Sulfoaluminate cement (SAC)-based grouting materials used for the filling and reinforcement of fractured rock masses in underground engineering are prone to moisture ingress and steel reinforcement corrosion under high-humidity and aggressive environments, thereby compromising structural durability. To improve the hydrophobicity of SAC pastes and mitigate steel corrosion under accelerated conditions, metakaolin (MK) was modified using methyltrimethoxysilane to produce hydrophobic metakaolin (HMK). The effects of varying dosages of MK and HMK on the hydration behaviour, mechanical properties, pore structure, hydrophobicity and corrosion resistance of SAC pastes were systematically investigated. The results indicate that an appropriate MK content (4%) promotes the formation of C–A–S–H (calcium aluminosilicate hydrate) gel and improves the 28-day compressive strength; however, its intrinsic hydrophilicity increases water absorption, which may be unfavourable for moisture resistance and steel corrosion protection. In contrast, HMK introduces hydrophobic functional groups while retaining partial pozzolanic activity, reducing water absorption by 28.5% and increasing the water contact angle to 145°. Under identical impressed-current conditions, the mass loss of steel bars embedded in HMK-modified specimens was reduced by 34.9–48.1% compared with that of the corresponding reference specimens. Correlation analysis further reveals a strong positive relationship between water absorption and steel mass loss (r = 0.97), while the proportion of pores within the 20–50 nm range is also positively correlated with steel mass loss. Through the synergistic effects of pore structure regulation and hydrophobic shielding, HMK reduced moisture transport and steel corrosion under accelerated conditions, demonstrating its potential to improve the durability of SAC pastes in humid and chloride-containing environments.

Abstract Graphene edges and topological defects are two important active sites in metal-free carbon-based electrocatalysts for various energy-related reactions such as the oxygen reduction reaction (ORR). However, quantitative measurement and exploration of the atomic origin of the activities of these defects remain challenging, largely due to the structural complexity and heterogeneity of carbon-based electrocatalysts. Their ORR selectivity toward either the two-electron pathway producing hydrogen peroxide or the four-electron pathway leading to water also remains controversial. Herein, we fabricate well-defined model electrocatalysts via chemical vapor deposition of nanocrystalline graphene domains with tunable edge densities. The ORR activities are determined to be dominated by the two-electron pathway producing hydrogen peroxide and scale linearly with the edge density, enabling the quantification of the specific activity per unit edge length. Using atomic-resolution differential phase contrast scanning transmission electron microscopy, we identified the favorable formation of topological defects at the edges, with significant fluctuations in localized electron states, providing an important atomic origin for their enhanced ORR activity. This was corroborated by the deliberate introduction of topological defects by Ar plasma treatment, leading to two-dimensional amorphous carbon and significantly enhanced two-electron ORR activity.

Twisted bilayer MoS2 forms a quantum-engineered sensing platform, where the moiré superlattice creates a configurable surface potential for molecular control. Here we present a periodically modulated landscape in bilayer MoS2 by twist-angle tuning, and use it for molecular trapping and selective sensing. The native 54 meV moiré potential confines aromatic molecules (e.g., rhodamine 6G, R6G; methylene blue, MB) at AA-stacking sites. Introducing extended vacancies deepens confinement to 238 meV, enhancing adsorption. Twist angle enables band alignment with molecules, driving charge-transfer resonances. This integrated design, moiré potentials, defect-enhanced trapping and band-aligned charge transfer, synergistically amplifies Raman signals, achieving single-molecule sensitivity down to 10−20 M. Importantly, the platform exhibits molecule-specific selectivity: R6G is optimally detected at 10° and 50° bilayer MoS2, while MB responds at 15° and 45°, demonstrating twist-angle encoding of molecular recognition. Our twisted MoS2 with extended vacancies establishes a moiré system as a versatile platform for selective molecular sensing. Twisted layers of van der Waals materials can generate moiré superlattices, forming reconfigurable surface potentials with nanoscale periodicity. Here, the authors show that the moiré potential in twisted bilayer MoS2 can be used to confine aromatic molecules, improving the surface-enhanced Raman spectroscopy sensitivity and selectivity of this platform.

Interfacial charge transfer in composite semiconductor channels provides a powerful and physically transparent route to achieving broadband and high-gain phototransistors, yet remains insufficiently explored in indium-free oxide-organic systems. Here, we report a broadband-responsive hybrid phototransistor based on an all-solution-processed composite channel composed of zinc-tin oxide (ZTO) and an organic bulk heterojunction PM6:Y6. In this architecture, amorphous ZTO serves primarily as a high-mobility, low-noise electron transport channel with excellent gate controllability, while the PM6:Y6 bulk heterojunction supplies strong and broadband optical absorption, enabling efficient photocarrier generation from the ultraviolet to the near-infrared region. Efficient interfacial charge transfer at the oxide/organic interface allows photogenerated electrons in the PM6:Y6 layer to be injected into the ZTO channel, where they are rapidly transported and amplified by the field-effect conduction pathway. Systematic optoelectronic characterizations reveal that the resulting high gain originates from interfacial carrier separation and accumulation at the composite channel, rather than from direct charge transport within the organic layer alone. As a result, the device exhibits pronounced photocurrent enhancement across the ultraviolet-visible-near-infrared spectral range, with a photosensitivity exceeding 5 orders of magnitude, a maximum responsivity of 9.13 × 103 A/W, and a specific detectivity on the order of 1015 Jones. By replacing indium-containing oxides with solution-processed ZTO, this work demonstrates that broadband high-gain photodetection can be realized without relying on indium-specific electronic properties. These results establish interfacial charge transfer as a general and scalable physical mechanism for designing indium-free, broadband, and high-performance oxide-based phototransistors.

The development of high-performance broadband absorbing materials is pivotal for advancing solar energy harvesting and storage. However, a facile and scalable one-step fabrication process for three-dimensional (3D) porous carbon scaffolds modified with high-entropy alloy nanoparticles (HEA NPs) remains challenging. This study introduces a straightforward laser-processing strategy for the direct synthesis of HEA NP-decorated laserinduced graphene (HEA@LIG) on flexible substrates in a single step under ambient conditions. The transient high temperature generated by the COQ laser simultaneously converts a liquid organic precursor into a 3D porous graphene network and induces the in-situ formation of homogeneous HEA NPs containing up to eight metallic elements. The obtained HEA@LIG films exhibit a maximum light absorption of 98.5% over 250-2500 nm. Under 1 sun illumination, they reach a high equilibrium surface temperature of 97.5 degrees C. We further use HEA@LIG as an efficient carrier for phase change materials to realize efficient solar energy storage. The resulting composite shows an energy storage density of 169.3 J/g and a solar-thermal conversion efficiency of 93.1%. Moreover, this fabrication strategy is compatible with roll-to-roll processing and patterned fabrication on transparent substrates, yielding dual-functional films that combine solar heating with transparency. This work provides a simple and scalable route for practical solar-thermal materials.

Two‐dimensional (2D) semiconductor materials are among the best candidates for maintaining Moore's Law. Due to their atomic‐scale thickness, high carrier mobility, and excellent gate control, 2D materials have become a significant area of research. However, intense electron doping caused by interfacial charge impurities and structural defects has led to many more reports of n‐type 2D semiconductors than p‐type. Moreover, p‐type 2D semiconductors face significant challenges, including inferior environmental stability of both materials and devices, and the difficulty of achieving high‐quality, controllable wafer‐scale synthesis. This paper reviews the latest progress in p‐type 2D semiconductors and their applications across various fields. We categorize them by type, such as monoelemental materials, chalcogenides, and oxides. First, we summarize relevant theoretical calculations, explore their hole‐dominated conduction mechanisms, and list several promising high‐quality new p‐type 2D semiconductors. Next, we review various synthesis and preparation methods for p‐type 2D semiconductors, including both top‐down and bottom‐up techniques such as mechanical exfoliation, liquid‐phase exfoliation, chemical vapor deposition, atomic layer deposition, and molecular beam epitaxy. We compare the advantages and disadvantages of each method. Then, we highlight several prototype device studies based on p‐type 2D semiconductors. Finally, we discuss their applications across various fields, including logic circuits, optoelectronic imaging, neuromorphic visual computing, and chemical/biological sensors. We also examine their opportunities, challenges, and prospects, and propose various research directions and technical pathways to advance their development. We hope this review will serve as a valuable resource for the future development of p‐type 2D semiconductors.

Polyethylene terephthalate (PET) plastics cause significant environmental harm. Traditional treatment methods, such as landfilling and incineration, can cause secondary pollution. Here, an efficient synergistic photocatalytic system is presented, based on Co3O4/CeO2 hollow nanotubes prepared by electrospinning, to activate peroxymonosulfate (PMS) and promote the degradation of PET-S plastics. The results show that the as-prepared CC-8 composite catalyst exhibits the best performance under illumination; the weight loss rate of PET-S can reach ~82.7% in the presence of a 3 mM PMS solution (pH 7). The effects of parameters (e.g., PMS dose and coexisting anions) on PET-S degradation were systematically investigated. Electron paramagnetic resonance (EPR) and free radical quenching experiments confirm that the •OH, 1O2, and SO4•- active species contribute the most to the degradation of PET-S plastics. Density Functional Theory analysis shows that Co-d-pDOS and Ce-f-pDOS modulations in Co3O4/CeO2 synergistically enhance the PET photocatalytic decomposition efficiency. Finally, we discuss the mechanism by which the catalyst/light/PMS system degrades PET in water. Overall, this study provides a feasible solution for treating waste microplastics.

With the growing emphasis on environmental consciousness and personal safety awareness, fiber electrodes featuring excellent environmental friendliness and safety performance are crucial for developing high-performance close-fitting wearable electronics. Herein, a flexible, degradable, and flame-retardant calcium alginate (CaAlg)/carbon nanotubes (CNTs)/polypyrrole (PPy) composite fiber electrode is developed for advanced fiber-shaped supercapacitors (FSSs). Benefiting from the intrinsic biodegradable and flame-retardant properties of CaAlg matrix, the composite fiber electrode exhibits controllable degradability and superior flame retardancy. Moreover, owing to the unique wrinkled PPy layer that synergistically improves both electrochemical and mechanical properties, the ternary CaAlg/CNT/PPy composite fiber electrode shows a remarkable areal capacitance of 1308 mF cm-2 at 2 mA cm-2 and an outstanding mechanical strength of 45 MPa. The as-fabricated FSS device delivers a high energy density of 10.9 μWh cm-2, outperforming most state-of-the-art flexible FSSs, especially those based on biomass-derived fibers. These flexible composite fiber electrodes hold great promise for the development of high-performance, high-safety energy storage devices toward sustainable portable and wearable electronics.

Terahertz (THz) laser pulses can drive coherent vibrations through nonlinear phonon coupling, inducing transient lattice distortions that provide an optical pathway for manipulating quantum phases on ultrafast timescales. The excitation of specific phonon modes, in particular, shifts the atomic equilibrium positions, leading to structural distortions and symmetry breaking that alter the properties of symmetry-protected topological quasiparticles. Here, we investigate THz laser-induced nonlinear phonon interactions in the chiral semimetal CoGe, which contains multiple types of topological fermions, and reveal a symmetry-governed switching mechanism of topological states. Under THz excitation, lattice anharmonicity induces net displacements along the A and E Raman modes, breaking the C3,111 rotational symmetry and lowering the space group from P213 to its subgroup P212121. Consequently, the unconventional chiral fermions with topological charges of 2 and 4 in CoGe transform into two and four Weyl fermions with the topological charge of 1 in the absence and presence of spin-orbit coupling, respectively. These findings demonstrate that ultrafast symmetry breaking driven by nonlinear phononics enables topological phase transitions of multifold fermions, offering a route for the dynamic control of topological quantum states.

Electrochemical advanced oxidation processes serve as effective technologies for organic wastewater treatment. Nevertheless, conventional single-metal electrodes and powdery LDH catalysts fail to achieve nanoscale bimetallic coupling, lack interfacial electronic modulation, and suffer high charge transfer resistance. In this study, a two-step hydrothermal strategy was adopted to in-situ construct hierarchical self-supported NiCo layered double hydroxide/nickel hydroxide electrodes (NiCo-LDH/Ni(OH)2/NF) on nickel foam substrate. The Ni–Co electronic synergy modulates metal valence states and surface electron density, optimizes charge-transfer kinetics, and promotes selective generation of singlet oxygen (1O2) via coupled transformation of reactive oxygen intermediates. Using minocycline (MNO) as a model pollutant, the electrode with Ni/Co molar ratio 1:2 showed optimal activity: charge-transfer resistance 19.7 Ω and 95.79% MNO removal within 30 min. It maintained stable performance across wide pH ranges, coexisting anions, and real water matrices, retaining ~90% removal after long-term operation. Mechanistic studies confirmed 1O2 as the dominant species (44.6% contribution), originating from cathodic H2O2 conversion and reactive oxygen coupling, while active chlorine oxidation and direct interfacial electron transfer also participated. Combined with density functional theory (DFT) calculations and liquid chromatography-mass spectrometry (LC-MS) analysis, the electrophilic, nucleophilic and radical attack sites on MNO molecules were identified, and three parallel degradation pathways were proposed. Ecotoxicity assessment showed significant reduction in intermediate toxicity after sufficient electro-oxidation. Benefiting from bimetallic synergy and hierarchical porosity, this self-supported electrode enables efficient, low-energy, and broad-spectrum antibiotic remediation, offering a viable material design for electrocatalytic treatment of saline organic 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.

The durability of platinum (Pt) electrocatalysts in electrochemical energy conversion is fundamentally challenged by surface oxidation and dissolution during electrochemical operation. Although Pt surface oxidation has commonly been discussed in terms of a "place exchange" mechanism between Pt and oxygen, atomic-scale insight into its potential-dependent progression has remained limited. Herein, we directly visualize atomic electrooxidation and dissolution of {111}-terminated surfaces of octahedral Pt nanoparticles by employing ex situ differential-phase-contrast scanning transmission electron microscopy combined with online inductively coupled-plasma mass spectroscopy and density functional theory calculations. We reveal the atomistic structural evolution of the {111} nanoparticle surface with progressively increasing electrode potentials (0.8-1.5 V), from the initial lattice expansion induced by adsorbed oxygen, to vacancy-induced formation of two-dimensional, lattice-contracted PtOx monolayers, and finally to a dimensional transition to three-dimensional PtO2 growth. Furthermore, we demonstrate how the potential cycling protocols (triangular versus square wave cycling) decisively control the final oxide's dimensionality (multilayer versus single layer) and stability. These atomic-scale insights establish how electrochemical conditions dictate Pt oxidation pathways and atomistic structural evolution, providing a mechanistic basis for understanding and improving the durability of Pt-based electrocatalysts.

The oxygen evolution reaction (OER) in electrochemical water splitting has always been a key bottleneck restricting efficient hydrogen production. An ideal electrocatalyst must not only exhibit high catalytic activity but also possess excellent stability, which is an equally crucial core indicator. Therefore, developing electrocatalysts that simultaneously achieve both high activity and long-term stability is of great significance. In this study, we successfully prepared a bulk high-entropy alloy electrode with a fully eutectic structure using arc melting technology. By adjusting the relative ratios of Cr and Mo elements, we not only optimized the intrinsic catalytic activity of the electrode but also observed a unique "performance improvement over time" phenomenon during prolonged stability tests. The dense eutectic structure of the electrode provides an ideal environment for electronic interactions among multiple metal atoms. During CV activation, the applied voltage drives the dissolution of the "unstable" IMC phase in the electrode. The dissolution of the Mo-rich phase and the leaching of Cr ions enhance the degree of surface reconstruction, leading to the formation of active high-valence oxygencontaining species, thereby promoting the enhancement of OER performance. After activation via cyclic voltammetry (CV), the Cr10Mo06-A electrode exhibited the most remarkable performance improvement, requiring only an overpotential of 380 mV to achieve a current density of 400 mA cm(-2). Moreover, the electrode demonstrated continuous and stable operation for nearly 500 h at a high current density of 500 mA cm(-2), successfully achieving a synergy between high activity and outstanding stability.

ABSTRACT Aqueous zinc‐based batteries (AZBs) have emerged as promising candidates for grid‐scale energy storage systems due to the high volumetric capacity, intrinsic non‐flammability, and cost‐effectiveness. However, their practical application is limited by insufficient reversibility and sluggish reaction kinetics. In this regard, anionic chemistry plays a key role in regulating the thermodynamics and kinetics of electrode reactions. Nevertheless, most discussions in the chemistry of AZBs focus on Zn 2+ behavior, and a comprehensive review of anionic chemistry is still lacking. In this review, we systematically summarize the key descriptors of commonly used anions, which affect the competitive coordination among anions, Zn 2+ , and H 2 O. We then critically analyze the effect of anionic chemistry on zinc anode reactions, including the hydrogen evolution reaction and Zn‐deposition process, elucidating structure–performance correlations between anionic properties and electrochemical behavior. Furthermore, we discuss the role of anions as charge carriers and their impact on the kinetics of cathode reactions. Finally, we conclude with a concise perspective of future research directions in anion design and mechanistic investigation. This review may provide guidance for the rational design of high‐performance AZBs for practical applications.

Exploring two-dimensional semiconductors with mechanical flexibility, auxetic behavior, and tunable physical properties is of great significance for the development of flexible electronics and optoelectronic devices. In this study, eight square-lattice monolayers MX2 (M = Si, Ge, Sn, Pb; X = Se, Te) were systematically studied by first-principles calculations. After thorough assessments of thermodynamic, dynamical, mechanical, and thermal stability, SiSe2 and SnSe2 were identified as stable candidates. These two monolayers exhibit maximum in-plane Young’s moduli as low as 76.55 and 45.08 N/m, respectively, and negative in-plane Poisson’s ratios of -0.05 and -0.045, indicating mechanical softness and intrinsic auxetic behavior. SiSe2 and SnSe2 were found to be indirect-band-gap semiconductors with band gaps of 2.08 and 2.14 eV, respectively, which can be effectively tuned by strain engineering. Carrier transport analysis indicates that SiSe2 and SnSe2 exhibit opposite transport preferences, with SiSe2 favoring holes (37.46 cm2V-1s-1) and SnSe2 favoring electrons (105.61 cm2V-1s-1). Moreover, optical absorption spectra of both monolayers demonstrate strain-induced redshifts and polarization-dependent anisotropy under uniaxial strain, whereas biaxial strain preserves in-plane isotropy and causes pronounced redshifts. These findings indicate that SiSe2 and SnSe2 monolayers are promising two-dimensional candidates for flexible electronic and strain-modulated optoelectronic applications.

New synthetic routes are required to create advanced Fe-N-C electrocatalysts for eventual substitution of commercial Pt/C toward acidic oxygen reduction reaction (ORR). Herein, we report the co-assembly of ORR-active hemin molecule, 2-methylimidazole (2-MI), and ZnII acetate to achieve single-molecule hemin locked in the nanocages of zeolite imidazolate framework-8 (ZIF-8). Density functional theory (DFT) and spectroscopic analysis show that coordination, H-bond and it-it interaction exist between ZIF-8 cage and hemin, which allow ZIF-8 nanocages to plentifully encapsulate and anchor distorted and shrunk single-molecule hemin. After pyrolysis, the resultant HD-Fe-N-C has 4.5 wt% of atomically dispersed Fe and exhibits excellent activity in terms of a half-wave potential (E1/2) of 0.856 V (vs. RHE) toward ORR, closely approaching that of commercial Pt/C (0.871 V vs. RHE). Furthermore, DFT indicates that the active sites of HD-Fe-N-C in the form of OH-FeIIIN4C12 and OH-FeIIIN2+2C10 have lowered Gibbs free energy for ORR rate determining step (H++*OH + e- -> H2O) relative to that of regular FeIIN4C12 and FeIIN2+2C10. Additionally, HD-Fe-N-C demonstrates an improved durability with 27 mV of E1/2 decay, superior to that of commercial Pt/C (29 mV). DFT and H2O2 decomposition experiments indicate that the excellent durability of HD-Fe-N-C is on account of suppressing the production of H2O2.

Electrocatalytic nitrogen reduction reaction (ENRR) offers a promising approach to synthesizing valuable ammonia (NH3) product, serving as a pivotal solution to the pressing energy shortage issue. While tungsten trioxide (WO3) has been widely investigated as electrocatalyst in various electrocatalytic reactions, their practical application in ENRR remains hindered by inherently weak hydrolytic capability and sluggish hydrogenation kinetics. Here, we report a rational strategy to accelerate the hydrogenation process during ENRR by engineering an atomically local electric field through Mo doping in WO3 catalyst. Experimental results combined with density functional theory (DFT) calculations reveal that Mo enhances hydrolysis process, while an atomically local electric field concomitantly optimizes the transfer of adsorbed hydrogen and lowers the energy barrier for key intermediate, particularly during N-NH formation. This work highlights the critical role of atomically local electric fields in regulating hydrogenation kinetics and provides a new paradigm for designing high-performance ENRR electrocatalysts.

Enhancing the oxygen evolution reaction (OER) performance of bulk electrodes through surface reconstruction represents a highly effective strategy. However, this phase-sacrificing approach for performance improvement inevitably compromises the structural stability of the electrode. Additionally, the inherently poor hydrogen evolution reaction (HER) performance of bulk electrodes hinders their application as bifunctional catalysts. Building upon our previous research on FeNiMo bulk electrodes, we introduced varying amounts of Co dopants to modulate both the degree of surface reconstruction and the eutectic structure. The resulting Co10 electrode exhibited the lowest extent of surface reconstruction while simultaneously delivering optimal OER performance, indicating the existence of multiple pathways (such as electronic structure modulation) for enhancing the OER activity of FeNiMo electrodes. With increasing Co content, the electrodes demonstrated a higher proportion of eutectic phase, improved electrical conductivity, optimized electronic structure, and favorable adsorption strength, leading to remarkable enhancement in HER performance. At a current density of 10 mA cm- 2, the overpotentials for OER and HER decreased from 230/229 mV to 192/186 mV, respectively. Furthermore, the electrode exhibited exceptional long-term stability, maintaining operation for over 200 h at 500 mA cm- 2 for OER and over 100 h at 100 mA cm-2 for HER. When configured in a two-electrode electrolyzer, the Co10 electrode required a low cell voltage of only 1.96 V to achieve 100 mA cm- 2. This work successfully balances the activity-stability relationship in FeNiMo bulk electrodes through Co doping while effectively addressing the longstanding challenge of applying bulk electrode materials in HER applications.