Boron modification has been validated as an efficient strategy for boosting Fe-based Fenton catalysis. Nevertheless, it remains challenging to synchronously achieve boron doping and heterostructure modulation while steering ROS generation pathways. Herein, a novel B-FeS2 nanocatalyst with dual modification was synthesized via a wet mechanochemical-thermal method. Boron modification constructs a FeS2/boron sheet heterostructure that suppresses oxidation and agglomeration, while introducing electron-donating BB and FeB bonds. The B-FeS2 Fenton system achieves >90% BPA removal across a wide pH range (3-10), exhibits Kobs and mineralization efficiency 1.4 and 1.89 times higher than those of bare FeS2, respectively, and maintains stable performance over five cycles and 12 h continuous operation. Mechanistic studies reveal that B doping upshifts the Fe d-band center, which correlates with an altered H2O2 cleavage pathway characterized by enhanced ·O2- generation alongside sustained ·OH production, suggesting a possible shift in the relative contribution of homolytic versus heterolytic pathways. The generated ·O2- directly degrades BPA and sustains Fe2+/Fe3+ cycling via the Haber-Weiss reaction, a synergy particularly advantageous under alkaline or anoxic conditions. This work demonstrates that B modification serves as an effective electronic modulator for FeS2, providing mechanistic insights into designing iron-based Fenton system with tailored ROS pathways.

We have recently shown that mixing green fatty acid 12-hydroxystearic acid (12-HSA) molecules with a low amount of various end-capped polyethylene glycol (PEG) chains (mono- or di-functionalized by 12-HSA or stearic acid (SA) moieties) provides a straightforward one-pot route to design PEGylated self-assemblies, either vesicles or multilamellar tubes. Tuning the concentration of end-capped PEG chains offers a simple strategy to precisely control the morphology of these PEGylated architectures.

The redox kinetics of lithium polysulfides (LiPSs) result from the intrinsic insulating nature of sulfur and the weak interaction between hosts and LiPSs. Constructing heterostructures with built-in electric fields is a promising strategy to accelerate charge transfer; however, the limited active sites and suboptimal electronic configuration at the interface often restrict their catalytic efficiency. Herein, we propose an atomic-level modulation strategy by incorporating isolated Cu atoms into a Mott-Schottky Ni/NiO heterostructure to create a multifunctional electrocatalytic layer for LiS batteries. The introduction of atomic Cu not only induces abundant oxygen vacancies but also triggers a selective upward shift of the d-band center, which synergizes with the interfacial electric field to optimize the electron redistribution. This electronic restructuring significantly enhances the orbital hybridization between the host and LiPSs, thereby strengthening the chemical adsorption and effectively lowering the decomposition energy barrier of Li2S. Consequently, the Cu-Ni/NiO modified separator exhibits superior catalytic activity, achieving a high initial capacity of 1353 mAh g-1 and an ultralow decay rate of 0.056% per cycle over 500 cycles at 1C. Even under harsh conditions with high sulfur loading (8.4 mg cm-2) and lean electrolyte, the pouch cell delivers a high areal capacity of 4.16 mAh cm-2 and excellent flexibility, demonstrating its great potential for practical applications.

Harnessing solar energy for the photocatalytic CO2 reduction into valuable fuels presents a sustainability strategy to simultaneously alleviate the global energy crisis and mitigate carbon emission. However, the efficiency of photocatalytic CO2 reduction is hindered by weak adsorption and sluggish charge separation in semiconductor materials. Herein, a sulfur/oxygen dual-vacancy engineered CuS-Sv/NiTiO3-Ov S-scheme heterojunction is constructed to achieve a remarkable CO production rate of 490.0 μmol g-1 h-1 with 89.1% selectivity. Experimental results reveal that sulfur vacancies probably strengthen CO2 adsorption and activation, while oxygen defects induced interfacial charge redistribution at the S-scheme heterojunction interface by intensifying the built-in electric field, promoting efficient separation and migration of photogenerated charge carriers. Density functional theory calculations further uncover that sulfur vacancies (Sv) are beneficial to CO2 adsorption and activation while promoting the stabilization of the key *COOH intermediate, thereby favoring the CO2 reduction reaction. Moreover, oxygen vacancies (Ov) promote charge redistribution and facilitate charge transfer across the heterojunction interface onto CuS-Sv. In-situ diffuse reflectance infrared Fourier transform spectroscopy and Gibbs free energy (ΔG) calculations clarify the reaction pathway, showing that the synergistic interaction of sulfur and oxygen vacancies efficiently decreased the energy barrier for *CO formation by reinforcing the interaction between *COOH intermediates and the catalyst surface. This study highlights a synergistic strategy combining defect engineering and S-scheme heterojunction design to achieve highly selective and efficient photocatalytic CO2 to CO conversion.

Hydrogen storage in activated carbons (ACs) via hydrate-based hybrid systems is governed by pore-scale wetting and interfacial phenomena rather than pore structure alone. We hypothesize that tetrahydrofuran (THF) saturation controls capillary-driven liquid redistribution across micro-, meso-, and macropores, thereby modulating interfacial accessibility and governing the redistribution of H2 among adsorption, pore-confined gas-phase compression, and hydrate-associated contributions.

Despite the inherent safety and low cost of aqueous Zn-ion batteries (AZIBs), the practical application of Zn metal anodes is severely hindered by dendrite growth and parasitic reactions. Herein, inspired by the adhesive and conformal characteristics of liquid bandages, we report a rigid-flexible nitrocellulose/ricinoleic acid (NCRA) interphase with ion-regulating capability for highly stable Zn metal anodes through a facile blade-casting approach. Ricinoleic acid is incorporated as a plasticizer to improve the flexibility of the otherwise rigid nitrocellulose film, enabling conformal and adhesive contact of the NCRA interphase with the Zn anode. The highly zincophilic and electronegative nitro and carboxyl groups endow the NCRA interphase with multifunctional ion-regulation functions, including a lowered nucleation energy barrier, accelerated desolvation kinetics of hydrated Zn2+ ions, uniform Zn2+ flux, and repulsion of SO42- anions, collectively contributing to dendrite-free Zn deposition. Meanwhile, the NCRA interphase serves as a physical barrier that effectively shields the Zn anode from bulk water, thereby suppressing water-induced side reactions. Furthermore, this conformal interphase accommodates volume fluctuations during repeated Zn plating/stripping, thereby effectively preserving interfacial integrity and long-term protection. Consequently, the NCRA@Zn anode demonstrates highly reversible and stable plating/stripping behavior for over 5000 h at 5 mA cm-2. After 2500 cycles at 10 A g-1, the full cell employing an NH4V4O10 cathode preserves 86.5% of its initial capacity. This work offers a simple yet powerful interfacial strategy toward long-life, dendrite-free Zn anodes for practical AZIBs.

High-entropy materials offer attractive electrocatalytic activity on account of their multiple elements that can provide abundant active sites. However, the sluggish diffusion effect impedes the reconstruction kinetics under electrochemical conditions. Herein, we rationally designed a hollow, self-supported amorphous ZnFeCoNiCu oxide (H-ZFCNC-O) using ZnO nanorods as a sacrificial template. The resulting hollow architecture provides dual-side electrolyte access. Meanwhile, its amorphous matrix eliminates long-range diffusion barriers, thus enabling multi-element synergism to create multivariate reconstruction pathways. Consequently, the H-ZFCNC-O exhibits accelerated reconstruction kinetics to form a high-activity phase, delivering an overpotential of 274 ± 5 mV at 50 mA cm-2 for the oxygen evolution reaction, with only a marginal increase to 288 ± 5 mV in simulated seawater. Meanwhile, an anion-exchange membrane water electrolyzer employing the reconstructed H-ZFCNC-O as the anodic catalyst demonstrates excellent durability, retaining stable performance for 200 h in freshwater electrolysis and 300 h in seawater electrolysis. This work indicates that amorphization strategy can overcome the sluggish diffusion effect and effectively drive electrochemical reconstruction, affording a fresh perspective on regulating the electrochemical reconstruction of electrocatalysts with high configurational entropy.

Water splitting for hydrogen production is regarded as one of the essential technologies for sustainable hydrogen generation due to its high efficiency, simplicity, and cleanliness. Nonetheless, a severe constraint is imposed on the overall efficiency and practical implementation of water electrolysis by the slow reaction kinetics of the oxygen evolution reaction (OER). Therefore, designing and developing efficient electrocatalysts is crucial for enhancing OER performances. In this work, Ni3Fe2 metallic aerogels (Ni3Fe2 MAs) precursors are fabricated via a one-step method and subsequently transformed into hollow-structured Ru24NiFe metallic aerogels (Ru24NiFe MAs) electrocatalysts through an electrochemical displacement approach, which enhances transport of mass species and migration of electrons efficiency. The Ru24NiFe MAs exhibit a reduced overpotential of 241 mV at 10 mA cm[-2] and a Tafel slope of 31.0 mV dec[-1]. First-principles calculations further reveal the electrocatalytic mechanism, demonstrating that Ru incorporation significantly reduces the reaction energy barrier and optimizes the adsorption of reaction intermediates on NiFe sites. Moreover, the dual-electrode system composed of Ru24NiFe MAs and PtNi4 MAs achieves a cell voltage of only 1.51 V for overall water splitting at 10 mA cm[-2], exhibiting electrocatalytic performance and stability far superior to those of Pt/C//RuO2.

Dopamine (DA) and uric acid (UA) are important biomarkers whose simultaneous determination is essential for clinical diagnosis and pathophysiological studies. However, prevailing electrochemical sensors rely on conductivity enhancement or complex architectures, often resulting in ill-defined active sites that obscure clear structure-activity relationships. We integrate single-atom electronic structure engineering with interfacial electrical property modulation to precisely define atomic-scale active sites and their interfacial environment, thereby establishing clear structure-activity relationships. A ternary MXene@Mn2O3@PtSA catalyst is constructed by anchoring atomically dispersed Pt sites on Mn2O3 grown on highly conductive MXene. Electronic interactions between Pt single atoms and the Mn2O3 support downshift the Pt d-band center, optimizing the adsorption energies of reaction intermediates and significantly lowering the energy barriers of the rate-determining steps for both DA and UA oxidation, while the negatively charged surface promotes electrostatic enrichment of DA. As a result, MXene@Mn2O3@PtSA enables sensitive and selective discrimination of DA and UA in serum samples, offering a versatile design paradigm for high-performance electrochemical biosensing.

All-in-one electrochromic devices (ECDs) integrate all active components into a single electrolyte layer, yet their performance remains constrained by the inherent trade-off between optical contrast and switching kinetics in single-component systems. Here we report a conceptually new design strategy based on inorganic-organic dual redox pairs, wherein the electrochromic function and the charge-balancing function are assigned to two distinct yet electrochemically coupled components within a poly(ethylene oxide) (PEO) composite electrolyte. More importantly, the resulting colorless electrolyte incorporates a dual redox couple: the organic pair of transparent tetramethyl-thiourea (TMTU) and its oxidized dimer tetramethylformaminium disulfide dication (TMFDS[2+]), mediates charge compensation and accelerates switching kinetics without introducing parasitic absorption, while the inorganic oxidized state of silicotungstic acid (STA) serves as the electrochromic component, providing multi-electron W[6+]/W[5+] redox capacity with intense blue coloration for electrochromic smart windows (ESWs). The advantages of this organic-inorganic hybrid dual redox couple include its non-corrosive nature, low cost, and easy handling. The all-in-one device adopts a simplified indium tin oxide (ITO)/composite electrolyte/ITO architecture, eliminating the electrochromic and ion-storage layers of conventional designs. The optimized device achieves an optical contrast of 93.8 ± 0.6% (without ITO), a coloration time of 3.2 ± 0.2 s, a coloration efficiency (CE) of 339.5 cm[2] C[-1], and 10,000-cycle stability with negligible degradation. Large-area prototypes (100 cm[2]) exhibit uniform coloration. This dual redox strategy establishes a modular platform for high-performance all-in-one ECDs with independently tunable components.

Poly(N-isopropylacrylamide) (PNIPAM) microgels are highly porous polymer networks whose mechanical properties are governed not only by environmental factors but also by their internal architecture. We hypothesize that the internal structure of microgels, together with interparticle interactions, synergistically regulates the macroscopic rheological behavior of microgel suspensions.

Tin dioxide (SnO2) is a promising anode material for sodium-ion batteries owing to its high theoretical capacity, yet its practical application is severely hindered by drastic volume expansion and intrinsically sluggish Na[+] diffusion kinetics. Herein, we report a mesoporous yolk-shell SnO2-based nanoreactor (SnO2mCNR) constructed via a facile interfacial polymerization assembly and selective etching strategy. The architecture features a SnO2 nanocube core, an internal void space, and a mesoporous carbon shell permeated with interconnected channels (∼7 nm). This unique design simultaneously accommodates the large volume changes during sodiation/desodiation and provides low-resistance pathways for rapid Na[+] transport. Compared with its non-porous counterpart (SnO2 CNR), SnO2mCNR exhibits a ∼ 3.5-fold higher Na[+] diffusion coefficient and a transition toward pseudocapacitive-dominated charge storage (b-value of 0.90). Consequently, SnO2mCNR delivers a high reversible capacity of 650.3 mAh g[-1] at 0.05 A g[-1], excellent rate capability (218.7 mAh g[-1] at 5 A g[-1]), and outstanding cycling stability with 95.1% capacity retention over 1800 cycles at 1 A g[-1]. A full pouch cell assembled with a Na3V2(PO4)3-based cathode achieves a high energy density of 292.2 Wh kg[-1], indicating promising application potential at the electrode-material level. This work establishes shell porosity engineering as a generalizable design principle for high-performance conversion/alloying-type anodes in sodium-ion batteries.

Electrocatalytic urea synthesis provides a promising alternative to conventional energy-intensive industrial processes, yet its progress remains largely limited by the unclear CN coupling mechanism and insufficient catalyst regulation strategies. Using density functional theory calculations, we screened a series of Cu-based single-atom alloys and identified the Zn1Cu(1 1 1) system as a promising candidate owing to its thermodynamic stability, favorable *CO adsorption behavior, and accessible first CN coupling kinetics. Electronic structure analyses reveal that Zn incorporation promotes its surrounding electron accumulation toward the adjacent Cu sites, thereby optimizing the adsorption of CO/NO-derived intermediates and then facilitating key CN coupling steps. Subsequently, the most favorable reduction pathways were identified by evaluating the stepwise competition among CN coupling, *CO protonation, and the protonation of N-containing intermediates. Compared with pristine Cu(1 1 1), Zn1Cu(1 1 1) lowers the maximum kinetic barrier from 1.02 eV to 0.85 eV toward urea formation at -0.35 V vs. RHE. More importantly, this study provides atomic-level insight into Cu-based single-atom alloys for electrocatalytic CN coupling and establishes a systematic theoretical workflow for other CN coupling reactions.

Electrocatalytic water splitting is a sustainable route for H2 production, yet the green synthesis of Pt-based alloy catalysts without external reducing agents remains challenging. Herein, we report a defect-rich activated N-doped mesoporous hollow carbon sphere (NMHCS-A) enabling the spontaneous formation of PtPd alloy under ambient conditions without reducing agents or thermal treatment. Structural analyses reveal that KOH activation generates abundant carbon defect-associated species, acting as electron reservoirs to promote the reduction of Pt and Pd precursors and subsequent alloy nucleation. Control experiments show that spontaneous alloy formation occurs only on NMHCS-A with the high defect density, whereas low-defect carbon supports fail to produce detectable PtPd alloy phases under identical conditions. Owing to the strong electronic interaction between Pt and Pd, electron transfer from Pd to Pt optimizes H adsorption and accelerates H2 evolution reaction (HER) kinetics. Consequently, PtPd/NMHCS-A exhibits an overpotential of 28 mV at 10 mA cm[-2] in 0.5 M H2SO4 and a Pt mass activity 49 times higher than that of commercial Pt/C. Theoretical calculations reveal that alloy-induced electronic structure reconstruction weakens PtH interactions and brings the H adsorption free energy closer to thermoneutrality. This work provides a defect-density-dependent spontaneous alloying strategy for noble-metal catalysts systhesis.

The rational exploration of lanthanide-doped fluoride nanoparticles (NPs) is of great significance for advanced optical applications. Nevertheless, developing highly efficient near-infrared (NIR) emitting NPs that can be excited by NIR light remains a considerable challenge. Herein, the concentration-gradient Nd[3+]-doped NaGdF4 NPs and NaGdF4:3%Nd@NaGdF4 core-shell NPs were synthesized. The prepared NPs exhibits intense NIR emission upon 794 nm excitation, the concentration quenching of Nd[3+] ions in the NaGdF4 host is ascribed to the dipole-dipole interaction. The fluorescence lifetime and luminescence efficiency of NPs are remarkably improved through coating the inert shell. In addition, the NaGdF4:3%Nd@NaGdF4 NPs displays obvious up-conversion luminescence under 808 nm laser irradiation, and the double-photon process is responsible for it. This research manifests that the title NPs is a potential dual-mode luminescent nanomaterial for advanced optical applications, especially photobiological application.