Latest ArticlesSupported catalysts are an effective approach in proton exchange membrane water electrolysis (PEMWE) owing to their enhanced metal-support interfacial interaction. We propose a novel high-temperature shock (HTS) technique by Joule-heating to construct an electronic coupling interface between IrO2 nanoclusters catalysts and TiO2 support (IrO2/TiO2-HTS). The HTS strategy features an ultrafast heating rate and compresses the synthesis time from hours to seconds (2 h to 60 s). The as-prepared catalyst features uniformly embedding the ultrafine IrO2 nanoclusters enrich oxygen vacancies within the redox-active metal oxide matrix, yielding exceptional mass activity and ultrastable performance. The mass activity of the catalyst is 1081 A/gIr at 1.6 V vs. RHE, 13 times higher than of commercial IrO2, and it demonstrates operation time for over 1100 h at 10 mA/cm2 with a voltage decay rate of only 40 μV/h. This HTS strategy offers a scalable route to accelerate vacancy engineering and strong metal oxide-support interaction (SMOSI) formation, enabling high activity at reduced Ir loading and long-term stability under acidic conditions. The approach is general and can be extended to other supported binary oxides, opening opportunities for the development of additional high–performance OER catalysts and PEM–relevant electrolysis systems.
Skin aging is a multifactorial biological process driven by oxidative stress (OS), chronic inflammation, cellular senescence, mitochondrial dysfunction, and non-enzymatic glycation (NEG), and is markedly accelerated by environmental stressors such as ultraviolet radiation (UVR) and air pollution. Natural bioactive compounds, including flavonoids, polyphenols, terpenoids, alkaloids, vitamins, polysaccharides, peptides, and indole derivatives, have demonstrated considerable potential in mitigating these processes through multi-target antioxidant, anti-inflammatory, anti-photoaging, and extracellular matrix (ECM)–protective mechanisms. However, their clinical and cosmetic translation is often limited by poor solubility, chemical instability, and insufficient skin penetration. Rather than providing a simple compilation of existing studies, this review offers a mechanism-oriented and delivery-driven synthesis of recent advances in natural anti-skin-aging research. We systematically integrate current knowledge on the molecular drivers of skin aging with a critical comparison of emerging transdermal and nanotechnology-based delivery systems, including lipid-based, polymer-based, inorganic/hybrid, and nucleic acid–assembled nanocarriers. Particular attention is given to how rational carrier design modulates stability, permeability, skin-layer targeting, and controlled release behavior. Furthermore, this review critically discusses current limitations, contradictory findings across studies, and key translational challenges, and identifies promising future research directions, such as stimuli-responsive systems, skin-layer-specific targeting, and mechanism-guided material selection. By bridging biological mechanisms with delivery material innovation, this work provides a forward-looking framework for the development of safer, more effective, and scientifically grounded anti-skin-aging therapeutics and cosmeceuticals.
The outer membrane (OM) of Gram-negative bacteria, with its unique and complex structure, serves as a critical structural foundation for their heightened pathogenicity and drug resistance. However, with a thickness of only 7–9 nm, the OM is highly fragile and undergoes continuous remodeling, making it difficult to elucidate its structural dynamics and functional mechanisms during bacterial growth, division, and host invasion. Here, we developed Rho-PMXB as an OM-specific fluorescent probe that incorporates a polymyxin-derived moiety for highly specific recognition of OM lipopolysaccharides (LPS) and a rhodamine fluorophore that confers excellent photostability and high fluorescence brightness. Rho-PMXB enables selective labeling of the OMs of various Gram-negative bacteria and supports super-resolution imaging, allowing real-time visualization of OM dynamics during bacterial growth, division, and antibiotic treatment, thereby providing insight into antimicrobial mechanisms. Furthermore, Rho-PMXB enables dynamic super-resolution imaging of pathogen-host cell interactions, visualizing OM behavior during Porphyromonas gingivalis invasion of human gingival epithelial (HGE) cells and revealing its interplay with the host plasma membrane and actin cytoskeleton.
Photoresponsive supramolecular polymers hold great promise for applications in sensing, actuation, and biomedicine. However, the role of photothermal effects in regulating supramolecular assemblies and their dynamic structural evolution at the microscopic level remains poorly understood, as most studies have primarily focused on molecular photochemical mechanisms. Herein, we report a photothermal-responsive supramolecular system based on 1,8-naphthalimide building blocks. By reducing hydrogen-bonding sites through modification of the amide N-substituent of BAze from 4-(hydroxymethyl)benzyl to benzyl, an OH-free derivative, PhAze, was obtained. This subtle structural change endows PhAze assemblies with photoresponsive behavior that markedly differs from that of BAze assemblies. Upon 488 nm laser irradiation, PhAze assemblies undergo nanofiber rupture accompanied by ~40% fluorescence enhancement, whereas BAze assemblies show only a slight fluorescence decrease without morphological change. Real-time in situ observation based on confocal laser scanning microscopy (CLSM) reveals the dynamic photoresponse of PhAze nanofibers. Localized fluorescence enhancement first appears along the fibers, followed by the formation of molten-like microspheres that ultimately lead to fiber rupture. Two distinct modes of microsphere formation, synchronous and asynchronous, are identified during this process. Moreover, thermal imaging further confirms that the response originates from a photothermal effect, where localized temperature rise weakens noncovalent interactions and induces partial melting of the supramolecular fibers. This study provides direct in situ insights into photothermal-driven structural evolution in supramolecular assemblies and offers a new strategy for designing photothermal-responsive supramolecular materials.
Photocatalytic conversion of polylactic acid (PLA) into high-value-added pyruvic acid (PA) presents a promising strategy for carbon-efficient resource cycling. However, successive dehydrogenation at the α-C of lactic acid (the monomer of PLA) remains a critical challenge. In this study, we fabricated an Au-modified CdS nanosphere photocatalyst (Au-CdS), where the introduction of Au facilitates the activation of the Cα-H bond in lactic acid (LA). Through combined theoretical calculations and in-situ EPR analysis, Au-CdS reduces the Cα-H bond cleavage energy barrier from 1.02 eV to 0.49 eV, substantially elevating the generation of carbon-centered radical intermediates. In addition, Au-CdS demonstrates enhanced separation efficiency of photogenerated electron-hole pairs relative to pristine CdS, thus efficiently activating O2 to generate O2•− radicals and further driving the conversion of O2•− to •OH radicals. The produced •OH radicals facilitate the successive dehydrogenation reactions via interacting with the Cα-H and α-OH bonds on the α-C of LA, thereby promoting the selective conversion of LA to PA. As a result, the Au-CdS catalyst achieves a PA production rate of 1340 ± 25 μmol g-1 h-1, surpassing that of pristine CdS by 8.9-fold. This work presents a novel strategy for the value-added upcycling of plastic waste.
To address the challenges of active metal leaching and sluggish redox cycling in heterogeneous metal-catalyzed peroxymonosulfate (PMS) activation, this study proposes a double heteroatom co-anchoring and regulation strategy to design a sulfur-nitrogen co-doped carbon-supported cobalt nanoparticle catalyst (Co-S-CN). This strategy successfully constructs a “S2--Co0” dual micro-reduction environment, significantly accelerating the Co3+/Co2+ redox cycle. Experimental results demonstrate that the Co-S-CN+PMS system achieves 100% phenol degradation within 5 min while exhibiting exceptional resistance to anion interference (SO42−, Cl−, HCO3−, H2PO4−). Low cobalt leaching rate (<1%) across various pH conditions confirms strong metal anchoring via S-N synergy. Structural characterizations verify the existence of S2- and Co0, and co-optimizing cobalt valence cycling. Electron paramagnetic resonance (EPR) and quenching experiments indicate the reaction proceeds primarily via a nonradical pathway, with singlet oxygen (1O2) as the key reactive species. Density functional theory (DFT) calculations reveal that S-N synergy enhances PMS adsorption strength (adsorption energy optimized from −3.51 eV to −3.77 eV), increases charge density (Bader charge increased from 0.75 e to 0.80 e), and optimizes the electronic structure of Co 3d orbitals (d-band center upshifted from −1.341 eV to −1.330 eV). This work provides a strategy for rational design of highly active and stable catalysts.
As an indispensable subset of functional materials, quadratic nonlinear optical (NLO) switches have garnered increasing attention owing to their vast potential in next-generation intelligent optoelectronic devices. Despite considerable progress in NLO switches based on solid-state phase transitions, identifying an effective strategy to design high-efficiency NLO switches remains a huge challenge. Herein, we present a molecular engineering approach to develop a high-efficiency lead halide organic-inorganic hybrid NLO switch, (C8H12N)2Pb2Cl6·H2O (NMPTPC). Through the substitution of hydrogen with a methyl group (-CH3) in protonated N-methylaniline, the initial compound (C7H10N)2Pb2Cl6·H2O (NMAPC) transformed into NMPTPC retaining the original space group, which gives rise to a dramatic enhancement of second harmonic generation (SHG) and phase transition temperature. As expected, NMPTPC exhibits high-efficiency modulation of the SHG property (2.6 times that of KH2PO4) and a high phase transition temperature of 372 K. Notably, NMPTPC exhibits a remarkable temperature-dependent SHG behavior, with an impressive "ON/OFF" ratio of approximately 70, underscoring its significant potential as a high-efficient solid-state NLO switch. Based on in-depth crystal structure analysis and theoretical calculations, the modulation of the NLO property is attributed to the asymmetric distortion of the [PbCl6]4− octahedra coupled with π-conjugated aromatic amines with a large dipole moment. This research highlights a promising strategy for advancing the development of high-efficiency NLO switches and provides insights into their applications in next-generation intelligent optoelectronic devices.
Near-infrared (NIR) light offers significant advantages in photocatalytic reactions due to its excellent penetration ability and low phototoxicity. However, the development and utilization of NIR light for efficient photocatalysis continue to encounter several challenges. In this work, we designed and synthesized two stable iron-oxo clusters functionalized with 1, 1-ferrocene dicarboxylic acid (Fcdc), Fe11-Fcdc and BiFe10-Fcdc, both of which can effectively utilize full-spectrum light to realize efficient oxidative coupling reaction of benzylamine (BA) with a product of selectivity over 90% and a conversion up to 97%. Particularly, under the NIR light, Fe11-Fcdc shows significantly better photocatalytic performance (a conversion of 82.3%) than BiFe10-Fcdc (41.0%), which may be responsible for the stronger metal-ligand charge transfer effect in Fe11-Fcdc. This work reports for the first time the study of ferrocene-modified crystalline clusters achieving effective utilization of NIR light.
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