPSs, thus promoting the reaction kinetics of the corresponding LSBs. This work unlocks the potential of heterostructures as promising catalysts to the design of high-energy and stabilized LSBs.

6.
Appl Opt ; 61(7): 1726-1733, 2022 Mar 01.
Artigo em Inglês | MEDLINE | ID: mdl-35297850

RESUMO

Efficient light management is critical to obtain high performance for organic solar cells (OSCs), which aims to solve the contradiction between limited carrier extraction and light absorption for the normally employed photoactive layers generally having both short exciton diffusion lengths and low extinction coefficients. In this study, we introduce a simple and efficient light management structure consisting of a front indium tin oxide nanocylinder (ITO-NC) array and a back square Al array. Thanks to the synergetic effects of antireflection and light scattering induced by the ITO-NC array, together with the secondary scattering and localized surface plasmon resonance because of the square Al array, remarkably enhanced light absorption in a broad spectral range can be achieved. Taking the most investigated photoactive layer of the P3HT:PC61BM blend as an example, simulation results reveal that, compared with the planar control device of the ITO/PEDOT:PSS/P3HT:PC61BM(80nm)/ZnO/Al, the short-circuit current density and power conversion efficiency can be enhanced by 36.58% and 38.38% after incorporating the light management structure with the optimal structural parameters. Furthermore, good omnidirectional light management can be achieved for the proposed device structure. Given the excellent performance and simple structure, we believe that this study would provide a meaningful exploration of developing light management structures applicable for thin film-based optoelectronic devices.

7.
Sensors (Basel) ; 20(12)2020 Jun 19.
Artigo em Inglês | MEDLINE | ID: mdl-32575568

RESUMO

Acetone is a biomarker in the exhaled breath of diabetic patients; sensitive and selective detection of acetone in human exhaled breath plays an important role in noninvasive diagnosis. Tungsten oxide (especially for γ-WO3) is a promising material for the detection of breath acetone. It is generally believed that the stable metastable phase of WO3 (ε-WO3) is the main reason for the improved response to acetone detection. In this work, pure and Cr-doped urchin-like WO3 hollow spheres were synthesized by a facile hydrothermal approach. Analyses of the resulting materials via X-ray photoelectron spectroscopy (XPS) and Raman confirmed that they are mainly composed by γ-WO3. The gas sensing performances of pure and Cr-doped WO3 to acetone were systematically tested. Results show that the sensor based on pure WO3 annealed at 450 °C has a high response of 20.32 toward 100 ppm acetone at a working temperature of 250 °C. After doped with Cr, the response was increased 3.5 times higher than the pure WO3 sensor. The pure and Cr-doped WO3 sensors both exhibit a tiny response to other gases, low detection limits (ppb-level) and an excellent repeatability. The improvement of gas sensing properties could be attributed to an optimized morphology of Cr-doped WO3 by regulating the crystal growth and reducing the assembled nanowires' diameter. The increasing number of oxygen vacancy and the introduction of impurity energy level with trap effect after Cr doping would lead to the wider depletion layer as well as a better gas sensing performance. This work will contribute to the development of new WO3 acetone sensors with a novel morphology and will explain the increased response after Cr doping from a new perspective.

8.
Small ; 15(40): e1902363, 2019 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-31419025

RESUMO

Lithium-sulfur batteries (LSBs) have shown great potential for application in high-density energy storage systems. However, the performance of LSBs is hindered by the shuttle effect and sluggish reaction kinetics of lithium polysulfides (LiPSs). Herein, heterostructual Nb2 O5 nanocrystals/reduced graphene oxide (Nb2 O5 /RGO) composites are introduced into LSBs through separator modification for boosting the electrochemical performance. The Nb2 O5 /RGO heterostructures are designed as chemical trappers and conversion accelerators of LiPSs. Originating from the strong chemical interactions between Nb2 O5 and LiPSs as well as the superior catalytic nature of Nb2 O5 , the Nb2 O5 /RGO nanocomposite possesses high trapping efficiency and efficient electrocatalytic activity to long-chain LiPSs. The effective regulation of LiPSs conversion enables the LSBs enhanced redox kinetics and suppressed shuttle effect. Moreover, the Nb2 O5 /RGO nanocomposite has abundant sulfophilic sites and defective interfaces, which are beneficial for the nucleation and growth of Li2 S, as evidenced by analysis of the cycled separators. As a result, LSBs with the Nb2 O5 /RGO-modified separators exhibit excellent rate capability (816 mAh g-1 at 3 A g-1 ) and cyclic performance (628 mAh g-1 after 500 cycles). Remarkably, high specific capacity and stable cycling performance are demonstrated even at an elevated temperature of 50 °C or with higher sulfur loadings.

9.
Small ; : e1801836, 2018 Jul 03.
Artigo em Inglês | MEDLINE | ID: mdl-29971944

RESUMO

Dual carbon-based potassium dual ion batteries (K-DCBs) have recently attracted ever-increasing attention owing to the potential advantages of high performance-to-cost ratio, good safety, and environmental friendliness. However, the reported K-DCBs still cannot simultaneously meet the requirements of high capacity, long cycling stability, and low cost, which are necessary for practical applications. In this study, a K-DCB with good comprehensive performance including capacity, cycling stability, medium discharge voltage, and energy density is developed by introducing the optimal cathode and anode materials, i.e., KS6 and natural graphite, respectively. An initial capacity of ≈54.6 mAh g-1 and 92.5% capacity retention after 400 cycles can be delivered in a wide voltage window of 2.4-5.4 V at the current density of 100 mA g-1 . A high medium discharge voltage around 4.2 V and an energy density up to 158.3 Wh kg-1 are meanwhile delivered by the K-DCB. In addition, the working mechanism of the devices is understood in detail. It is believed that valuable contributions to the electrochemical performance improvement of the related devices toward practical applications can be provided by this study.

10.
Small ; 13(45)2017 12.
Artigo em Inglês | MEDLINE | ID: mdl-29024532

RESUMO

To satisfy the increasing energy demands of portable electronics, electric vehicles, and miniaturized energy storage devices, improvements to lithium-ion batteries (LIBs) are required to provide higher energy/power densities and longer cycle lives. Group IVA element (Si, Ge, Sn)-based alloying/dealloying anodes are promising candidates for use as electrodes in next-generation LIBs owing to their extremely high gravimetric and volumetric capacities, low working voltages, and natural abundances. However, due to the violent volume changes that occur during lithium-ion insertion/extraction and the formation of an unstable solid electrolyte interface, the use of Group IVA element-based anodes in commercial LIBs is still a great challenge. Evaluating the electrochemical performance of an anode in a full-cell configuration is a key step in investigating the possible application of the active material in LIBs. In this regard, the recent progress and important approaches to overcoming and alleviating the drawbacks of Group IVA element-based anode materials are reviewed, such as the severe volume variations during cycling and the relatively brittle electrode/electrolyte interface in full-cell LIBs. Finally, perspectives and future challenges in achieving the practical application of Group IVA element-based anodes in high-energy and high-power-density LIB systems are proposed.

11.
Opt Lett ; 42(19): 3928-3931, 2017 Oct 01.
Artigo em Inglês | MEDLINE | ID: mdl-28957163

RESUMO

In this Letter, a light management structure composed of wedge-shaped semiconductor nanowall arrays is introduced. Theoretical investigation based on gallium arsenide (GaAs) indicates that a 1000 nm high array (wall base width/array periodicity: 500 nm) with an effective thickness of only 500 nm can deliver a maximum photocurrent density (Jph) of ∼29.0 mA/cm2 at AM1.5G illumination. (For an ideal absorber with the same bandgap, the corresponding value is ∼32.0 mA/cm2.) However, Jph of a 1500 nm thick flat GaAs film is only ∼19.2 mA/cm2 at the same illumination condition. The wedge-shaped nanowall arrays meanwhile exhibit good omnidirectional light confinement. At the incident angle of 60°, Jph of the aforementioned nanowall array is ∼12.7 mA/cm2, and the corresponding value for an ideal absorber is ∼16.0 mA/cm2. Considering the simple structure and excellent light confinement in a broad range of the system parameters, including array periodicity, the nanowall height, and the incident angle of light, the wedge-shaped semiconductor nanowall arrays provide a valuable platform for fabricating the related high performance-to-cost semiconductor optoelectronic devices.

12.
ACS Appl Mater Interfaces ; 16(7): 8922-8929, 2024 Feb 21.
Artigo em Inglês | MEDLINE | ID: mdl-38330215

RESUMO

Vanadium-based oxides have garnered significant attention as cathode materials for aqueous zinc-ion batteries (AZIBs) because of their high theoretical capacity and low cost. However, the limited reaction kinetics and poor long-term cycle stability hinder their widespread application. In this paper, we propose a novel approach by coinserting Ni2+ and NH4+ ions into V2O5·3H2O, i.e., NNVO. Structural characterization shows that the coinsertion of Ni2+ and NH4+ not only extends the interlayer spacing of V2O5·3H2O but also significantly promotes the transport kinetics of Zn2+ because of the synergistic "pillar" effect of Ni2+ and NH4+, as well as the increased oxygen vacancies that effectively lower the energy barrier for Zn2+ insertion. As a result, the AZIBs with an NNVO electrode exhibit a high capacity of 398.1 mAh g-1 (at 1.0 A g-1) and good cycle stability with 89.1% capacity retention even after 2000 cycles at 5.0 A g-1. At the same time, a highly competitive energy density of 262.9 Wh kg-1 is delivered at 382.9 W kg-1. Considering the simple scheme and the resultant high performance, this study may provide a positive attempt to develop high-performance AZIBs.

13.
Phys Chem Chem Phys ; 15(24): 9924-30, 2013 Jun 28.
Artigo em Inglês | MEDLINE | ID: mdl-23673428

RESUMO

We report a facile and reproducible synthesis of nanostructured Ni3S2 films by a hydrothermal route with Ni foam as the precursor reactant and substrate. The synthetic mechanism was examined by investigating the dependence of the films' crystal morphologies on the hydrothermal duration, and uniform nanostructured Ni3S2 films with a porous carpet-like morphology were synthesized on the substrates. The architectures were used as cathodes for lithium ion batteries (LIBs), and their electrochemical performances were evaluated as a function of the film thickness. The first discharge and charge capacities were 596 and 466 mA h g(-1) for the electrode with an optimal film thickness and a higher reversible capacity of 421 mA h g(-1) was obtained after 60 cycles at a current density of 50 mA g(-1). The simplicity of the synthetic methodology and the better electrochemical performance make the synthesized Ni3S2 films a promising cathode material for next-generation LIBs.

14.
ACS Appl Mater Interfaces ; 15(46): 53558-53567, 2023 Nov 22.
Artigo em Inglês | MEDLINE | ID: mdl-37939372

RESUMO

Herein, a dual-function strategy, in which CsPbI2Br is treated by CsPbBr3 nanocrystals (NCs) via addition and surface modification to construct the "electron bridge" and gradient heterojunction, respectively, to notably improve the performance of the CsPbI2Br solar cells, is proposed. The "electron bridge" formed by the CsPbBr3 NCs provides an extra transport channel for the photogenerated electrons in the CsPbI2Br layer, thus facilitating electron transport. Meanwhile, surface modification of CsPbI2Br by the CsPbBr3 NCs forms a gradient heterojunction between the CsPbI2Br layer and the P3HT layer, enhancing hole extraction accordingly. In addition, the CsPbBr3 NC treatment passivates the defects at the bulk and surface of the CsPbI2Br layers, thus suppressing carrier recombination. Thanks to these positive effects of the CsPbBr3 NCs, the demonstration device with a simple configuration of ITO/SnO2/CsPbI2Br/P3HT/Ag achieves a notable power conversion efficiency of 17.03%, which is among the highest efficiencies reported for CsPbI2Br-based solar cells.

15.
Nanoscale ; 15(32): 13411-13419, 2023 Aug 17.
Artigo em Inglês | MEDLINE | ID: mdl-37540038

RESUMO

Conductive-bridging memristors based on a metal ion redox mechanism have good application potential in future neuromorphic computing nanodevices owing to their high resistance switch ratio, fast operating speed, low power consumption and small size. Conductive-bridging memristor devices rely on the redox reaction of metal ions in the dielectric layer to form metal conductive filaments to control the conductance state. However, the migration of metal ions is uncontrollable by the applied bias, resulting in the random generation of conductive filaments, and the conductance state is difficult to accurately control. Herein, we report an organic polymer carboxylated chitosan-based memristor doped with a small amount of the conductive polymer PEDOT:PSS to improve the polymer ionic conductivity and regulate the redox of metal ions. The resulting device exhibits uniform conductive filaments during device operation, more than 100 and non-volatile conductance states with a ∼1 V range, and linear conductance regulation. Moreover, simulation using handwritten digital datasets shows that the recognition accuracy of the carboxylated chitosan-doped PEDOT:PSS memristor array can reach 93%. This work provides a path to facilitate the performance of metal ion-based memristors in artificial synapses.

16.
ACS Appl Mater Interfaces ; 14(25): 29197-29212, 2022 Jun 29.
Artigo em Inglês | MEDLINE | ID: mdl-35704847

RESUMO

Extracting clean energy by converting the salinity gradient between river and sea into energy is an effective way to reduce the global pollution and carbon emissions. Reverse electrodialysis (RED) is of great importance to realize the energy conversion assisting the ion-selective membrane. However, its higher ion resistance and lower conversion efficiency results in the undesirable power conversion performance. Here, we demonstrate a 1D/2D hybrid nanochannel system to achieve high osmotic energy conversion and output power. This heterogeneous structure is composed of two structures, in which the subnanometer nanochannels in graphene oxide membrane (GOM) can serve as a selective layer and reduce the ion diffusion energy barrier, while the nanochannel in the polymer can introduce asymmetry to enhance ionic rectification and conversion efficiency. This heterogeneous membrane exhibits excellent cation selectivity and enhanced ionic current rectification (ICR) performance. The application of the GOM/PET hybrid nanochannel system in osmotic energy harvesting is evaluated, and the output power can reach up to 118.2 pW with the energy conversion efficiency of 40.3%. Theoretical calculation indicates that the 1D/2D hybrid system can effectively take the advantage of excellent cation selectivity of 2D lamellar nanochannels to improve its RED performance significantly.

17.
ACS Appl Mater Interfaces ; 14(9): 11739-11749, 2022 Mar 09.
Artigo em Inglês | MEDLINE | ID: mdl-35200005

RESUMO

SnS2-based materials have attracted considerable attention in energy storage and conversion owing to their high lithium activity and theoretical capacity. However, the practical application is severely limited by the low coulombic efficiency and short cycle life due to irreversible side reactions, low conductivity, and serious pulverization in the discharge/charge process. In this study, sheet-like stacking SnS2/reduced graphene oxide (rGO) heterostructures were developed using a facile solvothermal method. It was found that the composites between SnS2 nanoplates and rGO nanosheets are closely coupled through van der Waals interactions, providing efficient electron/ion paths to ensure high electrical conductivity and sufficient buffer space to alleviate volume expansion. Therefore, the SnS2/rGO heterostructure anode can obtain a high capacity of 840 mA h g-1 after 120 cycles at a current density of 200 mA g-1 and maintain a capacity of 450 mA h g-1 after 1000 cycles at 1000 mA g-1. In situ X-ray diffraction tests showed that SnS2/rGO undergoes typical initial intercalation, conversion, and subsequent alloying reactions during the first discharge, and most of the reactions are dealloying/alloying in the subsequent cycles. The galvanostatic intermittent titration technique showed that the diffusion of lithium ions in the SnS2/rGO heterostructures is faster in the intercalation and conversion reactions than in the alloying reactions. These observations help to clarify the reaction mechanism and ion diffusion behavior in the SnS2 anode materials, thus providing valuable insights for improving the energy efficiency of lithium-ion batteries.

18.
ACS Appl Mater Interfaces ; 14(3): 4079-4090, 2022 Jan 26.
Artigo em Inglês | MEDLINE | ID: mdl-35005891

RESUMO

In the wake of shaping the energy future through materials innovation, lithium-sulfur batteries (LSBs) are top-of-the-line energy storage system attributed to their high theoretical energy density and specific capacity inclusive of low material costs. Despite their strengths, LSBs suffer from the cross-over of soluble polysulfide redox species to the anode, entailing fast capacity fading and inferior cycling stability. Adding to the concern, the insulating character of polysulfides lends to sluggish reaction kinetics. To address these challenges, we construct optimized polysulfide blockers-cum-conversion catalysts by accommodating the battery separator with covalent organic framework@Graphene (COF@G) composites. We settle on a crystalline TAPP-ETTB COF in the interest of its nitrogen-enriched scaffold with a regular pore geometry, providing ample lithiophilic sites for strong chemisorption and catalytic effect to polysulfides. On another front, graphene enables high electron mobility, boosting the sulfur redox kinetics. Consequently, a lithium-sulfur battery with a TAPP-ETTB COF@G-based separator demonstrates a high reversible capacity of 1489.8 mA h g-1 at 0.2 A g-1 after the first cycle and good cyclic performance (920 mA h g-1 after 400 cycles) together with excellent rate performance (827.7 mA h g-1 at 2 A g-1). The scope and opportunities to harness the designability and synthetic structural control in crystalline organic materials is a promising domain at the interface of sustainable materials, energy storage, and Li-S chemistry.

19.
ACS Appl Mater Interfaces ; 14(36): 40930-40938, 2022 Sep 14.
Artigo em Inglês | MEDLINE | ID: mdl-36049130

RESUMO

CsPbI2Br is promising in the application of perovskite solar cells (PSCs) owing to its reasonable bandgap and good thermal stability. However, the reported power conversion efficiency (PCE) of the CsPbI2Br solar cells is still much lower than that of the organic-inorganic hybrid PSCs, mainly due to relatively poor CsPbI2Br crystal quality. Herein, additive engineering to the photoactive layer of CsPbI2Br using the Ti3C2Tx MXene nanosheets is reported. Thanks to the improved crystallinity/reduced defect density, together with the formation of the Schottky junction between the MXene nanosheets and CsPbI2Br, enhanced separation and transfer of the photogenerated electron-hole pairs can be achieved for optimal MXene addition. A simple device configuration of ITO/SnO2/Ti3C2Tx-added CsPbI2Br/P3HT/Ag can thus deliver a significantly boosted PCE of 15.10%, i.e., a ∼16.69% relative increment compared with that (12.94%) of the control device without adding MXene. In addition, the enhanced humidity resistance is achieved for the MXene-added CsPbI2Br layers.

20.
ACS Appl Mater Interfaces ; 14(1): 1557-1567, 2022 Jan 12.
Artigo em Inglês | MEDLINE | ID: mdl-34957821

RESUMO

Ion-based memristive switching has attracted widespread attention from industries owing to its outstanding advantages in storage and neuromorphic computing. Major issues for achieving brain-inspired computation of highly functional memory in redox-based ion devices are relatively large variability in their operating parameters and limited cycling endurance. In some devices, volatile and nonvolatile operations often replace each other without changing operating conditions. To address these issues, it is important to observe directly what is happening in repeated operations. Herein, we use a planar device that enables direct capturing of microscopic behaviors in the nucleation and growth of metal whiskers under repeated switching to verify the microscopic origin of the large parameter variability. We report direct observations that reveal the physical origin for the large cycle-to-cycle and device-to-device variability in memristive switching, which was achieved using planar polymer atomic switches with a gap >1 µm. We find that the deposition location of metal atoms is closely related to the crystallinity of the ion transport layer (solid polymer electrolyte, SPE). The filament variability (shape, position, quantity, etc.) during different cycles and devices is indeed the main reason for the observed variability in the operating characteristics. The results shed unique light on the complexity of the operation of the ion device, that is, the evolution of the dielectric layer and metal filament must be considered.

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