JOURNAL OF HAZARDOUS MATERIALS
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2022
·
IF 14.224
Rongsheng Ning,Heliang Pang,Zhongsen Yan,Zhenyu Lu,Qiankun Wang,Zengling Wu,Wenxin Dai,Lingshan Liu,Zhongsheng Li,Gongduan Fan,Xianzhi Fu
The development of high efficient photocatalysts for antibiotics contamination in water remains a severe challenge. In this study, a novel step-scheme (S-scheme) photocatalytic heterojunction nanocomposites were fabricated from integrating AgCl nanoparticles on the MIL-100(Fe) octahedron surface through facile multi-stage stirring strategy. The S-scheme heterojunction structure in AgCl/MIL-100(Fe) (AM) nanocomposite provided a more rational utilization of electrons (e - ) and holes (h + ), accelerated the carrier transport at the junction interface, and enhanced the overall photocatalytic performance of nanomaterials . The visible-light-driven photocatalysts were used to degrade sulfamethazine (SMZ) which attained a high removal efficiency (99.9%). The reaction mechanisms of SMZ degradation in the AM photocatalytic system were explored by electron spin resonance (ESR) and active species capture experiments, which superoxide radical (•O 2 - ), hydroxyl radical (•OH), and h + performed as major roles. More importantly, the SMZ degradation pathway and toxicity assessment were proposed. There were four main pathways of SMZ degradation, including the processes of oxidation , hydroxylation, denitrification, and desulfonation. The toxicity of the final products in each pathway was lower than that of the parent according to the toxicity evaluation results. Therefore, this work might provide new insights into the environmentally-friendly photocatalytic processes of S-scheme AM nanocomposites for the efficient degradation of antibiotics pollutants.
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JOURNAL OF HAZARDOUS MATERIALS
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2021
·
IF 10.588
Jiang-Bo Huo,Guoce Yu
Efficient elimination of As(III) from drinking water and wastewater has been a challenge because of its neutral molecular form. To address this problem, a novel nanocomposite , mesoporous cerium oxide-anchored magnetic polyhedrons derived from MIL-100(Fe) was fabricated via a strategy combining impregnation and calcination . The resultant products (denoted as Fe 2 O 3 /CeO 2 -t) exhibited a unique octahedral nanostructure decorated by mesoporous cerium oxide . Surface modification of CeO 2 enhanced As(III) removal in comparison to unmodified Fe 2 O 3 . Particularly, Fe 2 O 3 /CeO 2 -4 h can reduce As(III) concentration from 180 to 10 µg/L within 20 min, which was almost 9 times faster than unmodified Fe 2 O 3 . The adsorption behavior conformed to the pseudo-second-order kinetic model ( R 2 = 0.9908) and the Freundlich isotherm model ( R 2 = 0.9943). The maximum adsorption capacity of As(III) by Fe 2 O 3 /CeO 2 -4 h was 68.25 mg/g, higher than those reported for similar adsorbents. Its enhanced removal mechanism can be attributed mainly to the mesoporous characteristics and oxidization ability of surface ceria. The composite can be separated from water by external magnets and easily regenerated. This study may offer a clue to the design of metal-organic framework-based composites as an alternative adsorbent for arsenite cleanup.
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Journal of Environmental Chemical Engineering
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2020
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IF 4.3
Shanshan Chen,Zhongyang Zang,Shusheng Zhang,Gangfeng Ouyang,Runping Han
Metal-organic framework and nano carbon materials were widely used in separation field in recent years. In this study, nanocomposite of MIL-100(Fe) and multi-walled carbon nanotubes (MIL-100(Fe)-CNTs) was prepared and characterized and its adsorption property towards Oxytetracycline (OTC) was presented. MIL-100(Fe)-CNTs exhibits higher adsorption capacity compared to MIL-100(Fe), making this composite as one of the favorable adsorbents. The adsorption capacity of MIL-100(Fe)-CNTs reached 429 mg·g −1 at 313 K. The langmuir model and Koble-Corrigan model were better to predict the equilibrium data while the pseudo-second-order kinetic model could well describe the kinetic process. The process was endothermic and spontaneous while the ion exchange was the main adsorption mechanism of OTC on MIL-100(Fe)-CNTs. The nanocomposite is promising to effectively remove OTC from solution.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2020
·Vol. 27
·期 30
·37839-37851
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IF 3.056
Xu Jun,Xu Jinmei,Jiang Shanqing,Cao Yu,Xu Kailin,Zhang Qiuya,Wang Liping
In this work, a novel visible light–driven heterostructure Ag 3 PO 4 /MIL-100(Fe) composite photocatalyst was successfully synthesized via facile chemical deposition method at room temperature. Especially when the mass ratio of Ag 3 PO 4 was 20% of MIL-100(Fe) (APM-2), it displayed the best photocatalytic performance, for which the degradation rate of tetracycline (TC) in conventional environment was 6.8 times higher than that of bare MIL-100(Fe). In addition, the effects of the initial concentration and pH of the solution on the degradation of tetracycline were also studied, and the results showed that the degradation of tetracycline was more favorable in a weakly alkaline environment. The excellent performance of Ag 3 PO 4 /MIL-100(Fe) composites was attributed to the fact that on the basis of having adequate photocatalytic active sites, modifying MIL-100(Fe) with an appropriate amount of Ag 3 PO 4 particles can more effectively separate photogenerated electron–hole pairs. Five cycles of experiments showed that APM-2 has good photostability. Lastly, it was proved through quenching experiments that •O 2 − , h + , and •OH all played corresponding roles in the degradation process, and a possible Z-scheme heterostructure photocatalytic degradation mechanism was proposed.
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Journal of Cleaner Production
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2021
·
IF 9.297
Lizhen Guo,Yuqi Wang,Meng Wang,Hiba Shaghaleh,Yousef Alhaj Hamoud,Xu Xu,He Liu
With the severe shortage of water resources and the low utilization efficiency of fertilizer, slow-release fertilizer equipped with water-absorbing and water-retaining capacity has captured much attention. Herein, by integrating metal-organic frameworks (MOFs) with cellulose nanofibres (CNFs) and sodium alginate (SA), a novel cellulose-based hydrogel (MIL-100(Fe)@CNF-SA) was fabricated that acted as a carrier for urea. The resultant hydrogel was not only qualified with a high surface area of 129.17 m 2 /g but also affluent in the hydrophilic groups . In parallel with the good water-holding capacity of 55% when the loading of the resultant hydrogel was only 0.5 g, the complete loss of the water in the treated soil was successfully slowed down by nearly 20 d compared with the soil without treatment. Urea (1.47 g/g) could be captured in the composite hydrogel , wherein the slow release of urea was achieved due to the synergism of the highly porous structure of the hydrogel and the crystals with a high specific surface area. Moreover, the positive effect of the resultant hydrogel on the growth of wheat was indexed to the germination rate, number of tillers, photosynthetic rate and chlorophyll content of the crop, which verified their further application in irrigating farming.
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MOLECULES
·
2019
·Vol. 24
·期 20
·3718
·
IF 3.06
Mao-Long Chen,Shu-Yang Zhou,Zhou Xu,Li Ding,Yun-Hui Cheng
MIL-100(Fe, Cr) and MIL-101(Cr) were synthesized by the hydrothermal method and applied to the adsorptions of five aromatic amines from aqueous solutions. These three metal-organic frameworks (MOFs) were well characterized by powder X-ray diffraction (PXRD), scanning electron microscope (SEM), transmission electron microscope (TEM), thermogravimetric analysis (TGA) and surface area analysis. The adsorption mechanism of three MOFs and the effects of the structures of MOFs on the adsorption of aromatic amines were discussed. The results show that the cavity system and suitable hydrogen bond acceptor were important factors for the adsorption for five aromatic amines of aniline, 1-naphthalamine, o-toluidine, 2-amino-4-nitrotoluene and 2-nitroaniline: (a) the saturated adsorption capacity of aniline, 1-naphthylamine and o-toluidine on MIL-100(Fe) were 52.0, 53.4 and 49.6 mg/g, respectively, which can be attributed to the intermolecular hydrogen bond interaction and cavity system diffusion. (b) The adsorption capacity of 2-nitroaniline and 2-amino-4-nitrotoluene on MIL-101(Cr) were 54.3 and 25.0 mg/g, respectively, which can be attributed to the more suitable pore size of MIL-101(Cr) than that of MIL-100(Fe, Cr). The MOFs of MIL-100(Fe) and MIL-101(Cr) can be potential materials for removing aromatic amines from aqueous solutions.Keywords:metal-organic framework;adsorption;aromatic amines;aniline;1-naphthalamine;o-toluidine;2-amino-4-nitrotoluene;2-nitroaniline
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RSC Advances
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2016
·Vol. 6
·期 43
·37110-37117
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IF 3.289
Mingjuan Han,Zheng Gu,Chong Chen,Zuowang Wu,Yigen Que,Qiang Wang,Hui Wan,Guofeng Guan
A new, simple and effective strategy to confine dicationic acid ionic liquids (DAILs, 1,4-bis[3-(propyl-3-sulfonate) imidazolium] butane hydrogen sulfate) in the cages of MIL-100(Fe) frameworks was constructed. The target catalyst, defined as MIL-100(Fe)@DAILs, was characterized by XRD, FTIR, SEM, TEM, EA, TGA and N2 adsorption–desorption. Meanwhile, the catalytic activity of the MIL-100(Fe)@DAILs catalyst was evaluated by the esterification reaction with oleic acid and methanol. The results indicated that the DAILs had been effectively encapsulated within the cages of the MIL-100(Fe) frameworks. Moreover, the influence of reaction time, reaction temperature, molar ratio of methanol to oleic acid and catalyst dosage on the conversion of oleic acid was studied by univariate analysis. The conversion of oleic acid decreased from 93.5% to 86.0% when the catalyst was reused five times, which indicated that the target catalyst possessed higher catalytic activity and superior catalytic activity. Finally, an esterification mechanism catalyzed by this novel catalyst was illustrated.
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MOLECULES
·
2017
·Vol. 22
·期 6
·920
·
IF 2.861
Youxun Liu,Yuanyuan Geng,Mingyang Yan,Juan Huang
The successful encapsulation of 2,2′-azino-bis(3-ethylbenzthiazoline-6-sulfonic acid) (ABTS), a well-known laccase mediator, within a mesoporous metal-organic framework sample (i.e., MIL-100(Fe)) was achieved using a one-pot hydrothermal synthetic method. The as-prepared ABTS@MIL-100(Fe) was characterized by scanning electron microscopy (SEM), X-ray diffraction (XRD), Fourier transform infrared (FT-IR) spectroscopy, nitrogen sorption, and cyclic voltammetry (CV). Our ABTS@MIL-100(Fe)-based electrode exhibited an excellent electrochemical response, indicating that MIL-100(Fe) provides an appropriate microenvironment for the immobilization and electroactivity of ABTS molecules. ABTS@MIL-100(Fe) was then evaluated as an immobilized laccase mediator for dye removal using indigo carmine (IC) as a model dye. Through the application of laccase in combination with a free (ABTS) or immobilized (ABTS@MIL-100(Fe)) mediator, decolorization yields of 95% and 94%, respectively, were obtained for IC after 50 min. In addition, following seven reuse cycles of ABTS@MIL-100(Fe) for dye treatment, a decolorization yield of 74% was obtained. Dye decolorization occurred through the breakdown of the chromophoric group by the Laccase/ABTS@MIL-100(Fe) system, and a catalytic mechanism was proposed. We therefore expect that the stability, reusability, and validity of ABTS@MIL-100(Fe) as a laccase mediator potentially render it a promising tool for dye removal, in addition to reducing the high running costs and potential toxicity associated with synthetic mediators.Keywords:laccase;ABTS;metal-organic framework;mediator;decolorization
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DALTON TRANSACTIONS
·
2018
·Vol. 47
·期 10
·3417-3424
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IF 4.099
Huairu Tian,Jun Peng,Qiuzheng Du,Xuanhong Hui,Hua He
A novel, rapid and simple method is described for the synthesis of magnetic MIL-100(Fe) with novel Fe3O4 morphology, which significantly improved the sustainability of conventional fabrication processes in several aspects. The magnetic MOFs were prepared (i) in one pot (instead of multiple steps), (ii) at room temperature (instead of temperatures over 150 °C), (iii) within a few hours with excellent yield (instead of in few days with low productivity) and (iv) in the absence of any corrosive inorganic acid and organic reagent. The materials were tested in the industrially demanded photocatalytic and photo-Fenton degradation of sodium sulfadiazine. The degradation results indicated that the Fe3O4 nanorods could accelerate the catalytic efficiency. The catalyst would be of potential application due to its stable catalytic activity in repeated reaction cycles and no need for regeneration. Therefore, the MIL-100(Fe) and magnetic MIL-100(Fe) proposed in this study are ideal catalysts for the heterogeneous degradation of sodium sulfadiazine.
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ACS Applied Materials & Interfaces
·
2022
·
IF 10.383
Zixia Tang,Hong Tao,Xiao Wang,Lu Chen,Chi Song,Guanhong Lu,Xiaofeng Xie,Jing Sun
The implantation of metal nanoparticles (MNPs) into metal–organic framework (MOF) hosts is a promising means to prepare high-performance photocatalysts for the degradation of gas pollutants. However, the uniform encapsulation of MNPs in MOFs is still challenging. Herein, a facile “quasi-in situ” encapsulation method is proposed by utilizing the spatial confinement effect of the colloidal network formed during the synthesis of the MIL-100(Fe) monolith [noted as m-MIL-100(Fe)]. Highly dispersed Ag NPs with an average diameter of ∼2 nm are encapsulated in the MIL-100(Fe) monolith to form a unique “watermelon-seed” structure, which ensures the large contact area between the two components and protects Ag NPs from being oxidized. The fast charge transfer between m-MIL-100(Fe) and Ag NPs enables the spatial separation of electron–hole pairs and promotes the generation of oxidative radicals. Compared with pristine m-MIL-100(Fe), the 0.2 wt % Ag@m-MIL-100(Fe) composite shows obviously enhanced photodegradation efficiencies for flowing o-xylene under both xenon (∼97%) and visible light (∼80.0%) with high stability. This work not only provides a promising Ag@m-MIL-100(Fe) material for eliminating air pollutants but also gives a versatile means for the design and synthesis of nanoparticles@MOFs composites with desired performance.
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Polymers
·
2026
·Vol. 18
·期 6
·772
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IF 5.8
Qianyi Wang,Guohan Wang,Sasa Ma,Zichen Wang,Lijie Luo,Yongjun Chen
The widespread use of plastics has inevitably led to the accumulation of persistent plastic debris in aquatic systems, where gradual fragmentation generates microplastics (MPs) that threaten ecological and biological health. Their small size, chemical stability, and resistance to degradation make effective removal particularly challenging. In this work, a composite adsorbent was fabricated through the in situ solvothermal growth of Materials of Institute Lavoisier 100 (Iron) (MIL-100(Fe)) onto coconut shell-derived activated carbon (CSAC), yielding a monolithic material denoted as CSAC@MIL-100(Fe). The integration of porous C with a metal–organic framework created a hierarchically structured adsorbent rich in accessible binding sites. The composite achieved a maximum polystyrene (PS) removal efficiency of 97.4% and maintained 91.44% efficiency after seven regeneration cycles. Stable adsorption performance was observed across a broad pH range. Structural and chemical analyses (scanning electron microscopy (SEM), Brunauer–Emmett–Teller (BET), X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FTIR), X-ray photoelectron spectroscopy (XPS)) combined with adsorption modeling revealed heterogeneous multilayer adsorption behavior consistent with the Freundlich isotherm and pseudo-second-order kinetics. π–π interactions, electrostatic attraction, and coordination effects jointly governed PS capture. The Langmuir maximum adsorption capacity reached 746.27 mg/g. These findings demonstrate a practical and recyclable strategy for efficient MP remediation in aquatic environments.
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WATER AIR AND SOIL POLLUTION
·
2026
·Vol. 237
·期 12
·702
·
IF 3.5
Yin Shiyu,Du Haiying,Yang Hong,Lai Chunrong
The treatment of industrial wastewater containing multiple heavy metals (MHMs) remains challenging, primarily because conventional adsorbents suffer from poor stability, limited adsorption capacity in mixed-metal systems, or high energy consumption during synthesis. To address these issues, this study employed a room-temperature in-situ impregnation method to load NH 2 -MIL-100(Fe) onto amine-functionalized magnetic hydrochar (HBAP). Three highly dispersible magnetic composites, designated as NM-100-HBAP-X (X = 0.75, 1, 1.25), were synthesized by adjusting the mass ratio of NH 2 -MIL-100(Fe) to HBAP. Experimental results demonstrated that the optimal material (NM-100-HBAP-1) exhibited high adsorption capacities for Pb(II), Cd(II), and Cr(VI) in a mixed-metal system. The maximum adsorption capacities determined by the Langmuir model were 181.13, 175.02, and 158.69 mg/g for Pb(II), Cd(II), and Cr(VI), respectively, which are comparable to previously reported values for hydrochars or MOF-based materials. Mechanistic analysis revealed that amino groups facilitate a synergistic process by reducing Cr(VI) to Cr(III), which is then immobilized via complexation and co-precipitation, thereby further enhancing Cd(II) removal. The material also demonstrated good cycling stability, retaining over 50% of its initial adsorption capacity after five regeneration cycles, and maintained effective performance in various real water samples. Furthermore, toxicity tests confirmed its environmental safety, and life cycle assessment quantified the GWP of producing 1 kg of NM-100-HBAP-1 as 41.224 kg CO 2 eq, with electricity and NH 2 -H 2 BDC synthesis as the dominant contributors. This study not only provides an efficient adsorbent for heavy metal removal but also offers a systematic research framework integrating material design, mechanistic investigation, and environmental assessment for pollution remediation.
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