FOOD CHEMISTRY
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2024
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IF 8.5
Mengyue Gao,Qiao Chen,ZhiHao Li,YiFang Zhan,LiHua Wang,Ting He,Qi Yao,Fengmei Jin,Jiming Hu
A SPE-SERS method was developed for the detection of several antibiotic residues in dairy products. Gold nanoparticles (Au NPs) encapsulated with an ultrathin Cr-MIL-101 shell (Au@Cr-MIL-101 NPs) have been synthesized, and the thickness of Cr-MIL-101 shell can be precisely controlled to 3 nm. As a superior solid phase extraction (SPE) adsorbent, Cr-MIL-101 acts as a shell layer to effectively enrich antibiotics within the localized surface plasmon resonance (LSPR) field of Au NPs, which enhances the SERS signal and eliminates background interference. The method can achieve highly sensitive and high-throughput detection for tetracycline hydrochloride, sulfapyridine and benzylpenicillin sodium in dairy products, and the detection limits (LOD) are as low as 2.237, 2.644 and 4.662 ppb respectively. The recoveries of antibiotic residues in spiked dairy products ranged from 72.31 % to 146.7 % with matrix effects (ME) of −15.13 % to 28.68 %. Thus, this method holds significant promise for rapid detection of antibiotics in milk.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
·
IF 24.319
Shihui Wang,Yuzhou Xia,Guiyang Yan,Meixia Chen,Xuxu Wang,Ling Wu,Ruowen Liang
Inspired by the concept of frustrated Lewis pairs (FLPs) from homogeneous catalysis, an organic supramolecular bridged metal-organic frameworks (MOFs) heterojunction, i.e., a perylene-3,4,9,10-tetracarboxylic diimide@MIL-125(Ti)-NH 2 (denoted PDI@MTi) composite is successfully fabricated via a two-step synthesis method. Experimental characterisations and theoretical calculations reveal that in the obtained “TiO 5−x -ligand-PDI” FLPs, the unsaturated Ti-O clusters function as a Lewis acid to accept photogenerated electrons, and the PDI sites act as a Lewis base to capture photogenerated holes. With the unique structure characteristics, the PDI@MTi shows excellent photocatalytic activity toward the disinfection of Staphylococcus aureus and Cr(VI) reduction, with 1.0- and 10.3-fold enhancements, respectively, compared with unadorned MTi. The synergic effects of the micro polarisation field, multiple active sites, and a C-N bonded interface contributed to photoactivity enhancement. This work demonstrates the potential of using MTi as a platform for constructing FLPs-containing heterogeneous photocatalysts and provides new strategies to control carrier separation.
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CHEMICAL ENGINEERING SCIENCE
·
2026
·
IF 5.1
Yingnan Ma,Zixuan Guo,Juan Chen,Shuyan Meng,Zijian Zhang,Jihong Tian,Yanxin Hu,Yijun Fang,Yawen Zhu,Panliang Zhang
High-temperature proton exchange membranes had attracted considerable interest for electrochemical devices such as fuel cells. However, it remained challenging to simultaneously achieve high proton conductivity, effective acid retention, and robust dimensional stability. To address the limitations of conventional filler incorporation, which was insufficient to realize both efficient acid utilization and the construction of continuous proton-conduction networks, we developed a PBI-based mixed-matrix membrane (MMMs) via the in-situ growth of MIL-101(Fe). The in-situ introduced MIL-101(Fe) not only formed a well-dispersed MOFs framework with excellent interfacial compatibility, but also reconfigured the spatial distribution and physicochemical state of phosphoric acid within the membrane, transforming it from disordered accumulation into a continuous hydrogen-bonded pathway for cooperative proton transport. As the extent of MIL-101(Fe) in-situ growth increased, the acid distribution became more uniform, the proton-conduction pathways became more interconnected, the transport resistance was significantly reduced, and the conductivity was markedly enhanced. Meanwhile, the confinement effect of the MOFs channels and their interfacial nanodomains on phosphoric acid effectively suppressed acid loss and substantially improved the dimensional stability of the membrane. This study demonstrated that in-situ grown MIL-101(Fe) not only increased acid accommodation, but more importantly enabled microenvironment regulation and reconstruction of the proton-transport network, thereby providing new insight into the design of high-performance and durable high-temperature proton exchange membranes.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2026
·
IF 8.3
Xuan Zhou,Lei Yuan,Zongbao Sun,Wen Zhang
Residual organophosphorus pesticides (OPs) frequently contaminate farm products, such as vegetables, and consequently threaten food safety. Herein, we present an enzyme-regulated dual-emission probe, MIL-53-OPH@S-S-AuNCs, for synchronous OPs hydrolysis and fluorescence determination. The probe, containing NH 2 -MIL-53(Al), organophosphorus hydrolase (OPH), and disulfide-functionalized Au nanoclusters (S-S-AuNCs), thus provides two emissive outputs (F 427 and F 655 ). Specifically, an OPH-assisted hydrolysis route is designed, where OPs are converted into class-informative products, including p-nitrophenol (PNP) and thiol/thiolate species (R-SH/S - ). PNP induces pronounced quenching of the blue emission (F 427 ) via resonance energy transfer, while sulfur-containing products perturb the disulfide-crosslinked state of S-S-AuNCs and attenuate the red emission (F 655 ). Stepwise optimizations are performed to promote efficient catalytic conversion and stable dual-channel readout, where quenching time, pH, and temperature are tuned to achieve pleasurable sensing conditions. This method provides log-linear quantification for OPs in a wide range of 6.5 × 10 −6 ∼20 μg mL −1 , with an impressive limit of detection of 3.4 × 10 −6 μg mL −1 . The proposed method is further validated by natural sample analyses and recovery tests in real vegetables, giving relative errors of 4.2∼8.6% and recoveries of 96.2∼105.2%.
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Journal of Environmental Sciences
·
2026
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IF 6.5
Mengqi Zhong,Hongrui Ma,Chao Zhu,Tingting Qu,Wenjie Quan
● The differences in the adsorption mechanisms of MIL-101(Fe) for small molecular ligands, larger molecular ligands, and mixed-ligand complexes were investigated. ● The adsorption capacity of MIL-101(Fe) for TA-Cr(Ⅲ) was superior to that of other ligands, with a maximum adsorption amount reaching 183.15 mg/g. ● The adsorption competitive of TA-Cr(Ⅲ) is stronger than that of EDTA-Cr(Ⅲ) and TA-EDTA-Cr(Ⅲ) in the mixed solution. ● The order of binding affinities for different interactions was clarified by combining DFT calculations. The ubiquity of diverse organic-Cr(Ⅲ) complexes in industrial effluents poses a significant challenge to water remediation due to their high stability and complex competitive behaviors. In this study, MIL-101(Fe) was employed to decipher the differential adsorption behaviors and mechanisms of single and co-existing Cr(Ⅲ) complexes, specifically targeting natural (Tannic acid (TA)) and anthropogenic (EDTA) ligands. The experimental results revealed a distinct selective hierarchy as TA-Cr(Ⅲ) > free Cr(Ⅲ) > EDTA-Cr(Ⅲ) > TA-EDTA-Cr(Ⅲ), with values of 183.15, 134.05, 93.02, and 73.80 mg/g, respectively. Among them, TA-Cr(Ⅲ) demonstrated an extremely strong adsorption capacity. Kinetic and isotherm analyses confirmed a chemisorption-dominated process. Crucially, the competitive mechanism was elucidated by integrating spectroscopic characterization with Density Functional Theory (DFT) calculations. The results revealed that while electrostatic interactions drive the initial approach, the specific affinity of phenolic hydroxyl groups in TA towards the Fe-clusters of metal organic frameworks (MOFs), combined with strong π-π stacking interactions, provides an advantage for TA-complexes. The differences of organic-metal complexes were revealed through analysis of electrostatic potential, frontier molecular orbitals and binding energy. This work provides a fundamental understanding of ligand-dependent competitive adsorption, offering a theoretical basis for the selective removal of complexed heavy metals in realistic aquatic environments. Download: Download high-res image (308KB) Download: Download full-size image
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ChemSusChem
·
2026
·Vol. 19
·期 7
·e202502250
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IF 5.9
Junjie Zhang,Jingai Shao,Liwen Fu,Zhong Lin,Xiong Zhang,Shihong Zhang,Haiping Yang,Hanping Chen
Developing biomass-based solid acid catalysts and converting biomass-derived molecules into high-value chemicals has a dual promoting effect on the high-value utilization of waste biomass. This study introduces a groundbreaking one-pot hydrothermal strategy integrating biomass with MIL-101(Cr) precursor to fabricate hierarchical carbon-based catalysts for the highly efficient and selective dehydration of xylose to furfural, achieving 67.2%–72.0% furfural yield (a 33% enhancement over conventional biomass-derived catalysts) under optimized conditions (180°C, 3 h) in a toluene/water biphasic system. The modified hydrochar exhibits an ultra-high surface area of 2119.3 m 2 /g, abundant dual Lewis/Brønsted acid sites, and dispersed Cr 3+ active centers, enabled by synergistic MOF-templated modification engineering and biomass hydrothermal carbonization. Moreover, the correlation between the physicochemical properties and catalytic performance of modified hydrochar was analyzed. Notably, biomass feedstocks with low ash content and high nitrogen content can yield modified hydrochar with more acidic active sites, which exhibits superior catalytic activity. This study provides new ideas for the high-value utilization of waste biomass.
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MICROCHEMICAL JOURNAL
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2026
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IF 5.2
Peng Du,Wei Gao,Zhaohui Huang,Chuqi Jiang,Jiahui Zhang,Dongjun Lv,Luyang Liang,Ling Yin,Xiaolei Zhang,Hongbo Zhang,Huiting Wu
Three-level ET cascade relieves bottleneck. • TMB: 5.8x act., 24.2x eff.. • GSH sensing + redox disruption (depletion/ROS). Nanozyme efficiency is fundamentally constrained by interfacial electron transfer (ET) bottlenecks, yet most strategies overlook the rational design of ET pathways. Herein, a ternary NiMo 6 @MIL-100(Fe)/g-C 3 N 4 nanozyme featuring a hierarchical three-level ET cascade was reported: TMB substrates are preconcentrated onto g-C 3 N 4 via π–π stacking (Level I); electrons transfer from g-C 3 N 4 to Fe 3+ nodes of MIL-100(Fe) through interfacial Fe O C bonds (Level II); and finally cascade into the encapsulated NiMo 6 cluster for H 2 O 2 activation and •OH generation (Level III). This design yields higher activity than binary (1.8-fold) and pristine counterparts (5.8-fold), with a 24.2-fold enhancement in catalytic efficiency for TMB. By leveraging glutathione (GSH) as a specific electron cascade interceptor, a colorimetric assay achieves a detection limit of 0.36 μM with excellent selectivity over structurally similar thiols. Beyond sensing, the same cascade efficiently depletes GSH and induces intracellular ROS bursts in HepG2 cells, disrupting tumor redox homeostasis and highlighting its therapeutic potential and establishing a mechanism-driven paradigm for biosensing and cancer therapy. A hierarchical three-level ET cascade transforms electron bottlenecks into a superhighway for GSH sensing and tumor redox therapy. Download: Download high-res image (274KB) Download: Download full-size image
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RSC Advances
·
2026
·Vol. 16
·期 6
·5501-5514
·
IF 4.6
Lian Yu,Baozi Lu,Zhen Liang,Dabin Wang,Jiarui Lu,Fengyi Wei,Cunzhen Liang
The slow rate of the Fe3+/Fe2+ cycle has decreased the efficiency of photo-Fenton technology for wastewater treatment. Here, a novel GO/MIL-100(Fe)@Fe3O4 heterostructure was constructed by growing Fe3O4 nanoparticles and MIL-100(Fe) onto GO, thus accelerating the Fe3+/Fe2+ cycle and improving catalytic activity, and it was used as a heterogeneous photo-Fenton catalyst for ERY degradation. The catalyst was fully characterized by TEM, XRD, Raman spectroscopy, XPS, N2 adsorption–desorption and UV-vis DRS. The influences of initial solution pH, H2O2 concentration and catalyst dosage on ERY degradation were investigated. Under optimal conditions (initial pH of 4.03, 10.0 mM H2O2, 0.1 g L−1 catalyst), the GO/MIL-100(Fe)@Fe3O4 + H2O2 + vis system removed 97.3% of ERY (0.1 mmol L−1) within 60 min, and the pseudo-first-order rate constant was 0.0575 min−1. Furthermore, the catalyst showed favorable stability, maintaining excellent catalytic activity even after 4 cycles. A possible degradation mechanism of ERY was proposed based on the results of characterization, ERY degradation, and reactive species analysis. Fe3O4, MIL-100(Fe) and GO in the catalyst showed synergistic effects; the photo-induced electrons from MIL-100(Fe) could be immediately transferred to Fe3O4, promoting Fe3+ reduction to Fe2+ in the photo-Fenton reaction. GO in the catalyst could promote electron transfer from MIL-100(Fe) and organics to Fe3O4, significantly promoting the Fe3+/Fe2+ cycle.
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Catalysis Science & Technology
·
2026
·
IF 4.2
Tao Liu,Zhenjie Xu,Guangming Zhou,Simiao Yu,Jie Liu,Jian Ke,Gang Lu
Chemical excess sludge, containing viruses, heavy metals, polycyclic aromatic hydrocarbons, and other components, exhibits high toxicity, making its safe disposal an urgent issue. In this work, MIL-100 (Materials of Institut Lavoisier – 100(iron)) was synthesized using 1,3,5-benzenetricarboxylic acid and iron extracted from excess sludge. Additionally, titanium dioxide was loaded onto MIL-100 via an impregnation–calcination method to form T@MIL-100, and their visible-light-driven photocatalytic activities for methylene blue (MB) degradation were evaluated. The results showed that the synthesized MIL-100 exhibited excellent photocatalytic performance for MB degradation, with a degradation efficiency of 92.44% and a corresponding kinetic constant (kobs) of 0.97612 h−1. The degradation efficiency of MB over 1%T@MIL-100 was enhanced to 98.42%, and the kobs value increased to 1.39943 h−1. Quenching experiments further revealed the catalytic mechanism: h+ was the dominant active species in the MIL-100 system, while ·O2− and h+ primarily contributed to MB degradation in the T@MIL-100 system. This study provides a low-cost, efficient, and sustainable approach to convert excess sludge into functional metal–organic frameworks (MOFs) and further load TiO2. This strategy not only promotes the recycling of residual iron in excess sludge to significantly reduce catalyst costs, but also enhances photocatalytic degradation performance, offering an excellent functional material for MB removal.
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2019
·
IF 4.182
Weina Shi,Yanqing Zhu,Cong Shen,Jifu Shi,Gang Xu,Xiudi Xiao,Runqiang Cao
Thermochemical heat storage based on inorganic salt hydrates is a promising approach to relieve the heat energy supply and demand conflicts, but there exist lots of defects of pure salts when applied to the thermochemical. This paper attempted to use functionalized Metal-Organic Frameworks (MOFs) as the porous matrices to improve the heat storage performance of inorganic salt hydrates. A series of MOFs/CaCl 2 composites based on MIL-101(Cr)-X (X = -NH 2 , –SO 3 H, H, –CH 3 , –F) were successfully synthesized and fully characterized by combining multiple techniques (i.e. powder X-ray diffraction, scanning electron microscopy , energy-dispersive X-ray analysis, N 2 adsorption-desorption, Fourier transform infrared spectroscopy , thermogravimetric and differential scanning calorimetry). The water sorption properties of the series of MOFs/CaCl 2 composites were studied during the hydration process, and a continuous adsorption/desorption experiment was also performed to investigate the cycle stability of the MOFs/CaCl 2 composites. The results show that the hydrophilic MOFs based composites have higher water sorption capacity (0.6 g(H 2 O)/g(sample) for MIL-101(Cr)–SO 3 H/CaCl 2 ) accompanied with higher heat storage density (1274 J/g for MIL-101(Cr)–SO 3 H/CaCl 2 ). Moreover, the series of MOFs all presented excellent cycle performance with little loss after continuous 17 adsorption/desorption cycles.
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Journal of Environmental Sciences
·
2026
·
IF 6.5
Xiaoxia Liang,Zewan Qin,Siwei Zhang,Rong Hai,Lingqing Gu,Xia Yang
30CNQDs@NMT/PMS achieved almost complete degradation of malathion within 30 min simulated sunlight irradiation. • CNQDs was integrated successfully to promote the charge separation efficiency as electron bridges and enhance the adsorption energy of PMS for activation revealed by DFT. • •OH and •SO 4 – were generated to attack the identified sites of malathion computed via Fukui function. • The intermediate products in the photocatalytic process were less toxic than malathion assessed by T.E.S.T. Malathion, an organophosphate pesticide widely used in agricultural fields across the world, has raised environmental concerns due to its persistence and toxicity. Thus, a novel photocatalyst was synthesized by integrating carbon nitrogen quantum dots (CNQDs) onto NH 2 -MIL-125(Ti) (NMT) via a solid-phase thermal polycondensation method. It was demonstrated that CNQDs served a dual function as electron bridges to facilitate charge separation and as peroxymonosulfate (PMS) adsorption activation sites substantially enhancing the photocatalytic activity, which was revealed by Density Functional Theory (DFT). Under simulated sunlight, 30CNQDs@NMT achieved nearly 100 % malathion removal within 30 min via PMS activation, exhibiting 8.1 times higher than NMT. While •OH and •SO 4 – acted as the dominant reactive species to attack the malathion sites. The toxicity of the intermediate products assessed by T.E.S.T. (Toxicity Estimation Software Tool) were much lower than malathion. Moreover, 30CNQDs@NMT performed effectively in real water matrices, demonstrating its potential for practical environmental applications. Download: Download high-res image (233KB) Download: Download full-size image
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2026
·
IF 6.7
Jun-Chuan Wang,Peng-Liang Zhang,Wen-Bo Zhang,Tai-Sen Zhang,Zi-Yan Zhen,Tian-Yu Wang,Xiang-Xiang Jia,Gang Yu
Modulating localized electronic structures and interfacial charge-transfer pathways in metal-organic framework (MOF)-based heterogeneous catalysts remains a critical challenge for achieving efficient and durable advanced oxidation processes. Herein, a highly crystalline S-scheme NH₂-MIL-101(Fe)@DQ-TFP (NM@DT) core-shell heterojunction was constructed through a microwave-assisted MOF-first in situ growth strategy. Distinct from conventional physical assembly, the anthraquinone-based β-ketoenamine covalent organic framework (COF) shell was integrated with the amino-functionalized MOF core through chemically coupled growth and interfacial hydrogen-bonding interactions, generating a robust core-shell interface. This intimate interfacial coupling induces spontaneous electronic redistribution and charge polarization, which are verified by X-ray photoelectron spectroscopy, ultraviolet photoelectron spectroscopy, and density functional theory calculations, thereby providing the electronic basis for an internal electric field-assisted S-scheme charge-transfer pathway. The optimized NM@DT-3 heterostructure exhibits enhanced photocatalytic tetracycline degradation performance, achieving 90.70% removal efficiency within 180 min without external H₂O₂ addition. The core-shell configuration not only promotes interfacial charge separation but also creates a spatially confined catalytic microenvironment, enabling efficient oxygen activation and reactive oxygen species evolution coupled with localized H₂O₂ activation at adjacent Fe centers. Mechanistic investigations reveal that freely diffusing hydroxyl radicals (·OH) make only a minor contribution under the tested conditions, whereas superoxide radicals (·O₂⁻), photogenerated holes (h⁺), and singlet oxygen (¹O₂) participate in TC oxidation. In this reaction network, ·O₂⁻ acts as a key intermediate linking photocatalytic O₂ reduction to both H₂O₂ formation and a proposed h⁺-mediated ¹O₂ generation pathway. The reduced reliance on conventional bulk ·OH-dependent chemistry is consistent with the retained catalytic activity of NM@DT-3 under alkaline conditions, with a TC removal efficiency of 77.74% at pH 10. Meanwhile, the chemically integrated core-shell structure effectively suppresses iron leaching, with only 0.107 mg L⁻¹ Fe released during the photocatalytic process. This work provides new insights into engineering chemically coupled MOF/COF interfaces for regulating interfacial charge migration and ROS evolution, offering an effective strategy for constructing stable photo-self-Fenton catalysts for environmental remediation.
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