The electrochemical urea oxidation reaction (UOR) is a promising strategy for hydrogen production coupled with the treatment of urea-rich wastewater. Herein, a Co-modified strategy is used to modulate the electronic structure and microstructure of FePS3, thereby enhancing catalytic activity and structural stability. The optimized Co-modified FePS3-Co/NF electrode achieves a current density of 300 mA cm−2 at 1.56 V versus RHE, which is 60 mV lower than that of pristine FePS3/NF. Comprehensive characterizations reveal that the enhanced UOR performance originates from a synergistic structural and electronic modulation effect. Structurally, Co-modified induces pronounced grain refinement, thereby exposing a larger number of catalytically active sites. Electronically, Co-modified modulates the electronic structure of FePS3 by increasing the proportion of Fe3+ species, which facilitates the adsorption and activation of urea molecules and reaction intermediates. This work elucidates the catalytic enhancement mechanism induced by Co-modification and provides valuable insights for the rational design of high-performance UOR electrocatalysts.
Aqueous zinc-ion hybrid capacitors (ZIHCs) have garnered significant attention due to their cost-effectiveness, safety, and high theoretical capacity. However, the use of carbon-based materials in ZIHCs faces challenges such as electrolyte ion and pore size mismatching, inadequate infiltration between electrolyte and electrode, and limited surface active sites and defects, all of which impede the device's ability to achieve optimal energy density and electrochemical performance. To address these issues, a three-dimensional N and O co-doping hierarchical porous activated carbon (3DNOHC) with an ultrahigh specific surface area of 3477.69 m2 g-1 is synthesized through the direct calcination of nitrilotriacetic acid sodium salt precursor followed by a chemical activation process. Density functional theory calculations demonstrate that the N/O co-doping of activated carbon significantly enhances the ion adsorption/desorption capabilities on the surface of the materials, thereby improving their kinetic and electrochemical properties. The structural changes in zinc metal anodes and 3DNOHC cathodes during charging/discharging are investigated using ex situ XRD and ex situ Raman tests. Due to its abundant porous structure and active sites, the 3DNOHC-6 sample exhibits rapid ion transport and impressive electrochemical performance in ZIHCs. In particular, the 3DNOHC-6//Zn device demonstrates a high reversible capacity of 171/102 mA h g-1 at 0.2/10 A g-1 and an outstanding energy density of 137 Wh kg-1@160 W kg-1. Moreover, it exhibits excellent capacity retention of 80% at 5 A g-1 after 45 000 cycles. This study serves as a valuable reference for the development of activated carbon cathode materials for aqueous hybrid capacitors aiming for high energy/power density.
3D-printed flexible zinc-ion hybrid microsupercapacitors (ZHMSCs) show immense promise as emerging energy storage units for flexible microelectronic systems, delivering intrinsic safety, high theoretical capacity, and designable architectures. However, the low intrinsic conductivity of electrode materials and the significant interfacial contact resistance hinder the development of all-printed devices with superior areal capacitance and power density. In this study, a hierarchical conductive optimization strategy is proposed to construct a high-performance flexible ZHMSC via a fully 3D-printing process. At the microscale, highly conductive PEDOT:PSS (PH1000) is introduced as an intercalation agent into the Ti3C2 MXene cathode, effectively suppressing the restacking of MXene layers and constructing efficient ion transport channels. At the macro scale, the interface contact resistance is effectively reduced by in situ printing of the silver current collector. The device exhibits excellent electrochemical performance enabled by a directly printable, high-mass-loading zinc-based composite anode and a water-retentive ZnSO4/hyaluronic acid gel electrolyte. The fabricated flexible ZHMSC delivers a remarkable areal capacitance of 1199.5 mF cm(-2) and an energy density of 326.5 mu Wh cm(-2). Moreover, the device demonstrates excellent cycling stability with 82% retention of the initial capacitance after 9000 cycles. This work confirms the effectiveness of a hierarchical conductive network design in enhancing all-printed energy storage and provides an efficient, scalable manufacturing paradigm for the next generation of integrated flexible micropower systems.
Sodium-ion batteries (SIBs) have garnered great attention owing to higher abundance of raw materials and better rate capability compared to lithium-ion batteries, making them promising for next-generation electrochemical energy storage systems that require high energy, high power and low cost. However, the rate performance of current SIBs remains unsatisfactory, mainly limited by the neglect on the compatibility of cathode-anode kinetics. Herein, an efficient design principle is proposed to construct an ultrafast-charging SIB by matching the reaction mechanisms and reaction rates of Na3(VOPO4)2F (NVOPF) cathode and TiO2 anode. The superior fastcharging performance originates from rapid solid-solution Na+ storage in the NVOPF cathode and fast redox pseudocapacitance in the nanosized anatase TiO2 anode during charge/discharge, coupled with their shared low impedance and comparable Na+ diffusion coefficients. Such kinetics matching allows the TiO2||NVOPF full cell to be charged at high rates up to 40 C within a wide potential window of 0.5-3.9 V without sodium metal plating. As a result, the cell delivers optimal power and energy densities of 5.8 kW kg- 1 and 170.6 Wh kg- 1, respectively, which are on par with some state-of-the-art sodium-ion capacitors and batteries. This work provides valuable guidance for designing ultrafast-charging SIBs and offers a practical demonstration of high-power sodium storage.
Zinc-iodine rechargeable batteries possess intrinsic safety and high energy density, showcasing promising potential for energy storage. However, their stability is significantly compromised due to the poor thermal stability and insulation properties of iodine, along with the diffusion characteristics of soluble polyiodides in aqueous media, slow kinetic behavior, and an unsatisfactory shuttle effect. In this paper, we propose a chemisorption constraint strategy for Zn-I2 batteries by employing a polyethyleneimine (PEI)-modified graphene material, which provides abundant nitrogen-containing active sites to significantly enhance battery performance. The initial iodide ion chemically interacts with PEI to form an N-I bond. Additionally, the incorporation of a layered structure of reduced graphene oxide enhances the kinetic properties of the material and facilitates the diffusion of Zn2+. Scanning electrochemical microscopy analysis reveals a trade-off where PEI stabilizes rGO against aggregation and ensures uniform micro-region current distribution. An optimal low PEI ratio (1:1) is crucial to balance these properties. DFT calculations confirm that PEI-induced I3-adsorption synergistically suppresses the shuttle effect and enhances I-/I2 redox kinetics, ensuring superior cycling stability. The results demonstrate that the rGO-PEI-I Zn-iodine battery exhibits excellent reversible rate capacity (266.2 mAh g-1 at 1 A g-1 and 100.0 mAh g-1 at 10 A g-1) and outstanding cycle performance (30,000 cycles at 10 A g-1). Thus, our strategy can be generalized to the engineering of Zn-I2 batteries that achieve prolonged lifespans.
Piezoresistive sensors are indispensable in advanced electronics and play a pivotal role in practical applications such as healthcare monitoring, intelligence recognition, and human interaction systems. Owing to its superior stimulus sensing performance, the piezoresistive sensor has always emerged as a prime candidate for sensing applications. However, realizing a sensor that simultaneously delivers high sensitivity and a wide detection range to accommodate various application scenarios remains a challenge. Herein, a three-dimensional (3D) interfacial structured MXene/polydimethylsiloxane (PDMS) sensor device is developed. Capable of large-scale continuous deformation and tunable interfacial contact sites, the sensor exhibits excellent sensing performance. The resulting sensor showcases a broad sensing range of 0–290 kPa, an ultrahigh sensitivity of 210 kPa−1, a low detection limit of 2.9 Pa, a rapid response of 7 ms, and an excellent stability over 5000 cycles. These excellent features enable potential applications in the domains of human health monitoring (wrist pulse and oral health), real-time manipulator control, and unique handwriting recognition assisted by a deep learning-based neural network. This work offers valuable insights into the design of cross-scale 3D interfacial structures for fabricating high-performance pressure sensors. It holds immense promise across scenarios from subtle stimulus detection to substantial force response, encompassing health monitoring, human–machine interaction, and deep-learning-powered intelligent systems.
The increasing demand for multifunctional protection in miniaturized military equipment has driven the development of lightweight, high-efficiency microwave-absorbing (MA) materials with infrared stealth capability. However, achieving multispectral stealth involves complex component engineering and hierarchical architectures. Herein, we propose a simple strategy to modulate the graphitic structure of graphene nanoplatelets (GNPs) by constructing edge-defect GNPs featuring an in-plane conductive network and an out-of-plane amorphous architecture. Through a radical-mediated preferential edge oxidation process, the defect sites and their density are precisely controlled via the H2O2/H2SO4 disproportionation reaction. Edge-defects enhance polarization and impedance matching without interrupting the continuous in-plane conductive network, enabling microwave absorption and infrared stealth. The optimized edge-defect GNPs achieve a minimum reflection loss (RLmin) of -48.38 dB at a thickness of 1.46 mm, while a 5 wt% composite in silicone rubber achieves -40.6 dB at 1.5 mm, demonstrating a favorable balance of strong absorption, ultrathin thickness, and low filler content. Furthermore, the materials maintain low surface temperatures at 80°C, 180°C, and 200°C, demonstrating excellent infrared stealth capability. This work provides an effective route for designing radar-infrared compatible stealth materials with simplified architecture and multifunctional performance.
The performance of lithium-ion capacitors (LICs) is critically dependent on the properties of their anode materials. In this work, we developed a 3D mesoporous nanocomposite consisting of appropriate oxygen vacancies (OVs) O-Nb2O5/T-NbO2 encapsulated in heteroatom (N, P, S, O)-doped carbon (denoted as m-Nb-O@C) via a soft-template approach. The mixed-valence states (Nb5+/Nb4+) generate abundant OVs while the synergistic combination of heteroatom-doped carbon coating and 3D mesoporous architecture enables exceptional pseudocapacitive behavior and ultrafast charge/discharge kinetics. The m-Nb-O@C nanocomposite demonstrates remarkable electrochemical performance, delivering a high specific capacity of 606 mAh g-1 at 0.1 A g-1 and maintaining 155 mAh g-1 at 10 A g-1, along with excellent cycling stability. By pairing this optimized m-Nb-O@C anode with a three-dimensional porous carbon (3DAC) cathode, a novel LIC system was assembled. This LIC had the advantages of wide voltage of 0-4 V and high coulomb efficiency, and can achieve high energy density of 163 Wh kg-1 and high power density of 70 kW/kg. Notably, it exhibited excellent long-term cycle stability. This study provides practical guidance for promoting the development of high-performance LICs technology.
Spinel oxides are promising electrocatalysts whose activity can be tuned by elemental composition, yet understanding multicomponent synergy remains challenging. Herein, a Spinel-type medium-entropy CoFeCrNiO4 electrocatalyst is developed, and a Cr-Ni synergistic strategy is proposed to regulate dynamic surface reconstruction during OER. The catalyst exhibits an overpotential of 263.4 mV at 10 mA cm- 2 and 365 mV at 300 mA cm- 2 in 1 M KOH, with a low Tafel slope of 37.12 mV dec- 1. It also shows excellent stability, with only 2.78% overpotential decay after 24 h operation. In-situ characterization reveals that the Cr-Ni interaction promotes the formation of active oxyhydroxide species during reconstruction. This work provides insights into synergy-driven activity enhancement and offers guidance for the design of high-performance spinel OER catalysts.
Lithium-air capacitor batteries (LACB) integrate the rapid charge-discharge capability of supercapacitors into conventional lithium-oxygen batteries, significantly enhancing their power density. However, their cycling stability remains unsatisfactory. In this study, we incorporated redox mediators (RMs) into an LACB featuring a dual-cathode configuration. This design facilitates sustained electron transfer between the electrode and Li2O2/Oxygen, thereby delaying RM deactivation caused by electrode passivation and improving the overall electrochemical performance of the LACB. The RM-enhanced battery achieved over 250 cycles at 2 mA cm−2 with a limited capacity of 0.5 mAh cm−2, while exhibiting a 0.54 V reduction in charging voltage at 0.1 mA cm−2 compared to the RM-free system. Furthermore, the application of an aluminum foil sealing technique enabled a power density of 13.8 mW cm−2 at 6 mA cm−2, overcoming mass transport limitations inherent in open-cell configurations. We also investigated the influence of oxygen barrier films with varying barrier capabilities on LACB performance. Results indicate that films with superior oxygen resistance better maintain a clean capacitor electrode surface, thereby providing more stable electron supply to the RMs and enhancing the rate capability and cycling performance of the battery. These findings underscore the potential of redox mediators in improving the performance and longevity of LACBs, offering a promising strategy for their future development.
Transition metal phosphorus sulfides, owing to their unique 2D layered structure and inherent cost-effectiveness, have emerged as promising electrocatalysts in the urea oxidation reaction (UOR). However, they encounter a notable challenge that the dense stacking of their layers drastically restricts the exposure of electrochemically active sites and diminishes electron transfer efficiency, thereby directly leading to subpar performance in the UOR. Herein, based on an intercalation-exfoliation method, a novel layer structural regulation strategy for achieving few-layer FePS3 has been proposed. The results demonstrated that the interlayer stacking of pristine FePS3 could be significantly diminished, with the average layer thickness reducing from 25 nm to an impressive 8 nm. Benefiting from the changes in the layer structure, the few-layer FePS3 exhibits excellent UOR activity, requiring only 1.371 V (vs. RHE) to deliver 10 mA cm-2 and maintaining a low potential of 1.545 V at 300 mA cm-2, which is due to the enhanced exposure of electrochemically active sites and the increased electron transfer efficiency. Simultaneously, the mechanism of enhancing the UOR has been elucidated through in situ Raman and XPS studies. When the UOR of the FePS3/NF couples with the HER of Pt to achieve full electrolysis, the few-layer FePS3/NF system could achieve a urea degradation efficiency of 67.88% after 12 hours, significantly exceeding that of the pristine FePS3/NF system (50.3%). Hence, this work presents a novel strategy for regulating the layered structure of 2D FePS3 to fulfil the synergistic demands of highly efficient urea degradation and low-energy H2 production.
Dual-ion batteries represent a promising energy storage technology, but suffer from low specific capacity of conventional graphite cathode -due to their single anion storage capability. Here, to break the capacity limit coming from anion storage, we propose a structural design strategy involving sulfur doping within the carbon lattice (forming -C-S-C- bonds) to enable the co-storage of both anions and cations. The introduction of sulfur atoms expands the interlayer spacing of the graphitized carbon cathode and enhances its electrical conductivity, thereby improving anion storage. More importantly, -C-S-C- bonds can reversibly react with Li+ to form Li2S during discharging, and release Li+ to reestablish the -C-S-C- bonds during charging, thereby enabling the storage of lithium ions in the cathode. Leveraging this unique energy storage mechanism, the built dual-ion battery demonstrates an unprecedented high specific capacity (280 mAh g- 1 at 50 mA g- 1), excellent rate capability (125 mAh g- 1 at 500 mA g- 1), and outstanding cycling stability (no significant degradation after over 2700 cycles). This work provides a simple and reliable strategy for designing high-capacity cathodes for dual-ion batteries.
Driven by the growing demand for lightweight and flexible microwave-absorbing materials, layered graphene assemblies have attracted significant attention, where interlayer spacing plays a crucial structural role. However, conventional regulation strategies, such as ionic intercalation, heteroatom doping, and chemical modification, introduce foreign species and obscure the intrinsic spacing-performance relationship. Herein, a high-pressure homogenization-based microfluidization approach is proposed to fabricate graphene with tunable interlayer spacing without chemical interference. This enables direct evaluation of the structural guidance effect of spacing on dielectric behavior. The results reveal that interlayer spacing serves as a structural driving factor that modulates conductive network formation and interfacial architecture. As spacing increases, permittivity and reflection loss exhibit a non-monotonic evolution, first increasing and then decreasing, due to spacing-induced microstructural rearrangement that progressively constructs an interconnected yet regulated conductive network. This configuration enhances interfacial polarization and suitable conduction loss while maintaining impedance matching. Consequently, the optimized 60% graphene nanoplatelets-reduced graphene oxide (60% GNPs-rGO) achieves a minimum reflection loss of-50.5 dB. Moreover, a flexible 60%GNPs-rGO/ polydimethylsiloxane (PDMS) composite film with only 5 wt% filler loading still delivers strong absorption of-44.1 dB, demonstrating promise for lightweight and wearable electromagnetic protection.
A thermoelectric generator (TEG) device is capable of converting heat into electrical energy, the thermoelectric efficiency of which is primarily determined by the ZT value of the thermoelectric materials and the internal temperature difference. Consequently, for a constant ZT value, augmenting the thermal energy capture capacity of the TEG device to establish a significant internal temperature gradient emerges as a pivotal strategy for enhancing its thermoelectric efficiency. Spinel-type photothermal conversion (PTC) materials are capable of efficiently capturing solar irradiation and converting it into thermal energy, making them formidable candidates in the synthesis of PTC coatings and the enhancement of thermoelectric conversion efficiency of solar thermoelectric generators (STEG). However, the inherent defects of solar irradiation cause STEG devices to encounter output voltage instability, poor stability, and even insufficient output voltage, hindering efficient energy conversion and storage. Herein, the synthesized CuCr2O4 spinel-type PTC material has been deposited onto the surface of the TEG device to construct the STEG device, which demonstrated a steady-state output voltage (Vopt) of 133.9 mV and a maximum output power density (Pmax) of 68.8 μW cm-2, exceeding 4.5 and 18.1 times that of the TEG device. Subsequently, a booster circuit was designed as the circuit control to stabilize and amplify Vopt, thereby enabling the charging of lithium batteries and the powering of small sensors. This work elucidates the mechanisms of coupling STEG devices with circuit control to achieve the conversion and storage of solar thermal energy into electrical energy.
The interfacial stability of zinc anodes depends primarily upon the electrical double layer (EDL) environment and interfacial electric field (IEF) in repeated Zn plating/stripping processes. Herein, a high-entropy electrolyte (HEE) with over 68 types of Zn2+ solvation configurations is proposed to modulate the EDL and IEF of Zn anode/electrolyte interface, achieving the improved electrochemical stability and low freezing point. The formation of multiple and water-poor Zn2+ solvation configurations facilitates the ion transport dynamics and the desolvation process in the inner Helmholtz plane (IHP), inducing the formation of an organic-inorganic hybrid solid electrolyte interphase (SEI) layer and synergistically guiding the preferential growth of the Zn (100) and (101) crystal planes with compact and dendrite-free deposition morphology. Consequently, the Zn//Cu asymmetric cells with this HEE demonstrate a high average Coulombic efficiency (ACE) of 99.6% for over 3700 cycles (7390 h) at 25 °C and a high ACE of 99.7% for over 4600 cycles (9100 h) at -20 °C. The Zn//Zn symmetric cells also achieve stable operation for more than 3300 and 6900 h at 25 °C and -20 °C, respectively. The Zn//PANI cells exhibit 82.0% capacity retention after 2000 cycles at 1.0 A g-1 at 25 °C and ∼100% capacity retention after 7000 cycles at 0.5 A g-1 at -20 °C. This work provides an in-depth insight into the design of HEEs for tailoring the EDL and IEF to enhance the stability of Zn-based batteries.
Fe-2(MoO4)(3)(FMO), a promising polyanionic cathode material for sodium-ion batteries (SIBs), offers a stable three-dimensional framework, high operating voltage, and exceptional thermal stability, positioning it as a suitable candidate for large-scale energy storage systems. However, its practical implementation is still hindered by sluggish reaction kinetics. In this study, we address the issues of low electronic conductivity and slow Na+ migration in FMO cathode material by an electrospinning-based nano-Synthesis strategy. By precisely regulating the pH of the precursor solution and optimizing the sintering process, the as-prepared FMO-4.25 electrode delivers a high specific capacity of 83.4 mAh center dot g(-1) at 2 C after 100 cycles and maintains a discharge capacity of 74.5 mAh center dot g(-1) even at an ultrahigh rate of 100 C. Moreover, it exhibits remarkable rate capability and long-term cycling stability even under low-temperature conditions. The electrochemical analysis reveals that the nano structuring of the FMO-4.25 electrode effectively enhances the kinetics of ion diffusion and electron transfer. Furtherover, the nanostructure effectively suppresses volume strain during Na+ (de)intercalation, promotes the formation of a stable cathode-electrolyte interphase (CEI), and preserves the integrity of the interfacial and conductive networks, thereby synergistically improving the structural stability of the material. This work provides new insights into the controlled synthesis and mechanistic understanding of high-performance iron molybdate-based cathode materials, offering a valuable reference for advancing the practical application of SIBs in high-power and low-temperature environments.
Aqueous zinc-ion batteries (AZIBs) are the low-cost and safe secondary battery technology with great application prospects, but remain hindered by the severe Zn-electrolyte interface compatibility, especially in extreme environmental temperature. Innovative electrolyte design is the key to solving the above problems. Here, we introduce an electrolyte additive of Poloxamer 407 (P407) as a solvation restructuring agent and H2 O cluster modulator, effectively stabilizing H2 O molecules and suppressing parasitic reactions. Meanwhile, P407 facilitates the formation of a stable solid electrolyte interphase (SEI) composed of organic-inorganic composite, thereby improving the interfacial chemistry. More importantly, the thermoreversible gelation property of P407 enhances the system's high-temperature stability by forming micelle network structures that effectively retains H2 O molecules, while at low temperature, it maintains the fluidity of the electrolyte, ensuring efficient ion transport. By using P407-containing electrolyte, the Zn anode achieves long cycling life of 40 0 0, 850, and 10 0 0 h at 30, 60 and -30 degrees C, respectively. Moreover, the modified electrolyte enables the Zn-V2 O5 full cells to achieve excellent rate performance and cycling stability in a wide temperature range from -30 degrees C to 60 degrees C. This study highlights a simple yet effective strategy for electrolyte modification using P407, providing a pathway toward the development of high-performance AZIBs with broad temperature adaptability. (c) 2026 Published by Elsevier B.V. on behalf of Chinese Chemical Society and Institute of Materia Medica, Chinese Academy of Medical Sciences.
Direct regeneration of spent LiFePO4 (SLFP) cathode materials is crucial for the sustainable development of new energy vehicles and other energy storage sectors. However, challenges persist in conventional regeneration technology, including severe secondary pollution, low economic efficiency, and a complex regeneration process. Herein, a direct regeneration strategy for SLFP is proposed through a water bath approach, wherein the synergistic interplay between Glycine as the reducing agent and Li2CO3 as the lithium source profoundly influences the regeneration of the SLFP. The direct regeneration mechanism reveal that the synergistic interaction of the reducing agent and the lithium source contribute to facilitating re-lithiation and lattice restoration, wherein Glycine as an electron donor to create a reductive environment to transform Fe(III) into Fe(II) and Li2CO3 as the lithium source is synchronously reintroducing to repair the FeLi anti-site defects in the lattice, thereby achieving the regeneration LFP (RLFP). Moreover, the nitrogen that derives from the amino groups in Glycine is doped into the carbon layer of the RLFP, offering more active sites to enhance Li+ migration kinetics, thereby endowing the RLFP with excellent rate capability. The RLFP demonstrates excellent electrochemical performance with an initial discharge capacity of 155.7 mAh g- 1 at 0.1C and capacity retention of 92% after 200 cycles at 0.5C. This strategy inspires novel insights into the in situ direct regeneration of the SLFP cathode materials.