Aqueous zinc-ion batteries (AZIBs) are leading candidates for large-scale energy storage, but their commercialization is hindered by Zn anode dendrites and hydrogen evolution reaction (HER), limiting cycle life to <200 h. Current strategies—interface engineering and alloying—offer marginal improvements but fail for scalability due to complex processing or high costs. Herein, we report a second-scale, room-temperature, low-stress ultrasonic vibration (UV) strategy that enables Ag/Cu/In doping of Zn anodes via enhanced atomic motion, concurrently achieving grain refinement and cost reduction with recyclable metal foils. The synergy of doping, grain refinement, and UV-induced stacking faults (SFs) and nanoscale defects enables uniform Zn deposition and suppressed HER. Ag-doped AZIBs deliver 5600 h cycle life at 0.5 mA·cm-2 and 0.5 mAh·cm-2, retaining 3180 h under rigorous conditions of 5 mA·cm-2 and 1 mAh·cm-2. Cu- and In-doped counterparts achieve 5350 h and 3090 h, respectively, at this high-current regime. This work resolves AZIBs’ cycle-life bottleneck, establishes a universal physical vibration paradigm for metal electrode engineering, and transcends AZIBs to enable scalable high-performance energy storage.
Transition metal oxides, particularly Fe3O4, are regarded as highly promising high-capacity anodes for lithium-ion batteries; however, their practical application is hindered by poor electronic conductivity, sluggish Li+ diffusion kinetics, and severe volume fluctuations during cycling. Herein, a scalable strategy is reported to construct a V and S co-doped Fe3O4 nanocomposite intimately hybridized with an S, N co-doped carbon matrix (denoted as VS-Fe3O4/SNC). In this design, dual conductivity enhancement—simultaneously improving both electronic transport and Li⁺ diffusion kinetics—is uniquely enabled by V/S co-doping within the Fe3O4 lattice, as evidenced by the substantially reduced charge transfer resistance and the increased Li⁺ diffusion coefficient. The Fe3O4 nanoparticles (10–50 nm) are uniformly anchored on the heteroatom-doped carbon framework, by which ion diffusion pathways are shortened and volume expansion is buffered. Benefiting from these synergistic effects, enhanced electrochemical performance is delivered by the VS-Fe3O4/SNC anode. A high reversible capacity of 934 mAh g–1 is achieved after 70 cycles at 0.1 A g–1, along with an improved rate capability (466 mAh g–1 at 5.0 A g–1), and remarkable long-term cycling stability is demonstrated, with a retained capacity of 434 mAh g–1 over 500 cycles at 5.0 A g–1. Moreover, the versatility of this approach is validated by its successful extension to the MnO system, for which significantly enhanced lithium storage performance is similarly achieved. Through this work, a facile and generalizable pathway is provided for the design of high-performance metal oxide/carbon composite anodes via synergistic cation–anion co-doping, offering critical insights into unlocking high-rate Li⁺ storage capabilities.
Transition metal oxides (TMOs) are promising electrocatalysts for non-enzymatic glucose (NEG) sensors; nevertheless, their electrocatalytic performance is impeded by sluggish electron transfer kinetics and inadequate reactant adsorption. The rational design of the electronic and geometric structures of TMOs is crucial for enhancing their electrocatalytic activity toward glucose oxidation. Here, an Au-decorated hollow microspherical N-doped CuO heterojunction (Au/N-CuO-HM) was successfully prepared by a solvothermal method followed by calcination. Density functional theory (DFT) calculations and experimental results indicate that the formation of the Au/CuO heterojunction creates a built-in electric field at the interface, promoting electron transfer and reducing charge transfer resistance. More importantly, the incorporation of Au results in an upward shift of the d-band center (epsilon d) for the Cu sites, thereby strengthening the interaction between the electrocatalyst and glucose, as confirmed by the more negative adsorption energy of glucose after Au decoration (-2.351 vs. -1.856 eV). Simultaneously, the hierarchical hollow architecture of Au/N-CuO-HM enhances the accessibility of active sites and boosts mass transport, thereby leading to a high electrochemical active surface area of 0.286 cm2. Benefiting from the synergistic effect of both electronic structure modulation and hierarchical hollow architecture, the Au/N-CuO-HM modified electrode delivers outstanding electrocatalytic properties. This study not only provides insights into the roles of electron transfer regulation, epsilon d modulation, and hollow architecture design in electrocatalytic properties, but also offers an effective strategy for developing high-performance electrocatalysts for NEG sensors.
Transition metal selenides (TMSes) are regarded as promising anode candidates for high‑efficiency sodium‑ion batteries (SIBs) owing to their outstanding theoretical capacity and low‑cost preparation. However, their practical implementation is severely restricted by sluggish reaction kinetics and rapid capacity fading upon long‑term cycling. Herein, sulfur-induced FeSe/Fe3Se4 heterostructures uniformly confined within porous multielement-doped carbon nanorods (denoted as S‑FeSe/Fe3Se4@C) are rationally fabricated and tested as anode for SIBs. Benefiting from the nanoscale spatial confinement, abundant FeSe/Fe3Se4 heterointerfaces, and robust porous carbon framework, the S‑FeSe/Fe3Se4@C electrode exhibits exceptional sodium storage properties, including a high reversible capacity (909 mAh/g at 0.2 A/g after 300 cycles) and superior rate capability (526 mAh/g at 10 A/g). Moreover, the full cell paired with commercial Na3V2(PO4)3 cathode delivers a stable reversible capacity of 377 mAh/g at 1 A/g after 200 cycles, with a power density of 153.4 Wh/kg at 27.3 W/kg. Pseudocapacitive energy storage is systematically verified to dominate the fast sodium‑storage process and greatly contribute to the outstanding rate performance. Density functional theory (DFT) calculations reveal that the FeSe/Fe3Se4 heterointerface effectively boosts Na⁺ diffusion and accelerates interfacial redox kinetics.
A Synergistic strategy that integrates the intrinsic polarization field with heterojunction interfacial engineering is demonstrated for boosting photocatalytic CO2 reduction. In the engineered Bi4O5Br2/Nb2O5 heterojunction, a structure has not been previously reported for CO2 photoreduction to date, the intrinsic polarization field of Bi4O5Br2 facilitates initial charge separation within the bulk phase. The type-ii interfacial field drives the transfer of separated electrons toNb2O5, achieving effective spatial separation of carriers. This efficient charge separation promotes surface reactions, as evidenced by in situ diffuse reflectance infrared fourier transform spectroscopy (DRIFTS), which reveals accelerated formation and transformation of key intermediates (*CO2, *COOH and *CHO) along the reaction pathways toward CO and CH4. Using ultrapure water as the proton source, the CO and CH4 production rates of the optimal composite reach 4.6 and 3.7 mu mol g-1 h-1, respectively, which are 2.0 and 4.6 times higher than those of pristine Bi4O5Br2. In contrast to conventional heterojunction strategies that focus solely on interfacial band engineering, this work simultaneously leverages the intrinsic properties of bulk materials, offering a new design paradigm for efficient CO2 photoreduction.
Driven by random charge movement and Coulombic force, the photogenerated electron-hole pairs in photo-catalysts tend to rapidly recombine, severely limiting their application. Atomic-level heterointerface engineering and oxygen vacancies (Ov) modulation hold tremendous potential in promoting charge separation and transfer. A series of S-scheme Ov-ZnO/CuO heterojunctions are in situ synthesized via a solvothermal method followed by calcination using bimetallic Zn/Cu-MOF as precursors. The atomic distances between O atoms in the ZnO (002) facet closely match those between Cu atoms in the CuO (-220) facet (5.76 vs. 5.80 & Aring;), while Zn2+ and Cu2+ have similar ionic radii (0.74 vs. 0.73 & Aring;). The structural compatibility enables the formation of Zn-O-Cu bonds at the tightly integrated ZnO/CuO interface, thus achieving atomic-level heterointerface. Owing to the unique structure of the precursors, Ov-ZnO/CuO form into hierarchical porous microspheres that are composed of ultrasmall nanocrystals. In addition, the Ov content of Ov-ZnO/CuO is tuned by changing the Cu:Zn molar ratios of the precursors. The S-scheme charge transfer mechanism reveals that the synergistic effect of atomic-level heterointerface, suitable Ov content, CuO-derived photothermal effect, and short charge diffusion distance effectively promotes the charge separation and transfer in Ov-ZnO/CuO-10%, ultimately achieving a superior CO production rate of 9.13 mu mol g-1 h-1 with 93.7 % retention after four cycles. This study offers an effective route to enhance photocatalytic CO2 reduction activity and sheds new light on purposeful design of heterojunctions based on the structural characteristics of components.
Transition metal oxides, particularly Fe3O4, hold great promise as high-capacity anodes for lithium-ion batteries, yet their practical application is hindered by poor electronic conductivity and severe volume fluctuations during cycling. Herein, we report a simple strategy to construct a V and S co-doped Fe3O4 nanocomposite intimately hybridized with an S, N-co-doped carbon matrix (denoted as VS-Fe3O4/SNC). The synthesis involves freeze-drying of a homogeneous precursor solution followed by a single-step thermal treatment, utilizing NaCl as a porogen and gluconate as both carbon source and reducing agent. The resulting composite features a mesoporous architecture (BET surface area: 324.17 m2 g-1) with V, S-co-doped Fe3O4 nanoparticles (10–50 nm) uniformly anchored on an S, N-co-doped carbon architecture. Benefiting from the synergistic effects of cation–anion co-doping, nanostructuring, and heteroatom-modified carbon encapsulation, the VS-Fe3O4/SNC anode delivers exceptional electrochemical performance. It exhibits a high reversible capacity of 934 mAh g-1 after 70 cycles at 0.1 A g-1, outstanding rate capability (466 mAh g-1 at 5.0 A g-1), and remarkable long-term cycling stability with a retained capacity of 434 mAh g-1 over 500 cycles at 5.0 A g-1 and an average Coulombic efficiency of 99%. Moreover, the synthetic versatility is demonstrated by successful extension to the MnO system, which likewise yields enhanced electrochemical performance. This work provides a facile and generalizable approach for designing high-performance metal oxide/carbon composite anodes through synergistic dual-doping strategies.
Glucose detection is essential in clinical medicine, and the reasonable design of metal oxide electrocatalysts plays a crucial role in developing efficient nonenzymatic glucose (NEG) sensors. Herein, grain boundary/doping/architecture engineering is used to tailor the structures of CuO nanomaterials and tune their surface/electron-transfer properties toward enhanced electrocatalytic oxidation of glucose. Hierarchical N-doped CuO microflowers (N-CuO-MF) are synthesized using a facile hydrothermal method, followed by calcination. N-CuO-MF consist of ultrathin nanoflakes (ca. 20 nm), endowing them with a large specific surface area. Moreover, the nanoflakes are composed of ultrasmall nanoparticles, resulting in abundant grain boundaries. Notably, N-CuO-MF are derived from a precursor of Cu-based metal-organic framework (Cu-MOF) architectures, which is fabricated through a bottom-up route using glycerol as the capping agent/solvent and 1-hexadecyl-3-methylimidazolium bromide ([C16mim]Br) as the template/N source. Glycerol competitively coordinates with Cu2+, leading to the formation of 2D subunits. Moreover, [C16mim]+ cations attach to the subunit surfaces via electrostatic interaction, thus achieving Cu-MOF with a 3D hierarchical structure. As expected, the synergistic effect of rich grain boundaries, N doping, ultrathin nanoflakes, and hierarchical architecture enhances the adsorption of glucose on the electrode surfaces, accelerates electron transfer, and exposes more active sites for glucose oxidation. Accordingly, N-CuO-MF exhibit wide linear ranges, high sensitivity, fast response time, low detection limit, excellent selectivity, and good stability. Owing to their highly efficient electrocatalytic properties, N-CuO-MF could be explored as potential electrocatalysts in NEG sensors for rapid diagnostic tests and health monitoring.
Micro-expression recognition (MER) is a challenging task due to the subtle and local movements of facial muscles. To get rid of redundant video frames, studies have been conducted on the use of apex frames for MER. However, these studies mainly focused on 2D frontal apex frames, ignoring side face information, which can result in insufficient extraction of features?. To address this issue, we propose a novel dual-stream network with coordinate attention (DSNCA) framework for MER, which comprises a multi-view coordinate attention module (MVCAM) and an apex frame coordinate attention module (AFCAM). The MVCAM initially employs 3D face reconstruction to acquire unobstructed multi-view images that are rich in micro-expression information and enhanced with geometric details. Subsequently, it adaptively learns micro-expression features from multiple angle views with coordinate attention, thus leveraging supplementary face information. In contrast, the AFCAM aims to adaptively locate key regions where micro-expressions occur, thereby minimizing redundant information. The proposed method achieved UF1 and UAR of 76.45, 75.16, 59.21, 59.6, 62.77, 62.06, 66.74, and 69.31 on the Chinese Academy of Sciences Micro-expression DatabaseII (CASMEII), the Spontaneous Micro-expression Corpus (SMIC), the Spontaneous Actions and Micro-Movements (SAMM), and the composite databases, respectively. The code is available for research purposes at https://github.com/pennypppp/DSNCA .
An Fe–V 2 O 3 /NC composite with alluring electrochemical performance was successfully constructed, and detailed mechanistic studies revealed that the Li + storage mechanism follows an insertion/extraction pathway rather than a conversion reaction.
The design of nanomaterials enclosed by high-index facets plays a critical role in the surface-sensitive properties. Herein, hierarchical CuCo2O4 microflowers (CCO-F) with highly exposed high-index (112) facets are rationally designed via a solvothermal method followed by calcination. CCO-F are composed of 30 nm-thick nanoflakes and have an ultrahigh specific surface area of ca. 205.48 m2 g-1. Additionally, nanoparticle-assembled CuCo2O4 microspheres (CCO-S) are prepared, and these nanoparticles are partly enclosed by the (110) facets. Abundant octahedrally coordinated Co3+ (Co3+Oh) and tetrahedrally coordinated Cu2+ (Cu2+Td) exist in the (112) facet, especially Co3+Oh (with a density of 0.063 Å-2); moreover, the (112) facet possesses a high surface Gibbs free energy (2.7367 J m-2). Therefore, CCO-F have significant advantages of adsorbing glucose and conducting the subsequent redox reactions. In addition, the hierarchical microstructure promotes the reaction kinetics of CCO-F. Benefiting from these features, the CCO-F-modified electrode exhibits high sensitivities (1351.2 and 598.7 μA mM-1 cm-2), wide linear ranges (1 μM-3 mM and 4-10 mM), rapid response time, low detection limit, excellent stability, and good selectivity. This work indicates that the exposure of a high percentage of high-index facets is an effective approach to exploring high-performance electrocatalysts for glucose detection.
Wadsley-Roth phase TiNb2O7 has been known as a potential anode material in high-power lithium-ion batteries (LIBs) owing to its enhanced safety, reliable cycling performance, and substantial theoretical capacity. However, its commercial application is restricted by poor electronic conductivity and slow Li-ion migration kinetics. Herein, we have developed urchin-structured TiNb2O7 microspheres with an ultrathin N-doped carbon coating through a two-step hydrothermal and polydopamine carbonization process. When used as LIBs anode, the TiNb2O7@N-C composite demonstrates a remarkable rate capability of 216 mAh g-1 at 30 C and a durable lifespan with a capacity retention of 89 % after 500 cycles (10 C). In addition, by pairing with LiNi0.5Mn1.5O4 cathode, the full cell also reveals outstanding electrochemical performance even at high rates. The enhanced lithium storage capabilities of TiNb2O7@N-C can be credited to the integrated superiorities of the multilevel urchin-like architecture and the external conductive layer, which shortens the Li+/electron transfer paths, buffer the volume fluctuations of active substance, and improves the overall conductivity of the composite electrode.
Fe-doped V2O3 nanoparticles hybridized with N-doped carbon were successfully constructed. The Fe-V2O3/NC anode presents exceptional rate performance in LIBs, achieving a large capacity of 361 mAh g-1 under 5 A g-1. In situ XRD analysis and theoretical calculations collectively elucidated, for the first time, that the Li+ storage mechanism follows an insertion and extraction pathway rather than a conversion reaction.
Spinel oxide anode materials are rarely employed in industrial lithium-ion batteries due to their significant volume swelling during the discharge process and low electronic conductivity. The aforementioned challenges can be effectively addressed through the preparation of composite materials comprising nanoscale spinel-type bimetallic oxide and porous carbon nanosheet, thereby enabling the realization of exceptional electrochemical performance. In this work, a general and convenient strategy was successfully developed for fabricating spinel AxFe3-xO4 (A= Co, Mn, Mg, Cu, Fe) nanoparticles anchored on porous carbon nanosheet. The integration of spinel Co0.5Fe2.5O4 nanoparticles with porous carbon nanosheets not only significantly mitigates the volume expansion issue but also remarkably enhances conductivity. The Co0.5Fe2.5O4/porous carbon nanosheet composite anode demonstrates excellent cycling stability and rate capability for lithium-ion batteries, delivering a high capacity of 490 mAh g-1 after 420 cycles at 2 A g-1. The general and facile synthesis approach, combined with the outstanding electrochemical performance demonstrated in this work, is anticipated to accelerate the development and practical application of spinel oxide-based anode materials.
The utilization of MnO anodes with high storage capacity is significantly hindered by rapid capacity fading and inadequate rate capability, stemming from substantial volume fluctuations and low electrical conductivity. Crafting a composite comprising sulfur and fluorine co-modified MnO nanoparticles integrated with sulfur and nitrogen co-doped carbon matrices promises enhanced electrochemical performance yet poses formidable obstacles. Here, we present a straightforward synthetic strategy for in situ growth of sulfur and fluorine co-modified MnO nanoparticles onto sulfur and nitrogen co-doped carbon scaffolds. This integration effectively mitigates volume variations and enhances electrical conductivity. As a result, the SF-MnO/SNC composite demonstrates remarkable cycling stability and rate capability when employed as a lithium-ion battery anode. Remarkably, it achieves a high reversible capacity of 975 mAh g−¹ after 80 cycles at 0.1 A g−¹ and retains a substantial capacity of 498 mAh g−¹ even at a high rate of 2.0 A g−¹. The concise synthesis method and exceptional rate properties render the SF-MnO/SNC composite a promising anode material for lithium-ion batteries. The strategy of simultaneously doping oxides and carbon will bring new ideas to the research of oxide anodes.
Spinel oxide anode materials are hardly used for commercial lithium-ion batteries because of their evident volume expansion in the discharging process and poor electronic conduction. Preparing a composite material of nanostructured spinel bimetallic oxides and carbon will solve the above problems and achieve outstanding electrochemical performance. In this study, an ultrafast approach (only 10min) to synthesize spinel AMn2O4 (A= Co, Mn, Zn) nanopolyhedras and their composites with GO was successfully developed. Integrating spinel CoMn2O4 nanopolyhedras with GO can profoundly inhibit the problem of volume expansion but also eminently upgrading conductivity. The CoMn2O4/GO composite anode displays competent cyclic life and rate capability for lithium ion battery, delivering a large capacity of 738 mAh g-1 after 340 cycles at 2Ag-1. The ultrafast approach and alluring electrochemical performance of this work will inevitably give impetus to the fast development and application of spinel oxides.
The development and application of V2O3-based anodes are hindered by their poor reversible capacity and rate performance. Doping F and combined with N-doped carbon at the same time would achieve excellent electrochemical performance, but the related materials are not prepared and employed to lithium-ion batteries due to the absent synthetic method. In this investigation, a simple strategy was firstly invented to achieve F-doped V2O3/N-doped carbon composite. The F-doped V2O3 nanoparticles are adhered to N-doped carbon, which would enhance electrochemical reaction kinetics. As a result, a high capacity of 481 mAh/g can be obtained at 2 A/g.
To effectively evaluate the gross motor ability of autistic children, we proposed a method of computerised evaluation of gross motor skills (CEGM). The CEGM integrates Dynamic Time Warping (DTW) method and OpenPose technology to automatically detect key joints and return a score. Ten items were selected for evaluation based on the gross motor subtest of the Psychoeducational Profile - Third Edition (PEP-3) scale, including upper limb movement, lower limb movement, and body coordination performance. 30 autistic participants (males: 23, female: 7) with an average age of 5.00 years were recruited in this study. Then we compared the results of evaluation using CEGM and the original PEP-3 gross motor subtest in autistic children. The results showed that in the evaluations using CEGM and PEP-3, Cronbach's alpha coefficients and Spearman-rank correlation coefficients were all greater than 0.80, intraclass correlation coefficient (ICC) were all greater than 0.90, indicating good agreement in evaluating the gross motor ability of autistic children. Moreover, compared to the PEP-3, the evaluation using CEGM provided precise quantitative indicators (trajectory, velocity, and angle of joint). Therefore, our findings demonstrate that CEGM can be used in the initial evaluation of the gross motor ability of autistic children.