INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
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2024
·Vol. 25
·期 18
·9855
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IF 4.9
Yiting Luo,Rongkui Su
Tetracycline’s accumulation in the environment poses threats to human health and the ecological balance, necessitating efficient and rapid removal methods. Novel porous metal–organic framework (MOF) materials have garnered significant attention in academia due to their distinctive characteristics. This paper focuses on studying the adsorption and removal performance of amino-modified MIL-101(Fe) materials towards tetracycline, along with their adsorption mechanisms. The main research objectives and conclusions are as follows: (1) NH2-MIL-101(Fe) MOF materials were successfully synthesized via the solvothermal method, confirmed through various characterization techniques including XRD, FT-IR, SEM, EDS, XPS, BET, and TGA. (2) NH2-MIL-101(Fe) exhibited a 40% enhancement in tetracycline adsorption performance compared to MIL-101(Fe), primarily through chemical adsorption following pseudo-second-order kinetics. The adsorption process conformed well to Freundlich isotherm models, indicating multilayer and heterogeneous adsorption characteristics. Thermodynamic analysis revealed the adsorption process as a spontaneous endothermic reaction. (3) An increased adsorbent dosage and temperature correspondingly improved NH2-MIL-101(Fe)’s adsorption efficiency, with optimal performance observed under neutral pH conditions. These findings provide new strategies for the effective removal of tetracycline from the environment, thus holding significant implications for environmental protection.
研究领域:
环境科学
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材料科学
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DOI
PubMed
高影响因子
LANGMUIR
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2025
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IF 3.9
Mingyang Xiong,Yao Zeng,Ruisi Qiu,Hongxing He,Yi Zhang,Zhifeng Nie,Bing Wang
Bisphenol A (BPA) is extensively utilized as an industrial chemical in the production of certain plastics and epoxy resins. They are frequently found in environmental water and have the potential to cause risks to both the environment and human health. To efficiently remove the endocrine disruptor BPA from aqueous solutions, sea urchin-like magnetic material Fe3O4@PDA@NH2-MIL-101 (Fe) was synthesized via hydrothermal methods. Fe3O4@PDA@NH2-MIL-101 (Fe) has excellent adsorption performance, with a theoretical maximum adsorption capacity of 300.47 mg/g for BPA. The adsorption kinetics of BPA by Fe3O4@PDA@NH2-MIL-101 (Fe) followed the pseudo-second-order kinetic model and Liu’s isotherm model. Magnetic separation experiments reveal a high recovery efficiency, maintaining 94.82% of its initial adsorption capacity after five cycles. The primary adsorption mechanisms of Fe3O4@PDA@NH2-MIL-101 (Fe) on BPA included pore filling, hydrogen bonding, π–π interaction, and Lewis acid–base interaction. Additionally, the material showed excellent removal performance of BPA, with a maximum adsorbed amount of 135.27 mg/g for total organic carbon (TOC) in the shale gas fracturing flowback fluid. These findings suggest that Fe3O4@PDA@NH2-MIL-101 (Fe) holds significant potential as an adsorbent for BPA removal from actual wastewater, offering promising prospects for practical applications.
研究领域:
环境科学
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材料科学
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DOI
PubMed
高影响因子
APPLIED CATALYSIS A-GENERAL
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2023
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IF 5.5
Huifang Feng,Yitong Sun,Qiaozhen Xu,Hong Liu
Developing efficient photocatalyst to promote the conversion of CO 2 into value-added chemicals remains challenging. Here, novel NH 2 -MIL-101(Fe)@Bi 2 MoO 6 S-scheme heterojunctions were fabricated via a solvothermal method, in which Bi 2 MoO 6 (BMO) nanoparticles uniformly growing on the NH 2 -MIL-101(Fe) (NM101) octahedrons with intimate contact interface. The resultant heterojunctions revealed significantly enhanced activity for CO 2 photoreduction. The optimal performance was achieved when the content of BMO was 10 wt%, and the formation rate of CO reached 67.0 μmol·g −1 ·h −1 under visible light illumination (with apparent quantum efficiency of 0.09 % at 450 nm), which was 3.2-fold of individual NM101. The boosting activity benefited from the formation of S-scheme heterojunction at the NM101 @BMO interfaces, which facilitated the separation of photoinduced electron-hole pairs with strong redox ability at the interface. This S-scheme charge transfer mechanism was further validated by the in-situ XPS and fluorescence probe molecular experiment. Besides, the intermediates and preliminary mechanism of photoreaction were unraveled based on in-situ DRIFTS analysis. This work provides some novel insights for designing efficient S-scheme photocatalysts for CO 2 photoreduction.
研究领域:
材料科学
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环境科学
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化学
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DOI
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2023
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IF 5.2
Shiyu Zhang,Qiuyu Qiao,Yangfeng Wen,Kena Ren,Xiaoyu Ma,Haisheng Tao
A novel composite of acetic acid-modulated AC-NH 2 -MIL-101(Fe) was prepared by mild chemistry . The catalyst was characterized by scanning electron microscopy (SEM), X-ray diffraction (XRD), thermogravimetric analysis (TGA), Fourier transform infrared spectroscopy (FTIR), Brunaure-Emmett-Teller (BET) and X-ray photoelectron spectroscopy (XPS). Acetic acid can control the crystal size, so that the catalyst had a large specific surface area (99.35 m 2 ·g −1 ) and pore size (0.13 cm 3 ·g −1 ), the adsorption amount of Rhodamine B (RhB) up to 446.965 mg·g −1 , after the addition of peroxydisulfate (PDS), the catalytic degradation efficiency of RhB was as high as 99.7%. Electronic paramagnetic resonance spectrometer (EPR) and quenching experiments showed that the catalytic process may involve radical (·OH, SO 4 -· and O 2 ·- ) and non-radical ( 1 O 2 ) processes, in which the contribution of 1 O 2 to degradation reached 63.55% and played a major role.
研究领域:
材料科学
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环境科学
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DOI
高影响因子
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.
研究领域:
材料科学
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环境工程
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化学工程
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DOI
PubMed
高影响因子
Journal of Environmental Chemical Engineering
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2024
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IF 7.4
Yuhang Ren,Yu Tian,Yating Lu,Dongyu Nie,Huayi Zhu,Xia Yang
Malathion (MA) is a widely used organophosphorus pesticide globally. Developing efficient photocatalysts is crucial for eliminating MA pollution in water by photocatalytic technology. This study focuses on preparing a series of H-PDI supermolecule/NH 2 -MIL-101(Fe) (PM) materials by amidating NH 2 -MIL-101(Fe) with the more stable H-PDI supermolecule, forming a covalent O C–NH bond. Among these materials, 40 %PM (indicating a mass percentage content of 40 % H-PDI supermolecule in PM) exhibited the best performance for degradation of MA. Under simulated sunlight irradiation of a 10 mg·L 1 MA solution for 180 min, the reaction rate constants of 40 %PM were 5.95 times and 3.13 times higher than those of NH 2 -MIL-101(Fe) and H-PDI supermolecule, respectively. The enhanced performance is attributed to the formation of Z-scheme heterojunctions in the 40 %PM composite lead to fast separation of photogenerated e − and h + . Combining the results of HPLC-MS with Fukui Function, the HOMO, LUMO, and pathway of degradation of MA attracted by 1 O 2 , •OH, and h + were speculated. The pathway involves oxidation, demethylation, P-S bond breakage, decarboxylation, and final conversion to some inorganic molecules. The toxicity of the degradation byproducts were lower than that of MA estimated by Toxicity Estimation Software Tool.
研究领域:
环境科学
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材料科学
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DOI
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
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2025
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IF 4.7
Jian Luo,Yonghui Lin,Yanfeng Liu,Siliang Wang,Yiduo Chen,Xudong Tian,Weiting Yang,Zhongmin Su
Roxarsone (3-nitro-4-hydroxyphenylarsenic acid, ROX) is easily converted into highly toxic inorganic arsenic compounds, therefore, the development of highly efficient adsorbents for the removal of ROX from wastewater is necessary but remains challenging. In this study, NH 2 -MIL-101 (Fe) was synthesised and modified with TPA-CHO (4-(N, N-diphenylamine) benzaldehyde) to obtain TPA-MIL-101(Fe) with triphenylamine functionalised groups. The modified TPA-MIL-101(Fe) exhibits the very high adsorption capacity (728.2 mg g −1 ) and fast adsorption equilibrium (2 h). The TPA-MIL-101(Fe) showed excellent selectivity, and the adsorption efficiency hardly decreased in the presence of competing ions (Cl − , NO 3 − , SO 4 2− ). The TPA-MIL-101(Fe) showed good adsorption performance for ROX at pH 3–13, with the best performance at pH = 9. In addition, TPA-MIL-101(Fe) was able to remove trace amounts of ROX from actual water samples (<5 mg L −1 ) with an efficiency of 99.46 %, and the remaining ROX content meets the international drinking water standards of the World Health Organization (29 μg L −1 ). The mechanism studies have shown that the Fe-O-As coordination and the π-π stacking interaction between TPA-MIL-101(Fe) and ROX greatly enhance its adsorption performance. In conclusion, this work provides a promising material for effective removal of ROX from the environmental water.
研究领域:
环境科学
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材料科学
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环境污染与控制
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水处理技术
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配位化学
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产品关联
DOI
高影响因子
JOURNAL OF SOLID STATE CHEMISTRY
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2025
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IF 3.5
Tongxin Xiao,Kangyue Qiao,Guodong Hao,Songyao Du,Yue Wang,Chao Sui
This study employed a solvothermal method to prepare an NH 2 -MIL-101(Fe, Co) bimetallic organic framework composite catalyst aimed at enhancing the photocatalytic reduction performance of Cr(VI). The experimental results show that introducing Co into the single-metal NH 2 -MIL-101(Fe) does not alter the material's octahedral structure. However, the bimetallic synergistic effect shifts the light absorption range to the red end of the spectrum, reduces the bandgap, and significantly improves carrier separation efficiency. Under visible light irradiation, the NH 2 -MIL-101(Fe, 0.15Co) catalyst exhibited outstanding photocatalytic performance, achieving a reduction efficiency of 94.7% for Cr(VI) within 40 minutes and 100% within 50 minutes, with a reaction rate constant 4.7 times that of the single-metal NH 2 -MIL-101(Fe). Free radical capture experiments further revealed that ·O 2 - is the key active species in the Cr(VI) reduction process, while photo-generated holes in the valence band can oxidise OH - to ·OH, synergistically participating in the reaction. Additionally, cyclic stability experiments showed that the catalyst maintained 85.8% reduction efficiency after five cycles, demonstrating excellent stability and practical application potential.
研究领域:
环境科学
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催化
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材料科学
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化学工程
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DOI
高影响因子
ACS Omega
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2023
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IF 4.1
Qiyue Zhang,Aori Qileng,Jiale Li,Yiran Cao,Weipeng Liu,Yingju Liu
Organic dyes can produce harmful effects on the water environment, such as affecting the growth of aquatic organisms, reducing the transparency of water bodies, and causing eutrophication of water bodies, so it is necessary to mitigate the hazards of organic dyes. In this study, a metal–organic framework [NH2-MIL-101(Fe)] was synthesized by the solvothermal method as a carrier for the in situ uniform deposition of AgCl nanoparticles on its surface, which was successfully used for both adsorption and degradation of Congo red. Adsorption results showed that the adsorption kinetics conformed to the proposed secondary adsorption kinetics equation with a maximum adsorption capacity of 248.4 mg·g–1. Furthermore, the degradation results indicated that with the aid of sodium borohydride as a reducing agent, the degradation of Congo red followed pseudo-first-order kinetics with a degradation rate of 0.077 min–1, and the complete degradation of Congo red was finished within 18 min. Therefore, AgCl/NH2-MIL-101(Fe) may find a potential application in the removal of dyes from wastewater.
研究领域:
环境科学
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材料科学
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产品关联
DOI
PubMed
高影响因子
Journal of Environmental Chemical Engineering
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2023
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IF 7.7
Huihu Wang,Hao Tu,Feng Chen,Huang Xu,Ziguan Zhang,Guode Chen,Chenhuinan Wei,Xing Xiang,Zhixiong Xie
Through a facile oil bath method, a novel highly dispersed NH 2 -MIL-101(Fe)/carboxylated g-C 3 N 4 (NM-101(Fe)/CCN) heterostructure was prepared using the chemical bonding between carboxyl groups and -NH 2 groups. Compared with the octahedral morphology of pure NM-101(Fe), the chemical bonding interaction promoted the heterogeneous nucleation and growth of NM-101(Fe) to form nanometer-sized granular morphology, which was homogeneously dispersed on CCN surface. Cr(Ⅵ) and ciprofloxacin (CIP) were selected as the typical pollutant models in micro-polluted water sources. The results showed that 10 %NM-101(Fe)/CCN heterostructure could remove 97 % of Cr(Ⅵ) in 60 min and 88 % of ciprofloxacin (CIP) in 120 min. In the dual pollutant system of Cr(Ⅵ) and CIP, Cr(Ⅵ) reduction and CIP degradation can promote each other, and the degradation efficiency of CIP reached 96 % within 120 min. The apparent rate constant of 10 %NM-101(Fe) /CCN heterostructure for Cr(Ⅵ) reduction was 4.30 and 9.67 times of that of NM-101(Fe) and CCN, respectively, which may be ascribed to the interface electric field and good interface bonding of heterojunction . The charges separation efficiency was significantly improved, which effectively enhanced the photocatalytic activity.
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
SOLID STATE SCIENCES
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2021
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IF 3.059
Cong Huang,Jun Wang,Mengjun Li,Xiaofang Lei,Qiang Wu
The construction of Z-scheme systems is a valid strategy to effectively enhance photocatalytic property in the field of photocatalysis . In the present work, a novel Z-scheme V 2 O 5 /NH 2 -MIL-101(Fe) heterojunction photocatalyst was prepared via a simple one-pot solvothermal method for the first time. The phase structure, morphology and optical property of the as-prepared V 2 O 5 /NH 2 -MIL-101(Fe) composite were carried out by a series of characterizations. The photocatalytic property of V 2 O 5 /NH 2 -MIL-101(Fe) heterojunction photocatalyst was investigated by photodegrading tetracycline (TC) under ultraviolet–visible light irradiation. The systematic studies indicate that the obtained V 2 O 5 /NH 2 -MIL-101(Fe) heterojunction photocatalyst possesses superior photocatalytic performance toward TC removal. Furthermore, a Z-scheme photocatalytic degradation mechanism for TC over V 2 O 5 /NH 2 -MIL-101(Fe) composites was proposed. The results show that Z-scheme V 2 O 5 /NH 2 -MIL-101(Fe) heterojunction photocatalyst has potential application in the treatment of TC wastewater. This research will broaden the studies of NH 2 -MIL-101(Fe)-based Z-scheme photocatalysts.
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
Desalination and Water Treatment
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2024
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IF 1
Hui Huang,Bin Huang,Yichun Huang,Jinbei Yang,Yinnv Ye,Yucheng Chen
Attractive environmentally friendly magnetic metal-organic framework (MOF) nanocomposite GO@Fe 3 O 4 -COOH@NH 2 -MIL-101(Fe) was synthesized by a solvothermal method and characterized by X-ray diffraction, Fourier transform infrared, scanning electron microscopy, Brunauer– Emmett–Teller, and vibrating sample magnetometer, and used as an effective adsorbent for the removal of orange G from aqueous solution. The various operating parameters that effect the adsorption process, such as adsorbent dosage (0.01–0.2 g), pH (1.0–10.0), initial concentration (50–400 mg L –1 ), and temperature (298.15–318.15 K) were studied. The percent removal of orange G increases with the increment of the adsorbent dosage and decrease of the initial concentration, and the optimum pH is 6.0. The Redlich–Peterson model can be favorably applied to describe the adsorption equilibrium data, indicating that the surfaces of GO@Fe 3 O 4 -COOH@NH 2 -MIL-101(Fe) nanocomposite for the orange G adsorption are made up of homogeneous adsorption patches. The adsorption kinetics indicate that the adsorption process of GO@Fe 3 O 4 -COOH@NH 2 -MIL-101(Fe) toward orange G obeys the pseudo-second-order model and the activation energy is 16.5 kJ mol –1 . Thermodynamic parameters, ΔH = 39.81 kJ mol –1 , ΔS = –46.80 J mol –1 K –1 , and ΔG < 0, exhibit that the adsorption is exothermic and spontaneous. The maximum adsorption capacity of orange G onto GO@Fe 3 O 4 -COOH@NH 2 -MIL-101(Fe) nanocomposite is 128.8 mg g –1 . Therefore, magnetic GO@ Fe 3 O 4 -COOH@NH 2 -MIL-101(Fe) nanocomposite can be employed as an environmentally friendly and efficient adsorbent for the orange G removal from wastewater.
研究领域:
环境科学
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纳米技术
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材料科学
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化学工程
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水处理
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DOI
高影响因子
危险品化学品经营许可证（带存储）