MICROCHIMICA ACTA
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2021
·Vol. 188
·期 10
·1-11
·
IF 5.833
Qin
Peige,Han Lizhen,Zhang Xiaowan,Li Mengyuan,Li Dan,Lu Minghua,Cai Zongwei
Abstract Using MIL-101(Fe) as the source of carbon and Fe, a magnetic porous carbon (MPC) material with Fe 3 C nanoparticles encapsulated in porous carbon was prepared through one-pot pyrolysis under N 2 atmosphere. With MPC as adsorption material, a stir bar sorptive-dispersive microextraction (SBSDME) method was proposed to extract and preconcentrate sulfonamides (SAs) prior to HPLC-DAD determination. To investigate their extraction ability, different MPC materials were prepared under different carbonization temperatures (600, 700, 800, 900, and 1000 °C). The material prepared under 900 °C (MPC-900) exhibited the highest extraction ability for SAs. The as-prepared MPC materials were also characterized by Raman spectroscopy, scanning electron microscopy, X-ray photoelectron spectroscopy, zeta potential, and other techniques. The main parameters that affect extraction were systematically studied. Under optimal conditions, favorable linearity ( R 2 ≥ 0.9938) and detection limits (0.02–0.04 ng mL −1 ) of sulfonamides were obtained. The average recoveries for spiked milk and lake water samples ranged from 76.9 to 109% and from 75.4 to 118% with RSDs of 3.10–9.63% and 1.71–11.3%, respectively. Sulfameter and sulfisoxazole were detected in milk sample. Sulfisoxazole was detected in the lake water sample. The MPC-900 material demonstrated excellent reusability. It can be reused 24 times with peak areas having no obvious decline. The method can be applied to extract ultra-trace compounds in complex sample matrices. Graphical abstract
Schematic presentation of a stir bar sorptive-dispersive microextraction (SBSDME) by using magnetic porous carbon (MPC) composites as sorbent combined with high-performance liquid chromatography for sensitive analysis of sulfonamides in milk and lake water samples.
研究领域:
分析化学
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环境科学
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF MATERIALS CHEMISTRY
·
2012
·Vol. 22
·期 34
·17833-17841
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IF 5.968
Cheng-Xiong Yang,Xiu-Ping Yan
The adsorption and extraction of fullerenes on the metal–organic framework MIL-101(Cr) were studied in detail in terms of kinetics, thermodynamics, adsorption isotherms, competitive adsorption, and breakthrough curves. The adsorption of C60 and C70 on MIL-101(Cr) follows a pseudo-second-order kinetic model. The adsorption rate constant for C70 is 3 to 5 times that for C60, showing faster and easier adsorption of C70 over C60 on MIL-101(Cr). Intraparticle diffusion model analysis reveals that the adsorption of C60 and C70 on MIL-101(Cr) proceeds by two phases, surface sorption and intraparticle/pore diffusion. The adsorption of fullerenes on MIL-101(Cr) is controlled by entropy changes. The maximum adsorption capacity for C70 at 30 °C (198.4 mg g−1) is 29 times that for C60 (6.76 mg g−1). MIL-101(Cr) shows much more favorable adsorption of C70 and higher fullerenes than C60 with a high selectivity (αC70/C60 = 24). Selective extraction of C70 and higher fullerenes from crude carbon soot can be easily achieved on MIL-101(Cr) via a simple adsorption–desorption process. The used MIL-101(Cr) can be regenerated by washing with o-dichlorobenzene under ultrasonication. The high selectivity, fast adsorption, easy desorption, and excellent reusability makes MIL-101(Cr) attractive as a novel adsorbent for the enrichment and extraction of C70 and higher fullerenes.
研究领域:
材料科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF CLUSTER SCIENCE
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2023
·Vol. 34
·期 6
·3095-3103
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IF 2.8
Liu Xiangyi,Zheng Qianye,Jia Deqi,Wang Wenwen,Zhao Hong,Tao Xiansen,Sha Jingquan
To explore novel nanozymes as colorimetric biosensors with highly activities, the ternary MIL-101(Fe)@P 2 W 18 @SWNT nanocomposite was successfully fabricated based on the optimal matching principle, namely, Wells–Dawson-type polyoxometalates (POMs, H 6 P 2 W 18 O 62 abbreviated as P 2 W 18 ) were encapsulated in a custom MIL-101(Fe) cavity, and single-walled carbon nanotubes (SWNT) was then fixed. The peroxidase-like activities of MIL-101(Fe)@P 2 W 18 @SWNT nanocomposite were evaluated by detecting hydrogen peroxide (H 2 O 2 ) and glucose (GLC). Compared with the MIL-101(Fe), P 2 W 18 and SWNT, the MIL-101(Fe)@P 2 W 18 @SWNT exhibits better peroxidase-like properties and stability due to the nature of all components and their optimal synergy. Based on the excellent catalytic activity of MIL-101(Fe)@P 2 W 18 @SWNT , two colorimetric biosensors for detecting H 2 O 2 and GLC with linear ranges of 0–80 μM (H 2 O 2 ) and 0–150 μM (GLC) were constructed, and the low detection limit of 0.3 μM for H 2 O 2 and 0.2 μM for GLC are superior to the most reported nanozymes. The work opens a promising route in constructing heterogeneous MOFs and POMs-based nanozymes for biosensing application.
研究领域:
生物传感
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材料科学
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化学
✓ 已验证
产品关联
DOI
高影响因子
NANO
·
2020
·
IF 1.566
Heng Chen,Mengbing Cui,Cuilan Miao,Gairong Chen,Yongchun Zhang
In this work, the function of 4-nitroimidazole (4-NIm) in the formation of Cr-MIL-101 was confirmed. It was found that 4-NIm is an effective additive in the formation of Cr-MIL-101 synthesized at lower temperature. The investigation of crystallization time showed that 4-NIm can prevent Cr-MIL-101 phase converting into Cr-MIL-53 phase. The effect of concentration of 4-NIm on the morphology and the yield of Cr-MIL-101 may therefore be explained by increasing the nucleation rate. The investigation of crystallization temperature revealed that 4-NIm changes the synthesis temperature range of Cr-MIL-101 into 423–463 K. The assistant function of 4-NIm was played through interaction with H + and NO 3 − in the synthesis system, which may lead to enhancement of the deprotonation of H 2 BDC.
研究领域:
材料化学
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配位化学
✓ 已验证
产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2021
·
IF 3.764
Ju Liu,Dandan Hao,Huiwen Sun,Yu Li,Jianlin Han,Bo Fu,Jiancheng Zhou
In this Article, a hybrid foam was fabricated through the integration of amine-functionalized Fe-MOF (MIL-101-NH2) into cellulosic matrix. The existence of enormous group linkages and ionic bonding interactions among the composite foam network leads to a uniform dispersion of MIL-101-NH2 and high affinity between the MOF and cellulose skeleton. As-prepared hybrid foams were utilized as photocatalysts to reduce toxic hexavalent chromium ions (Cr(VI)) under visible light. Optimal performance was observed over CM-1 (with a MIL-101-NH2 and nanocellulose mass ratio of 1:1). When compared to pure MOF nanoparticle counterparts, the CM-1 foam presented preferable and more efficient Cr(VI) removal performance. The reasons could be attributed to the hierarchal pore structure and uniform MOF loading. Moreover, the flexible foams could be easily separated from the solution and preserved more than 80% removal efficiency of Cr(VI) after 10 runs. This work would shed light on how to construct high-efficiency photocatalysts for environmental governance from sustainable materials.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF POROUS MATERIALS
·
2019
·Vol. 26
·期 6
·1839-1850
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IF 1.947
He Lei,Zhang Yaqin,Zheng Yane,Jia Qingming,Shan Shaoyun,Dong Yanan
An effective catalyst of MIL-101(Fe)/TiO 2 composite was synthesized by solvothermal method. The resultant MIL-101(Fe)/TiO 2 was used for advanced oxidation degradation of tetracycline (TC) for the first time. The results indicated that the MIL-101(Fe)/TiO 2 showed higher TC degradation efficiency than pure MIL-101(Fe) or TiO 2 with the persulfate. Using 1 g L −1 MIL-101(Fe)/TiO 2 and persulfate at pH 7, 90.15% degradation rate was achieved under xenon lamp irradiation in 5 min for 20 mg L −1 TC. TiO 2 introduced in the composite played an important role in the degradation process, in which TiO 2 had a synergetic effect with Fe 3+ to generate Fe 2+ , Ti 3+ and radicals. Fe 2+ reacted with persulfate to produce Fe 3+ and a number of · OH to degrade TC. This reaction process was so fast that MIL-101(Fe)/TiO 2 with persulfate could degrade TC fairly rapidly. A novel TiO 2 -based metal–organic frameworks (MOFs) composite was more efficient for degrading pharmaceutical wastewater.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
Polymers
·
2021
·Vol. 13
·期 20
·3498
·
IF 4.329
Shengqi Liu,Ye Meng,Hu Li,Song Yang
Considering economic and environmental impacts, catalytic biomass conversion to valuable compounds has attracted more and more attention. Of particular interest is furfural, a versatile biorefinery platform molecule used as a feedstock for the production of fuels and fine chemicals. In this study, the Cr-based metal-organic frameworks (MOFs) MIL-101 were modified by chlorosulfonic acid, and MIL-101 was changed into a hierarchical MOF structure with smaller particles and lower particle crystallinity by CTAB, which significantly improved the acidic sites of the MOFs. The original and modified MIL-101(Cr) catalysts were characterized by XRD, N2adsorption-desorption, SEM, TEM, and FT-IR. The effects of different catalysts, reaction temperature, catalyst amount, and alcohol type on the reaction were studied. Under the action of the MOFs catalyst, a new mild route for the condensation of furfural with various alkyl alcohols to the biofuel molecules (acetals) was proposed. The conversion route includes the conversion of furfural up to 91% yield of acetal could be obtained within 1 h solvent-free and in room-temperature reaction conditions. The sulfonic acid-functionalized MIL-101(Cr) is easy to recover and reuse, and can still maintain good catalytic activity after ten runs.Keywords:biomass conversion;MIL-101(Cr);furfural;green chemistry;heterogeneous catalysis
研究领域:
化学工程
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环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Hesong Wang,Jinlong Wang,Jing Zhao,Han Zhang,Luming Liu,Xueying Sun,Guibai Li,Heng Liang
As an emerging metal organic framework (MOF) material, MIL-101(Cr) has a large specific surface area and good hydraulic stability, making it ideal in applications before ultrafiltration (UF). However, the unclear interaction between MIL-101(Cr) and natural organic matter (NOM) was identified as the main limitation to understand membrane fouling. To reveal the working mechanisms of NOM removal using MIL-101(Cr), an integrated system of MOF and UF was constructed and operated in separation mode (SM) and coating mode (CM). Based on the results, MIL-101(Cr) had a high NOM adsorption capacity of 68.454 mg/g for HA and 174.725 mg/g for BSA at saturation. Permeate quality improvement occurred in both modes over a 37.7% UV 254 removal rate and a 15% fluorescence intensity decrease, and permeation performance of the hybrid system was simultaneously enhanced. We found that MIL-101(Cr) influenced membrane fouling behaviors and models because of the foulant transformation in SM and dispersed NOM in the MIL-101(Cr) layer in CM. Furthermore, MIL-101(Cr) played a dual role in the integrated system. It could remove NOM by adsorption, leading to membrane fouling reduction, but also caused additional filtration resistance. Notably, MIL-101(Cr) showed the overall positive effects due to its open hollow structure and good hydrophilicity. The π-π interactions and salt-bridges between MIL-101(Cr) and NOM played a dominant role in adsorption. Whilst SM was more efficient in membrane fouling mitigation due to reduced membrane fouling resistance and a normalized flux increase above 15%, CM could achieve the same permeate quality with less MIL-101(Cr) usage and reaction time. This study reveals the interaction between MIL-101(Cr) and NOM and their effects on UF, providing a scientific basis for the widespread application of MOFs.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
DALTON TRANSACTIONS
·
2018
·Vol. 48
·期 3
·989-996
·
IF 4.099
Ling Yang,Tian Zhao,Ishtvan Boldog,Christoph Janiak,Xiao-Yu Yang,Qiang Li,Yan-Jia Zhou,Yong Xia,Deng-Wang Lai,Yue-Jun Liu
The concentration of benzoic acid was found to exercise efficient control over the formation of either MIL-101(Cr) or MIL-88B(Cr) under otherwise similar hydrothermal synthetic conditions. Nanocrystals of MIL-101(Cr) with ∼100 nm average size and excellent SBET = 3467 m2 g−1 are obtained at lower concentrations of benzoic acid, while at higher concentrations the microparticulated MIL-88B(Cr) product is formed. Hereby a new efficient synthetic method towards the elusive MIL-88B(Cr), yet reported only once without synthetic details, is proposed. The obtained MIL-88B(Cr) has an interesting and potentially valuable property of retaining its high-volume form (Vcell ∼ 2000 Å3) after thermal activation. The degassing of MIL-88B(Cr) in a vacuum at 250 °C yields a porous material with a SBET area of 1136 m2 g−1, which is around the theoretical maximum. The transition to the denser ‘closed’ form (Vcell ∼ 1500 Å3) occurs only at 350 °C, when all of the benzoate/benzoic acid, hindering the process, is removed.
研究领域:
材料科学
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化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Catalysts
·
2019
·Vol. 9
·期 11
·906
·
IF 3.444
Jieyang Yang,Zequan Zeng,Zhanggen Huang,Yan Cui
In this work, the activation effect of vacuum thermal treatment on MIL-101(Fe) (MIL: Materials of Institute Lavoisier) was investigated for the first time. It demonstrated that vacuum thermal activation could accelerate the activation of persulfate (PS) by MIL-101(Fe), and the enhancement of the catalytic capacity of MIL-101(Fe) was mainly attributed to the change in the FeII/FeIII mixed-valence center. The results of the SEM and XRD showed that vacuum thermal activation had a negligible effect on the crystal structure and particle morphology of MIL-101(Fe). Meanwhile, the higher temperature of vacuum thermal activation caused a higher relative content ratio of FeII/FeIII. A widely used azo dye, X-3B, was chosen as the probe molecule to investigate the catalytic performance of all samples. The results showed that the activated samples could remove X-3B more effectively, and the sample activated at 150 °C without regeneration could effectively activate PS to remove X-3B for at least 5 runs and approximately 900 min. This work highlights the often-overlooked activation effect of vacuum thermal treatment and provides a simple way to improve the catalytic capacity and reusability of MIL-101(Fe) which is beneficial for the application of MIL-101(Fe)/PS systems in azo dye wastewater treatment.Keywords:vacuum thermal activation;MIL-101(Fe);persulfate;azo dye
研究领域:
环境科学
·
催化
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2017
·
IF 3.133
Kun Yang,Kangkang Yang,Shiliang Zhang,Yan Luo,Qilu Yao,Zhang-Hui Lu
Trimetallic NiFePd nanoparticles (NPs) anchored on metal-organic framework (MOF) MIL-101 have been facilely prepared via a simple impregnation method. The as-prepared NiFePd/MIL-101 catalysts have been characterized by powder X-ray diffraction (XRD), scanning electron microscope (SEM), transmission electron microscope (TEM) equipped with energy dispersed X-ray detector (EDX) and selected area electron diffraction (SAED), inductively coupled plasma-atomic emission spectroscopy (ICP-AES), N 2 adsorption/desorption isotherms and X-ray photoelectron spectroscopy (XPS) techniques. And the as-synthesized catalysts have been applied for hydrogen generation from aqueous alkaline solution of hydrazine borane (HB, N 2 H 4 BH 3 ). Compared to the pure Ni 0.36 Fe 0.24 Pd 0.4 NPs, MIL-101 supported mono- and bi-metallic counterparts, the Ni 0.36 Fe 0.24 Pd 0.4 /MIL-101 catalyst exhibits much higher catalytic performance for complete conversion of N 2 H 4 BH 3 to H 2 with 100% selectivity at 323 K. The turnover frequency ( TOF ) value for the dehydrogenation of N 2 H 4 BH 3 in the presence of Ni 0.36 Fe 0.24 Pd 0.4 /MIL-101 catalyst reaches 60 h −1 . Remarkably, the Ni 0.36 Fe 0.24 Pd 0.4 /MIL-101 catalyst also shows high catalytic activity and 100% selectivity towards hydrogen generation from hydrous hydrazine (N 2 H 4 ·H 2 O) at 323 K with a TOF value of 40.8 h −1 . In addition, the durability tests exhibit that the Ni 0.36 Fe 0.24 Pd 0.4 /MIL-101 catalyst is still highly active in the complete dehydrogenation of N 2 H 4 BH 3 and decomposition of N 2 H 4 ·H 2 O with 100% hydrogen selectivity even after five recycles.
研究领域:
材料科学
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催化化学
✓ 已验证
DOI
高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2024
·Vol. 31
·期 6
·9764-9783
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IF 0
Zhang Zhenhong,Zhong Yuye,Sun Peng,Zhao Pingping,Li Houbin,Liu Xinghai
The development of effective and practical adsorbents for eliminating pollutants still remains a significant challenge. Herein, we synthesized a novel magnetically separable composite, Co 0.6 Fe 2.4 O 4 /MIL-101-NH 2 , through the in-situ growth of MIL-101-NH 2 on magnetic nanoparticles, designed specifically for the removal of Congo red (CR) from aqueous solutions. MIL-101-NH 2 possessed high BET surface area (240.485 m 2 •g −1 ) and facile magnetic separation function and can be swiftly separated (within 30 s) through an external magnetic field post-adsorption. The investigation systematically explored the influence of crucial parameters, including adsorbent dosage, pH, adsorption duration, temperature, and the presence of interfering ions, on CR adsorption performance. Findings indicate that CR adsorption adheres to the pseudo-second-order (PSO) kinetic model and the Langmuir isotherm model. Thermodynamic analysis reveals the spontaneity, endothermic nature, and orderly progression of the adsorption process. Remarkably, the adsorbent with 0.1 g•L −1 boasts an impressive maximum adsorption capacity of 1756.19 mg•g −1 for CR at 298.15 K, establishing its competitive advantage. The reuse of the adsorbent over 5 cycles remains 78% of the initial adsorption. The CR adsorption mechanisms were elucidated, emphasizing the roles of π-π interactions, electrostatic forces, hydrogen bonding, and metal coordination. Comparison with other dyes, such as methylene blue (MB) and methyl orange (MO), and exploration of adsorption performance in binary dye systems, demonstrates the superior capacity and selectivity of this adsorbent for CR. In conclusion, our magnetically separable metal–organic framework (MOF)based composite presents a versatile and effective solution for CR removal, with promising applications in water treatment and environmental remediation. Graphical
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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纳米技术
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物理化学
✓ 已验证
DOI
危险品化学品经营许可证（带存储）