ABSTRACT Seawater electrolysis is crucial for large‐scale green hydrogen production, yet high concentrations of chloride ions (Cl − ) result in competitive adsorption, leading to severe catalyst degradation and electrode corrosion. To address this challenge, we develop a Co 3 O 4 @carbonized polymer dots (CPDs) electrocatalyst, which achieves a low overpotential of 270 mV at 500 mA cm −2 , together with outstanding durability of 4200 h at 600 mA cm −2 and 3200 h at 800 mA cm −2 . An anion exchange membrane simulated‐seawater electrolyzer (AEMSE) based on Co 3 O 4 @CPDs achieves stable seawater electrolysis for over 1500 h at 1.0 A cm −2 with a very low cell voltage of 1.73 V. The combined experimental and theoretical studies reveal that CPDs stabilize the lattice oxygen and decrease the reaction energy barrier, thereby switching the lattice oxygen‐mediated mechanism (LOM) pathway to more desired adsorbate evolution mechanism (AEM). Furthermore, surface‐anchored CPDs generate CO 3 2− through electro‐oxidation, forming a protection system that blocks Cl − adsorption and penetration. This strategy successfully overcomes the corrosion bottleneck in seawater electrolysis and opens new avenues for sustainable hydrogen energy development.
Proton exchange membrane (PEM) water electrolysis is a promising strategy for large-scale hydrogen production; however, its industrial feasibility is hampered by the lack of highly active and durable oxygen evolution reaction (OER) catalysts in acidic environments. Ru-based catalysts offer high intrinsic activity but are susceptible to dissolution and structural degradation. To address this, this study proposes an electrically induced "nanoshield" strategy. A Ru single atom-doped Mn3O4 (Ru-Mn3O4) catalyst enables the in situ spontaneous reconstruction of the catalyst surface structure. Under an electric field, Mn3O4 crystals undergo interlayer slip and polarization rotation, inducing the growth of a porous MnO2 nanoshield on the catalyst surface, that effectively inhibits the dissolution of Ru active sites without compromising reaction activity. The catalyst exhibits excellent OER performance, delivering 10 mA cmgeo-2 at an overpotential of only 176 mV in 0.5 M H2SO4, and remains stable for over a year (8800 h) at a current density of 50 mA cmgeo-2. The PEM electrolyzer based on Ru-Mn3O4 shows a decay rate of 0.15 mV h-1 at 1000 mA cmgeo-2 and only 0.06 mV h-1 at 500 mA cmgeo-2, outperforming commercial RuO2. This study provides a new path for the construction of high-performance acidic OER catalysts and demonstrates the great potential of the nanoshield strategy in electrocatalytic structural protection.
Smart afterglow materials can dynamically regulate emission intensity, color, and lifetime in response to external stimuli, offering unique opportunities for multidimensional information output and environmental sensing. Among various luminescent platforms, carbon dots (CDs), particularly carbonized polymer dots (CPDs), have emerged as promising candidates for constructing intelligent afterglow systems owing to their tunable structures, abundant surface chemistry, multiple emissive centers, and processability. These features provide diverse excited state pathways and enable flexible modulation of afterglow behaviors under external stimuli. Recent advances have demonstrated that, through rational engineering of emissive centers, interfacial microenvironments, and excited state processes, various stimuli-responsive afterglow behaviors, including photoresponsive, temperature-responsive, time-dependent, chemical/mechanical responsive, and multi-stimulus responsive luminescence, can be achieved. Unlike previous reviews that mainly focused on static CPDs afterglow materials and their photophysical properties, this review summarizes recent progress in stimuli-responsive afterglow CPDs from the perspectives of structural design, emissive center construction, and regulation. Particular emphasis is placed on the roles of multiple emissive centers and excited state evolution in determining responsive afterglow outputs. Emerging applications in information security and biomedicine are highlighted. Finally, current challenges and future opportunities are discussed, including precise emissive center engineering, excited state mechanism elucidation, and multi-stimuli synergistic regulation.
Carbon dots (CDs) are an emerging class of carbon-based nanomaterials with broad applications in sensing, bioimaging, optoelectronics, and catalysis. However, a unified understanding of the relationship between their structural composition and functional evolution remains lacking due to the coexistence of various structural units generated during their synthesis via polymerization, crosslinking, carbonization, and surface reconstruction processes. In this review, CDs are revisited from the perspective of structural units, including rigid domains, flexible domains, and surface chemical structures. Their structural characteristics, regulation strategies, and functional roles are systematically summarized. Particular emphasis is placed on how these structural units regulate key electronic-state processes, including exciton localization, exciton recombination, and electron transfer. Furthermore, a structural-unit-driven functional evolution model is proposed, revealing the continuous transition of CDs from exciton-localization-dominated systems to electron-transfer-dominated systems. This framework provides new insights into the structure-property relationships of CDs and guides the rational design of carbon-based functional materials.
Wavelength-versatile laser systems play a critical role in the fields of spectroscopy, biomedical, light detection and ranging (LIDAR), precision measurement, and nonlinear frequency conversion. Among the various techniques for realizing this wavelength versatility, crystalline Raman lasers have emerged as a prominent solution. Such scheme overcomes inherent limitations of conventional techniques, including strict phase-matching and spatial hole burning, while offering additional benefits such as beam purification and pulse compression, making them an ideal platform for realizing wavelength-versatile lasers. This article provides a systematic review of the wavelength-versatile crystalline Raman lasers, detailing their operational mechanisms and technological progress in four types of wavelength operation: wavelength-tunable, wavelength-switchable, dual-wavelength, and multi-wavelength. Finally, future development trends are also discussed to offer theoretical references for wavelength-versatile crystalline Raman lasers.
Carbon dots (CDs), a class of emerging fluorescent nanomaterials, have garnered notable attention in the biomedical field owing to their outstanding photoluminescence properties, excellent biocompatibility, and ease of synthesis and functionalization. Recently, numerous CDs have been developed that allow precise subcellular localization through surface modifications or covalent conjugation with targeting ligands such as peptides, small molecules, Golgi-specific agents, and cell membrane-specific agents. This review begins with an overview of the synthesis strategies of CDs, highlighting their exceptional optical properties, stability, biocompatibility, and significance for subcellular imaging. The mechanisms by which CDs target specific organelles, including the nucleus, mitochondrion, lysosomes, Golgi apparatus, and cell membrane, are discussed. These mechanisms include specific targeting molecules, pH-sensitive targeting, charge-driven interactions, and hydrophobic and hydrophilic dynamics. Furthermore, we summarize their applications in subcellular imaging, such as the long-term dynamic monitoring of organelles, sensing, reactive oxygen species scavenging, and therapy. By presenting a comprehensive review of CDs in subcellular imaging, we aim to pave the way for further development of CDs in bioimaging and related biomedical applications.
A visible-light-driven, site-selective C(sp3)-H functionalization reaction was developed, which couples N-alkoxyphthalimides with readily available allylic peroxides to provide diverse epoxy alcohols under mild conditions without external oxidants. The sequence involves photoexcitation to generate oxygen-centered radicals, intramolecular 1,5-HAT to form remote carbon-centered radicals, and a subsequent radical homolytic-substitution cyclization to furnish the epoxide products. This operationally simple, modular protocol tolerates a broad range of functional groups, accepts varied N-alkoxyphthalimides and peroxide partners, and is amenable to scale-up and diversity-oriented synthesis, highlighting its potential for the assembly of complex molecules.
Self-powered ultraviolet photodetectors (SUVPDs) based on wide-bandgap semiconductors have attracted extensive attention; however, further performance improvement is still limited by bottlenecks such as insufficient carrier separation and inefficient interfacial charge transport. In this work, an electrochemical-type SUVPD is reported, in which Ru-derived species modified TiO2 nanorod arrays (Ru-TNRAs) are employed as a nanostructured photoanode to enhance photoelectric conversion capability. Compared with the unmodified TiO2 nanorod arrays (TNRAs), the Ru-TNRAs-based device exhibits a higher short-circuit current density (1.514 mA cm-2) and maximum power density (0.083 mW cm-2), together with a fastest decay time of 80 ms. After a cumulative UV irradiation time of 18,000 s, the device still retains 92.92% of its initial photocurrent density, demonstrating excellent operational stability. The enhanced performance is mainly attributed to the synergistic effect of Ru-derived species and defect states, which introduce sub-bandgap absorption and interfacial states and accelerate interfacial charge separation, thereby improving the "generation-separation-transport" efficiency of charge carriers under 365 nm UV excitation. This work proposes a synergistic interfacial modulation strategy involving Ru-derived species, defect states, and a quasi-solid-state electrolyte (QSE), enabling the simultaneous optimization of output, response speed, and operational stability under zero bias, and providing a generalizable route for the engineering design of photoanodes in electrochemical-type SUVPDs.
Most of phosphors undergo thermal quenching (TQ) at high temperature, due to thermal-activated non-radiative transitions. TQ effects lead to significant reduced luminous efficiency of phosphors at high operation temperature, hindering their application in high power phosphor-converted white light-emitting diodes (WLED). Here, we report a zero-dimensional metal halide perovskite: Cs2ZrCl6:Sb3+, exhibiting robust anti-TQ red emission up to 500 K, comparable to the mainstream anti-TQ phosphors (e.g. K2SiF6:Mn4+). The hetero-valent doping of Sb3+ induces structure defects of host and thus compensate the non-radiative emission loss through thermal accelerated energy transfer from defects to emitter at high temperature. We assembled the red anti-TQ phosphor into a white light-emitting diode (WLED) device, achieving stable output light intensity and chromaticity up to 2000 mA.
Near-infrared carbon dots (NIR CDs) have been used in optoelectronics and laser devices owing to their exceptional optical properties and remarkable laser gain performance. However, achieving anti-thermal-quenching steady-state NIR emission remains a significant challenge. Herein, we synthesized high-performance, anti-thermal-quenching aqueous NIR CDs exhibiting a maximum emission wavelength of 727 nm. Detailed characterizations indicated that the rigid conjugated carbon core with high graphitic nitrogen content promoted NIR emission. The CDs exhibited high exciton binding energy and minimal structural defects, which suppressed nonradiative transitions and enabled anti-thermal-quenching optical properties. Notably, thermally enhanced laser emission was successfully achieved. The lasing threshold decreased gradually with increasing temperature, and the system maintained stable operation for 6 h without significant attenuation, thereby fully verifying its excellent optical stability and feasibility as a laser source. The results demonstrate that the anti-thermal-quenching NIR CDs have significant potential for the development of high-performance steady-state optoelectronic and laser devices.
Chirality is ubiquitously present in nature and assumes a pivotal role in a vast array of fields. With the rapid advancements in chiral science and nanotechnology, chiral carbon dots (Ch-CDs), a class of nanomaterials featuring circularly polarized luminescence (CPL) properties, have emerged as a research hotspot. These materials possess remarkable optical properties, excellent biocompatibility, high stability, and abundant raw materials. Furthermore, the intrinsic chirality of Ch-CDs endows them with distinctive photophysical and chemical characteristics, making them a carbon nanomaterial with substantial development potential. They have been extensively applied in photoelectric detection, optical devices, biomedicine, information anti-counterfeiting, and encryption, thereby sparking intense interest and research within the academic community. This paper presents the first systematic refinement and summary of the construction strategies for Ch-CDs, encompassing one-step synthesis, surface modification, and assembly methods. It also reviews the advances in the optical properties of Ch-CDs, with a comprehensive elaboration on the latest research progress in tunable multicolor CPL, CPL enhancement, and triplet-state emission, thereby addressing the gap in reviews focused on triplet-related chiral functionalities. On this basis, the challenges and future perspectives pertaining to the diversified applications and development of Ch-CDs are proposed. This review not only summarizes the current state and achievements in the Ch-CDs field but also aims to pique readers’ curiosity regarding chiral materials. By doing so, we anticipate that this review will further propel fundamental research and future practical applications, thereby fostering the rapid development of the Ch-CDs field.
The symmetric FeN4 configuration in conventional single-atom catalysts strongly binds oxygenated intermediates, creating a high energy barrier for the rate-determining *OH desorption step and limiting ORR kinetics. Herein, we construct an asymmetric Mo–Fe dual-atom catalyst on a defect-rich N-doped carbon matrix (Mo–Fe–NC (MA)) to overcome this limitation. The FeN3–MoN3 coordination enables electron donation from Mo to Fe, weakening Fe–OH bonds and facilitating the rate-determining *OH desorption. The catalyst demonstrates outstanding oxygen reduction activity in 0.1 M KOH, with a half-wave potential of 0.918 V vs. RHE, surpassing Pt/C and single-atom references. In zinc-air batteries, it delivers a peak power density of 147.7 mW cm−2 and operates stably for over 725 h. Flexible solid-state devices also show robust performance under bending, highlighting their promise for wearable energy applications.
Rare-earth (RE) elements, owing to their unique electronic configurations and exceptional optical characteristics, have found increasingly broad applications in functional nanomaterials. However, the overall performance and aqueous stability of single-component RE-based materials remain insufficient for fulfilling the demands of multifunctional applications. Carbon dots (CDs), as an emerging class of fluorescent nanomaterials, have garnered significant attention due to their excellent water dispersibility, low toxicity, and robust photostability. Incorporating RE into CDs systems not only enriches their optical functionalities but also opens new avenues for the construction of multifunctional nanoplatforms. Despite these promising prospects, a comprehensive and in-depth understanding of the synthetic strategies, integration mechanisms, and tunable properties of RE-doped CDs is still lacking. To address this gap, this review summarizes the recent advancements in RE-CDs hybrid systems, focusing on fabrication approaches, coordination modes, optical property modulation, and practical applications. Finally, current challenges and future prospects of RE-CDs are discussed. We hope that this review will provide theoretical references and development ideas of RE functional materials and CDs optical modulation research.
ABSTRACT Carbon dots (CDs) exhibiting dual‐phase photoluminescence (PL) in the second near‐infrared window (NIR‐II, 900–1700 nm) region have shown considerable potential for applications in information encryption, lighting, and bioimaging. However, significant challenges remain owing to a lack of reliable design strategies. In this study, high‐brightness dual‐phase NIR‐II PL CDs (NIR‐CDs) were successfully prepared for the first time employing innovative strategies. NIR‐CDs possess a distinctive core–shell structure, and the donor–acceptor interactions between the carbon core and strong electron‐donating groups on the shell effectively induce a charge‐transfer state. The NIR‐CDs exhibited a fluorescence quantum yield (QY) of up to 5.91% at 920 nm in conjunction with excellent stability. Notably, the rich functional groups on the shell of NIR‐CDs provided hydrogen bonding sites, enabling a 960 nm fluorescence emission and high absolute QY of 3.82% in the solid state. The dual‐phase PL of NIR‐CDs enables their use in NIR‐II multilevel information encryption and fingerprint authentication. The NIR‐II flexible film based on NIR‐CDs exhibits excellent fluorescence stability under various external stimuli. Furthermore, the quick response code based on NIR‐CDs remains clearly identifiable beneath 3 mm porcine tissue, which highlights their potential for anti‐counterfeiting, encryption, and bioimaging sensing.
Gas adsorption enhances the field emission of carbon nanotube (CNT) cathodes, enabling the detection of low-pressure gases. This work investigated the structural characteristics of multi-walled carbon nanotubes (MWNTs) with excellent helium sensing effects which is closely related to the defect structures, and explored the controllable preparation of MWNT sensing cathode by modifying the catalytic substrate surface from the anodization process for the CVD growth. MWNTs with small diameters and short tube length may behave poor crystallinity, and the crystallinity could be improved by increasing the growth time from Raman and XRD analysis. MWNTs with high Raman ID/IG ratio of 0.83 and high XPS sp3 content at the anodization power of 35 W presented excellent helium sensing performance in the range of 10−8 to 10−4 Pa. The controllable growth of MWNTs is not only essential for helium sensing, but significant for defective CNT applications.
Anion exchange membranes (AEMs) have emerged as a key platform for next-generation alkaline electrochemical energy technologies, enabling the use of earth-abundant catalysts and offering a pathway toward cost-effective hydrogen production and energy conversion. However, their widespread deployment remains fundamentally limited by the intrinsic trade-offs among hydroxide conductivity, chemical stability, and mechanical robustness. Here, we provide a unified perspective on AEM design based on multi-scale structural engineering, highlighting that these trade-offs can only be overcome through coordinated multi-scale regulation across molecular, nanoscale, and macroscopic levels. We identify four interdependent design dimensions that govern AEM performance: polymer backbone engineering for intrinsic chemical stability, cation chemistry for controlling degradation pathways and ion dissociation, side-chain architecture for tuning ion transport and hydration structures, and organic-inorganic hybridization for reinforcing mechanical and functional properties. By integrating insights across these dimensions, we elucidate the fundamental structure-property relationships that dictate AEM behavior. Future AEM development will depend on precision polymer synthesis, biomimetic transport design, multi-scale modeling, and sustainable manufacturing. This review establishes a comprehensive framework for bridging molecular design and practical device performance, providing guidance for the rational development and scalable implementation of advanced AEM materials.
Electrides,characterized by interstitial quasi-atoms(ISQs)where electrons occupy lattice voids instead of atomic orbitals,provide a unique platform for discovering novel superconductors and mixed-conduction materials.Here,us-ing crystal structure prediction combined with first-principles calculations,we systematically explore lithium-rich Li-Bi compounds under high pressure.Several new Li-rich stoichiometries,LiBi,Li11Bi2,Li9Bi,and Li10Bi,are identified as thermodynamically stable.Among them,the C2/m phase of Li10Bi features one-dimensional ISQ networks,exhibit-ing both metallic and electride characteristics.Electron-phonon coupling analysis reveals a dome-shaped evolution of superconducting transition temperature(Tc),reaching a maximum value of 9.9 K at 35 GPa,where the superconductiv-ity is primarily driven by strong Li-derived phonon modes.Ab initio molecular dynamics simulations further reveal a temperature-induced superionic transition above 700 K,where Li+ions diffuse freely while Bi atoms remain fixed within the lattice.This coexistence of superconductivity and superionicity within a single crystalline framework highlights Li10Bi as a prototype dual-functional electride,bridging the gap between quantum superconductors and solid-state lithium-ion conductors.These findings open a new route for designing multifunctional materials that integrate electronic and ionic transport for next-generation energy and quantum applications.
Multimetal doping is widely employed to enhance oxygen evolution reaction electrocatalysis; however, the underlying mechanism remains poorly understood due to the complex interplay. Herein, we rationally integrate rare-earth Ce and transition-metal Ru into NiFe-MOFs (Ce,Ru-NiFe-MOFs) to achieve orbital complementarity between localized 4f and delocalized 4d states, thereby enabling a fundamentally distinct electronic regulation strategy beyond conventional charge transfer. This coupling effect fundamentally alters the dynamic evolution of the catalyst by accelerating the transformation of NiFe-MOFs into active NiFeOOH species. We further demonstrate that Ce/Ru codoping induces oxygen-bridged multicenter orbital coupling (3d-4d-4f), as evidenced by soft- and hard-X-ray absorption spectroscopy and aberration-corrected high-angle annular dark-field scanning transmission electron microscopy, together with density functional theory calculations, thereby establishing nonadditive electronic interactions and multilevel electron-transfer pathways. Consequently, the reconstructed catalyst exhibits an optimized electronic structure with enhanced OH- adsorption, suppressed proton-induced corrosion, and reduced energy barrier for the rate-determining step. Therefore, the catalyst delivers an overpotential of 199 mV at 10 mA cm-2 and outstanding durability exceeding 1600 h at 400 mA cm-2. Additionally, when integrated into an anion-exchange membrane water electrolysis system, it achieves a low cell voltage of 1.747 V at 1000 mA cm-2 (meeting the U.S. DOE 2026 target) and maintains stable operation for over 95 h at 500 mA cm-2. This work establishes a clear mechanistic framework linking orbital-level coupling, reconstruction kinetics, and catalytic performance, and provides a general design principle for engineering advanced electrocatalysts via multicenter orbital interactions.
This study investigates the morphological structure,polarization mechanism,and fluorescence regulation effect of Polymer Dispersed Liquid Crystal(PDLC)composite materials doped with Carbon Quantum Dots(CQDs)nanomaterials.Based on the micro-morphological structure of PDLC films,the influence of this structure on liquid crystal droplet size is analyzed.Using dielectric measurement data and Cole-Cole plots,the CQDs-induced non-Debye relaxation polarization process of the composite film under different frequencies is studied,while the effects of CQDs doping on relaxation time and relaxation distribution parameter are also analyzed.Furthermore,the impacts of these two factors on the electro-optical properties of the films are explored.Under the synergistic regulation of CQDs mass fraction and exposure intensity,the effects of PDLC's dielectric properties and scattering performance on the film's fluorescence performance are investigated.The experimental results show that:when the CQDs doping amount is 0.2%(mass fraction),compared with undoped PDLC,the relaxation time of the PDLC composite film decreases by 56%,and the threshold voltage and saturation voltage decrease by 19.9%and 11.8%respectively,and the on-state and off-state switching response times decrease from 32 ms and 50 ms to 10 ms respectively;when the exposure intensity decreases from 30 mW/cm2 to 1 mW/cm2,the peak fluorescence intensity of PDLC increases by approximately 130%.This work effectively realizes the synergistic improvement of electro-optical properties and fluorescent characteristics of PDLC,providing valuable insights for the development of PDLC composite materials.