Hard carbon anodes are important to the commercialization of sodium-ion batteries (SIBs), but their electrochemical performances are still limited by low reversible capacity and poor Coulombic efficiency. Lignocellulosic biomass waste is a promising precursor, but the thermochemistry of biochar formation that controls the development of its critical microstructure, closed nanopores and enlarged interlayer distance remains poorly understood. The temperature-driven pyrolysis of the biomass is inevitably accompanied by decomposition, leading to porous structures that facilitate electrolyte side reactions. Here, we show that a pre-carbonization strategy can regulate biochar microstructure through tuning the competition between decomposition and cross-linking in a model biomass waste, mangosteen shells. By optimizing pre-carbonization and the subsequent carbonization, we guide the microstructure evolution to produce a hard carbon that possesses both short-range ordered carbon layers with expanded interlayer distance and abundant closed nanopores, while minimizing specific surface area. These structural features enable highly reversible pore-filling charge storage and rapid Na+ diffusion, delivering a high reversible capacity of 309 mAh g-1 and a high initial Coulombic efficiency (ICE) of 81.8%. Our findings highlight the importance of temperature-driven thermochemistry and microstructure evolution of biomass, which can shed light on electrochemical reactions wherever carbon plays a crucial role.
The stable modulation of the local charge distribution behavior induced by unsaturation sites within photocatalysts continues to pose a significant challenge in the quest to achieve notable enhancements in photocatalytic activity. Herein, we harnessed the hydrogen annealing reduction technique to deliberately introduce oxygen vacancies (OVs) into the BiOCl lattice for constructing the OVs-Bi-O structure, which decreases the valence state of Bi, and diminishes the Bi─O coordination, further establishing a charge asymmetric region within the material. This distinctive structural arrangement facilitates the sufficient migration of electrons to adjacent Bi sites that are closely linked to the OVs, significantly promoting the capture capability of electrons, leading to more adsorption and activation of water and oxygen as well as the conversion of reactive oxygen radicals. The engineered OVs-BiOCl variant showcases potential photocatalytic prowess, boasting a satisfactory photocatalytic application than that of its unmodified BiOCl counterpart. Under low-light conditions, this variant impressively achieves a ∼98.1% removal efficiency for RhB, while concurrently achieving an almost complete elimination of E. coli. This finding presents an insightful approach for manipulating unsaturation coordination active sites through the strategic introduction of controllable defects and elucidates the impact of unsaturation coordination on photocatalytic efficiency.
Ultraviolet radiation induces skin carcinogenesis through DNA damage and oxidative stress, driving demand for high-efficacy sunscreens. Current organic filters (e.g., octyl methoxycinnamate, OMC) suffer from narrow spectral coverage and phototoxicity. To address these limitations, we engineered OMC-loaded hollow mesoporous silica nanoparticles with polydopamine coating (OMC@HMSN@PDA). This nanoplatform achieved: (i) synergistic broad-spectrum protection, the sun protection factor (SPF) and UVA protection factor (UVAPF) up to 54 ± 0.74, 26.8 ± 6 with the concentration of 6 wt% OMC respectively, exceeding OMC@HMSN by 10.4-fold in UVB and 11.2-fold in UVA attenuation; (ii) 93.1 ± 1.2 % of DPPH and 98.5 ± 2.5 % of ABTS radical scavenging at 10 µg mL-1, and 94.6 ± 0.03 % intracellular reactive oxygen species (ROS) suppression; and (iii) prevention of the payload leakage and photo-instability of OMC, resolution of OMC's phototoxicity with above 80 % cell viability in vitro. In vivo studies demonstrated prevention of UV-induced epidermal hyperplasia and lower inflammation. This technology establishes a promising approach for photoprotection integrating UV filtering, antioxidant activity, and enhanced safety.
The global shortage of freshwater resources and the increasing contamination from dye wastewater have made the development of efficient and stable water treatment materials a critical research focus. In this study, a micronano composite porous carbon-based filter membrane, denoted as PF-AC, was fabricated using phenolic resin (PF) as the carbon precursor, activated carbon (AC) as the functional adsorbent unit, and polyethylene glycol (PEG) as a pore-forming agent via hot-pressing and high-temperature carbonization. The work systematically examined the influence of PEG content on the membrane's microstructure, thermal stability, mechanical properties, hydrophilicity, and dye adsorption-separation performance. Additionally, the effects of solution pH and initial dye concentration on methylene blue (MB) removal were investigated, along with the membrane's regenerability and continuous operational stability. The results demonstrated that under optimal conditions-with a PF:AC mass ratio of 11:9 and PEG content of 5 wt%-the membrane exhibited a specific surface area of 415.2 m2 & sdot;g- 1, a removal efficiency of 92.11% for 200 mg & sdot;L- 1 MB solution, a pure water flux of 147.81 L & sdot;m-2 & sdot;h-1 at 3.5 bar, and a tensile strength of 0.08 MPa. Alkaline conditions significantly enhanced MB adsorption performance. After 10 consecutive adsorption-desorption cycles, the removal rate remained as high as 99.25%, and the membrane showed stable performance during continuous filtration of 5 L of MB solution. This composite membrane achieves a synergistic combination of efficient adsorption and separation, offering a novel, high-performance, and low-cost carbon-based material for the treatment of dye-contaminated wastewater.
Designing heterostructured electrode materials with tunable morphology can effectively enhance energy storage performance. Herein, we report a synergistic hydrothermal-carbonization strategy to construct a carbon-assisted graphitic carbon nitride and cobalt oxide composite for high-performance supercapacitors. This method creates a tightly integrated ternary architecture in which cobalt oxide nanoparticles are anchored on graphitic carbon nitride and interconnected by a cotton-derived conductive carbon framework. Structural and morphological analyses confirm the formation of a uniform, tightly integrated composite with cobalt oxide nanoparticles well-dispersed within the carbon-assisted graphitic carbon nitride framework. This configuration provides a dense array of electrochemically active sites, creates a favorable interfacial environment, and facilitates efficient charge transport. Consequently, the composite electrode delivers a remarkable specific capacitance of 346.22 F g(-1) at 1 A g(-1), significantly surpassing its individual components. Furthermore, the electrode exhibits good rate capability (84.91% retention from 1 to 2 A g(-1)) and remarkable cycling stability (87.95% after 10,000 cycles at 15 A g(-1)). These results highlight the strong potential of carbon-assisted graphitic carbon nitride and cobalt oxide as a scalable, eco-friendly electrode material for high-performance supercapacitors.
Polymer-based dielectric capacitors with high discharge energy density (U-dis) at high temperatures are urgently demanded in advanced power electronics (e.g., electric vehicles, aerospace). However, existing polymers suffer from low U-dis at high temperatures owing to low thermal conductivity (k), dielectric constant (epsilon(r)) and breakdown strength (E-b), hindering their applications in high-performance devices. Herein, we propose a multi-scale strategy to design a bamboo-structured multilayer composite by introducing 2D Na0.5Bi4.5Ti4O15 (NBT) microsheets and boron nitride (BN) nanosheets to the Polyetherimide-co-Polysulfone (PEIS) matrix to resolve the above issue. Excitingly, the k, epsilon(r) and E-b values of the composites were significantly enhanced at high temperatures owing to much higher k value of BN, the effective electric barrier effect of NBT fillers, and the combination of those merits via designing bamboo structure. Consequently, a record-high U-dis of 9.66 J cm(-)(3) was achieved from the six-layer bamboo-structured NBT-PEIS/BN-PEIS (PEIS-6) composite at 150 degrees C together with a high efficiency (eta) > 90 %, and it maintains to be high as 7.30 J cm(-)(3) at 200 degrees C together with eta > 90 %. Those properties are much superior to those of previously reported polymer-based dielectric materials. Moreover, the cyclic charge-discharge measurements prove that the PEIS-6 composite can work stably at high temperatures. This work provides a novel strategy for developing high-performance polymer-based dielectric capacitors at high temperatures.
A dual-modification strategy integrating hydrogenation with plasma-enhanced atomic layer deposition (PE-ALD) is developed to address bulk carrier recombination and sluggish OER kinetics in TiO₂ photoanodes. Oxygen vacancies (Ov) introduced by hydrogenation broaden light response and suppress bulk charge recombination, while ALD-deposited Co nanoparticles form a Schottky junction serving as hole-trapping centers, reducing OER overpotential and extending carrier lifetime. The optimized TNB-H2@Co-200 photoanode achieves a photocurrent density of 1.02 mA cm−2 at 1.23 V vs. RHE under AM 1.5G illumination — about five times that of pristine TiO₂ — demonstrating outstanding PEC performance.
Graphene exhibits exceptional physical properties, yet its strong interlayer van der Waals interactions and hydrophobic nature lead to severe aggregation in aqueous environments, limiting scalable processing. While peptide-assisted dispersion offers a promising green strategy, the molecular mechanisms linking peptide structure to dispersion efficiency remain unclear. Here, all-atom molecular dynamics simulations selected homo-peptides polymerized from a single amino acid to investigate the role of peptide side-chain chemistry in regulating graphene dispersion systematically. Ten representative peptides with distinct side-chain structures were examined by analyzing water intercalation behavior, interlayer solvent-layer stability, and graphene re-aggregation dynamics. Radial distribution functions, graphene normal-vector evolution, and peptide density distributions were used to resolve interfacial interactions at the molecular scale. The results reveal that graphene dispersion is governed by a synergistic "anchoring-attraction" mechanism. N-containing peptides simultaneously achieve strong surface anchoring and effective hydration, which promote water intercalation, stabilize interlayer solvent layers, and suppress re-aggregation. In contrast, non-N-containing peptides fail to achieve efficient dispersion due to a deficiency in either anchoring (e.g., negatively charged carboxyl peptides) or attraction (e.g., hydrophobic alkyl peptides). Among the N-containing structures, positively charged side-chains exhibit the highest dispersion efficiency. Moreover, dispersion performance increases with polymerization degree and concentration within an optimal range, beyond which chain entanglement or self-aggregation deteriorates stability. This work establishes a clear structure-interfacial behavior-dispersion relationship, providing molecular-level guidance for designing efficient and environmentally benign graphene dispersants centered on N-containing structural motifs.
Achieving both high energy storage density and excellent thermal stability in lead-free multilayer ceramic capacitors (MLCCs) has long been a critical challenge for advanced electronic systems. To address this issue, we propose an innovative strategy to simultaneously improve both properties by constructing ordered heterogeneous interfaces through embedding parallel-aligned Al2O3 plates in 0.6SrTiO(3)-0.4Bi(0.5)Na(0.5)TiO(3) (0.6ST-0.4BNT) lead-free ceramics. This approach effectively suppresses the charge carrier injection and transport, yielding an ultrahigh recoverable energy storage density of 16.0 J cm(-3) with a giant breakdown strength of 1140 kV cm(-1) in Al2O3 modified 0.6ST-0.4BNT based MLCCs, which outperforms most state-of-the-art dielectric ceramics. Furthermore, the MLCCs exhibit superior thermal stability with variation less than 3% across a broad temperature range of 20-160 degrees C. The overall superior performance underscores the potential of the ordered heterogeneous interface engineering in advancing the thermally stable high-density energy storage materials for next-generation MLCC applications.
Li-rich layered oxide (LLO) cathodes possess high theoretical capacity and voltage, but constructing cathodes with high active material fractions to achieve high energy density in all-solid-state batteries (ASSBs) remains challenging. In this work, it is demonstrated that the main limitation to electrochemical performance lies not in interfacial instability but in sluggish Li+ transport arising from intra- and interparticle voids. Intraparticle voids are found to hinder ion diffusion within polycrystalline LLO, while extensive interparticle voids are introduced in reduced-particle-size LLO due to particle aggregation under limited solid-state electrolyte content. In these aggregated domains, Li+ conduction is restricted to isolated LLO regions and the intrinsically low ionic conductivity of LLO further aggravates transport limitations. To address these issues, a composite cathode with a Li3InCl6 coating was designed to improve the interfacial contact and Li+ conduction pathways. The resulting ASSB delivers 245.2 mAh/g at 0.1 C, retains 80.9% capacity after 250 cycles at 0.3 C, and maintains 75.9 mAh/g at 5 C with only 27.5 wt % Li3InCl6. This work provides a practical cathode design strategy for realizing high-energy-density LLO-based halide ASSBs.
Anode-free sodium metal batteries (AFSMBs) are promising because of their high energy density, sustainability and affordability. However, their solid electrolyte interphase (SEI) must be improved to mitigate the deterioration of cycling stability due to the zero-sodium inventory at the anode. SEI stabilization for AFSMBs has been widely executed with fluorinated solvents and high-concentration salts, yet their high cost and environmental impact limit practical viability. Herein, we demonstrate interphasial catalytic anion reduction (ICAR) effect that selectively forms a stable NaF-rich SEI for improved cycling performance of AFSMBs. We found that malonic acid, as a molecular electron transfer facilitator, can expedite the anion reduction kinetics by the dipole moment effect that selectively decreases the P-F bond dissociation energy. This process results in enriched inorganic NaF in SEI, thereby enhancing its stability. This ICAR strategy allows an average Coulombic efficiency (CE) of 99.95% over 1000 cycles for sodium plating/stripping. This strategy further enables a high-loading cathode (>14 mg cm-2) AFSMB with 0.11% capacity decay per cycle over 300 cycles, and a 3-Ah pouch cell delivering 212 Wh kg-1. Such performance surpasses most previously reported values. This work offers a new avenue for building robust interphases toward next-generation anode-free batteries.
Faced with global energy sustainability and carbon neutrality demands, single-walled carbon nanotubes (SWCNTs) are promising for flexible thermoelectric (TE) applications but limited by severe agglomeration, high intrinsic thermal conductivity, and poor air stability of n-type derivatives. Herein, we report a novel n-type triethylene glycol/polyethyleneimine/SWCNT (TEG/PEI/SWCNT) composite film via facile drop-casting, where TEG (key co-dopant) dominates PEI/SWCNT interfacial regulation. TEG forms strong intermolecular interactions with PEI, remarkably enhancing PEI wettability on SWCNTs. This TEG-mediated interface modulation facilitates SWCNT dispersion into uniform networks (well-controlled bundle diameters), strengthens inter-bundle bonding (boosting carrier mobility and suppressing air molecule intrusion), and optimizes PEI-to-SWCNT carrier injection, alleviating excessive carrier concentration while increasing the Seebeck coefficient. The TEG-modulated film exhibits excellent performance: maximum power factor (PF) of 122 mu Wm-1K-2 at room temperature, 13-day stable n-type characteristics in ambient air, and monotonically increasing electrical conductivity up to 160 degrees C. A flexible TE device (five p-n junction pairs) based on this composite delivers 2.9 mu W maximum output power under a 50 K temperature gradient. This TEG co-doping strategy, centered on precise PEI/SWCNT interface regulation, offers a simple, scalable route to high-performance flexible n-type carbon-based TE films, addressing key SWCNT-based TE bottlenecks.
Achieving ultrahigh energy storage in lead-free dielectric ceramics is fundamentally constrained by the intrinsic trade-off between large polarization and high dielectric breakdown strength. Here, we establish an interpretable machine-learning-guided design framework that quantitatively links ionic descriptors with polarization behavior in ABO3-based dielectric matrices, enabling the rational identification of compositions with intrinsically high polarization potential. Guided by this strategy, a (Bi0.275Na0.2255K0.0495Ba0.3)(Ti0.985Hf0.015)O3-0.15(La0.5Sm0.5)2Ti2O7 (BNBT-3) composition is discovered that exhibits an exceptional maximum polarization of 50.19 µC cm-2. When processed via a viscous polymer process, the resulting BNBT-3-VPP capacitors achieve an ultrahigh breakdown strength of 1400 kV cm-1 and a recoverable energy density of 25.1 J cm-3 with high efficiency, placing them among the best-performing lead-free dielectric ceramics reported to date. Structural characterization combined with phase-field simulations reveals that the outstanding performance originates from polarization-lattice decoupling, where nanoscale polarization clusters and multiphase coexistence suppress long-range ferroelectric order while enabling reversible polarization rotation. This work establishes a generalizable strategy that integrates interpretable machine learning with physically grounded materials design, providing a powerful route for discovering high-performance dielectric energy storage materials.
Piezocatalysis facilitates the transduction of mechanical energy into chemical redox processes, but its practical application is hindered by intrinsically low catalytic efficiency and complex catalyst fabrication. Herein, we employ high-energy ball milling (HBM) to convert bulk lead-free Sr0.5Ba0.5Nb2O6 (SBN) ceramics into nanoscale piezocatalysts (SBN-HBM) with enhanced activity, and integrate them with peroxymonosulfate (PMS) activation to promote reactive oxygen species generation, thereby boosting overall catalytic performance. HBM refines grain size from the microscale to similar to 240 nm and introduces abundant oxygen vacancies, enhancing both piezoelectric polarization and surface reactivity. Under mechanical excitation, the integrated SBN-HBM/PMS system triggers synergistic oxidation featuring hydroxyl radicals (center dot OH), sulfate radicals (SO4 center dot-), and piezo-induced holes, resulting in markedly accelerated degradation kinetics (e.g., k = 0.520 min(-1) for methyl orange, 0.356 min(-1) for tetracycline) and achieving > 99% bacterial inactivation. Experimental results and theoretical analyses reveal that defect-polarization coupling critically governs carrier separation dynamics and facilitates efficient redox reactions. This work offers a green and scalable strategy for transforming bulk piezoceramics into highly efficient piezocatalysts for decentralized wastewater treatment.
Polymer dielectrics capable of operating at elevated temperatures are essential for advanced capacitive energy-storage systems. However, thermally activated charge injection and interfacial electric-field distortion severely degrade breakdown strength and energy density under high-temperature conditions. Here, we report a CaF2@SiO2 core-shell architecture to regulate the interfacial electronic structure in polyetherimide (PEI) dielectrics. The ultrathin SiO2 shell simultaneously establishes a dielectric gradient and a stepwise energy-level barrier across the CaF2-SiO2-PEI interface. This dual-gradient (dielectric and energy-level) interfacial configuration suppresses thermally activated carrier transport, mitigates interfacial charge accumulation, and homogenizes local electric-field distribution. Consequently, the PEI/CaF2@SiO2 composite achieves a high recoverable energy density of 6.71 J cm-3 at 150 degrees C under 650 MV m-1 with high efficiency and maintains 5.68 J cm-3 at 200 degrees C. The composite also exhibits excellent cycling stability over 50,000 cycles and ultrafast discharge characteristics. This work provides an effective strategy for integrating energy-level regulation, trap engineering, and electric-field homogenization in polymer dielectrics for reliable high-temperature energy storage.
Dielectric capacitors, characterized by ultra-fast charge/discharge speeds and high power densities, are widely used in modern electronic power systems. However, their low energy density and poor thermal stability limit applications. In this study, SrBi3.25La0.75Ti4O15 (SBLT) ferroelectric thin films were prepared by the sol–gel method. We systematically investigated the effect of annealing temperature on microstructural evolution, electrical properties, and energy storage performance. The SBLT film annealed at 700 °C exhibited optimal performance, achieving a balanced enhancement in polarization and breakdown strength, with an energy storage density of 48.66 J cm−3 and an efficiency of 78%. The material also demonstrated excellent thermal stability (30–175 °C) and frequency stability (0.1–100 kHz). These findings not only validate the potential of SBLT as a next-generation energy storage dielectric but also provide a practical solution for applications in semiconductor technology.
Lignin, a natural aromatic biopolymer, is often recovered as low-value by-product during the delignification process of lignocellulosic biomass for producing cellulosic pulps. In this study, crude alkaline lignin (CAL) derived from the NaOH-pretreated sugarcane bagasse was used to produce hard carbon (HC) for sodium-ion battery anode applications. The results showed that the direct use of CAL led to HC with a maximum initial Coulombic efficiency (ICE) and reversible capacity of only 60.2% and 198.5 mAh g ^−1, respectively. To improve the electrochemical performance, solvent extraction was applied to purify CAL. The use of purified alkaline lignin (PAL) led to HC with a maximum ICE of 76.1% and reversible capacity of 277.5 mAh g ^−1 , which were significantly higher than CAL-derived HC. The effects of carbonization temperature (1200 °C–1400 °C) and heating rate (1 °C–8 °C min ^−1 ) were also examined. Structural analyses revealed that hemicellulose removal resulted in HC with favorable microstructural structures, including short-range graphitic layers, closed pores, and reduced defects, facilitating the storage of Na ions. Additionally, the overall yield of PAL-HC was comparable to CAL-HC. These results demonstrated that the removal of hemicellulose is a critical initial step toward improving the electrochemical performance of HC before the application of other strategies.
Metastable materials are considered promising electrocatalysts for clean energy conversions by virtue of their structural flexibility and tunable electronic properties. However, the exploration and synthesis of metastable electrocatalysts via traditional equilibrium methods face challenges because of the requirements of high energy and precise structural control. In this regard, the rapid synthesis method (RSM), with high energy efficiency and ultra-fast heating/cooling rates, enables the production of metastable materials under non-equilibrium conditions. However, the relationship between RSM and the properties of metastable electrocatalysts remains largely unexplored. In this review, we systematically examine the unique benefits of various RSM techniques and the mechanisms governing the formation of metastable materials. Based on these insights, we establish a framework, linking RSM with the electrocatalytic performance of metastable materials. Finally, we outline the future directions of this emerging field and highlight the importance of high-throughput approaches for the autonomous screening and synthesis of optimal electrocatalysts. This review aims to provide an in-depth understanding of metastable electrocatalysts, opening up new avenues for both fundamental research and practical applications in electrocatalysis.