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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Catalysts
·
2025
·Vol. 15
·期 12
·1105
·
IF 4
Xin Wang,Longxue Yu,Shuo Wang,Lingyun Xue,Yi Liu,Zhuhui Qiao,Xunyong Liu
Tetracycline (TC) is chemically stable and recalcitrant to natural degradation. Peroxymonosulfate (PMS)-based advanced oxidation processes offer an effective removal strategy, the efficacy of which relies on high-performance heterogeneous catalysts. Titanium dioxide (TiO2) is an ideal material due to its stability and environmental compatibility, yet its practical application is hindered by inadequate PMS activation capacity, particle agglomeration, and difficult recovery. To address these limitations, a heterogeneous Fe/TiO2catalyst was constructed via Fe3+doping, innovatively utilizing polyvinylpyrrolidone (PVP) as a structure-directing agent. PVP’s steric hindrance effectively suppressed nanoparticle agglomeration and enabled high dispersion of Fe active sites, simultaneously enhancing catalytic activity and stability. Under optimized conditions, the Fe/TiO2/PMS system achieved 94.3% TC degradation, following pseudo-first-order kinetics and significantly outperforming pure TiO2used in this experimental system. Radical quenching verified sulfate radicals (SO4•−) as the dominant species. The catalyst demonstrated excellent recyclability, retaining over 80% degradation efficiency after six cycles and enabling convenient magnetic separation. Moreover, in complex water matrices (tap water and seawater), it sustained high removal efficiency (>90% initially, >70% after six cycles), highlighting its superior anti-interference capability and practical potential. This work offers a strategic material design strategy for efficient and robust TC removal in challenging water environments.
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Journal of Energy Storage
·
2025
·
IF 9.8
Chenglin Wei,Mengdi Sun,Baoguo Zhang,Zhangyong Yan,Zihao Dang,Yongkang Xu,Lin Wu,Ya Hu
Benefiting from the low cost and natural abundance of sulfur, as well as its excellent theoretical performance metrics - including a capacity of 1675 mAh g −1 and an energy density of 2600 Wh kg −1 - lithium-sulfur (Li-S) batteries have attracted considerable attention for next-generation energy storage. However, their practical deployment is severely hindered by the intrinsic shuttle effect of lithium polysulfides (LiPSs), which leads to the loss of active materials and poor cycling stability. In this work, we report a facile hydrothermal-calcination strategy to synthesize porous nanosheet-structured Fe-doped nickel oxide (Fe-NiO) as a functional separator modifier for Li-S batteries. The polar nature of NiO enables strong chemical interactions with LiPSs, effectively anchoring polysulfides on the cathode side and suppressing the shuttle effect. Furthermore, Fe doping significantly increases the density of surface active sites, thereby enhancing the adsorption and catalytic conversion of LiPSs into insoluble Li 2 S 2 /Li 2 S species, which promotes redox kinetics and mitigates capacity fading. When applied to Li-S cells, the Fe-NiO-modified separator markedly improves the electrochemical performance, delivering a high reversible capacity of 1150 mAh g −1 at 0.2C, an excellent rate capability of 505 mAh g −1 at 5C, and outstanding long-term stability with a minimal capacity decay of 0.091 % per cycle over 500 cycles at 1C. This study presents a simple and scalable strategy for separator engineering, providing a promising pathway toward high-performance Li-S batteries.
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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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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
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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APPLIED PHYSICS A-MATERIALS SCIENCE & PROCESSING
·
2025
·Vol. 131
·期 3
·196
·
IF 2.8
Zhao Xinyue,Zhang Xijun,Gao Chenyu,Wang Peng,He Yan,Chu Dianming,Bai Wenjuan
Carbon nanotubes (CNT) have attracted much attention due to their wide range of applications, but the complex and time-consuming preparation of CNT by the traditional chemical vapor deposition (CVD) method has limited their large-scale production. In this study, we propose an innovative “one-step” CNT growth process to simplify catalyst preparation. The significant advantage of this method is that it reduces the time consumption by 90% compared with other catalyst preparation methods. Aluminum foil was found to outperform other materials as a substrate and catalyst loading significantly affected the morphology and quality of CNT. High-density, low-defect, high-crystallinity, and high-quality CNT could be grown on aluminum foil at the optimal loading (e.g., 0.10 mol/L.) In addition, the growth of CNT is affected synergistically by catalyst-substrate interfacial interactions, temperature, and aqueous solution content. In particular, CNT arrays with a diameter of 20 nm were successfully prepared on an iron catalyst calcined at 660 °C. These findings are important for large-scale, low-cost production of high-quality CNT.
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Materials Today Bio
·
2025
·
IF 10.2
Hongping Wan,Zhengqun Huang,Mingrun Tang,Huirong Tan,Kai Deng,Yingnan Liu,Xinghong Zhao,Hongjun Chen
Enveloped viruses such as coronaviruses are highly transmissible, necessitating effective prevention and inactivation strategies. In this study, we engineered uniform, small-sized (∼57 nm) iron-phenolic nano-networks (NA-Fe) that exhibit high lipoxidase-like activity for the inactivation of enveloped virus, encompassing both DNA virus (Pseudorabies, PRV) and RNA virus (Transmissible Gastroenteritis, TGEV; and Porcine epidemic diarrhea virus, PEDV). Theoretical studies indicate that NA-Fe facilitates the adsorption of pentadiene moieties within the viral envelope through interactions between the d -orbital electrons of iron and the π-electrons of pentadiene. This interaction leads to activation of the C=C bonds, potentially resulting in disruption of the viral envelope. Besides its extracellular antiviral effects, NA-Fe also suppresses intracellular viral replication by stimulating antiviral innate immune responses, and upregulate the expression of interferon-stimulating genes (ISGs). In vivo studies demonstrate that NA-Fe exhibits favorable biosafety, and intranasal administration significantly reduces viral titers while providing effective antiviral protection in PRV-infected mice. Notably, surfaces coated with NA-Fe, such as fences and air purifiers in farm facilities, provide effective antiviral protection. Collectively, these findings demonstrate that NA-Fe exhibits potent broad-spectrum antiviral activity against both extracellular and intracellular viruses, highlighting its potential for application in comprehensive biosecurity and infectious disease control.
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LANGMUIR
·
2025
·
IF 3.9
Yingjin Ma,Qifeng Li,Xueqing Qiu,Zhixian Li
Single-atom nanozymes can accurately mimic the catalytic centers of enzymes at the atomic scale, showing high catalytic efficiency and selectivity. Inspired by the active center of natural laccase, we constructed a nitrogen-doped carbon-based single-atom nanozyme (Fe-NC) featuring planar Fe–N4 active sites using a zeolitic imidazolate framework (Fe/ZIF-8) as a precursor. The resulting Fe–NC showed high laccase-like activity toward phenolic substrates such as 2,4-dichlorophenol, with a catalytic efficiency 77 times higher than that of natural laccase. Furthermore, Fe–NC efficiently catalyzed the degradation of tetracycline hydrochloride (77.14%) under mild conditions, with an activity 13 times that of laccase. It also selectively and oxidatively depolymerized birch lignin into valuable aromatic monomers, including vanillin and vanillic acid. These findings highlight the key role of planar Fe–N4 coordination in improving bioinspired catalysis and reveal the great potential of single-atom nanozymes in biomass valorization.
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JOURNAL OF SOLID STATE CHEMISTRY
·
2021
·
IF 3.498
Li Zeng,Tongjiang Peng,Hongjuan Sun,Jingjie Yang,Yao Li,Yating Qin
A series of Fe-doped LaNi 1-x Fe x O 3 perovskite oxide photocatalytic materials was prepared using a sol-gel method. The phase composition and morphology of LaNi 1-x Fe x O 3 samples were characterized via X-ray diffraction, scanning electron microscopy, transmission electron microscopy , X-ray photoelectron spectroscopy, and other analytical methods. The photocatalytic performance of the samples was tested by assessing the degradation rate of methyl orange. According to the results, Fe-doping caused the lattice distortion of the initially cubic of LaNiO 3 to a rhombohedral crystal system . In turn, partial substitution of Ni with Fe was found to increase the amount of oxygen vacancies , resulting in the higher mobility of lattice oxygen and thus improving the photocatalytic activity . The best photocatalytic performance was found in a LaNi 0.95 Fe 0.05 O 3 sample with a 5% Fe dopant concentration. Furthermore, the degradation rate of methyl orange in LaNi 0.95 Fe 0.05 O 3 within 120 min of visible light irradiation was as high as 98.89%, and its good degradation effect even with respect to other organic dyes such as methylene blue and rhodamine B. Finally, LaNi 0.95 Fe 0.05 O 3 was shown to maintain high photocatalytic activity and excellent recyclability even after numerous operation cycles.
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Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Zhenxing Liu,Zhan Hu,Faxiong Li,Xinting Lai,Yuan Zhou,Jiaqi Song,Zhihui Yang,Cong Peng,Fenghua Ding,Junfang Nan,Yexin Zhang,Yanjie Liang
Icosahedral boron arsenide B 12 As 2 is a self-healing semiconductor potentially applied in harshly irradiated environments. However, doping effects were rarely investigated to expand their applications. Hereby, a low-cost mechanochemical strategy is proposed to synthesize B 12 As 2 nanocrystals with a boron transformation rate of ∼70%. Nano-B 12 As 2 of 40–50 nm could be self-doped with Fe element and purified by aqua regia. Fe accounts from ∼0.00–1.77 at% with rotational speeds. Based on nano-size effects and Fe-doping effects, the photoluminescence process shows an indirect band-gap at E g = 2.81 eV and the presence of impurity energy level at E′= 2.11 eV. The optical absorption is red-shifted from the reported UV region to the visible region. The multiply increased photocatalytic hydrogen production (249 μmol∙h −1 ∙g −1 vs. 92.2 μmol∙h −1 ∙g −1 ) and photocurrent density (∼6 times) indicate that Fe-doping enhances the photo-excitement and the separation of the photoinduced carrier. First-principles calculations reveal a robust B 12 As 2 structure doped by Fe, bonding to icosahedral B 12 clusters and its nearest As via the Fe(III) style. Doped-Fe alters HOMO and LUMO orbital components, reduces the optical band-gap and becomes the activated carrier-separation center. Overall, a novel synthetic method and mechanism of Fe-doping are revealed that would facilitate optical applications of B 12 As 2 crystals under extreme conditions.
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CERAMICS INTERNATIONAL
·
2018
·
IF 3.057
Jiangbo Shi,Guiqiu Chen,Guangming Zeng,Anwei Chen,Kai He,Zhenzhen Huang,Liang Hu,Jingwen Zeng,Jing Wu,Weiwei Liu
In this study, graphene wrapped Fe-doped TiO 2 (G-TiO 2 -Fe) spheres were prepared through a simple hydrothermal process. The structural, optical and photocatalytic properties of synthesized composite were characterized by field emission scanning electron microscope (FE-SEM), X-ray diffraction ( XRD), Raman Microprobe (Raman), X-ray photoelectron spectroscopy (XPS) and UV–Vis diffuse reflectance spectrophotometer (DRS). The G-TiO 2 -Fe composite showed a significant red-shift in light response edge as compared with TiO 2 . Meanwhile, the band gap exhibited an obvious decline from 3.24 to 2.99 eV. The photocatalytic capacity of G-TiO 2 -Fe was further evaluated by methylene blue (MB) degradation experiments, and the results indicated that the optimized G-TiO 2 -Fe exhibited a remarkable increase in photocatalytic activity. The superior photocatalytic performance of the novel material could be ascribed to the synthetic effects of doped Fe and wrapped graphene shells. The unique geometrical configuration and constructive component which modified the TiO 2 electronic structure will largely improve the electron transporting efficiency and restrain the electron-hole recombination.
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Nanoscale Advances
·
2022
·Vol. 4
·期 9
·2171-2179
·
IF 5.598
Dawei Xu,Xuhui Li,Tingting Zheng,Ruixue Zhao,Pengyu Zhang,Kai Li,Zhongfeng Li,Lirong Zheng,Xia Zuo
Here, a series of Fe/N/C catalysts with different proportions and pyrolysis temperatures are prepared by co-pyrolysis of melamine with a γ-cyclodextrin metal–organic framework (γ-CD-MOF) containing iron(II) phthalocyanine (FePc). Due to the restriction effect of the host and guest at the molecular level, γ-CD-MOF can effectively avoid the π–π stacking of FePc and restrain the agglomeration of Fe atoms during pyrolysis. The phases and structures of the catalysts are characterized, which proves that the obtained catalyst has a three-dimensional porous and internal cavity structure with abundant surface area (1055.317 m2 g−1) and Fe is atomically dispersed in nitrogen-doped carbon. The onset potential (0.988 V vs. RHE) and half-wave potential (0.846 V vs. RHE) of FePc@CD/M (1 : 20)-1000 are superior to those of a commercial 20% Pt/C catalyst. FePc@CD/M (1 : 20)-1000 also exhibits an approximately four-electron (3.84) transfer process, good stability and excellent methanol tolerance.
研究领域:
材料科学
·
催化化学
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