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Heterogeneous catalysis triggered in the novel copper-palladium spinel oxides through electron delocalization and oxygen vacancies for efficient degradation of organic contaminants

Yanbin Wang,Liling Wang

In Fenton-like reactions, enhancing the activation efficiency of peroxymonosulfate (PMS) is a critical factor for generating diverse reactive oxygen species, but improving PMS adsorption capacity and accelerating electron transfer remain major challenges to boost reaction kinetics. This study designed and synthesized a novel copper-palladium (Cu-Pd) bimetallic spinel oxide, where Pd doping into spinel-structured and layered copper oxides effectively generated a substantial number of oxygen vacancies and precisely regulated the electronic structure–two core factors that dominate PMS activation efficiency. A key finding of this work is that electron delocalization at highly active Cu-Pd sites, coupled with abundant oxygen vacancies, enables rapid PMS activation and significantly promotes the cycling efficiency of Pd 2+ /Pd 0 and Cu 2+ /Cu +  at the catalyst interface. In the Cu 2 PdO 3 /PMS system, the degradation efficiency of bisphenol A (BPA) reached 100% within 5 min, with a corresponding rate constant of 0.501 s −1 , which was 11.65 and 22.77 times higher than those of pure Pd oxide and Cu oxide, respectively. The integration of experimental characterization with density functional theory (DFT) calculations reveals that oxygen vacancies and electron transfer are the primary catalytic mechanisms: the pronounced electron delocalization at Cu/Pd sites facilitates the adsorption of ∗HSO 5 /∗OH intermediates on the “metal-Vo bridge” structure. This study provides a representative case and for spinel oxides-based PMS activation, offers novel insights into the regulatory roles of oxygen vacancies and electron delocalization, and lays critical references for the development of advanced environmental remediation catalysts.

Nucleotide coordinated polymer nanoparticle-based hydrogel sensing platform for visual detection of organophosphorus and carbamate pesticides

Yahui Guo,Yu Wang,Feifei Wang,Zongcheng Zhang,Gairu Li,Chuanxia Chen,Zongjun Li,Jian Sun

Rapid and reliable on-site detection of pesticide residues is crucial for safeguarding public health and environmental safety. This study developed a rapid detection method for pesticide residues based on iron-guanosine monophosphate coordination polymer nanoparticles (Fe-GMP CPNs). Fe-GMP CPNs possess peroxidase-like activity and can catalyze the H 2 O 2 -3,3′,5,5′-tetramethylbenzidine (TMB) colorimetric reaction. By integrating acetylcholinesterase (AChE), a colorimetric detection platform was constructed: in the absence of pesticides, AChE hydrolyzes acetylthiocholine (ATCh) to produce thiocholine (TCh), TCh inhibits the color development; in the presence of pesticides, the inactivation of AChE restores the blue color, enabling the visual detection of organophosphorus and carbamate pesticides. To further achieve on-site analysis, the detection reagents were encapsulated in agarose hydrogels and combined with smartphone colorimetric technology to realize on-site rapid detection of carbaryl and trichlorfon. This research promotes the development of nanozyme sensing technology and provides a new approach for the next generation of food safety detection.

Electron transport channel-mediated Z-type α-MnO2/Cd1.7In2S4.7 heterojunction for photocatalytic conversion of 5-hydroxymethylfurfural to 2,5-dicarbonylfuran

Liang Yuwei,Huang Yufan,Hu Chunling,Cai Jinyu,Cao Yifan,Meng Guihua,Wu Jianning,Li Qi,Liu Zhiyong

Designing catalysts with suitable valence conduction band positions to generate reactive oxygen species (ROS) with moderate redox capacity is to achieve efficient photocatalytic biomass-selective value-added oxidation. This protocol addresses the issue by tuning material structural defects, altering the surface electronic structure, and ultimately enhancing the raw material’s performance. Here, an appropriate amount of one - dimensional nanorods α -MnO 2 adjusted material structural defects, increased the adsorbed oxygen (O ads )/lattice oxygen (O latt ) and Mn 3+ ratios, and served as an electron transport conduit, facilitating O₂ activation to generate ROS. The Cd 1.7 In 2 S 4.7 solid solution enables the optimal valence band position by adjusting the Cd 2+ : In 3+ ratio, thus selectively oxidizing 5-hydroxymethylfurfural (HMF) to 2,5-dicarbonylfuran (DFF). In situ XPS revealed that photogenerated electrons in Cd 1.7 In 2 S 4.7 quickly transferred to the conduction band of α -MnO 2 , and photogenerated holes from α -MnO 2 moved to the valence band of Cd 1.7 In 2 S 4.7 . This significantly enhanced the separation and transfer efficiency of photogenerated carriers at the interface. The optimal sample achieved 56% conversion of HMF and 72% selectivity of DFF under simulated sunlight. This protocol provides a new approach for the establishment of electron transport channel structures based on α -MnO 2 constructs and value-added biomass photocatalytic conversion under simulated sunlight.

Polymer-Zn(II) sunscreens for protection against harmful blue ray

Rui Yuan,Sa Du,Jieyao Cheng,Zeyu Ma,Ruoxi Wang,Xiue Yan,Yonghui Huang,Yuwei Wu,Lei Tao

Harmful blue rays (HBRs, 400-450 nm) originating from the sun and numerous electronic devices are similar to ultraviolet rays (UVRs) and can induce skin photoaging. Ordinary sunscreens exhibit poor HBR-blocking capability, and traditional anti-HBR materials are unsuitable for skin protection. Herein, we develop a polymer-metal complex that can be applied to the skin to effectively block HBRs. Hydroxyquinoline is introduced into the polymer backbone via the Biginelli reaction. This polymer (P) exhibits strong coordination with Zn(II). The resulting P-Zn(II) complex undergoes a spectral redshift through metal-ligand orbital transitions, enabling effective shielding of both UVRs and HBRs. The P-Zn(II) complex protects fibroblasts from HBR-induced cell death, oxidative stress, and cellular aging by preventing HBR-triggered dysregulation of multiple photoaging-related signaling pathways and genes. In mouse experiments, the P-Zn(II) complex exhibits minimal skin irritation and low hepatic and renal toxicity. It can be applied to the skin in a manner similar to sunscreens and effectively prevents HBR-induced skin damage, which fills the gap in HBR protection left by current commercial products. This study highlights the potential of polymer-metal ion complexes as advanced photoprotective materials and provides valuable insights into the development of anti-HBR biomaterials.

Preparation of Oxygen-Doped Amorphous MoS2 and Its Electrocatalytic Performance for Nitrogen Reduction to Ammonia

The electrocatalytic nitrogen reduction reaction (NRR) is a key approach for synthesizing green ammonia under mild conditions. However, the high bond energy of the N≡N triple bond makes N2difficult to activate, limiting the Faradaic efficiency. MoS2offers advantages such as low cost and abundant reserves as a non-precious-metal NRR electrocatalyst. Nevertheless, pure MoS2suffers from insufficient conductivity and a limited number of active sites, resulting in suboptimal catalytic performance. Herein, we develop a solvent-regulated one-step hydrothermal strategy using ethylene glycol as the sole reaction medium to fabricate an oxygen-substituted amorphous MoS2(O-MoS2) electrocatalyst. XRD, SEM, and HRTEM characterization revealed that, as the ethylene glycol ratio increased, the product gradually transformed from a layered crystalline structure to a completely amorphous structure. XPS confirmed that oxygen atoms were uniformly incorporated into the MoS2lattice via substitution doping. Electrochemical testing showed that O-MoS2achieved an ammonia yield of 97.16 μg h−1mg−1and a Faradaic efficiency of 46.44% in a 0.1 M Na2SO4electrolyte at −0.70 V vs. RHE, significantly outperforming undoped MoS2and semi-doped S-MoS2. DFT calculations indicate that O doping reduces the N2adsorption energy, thereby synergistically promoting N2adsorption and activation. This dual-modification strategy provides a facile and universal guidance for electronic structure regulation of MoS2-based catalysts and sheds new light on the design of high-efficiency ambient nitrogen fixation electrocatalysts toward practical green ammonia synthesis.

NiFe-LDH/ZnCdS bimetallic hydroxide heterostructures for efficient multi-electron CO2 reduction

Jie Liu,Kaiyu Li,Shizhen Gao,Guohua Wu,Jing Fan

Efficient photocatalytic CO 2 reduction is limited by rapid carrier recombination and sluggish interfacial kinetics. Here, NiFe-LDH/ZnCdS (ZCS) heterostructures were fabricated by hydrothermal synthesis followed by electrostatic self-assembly. Mott–Schottky analysis, XPS, photoelectrochemical measurements, and density functional theory calculations collectively reveal staggered band alignment and interfacial charge redistribution, supporting a type-II charge-transfer pathway with improved carrier separation. The optimized 15NiFe-LDH/ZCS produced CO, CH 4 , C 2 H 4 , and C 2 H 6 at 16.54, 8.30, 1.22, and 4.70 μmol g −1 h −1 , respectively, while maintaining stable activity over 16 h. The enhancement originates from intimate interfacial contact, stronger visible-light harvesting, faster charge transport, and increased accessible active sites. These results establish a practical heterostructure-design strategy for multi-electron photocatalytic CO 2 conversion.

Shallow-Trap Relay and Type-II Band Alignment Synergy in Vs-ZnS/In2S3 for Accelerated Photoelectrochemical Water Splittin

Hao Yan,Zhou Li,Wang Chengyi,Ruan Mengnan,Liu Zhifeng

In conventional photoelectrochemical (PEC) water-splitting systems, the high recombination rate of photogenerated charge carriers and sluggish interfacial charge transfer kinetics serve as the core bottlenecks restricting energy conversion efficiency. In this study, a sulfur-vacancy-engineered Vs-ZnS/In 2 S 3 heterojunction was constructed to demonstrate the “electron relay” function of sulfur vacancies within a Type-II heterojunction. Specifically, sulfur vacancies create a localized shallow trap level below the conduction band of In 2 S 3 , amplifying the potential driving force for interfacial electron transfer. Concurrently, these defect states effectively capture photogenerated electrons transitioning across the interface and serve as highly active sites directly participating in surface reactions, thereby significantly suppressing both the bulk and surface recombination of charge carriers. Benefiting from this synergistic mechanism, the as-prepared Vs-ZnS/In 2 S 3 photoelectrode exhibits exceptional PEC performance, achieving a maximum photocurrent density of 1.26 mA·cm –2 and an applied bias photon-to-current efficiency of approximately 0.26%. This is substantially superior to pristine ZnS and conventional ZnS/In 2 S 3 electrodes. Kinetic and separation efficiency characterizations indicate that the bulk and surface charge separation efficiencies are drastically improved to 68.4% and 38.1%, respectively. This exceptional performance stems from the synergistic interplay between the heterojunction and the sulfur vacancies: the localized electronic structure modulated by defect states facilitates the directional transfer of interfacial electrons and accelerates the hydrogen evolution reaction kinetics. This work provides a novel design paradigm for regulating charge transport pathways within heterojunctions via defect engineering to realize highly efficient energy conversion.

Breaking the barrier of Algal resistance: FeMoS₂/g-C₃N₄/Vis system for enhanced peroxydisulfate activation and Chlorella vulgaris inactivation

Lei Hu,Yuxuan Tian,Ning Ding,Hong Liu

In this study, iron-doped molybdenum disulfide (FeMoS 2 ) was hydrothermally synthesized and subsequently coupled with calcined graphitic carbon nitride (g-C 3 N 4 ) to construct a heterojunction . Comprehensive characterization confirmed the stable crystalline structure of the composites and the formation of robust interfacial coupling, which facilitated efficient photogenerated charge separation. Furthermore, UV-Vis diffuse reflectance spectroscopy revealed a significant extension of the visible-light absorption edge compared to pristine FeMoS 2 , with the bandgap narrowing to 1.99 eV. Under optimized conditions (0.6 g/L catalyst dosage, 1.0 mM peroxydisulfate (PDS), pH 6), the FeMoS 2 /g-C 3 N 4 /PDS system achieved 88 % Chlorella vulgaris inactivation in 60 min under visible light, retaining more than 60 % efficiency after five cycles. Mechanistic investigations revealed that superoxide radicals (·O 2 - ) and photogenerated holes (h + ) synergistically inactivated Chlorella via reactive oxygen species (ROS)-induced membrane peroxidation and antioxidant system disruption. Algal physiological assays and microscopic imaging further corroborated that photocatalytically generated ROS compromised cellular membrane integrity and induced chloroplast degradation.

Supramolecular Interaction-Mediated Diffusion Enhancement for Facilitated Synthesis of the Pharmaceutically Active Ingredient Dantrolene and Its Analogues via Spiral Gas–Solid Two-Phase Flow

Yong Song,Jinsong Li,Shikang Liu,Bo Jin,Rufang Peng

Although mechanochemical synthesis has gained widespread application, our understanding and enhancement of the control of the reaction need to be improved. In this work, we confirm that the mechanochemical reaction of the active pharmaceutical ingredient dantrolene is controlled by diffusion-controlled kinetics. On this basis, we demonstrate a novel approach to modulate mechanochemical reactivity through a diffusion enhancement strategy mediated by supramolecular interactions. The method employs a highly efficient spiral gas–solid two-phase flow technique, in which urea, an additive that can establish supramolecular interactions with 1-aminohydantoin hydrochloride, is introduced into the reaction system to substantially enhance diffusion, thus facilitating the efficient synthesis of dantrolene. Notably, in this diffusion enhancement process, the weakening of mechanical forces triggers the nucleation and growth of the active substrate to form structurally well-defined eutectic crystals that inhibit the reaction. This strategy reduces the mechanochemical reaction time of dantrolene and its analogs to less than 30 s. In addition, thiourea and acetamide, which are structurally similar to urea, promote the reaction, and their effects correlate with the number of supramolecular sites of action.

Electrospinning Construction of 3D Networked CuS/Fe3O4/C Nanocomposites for Broadband Microwave Absorption

Juan Ding,Ligang Cheng,Na Zhang,Jiale Sun,Jin Gao,Mengkang Bi

The development of electromagnetic microwave (EMW) absorbers featuring broad bandwidth, low cost, and engineering feasibility is considered strategically important to address the application demands of 5G/6G communications and stealth technologies. In this study, the CuS/Fe3O4/C nanocomposites with enhanced absorption properties were synthesized through the incorporation of CuS into a polyacrylonitrile (PAN) precursor using electrospinning technology. The obtained composites demonstrate an ultrawide effective absorption bandwidth (EAB) in the X and Ku bands, achieving a minimum reflection loss (RLmin) of −50.37 dB at 15.44 GHz with a thickness of 1.9 mm, along with an EAB of 4.8 GHz (RL ≤ −10 dB, 13.2–18 GHz). For the CuS/Fe3O4/C nanocomposites with 10% CuS loading, optimal EMW absorption performance was observed at 3.5 mm, exhibiting an RLmin of −40.09 dB at 6.96 GHz and an ultrawide EAB covering 9.6 GHz (RL ≤ −10 dB, 8.4–18 GHz). Based on Cole–Cole curve analysis, the nanocomposite with 20% CuS loading is characterized by five distinct and well-defined relaxation arcs, confirming its remarkable dielectric loss capability. Furthermore, CST simulation results indicate that the radar cross-section (RCS) values of compressed samples were significantly reduced, which is attributed to improved magnetic absorption. These findings substantiate that the superior EMW absorption performance of the nanocomposites stems from a strong polarization loss mechanism and considerable eddy current loss. This study underscores the significant potential of the CuS/Fe3O4/C nanocomposites in ultrabroadband EMW absorption research and offers valuable guidance for further in this area.

Preparation of g-C3N4-based photocatalytic nanofibers and antibiotic degradation performance research

Yanjin Wang,Zhuo Zhang,Lin Shi,Lidong Kou,Yasong Li

With the extensive use of antibiotics around the world, their contamination problem has now attracted increasing attention, and seeking effective antibiotic contamination management technologies has been imminent. Visible light photocatalytic technology, as an emerging green technology with low cost, high efficiency and good application prospect, has become a research focus both at home and abroad. In this paper, graphitic phase carbon nitride (g-C 3 N 4 ) was used as a photocatalytic material, and the composite photocatalysts g-C 3 N 4 /MoS 2 , g-C 3 N 4 /CuS, g-C 3 N 4 /CdS were produced by compounding it with a series of metal sulfides, and the physical and chemical properties of the composite photocatalysts were characterized by means of SEM, TEM, BET, XRD, XPS, FT-IR, and UV-VIS-NIR. The results show that the prepared composite photocatalytic materials do not change the morphological structure of g-C 3 N 4 , and the introduction of metal sulfides can effectively enhance the light absorption performance and photocatalytic activity of the composites. The best removal of typical antibiotic sulfadimethylpyrimidine (SMT) in water was achieved by g-C 3 N 4 /CdS, with the most stable photocatalytic performance, and the complete removal of SMT could be achieved after 6 h of photocatalysis under LED illumination conditions at wavelengths of 420 nm and 365 nm. g-C 3 N 4 /CdS had the highest photocatalytic activity at pH = 3. Optimal g-C 3 N 4 /CdS was used to prepare flexible polyacrylonitrile carrying carbon nitride nanofiber photocatalysts (PAN/g-C 3 N 4 /CdS) by electrostatic spinning method, which had excellent light absorption properties in UV and visible light regions. SMT removal of PAN/g-C 3 N 4 /CdS reached 100.00% after the light was turned on for 6 h at a wavelength of 365 nm, indicating that the nanofiber photocatalytic materials prepared in this study have excellent photocatalytic activity and antibiotic degradation performance. This paper has important theoretical and practical significance for solving the problem of antibiotic pollution in water bodies.

Atomic-shell engineering in manganese-doped palladium@iridium nanozymes: d-Band optimization for enhanced peroxidase-like activity in ultrasensitive lateral flow immunoassays

Ting Tan,Qianqian Cao,Ming-Hui Duan,Junmin Li,Yafeng Xie,Min Tan,Xiwu Yin,JiKai Wang,Weiguo Wang

Lateral flow immunoassay (LFIA) has been widely used in clinical diagnosis, food safety, and environmental protection due to the simple operation and high detection efficiency. However, the sensitivity of LFIA still falls short of the requirements when dealing with low levels of biomarkers. In this work, a type of manganese-doped core-shell nanozyme (Pd@Ir-Mn) with an ultrathin iridium (Ir) shell (~2 nm) was synthesized and utilized for the signal amplification of LFIA. By doping with other metals (Mn, Fe, Co, Ni, Cu, and Zn), the d-band center of Ir was tuned. The relationship between the d-band center and the conversion coefficient followed a volcano plot, with Mn-doped Pd@Ir located at the peak of the volcano. The as-prepared Pd@Ir-Mn was finally applied to LFIA (HT-Pd@Ir-Mn-LFIA) for the detection of hCG, the sensitivity was improved by 41 times compared to the traditional gold nanoparticles based LFIA (AuNPs-LFIA). Moreover, this method exhibited good specificity, stability, precision, and accuracy, making it suitable for clinical detection.