JOURNAL OF CHROMATOGRAPHY A
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2026
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IF 4
Xueyun Wei,Lanrui Yang,Zhuomin Zhang,Gongke Li
Trace disinfection by-products (DBPs) in aquatic products may have serious impact on human health via direct or indirect consumption. However, the accurate and sensitive quantification of trace chlorophenol DBPs in complex aquatic products still remains a great challenge. In this work, the defective MIL-101(Fe)-NH 2 enrichment medium was prepared for developing a selective membrane solid phase extraction (M-SPE) technology for quantifying trace chlorophenol DBPs in fish, coupled with high performance liquid chromatography-ultraviolet-visible spectroscopy (HPLC-UV). The established analytical method showed good selectivity, sensitivity and accuracy, achieving the limits of detection from 0.03 to 0.15 ng/mL and the recovery from 80.0% to 117%, achieving sensitivity comparable to that of HPLC-mass spectrometry (MS)-based methods. The validated method was successfully applied to quantify chlorophenol DBPs in grass carp and crucian carp, offering a selective and sensitive alternative for monitoring chlorophenol DBPs in fish, with practical advantages for routine analysis via compatibility with widely available HPLC-UV.
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JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
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2026
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IF 4.4
Bingkun Liu,Juncheng Guo,Ziyang Liang,Yuhan Yang,Beibei Liu,Bing Han,Yonghui Zhang
NH 2 -MIL-101(Fe)/few-layer Ti 3 C 2 Schottky heterojunctions are constructed. • NH 2 -MIL-101(Fe)/Ti 3 C 2 composite shows higher photocatalytic activity for Cr(VI) removal. • The Schottky heterojunctions boost the separation of photogenerated charges. • The photogenerated electrons and •O 2 − dominate the Cr(VI) reduction process. The limited charge transfer efficiency of single-component semiconductor photocatalysts remains a critical bottleneck restricting the photocatalytic elimination of harmful pollutants. Here, NH 2 -MIL-101(Fe) nanoparticles are anchored onto few-layer Ti 3 C 2 nanosheets via electrostatic self-assembly to construct NH₂-MIL-101(Fe)/Ti 3 C 2 heterostructure. The few-layered 2D Ti 3 C 2 supplies abundant adsorption and catalytic active sites. Furthermore, benefiting from the Schottky junction and the superior conductive feature of Ti 3 C 2 MXene, the separation and transport of photoinduced carriers are remarkably promoted in the NH 2 -MIL-101(Fe)/Ti 3 C 2 . Accordingly, the optimized NH 2 -MIL-101(Fe)/Ti 3 C 2 –10% sample can remove 95.7% of Cr(VI) after 150 min of visible-light irradiation and still exhibits favorable reusability after three cycles. The electrons and •O 2 − are confirmed as the primary active species driving Cr(VI) reduction. Combined with comprehensive characterizations, a plausible photocatalytic mechanism of Cr(VI) reduction is put forward. This work offers fundamental guidance for developing MXene-based Schottky heterostructures toward improved photocatalytic activity.
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Results in Chemistry
·
2025
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IF 4.2
Wei Zhang,Ku Yu,Wang Aihe
In this study, pyridine-a representative nitrogen-containing heterrocylic contaminant in coal chemical wastewater-was targeted for photocatalytic degradation. We developed a novel ternary composite photocatalyst through the in-situ integration of layered double hydroxide (LDH) and iron-based metal-organic framework (MIL-101(Fe)) with lanthanum‑iron co-doped TiO 2 via hydrothermal synthesis. These contaminants are characterized by high environmental persistence, low biodegradability, and potential teratogenic/carcinogenic risks. The synthesized LDH/MIL-101(Fe)/La-Fe-TiO 2 composite was systematically characterized using scanning electron microscopy (SEM), UV–Vis diffuse reflectance spectroscopy (DRS), X-ray photoelectron spectroscopy (XPS), and Brunauer-Emmett-Teller (BET) analysis. Key findings revealed that: (1) The composite architecture achieves an exceptional specific surface area of 168.96 m 2 /g through synergistic LDH/MIL-101(Fe) integration; (2) La–Fe co-doping effectively extends the photoresponse threshold of TiO 2 to the visible-light region. Under optimized conditions (25 °C, 300 rpm agitation, 400 W irradiation), the system achieved 96.1 % pyridine degradation (initial concentration: 100 mg/L) within 4 h, following pseudo-first-order kinetics (R 2 = 0.99). Remarkably, the catalyst maintained 94.5 % efficiency after five consecutive cycles, demonstrating superior stability. Mechanistic investigations combining GC–MS analysis, electron paramagnetic resonance (EPR) detection, and radical quenching tests identified the reactive species activity sequence as ∙ h + > ∙ OH > O 2 − , ultimately elucidating the complete pyridine mineralization pathway.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2026
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IF 5.4
Bolong Liang,Hongbin He,Xi Zhu,Shu-Xuan Liang
The residue of oxytetracycline hydrochloride (OTC) has emerged as a significant concern impacting both human health and the ecological environment. Photocatalysis has a good application prospect in the treatment of antibiotic pollution due to its advantages of lost cost, high efficiency and environmental friendliness, and the development of photocatalyst has become crucial for achieving effective photocatalytic degradation. The preparation of Z-scheme heterojunction is regarded as an effective strategy to enhance photocatalytic activity. Herein, double Z-scheme MIL-101(Fe)@AgI@TPA/TPB heterojunction materials were innovatively designed and successfully prepared. MIL-101(Fe)@AgI@TPA/TPB could achieve 95.09 % OTC removal efficiency under visible light irradiation in 70 min. The investigation of photoelectric properties and mechanisms revealed that MIL-101(Fe)@AgI@TPA/TPB had a broader range and enhanced ability for light absorption, along with a narrower band gap. It was determined that ·O 2 - and ·OH were the primary active species involved in the photocatalysis process. The mechanism of double Z-scheme heterojunction capable of facilitating efficient photocatalytic degradation was proposed, and the intermediate products and decomposition pathways of OTC in the photocatalytic degradation process were analyzed. This study provides innovative insights into practical application through the prepared double Z-scheme heterojunction photocatalyst aimed at remediating OTC contamination in water environments.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2026
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IF 9.1
Jing Li,Jinquan Wan,Yan Wang
In peroxymonosulfate (PMS)-based advanced oxidation processes (AOPs), the precise regulation of reactive oxygen species (ROS) generation pathways is a core challenge for achieving selective degradation of target pollutants. In this study, we propose an electronic effect-guided ligand functionalization strategy by systematically introducing electron-donating (-OH, -NH 2 ) and electron-withdrawing (-NO 2 ) groups into the MIL-101 (Fe) framework, thereby establishing a quantitative structure-activity relationship between the electronic structure, coordination environment of Fe centers and ROS generation. The results demonstrate that electron-donating groups (-OH, -NH 2 ) significantly promote the non-radical pathway dominated by singlet oxygen ( 1 O 2 ), achieving efficient degradation of the electron-rich pollutant sulfamethoxazole (SMX) with removal efficiencies of 93.0% and 91.2%, respectively. Notably, the 1 O 2 contribution rate in the MIL-101(Fe)-OH system reached 95.07%. Correlation analysis reveals a significant positive correlation between C O content and 1 O 2 contribution. Combined experimental characterization and DFT calculations indicate that the selective generation of ROS results from the synergistic effects of multiple factors, including electronic structure, adsorption energy, and charge transfer. Electron-donating groups enhance the electron density at the Fe center, elongate the Fe O bond length, and optimize PMS adsorption energy, thereby promoting the self-disproportionation of the key SO 5 •- intermediate to generate 1 O 2 . This work highlights the promotional role of functional group electronic effects on the non-radical pathway, elucidates the core mechanism governing ROS generation, and provides a mechanistic framework for the design of highly selective Fenton-like catalysts. Environmental implication This study employs an electron-effect-guided ligand functionalization strategy to systematically reveal the structure–activity relationship between the electronic structure and coordination environment of metal nodes in Fe-MOFs and the ROS generation. The electronic effects of functional groups enable the precise regulation of ROS, and electron-donating groups significantly promote nonradical pathways, thereby achieving efficient degradation of the electron-rich contaminant sulfamethoxazole. This work highlights the promotion of nonradical pathways by the electronic effects of functional groups, clarifies the core mechanism governing ROS generation, and provides new insights for the design of highly efficient and selective catalysts.
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JOURNAL OF CHROMATOGRAPHY A
·
2026
·
IF 4
Lin Lv,Hongmei Liu,Tao Song,Yan Zhao
Given the extensive use of amphenicol antibiotics and their potential adverse effects on human health, the development of simple and highly sensitive detection methods is essential to ensure food safety. In this work, a novel and highly efficient magnetic sorbent based on β-cyclodextrin-modified magnetic multi-walled carbon nanotubes functionalized with MIL-101(Cr) (Fe 3 O 4 @β-CD@MWCNTs@MIL-101(Cr)) was developed and combined with ultra-high-performance liquid chromatography-mass spectrometry (UHPLC-MS/MS) to achieve highly sensitive detection of three amphenicol antibiotics (chloramphenicol, thiamphenicol, and florfenicol) in honey samples. The key factors influencing extraction efficiency in the magnetic solid-phase extraction process were identified using the Plackett-Burman experimental design, whereas the optimal experimental conditions were determined through Box-Behnken design-based response surface methodology optimization. Under these optimized conditions, favorable linear relationships for amphenicol antibiotics were observed within the concentration range of 0.5–250 ng mL − 1 (R 2 ≥ 0.9951). The method exhibited detection limits of 0.04–0.07 μg kg − 1 . Recovery rates ranged from 83.2% to 97.9%, with intra-day and inter-day precisions both below 7.2%. This method provides an efficient tool for monitoring amphenicol antibiotics in complex matrices.
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CHEMOSPHERE
·
2023
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IF 8.8
Gangya Cheng,Chen Yuan,Wansheng Ruan,Ben Ma,Xinyu Zhang,Xinjing Yuan,Zhihui Li,Dan Wang,Fei Teng
In this work, Fe-based metal-organic frameworks (Fe-MOFs) are prepared by a simple solvothermal method, in which acetic acid/N, N-dimethylformamide (HAc/DMF) mixture solvents are employed to regulate the particle morphology, exposed facets and ligand defects. At HAc/DMF = 0/50, 5/45 and 8/42 (volume ratio), the irregular particles (MIL-53(Fe)), elongated icosahedrons (5H-MIL-101(Fe)) and icosahedrons (8H-MIL-101(Fe)) are obtained, respectively. Under visible light irradiation (λ > 420 nm) and the addition of sodium persulfate (PS), 5H-MIL-101(Fe) shows the highest degradation activity for tetracycline (TC). Specifically, 80% of TC has been removed by 5H-MIL-101(Fe) within 25 min, and the degradation kinetics rate is 3.03 times higher than that over MIL-53(Fe). The improvement of catalytic activity is mainly attributed to the active facets exposed and ligand defects of 5H-MIL-101(Fe). Density functional theory (DFT) calculation further confirms that the active facets exposed and ligand defects of 5H-MIL-101(Fe) favor the adsorption and activation of PS, benefiting the generation of •SO 4 − . Besides, a probable degradation pathway of TC is proposed based on trapping experiments and liquid chromatography-mass spectrometry (LC-MS) test. Furthermore, the toxicities of intermediates are predicted by the quantitative structure-activity relationship (QSAR) mathematical model. This work demonstrates that visible light enhanced PS activation (Vis-PSA) can more effectively degrade organic pollutants, and this work also provides a simple strategy to precisely regulate ligand defects and actively exposed facets of Fe-MOFs to enhance the adsorption and activation of PS.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2023
·
IF 5.2
Xiao-Ying Li,Wen-Qing Ding,Pan Liu,Lei Xu,Ming-Lai Fu,Baoling Yuan
The p -arsanilic acid ( p -ASA) and roxarsenic (ROX) are typical organic arsenic compounds (OACs), which can be evolved into highly poisonous inorganic arsenic species in the aqueous solution. Herein, a magnetic MOFs-based composite of Fe 3 O 4 /MIL-101 was successfully obtained by a stepwise solvothermal method and further used in the adsorption of p -ASA and ROX. The structural and physicochemical characteristics of Fe 3 O 4 /MIL-101 were firstly investigated in detail. It was found that Fe 3 O 4 microspheres were evenly embedded on the polyhedral MIL-101 surface after the solvothermal process and exhibited a strong superparamagnetic property. After adsorption, a simple external magnetic field can be used to quickly separate the composite from the aqueous solution. The adsorption experiments indicated that the composite is an excellent adsorbent with maximum adsorption capacities of 683.44 and 946.57 mg·g −1 for p -ASA and ROX, respectively. In addition, the effects of composite dosage, initial pH and co-existing anions on the adsorption efficiency were investigated. The main adsorption mechanism consists of the existence of hydrogen bonding , π-π stacking and As-O-Fe coordination between Fe 3 O 4 /MIL-101 composite and OACs. We believe that this study would be very meaningful to promote the application of magnetic MOFs based composites for effective adsorption for OACs in the environmental remediation.
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POLYHEDRON
·
2022
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IF 2.975
Chunqing Wang,Na Xia,Siming Zhu,Lin Chen,Liang Chen,Zhendong Wang
In this study, α- l -rhamnosidase was immobilized on magnetic Fe 3 O 4 /MIL-101 (Cr) nanoparticles using MIL-101(Cr) as precursor by crosslinking method. The crosslinking agent concentration ratio and crosslinking time were EDC/NHS 1:1 and 2 h, respectively. The immobilized materials were characterized by FT-IR, XRD, SEM and VSM. The saturation magnetization of the prepared magnetic nanoparticles was 46.2 emu/g. The optimum pH and temperature of immobilized enzyme were 6 and 60 °C. The application of immobilized enzyme in the preparation of hesperidin dihydrochalcone glucoside (HMGDC) by hydrolysis of hesperidin dihydrochalcone (HSDDC) was studied. The results showed that immobilized enzyme had better temperature resistance, repeatability and stability than free enzyme. The immobilized enzyme activity was 293.55 U/g, and the recovery was 116.03%. After treatment at 60 °C for 4 days, the enzyme activity remained at 24.6%. The conversion rate of HSDDC reached 93.1%.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
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IF 9.965
Yichen Jiang,Dazhi Li,Yifei Zhao,Jianmin Sun
Hydrogen bond donor functionalized poly(ionic liquids) were incorporated into MIL-101 framework for synthesis of composites PIL-R@MIL-101 (R = COOH, OH, NH 2 ). The effect of different hydrogen bond donors on CO 2 -epoxide cycloaddition reaction was discussed through XPS, NH 3 -TPD characterizations. Thereinto, PIL-COOH@MIL-101 showed efficient catalytic performance in the cycloaddition reaction of CO 2 and epichlorohydrin , 92.7% substrate conversion was obtained under 70 °C, 1.0 MPa, cocatalyst- and solvent-free conditions for 2.5 h. The improved activity was benefited from the synergistic effects of Lewis acidic Cr centers, carboxyl group, and nucleophilic Br - , together with the high surface area (1178 m 2 /g), and good CO 2 affinity. In addition, PIL-COOH@MIL-101 also showed facile recovery method by easy centrifugation and good recycling stability. Considering the good CO 2 affinity, excellent catalytic performance in CO 2 cycloaddition reaction, better thermal and recycling stabilities, the facilely prepared functionalized poly(ionic liquid)@MIL-101 composite would exhibit promising application prospect in CO 2 capture and conversion.
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2021
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IF 5.455
Jingjing Zhu,Huaqiang Chen,Lan Wang,Engang Fu,Jianping Wu,Qilei Zhang,Lirong Yang,Gang Xu
A composite hollow mesoporous MIL-101@Pd@ZIF-8-30min (HM-MIL@Pd@ZIF-30min) nanocatalyst with hollow core and stable shell was developed in this study. Hollow mesoporous MIL-101(HM-MIL) was hydrothermally synthesized and employed as the supports of Pd nanoparticles by adopting a facile HM-MIL-template strategy to make ZIF-8 crystals uniformly overgrew on HM-MIL-101@Pd microcrystal cores. The obtained core-shell catalyst possessed hollow mesoporous structure, and the shell layer of ZIF-8 had additional advantages of abundant Lewis basic sites for heterogeneous racemization reaction. Compared with unmodified HM-MIL@Pd and solid MIL-101(Cr)@Pd@ZIF-8 (S-MIL@Pd@ZIF-8), HM-MIL@Pd@ZIF-8-30min had higher racemic chemical activity (conv. 99%) and selectivity (sel. R-amide 94%) in one-pot dynamic kinetic resolution (DKR) reaction system of rac -1-phenethylamine. The catalyst showed excellent stability, and the conversion and selectivity reached 95% and 93% respectively after ten catalytic cycles.
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Energy & Environmental Materials
·
2021
·Vol. 6
·期 1
·e12254
·
IF 15.122
Ailin Li,Jian Xiong,Ye Liu,Liming Wang,Xiaohong Qin,Jianyong Yu
MIL-101(Cr) is a promising moisture absorbent for solar-driven water harvesting from moisture to tackle the worldwide water shortage issue. However, the MIL-101(Cr) powder suffers from a long ab/desorption cycle due to the crystal aggregation caused by its inherent powder properties. Here, we demonstrate a MIL-101(Cr) nanofibrous composite membrane with a nanofibrous matrix where MIL-101(Cr) is monodisperse in the 3D porous nanofibrous matrix through a simple spray-electrospinning strategy. The continuous porous nanofibrous matrix not only offers sufficient sites for MIL-101(Cr) loading but also provides rapid moisture transport channels, resulting in a super-rapid ab/desorption duration of 50 min (including an absorption process for 40 min and a desorption process for 10 min) and multicycle daily water production of 15.9 L kg −1 d −1 . Besides, the MIL-101(Cr) nanofibrous composite membrane establishes a high solar absorption of 92.8%, and excellent photothermal conversion with the surface temperature of 70.7 °C under one-sun irradiation. In addition, the MIL-101(Cr) nanofibrous composite membrane shows excellent potential for practical application due to its flexibility, portability, and use stability. This work provides a new perspective of shortening MOF ab/desorption duration by introducing a porous nanofibrous matrix to improve the specific water production for the solar-driven ab/desorption water harvesting technique.
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