Efficient and sustainable photocatalytic hydrogen peroxide (H2O2) synthesis is crucial due to its role as an eco-friendly oxidant and the limitations of conventional industrial methods. Graphitic carbon nitride (g-C3N4) is a promising photocatalyst but suffers from inefficient charge separation and limited visible light absorption. This study introduces a dual-modified g-C3N4, incorporating Na+/K+ ions and cyano groups, coupled with ultrathin BiOCl nanosheets to form an S-scheme heterojunction (CN-NH-NaK/BiOCl). The modification enhances the electronic structure, visible light absorption, and charge separation. The CN-NH-NaK/BiOCl photocatalyst achieved an outstanding H2O2 production rate of 33.15 mmol & centerdot;g(-1)& centerdot;h(-1) under visible light (lambda >= 400 nm), outperforming pristine g-C3N4 (118-fold) and BiOCl (83-fold), and surpassing all previously reported g-C3N4- and BiOCl-based photocatalysts. Even in pure water, the production rate reached 5.18 mmol & centerdot;g(-1)& centerdot;h(-1), exceeding that of most previously reported catalysts. Comprehensive characterization revealed an efficient S-scheme charge transfer mechanism, enabling selective 2e(-) oxygen reduction reaction (94.06% selectivity) and water oxidation. The heterojunction demonstrated excellent stability, reusability, and enhanced degradation of tetracycline hydrochloride. This work provides a promising strategy for advanced S-scheme photocatalysts in sustainable H2O2 production and environmental remediation. (c) 2026, Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. All rights reserved.
Silicon-based anodes are among the most promising options for next-generation high-energy lithium-ion batteries because of their high room-temperature theoretical capacity (3579 mAh g−1 for Li15Si4), natural abundance, and favorable cost-to-performance ratio. Their practical use, however, is still limited by severe volume variation during cycling, which causes particle fracture, repeated interphase rupture/regrowth, transport heterogeneity, and rapid loss of Coulombic efficiency. This review examines electrolyte engineering as the key lever for addressing these coupled failure modes across liquid, quasi-solid, and all-solid-state systems. Liquid electrolytes remain the most mature route for near-term deployment, but their performance is constrained by unstable and continuously evolving SEI chemistry. Quasi-solid electrolytes offer a more balanced pathway by combining liquid-like ionic transport with mechanical confinement and interfacial regulation. All-solid-state electrolytes provide the strongest long-term prospects for safety and energy density, yet their current performance is limited by solid–solid contact loss and chemo-mechanical instability. On this basis, we summarize practical design principles for solvation regulation, interphase chemistry, mechanical adaptability, full-cell compatibility, and manufacturability. The review is intended to provide an application-oriented framework for designing silicon anodes and related high-capacity alloying anodes for high-energy batteries.
The detection of toxic triethylamine (TEA) is crucial for environmental monitoring and human health protection. However, developing TEA sensors with both high sensitivity and selectivity remains challenging. In this work, we report a high-performance gas sensor constructed from hamburger-like ZnO microspheres modified with graphene oxide (GO), forming well-defined GO/ZnO heterojunctions. The optimized 10% GO/ZnO composite exhibits an outstanding response of 1230 to 100 ppm TEA at 260 degrees C, approximately 820 times higher than that of pristine ZnO. The remarkable enhancement arises from the synergistic effect of the hierarchical hamburger-like structure, the excellent electrical conductivity of GO, and the formation of a p-n heterojunction, which collectively amplify the gas-sensing signal. Moreover, the sensor achieves a low detection limit of 500 ppb and excellent selectivity against various interfering gases. This work not only demonstrates a superior TEA sensor but also provides a rational strategy for heterostructure design in advanced gas-sensing applications.
In theory, the utilization of a Z-scheme photogenerated carrier transport system has the potential to significantly enhance the photogenerated voltage for photoelectrochemical overall water splitting. However, thus far, there have been no previous reports on such phenomena with silicon-based semiconductor photoelectrodes. In this study, we fabricated an n-Si/Pt/Mo-doped BiVO4 (Mo: BVO) sandwich-like film with an intermediate carrier transfer layer to prepare a silicon-based photoelectrode with an indirect Z-scheme system. Additionally, by leveraging the lattice distortion effect over Mo: BVO, we increased the fusion ability of the sandwich-like interface between different substances. For the first time, we achieved generation of anodic displacement current via negative voltage (-0.57 V (vs. RHE)), resulting in a photocurrent density of 1.56 mA/cm(2) and a photogenerated voltage five times higher than that of the n-Si/Mo: BVO structure. Through combining experimental approaches with theoretical calculations, it has been confirmed that this realization is attributed to the contribution of the transport process within the Z-scheme system in the n-Si photoelectrode. Furthermore, milliampere-level photocurrent under negative bias was observed for the first time on an n-Si photoelectrode, providing a novel approach for constructing silicon-based photoelectrodes for overall water splitting.
Detecting ethanol is critically important due to its widespread industrial applications and potential safety hazards, posing significant risks to both industrial production and human health.
This work presents a BiVO 4 -based photoanode co-modified with SnO 2 quantum dots and a FeOOH cocatalyst, enhancing the photocurrent, charge separation, and oxygen evolution for efficient solar-to-hydrogen conversion.
Metallic Zn anodes are pivotal for high-energy Zn-ion storage but face intractable challenges, typically including dendrite proliferation, parasitic hydrogen evolution reaction (HER), and sluggish ion transport. Here, we report a temporally programmed dual-phase strategy, coordinating electrolyte solvation manipulation for rationally designed growth of three-dimensional (3D) Zn architectures. By modulating ZnCl2 concentrations, we dynamically configure the solvation complexes from [Zn(H2O)6]2+ to [ZnCl(H2O)5]+, which steers the epitaxial growth of Zn nanosheet arrays with dominant exposed crystal faces from (101) to (002), thus fundamentally suppressing the dendrites and HER with reduced interfacial impedance (down to only 6.8 Omega s-1). Such a crystal plane-engineered anode exhibits excellent performance with 97.8% capacity retention over 10 000 cycles in Zn-HSCs, delivering an energy density of 54.1 mu Wh cm-2 (1.08 mW cm-2) and retaining 77% efficiency at 16.7 mW cm-2. Based on the molecular dynamic simulations and experimental analyses, the mechanism of crystal plane engineering based on concentration-driven solvation-topology interplay has been demonstrated, establishing a metastable crystallization paradigm for scalable fabrication of ultra-stable metal electrodes.
ABSTRACT Developing efficient and durable photocatalysts for solar‐driven hydrogen production remains a critical challenge for sustainable energy technologies. Herein, we report a robust ZnO/ZnS heterojunction nanocomposite prepared via a facile hydrothermal sulfidation strategy, in which the surface transformation of flower‐like ZnO into ZnS can be precisely regulated by adjusting the sulfidation time. Among the obtained samples, the optimized ZnO/S‐24 delivers an outstanding hydrogen evolution rate of 21.08 mmol·g −1 ·h −1 under visible light irradiation, approximately 22 times higher than that of pristine ZnO, and shows excellent cycling stability. Comprehensive structural and physicochemical characterizations reveal that the superior performance arises from the synergistic integration of three key factors: a well‐constructed interfacial S‐scheme heterojunction, which promotes directional charge separation while preserving strong redox potentials; an almost twofold increase in specific surface area, which provides abundant accessible active sites; and reduced interfacial charge‐transfer resistance, as confirmed by photoelectrochemical measurements. XPS, UPS, EPR, and Mott‐Schottky analyses collectively verify the formation of an internal electric field and the S‐scheme charge transfer pathway across the ZnO/ZnS interface. This work not only demonstrates an effective route to engineer high‐performance ZnO‐based heterostructures, but also offers valuable insight into the rational design of sulfide‐modified oxide photocatalysts for efficient solar‐to‐hydrogen conversion.
Detecting ethanol is critically important due to its widespread industrial applications and potential safety hazards, posing significant risks to both industrial production and human health. However, the development of ethanol sensors with high sensitivity and selectivity remains a substantial challenge. In this study, we demonstrate a highly sensitive and selective ethanol sensor based on rationally-designed heterojunctions, fabricated by decorating In2O3 nanotubes with Ag nanoparticles (NPs) through solvothermal and coprecipitation methods. The obtained Ag/In2O3 sensor exhibits exceptional ethanol sensing performance (S = 110.5 to 100 ppm), which exhibits an approximately 11-fold enhancement compared to that of pristine In2O3, and surpasses those of most ethanol sensors ever reported. Such improvement is mainly attributed to the synergistic effects of Schottky junction formation, electronic sensitization, and chemical catalysis, which collectively enhance electron transfer efficiency and surface reaction kinetics. Moreover, the as-constructed sensor demonstrates rapid response/recovery characteristics (50/70 s), excellent selectivity against interfering gases, and remarkable long-term stability, representing its promise toward practical applications.
Uncontrolled dendrite growth and parasitic side reactions at defect‐rich regions severely limit the cycling stability of aqueous Zn‐ion batteries (AZIBs). Here, we propose a simple, carbon‐nanopatch strategy based on candle‐flame pyrolysis for stabilizing Zn anodes. After rinsing, the introduced carbon nanoparticles are mainly retained in microscopic defect‐rich regions, forming localized carbon nanopatches (CNPs) on the Zn surface. Experimental characterization and theoretical analysis suggest that these localized CNPs can help alleviate local electric‐field intensification, promote more uniform current‐density and interfacial Zn 2+ distribution, and reduce direct electrolyte exposure at defect‐rich regions. In addition, flame treatment may promote grain growth within the Zn foil, which can further improve interfacial stability. As a result, Zn@CNPs symmetric cells achieve cycling lifetimes of 3450 h at 1 mA cm −2 /1 mAh cm −2 and 3500 h at 5 mA cm −2 /1 mAh cm −2 . When paired with a β‐MnO 2 cathode, the full cell retains 74% of its capacity after 1000 cycles at 1 A g −1 , compared with 28% for the cell using Bare Zn. This work provides a simple and cost‐effective strategy for developing more stable aqueous Zn‐based batteries.
Efficient photocatalysts for hydrogen production are essential for the development of sustainable energy technologies. Among them, zinc sulfide (ZnS) has emerged as a highly promising candidate. Nevertheless, its photocatalytic efficiency remains severely constrained by rapid charge carrier recombination and insufficient light absorption. This work presents an anion-exchange-triggered strategy that simultaneously introduces sulfur vacancies (VS) and incorporates chloride ions (Cl-) into mesoporous ZnS nanospheres, resulting in the formation of VS-Cl-ZnS. This synergistic defect engineering effectively narrows the band gap, shifts the conduction band to a more negative potential, and optimizes the hydrogen adsorption free energy, thereby enhancing the proton reduction efficiency. Consequently, the resultant VS-Cl-ZnS catalyst achieves an exceptional H2 evolution rate of 17.29 mmolg-1h-1, surpassing that of pristine ZnS by 8-fold and exceeding those of most reported ZnS-based photocatalysts. Furthermore, the catalyst demonstrates outstanding stability, maintaining activity over 15 h of continuous operation without significant degradation. The enhanced photocatalytic behaviors could be mainly attributed to improved charge separation, extended carrier lifetime, and optimized surface reaction kinetics, enabled by targeted defect engineering. Additionally, the mesoporous structure of VS-Cl-ZnS facilitates efficient mass transfer and active site accessibility. This work provides a paradigm for enhancing sulfide-based photocatalysts through precise defect manipulation, offering valuable design principles for high-performance solar-driven hydrogen production systems.
ABSTRACT Photocatalysis has emerged as a promising approach for solar energy conversion and environmental remediation. However, its practical implementation is still hindered by limited charge‐separation efficiency, slow surface reaction kinetics, and insufficient catalyst stability. High‐entropy alloys (HEAs), with their complex multicomponent structures, lattice distortion, diverse atomic environments, and tunable electronic properties, have gained significant attention as a new class of photocatalytic materials. This review summarizes recent advancements in HEAs‐based photocatalysis, focusing on key characteristics that enhance photocatalytic performance, including entropy stabilization, electronic structure modulation, surface‐site heterogeneity, and interfacial charge‐transfer behavior. HEAs function both as cocatalysts with semiconductor photocatalysts and as direct catalytic phases in photocatalytic and photo‐Fenton processes. Applications include hydrogen evolution, CO 2 conversion, pollutant degradation, and advanced oxidation reactions. The review also critically addresses current challenges such as precise composition control, active‐site identification, mechanistic understanding under operating conditions, standardized performance evaluation, and long‐term stability. Finally, it discusses future research directions, including theory‐guided compositional design, operando characterization, scalable synthesis, and integration into practical solar‐energy systems.
Abstract The efficient conversion of solar energy into chemical fuels and value-added products requires simultaneous optimization of photogenerated carrier utilization and surface reaction kinetics. However, conventional photocatalytic systems are generally limited by inefficient charge separation, while thermal catalytic strategies often require external energy input and harsh operating conditions. From a fundamental perspective, the development of photothermal S-scheme heterojunction photocatalysts represents a charge-thermal coupling strategy, in which S-scheme heterojunctions primarily regulate the thermodynamic pathway of photogenerated carriers by inducing directional charge transfer, internal electric fields, and selective carrier recombination, whereas photothermal effects provide kinetic activation through localized heat generation and accelerated surface reaction processes. This review systematically summarizes recent advances in photothermal-assisted S-scheme heterojunction catalysis based on this thermodynamic-kinetic synergy. The fundamental principles governing S-scheme charge migration and photothermal energy conversion are discussed, with particular emphasis on their complementary roles in improving carrier utilization and catalytic reaction efficiency. Representative photothermal S-scheme architectures, including self-heated, dual-thermogenic, and externally assisted systems, are comprehensively analyzed by correlating material composition, interfacial structure, defect engineering, and thermal-management strategies with catalytic performance. Furthermore, the influence of localized photothermal fields on interfacial charge dynamics, reactant activation, and reaction pathways is critically evaluated to clarify the intrinsic charge-thermal interactions. Finally, the current challenges and future perspectives for rationally designing high-performance photothermal S-scheme catalytic systems are proposed. This review provides a mechanistic understanding of charge-thermal coupling in advanced solar-driven catalysis and offers valuable insights into the development of next-generation photocatalytic materials.
The advancement of non-enzymatic glucose sensors is essential for enhancing the cost-effectiveness and continuous monitoring capabilities of glucose detection systems. Employing innovative materials and device structures constitute key strategies to achieve this objective. Herein, an in-situ growth method of laser-induced graphene (LIG) using dye-stained polyimide colloids formed films on various substrates was introduced. The costefficient, rapid, and portable glucose sensor was developed based on LIG patterned via direct laser writing (DLW), combining with a layer-by-layer growth method to deposit Cu3(HHTP)2 (HHTP, 2,3,6,7,10,11-hexahy-droxytriphenylene) onto the surface of LIG. By utilizing the first-principles density functional theory (DFT) calculations, the results shows that the LIG result in an upward shift of the d-band of Cu3(HHTP)2, hindering electrons from filling into the anti-bonding orbitals and improving the adsorption ability of the intermediate product on the surface, enhancing electrode catalytic activity. The glucose sensor has achieved a wide detection range (0.01-22 mM), a low detection limit (3 mu M) and an excellent sensitivity (5276 mu A mM-1 cm-2) in the low concentration range. This work provides novel insights into the growth of LIG on various substrates and offers a non-enzymatic sensor capable of accurate glucose measurements, while demonstrating exceptional reliability, stability and precision.
In the realm of photodetector (PD) technology, photoelectrochemical (PEC) PDs have garnered attention owing to their inherent advantages. Advances in this field depend on functional nanostructured materials, which are pivotal in improving the separation and transport of photogenerated electron-hole pairs to improve device efficiency. Herein, a highly photosensitive PEC UV PD is built using integrated self-supporting SiC/ZnS heterojunction nanowire array photoelectrodes through anodization and chemical deposition. Compared with the original SiC nanoarrays, the optimized SiC/ZnS-25 nanoarrays exhibit high photocurrent density (Dph, 809.2 mu A cm-2), rapid rise/decay times (tau r/tau d, 4/21 ms), high responsivity (R lambda, 1.226 A W-1), remarkable detectivity (D*, 2.517 x 1011 Jones), and large external quantum efficiency (EQE, 40.57%) under 375 nm UV light with a bias voltage of 0.6 V. Furthermore, SiC/ZnS-25 delivers excellent self-powered performance, with R lambda, D*, and EQE reaching 0.91 A W-1, 1.69 x 1011 Jones, and 30.24%, respectively. In addition, the device exhibits excellent long-term operation and aging stability under a bias voltage of 0.6 V and under self-powered conditions. The excellent photodetection behaviors of the SiC/ZnS PEC PD are mainly ascribed to the synergistic effect of the novel well-aligned nanowire geometry, heterojunction with ZnS nanofilms of optimal thickness, and integrated self-supporting configuration of the photoelectrode.
Efficient photocatalytic water splitting can be significantly enhanced through the careful design of S-scheme heterostructures, which play a pivotal role in optimizing performance. Herein, we report the construction of ZnIn2S4/CdS S-scheme heterojunctions under ambient conditions, based on a sonochemical strategy. This structure is facilitated by the well-matched interface between the (007) plane of layered ZnIn2S4 and the (101) plane of CdS, leading to a threshold optical response of 2.12 eV, which optimally aligns with visible light absorption. As a proof of concept, the resulting ZnIn2S4/CdS catalysts demonstrate a remarkable improvement in photocatalytic H-2 evolution, achieving a rate of 5678.2 mu mol h(-1)g(-1) under visible light irradiation (lambda > 400 nm). This rate is approximately 10 times higher than that of pristine ZnIn2S4 nanosheets (NSs) and about 4.6 times higher than that of CdS nanoparticles (NPs), surpassing the performance of most ZnIn2S4-based photocatalysts reported to date. Moreover, they deliver a robust photocatalytic performance during long-term operation of up to 60 h, showing their potential for use in practical applications. Based on the theoretical calculation and experimental results, it is verified that the movements of electrons and holes in the opposite direction could be induced by the disparity in the work function and the internal electric field within the interfaces, thus facilitating the construction of S-scheme heterojunctions, which fundamentally suppresses carrier recombination while minimizing photocorrosion of ZnIn2S4 toward enhanced photocatalytic behaviors.
An ultra-sensitive photoelectrochemical (PEC) biosensor for amyloid-beta 40 (Aβ40), a biomarker for Alzheimer’s disease (AD), was developed using g-C₃N₄ modified with gold nanoparticles (Au NPs) to form Au-C₃N₄. This was further combined with TiO₂ to create a tightly bonded TiO₂/Au-C₃N₄ heterojunction, leading to a highly responsive photocatalytic process. Furthermore, the incorporation of noble metal Au NPs not only enhances photocurrent generation but also securely immobilizes the aptamer through Au–S bonds, providing additional surface binding sites. This significantly increases the sensor's capture efficiency. The sensor exhibited excellent performance, featuring a linear detection range from 10−15 to 10−11 g/mL and a remarkably low detection limit (LOD) of 0.33 fg/mL. Moreover, the validation in clinical settings demonstrated the successful detection in real cerebrospinal fluid (CSF) and plasma, from AD patients and non-AD controls. These results strongly suggest that PEC biosensors possess significant potential as cost-effective and highly sensitive tools for detecting ultra-trace substances in human body fluids, which offers promising opportunities for the early screening of high-risk populations for AD.
Graphitic carbon nitride (g-C3N4) is recognized as a sustainable and cost-effective alternative for hydrogen peroxide (H2O2) production, but its efficiency is fundamentally hindered by intrinsic limited surface area, charge separation, and light absorption. In this study, we propose an innovative strategy to address these issues by engineering vacancy-defective g-C3N4 nanowire clusters. The resulting nanowire clusters, with enhanced surface area and uniformly distributed carbon vacancies, exhibit a remarkable H2O2 production rate of 4.11 mmol g-1 h-1 under visible light irradiation, representing an approximately 15-fold improvement over bulk g-C3N4. The engineered carbon vacancies are shown to enhance O2 adsorption and reduce the energy barrier for *OOH hydrogenation to H2O2, thereby enabling a highly efficient and selective oxygen reduction reaction (ORR). Furthermore, the material demonstrates a tetracycline hydrochloride degradation rate of up to 81.98%, highlighting its promising potential for environmental applications. Notably, this work is the first to report the unique nanowire cluster morphology of g-C3N4, which, in conjunction with defect engineering, offers new insights into the development of advanced photocatalysts for H2O2 production. Compared to most previously reported defect-modified g-C3N4 materials, the photocatalytic performance of our nanowire clusters is significantly superior, marking an important advancement in the field.
Stretchable supercapacitors are crucial for powering the next generation of wearable devices, but they face the challenge of insufficient areal capacitance. Although 3D electrodes improve the amount of active materials, their considerable thickness can increase stiffness and restrict deformability. Inspired by Armadillo's armor that incorporates rigid bony plates within elastic skin for optimal protection and flexibility, this study presents a 3D electrode designed to balance these conflicting requirements. The electrode comprises an array of densely packed, porous conductive pillars anchored to a soft current collector, effectively decoupling electrochemical and mechanical functions. The 900 mu m-thick pillars act as a porous scaffold, enabling high loading of active material PEDOT at 10 mg cm-2. Meanwhile, the current collector efficiently dissipates applied tension, resulting in exceptional deformability for the electrode. To demonstrate their practical application, these supercapacitors are integrated into a soft, untethered electronic system featuring a wireless charging circuit with a skin-conformal LED array for sustained operation. By effectively addressing the longstanding challenge of balancing high capacitance with mechanical compliance, this bioinspired electrode design establishes a transformative approach to create high-performance, deformation-resilient energy storage devices for wearable technologies.
To address safety and economic issues in hydrogen storage and transportation, developing liquid organic hydrogen carriers to deliver hydrogen to where it can be utilized for in situ hydrogen production is an attractive approach. Herein, a spinel phase high‐entropy oxide (HEO) (FeCrCoNiCu) 3 O 4 comprising of non‐noble metals is synthesized via the PVP (Polyvinyl Pyrrolidone)‐templated method as a catalyst for solar‐driven hydrogen production through methanol decomposition. Benefiting from the synergistic effects of various components in high‐entropy materials, (FeCrCoNiCu) 3 O 4 HEO achieves an optimized hydrogen production rate of 49.4 mmol g −1 min −1 , with a surface temperature of 279 °C under full‐spectrum illumination of 2.68 W cm −2 . The performance is significantly higher than that under thermocatalytic conditions at the same temperature and surpasses the activity of the state‐of‐the‐art catalysts. The catalyst exhibits long‐term stability over 80 h through in situ removing deposited carbon, and thus HEOs show great promise for efficient hydrogen production from methanol decomposition under mild conditions.