TALANTA
·
2025
·
IF 6.1
Bowen Shen,Biao Hong,Xinyue Guo,Ruonan Hu,Luodi Wang,Yuchuan Jiang,Wei Li,Wenqing Liu,Zhengyan Wu,Pengqi Yang
Precise detection of ultralow-level antibiotics, such as picomole, in aqueous environments is significant for human health, however, it presents a great challenge to the adsorption capacity and electrocatalytic ability of sensing materials. Here, we used a one-step hydrothermal method to in situ grow spindle-like CoFe-based metal-organic frameworks (MOFs) with a size of about 50 nm in the region of hydrophilic MXene-loading hydrophobic carbon paper. By combining MOFs with abundant adsorption sites and MXene with high conductivity, the problems of adsorption and electrons transfer of ultralow-level antibiotics have been solved, and achieving precise detection of picomole-level antibiotics. As a result, the CoFe-MOFs/MXene/HCP sensing electrode exhibits the ultralow limit of detection with 33 pM and a wide detection range with 0.1 nm–2.0 mM for chloramphenicol (CAP) detection, as well as the designed sensor has excellent anti-interference, reproducibility, and stability. Importantly, the prepared sensing electrode exhibits reliable analytical results for CAP in real water samples, such as bottled water, milk, and urine, indicating that the prepared sensors have a great potential for application in the analysis of antibiotics in real samples.
研究领域:
材料科学
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分析化学
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环境科学
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DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Wenjuan Wang,Yanfang Huang,Junpeng Zuo,Lulu Kou,Bingbing Liu,Hu Sun,Guihong Han
Microfine metal–organic frameworks (MOFs) are promising adsorbents for water treatment, but their commercial applicability is severely constrained by poor separability. Herein, we designed a feasible bubble flotation strategy for achieving the effective separation of oxyanions-loaded Fe-MOF particles in the solution after adsorption, by modifying the particle interface properties and introducing bubbles mineralization. The results showed that the separation of P(V), Mo(VI) and W(VI) oxyanions-loaded Fe-MOF could be completely achieved under optimum conditions. FTIR, XPS and DFT analyses revealed that the particle size and hydrophobicity of oxyanions-loaded Fe-MOF increased by sodium dodecyl sulfate (SDS) collector via chemisorption and electrostatic interactions. The collision and attachment models analysis of bubbles with particles demonstrated that the separation efficiencies of collector modified oxyanions-loaded Fe-MOFs were significantly enhanced with increasing bubble mineralization. EDLVO theoretical calculations and bubble-particle carrying ability analysis demonstrated that the gravitational interactions between oxyanions-loaded Fe-MOF particles and particles/bubbles were intensified by the collector. The gravitational interaction further induced particle aggregation and enhanced the carrying capacity of individual bubbles. This work provides a feasible strategy for the removal of oxyanions and the separation of oxyanions-loaded microfine Fe-MOF in the adsorption process.
研究领域:
环境科学
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材料科学
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化学工程
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产品关联
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2022
·
IF 14.224
Limin Duan,Huihao Jiang,Wenhao Wu,Daohui Lin,Kun Yang
Introducing crystal defects into iron based metal-organic frameworks (Fe-MOFs) is regarded as a promising strategy to enhance Fenton-like performance. However, developing a facile and effective strategy to construct defective Fe-MOFs as highly efficient Fenton-like catalyst is still a challenge. Herein, MIL-100(Fe) (Def-MIL-100(Fe)) with missing ligands defects was synthesized by a simple heterogeneous reaction using zero-valent iron. The bisphenol A degradation efficiency in the Def-MIL-100(Fe)/H 2 O 2 system reached up to 91.26% within 10 min at pH 4 with a low catalyst dosage of 0.05 g/L, while the perfect MIL-100(Fe) has almost no Fenton-like performance. It was observed that missing ligands defects in the Def-MIL-100(Fe) play a key role in the Fenton-like reaction. The missing ligands defects could increase the Lewis acidity for fast H 2 O 2 adsorption and accelerate the electron transfer between Fe II and Fe III cycling, leading to faster and more·OH generation. Moreover, the missing ligands defects could promote the mass transfer for improving·OH utilization efficiency. This work provides a novel strategy to construct defective Fe-MOFs as highly efficient Fenton-like catalyst to degrade organic pollutants in water.
研究领域:
环境科学
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材料科学
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产品关联
DOI
PubMed
高影响因子
ACS Applied Nano Materials
·
2023
·
IF 5.9
Xiang-Yu Wang,Meng Zhu,Qing-Nan Bian,Ben-Shuai Guo,Wei-Qing Kong,Chong-Bin Wang,Yuan-Yuan Feng
Hydrogen, carrying a high energy density and emitting zero greenhouse gases when in use, is particularly promising as an alternative for traditional fossil fuels. Electrochemical water splitting is an economical technology for producing sustainable and high-purity hydrogen gas. However, the intrinsically sluggish kinetics of the anode oxygen evolution reaction (OER) always decreases the efficiency of hydrogen production; the development of highly active and durable electrocatalysts with improved OER kinetics is thus desirable and crucial. Herein, Fe-based metal–organic framework (MOF)-Ni3S2 heterostructure nanocomposites are synthesized on a nickel foam (NF) substrate. The self-supporting Fe MOF-Ni3S2/NF catalyst shows excellent catalytic activities for OER. In alkaline media (1.0 M KOH), only 243 mV of overpotential is needed to reach the current density of 100 mA·cm–2. Even at the commercially viable high current densities of 500 and 1000 mA·cm–2, ultralow overpotentials of 283 and 309 mV are required, respectively. The catalytic activity of Fe MOF-Ni3S2/NF far exceeds that of the noble metal catalysts (e.g., RuO2) and most non-noble metal OER catalysts reported in the literature. In addition, the Fe MOF-Ni3S2/NF nanocomposite exhibits ultrahigh long-term stability at high current densities, with almost no activity attenuation in the chronopotentiometry test conducted at 100 mA·cm–2 and a negligible attenuation (23 mV) at 500 mA·cm–2 for 20 h. Our findings provide insights into designing and preparing cost-effective, highly active, and durable electrocatalysts for OER at high current densities.
研究领域:
材料科学
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电化学
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产品关联
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2024
·
IF 2.7
Yu Gao,Siyu Liu,Xu Huang,Weiwen Lu,Jian Huang,Hua Zhang,Yong Zhang,Jinhua Wang,Shanshan Xi,Jun Liu,Tao Luo
Considering the difficulty in recovering powder materials and the low photocatalytic efficiency, we have developed a series of Fe-MOFs (MIL-53(Fe), NH2-MIL-53(Fe), MIL-101(Fe), NH2-MIL-101(Fe) and MIL-100(Fe)) on pure iron mesh. In this study, the growth of Fe@MILs on the iron mesh was confirmed through SEM, XRD, and FT-IR characterizations. Among the photocatalytic experiments, Fe@NH2-MIL-53(Fe) and Fe@NH2-MIL-101(Fe), which are amine-functionalized, showed improved photocatalytic activity. This improvement is believed to be due to the combination of NH2 functionality and electron transfer to the Fe-O cluster centre, resulting in dual excitation pathways. Furthermore, Fe@MIL-100(Fe) showed the highest performance for the removal of Cr(VI), with over 92% of Cr(VI) being removed in the fifth photocatalytic cycle. Mechanism indicated that the close connection between the compact structure of Fe-MOFs and effective electron migration. Additionally, sacrificial reagent experiments identified two important species for Cr(VI) reduction: electrons (e-) and superoxide radicals (O2-). The photocatalytic recovery tests showed a 97% recovery rate of Cr(VI). This work offers a novel solution for the treatment of water sources contaminated with Cr(VI).
研究领域:
环境科学
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材料科学
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化学工程
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产品关联
DOI
高影响因子
Journal of Physical Chemistry C
·
2024
·
IF 3.3
Qianglong Qi,Yue Zhang,Chengxu Zhang,Feng Liu,Rongjiang Liu,Jue Hu
Iron-based metal–organic frameworks (MOFs) have shown potential as catalysts for the electrocatalysis oxygen evolution reaction (OER). Despite numerous methods being employed to enhance the OER performance of MOFs, the influence of halogen-containing linkers on the electronic structure of iron-based MOF catalysts remains unexplored. In this study, a series of Fe-based MOFs (denoted as MOF-R, where R = H, Cl, or Br) with comparable structures are synthesized by changing the organic linkers coordinated with the Fe metal active center, with the aim of investigating the influence of halogen-containing linkers on the OER activity. Significantly, MOF-Br exhibited superior OER activity compared to MOF-Cl and MOF-H. Density functional theory calculations reveal that the tuning of halogen groups on organic linkers can modulate the electronic structure of the metal active sites and effectively regulate the adsorption behavior of key intermediates near the optimal d-band center, leading to the enhancement of electroactivity. Notably, the bromine-substituted MOF-Br catalyst displayed remarkable intrinsic OER activity, including a low overpotential of 251.2 mV at a current density of 10 mA cm–2 and a low Tafel slope of 44.5 mV dec–1, surpassing the halogen-unsubstituted MOF-H (262.6 mV and 63.4 mV dec–1) and commercial IrO2 (335.3 mV and 98.6 mV dec–1). Moreover, the high turnover frequency at an overpotential of 300 mV was measured to be 0.537 s–1, which is 30 times greater than that of the commercial IrO2 catalyst (0.018 s–1). This research offers a potential strategy for designing MOF electrocatalysts with superior OER activity, laying a solid foundation for the rational design and synthesis of excellent OER electrocatalysts in the future.
研究领域:
材料科学
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电化学
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产品关联
DOI
高影响因子
MICROCHEMICAL JOURNAL
·
2024
·
IF 4.9
Kaiwen Zhang,Zhuanzhuan Shi,Yunpeng Li,Xiaoshuai Wu,Zuqiang Ma,Wei Sun,Chang Ming Li,Chunxian Guo
Chloramphenicol (CAP), a broad-spectrum antibiotic agent that can inhibit protein synthesis, has caused environmental and human health problems upon excessive usage but to realize its ultrasensitive detection is still a great challenge. We report here the design and fabrication of a nanocomposite comprising graphdiyne (GDY) chelated iron-based metal–organic framework (Fe-MOF@GDY) with strong interfacial interaction to achieve high performance electrochemical sensing of CAP. Fe-MOF@GDY exhibits good selectivity, a linear range of 1 pM−24 mM and an ultralow detection limit down to 0.54 pM, among the best performance for CAP detection. It displays good reproducibility and storage stability with retained 98.4% of its initial response after 3 weeks. GDY with unique electronic structure enhances charge transfer of Fe-MOF for improved conductivity, and Fe-MOF nanoparticles are uniformly chelated on GDY for rich active sites towards CAP reduction. Fe-MOF also prevents GDY from being degraded, promoting long-term stability. A portable electrochemical chip is fabricated based on Fe-MOF@GDY, and is successfully used for accurate detection of CAP in lake water with recovery rates of 97.2–104.7%, demonstrating the practical on-site applications.
研究领域:
分析化学
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材料科学
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环境科学
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Shumin Li,Fan Wu,Rongbin Lin,Jin Wang,Chunxia Li,Zhengquan Li,Jun Jiang,Yujie Xiong
Fe-based metal-organic frameworks (MOFs) have shown promising applications in photocatalysis, yet they are incapable of photocatalytic H 2 production due to their inappropriate conduction band (CB) position and large overpotential for H 2 evolution. Herein, we present a facile strategy enabling the photocatalytic H 2 production over Fe-based MOFs through dye sensitization. A combination of characterization techniques with theoretical simulation reveals that dye sensitization can effectively inject energetic electrons into Fe-MOFs and elevate their quasi-Fermi level under light irradiation, overcoming the surface overpotential for H 2 production from water. Furthermore, deposition of Pt nanoparticles on Fe-MOFs can lower the overpotential for H 2 evolution toward further enhanced photocatalytic activity. This work provides insights into MOF band structure engineering at electronic level, and proves a concept that harnesses MOF materials for targeted photocatalytic applications they are originally not fit for.
研究领域:
材料科学
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化学工程
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能源科学
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产品关联
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2020
·Vol. 44
·期 48
·21183-21191
·
IF 3.288
Pengyao Yu,Sheng Liu,Yuchen Cui,Kun Sun,Ling Zhang,Hailing Guo,Yongming Chai,Chenguang Liu,Lili Fan,Ge Yang,Chunzheng Wang,Svetlana Mintova
A uniform bimetallic hollow ZnFe–N/C (80–180 nm) electrocatalyst is synthesized using a precursor ZnFe-ZIF-8 (100–200 nm) subjected to pyrolysis in an argon atmosphere at 800 °C for 2 hours. The ZnFe–N/C catalyst was deposited on a glassy carbon electrode (GCE), and exhibited a superior electrocatalytic activity with a high onset potential (0.97 V vs. RHE) and half-wave potential (0.85 V vs. RHE), high stability in an alkaline electrolyte, and remarkable resistance to methanol. The high performance of the ZnFe–N/C-3 electrocatalyst is attributed to the hollow structure containing metallic Fe/Fe3C and N doping.
研究领域:
材料科学
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电化学
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产品关联
DOI
高影响因子
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2020
·
IF 3.807
Lili Cui,Qiaoling Zhang,Xingquan He
The Fe 3 C encapsulated in nitrogen doped carbon nanotubes electrocatalysts (Fe 3 C@N-CNTs) are constructed derived from iron metal-organic framework (Fe-MOF) by a facile method. It is well accepted that the catalytic performance is dependent on the morphology of the electrocatalyst. Thus, here, the morphology of the carbon nanotubes is obtained by tuning the species of iron salt and the annealing temperature, the optimal material shows nanotube morphology and high surface area. Also, it is noted that FeNC-Cl/800 has higher N content compared to FeNC-NO 3 /800, indicating that Cl − favor in promoting nitrogen doping. In alkaline condition, the optimized Fe 3 C@N-CNTs catalyst exhibits more positive onset and half-wave potentials (0.98, 0.85 V vs RHE) than other contrast samples. Importantly, it displays a more positive onset and half-wave potentials of 0.82, 0.68 V vs RHE in acidic medium. It shows a 4e − pathway towards ORR, good capacity of stability and methanol tolerance in both alkaline and acidic media. The excellent electrocatalytic performance arises from various active sites (Fe 3 C and N doping), pretty morphology and hierarchically porous structure.
研究领域:
材料科学
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电化学
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产品关联
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2019
·Vol. 43
·期 24
·9725-9731
·
IF 3.069
Suresh Mutyala,Sobhy M. Yakout,Shebl S. Ibrahim,Madhavi Jonnalagadda,Harisekhar Mitta
Iron metal–organic framework, MIL-100(Fe) was prepared by a hydrothermal method and used as a support to incorporate diethylenetriamine (DETA) for the study of CO2 adsorption and separation of CO2/N2. All synthesized adsorbents were characterized by PXRD, N2 adsorption–desorption isotherms, FT-IR, TGA, SEM, and elemental analysis. Structural characterization results have revealed that the structure of MIL-100(Fe) was not changed by the incorporation of diethylenetriamine. The CO2 adsorption capacities were 29 cm3 g−1 and 41 cm3 g−1 at 298 K, 1 bar for MIL-100(Fe) and DETA–MIL-100(Fe), respectively. Adsorption of CO2 on DETA–MIL-100(Fe) was higher than that on MIL-100(Fe). The enhancement was due to the presence of amine groups which could form ammonium carbamate by interaction with CO2. Similarly, the N2 adsorption capacities were 3 cm3 g−1 and 0.9 cm3 g−1 at 298 K, 1 bar for MIL-100(Fe) and DETA–MIL-100(Fe), respectively. The decrease in N2 adsorption capacity was due to the decrease in surface area. The selectivity of CO2/N2 on DETA–MIL-100(Fe) was four times higher than that on MIL-100(Fe). The heat of CO2 adsorption was 74.2 kJ mol−1 at low coverage of CO2 on DETA–MIL-100(Fe) and the CO2 adsorption capacity was constant in each adsorption cycle over the same adsorbent.
研究领域:
材料科学
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环境科学
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产品关联
DOI
高影响因子
Journal of Water Process Engineering
·
2021
·
IF 5.485
Qiuya Zhang,Jun Xu,Xiaoyan Ma,Jinmei Xu,Zeping Yun,Qiaosheng Zuo,Liping Wang
Metal-organic frameworks (MOFs) are new porous materials that attract wide attention due to their environmentally-friendly photocatalytic characteristics. However, poor charge separation in most MOFs largely limits their photocatalytic activity. In this study, a novel Fe-based bi-MOFs heterojunctions material, namely NH 2 -MIL-88B(Fe)@MIL-100(Fe) was prepared by internal extended growth of MIL-100(Fe) on spindle-like NH 2 -MIL-88B(Fe). Compared with pure NH 2 -MIL-88B(Fe) and MIL-100(Fe), the synthesized Fe-based bi-MOFs structure catalyst displayed excellent photocatalytic degradation of tetracycline (TC), with optimal removal of 99.9% achieved in 90 min under neutral conditions. This result is attributed to the sufficient visible light absorption , and the enhanced separation and transfer of h + and e − by the bi-MOFs structure. In particular, ∙O 2 − , h + and ∙OH showed synergistic effects in the photodegradation process, and Fe-based bi-MOFs displayed high stability after five cycles. The inhibition ratio of luminescent bacteria of the degraded solution was lower than 24%, indicating the high efficiency and safety of this Fe-based bi-MOFs for the treatment of antibiotic-contaminated water.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子