Advanced Energy Materials
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2025
·
IF 26
Zongge Li,Wenjun Kang,Jingkai Lin,Rui Li,Konggang Qu,Suyuan Zeng,Lei Wang,Fanpeng Meng,Huayang Zhang,Haibo Li
The oxygen electrocatalytic activity of transition metal catalysts can be tuned by tailoring their microstructure to optimize electronic configuration. Here, a one-step Coordination-Selective Synthesis strategy is developed to integrate Co single-atom sites and Fe-based nanoparticles within the same matrix, enabling long-range electronic interactions that enhance Co-N 4 reactivity and improve oxygen reduction reaction performance. X-ray absorption spectroscopy confirmed that remote Fe-based nanoparticles modulate the electron distribution at Co-N 4 sites. Structural characterizations reveal that the optimal catalyst, Co 50% Fe 50% -NC, contains metallic Fe, Fe 3 O 4 , and Fe 4 N species. Electrochemical measurements show that it achieves onset and half-wave potentials of 0.984 and 0.927 V versus RHE, surpassing Co 100% -NC with only Co-N 4 sites. Additionally, it demonstrates efficient oxygen evolution reaction performance, achieving an overpotential of 298 mV at 20 mA cm −2 , comparable to RuO 2 . Density functional theory calculations reveal that Fe 4 N optimizes O-containing intermediate adsorption/desorption, lowering the theoretical overpotential. Zn-air batteries assembled with Co 50% Fe 50% -NC exhibited superior performance to Pt/C, highlighting its potential for bifunctional oxygen electrocatalysis. This study provides an approach for designing high-performance catalysts by utilizing synergistic interactions between atomic and nanoscale metal species.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2025
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IF 6.3
Xingyu Zhong,Baoan Xu,Jianing Li,Weiyu Fang,Yuxuan Shen,Mei Bai,Xiulan Hu
High-efficiency oxygen reduction electrocatalysts is crucial for low-carbon development. Iron-nitrogen co-doped carbon materials (Fe-N-C) prepared from ZIF-8 are well recognized for their remarkable potential to enhance ORR reaction rates. However, the challenge of limited and singular active sites due to insufficient metal loading has impeded the progress of Fe-N-C-based materials. In this paper, the above-mentioned problems were alleviated by introducing a second transition metal (Co, Mn, Zr) to form a bimetallic catalyst with Fe. Carboxylates are also introduced for assistance to generate one-dimensionally entangled carbon nanotubes, then the material can perform charge transfer better. In the alkaline medium, the half-wave potential of FeCo-N-C-OAc synthesized with carboxylate added reached 0.907 V, FeMn-N-C-OAc was 0.893 V, and FeZr-N-C-OAc was 0.892 V, which was improved compared with the samples without carboxylate added. In the range of 100–1000 ppm oxygen concentration, the oxygen sensors based on three catalysts that with carboxylate added showed good linearity and high response currents, especially FeMn-N-C-OAc showed an average response time of 53 s and a relative current fluctuation of only 4 % after 28 days. When improving the performance of Fe-N-C-based catalysts used in coulometric electrolytic oxygen sensors, this work can be regarded as a new strategy.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2025
·
IF 8.3
Ruina Li,Xuwen Li,Qingcheng Liu,Hua Yue,Yang Meng,Yuanyuan Tian
With the continuous advancement of fuel cell technology, the exploration and development of highly efficient non - precious - metal catalysts for the oxygen reduction reaction (ORR) have emerged as a focal point of research. Fe–N–C catalysts have attracted much attention due to their excellent performance and low cost, and coupling single-atom catalysts (SACs) with atomic clusters (ACs) is an effective method to improve catalyst activity. This study used the pyrolysis method to synthesize iron atom catalysts (Fe–N–C SACs) and iron cluster coupled catalysts (Fe–N–C SACs/ACs) on ZIF-8 carbon support. It evaluated the catalyst performance through electrochemical testing. The experimental results showed that the introduction of Fe clusters improved the half-wave potential of the catalyst to 0.399 V, which represented an 8.2 % enhancement compared to the SAC catalyst and reached 87.1 % of that of the commercial Pt–C catalyst, and reduced the Tafel slope to 61.47 mV dec −1 , effectively improving the ORR activity of the catalyst. We constructed FeN 4 single atom catalyst models and FeN 4 /Fe 4 N 6 single atom cluster catalyst models using density functional theory (DFT), analyzed their electronic structures and reaction mechanisms, and revealed the mechanism of action of iron clusters. DFT calculations showed that iron clusters altered the charge distribution of FeN 4 sites, reducing the rate determining step (RDS) (OH desorption) energy to 0.5 eV, which promoted the desorption of products and the re-adsorption of reactants. As a result, the superior electrocatalytic performance of Fe–N–C SAC/AC is attributed to the synergistic effect between iron clusters and single atoms, which is influenced by the coordination environment and provides new ideas for designing efficient ORR catalysts.
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JOURNAL OF MAGNETISM AND MAGNETIC MATERIALS
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2025
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IF 3
Qi Li,Zhangqiao Zhou,Yan Nie,Lu Yang,Yu Wang,Jinsong Chen,Xian Wang
The preparation of soft magnetic composites requires effective surface modification of alloy powder to enhance insulating properties and achieve dense, uniform coating layers. Firstly, the gas-atomized Fe-Ni-Mo powder was surface modified using the atomic layer deposition method, forming a uniform and dense Al 2 O 3 insulating layer. The secondary surface modification of organic polymers further improves the properties of soft magnetic composites. This study systematically evaluates the effects of the primary and secondary surface modification on the properties of powder particles and soft magnetic composites. The primary modification generates an extremely thin insulating layer of approximately 2.5 nm, which increases the particle resistivity by 9 orders of magnitude. The permeability frequency stability of the soft magnetic composites increased from 11.3 % to 96.5 %, resulting in significant core loss reduction. The secondary modification effectively enhances the formability of soft magnetic composites. Optimal permeability of 242.7 at 1 kHz is achieved, maintaining 95.2 % frequency stability up to 1 MHz, while core loss remains below 570 mW cm −3 under 100 kHz/100 mT conditions. The surface treatment method in this work can provide a reference for the surface insulation modification of soft magnetic composites.
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Journal of Materials Chemistry B
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2025
·
IF 5.7
Jiale Zhang,Pengtao Chen,Jinlong Hu,Shuqing Wu,Yue Lin,Yao Lu,Junyu Xia,Jingcheng Wang,Jie Li,Yuan Liang
Implant-related infections (IRIs) pose a major challenge in orthopedic applications due to the persistence of biofilms, which are highly resistant to conventional antibiotics. This study introduces oxygen vacancy-engineered Zn–Fe spinel nanoparticles as microwave-responsive antibacterial agents. The oxygen vacancies in the spinel structure enhance reactive oxygen species (ROS) generation under microwave irradiation, providing a dual-mode antibacterial mechanism of thermal and oxidative stress. Zn–Fe spinel nanoparticles were synthesized using a sol–gel method and evaluated for their antibacterial efficacy against Staphylococcus aureus biofilms. Under microwave irradiation, the Zn–Fe spinel demonstrated significant biofilm disruption and bacterial eradication. Mechanistic studies revealed that oxygen vacancies promoted ROS generation, leading to bacterial membrane damage. In vivo experiments using a mouse infection model confirmed the material's antibacterial efficacy and biocompatibility, with no observed toxicity. This study highlights the potential of oxygen vacancy-enhanced Zn–Fe spinel as a microwave-assisted, antibiotic-free strategy for treating deep-seated infections associated with orthopedic implants.
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Surfaces
·
2025
·Vol. 8
·期 3
·60
·
IF 2.9
Yanying Zhu,Yanxiang Wang,Jianwei Zhang,Jinghe Guo,Yingfan Li,Siao Xin,Ziyi Xu,Yanru Yuan,Dong Zhang
Surface modification of carbon fibers (CFs) is a critical step in preparing carbon fiber-reinforced composites. This study developed a continuous experimental process that integrates electrochemical anodic oxidation and chemical vapor deposition to fabricate carbon nanotubes/carbon fiber (CNTs/CF) reinforcements. The effects of temperature and hydrogen flow rate during CNT growth on the resulting reinforcements were systematically investigated. The surface morphology and mechanical properties of the modified materials were characterized using scanning electron microscopy, Raman spectroscopy, and single-fiber tensile testing. Employing an Fe0.5Ni0.5bimetallic catalyst under optimized conditions (550 °C, H2flow rate: 0.45 mol/min, C2H2flow rate: 0.30 mol/min), the resulting reinforcement exhibited an 8.7% increase in tensile strength compared to as-received CF.
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JOURNAL OF WUHAN UNIVERSITY OF TECHNOLOGY-MATERIALS SCIENCE EDITION
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2025
·Vol. 40
·期 2
·382-388
·
IF 1.1
Cao Tian,Li Wei,Ren Lin,Song Tao,Song Jie,Lin Jiacheng,Yang Li,Liu Wenxiu,Wang Ping,Feng Shaojie
The adsorption of phosphate was conducted by the complex of chitosan/polyacrylamide/ferric(CS/PAM/Fe(III)) prepared. The SEM images and XPS spectra confirmed the successful adsorption of phosphate. The adsorption process was studied by varying the influencing aspects like pH, co-existing ions, contact time, and initial phosphate concentration. The experimental results indicate that the adsorptive capacity decreases with the increase of pH. However, it is commendable that there is still a adsorption capacity of more than 5 mg/g when the pH is 8–11. The adsorption kinetics can be accurately described by the pseudo-second-order model and is controlled by both chemisorption and surface diffusion. The adsorption process is a single layer adsorption. This paper proposed that the adsorption mechanism of CS/PAM/Fe(III) complex is the joint action of electrostatic attraction and ligand exchange.
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JOURNAL OF POLYMER SCIENCE
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2025
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IF 3.6
Yang Liu,Guodong Cao,Xuelong Zhu,Yi Zhang,Chenglu Liang,Yukun Chen
Upcycling the wasted polyamide 6 (PA6) to its monomer caprolactam via depolymerization is a promising way to build the resource cycling and alleviate the environmental pollution. High efficient catalyst for PA6 depolymerization is desirable and crucial. Herein, a sulfonated Fe-MOF catalyst was designed and performed as solid acid catalyst for the PA6 depolymerization for the first time. Results showed that a 100% conversion of PA6 solid to water-soluble liquid products can be achieved at temperatures of 250°C after only 1-h reaction. LC/MS results indicated that the water-soluble products were mainly composed of caprolactam and their oligomers. Without catalyst, nearly no water-soluble products can be obtained at the same condition. Moreover, a high selectivity of 90% caprolactam production in the water-soluble liquid products was achieved at 260°C, 5 h. The reaction rate constants at 240°C, 250°C, and 260°C were determined to be 0.024, 0.033, and 0.064, respectively, with a Ea value of 101.8 kJ/mol, showing positive temperature dependent relationship. The comparison of catalytic performances over sulfonated Fe-MOFs, FeCl 3 ·6H 2 O and the pristine un-sulfonated Fe-MOF suggested the synergistic contribution of Fe sites (Lewis acid centers) and the sulfonic acid sites to the catalytic performances. Graphical Water soluble liquid products (100 wt.%) with a high selectivity of 90% caprolactam can be achieved by the addition of Fe-MOF catalyst under a mild condition through the synergistic catalytic contribution of Fe sites (Lewis acid centers) and the sulfonic acid sites.
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Molecular Catalysis
·
2025
·
IF 4.9
Can Sun,Runze Guo,Zhexiao Zhu,Shouxin Zhu,Jingyi Qu,Zijie Fang,Xiaolu Xu,Jiahui Lin,Yangben Chen,Shijie Zhang,Hui Zheng
Photocatalytic nitrogen fixation as a green, environmentally friendly, mild and low energy-consuming nitrogen fixation is considered as an ideal way to produce ammonia. Herein, inspired by nitrogen-fixing enzymes, the MOF materials Fe-sdc and Ti-sdc were synthesized by a simple solvothermal synthesis method using Fe and Ti as metal nodes and 4,4′-stilbenedicarboxylic acid (H 2 sdc) as a ligand. The ammonia production rates of Fe-sdc and Ti-sdc were 61.01 μmol g −1 h −1 and 46.84 μmol g −1 h −1 . The 15 N 2 isotope experiments were utilized to determine the nitrogen source for ammonia synthesis during the nitrogen fixation process of Fe-sdc. Various characterization analyses were also utilized to analyze the reasons for the better nitrogen fixation performance of the two catalysts.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
·
IF 9.7
Runlai Liu,Qi Chen,Jinjing Qiu,Cheng Liu,Jionghua Wu,Jimmy C. Yu,Ling Wu
The construction of metal–organic frameworks that possesses the tunable metal active sites and synergistic effect for the reactant activation is an attractive strategy for the optimization of photocatalytic performance. Herein, a series of MIL-88A(Fe 1-x Cu x ) were synthesized for photocatalytic nitrogen reduction reaction (NRR). It was characterized that the Fe 2+ and oxygen vacancies were produced in MIL-88A(Fe) due to the partly reduction of ligand fumaric acid in synthesis process. The substitution of Fe 3+ with Cu 2+ induces charge imbalance and lattice distortion, further increasing the content of Fe 2+ and oxygen vacancies. The optimal sample MIL-88A(Fe 0.95 Cu 0.05 ) (CMA-5 %) exhibits the highest nitrogen fixation performance of 68.6 μmol·g −1 ·h −1 , which is 8 times higher than that of the pristine material. It is attributable to the synergistic effect of the abundant Fe 2+ and oxygen vacancies as active sites to promote N 2 coordination and photogenerated carrier separation, resulting in the efficient conversion of activated N 2 to NH 3 . Furthermore, the in-situ Diffuse Reflectance Infrared Fourier Transform Spectroscopy provide clear evidence of the behavior of the N 2 adsorption and activation on the catalyst. Finally, we propose a potential mechanism at molecular level regarding the relationship between the synergistic effect and the nitrogen fixation activity.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2019
·Vol. 26
·期 14
·14350-14361
·
IF 2.914
Wu Kang,Si Xiongyuan,Jiang Jin,Si Youbin,Sun Kai,Yousaf Amina
In this study, a novel Fe–Mn binary oxide (FMBO), which combined the oxidation capability of iron and manganese oxides, was constructed to remove sulfamethoxazole (SMX) effectively using the simultaneous co-precipitation and oxidation methods, and the reaction products were probed by liquid chromatography-mass spectrometry (LC/MS). Particularly, FMBO-mediated transformation mechanisms of SMX were explored using radical scavengers and electron paramagnetic resonance (EPR). Results indicated that the best removal efficiency was obtained at a pH of 4.0, with the H 2 O 2 of 6.0 mmol/L and the FMBO dosage of 2.0 g/L, giving 97.6% removal of 10 mg/L SMX within 60 min. More importantly, we found that the hydroxyl (•OH) radicals generated by FMBO through Fenton-like reaction were responsible for the SMX oxidation. EPR studies were confirmed that the peak intensities of hydroxyl adduct decreased remarkably with increasing pH values. Moreover, the four SMX degradation intermediate products were detected by LC/MS and a reaction pathway for the possible mineralization of SMX, with •OH radicals as the main oxidant, was proposed. These findings provide a novel insight into the removal of SMX by FMBO-mediated radical reactions in aquatic environments. Moreover, this research suggested that FMBO can act as an efficient catalyst to remove SMX in hospital wastewater.
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ACS Nano
·
2025
·
IF 16
Ruonan Li,Runlin Ma,Li-Li Zhang,Wei Ma,Gonglei Shao,Xu Zhang,Yun Tian,Menggai Jiao,Zhen Zhou
To tackle the challenge in electrochemical nitrogen fixing and reduction in aqueous electrolytes, the conventional approach has been to suppress the competitive hydrogen evolution reaction. Nonetheless, proton provision is a crucial step in the nitrogen reduction pathway to produce ammonia, and a single active site faces the daunting task in striking a balance between high nitrogen fixation efficiency and fast protonation kinetics. This work presents a harmonic strategy featuring atomically dispersed dual Fe–Mo sites anchored in an N-doped carbon (FeMoNC) substrate, where a low-spin Fe center with enriched empty d orbitals aids in nitrogen fixation and activation, and the adjacent Mo site accelerates the protonation kinetics of N-containing intermediates at the Fe site via a distal associative mechanism. Driven by this co-catalytic mechanism, the FeMoNC catalyst achieves a Faradaic efficiency of 37.42%, marking a significant improvement of 7.8- and 10.6-fold over Fe or Mo single-atom catalysts, respectively. Furthermore, an excellent NH3 yield of 54.40 μg h–1 mgcat.–1 is realized in a flow cell by enhancing mass transfer. This study provides valuable insights into diatomic co-catalytic mechanisms for electrochemical ammonia synthesis.
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