PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
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2025
·
IF 7.8
Weitao Kong,Zhongmou Liu,Jinghui Wu,Chenying Wen,Juncheng Yan,Yidi Gao,Guanqiao Li,Xianze Wang,Mingxin Huo
This study investigates the degradation of sulfamethoxazole (SMX), a widely detected and persistent antibiotic in the environment, using a novel photocatalytic system based on MIL-101(Fe) supported Mo single-atom with oxygen vacancies (Mo/Ov-MOF). Anchoring Mo single-atoms into the MOF structure enhances catalytic activity by effectively improving charge separation and reducing electron-hole recombination. The Mo/Ov-MOF efficiently activates peroxymonosulfate (PMS) under visible light, generating singlet oxygen ( 1 O 2 ) as a primary reactive species responsible for SMX degradation. Degradation experiments demonstrated that the degradation efficiency reached 96.8 % in the presence of PMS and visible light. Through quenching and trapping experiments on active species, an in-depth investigation into the source of 1 O 2 was performed, demonstrating the crucial role of holes in the rapid and selective generation of 1 O 2 under visible light. Additionally, the reusability of the Mo/Ov-MOF catalyst was confirmed, maintaining over 70 % degradation efficiency after five cycles. Toxicity assessments indicated that the degradation by-products exhibited significantly lower toxicity than the parent compound SMX, thus mitigating potential ecological risks. The mechanistic insights reveal that oxygen vacancies and Mo single-atom enhance electron transport and facilitate efficient PMS activation, ultimately leading to effective pollutant degradation. The findings underscore the potential of the Mo/Ov-MOF photocatalytic system for practical applications in wastewater treatment, particularly for removing persistent organic pollutants from aquatic environments.
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JOURNAL OF SEPARATION SCIENCE
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2025
·Vol. 48
·期 3
·e70118
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IF 2.8
Yu Jiang,Hong Pan,Menghong Xie,Huifeng Deng,Guihua Ruan,Yipeng Huang
In this study, magnetic Fe 3 O 4 -coated metal-organic framework composites, CONH 2 -MIL-101(Cr)/Fe 3 O 4 , were synthesized by depositing Fe 3 O 4 particles on the surface of amidated MIL-101(Cr). The scanning electron microscope images show that the MIL-101(Cr) crystals were uniformly coated by Fe 3 O 4 particles. The magnetic hysteresis curve of CONH 2 -MIL-101(Cr)/Fe 3 O 4 reveals a saturated magnetization value of 23.47 emu/g. The water contact angle decreases from 61.00° to 12.88° after amidation and Fe 3 O 4 coating. The magnetic solid-phase extraction (MSPE) efficiency of CONH 2 -MIL-101(Cr)/Fe 3 O 4 for benzoic acid derivatives was studied. Under optimal conditions, the adsorption and desorption processes can be completed within 5 min, and the maximum adsorption capacity to protocatechuic acid (PCA) and vanillic acid (VA) is 10.31 and 17.30 mg/g. Coupling the MSPE with high-performance liquid chromatography-ultraviolet detection, the detection limit for PCA and VA was 0.29 and 0.58 ng/mL, respectively. The mean recoveries of PCA and VA in spiked samples ranged from 82.85%–91.27% with relative standard deviations lower than 0.33%–5.33%. This study provides inspiration for the fabrication of novel magnetic sorbents, and a reliable method for the adsorption and analysis of benzoic acid derivatives.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2022
·
IF 11.357
Huimin Zhou,Ruobin Dai,Tianlin Wang,Zhiwei Wang
Tannic acid (TA)-FeIII nanofiltration (NF) membrane has been demonstrated to possess more favorable removal of trace organic contaminants (TrOCs) over the conventional polyamide NF membrane. However, the drawback of acid instability severely hinders the practical application of TA-FeIII NF membrane in the treatment of (weak) acidic wastewater containing TrOCs (e.g., pharmaceutical wastewater, surface water, and drinking water). Herein, we introduced the MIL-101(Cr) nanoparticle, a kind of metal–organic framework (MOF), into the TA-FeIII selective layer to enhance the membrane acid stability. The acid-tolerance parameter of MIL-101(Cr)-stabilized TA-FeIII membrane (TA-FeIII-MOF membrane, 12,000 ppm/s–1) was two orders of magnitude larger than that of the TA-FeIII membrane (50 ppm/s–1), and the TA-FeIII-MOF membrane can withstand acid treatment at pH = 4 for more than 30 days. Meanwhile, the TA-FeIII-MOF membrane displayed increased water permeance from 9.5 to 12.7 L/(m2·h·bar) after the MOF addition, without compromising the selectivity. The enhanced acid stability for the TA-FeIII-MOF membrane was ascribed to an intercoordination mechanism, where FeIII centers (from TA-FeIII complex) coordinated with −COOH groups (from terephthalic acid of MOF) and CrIII centers (from MOF) coordinated with −OH groups (from TA of TA-FeIII complex), which was verified by the density functional theory calculation. This study highlights a new approach for the development of a TA-FeIII-based NF membrane with markedly enhanced acid stability, which is important for its real application in wastewater treatment and water reuse.
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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水处理技术
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CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Kai Liu,Ziying Liu,Kaixiang Zhi,Chang Liu,Huarui Zhang,Zhenyuan Hu,Yunfeng Zhang,Fan Xia,Chen Li,Hansong Cheng
Fluorinated MOFs material F-MIL-101 simply synthesized by hydrothermal method. • A gel polymer electrolyte that can fully dissociate LiTFSI. • The t Li + of FM-10 is 119% higher than M-10. • The FM-10 formed a LiF-rich SEI layer on the lithium anode. • LFP||Li cells achieve excellent rate and cycling characteristics. Development of an attractive inorganic filler plays a vital role in effectively enhancing the comprehensive performance of a polymer electrolyte. Herein, a fluorine-functionalized metal organic framework (fluorinated MIL-101, F-MIL-101) is intentionally designed as filler for fabricating a novel composite polymer electrolyte (FM-10). Spectroscopic analysis and density functional theory calculations reveal that F-MIL-101 exhibits high effective dissociation and transportation of Li + for LiTFSI salt. Notably, the F functional group hinders anion transport, thereby giving the FM-10 GPEs a high transfer number of 0.81 for a uniform deposition of Li + on the Li anode surface. Furthermore, the F group of F-MIL-101 is greatly favorable for the formation of a stable LiF-rich solid electrolyte interface (SEI) on the Li anode surface during cycling to hinder the uninterrupted reaction. Consequently, the FM-10 GPEs demonstrates an excellent stable Li anode with a long cycle-life of 600 h in Li||Li cell at 2 mA cm −2 . More importantly, the FM-10 GPEs assembled LiFePO 4 (LFP) || Li cell exhibited an initial discharge capacity of 120.5 mAh g −1 at a high 6C-rate and a retention of 98.68% after 300 cycles, implying that the F-MIL-101 filler shows great potential as a strategy for fast charging, long cycle life, and high safety SSLMBs.
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JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
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2026
·
IF 6.2
Jie Gao,Leiyu Yang,Yijia Yao,Meiyi Wang
To mitigate the ecological risks of trifluralin (TFL) from volatilization, photolysis, and leaching, a stimuli-responsive composite, TFL/CMC-GEL/MIL-101(Fe), was developed by encapsulating MIL-101(Fe) within a carboxymethyl cellulose–gelatin semi-interpenetrating hydrogel. The composite enhanced light stability of TFL by 1.5 times, reduced leaching by 17.8%, and extended soil retention beyond 14 days, minimizing groundwater contamination. In addition, the herbicidal activity of TFL/CMC-GEL/MIL-101(Fe) against Portulaca oleracea L. and Setaria viridis (L.) P. Beauv. were 95% and 94%, respectively, which was equivalent to TFL technical. Meanwhile, this herbicidal delivery system markedly enhanced crop safety, with rice seed germination rising from 13% under TFL technical alone to 36%. The dual-network design enables on-demand herbicide release by integrating MIL-101(Fe)-mediated protection with hydrogel-based stimuli responsiveness, effectively mitigating herbicide migration in the environment and offering a sustainable plant protection platform.
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Journal of Water Process Engineering
·
2023
·
IF 7
Shuangli Li,Yu Zhang,Sen Qiao,Jiti Zhou
Although MIL-101(Fe) has a homogeneous distribution of active metal sites, the relatively low stability of its coordination bonds limits its potential for application, especially in harsh environments. Here, a novel lanthanum-doped MIL-101(Fe)-NH 2 @mesoporous SiO 2 yolk-shell (LMFN-YS) material, synthesized by green water-etching, has effectively improved the adsorption capacity and stability of MIL-101(Fe)-NH 2 . Compared to traditional acid-base etching methods, water etching offered a more co-friendly and cost-effective approach to producing yolk-shell structures. Due to the mesoporous protective shell of mesoporous SiO 2 and more exposed active sites, the yolk-shell materials showed a faster adsorption rate (30 min) and a larger uptake capacity (240.0 mg P/g) than those of MIL-101. The material also exhibited broad range of pH stability from 2 to 10 and displayed good cyclic regeneration ability, with a removal efficiency of 75.9 % after three cycles. Additionally, it demonstrated excellent selectivity towards various coexisting anions such as Cl − , NO 3 − , SO 4 2− , CO 3 2− and HCO 3 − at diverse ionic strengths ranging from 0.001 to 1 M. The superior performance of L 1 MFN-YS (yolk-shell materials of La: Fe = 1:1) was attributed to a combination of factors, including ligand exchange between La(Fe)-OH and phosphates, Lewis acid-base interaction and electrostatic attraction. Additionally, high phosphate removal performance was observed in the real petrochemical wastewater (initial concentrations of 5.48 mg P/g) with a residual effluent concentration of 0.05 mg P/L, which was below the A-level standard of phosphate effluent in China (0.5 mg/L). This work provides a green method for preparing yolk-shell materials with improved ability to treat phosphate wastewater.
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Environmental Science-Water Research & Technology
·
2022
·Vol. 8
·期 6
·1211-1222
·
IF 5.819
Boming Fu,Yifei Xing,Changbao Gong,Huimin Zhao
N-Acyl homoserine lactones (AHLs), as typical signaling molecules in quorum sensing systems, play a key role in identifying the performance of activated sludge and microbial activities. Herein, a molecularly imprinted polymer composite material (CQDs@MIL-101@MIPs) was prepared under controlled conditions using a metal–organic framework (MIL-101) as the carrier material, carbon quantum dots (CQDs) as the fluorescent probe, and 2,5-dimethyl-4-hydroxy-3(2H)-furanone (DMHF) as the template molecule by a surface imprinting technique, which was utilized for the rapid and sensitive detection of activated sludge quorum-sensing signaling molecules. After the elution of the template molecules, blotted cavities capable of selectively recognizing AHLs were formed on the surface of CQDs@MIL-101@MIPs. This composite material showed a linear fluorescence intensity with different target concentrations; the linear detection range was 0.2–2.0 μM, and the limit of detection (LOD) was 0.21 μM. The fluorescence method based on CQDs@MIL-101@MIPs was utilized to detect and analyse activated sludge samples with recoveries of 95.2–117.9%. As a stable and straightforward detection method, the CQDs@MIL-101@MIPs based fluorescent sensor has the potential to be utilized for the rapid and sensitive detection of AHLs in real samples.
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CHEMOSPHERE
·
2021
·
IF 7.086
Peipei Huang,Lili Yao,Qing Chang,Yunhan Sha,Guodong Jiang,Shenghua Zhang,Zhe Li
The slow redox rate of Fe(III)/Fe(II) couples is a rate-limiting step for Fenton-like performance of Fe-MOFs. In this study, a series of catalysts (MIL-101) with various p-phthalic acid/2-aminoterephthalic acid (H 2 BDC/NH 2 –H 2 BDC) molar ratios were prepared using a simple and mild chemical method and applied for catalyzed degradation of bisphenol A (BPA). Interestingly, the –NH 2 modified MIL-101(Fe) can adjust Fe-Oxo node by increasing the electron density of Fe(III) in the presence of –NH 2 group with high electron density, thus forming Fe(II) in situ in MOFs. Meanwhile, the –NH 2 groups used as electron-donors can promote electron transfer , resulting in faster Fe(III)→Fe(II) half-reaction and active H 2 O 2 to continuously generate •OH radical. The BPA degradation and rate constant of Fe-BDC-NH 2 /H 2 O 2 system are 15.4-fold and 86.8-fold higher than that of Fe-BDC/H 2 O 2 system, respectively. The density functional theory (DFT) calculations showed that Fe-BDC-NH 2 possesses higher Fermi level energy (−4.88 eV) and lower activation energy barriers (0.32 eV) compared with Fe-BDC. Moreover, Fe-BDC-NH 2 showed good reusability and stability. This work offers a highly efficient and stable MOFs-based Fenton-like catalyst to rapidly degrade organic pollutants over a wide pH range for potential applications in wastewater treatment .
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ACS Omega
·
2020
·
IF 2.87
Jia Wang,Yansong Liu,Xiuyan Guo,Hongqiang Qu,Ran Chang,Jing Ma
Metal–organic frameworks (MOFs) exhibit highly designable properties and have been used in wide applications. To further improve their performance, the modification of MOFs is an effective method. However, the modification process is usually complicated. Besides, the sustainable use of MOFs is difficult to achieve due to the complicated recycling treatment. Herein, we designed a polyethyleneimine (PEI)-modified NH2-MIL-101(Al) composite (PEI@NH2-MIL-101(Al)). This composite showed excellent dye removal performance of methyl orange (MO, 89.4%) and Direct Red 80 (DR80, 99.8%). Remarkably, the dye removal application of PEI@NH2-MIL-101(Al) also acted as a modification process toward flame retardant application. Thus, the dye-adsorbed PEI@NH2-MIL-101(Al) composite (MO-PEI@NH2-MIL-101(Al) and DR80-PEI@NH2-MIL-101(Al)) was sustainably used as an effective flame retardant for an epoxy resin (EP) at low additions (4.0 wt %). The limiting oxygen values of EP/MO-PEI@NH2-MIL-101(Al) and EP/DR80-PEI@NH2-MIL-101(Al) increased to 26.5 and 26.7%, respectively. The heat release and the smoke production of dyes-PEI@NH2-MIL-101(Al)/EP were greatly reduced compared with those of EP. This strategy provides a simple and effective modification method for MOFs. Meanwhile, the modified MOF composite can achieve sustainable application, giving full play to the advantages of MOFs.
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Nano Research
·
2020
·Vol. 14
·期 7
·2383-2389
·
IF 8.183
Zhang Yuwei,Liu Fei,Yang Zhichao,Qian Jieshu,Pan Bingcai
In the pursuit of heterogeneous catalysts with high reactivity, metal organic framework (MOF) nanomaterials have received tremendous attentions. However, many MOF catalysts especially Fe-based MOFs need to be utilized immediately after synthesis or being activated using high temperature, because of the easy loss of reactivity in humid environments resulting from the occupation of active Fe sites by water molecules. Here, we describe an inspiring strategy of growing MIL-101-Fe nanoparticles inside the three-dimensional confined space of graphene aerogel (GA), generating shapeable GA/MIL-101-Fe nanocomposite convenient for practical use. Compared to MIL-101-Fe, GA/MIL-101-Fe as catalyst demonstrates much higher reactivity in Fenton-like reaction, attributing to smaller MIL-101-Fe particle size, presence of active Fe(II) sites, and abundant defects in GA. Strikingly, the weakly hydrophobic nature of the composite greatly inhibits the loss of catalytic reactivity after being stored in humid air and accelerates the recovery of reactivity in mild temperature, by resisting the entrance of water molecules and helping to exclude water molecules. This work demonstrates that a delicate design of nanocomposite structure could not only improve the reactivity of the catalytic component, but also overcome its intrinsic drawback by taking advantage of the properties of host. We hope this functional nanoconfinement strategy could be extended to more scenarios in other fields.
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JOURNAL OF MOLECULAR LIQUIDS
·
2020
·
IF 5.065
Wei Zhang,Run-Zhi Zhang,Yun Yin,Ji-Min Yang
We herein report that the forces driving the adsorption of dyes onto MIL-101-NH 2 micro/nanoparticles, which are electrostatic , hydrogen bonding , and π-π stacking interactions, pore-volume, and steric hindrance , can be modulated by varying the molar ratio of terephthalic acid and 2-aminoterephthalic acid in the reaction system. The adsorption capacities of MIL-101-NH 2 -1 were determined to be 2967.1 mg g −1 for Congo red (CR), 461.7 mg g −1 for methyl orange (MO), and 259.8 mg g −1 for acid chrome blue K (AC), which were higher by 117.0%, 102.2%, and −19.6%, respectively, compared with those of pristine MIL-101. This adsorption behavior could be rationalized based on the molecular structure of the dye, its zeta potential , BET specific surface area, and the adsorption characteristics of the dye. The study revealed that free –NH 2 groups increase the hydrogen bonding and electrostatic interactions between MIL-101-NH 2 micro/nanoparticles and linear anionic dyes, thereby improving the adsorption performance for linear anionic dyes by overriding the effect of pore-volume. On the other hand, the increased steric hindrance between MIL-101-NH 2 micro/nanoparticles and a nonlinear anionic dye decreased the adsorption performance for the nonlinear dye, overriding the effects of hydrogen bonding, and electrostatic interactions. The adsorption uptakes of MIL-101-NH 2 -1 toward the linear anionic organic dyes (CR and MO) were found to be much higher than those of the other two MIL-101-NH 2 adsorbents investigated herein. However, the adsorption uptake of MIL-101-NH 2 -1 toward the nonlinear anionic organic dye (AC) was the smallest owing to different adsorption mechanisms. The adsorption performance of MIL-101-NH 2 is governed by the synergetic interplay between the hydrogen bonding, electrostatic and π–π stacking interactions, pore-volume, and the steric hindrance of the adsorbent.
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MICROCHEMICAL JOURNAL
·
2018
·
IF 2.746
Man Gao,Wei Liu,Xuran Wang,Yanyan Li,Peipei Zhou,Liwan Shi,Buxing Ye,Randy A. Dahlgren,Xuedong Wang
Herein, we investigated in detail the relationship between surface properties and extraction performance of virgin and amino-functionalized MIL-101s(Fe) for the extraction of 10 bisphenols (BPs) and their derivatives. These BPs were used as model contaminants due to their different hydroxyl groups and contrasting polarities. The differential sorption efficiencies for relatively polar BPs (BPF, BPE, BPA , BPB , BPZ, BPAP and BPP) lies in the formation of hydrogen-bonding between OH of target analytes and NH 2 of two MIL-101s(Fe). However, the surface properties of MIL-101(Fe) and NH 2 -MIL-101s(Fe), such as S BET and pore structure , determined the extraction recoveries for BPs derivatives (BADGE, BADGE·2H 2 O and BFDGE·2H 2 O) due to lack of OH in their molecular structures. NH 2 -MIL-101s(Fe) nanosorbent was successfully applied to the preconcentration/extraction of trace BPs and their derivatives by dispersive solid-phase extraction (DSPE) method. Following optimization of the main factors, recoveries for BPs ranged from 90.8 to 117.8% and their LODs were 0.016–0.131 μg L −1 in environmental waters. Experimental precisions based on relative standard deviations were 0.9–4.9% for intra-day and 1.3–7.6% for inter-day analyses, respectively. These findings provide important information on how to design and modify nanosorbents for highly efficient extraction of pollutants having contrasting polarities. Moreover, the newly developed NH 2 -MIL-101s(Fe)-based DSPE method has a good application prospect in pretreatment of trace pollutants in real-world waters.
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