JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2019
·
IF 6.361
Zongchen Li,Xuemin Liu,Wei Jin,Qingsong Hu,Yaping Zhao
Arsenic species are regarded as typical water pollutants due to their toxicity. The chemical structures of arsenic species greatly influence their migration and transformation in the environment. Metal-organic frameworks (MOFs) are used as reliable adsorbents to control arsenic contamination, so it is urgently needed to study the effect of chemical structure of arsenic species during adsorption process. The adsorption behaviors of arsenate (As(V)) and its organic forms such as roxarsone (ROX), p-arsanilic acid (p-ASA) and dimethyl arsenate (DMA) by MIL-101(Fe), a type of highly porosity iron-based MOFs in aqueous environment were detailed investigated. The adsorption kinetics of those arsenic species on MIL-101(Fe) is rapid followed with pseudo-second-order kinetic model. MIL-101(Fe) exhibits excellent adsorption capacities for As(V), ROX, p-ASA and DMA with maximum adsorption capacities of 232.98, 507.97, 379.65 and 158.94 mg g −1 , respectively. The formed Fe O As inner-sphere coordination between arsenic species and the incomplete-coordinated cationic Fe in the MIL-101(Fe) cluster is the primary adsorption mechanism based on FTIR and XPS analysis. Substituent aromatic units in ROX and p-ASA strengthen the adsorption on MIL-101(Fe) through hydrogen bonds and π-π stacking interaction, resulting in higher adsorption capacities far beyond that of As(V) and DMA. The reusability of MIL-101(Fe) is limited by the strong Fe O As coordination. These results confirm MIL-101(Fe) a reliable adsorbent to control the aqueous arsenic species contamination and emphasize the significant role of the chemical structure of arsenic speciation on adsorption performances of MOFs.
研究领域:
环境科学
·
材料科学
·
化学
✓ 已验证
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Bao-Lin Zhang,Wei Qiu,Pan-Pan Wang,Yu-Lei Liu,Jing Zou,Lu Wang,Jun Ma
This study examined the effects of two kinds of iron-trimesic metal-organic frameworks (MOFs) [MIL-100(Fe) and Fe-BTC] on adsorption of Pb(II) and Cd(II). For both materials, adsorption of Pb and Cd nearly approached equilibriums in the initial 2 min with high pseudo-second-order kinetics rate constants (0.895 g·mg −1 ·min −1 for Pb and 1.416 g·mg −1 ·min −1 for Cd). Both materials showed better adsorption performance with the increase of solution pH (from 2 to 7). Adsorption processes were endothermic, entropy-increased and spontaneous. The higher enthalpy change ( Δ H 0 ) and entropy change ( Δ S 0 ) values for Cd adsorption reflected the more difficult adsorption of Cd compared with Pb, which is related with more negative hydration enthalpy ( Δ H hyd Θ ) and larger ionic radius of Cd. Multilayer adsorption phenomena appeared with no maximum adsorptive capacity observed. Both Langmuir-Freundlich and Freundlich-BET models could well describe isotherms. Multilayer adsorption may be attributed to the formation of inner-sphere complexation and outer-sphere complexation. Bockris-Devanathan-Muller (BDM) electrical double layer theory was used for illustrating adsorption mechanism. The fixed-bed adsorption experiments with Fe-BTC showed outstanding elimination performance in initial operating period (>99.8% for Pb and >99.6% for Cd), with effective filtration volume of 980 mL for Pb and 300 mL for Cd. Recyclability test showed that Fe-BTC could be well regenerated by ethylenediamine tetraacetic acid disodium salt (EDTA-2Na). This study showed that MIL-100(Fe) and Fe-BTC are potential for practical heavy metal removal applications.
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
Small
·
2024
·Vol. 20
·期 34
·2401024
·
IF 13
Yuquan Wu,Da Lei,Jiawen Li,Ying Luo,Yuwan Du,Shi Zhang,Baiyi Zu,Yuhong Su,Xincun Dou
Exposing different facets on metal-organic frameworks (MOFs) is highly desirable to enhance the performance for various applications, however, exploiting a concise and effective approach to achieve facet-controlled synthesis of MOFs remains challenging. Here, by modulating the ratio of metal precursors to ligands, the facet-engineered iron-based MOFs (Fe-MOFs) exhibits enhanced catalytic activity for Fenton reaction are explored, and the mechanism of facet-dependent performance is revealed in detail. Fully exposed (101) and (100) facets on spindle-shaped Fe-MOFs enable rapid oxidation of colorless o -phenylenediamine (OPD) to colored products, thereby establishing a dual-mode platform for the detection of hydrogen peroxide (H 2 O 2 ) and triacetone triperoxide (TATP). Thus, a detection limit as low as 2.06 n m is achieved, and robust selectivity against a wide range of common substances (>16 types) is obtained, which is further improved by incorporating a deep learning architecture with an SE-VGG16 network model, enabling precise differentiation of oxidizing agents from captured images. The present strategy is expected will shine light on both the rational synthesis of nanomaterials with modulated morphologies and the exploitation of high-performance trace chemical sensors.
研究领域:
材料科学
·
化学传感
·
纳米技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Yi Han,Mingjie Huang,Wei Xiang,Chen Wang,Yongjie Li,Xiaohui Wu,Juan Mao,Tao Zhou,Hong Li,Deming Wu
Fe-based metal–organic frameworks (MOFs) are popular in activating oxidants e.g·H 2 O 2 and persulfate (PS) for degrading recalcitrant organic substances, generally regarded with a simple interfacial efficient iron cycle. This study has revealed that a novel two-steps single-electron transfer mechanism would occur initially to activate the rapid degradation 4-chlorophenol (4-CP) in the MIL-88B(Fe)/H 2 O 2 system (88B/H 2 O 2 system). The degradation of 4-CP was acidic favorable (pH 0 ≤ 6.0) and could be divided into two reaction stages, i.e., initial lag phase (0–10 min) and following rapid decay phase (10–50 min). In the first stage, H 2 O 2 was slowly activated on the surface of 88B to form superoxide radical (O 2 •– ), which would lead to the accumulation of the key intermediate hydroquinone (HQ) through reducing 4-CP. Afterwards, HQ could reductively dissolve iron ions which would lead to the subsequent efficient homogeneous Fenton reaction for the rapid oxidation of 4-CP by hydroxyl radical (•OH) in the following rapid decay phase. It was interesting to note that specific aromatic compounds, which would form reductive benzenediols intermediates by O 2 •– , could be efficiently degraded in the 88B/H 2 O 2 system. The result of this study is expected to provide a new insight for understanding the catalytic oxidation process based on MOFs, and its application if possible.
研究领域:
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
DALTON TRANSACTIONS
·
2017
·Vol. 46
·期 47
·16525-16531
·
IF 4.029
Fu-hua Wei,Ding Chen,Zhao Liang,Shuai-qi Zhao,Yun Luo
Fe-Based metal–organic frameworks (Fe-MOFs) were prepared with trimesic acid and FeSO4·7H2O via a microwave-assisted ball milling approach. The structure and thermal stability of the as-prepared Fe-MOFs were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), Fourier transform infrared spectrometry (FTIR), X-ray photoelectron spectroscopy (XPS), and thermogravimetric analysis (TGA). When used to degrade 20 mg L−1 hexavalent chromium in aqueous solution, the Fe-MOFs were found to completely reduce a 100 mL solution within 120 min under natural light and a 400 mL solution within 90 min under Xe lamp irradiation. Under natural sunlight, 98% of the Cr(VI) was removed from a 40 mL solution after 40 min.
研究领域:
环境化学
·
材料科学
·
纳米技术
·
污染控制
·
光催化
·
水处理
✓ 已验证
DOI
高影响因子
NANOTECHNOLOGY
·
2024
·Vol. 35
·期 42
·425702
·
IF 2.9
Rui Li,Huilin Hu,Furong Xiong,Xiang Xue,Minqi Wu,Xuan Zuo,Wang Zhang,Xiangliang Pan
Efficient metal–organic frameworks (MOFs) photocatalytic bactericidal catalysts are urgently needed in water purification. Herein, a Fe-MOF (MIL-88B-NH2(V1Fe5) with promoted electron transport was achieved by vanadium (V) ions doping and V/Fe ratio optimization, showing excellent photocatalytic bactericidal activity against E. coli under visible light irradiation (99.92%). The efficient antibacterial mechanism, V as a Ti-like mediator boosting electronic transmission in MIL-88B-NH2(V1Fe5), was revealed by its band structure, transient photocurrent, electrochemical impedance spectroscopy, and scavenger quenching experiments. The enhancement of photocatalytic bactericidal performance of Fe-MOFs by V–ion-doping was confirmed by two other Fe-MOFs, MIL-53-NH2(V1Fe5) and MIL-101-NH2(V1Fe5), with the same metal ions and ligands, both of which have higher performance than the corresponding undoped MOFs. Among them, MIL-88B-NH2(V1Fe5) exhibits the highest photocatalytic bactericidal activity due to its suitable metal clusters ([M(μ3-O)] cluster) and topological structure (three-dimensional rhomboid network structure). This work demonstrated the amplification effect of V ion doping on electron transport in Fe-MOFs photocatalysts.
研究领域:
材料科学
·
环境科学
·
化学
·
光催化
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）