CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Yanni Jiang,Zhongjuan Wang,Jianbo Huang,Feng Yan,Ye Du,Chuanshu He,Yang Liu,Gang Yao,Bo Lai
Singlet oxygen ( 1 O 2 ) is an effective reactive oxygen species in disinfection due to its long lifetime and sensitivity to bacteria. This study tried to develop a 1 O 2 dominated process for bacterial inactivation by visible light (vis) photocatalysis assisted by PMS. A novel CuS-modified MIL-101(Fe) (CSMF) photocatalyst was synthesized for the first time. Compared with MIL-101(Fe), CuS-modified MIL-101(Fe) enhanced the photocatalytic performance by increasing absorption of visible light, narrowing down the bandgap and promoting photo carrier separation efficiency. 7.5-log Gram-negative Escherichia coli (E. coli) could be inactivated by Vis/CSMF/PMS system within 40 min, showing much better performance of 3.5-log E. coli inactivated by Vis/PMS system. The Vis/CSMF/PMS system is applicable in a broad pH range from 3.0 to 9.0, remaining quite steady disinfection efficiency after regenerations of the catalyst. Quenching experiments and electron paramagnetic resonance (EPR) analysis demonstrated 1 O 2 was the dominated ROS rather than OH • and SO 4 •− . Three pathways, including photo-generated electrons (e − ) and O 2 dependent pathway, photo-generated holes (h + ) dependent pathway and CSMF enhanced PMS dissociation pathway, were evidenced to responsible for 1 O 2 formation by aeration experiments and specific 1 O 2 fluorescence probe. 1 O 2 in water attacked the bacterial cell membranes first, got inside the cell and up-regulated the level of intracellular ROS, which further led to cell membrane damage and DNA degradation so as to irreversible cell death. In addition, the developed Vis/CSMF/PMS system could also efficiently inactivate gram-positive bacteria Staphylococcus aureus and fecal coliform bacteria in practical wastewater, suggesting its wide applicability as a promising alternative to conventional disinfection process.
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TALANTA
·
2025
·
IF 6.1
Haotian Chen,Zimo Chen,Hanbing Yao,Yujuan Zhan,Binyu Xiao,Shuangshuang Liu,Jiayi Yan,Yifu Li,Chang Shu
Dopamine (DA) is an essential biomarker implicated in the diagnosis of neurological diseases. In this work, we designed a dual-enzyme mimetic activity MIL-101(Fe) that catalyzed specific cyclization reaction between 1,3-dihydroxynaphthalene (NR) and dopamine. As the concentration of dopamine increased, the fluorescence emission of NR at 440 nm was markedly quenched, concomitant with the emergence of a new fluorophore exhibiting enhanced emission at 480 nm and increased absorbance at 462 nm. The ratiometric fluorescence/colorimetric dual-mode detection strategy provided intrinsic self-calibration to effectively mitigate signal variations. Furthermore, a linear correlation was established for ratiometric fluorescence signal across the range of 0.25–35 μM (R 2 = 0.999), and similarly for colorimetric absorbance (R 2 = 0.999). This method provided an accurate, specific, sensitive and high-throughput detection of dopamine in human serum.
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JOURNAL OF SOILS AND SEDIMENTS
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2022
·Vol. 22
·期 7
·2009-2021
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IF 3.536
Liu Quanfeng,Yu Jiang,Jiang Yinying,Zhong Chengwei,Ding Senxu,Zhou Peng,Jin Yuanxiao
Purpose Soil organic matter pollution is a serious threat to the human living environment. The purpose of this paper is to investigate the effect of MIL-101(Fe)/g-C 3 N 4 catalyzed peroxynitrite degradation of 2-chlorophenol in soil and to analyze the reaction mechanism and further to explore the optimal parameters of this reaction system with utilizing the mathematical model. Methods MIL-101(Fe)/g-C 3 N 4 was successfully obtained by hydrothermal synthesis method by growing MIL-101(Fe) on the surface of g-C 3 N 4 to catalyze the degradation of 2-CP (2-chlorophenol) in soil by sodium persulfate. The influence factors on the removal rate of 2-CP were analyzed by the response surface methodology (RSM) and combined with theoretical calculations. RSM can be used to model continuous variable surfaces with less data and determine the optimal level range. Results MIL-101(Fe)/g-C 3 N 4 had a good catalytic performance due to its good catalytic properties and the adsorption of g-C 3 N 4 on 2-CP in the system and made the best removal rate of 2-CP increase to 91.2%. The correlation of model fitting results was significant, and the verification of its optimal parameters yielded results with an error of only 4.1%. Conclusion Further studies revealed that SO 4 •− and • OH were the reactive radicals, and SO 4 •− was the dominant, which impelled Fe 2+ and Fe 3+ to interconvert in the complex system. Possible degradation pathways were derived by analyzing the intermediates. Generally, this experiment provides some ideas for future research of MOFs in soil organic pollutant removal systems. Graphical abstract
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INORGANIC CHEMISTRY
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2024
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IF 4.3
Jingyu Cai,Junjie Shi,Jian Zhang,Xiaoyu Miao,Sen Wang,Longqiang Xiao,Dan Liu,Linxi Hou
Electronic-grade isopropyl alcohol is widely utilized in the cleaning of semiconductors and microelectronic components. Removing ions like Pb2+ is crucial since the presence of impurities may cause degradation of electronics, increased failure rates, and short circuits. Membrane materials offer a number of advantages in the field of adsorption separation; however, the lack of adsorption sites results in limited adsorption capacity. In the current work, guanidino-grafted NH2-MIL-101(Fe) was incorporated into polyvinylidene fluoride (PVDF) to prepare MOF/PVDF mixed matrix membranes (NM/PVDF) for the removal of Pb2+ from isopropanol. Benefiting from the larger specific surface area and more lone electron pairs in the guanidine group, the Pb2+ adsorption capacity of the as-prepared NM/PVDF membrane was 29.4458 mg/g, which was higher than that of the NH2-MIL-101(Fe)/PVDF membrane (20.9306 mg/g) and the pure PVDF membrane (6.7324 mg/g). The NM/PVDF membrane was able to reduce the concentration of Pb2+ from 500 to 86.73 ppb. This work highlights the potential of guanidine-grafted Fe-based MOFs/PVDF membranes as adsorbents for acquisition of electronic-grade solvents.
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Journal of Inorganic and Organometallic Polymers and Materials
·
2023
·Vol. 34
·期 4
·1751-1764
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IF 4
Zhou Zhuyou,Zou Congyang,Wang Yong,Liu Menghe,Ji Yufeng
A one-step solvothermal synthesis technique was employed to fabricate C 60 /MIL-101(Fe) composites. The C 60 /MIL-101(Fe) composites showed a better performance in the degradation of methylene blue (MB) and tetracycline hydrochloride (TCH) when compared to MIL-101(Fe) in the photo-Fenton system, which can be credited to the charge transfer and separation facilitated by the addition of C 60 . Results showed that C 60 /MIL-101(Fe) had the capacity to nearly completely eliminate TCH and MB over a broad pH range. The catalysts demonstrated remarkable catalytic degradation on various organic pollutants and water samples. Through active substance quenching experiments and EPR, it was determined that hydroxyl radical (·OH) is the main factor in the photocatalytic reaction process.
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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
·
2026
·
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 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
·
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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JOURNAL OF CHROMATOGRAPHY A
·
2026
·
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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CHEMOSPHERE
·
2023
·
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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ENVIRONMENTAL RESEARCH
·
2023
·
IF 8.3
Chunyan Hu,Jinke He,Jianjun Liang,Tao Lin,Qiuliang Liu
A novel photo-Fenton catalyst α-Fe 2 O 3 @g-C 3 N 4 @NH 2 -MIL-101(Fe) (FGN) with dual Z-scheme heterojunction was successfully prepared by hydrothermal method to degrade tetracycline (TC). The preparation conditions were optimized by orthogonal test, and the successful synthesis was confirmed by characterization analyses. The prepared FGN showed better light absorption performance, higher photoelectrons-holes separation efficiency, lower photoelectrons transfer resistance, and higher specific surface area and pore capacity compared with α-Fe 2 O 3 @g-C 3 N 4 and α-Fe 2 O 3 . The effects of experimental conditions on the catalytic degradation of TC were investigated. The degradation rate of 10 mg/L TC could reach 98.33% within 2 h when the dosage of FGN was 200 mg/L, and the degradation rate could remain 92.27% after 5 times of reuse. Furthermore, the XRD spectra and XPS spectra of FGN before and after reuse were compared to explore the structural stability and catalytic active sites of FGN, respectively. According to the identification of oxidation intermediates, three degradation pathways of TC were proposed. Through H 2 O 2 consumption experiment, radical-scavenging experiments, EPR results, the mechanism of the dual Z-scheme heterojunction was proved. The improved performance of FGN was attributed to the dual Z-Scheme heterojunction effectively promoting the separation of photogenerated electrons from the holes and accelerating the electrons transfer , and the increase of the specific surface area.
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