APPLIED SURFACE SCIENCE
·
2025
·
IF 6.9
Jieling Liu,Changjin Mo,Yutong Wu,Jihui He,Xian Wang,Tao Wang,Rongzhou Gong,Yan Nie
Low-dimensional hybrid carbon networks with high electrical conductivity and low density are essential for designing lightweight and efficient microwave absorbing materials (MAMs). In this study, low-dimensional hybrid carbon networks with tailorable electromagnetic properties were successfully fabricated by a one-step method. These networks consist of (i) magnetic Fe nanoparticle-embedded, two-dimensional (2D) carbon lamellar structure and (ii) intertwined one-dimensional (1D) carbon nanotubes grown on the structure. These 1D-2D hybrid networks exhibit excellent electron transport, enhanced interfacial polarization, multiple loss mechanisms, and improved impedance matching. Consequently, they significantly boost MAM performance. With a 30 wt% absorbent filling fraction, the material achieves a reflection loss of less than − 10 dB across a frequency range of 5.0 GHz in the Ku band, with a matching thickness of only 1.67 mm. By tuning absorber thickness from 1.0 to 5.0 mm, the effective absorption bandwidth can reach up to 14.3 GHz, covering 89 % of the frequency range measured, and achieving a bandwidth of 10.0 GHz with 99 % absorption intensity. These results underscore a simple and effective strategy to construct low-dimensional hybrid carbon networks having tunable electromagnetic properties, that offers a promising pathway for the design of lightweight, broadband and efficient MAMs.
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ENVIRONMENT INTERNATIONAL
·
2025
·
IF 9.7
Jiaqi Shi,Yan Li,Qi Wei,Xin Zhu,Shaohua Cao,Wenyi Xie,Yang Guo,Jing Wei,Zekai Li,Tao Long
The widely used rubber antioxidant N-(1,3-Dimethylbutyl)-N’-phenyl-p-phenylenediamine (6PPD) and its ozonated product, 6PPD-quinone (6PPD-Q), are highly toxic to aquatic life, yet understanding on their environmental behaviors is limited. This study comprehensively investigated their adsorption and transformation processes on natural Fe-Mn nodules (NFMN), which commonly exist in sediments and soils through a combination of diverse experimental and computational methods. The maximum adsorption capacity of 6PPD-Q (719.2 μg·g −1 ) is significantly higher than that of 6PPD (133.8 μg·g −1 ) at 293 K, and it is more difficult to desorb. They follow different kinetic and isothermal adsorption models, and environmental conditions (including temperature, pH, and anions) exert distinct influences on the adsorption of the two substances. Adsorption mechanisms involving electrostatic attraction, charge transfer, hydrogen bonding, and Lewis acid-base complexation were unveiled. For 6PPD, electrostatic adsorption and Lewis acid-base complexation contribute significantly to its adsorption. Conversely, for 6PPD-Q, the contribution of Lewis acid-base complexation outweighs that of hydrogen bonding, while the effect of electrostatic adsorption is relatively negligible. The stronger electrostatic attraction, more efficient charge transfer, and a greater number of binding sites for hydrogen bonding and Lewis acid-base complexation with NFMN results in more robust adsorption of 6PPD-Q. Furthermore, 6PPD can transform into 6PPD-Q on NFMN, facilitated by dissolved Mn(III). This study advances understanding of the adsorption behavior and mechanism of 6PPD and 6PPD-Q, and highlights a new pathway for 6PPD-Q formation, which provides valuable reference for assessing the water body exposure risks and formulating environmental remediation strategies for such pollutants. Environmental Implication This study offers the first comprehensive insight into the interactions between 6PPD/6PPD-Q and NFMN, illuminating their environmental behavior in water and soil systems. It reveals the adsorption discrepancy between 6PPD and 6PPD-Q, and elucidates the mechanisms underlying the difference in adsorption. Additionally, it uncovers a novel pathway for 6PPD-Q formation, offering valuable implications for risk assessment and environmental remediation strategies.
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Applied Catalysis O: Open
·
2025
·
IF 0
Yiyin Zhu,Qibing Dong,Atif Sial,Abdelkader Labidi,Ke Zhao,Ximing Li,Junjun Wang,Chuanyi Wang
Achieving efficient ligand-metal charge transfer remains a significant challenge for constructing high-performance N 2 -fixing MOF photocatalysts. Herein, we successfully fabricated mixed-metal MIL-101(Fe/Cr) materials to achieve ligand-metal charge transfer, leading to significantly improved N 2 fixation performance. Performance test under visible light demonstrated that MIL-101(Fe/Cr) achieved nitrogen fixation activity of 125.19 μmol h −1 g −1 , which is 1.7 times greater than that of pure MIL-101(Fe). The experimental confirm that the incorporation of Cr metal enables the more favorable accumulation of photogenerated electrons at the Fe catalytic centers, attributed to increased electronic interactions and enhanced charge transfer efficiency, thus facilitating the activation process of N 2 , and consequently enhancing ammonia (NH 3 ) production. This work provides new insights into strategies for improving the ligand-metal charge transfer efficiency of MOF-based photocatalytic nitrogen fixation materials.
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MICROCHIMICA ACTA
·
2025
·Vol. 192
·期 7
·1-12
·
IF 5.3
Gu Yaohong,Li Qiulan,Yang Dezhi,Yang Yaling
A phosphomolybdate nanozymes doped with copper and iron particles (Cu,Fe-PMs) with excellent peroxidase (POD)-like activity was prepared by one-step microwave digestion method. It can oxidize the positively charged substrates such as 3,3′,5,5′-tetramethylbenzidine (TMB) in the presence of H₂O₂, resulting in the formation of a blue compound. It is noteworthy that the POD-like activity of Cu,Fe-PMs was significantly boosted upon the incorporation of sodium dehydroacetate (DHA). This was attributed to the formation of complex between the Cu,Fe-PMs and DHA. On the one hand, DHA enhances the affinity of Cu,Fe-PMs for the substrate and exhibits superior catalytic properties. On the other hand, DHA also accelerated the valence state transformations between Fe 3+ /Fe 2+ and Cu + /Cu 2+ , increased catalytic active sites and facilitate the generation of more reactive oxygen species (ROS) such as •OH with strong oxidation. Therefore, the current study successfully established a highly sensitive and reliable colorimetric sensor for detecting the DHA content in foods. The results indicated that the absorbance at 652 nm exhibited a linear relationship with DHA concentration within the range of 0.0017—2.5 μg mL −1 , achieving a minimum limit of detection (LOD) as low as 0.83 ng mL −1 . The sensor was successfully applied to detect DHA in actual samples, with recoveries ranging from 91.59% to 103.35% and a relative standard deviation (RSD) not exceeding 3.64%. This demonstrates the reliable performance and consistent reproducibility of the analytical approach. Graphical
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MOLECULES
·
2024
·Vol. 29
·期 9
·1946
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IF 4.2
Yan Ma,Kai Wang,Sikai Liang,Zhongqing Li,Zhiyuan Wang,Jun Shen
The Mn-Fe oxide material possesses the advantages of abundant availability, low cost, and non-toxicity as an energy storage material, particularly addressing the limitation of sluggish reoxidation kinetics observed in pure manganese oxide. However, scaling up the thermal energy storage (TCES) system poses challenges to the stability of the reactivities and mechanical strength of materials over long-term cycles, necessitating their resolution. In this study, Mn-Fe granules were fabricated with a diameter of approximately 2 mm using the feasible and scalable drop technique, and the effects of Y2O3-stabilized ZrO2(YSZ) and SiO2doping, at various doping ratios ranging from 1–20 wt%, were investigated on both the anti-sintering behavior and mechanical strength. In a thermal gravimetric analyzer, the redox reaction tests showed that both the dopants led to an enhancement in the reoxidation rates when the doping ratios were in an appropriate range, while they also brought about a decrease in the reduction rate and energy storage density. In a packed-bed reactor, the results of five consecutive redox tests showed a similar pattern to that in a thermal gravimetric analyzer. Additionally, the doping led to the stable reduction/oxidation reaction rates during the cyclic tests. In the subsequent 120 cyclic tests, the Si-doped granules exhibited volume expansion with a decreased crushing strength, whereas the YSZ-doped granules experienced drastic shrinkage with an increase in the crushing strength. The 1 wt% Si and 2 wt% Si presented the best synthetic performance, which resulted from the milder sintering effects during the long-term cyclic tests.
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NANOTECHNOLOGY
·
2025
·Vol. 36
·期 39
·395401
·
IF 2.8
Wang Zhang,Tianci Feng,Shiqi Li,Xin Zhang,Tang Wang,Yu Zhou,Long Lin,Lin Qiao,Xiao Han,Rui Li
Electrocatalytic nitrate reduction has emerged as a promising strategy for sustainable ammonia synthesis, providing the dual advantage of mitigating nitrate pollution and producing value-added green ammonia. However, enhancing intrinsic catalytic activity and catalytic site accessibility remains a challenge for further improving the performance of nitrate electroreduction to ammonia. Herein, a series of gradient Cu2+-doped MIL-53(Fe) electrocatalysts were synthesized via an all-solid-state mechanochemical synthesis method for electrocatalytic nitrate-to-ammonia conversion. MIL-53(Fe)–CuB exhibits a large NH3 production rate of 2391 ± 327 μg h−1 mgcat−1 at −0.6 V vs RHE and a high Faradaic efficiency of 82.1% ± 1.2% at −0.3 V vs RHE in 1 M KOH with 100 ppm NO3−, demonstrating an excellent electrocatalytic performance for nitrate reduction. This work reveals that Cu2+-doping in mechanochemically synthesized Fe-metal-organic frameworks (MOFs) boosts nitrate reduction efficiency and selectivity, while broadening research on foreign metal ion anchoring in MOF electrocatalysis.
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IONICS
·
2026
·
IF 3.4
Wu Keying,Xie Wenda,Liu Xingjian,Chen Jing,Pu Haitao,Luo Bing
Separator design can improve electrolyte wetting, ion transport and dimensional stability in lithium metal cells with LiFePO 4 cathodes. Here, an Fe–Ti metal–organic framework (MOF) was prepared by a solvothermal route and incorporated into poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP) nanofiber membranes by electrospinning. The effects of filler loading were evaluated against pristine PVDF-HFP and a commercial Celgard separator. Among the investigated compositions, PVDF-HFP/MOF-10 exhibited an electrolyte contact angle of 18°, an ionic conductivity of 1.7 × 10⁻ 3 S cm⁻ 1 at 30 °C, and an apparent Li⁺ transference number of 0.56 under the Bruce–Vincent measurement protocol. The composite also showed improved thermal dimensional stability. Li‖Li cells operated for over 500 h at 1 mA cm⁻ 2 and 1 mAh cm⁻ 2 , while LiFePO 4 ‖Li cells retained 92.3% of their initial discharge capacity after 500 cycles at 1 C. These observations support the use of the composite separator for improving performance under the tested conditions. Adsorption calculations provide a possible molecular explanation for electrolyte affinity, but do not establish ion desolvation, selective anion immobilization or a unique bimetallic synergy in the operating electrolyte. The contribution is the integration and loading optimization of an Fe–Ti MOF within a porous PVDF-HFP separator, with the microscopic transport mechanism remaining to be resolved.
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MICROCHIMICA ACTA
·
2021
·Vol. 188
·期 8
·1-11
·
IF 5.833
Zhang Youxiong,Li Bing,Wei Xianhu,Gu Qihui,Chen Moutong,Zhang Jumei,Mo Shuping,Wang Juan,Xue Liang,Ding Yu,Wu Qingping
A facile and versatile competitive electrochemical aptasensor for tobramycin (TOB) detection is described using electrochemical-deposited AuNPs coordinated with PEI-functionalized Fe-based metal-organic framework (AuNPs/P-MOF) as signal-amplification platform and a DNA probe labeled with methylene blue (MB) at the 3′-end (MB-Probe) as a signal producer. First, F-Probe (short complementary DNA strands of both the aptamer and the MB-Probe label with a sulfhydryl group at the 5′-end) was immobilized on the AuNPs/P-MOF modified electrode as detection probes, which competed with TOB in binding to the aptamer. TOB-aptamer binding resulted in F-Probe remaining unhybridized on the electrode surface, so that a significant current response was generated by hybridizing with MB-Probe instead. The developed strategy showed favorable repeatability, with a relative standard deviation (RSD) of 4.3% computed over five independent assays, and high stability, with only 6.8% degradation after 15 days of storage. Under optimal conditions, the proposed aptamer strategy exhibited a linear detection range from 100 pM to 500 nM with a limit of detection (LOD) of 56 pM (S/ N = 3). The electrochemical aptasensor demonstrated remarkable selectivity, and its feasibility for accurate and quantitative detection of TOB in milk samples was confirmed (RSD < 4.5%). Due to its simple design, easy operation, and high sensitivity and selectivity, the proposed method could expect to detect other antibiotics by replacing the aptamers. In summary, this study provides a simple and effective new strategy for electrochemical aptasening based on MOF-based sensing interface. Graphical abstract
Scheme illustration of label-free competitive electrochemical aptamer-based detection of tobramycin based on electrochemically deposited AuNPs coordinated with PEI-functionalized Fe-based metal-organic framework as signal-amplification platform.
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Environmental Technology & Innovation
·
2025
·
IF 7.1
Jun Dong,Yuanjun Tang,Jiayin Ma,Peikun Jiang,Yinxiu Liu,Ruohui Lu,Yin Li,Shuqi Li,Yangqing Hu,Fei Wang
The widespread use of antibiotics has led to their accumulation in water, posing serious environmental risks. Biochar has emerged as a promising adsorbent for antibiotic removal, but its performance is often limited by low capacity and slow kinetics, especially for high-molecular-weight antibiotics. In this study, a hierarchical porous Fe-supported biochar (HPFeBC) was synthesized via one-step pyrolysis of pine sawdust using Fe(NO 3 ) 3 as both activator and template. The obtained HPFeBC exhibited a well-interconnected pore structure with a high surface area (417.23 m 2 /g) and enhanced mesoporosity, significantly improving mass transfer and accessibility of adsorption sites. HPFeBC demonstrated exceptional adsorption performance for both low-molecular-weight antibiotic tetracycline (TC) and high-molecular-weight antibiotic tylosin (TYL), with maximum capacities of 361.23 mg/g and 173.61 mg/g, respectively. Notably, HPFeBC achieved rapid adsorption equilibrium within 5 mins for TC and 30 mins for TYL, far surpassing commercial adsorbents. The adsorption process followed the pseudo-second-order kinetics and the Freundlich isotherm model, and thermodynamic analysis confirmed the spontaneous and endothermic nature of adsorption. The adsorption mechanism involved pore filling, π-π interactions, hydrogen bonding, surface complexation, and limited redox reaction. HPFeBC also exhibited excellent stability over a wide pH range, strong anti-interference ability, and good reusability. Overall, the synthesis HPFeBC can act as an effective candidate for rapid and efficient removal of antibiotics from water.
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Chemical Engineering Journal Advances
·
2025
·
IF 7.1
Xiaoyu Fang,Shucai Zhang,Yan Xie,Meng Yao,Diannan Lu,Yakui Chen
The widespread use of methyl tert-butyl ether (MTBE) in gasoline has led to persistent groundwater contamination. Recently, permeable reactive barriers (PRBs) have emerged as a key in situ remediation technology for treating with such contamination. Various reactive media have been employed to intercept and degrade pollutants, but their short half-lives, instability, and poor dispersion in heterogeneous geological conditions limit their effectiveness and further applications. In this study, we designed a double-column PRB system incorporating slow-release oxidants (PLA@CP-CA) and Fe-based zeolite as heterogeneous Fenton catalysts. Calcium peroxide (CaO₂) was selected as the oxidant instead of hydrogen peroxide (H₂O₂) due to its higher stability, ease of transport, and prolonged release, facilitating sustained pollutant degradation. However, the direct use of CaO₂ raises groundwater pH, so citric acid (CA) was employed as a buffer to regulate pH during CaO₂ dissolution, thereby enhancing the efficiency of the heterogeneous Fenton process. Electron paramagnetic resonance (EPR) spectroscopy and radical trapping experiments confirmed that multiple reactive species, including ·OH, O 2 – ·, and ¹O₂, contributed synergistically to MTBE degradation. To mitigate calcium peroxide leakage, polylactic acid (PLA) was used to encapsulate the oxidant (PLA@CP-CA) under anhydrous conditions. The Box–Behnken design (BBD) in response surface methodology (RSM) optimized the PLA@CP-CA formulation, achieving an optimal H₂O₂ release capacity of 3.22 mmol/g with a mass ratio of PLA/CP/CA at 0.67:1.77:1.17. Approximately 97% of MTBE was remediated within 192 hours using the double-column PRB, demonstrating the efficacy of the controlled oxidant release from PLA@CP-CA in promoting MTBE degradation. This heterogeneous Fenton system, combining PLA@CP-CA with Fe-S-1, offers a promising approach for in situ remediation in MTBE-contaminated environments.
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ACS ES&T Water
·
2025
·
IF 4.3
Neng Tao,Longjian Guo,Xiu Wu,Di Fang,Lixiang Zhou
To address the technical bottlenecks of the classic Fenton oxidation for anaerobically digested sludge (ADS) dewatering (e.g., high doses of Fe2+/H2O2/acid usage and slow reduction of Fe3+), we employed biodegradable tannin compounds as iron chelating and reducing agents to improve the Fenton reaction. Compared with the classic Fenton (pH 3.0), tannic acid (TA)-assisted Fenton enhanced the degree and rate of ADS dewatering (pH 5.2) with reductions of 99% in specific resistance filtration, 96% in capillary suction time, and 97% in filtration–compression time. Besides, this modification reduced the consumption of Fe2+/H2O2 by 50%. Mechanistically, TA could chelate Fe3+ to generate iron complexes while facilitating the reduction of Fe3+ to Fe2+. This phenomenon avoided Fe3+ precipitation and accelerated Fe3+/Fe2+ cycling to produce more hydroxyl radical (•OH).•OH oxidation disintegrated CHOP-, CHONS-, and CHONSP-containing protein-/lipid-like substances within tightly bound extracellular polymeric substances. Bioflocs were dispersed into an irregular block-shaped structure with smaller particle sizes. Employing low-cost and readily accessible tannin-rich plant crude extracts derived fromAcacia mangiumas an alternative to purified TA in Fenton conditioning of ADS exhibited comparable enhancements in dewaterability characteristics. These findings demonstrated that the synergy between tannin compounds and Fenton oxidation could facilitate the cost-effective dewatering of ADS.
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高影响因子
FUEL
·
2025
·
IF 7.5
Chi Li,JiXiang Guo,Li Wang,PengCheng Xue,WenLong Zhang,KunPeng Li
Heavy oil in-situ catalytic technology faces challenges like complex reservoirs, harsh environments, and high viscosity. Developing efficient in-situ catalysts is a key research focus. This study synthesized a Fe/Ce bimetallic organic framework (Fe/Ce-MOF) that addresses critical issues in heavy oil recovery. Under mild conditions at 140℃ with 0.5 wt% catalyst and 2 wt% hydrogen donor for 24 h, Fe/Ce-MOF achieved a 90.15 % reduction in viscosity and a 16.51 % decrease in asphaltene content. The characterization analysis and simulation results collectively reveal that the bimetallic MOF has a synergistic effect. On the one hand, the Fe 3+ /Fe 2+ redox cycle promotes the cracking of large molecules into smaller ones. On the other hand, the Ce 4+ /Ce 3+ redox cycle facilitates the formation of oxygen vacancies (O v ). Under the combined effect of the dynamic redox cycles of Fe 3+ /Fe 2+ and Ce 4+ /Ce 3+ , the electron transfer efficiency of the catalyst is significantly enhanced, increasing the rate of heavy oil pyrolysis and hydrogenation. The coexistence of Fe and Ce modifies the charge distribution in heavy oil MOF, enhancing Lewis acidity and promoting interaction with heteroatoms. Additionally, the coexistence of mesoporous and macropores in the bimetallic framework not only facilitated mass transfer and fully utilized the catalytic activity of active sites but also effectively resolves the issue of traditional microporous MOFs are prone to being blocked by larger asphaltene molecules, thereby improving their operational stability. This study proposes a novel strategy for the design and development of in-situ catalytic viscosity reduction catalysts for heavy oil, highlighting the high efficiency, excellent stability, and environmental compatibility of bimetallic MOF in low-temperature catalytic pyrolysis, and demonstrating their significant potential for practical applications.
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