

Halogen Ion‐Mediated Hydrothermal Synthesis of Diverse MXenes with Tailored Heterostructures
A halogen ion-mediated strategy is proposed for the controllable preparation of diverse MXenes and their heterostructures with well-defined interfacial architectures. NH4F etchant enables potential high-throughput synthesis of Mo2CTx, while NH4X -intercalant (X = Cl, Br, I) combinations facilitate large-scale production of hetero-Mo2CTx. This moderate hydrothermal strategy achieves precise structural control on a variety of MXenes and hetero-MXenes.
Abstract
Two-dimensional transition metal carbides and nitrides (MXenes) have attracted significant attention due to their exceptional physicochemical properties. Despite extensive studies, efficient methods for the production of MXenes with precise structural control still remain a challenge, thus hindering their potential in many specific applications. Herein, a halogen ion-mediated hydrothermal approach is proposed for the controllable preparation of diverse MXenes and their heterostructures with well-defined interfacial architectures, demonstrating its potential as a high-throughput synthesis strategy. As proof of concept, Mo2C can be synthesized on a gram scale by employing NH₄F in the hydrothermal etching process of Mo2Ga2C. Subsequently, this approach is applied to various MXenes, including Ti3C2, V2C, and Nb4C3. Moreover, NH4X (X = Cl, Br, I) etchants combined with small-molecule intercalants enabled the targeted synthesis of MXene-based heterostructures, such as Mo2CTx@MoS2 featuring ≈15 nm amorphous MoS2 surface layers. Notable, the Mo2CTx(Br) heterostructure exhibited outstanding electrochemical stability, delivering a capacity of 465.5 mAh g⁻¹ after 300 cycles at 1 A g⁻¹, and achieving high coulombic efficiency of 99.8% during lithium-ion battery cycling. This work establishes a versatile and scalable platform for the synthesis of MXene-based materials, thus paving the way for accelerating their potential in various fields.
Immobilization of H2O in Diffusion Channel of Metal–Organic Frameworks for Long‐Term CO2 Capture from Humid Flue Gas
A strategy to immobilize water molecules within a robust metal–organic framework significantly enhances CO2 adsorption at low concentrations. The optimized channels by functional group regulation and water molecules immobilization in this unique MOF material facilitate the long-term viability of CO2 capture in humid flue gas. This counter-intuitive approach transforms the presence of water into favorable conditions for CO2 capture.
Abstract
Utilizing physisorption for CO2 capture in humid flue gas presents challenges, with H2O molecules either damaging the adsorbent or competing with CO2 for adsorption, compromising long-term stability. Herein, a counter-intuitive strategy is proposed to address this issue by immobilizing H2O into metal–organic framework (TYUT-ATZ, TYUT = Taiyuan University of Technology, ATZ = 3-amino-1,2,4-triazole) as binding sites for CO2 capture from humid airflow. Through tailoring the -NH2 group numbers and pore sizes creates ingenious H2O sites, preserving CO2 adsorption space and enhancing CO2 adsorption interactions in 1D channels. The well-constructed TYUT-ATZ-β demonstrates a high CO2 adsorption capacity (62.7 cm3 cm−3) at 0.15 bar and outstanding CO2/N2 (15/85) selectivity (2031) at 298 K, while also exhibits the highest CO2/H2O uptake ratio in humid flue gas due to its excellent water stability and unique H2O site. Consequently, it shows top-performing CO2 enrichment ability with easy regeneration in long-term separation experiments (over 100 cycles) under high-humidity (75% RH). Gas adsorption isotherms, single-crystal analysis, selectivity calculations, and contrastive breakthrough experiments comprehensively validate this artful H2O immobilization strategy in MOFs for efficient CO2 capture in humid flue gas, satisfying the application requirements of high selectivity, rapid regeneration, and long-term stability.
A Non‐Concentrated Gradient‐Solvation Electrolyte Enables a High‐Voltage Lithium Metal Battery with 447.6 Wh Kg−1
A novel non-concentrated gradient-solvation electrolyte, featuring a DEE-rich Li+-solvated core and a FEC-rich Li+-solvated shell, is designed for high-voltage lithium metal batteries. The hierarchical solvent coordination environments offer high redox stability and fast charge transfer kinetics, thereby greatly stabilizing the high-voltage NCM811 cathode phase structure and lithium metal interface during long cycles.
Abstract
High-voltage lithium (Li) metal batteries (LMBs) emerge as a pivotal strategy for achieving high energy density applications. However, the electrolyte instability leading to inferior rate performance and short lifespan remains to be addressed. In this study, a new non-concentrated gradient-solvation electrolyte by solvent polarity discrepancy is developed. A highly donor-capable ether forms the Li⁺-solvated core through strong ion-dipole interactions, while a weakly donating carbonate creates the shell structure. Such a gradient-solvation structure enables the electrolyte with a high oxidation voltage (4.6 V vs. Li/Li+) and rapid Li+-desolvated kinetic. Consequently, the electrolyte facilitates the LiNi0.8Co0.1Mn0.1O2 (NCM811)||Li cells to attain a specific capacity of 165.8 mAh g−1 at 5C, alongside 1000 stable cycles at 1C charge/3C discharge with 66% capacity retention. Even under lean conditions (N/P = 1.5, electrolyte: 20 µL), NCM811||Li cell still maintains 97.5% capacity retention over 100 cycles. Furthermore, a 3.2 Ah pouch cell achieves a specific energy density of 447.6 Wh kg−¹ with stable cycling. These findings highlight the promise of gradient-solvation electrolytes for high-voltage LMBs applications.
Spin‐polarized Acidic Water Electrolysis with Antenna‐Reactor Plasmonic Electrocatalysts
A chiral plasmonic antenna–reactor electrocatalyst, integrating Au nanoflowers as the antenna and iridium single atoms as the reactor, achieves spin-polarized and light-driven water electrolysis in acidic media. The catalyst exhibits high activity and durability, enabled by hot-carrier transfer and the CISS effect, as supported by operando spectroscopy and DFT simulations.
Abstract
Water electrolysis, driven by renewable electricity, offers a sustainable path for hydrogen production. However, efficient bifunctional electrocatalysts are needed to overcome the high overpotentials of both the oxygen evolution reaction and hydrogen evolution reaction. To address this, a novel catalyst system is developed integrating plasmonic nanoreactors with chirality-induced spin selectivity. In this system, chiral Au nanoparticles act as antennae, while single-atom iridium serves as the catalytic reactor, achieving a 3.5 fold increase in reaction kinetics (at 1.57 V vs RHE) compared to commercial IrO2 catalysts and enhancing durability by over 4.8 times relative to conventional Pt/C || IrO2 systems. Density functional theory and operando X-ray absorption spectroscopy reveal that plasmon-driven spin alignment polarizes the Ir atom, significantly enhancing stability (>480 h at 100 mA cm−2) under acidic conditions. This work represents a major advance in spin polarization for plasmonic electrocatalysis, offering a new route to sustainable energy solutions.
Enhanced Electrical Interfaces in Flexible 2D Material Transistors via Liquid Metal and Ionic Liquid Injection
A novel paradigm of flexible transistor featuring solid–liquid hybrid interfaces is presented, where liquid metal and ionic liquid, confined in microchannels, serve as the source/drain electrodes and gate dielectric, respectively. Benefiting from the liquids' inherent softness and damage-free processing, Fermi level pinning is significantly mitigated to a factor of ∣s∣= 0.7, achieving a subthreshold swing of 60.7 mV dec−1, near the theoretical limit.
Abstract
Contact engineering at the semiconductor–electrode and semiconductor–dielectric interfaces is critical to the performance of electronic devices, especially for delicate 2D semiconductors. Here, this study proposes a new paradigm of flexible field-effect transistors featuring solid–liquid hybrid interfaces, in which liquid metal and ionic liquid, confined within microchannels, function as the source/drain electrodes and gate dielectric, respectively. These interfaces provide MoS₂ with undisturbed, atomically smooth electrical contacts, and enable efficient gate control via electric double layers. Benefiting from the inherent softness of liquids and their damage-free processing, Fermi level pinning is significantly mitigated by the liquid metal, achieving a pinning factor |s| = 0.7. Meanwhile, the ionic liquid enables a subthreshold swing of 60.7 mV dec−1, approaching the theoretical thermal limit. Furthermore, our flexible transistors demonstrate multifunctionality as enhanced logic gates, low-voltage inverters, and ultra-high-linearity synaptic devices. This work underscores the promise of liquid-enabled contact strategies for advancing low-power, flexible electronics and soft robotic systems.
Reversible Phase Transitions of Anionic and Cationic Surfactant Mixtures Drive Shape Morphing Droplets
A light-controlled, reversible phase transition of ionic surfactant assemblies, coupled with dynamic partitioning between bulk phases and interfaces, induces rapid, and order-of-magnitude changes in oil–water interfacial tension. Surpassing the capabilities of conventional stimuli-responsive surfactants, this transient, collaborative mechanism enables multimodal droplet shape transformations and offers a new strategy for the design of programmable, hierarchically structured, all-liquid matter acting with physicality.
Abstract
Converting chemical signals into mechanical responses is fundamental to biological systems, driving processes such as cellular motility and tissue morphogenesis. Yet, harnessing chemo-mechanical signal conversions in synthetic systems remains a key challenge in energy-dissipative materials design. While droplets can move and interact with their environment reminiscent of active biological matter, chemo-mechanical interactions are limited by the translation of chemical changes into extensive force variations required on small timescales. Droplets naturally adopt spherical shapes to minimize surface-energy and restructuring liquids into non-equilibrium geometries requires mechanisms beyond current stimuli-responsive surfactant systems, which lack the force-amplifying mechanisms needed for transient liquid structuring. Here, a spring-like charging and latch-controlled release mechanism is introduced for actuating droplets. This is based on reversible, light-induced crystal-to-coacervate phase transitions of photo-responsive surfactant assemblies, namely between anionic sodium dodecylsulfate and cationic azobenzene-based surfactants. During phase-transition, reversible partitioning of the surfactants into the oil or aqueous phases of the emulsion transiently induce rapid changes in interfacial tensions, which are up to 900 times greater than those observed for conventional stimuli-responsive surfactant systems. The insights into this novel chemo-mechanical transduction mechanism provide new control over purely liquid systems, paving the way for programmable, hierarchically structured, all-liquid matter acting with physicality.
Semiconducting Pt Structures Stabilized on 2D MoS2 Crystals Enable Ultrafast Hydrogen Evolution
The interaction of small Pt particles with 2D MoS2 crystals can stabilize bilayer Pt structures, with a semiconducting electronic structure. The semiconducting electronic structure of Pt bilayers constitutes the so far unexplored transition domain between the bulk-like, metallic band structure of compact nanoparticles and the discrete atomic orbitals of single atoms, while, remarkably, displaying the highest intrinsic activity among them.
Abstract
Metallic platinum is the best and most widely investigated catalyst for hydrogen evolution, yet little is known about Pt in its semiconducting form. Here, it is shown that semiconducting Pt structures with a thickness of only two atomic layers (0.4 nm) can be stabilized on 2D MoS2 crystals. Reducing the thickness of Pt particles below the Fermi wavelength (0.5 nm) opens a sizeable (0.3–0.4 eV) gap in their electronic structure. The resulting electronic structure is qualitatively different from both the metallic bands of larger Pt nanoparticles and the atomic orbitals of Pt single atom catalysts while displaying the highest intrinsic activity among them. Semiconducting Pt bilayers enable H2 production at ten times higher rates (≈1400 H2 s−1 @ η = 100 mV) than Pt single atom catalysts, and match the activity of commercial Pt nanoparticles (Pt /C catalysts) at three orders of magnitude lower Pt loadings.
Revealing Redox‐Mediated CO2 Reduction Reaction Mechanisms in Aprotic Li–CO2 Batteries
A current-density-dependent redox-mediated CO₂ reduction reaction (CO2RR) pathway is unveiled in aprotic Li–CO2 batteries through multimodal in situ spectroscopic techniques. It is found that the low-current-densities operation reduces the activation barrier of CO2RR while facilitating PQ regeneration for sustained redox cycling, thereby enabling a remarkable reduction in overpotential and increase in discharge capacity.
Abstract
Redox-mediated electrocatalysis represents an innovative strategy to unlock the energy capabilities of aprotic Li–CO2 batteries by enabling solution-mediated CO2 reduction reaction (CO2RR). However, the underlying reaction pathways remain incompletely understood due to the lack of direct molecular evidence. Herein, multimodal in situ spectroscopic techniques are integrated with theoretical calculations to interrogate a model 9,10-phenanthrenequinone (PQ)-mediated CO2RR. Direct spectroscopic evidence reveals a current-density-dependent CO2RR pathway: the reduced PQ reacts with CO2 to form metastable Li2(PQ-CO2) adduct via ECE and EEC pathways at low and high current densities, respectively. Subsequently, the metastable Li2(PQ-CO2) adduct dissociates to form the LiCO2 intermediate and regenerate LinPQ (n = 0 and 1 at low and high current densities, respectively). Two LiCO2 intermediates dimerize to produce the final discharge products of Li2CO3 and CO in bulk solution. Therefore, the operation of Li–CO2 batteries at low-current densities reduces the activation barrier of CO2RR and regenerates PQ for sustained redox cycling, enabling significantly minimized overpotential and enhanced discharge capacity. Additionally, the suppression effects of weakly acidic cations (e.g., K+, TBA+) are elucidated for the redox-mediated CO2RR. This work highlights the pivotal chemical dissociation step in PQ-mediated CO₂RR and provides a mechanistic framework for designing better metal–CO2 batteries.
Ion‐Framework Electrolyte Featured Zinc‐Ion Transport for Solvent and Interphasial Co‐Passivation
This report designs an ion-framework electrolyte to passivate solvent and interphase. Such electrolyte systems simultaneously yield a wide electrochemical stability window and robust SEI, which fill a gap in current Zn2+ electrolytes.
Abstract
The rapid application of zinc-ion (Zn2+) energy storage lacks favorable solvation structures to simultaneously form inert electrolyte environments and robust solid electrolyte interphase (SEI), which means that Zn2+ devices cannot synchronously against the side reactions, Zn dendrites and narrow electrochemical stability windows, further hindering their wide operative voltage window and ultra-long service life. Here, ion-framework electrolytes are designed by using large-sized inert-ammonium salts as the main solute. The ion framework, assembled from ultra-large solvation ion clusters containing large tetraethylammonium cations, large anions, and abundant solvents via electrostatic interactions, not only forms suitable channels for Zn2+ transport but also constrains free solvents to passivate their electrochemical activity, achieving an ultra-wide electrochemical stability window about 3.72 V. More importantly, the enrichment of the ion framework at Zn interface generates a homogenous SEI with the dense polymer-inorganic hybrid structure to passivate the interphasial chemistry, which eliminates the Zn dendrites and side reactions. Therefore, Zn anode using this electrolyte achieves the ultra-long cycling stability of 8,150 h, and Zn metal||activated carbon capacitors exhibit a high operative voltage (0–2.1 V) and ultra-long cycle life (≈170,000 cycles at 10 A g−1). This electrolyte design principle is promising for addressing the typical challenges in other metal-ion systems.
Restoring Ultra‐Flat Bridgman‐Fabricated Single‐Crystal Cu(111) Wafers via Recrystallization Arrest Strategy for High‐Quality Graphene Epitaxy
By investigating strain- and dislocation-induced recrystallization, a tailored staged annealing method with recrystallization arrest is developed to preserve single-crystallinity. Ultra-flat Bridgman-fabricated Cu(111) wafers are restored, enabling high-quality graphene heteroepitaxy on wafer-scale substrates.
Abstract
Single-crystal Cu(111) and its ultra-flat surface are crucial for the heteroepitaxy of high-quality, single-crystal graphene films with minimal folds and additional layers. Bridgman method coupled with cutting and chemical-mechanical polishing presents a straightforward and cost-effective approach for preparing ultra-flat Cu(111) wafers but is simply discarded due to its incompatibility with standard high-temperature procedures for annealing and graphene growth. Herein, an in-depth investigation is conducted into the mechanisms of recrystallization and reverse single-crystallization induced by processing strain and dislocations. A recrystallization arrest strategy is proposed for Bridgman-cutting-polishing (BCP) derived Cu(111) wafers, guaranteeing the high single-crystallinity (96.6%) and flatness (0.81 nm) of epitaxy substrates. The thorough investigation has provided a comprehensive understanding of the effects of surface roughness on the orientation, proportion of adlayers, as well as transfer qualities of graphene films. By highlighting the paramount importance of the Bridgman cutting-polishing methodology, the efforts set the stage for achieving notable cost savings in the manufacture of ultra-flat, single-crystal graphene wafers.
Unlocking the Potential of MOFs Anodes via Solid‐State Corrosion Prelithiation for High‐Energy Li‐Ion Batteries
The solid-state corrosion prelithiation strategy (SSC) is applied to MOFs. The full cell with SSC-prelithiated metal-organic frameworks (MOFs) anode enables an energy density of 493 Wh kg−1 with 83.3% capacity retention after 240 cycles at 0.2 C. The Ni dissolution percentage is reduced from 15.32% to 1.16%, identified as the key factor underpinning the enhanced full cell performance.
Abstract
Pristine metal-organic frameworks (MOFs) with their excellent cycling stability and high capacity are considered as promising next-generation anode materials for advanced high-performance lithium-ion batteries. Despite extensive efforts to improve initial Coulombic efficiency (ICE) via electrochemical prelithiation, the fundamental processes governing transition metals (TMs) dissolution and associated degradation mechanisms in MOFs-based full cells remain unclear. In this study, crystalline cobalt-nickel bimetallic metal-organic frameworks CoNix-MOF (CoNix-Benzene dicarboxylic MOFs), specifically derived from benzene dicarboxylic (BDC) ligands, are selected as the target material for investigation. A solid-state corrosion (SSC) strategy for prelithiating MOFs anodes with corrosion of lithium metal is proposed for the first time. The full cell with prelithiated MOFs anode achieves an energy density of 493 Wh kg−1 and demonstrates superior cycling stability with 83.3% capacity retention after 240 cycles at 0.2 C. The SSC prelithiation strategy effectively passivates Co/Ni nanoparticles, reducing Ni dissolution percentage by an order of magnitude (from 15.32% to 1.16%), which is identified as the key factor underpinning the enhanced full cell performance. This study underscores the practical applicability of MOFs-based anodes prelithiated by the SSC strategy for achieving high-energy-density and long-cycling lithium-ion batteries.
Fiber‐Shaped Photodetectors: Fundamentals, Advances, and Perspectives
Fiber-shaped photodetectors (FPDs) are advanced wearable optoelectronic devices offering omnidirectional detection, flexibility, and weavability. This review describes the recent advances of FPDs in terms of materials engineering, fabrication technology, device design, multi-spectral detection, and wearable applications. The current challenges and prospective future directions for the development of high-performance FPDs are deeply discussed.
Abstract
Fiber-shaped photodetectors (FPDs) have emerged as a highly promising category of wearable optoelectronic devices, distinguished by their unique advantages such as omnidirectional detection capability, exceptional flexibility, weavability, and high integration potential, representing the advanced development of semiconductor fibers. This comprehensive review commences by elucidating the fundamental working principles and critical performance metrics of FPDs, with a particular focus on their responsivity, response speed, and detectivity. Key design strategies are systematically explored, encompassing material selections, device configurations, and advanced fabrication technologies. Following this, a detailed summary of recent advancements in FPDs across various spectral ranges, including ultraviolet, visible, infrared, and multi-band light detection, is provided. Additionally, the review delves into the emerging wearable applications of FPDs, such as health monitoring, optical communication, imaging sensing, and bionic perception. Finally, the current challenges and prospective future directions for the development of high-performance FPDs are outlined, particularly highlighting their integration into smart textiles for next-generation wearable systems. This review aims to furnish researchers and engineers in the field of next-generation wearable electronics with valuable insights and a strategic roadmap for further innovations in the realm of FPDs.
Reticular Photoelectrochemical Transistor with Biochemical Metaplasticity
Based on the ambipolar behavior of a metal–organic framework channel gated by a photosensitive hydrogen-bonded organic framework electrode, a reticular photoelectrochemical transistor is proposed and constructed. The device enables the biochemically modulated positive/negative photoconductivity and the aqueous metaplasticity with typical nonmonotonic enhanced depression effect region and the threshold sliding, which are explored for image recognition.
Abstract
Close imitation of synaptic metaplasticity is an important objective in the neuromorphic domain. Progress has been made in solid-state electronics with high-voltage dynamics, which, nevertheless, marks a significant inconsistency with the biological systems in aqueous media. Here, the concept of reticular photoelectrochemical transistor (RPECT) is proposed and devised that can realize metaplasticity with biochemical modulation. Based on the ambipolar behavior of a metal–organic framework channel gated by a photosensitive hydrogen-bonded organic framework electrode, biochemically modulated positive/negative photoconductivity and metaplasticity with the typical features, e.g., the nonmonotonic enhanced depression effect region and the threshold sliding are achieved. Taking advantage of such unique properties, in-sensor preprocessing and in-memory computing are further implemented for efficient image recognition. This work realizes the aqueous metaplasticity by a new device of RPECT, which also introduces the biochemical modulation into image recognition, providing a perspective for future development of machine vision processing.
Hardware Implementation of On‐Chip Hebbian Learning Through Integrated Neuromorphic Architecture
This work presents a neuromorphic hardware platform that integrates presynaptic transistors, threshold switching neurons, and adaptive feedback synapses. The architecture enables on-chip Hebbian learning through correlation-based weight updates without external training circuits. A 6 × 6 device array demonstrates stable real-time operation, offering a pathway toward efficient, scalable brain-inspired computing systems.
Abstract
The von Neumann bottleneck and growing energy demands of conventional computing systems require innovative architectural solutions. Although neuromorphic computing is a promising alternative, implementing efficient on-chip learning mechanisms remains a fundamental challenge. Herein, a novel artificial neural platform is presented that integrates three synergistic components: modulation-optimized presynaptic transistors, threshold switching memristor-based neurons, and adaptive feedback synapses. The platform demonstrates real-time synaptic weight modification through correlation-based learning, effectively implementing Hebbian principles in hardware without requiring extensive peripheral circuitry. Stable device operation and successful implementation of local learning rules are confirmed by systematically characterizing a 6 × 6 array configuration. The experimental results demonstrate a correlation between input–output signals and subsequent weight modifications, establishing a viable pathway toward hardware implementation of Hebbian learning in neuromorphic systems.
Biomimetic Engineering of Robust Gradient Antibacterial Coatings using Hollow Nanoframes of Prussian Blue Analogues
An artificial reef-like manganese-doped Prussian blue analogue (PBMn) is designed as a biomimetic cross-linker to enhance the mechanical robustness of the phytic acid-cationic polymer (PC) network. This approach enables the efficient deposition of PC-PBM on diverse material surfaces and complex geometries, facilitating the fabrication of gradient coating with optimized antibacterial performance while minimizing heat generation.
Abstract
Photothermal therapy for bacterial infections poses a significant challenge due to the high temperatures required for effective bacterial eradication, which can also harm surrounding healthy tissues. Determining the minimal effective temperature for bacterial destruction is therefore critical. In this study, artificial reef-like manganese-doped Prussian blue (PBMn) nanoframes are developed as photothermal agents and physical cross-linkers to reinforce a phytic acid and cationic polymer network coating. This innovative deposition approach facilitates the creation of a gradient PBMn-enhanced phytic acid-cationic polymer (PC-PBM) coating, achieving a balance between effective photothermal antibacterial activity and reduced heat-induced collateral damage. When applied to a polyurethane (PU) substrate, the gradient PC-PBM coating exhibits excellent photothermal efficiency, biocompatibility, and tunable antibacterial activity. Gene transcriptomics analysis demonstrates significant downregulation of virulence genes and biofilm-forming genes in pathogens following PC-PBM treatment, confirming the antibacterial efficacy of the coating. Both in vitro and in vivo evaluations, including studies in an infected hernia model, underscore the coating's excellent anti-infection performance. This work introduces a robust and biomimetic strategy for constructing gradient coating, advancing photothermal therapy by achieving effective bacterial eradication with reducing collateral damage to healthy tissues.
Fukui Function‐Engineered Gel Electrolytes: Thermodynamic/Kinetic‐Synergistic Regulation for Long‐Cycling Zinc Metal Batteries
The designed gel electrolyte, engineered through the Fukui function to synergistically modulate the thermodynamic and kinetic properties of the zinc anode interface, enables both symmetric and full-cell configurations to achieve exceptional cycling stability. Notably, the cells maintain remarkable electrochemical performance even under elevated temperature conditions. Furthermore, the corresponding pouch cells demonstrate achieved superior cycling durability and excellent mechanical robustness.
Abstract
While traditional gel electrolytes address critical issues such as electrolyte leakage and dendrite growth in zinc metal batteries (ZMBs), their intrinsic inability to suppress the competing hydrogen evolution reaction (HER) remains a fundamental limitation. Herein, a Fukui function-guided molecular engineering approach is proposed to develop a gel electrolyte (HG-3TP) with higher Gibbs free energy of HER (ΔG HER). The reduced electrophilic Fukui function inhibits Zn electron extraction while participating in Zn2⁺ solvation to decrease free water activity. Simultaneously, attenuated nucleophilic Fukui function creates an inert barrier on Zn anodes, raising H⁺ desorption energy and lowering proton diffusion. These synergistic effects suppress the Volmer/Heyrovsky step, significantly increasing ΔG HER and inhibiting HER. Meanwhile, optimized interfacial energetics facilitate uniform Zn plating/stripping while maintaining cathode compatibility. As a result, Zn batteries with HG-3TP exhibit excellent long-term cycling stability, achieving 4,000 h in Zn||Zn symmetric cells and maintaining operation for 710 h at 60 °C, while demonstrating 83.5% capacity retention over 11 000 cycles in Zn||VO2 full cells. This work establishes a thermodynamics-kinetics orchestrated paradigm through Fukui function-guided electrolyte design, advancing ultrastable ZMBs for scalable energy storage.
Unraveling the Impact of Electrosorbed Ions on the Scaling Behavior of Fast‐Charging Dynamics of Nanoporous Electrodes Toward Digital Design of Iontronic Devices
Electrosorbed ions under nanoconfinement (see TOC figure) critically reshape electrochemical potentials and impact ion transport in porous electrodes. By integrating modified Poisson–Nernst–Planck simulations with multilayered graphene membrane experiments, this study establishes a scaling relation and reveals electrosorption-enhanced transport, offering a computationally efficient framework for designing high-performance, fast-charging electrochemical and iontronic devices.
Abstract
Electrolyte-filled nanoporous electrodes with fast-charging capability are critical for advanced energy storage and iontronic devices. However, experiments and simulations consistently show that increasing electrode thickness degrades performance by limiting ion access to effective electrode/electrolyte interfaces, especially under fast-charging conditions. While often attributed to sluggish ion transport, the underlying mechanisms and the quantitative link between thickness and performance remain unclear due to complex pore structures and nanoconfined ion dynamics. Here, using multilayered graphene membranes as a model system, modified Poisson–Nernst–Planck simulations with experiments are combined to reveal how electrosorbed ions reshape local electrical and chemical potentials, particularly as the surface-to-volume ratio increases with reduced pore size. It is shown that electrosorbed ions substantially influence the scaling behavior of capacitance across electrode thicknesses, causing marked deviations from classical transmission line models as pores approach nanometric dimensions. Despite the complexity introduced by nanoconfinement, introducing a correction factor enables capacitance–scan rate relationships to collapse into a unified curve across various electrode architectures, allowing computationally efficient design of high-performance fast-charging electrochemical and iontronic devices. This work highlights the unique role of 2D nanomaterials as a versatile platform for bridging experiments and theory to address long-standing challenges in ion transport dynamics.
Ancestral Protein‐Based Lighting
The ancestral sequence reconstruction (ASR) method applied to a large dataset of modern fluorescent proteins (FPs) led to a bright ancestral-like FP suitable for photon down-conversion in bio-hybrid light-emitting diodes (Bio-HLEDs).
Abstract
Protein-optoelectronics is a paradigm toward eco-designed and sustainable technologies. The challenge is, however, how to preserve the native activity of proteins upon device fabrication/operation in non-native environments (solvents, organic/inorganic interfaces, and working temperatures/irradiations). Herein, a new vision to identify and design ancestral-like fluorescent proteins (FPs) is proposed. Using ancestral sequence reconstruction (ASR) out of a large dataset (221) of the best modern FPs suitable for photon down-conversion in bio-hybrid light-emitting diodes (Bio-HLEDs) a historical-genetic reconstruction (family tree) was obtained, identifying a possible common ancestral FP. This computationally designed protein is produced in bacteria, featuring outstanding photoluminescence quantum yields in solution (e.g., 90%/80% for green-/red-emitting forms) and a strong tendency to agglomerate in polymer coatings. This resulted in red-emitting Bio-HLEDs that outperformed the reference with ≈2-fold enhanced stabilities. The resplendent green-/red-emission of ancestral-like FP itself and its respective devices led us to coin this new protein as QuetzalFP. Overall, it is set in ASR as an effective concept to reshape protein-optoelectronics allowing us to identify i) many interesting ancestral FPs for lighting and ii) QuetzalFP as stepping-stone platform for protein engineering.
Early Terminating Solid Electrolyte Interphase Formation via Nucleophilic Fluorination to Achieve High Initial Coulombic Efficiency
It is demonstrated that the initial Coulombic efficiency (ICE) can be effectively enhanced by early terminating solid electrolyte interphase (SEI) formation via equivalent chemical fluorination. This study presents novel insights into optimizing SEI compositions and electrochemical performance by manipulating the inherent self-terminating chemistry.
Abstract
The initial Coulombic efficiency (ICE) of lithium-ion batteries, quantifying the irreversible Li+ loss during the first cycle, is critical for determining practical energy density. Many electrode materials exhibit substandard ICEs (<90%) due to excessive formation of solid electrolyte interphase (SEI). Traditional strategies modifying SEI formation mainly focus on the generating process but often consume extra Li+ and yield limited improvements. Here, a strategy is introduced that targets the terminating process of SEI formation, usually impeded by interfacial parasitic reactions, to achieve ICEs exceeding 90%. Using TiO2 as a model electrode, it is demonstrated that equivalent chemical fluorination suppresses the parasitic reaction between phosphorus pentafluoride (PF₅) and surface hydroxyl groups (─OH), early terminating SEI formation. Interfacial analysis and theoretical simulations reveal that this approach reduces organic SEI formation while preserving the beneficial LiF-rich inner SEI layer. As a result, the fluorinated TiO2 anode exhibits an ICE of 92.1%, significantly higher than the 74.1% of pristine TiO2, without compromising other electrochemical performance metrics. Pouch cell tests confirm the practical applicability of the method. This work provides deep insights into mechanisms of terminating SEI formation and opens a new pathway for optimizing the battery performances through inherent SEI manipulation.
Coaxial Electroluminochromic Fibers with Dynamic RGB Switching for Pixelated Smart Textiles
A coaxial electroluminochromic fiber with integrated electroluminescent cores and electrochromic shells is constructed on carbon nanotube fibers, enabling dynamic RGB switching and pixelated control. The design features low-voltage operation, fast and reversible color modulation, and high durability, offering a significant advance for multicolor smart textiles in wearable electronics and textile-based display technologies.
Abstract
The immense potential of electronic textiles for wearable applications has spurred extensive research into luminescent fibers suitable for smart textile displays. However, current electroluminescent (EL) fibers, while flexible and wearable, typically emit only a fixed color and have a 1D structure, which confines fiber-based displays to pre-designed patterns. Here, a coaxial hierarchical fiber structure is fabricated with an insulating polymer layer sandwiched between an EL core and an electrochromic (EC) shell based on carbon nanotube fibers. Acting as a dynamic optical filter with RGB tri-state switching capabilities, the EC shell can effectively modulate the optical properties of inner emitted lights via a low voltage, enabling a new “electroluminochromic” fiber with multicolor luminescence and rapid on-demand color switching. Moreover, electroluminochromic bare fibers can be woven with orthogonal electrodes at discrete gel polymer electrolyte junctions, forming individually addressable luminescent pixels. Using a warp-weft knitting approach and integration with the Internet of Things, this display textile can transmit information, exhibiting great potential for applications in smart displays and wearable electronic devices.