ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Chenghan Ji,Hang Yu,Junhe Lu,Yi Ren,Lu Lv,Weiming Zhang
Adsorption as a desalination approach has the advantages of energy efficiency, low cost, and operational convenience, but its practical application is limited by low desalination capacity, consumption/disposal of strong acids/bases as regeneration reagents, and poor reusability. Herein, we synthesized a thermo-regenerable salt absorbent by grafting ethylenediaminetetraacetic acid (EDTA) onto a metal–organic framework (MOF), MOF-808-EDTA, which could rapidly adsorb NaCl within 30 min from saline water at 25 °C with a desalination capacity as high as 9.4 mmol/g. Moreover, the saturated adsorbent could be facilely regenerated in 80 °C water. Fourier transform infrared spectroscopy and derivative thermogravimetry revealed that temperature-regulated proton transfer between amino and carboxyl groups was the mechanism of thermo-regeneration. EDTA on MOF-808-EDTA appears in a zwitterionic state in water at room temperature, which allowed simultaneous adsorption of Na+ and Cl–. At elevated temperature, it returned to a nonionic state accompanied by the desorption of ions. A similar temperature-dependent adsorption–regeneration process was also observed for other salts, including LiCl, KCl, CaCl2, and MgCl2. Column experiments of brackish groundwater showed that 1 g of MOF-808-EDTA could produce ∼106 mL of fresh water (total dissolved solids < 600 mg/L) without significant capacity loss after 10 successive adsorption–regeneration cycles. This study is the first to propose an EDTA-based MOF for desalination and indicates the potential of MOF-808-EDTA as a green adsorbent for sustainable water desalination.
研究领域:
材料科学
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环境科学
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化学工程
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DOI
PubMed
高影响因子
JOURNAL OF ENVIRONMENTAL ENGINEERING
·
2024
·Vol. 150
·期 11
·04024050
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IF 1.6
Huanglong Zhuang,Guiyang Yan,Jiwei Wang,Zhuang Hu,Siqi Yan,Yinkai Sun,Tuanyu Guo,Jianshe Hu,Aikebaier Reheman
This study presents a groundbreaking composite adsorbent, STB@MOF-808-SH, developed through the innovative amalgamation of thiol-functionalized metal-organic framework material (MOF-808-SH) with sulfur-doped C3N4 tubular bundles (STB), targeting the effective elimination of toxic mercury [Hg(II)] ions from polluted water. Our investigation explores crucial determinants of the adsorption process, including pH, initial Hg(II) concentration, and the impact of coexisting ions, while revealing the significant enhancement in mercury ion removal efficiency and adsorption capacity due to the synergistic interaction between STB and MOF-808-SH. Remarkably, under optimal conditions at pH 4.0, STB@MOF-808-SH achieves a removal rate of 91.35% and an impressive adsorption capacity of 228.38 mg/g. These outcomes suggest that the development of the STB@MOF-808-SH composite adsorbent introduces a novel and efficacious approach to tackling water pollution issues, highlighting its potential as a cost-effective and efficient solution for the remediation of toxic Hg(II) ions in wastewater.
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
CATALYSIS TODAY
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2020
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IF 5.825
Yulong Gu,Wei Xu,Yinyong Sun
The development of active oxidative desulfurization (ODS) catalysts is of practical importance. Recently, MOF-808(Zr) has been attempted to use as ODS catalyst due to its various advantages. However, generally MOF-808(Zr) prepared by conventional method was less active in the oxidation reactions due to the lack of defect sites in the structure. In this contribution, we report that the catalytic oxidative performance of MOF-808(Zr) can be enhanced by acid treatment due to the formation of defect sites resulting from the partial removal of organic linkers in the structure. During the experiment, the effect of acid concentration, treatment time, the addition amount of oxidant and reaction parameters on the performance of MOF-808(Zr) was studied. The catalytic results show that MOF-808(Zr) treated with 0.4 M HCl for 1h can catalyze the oxidation of dibenzothiophene completely at 60°C in 15 min. The activity (mole number of converted DBT per hour per unit mass) is 70 mmol h −1 g −1 , which is much higher than that (45 mmol h −1 g −1 ) of parent MOF-808(Zr). In addition, the catalyst can be reused several times without obvious loss of catalytic performance.
研究领域:
材料科学
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催化化学
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
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IF 8.1
Kaili Shi,Honghao Su,Keke Liu,Yatao Zhang,Junyong Zhu
Zr Ⅳ -based metal–organic frameworks (MOFs)–featuring exceptional water stability, large surface area, and structural tunability–hold promise for efficient antibiotics adsorption from water. However, their inherent positive charge in neutral environments and the harsh conditions required for their synthesis hinder their effective removal of cationic antibiotics. To address this challenge, a green one-pot synthesis approach was proposed to fabricate phosphotungstic acid-functionalized MOF-808 (termed as PTA@MOF-808) at room temperature for elevated antibiotic adsorption. This approach not only leverages the strong electronegativity of PTA to improve electrostatic interactions and π-π stacking but also finely tailors the pore size of MOF-808, resulting in enhanced adsorption capacity of PTA@MOF-808. The influence of PTA loading, solution pH, and absorbent dosage on the performance of PTA@MOF-808 were studied in detail. Adsorption experiments demonstrated that PTA@MOF-808 outperformed unmodified MOF-808 in removing various positively charged antibiotics, with 5 % PTA@MOF-808 exhibiting maximum adsorption capacities of 548.1 mg g −1 and 482.9 mg g −1 , for DOX and TCHC, respectively. The adsorption process followed the Langmuir isothermal model and the pseudo-second-order kinetic equation. Furthermore, the composite PTA@MOF-808 displayed excellent reusability after multiple adsorption–desorption cycles. These findings highlight the potential of PTA@MOF-808 as a promising absorbent for removing specific antibiotics from water, with significant implications for wastewater treatment.
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
ANALYTICAL CHEMISTRY
·
2025
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IF 6.7
Yuan Qin,Huimei Liang,Jia Wu,Zheyang Chi,Shulin Zhao,Fanggui Ye
Natural enzyme cascades, including the same and different kinds of enzymes, have been widely used in biosensing. However, it is still a challenge for nanozymes, the mimics of natural enzymes, to achieve biosensing with different types of enzyme-like activities based on cascade reactions, such as hydrolase and oxidoreductase. Considering the characteristics of the multienzyme-like activity of some nanozymes, as a proof of concept, this study demonstrates a Cu/Ce-MOF-808 nanozyme as a self-cascade catalyst with hydrolase-like and catechol oxidase-like activities. Taking organophosphorus pesticides as an example, we constructed a self-cascade catalytic reaction for the one-step colorimetric detection of isocarbophos. Specifically, the hydrolase-like activity of Cu/Ce-MOF-808 can hydrolyze isocarbophos to produce colorless isopropyl salicylate, which is further oxidized by the catechol oxidase-like activity of Cu/Ce-MOF-808 and complexed with 4-aminoantipyrine (4-AAP) to produce red quinoneimine under neutral conditions with illumination. Thus, a colorimetric strategy for sensitive isocarbophos analysis is developed, with a linear range of 0.90–400.00 μg·mL–1 and a detection limit of 0.42 μg·mL–1. This research presents a new approach to the design and synthesis of nanozymes and has great application potential in the field of nanozyme cascade biosensing.
研究领域:
生物化学
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纳米生物学
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分析化学
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产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Chenghan Ji,Yi Ren,Hang Yu,Ming Hua,Lu Lv,Weiming Zhang
Mercury pollution poses a serious threat to the ecological environment and public health due to its high toxicity and persistence, but there is still a lack of rapid and effective Hg(II) removal technology, especially emergency response of Hg(II) leakage. Herein, an effective metal-organic framework adsorbent, MOF-808-SH, was fabricated by grafting thioglycollic acid on MOF-808 for Hg(II) removal. The MOF-808-SH demonstrated high adsorption capacity of 977.5 mg/g, impressively ultrafast adsorption kinetics (C 0 = 10 mg/L, removal > 99 % in 10 s) with a rate constant k of 36.89 g mg −1 min −1 , which is dozens of times faster than that of ever reported Hg(II) adsorbents. Batch experiments show that MOF-808-SH exhibits high selectivity toward Hg(II) with a distribution coefficient K d as high as 5.0×10 6 mL/g. Moreover, MOF-808-SH exhibits excellent recyclability with a negligible loss of capacity after 6 adsorption-regeneration cycles. Fourier transform infrared spectroscopy (FTIR) and X-ray photoelectron spectrometry (XPS) unveil that the –SH groups in MOF-808-SH are the key adsorption sites, and specific inner-sphere coordination with Hg(II) is responsible for the high selectivity. In addition, large surface area, well-developed porous structures and high –SH loading of MOF-808-SH reasonably explains ultrafast kinetics and high adsorption capacity for Hg(II). This study indicates the potential of MOF-808-SH to remove Hg(II) 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
高影响因子
ChemSusChem
·
2023
·Vol. 16
·期 24
·e202300864
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IF 8.4
Chen Zhang,Tingyu Su,Xinqi Zhang,Duoyong Zhang,Tao Xuan,Liwei Wang
Graphical A kind of ionic liquid, namely deep eutectic solvents, are introduced to load on the surface of porous MOF-808 core as membranes to construct porous core-membrane microstructured nanomaterials for CO 2 capture at room temperature with the sorption mechanism coupling of diffusion, physisorption, and chemisorption. It shows excellent development potential for future application in CO 2 capture. A series of porous core-membrane microstructured nanomaterials, constructed of a deep eutectic solvent (DES) membrane and porous MOF-808 core via liquid surface tensions and electrostatic interactions, are introduced for carbon dioxide capture with the sorption mechanism coupling diffusion, physisorption, and chemisorption. MOF-808 as the porous core considerably improves the diffusion interactions for DES membranes, hence significantly enhancing the sorption performance of DESs. Although the DES consisted by monoethanolamine and tetrapropylammonium chloride (MEA-TPAC-7) has the highest sorption capacity among all DESs, it is only 4.39 mmol g −1 at 2.4 bar and further attenuates by fastidious diffusion interactions when increasing viscosity or dose. The sorption capacities of DES@MOF-120 are 5.18 mmol g −1 at 3.0 bar and 4.78 mmol g −1 at 2.4 bar without apparent sorption hysteresis in pressure swing sorption, which are substantially improved contrasted to MEA-TPAC-7. The sorption isotherms are reconstructed via Sips models considering surface heterogeneity with regression correlation coefficients over 0.9454 to forecast maximum sorption capacity over 6.33 mmol g −1 .
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
SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Honghao Su,Jingwei Hou,Junyong Zhu,Yatao Zhang,Bart Van der Bruggen
Zr IV -based metal–organic frameworks (MOFs) featuring distinguished water stability, large surface area, and intriguing functionalities have immense potential for practical usage. However, conventional MOF synthesis approaches generally require high reaction temperatures and organic solvents to initiate and template the nucleation and growth, hindering sustainable and cost-effective manufacturing and application of Zr-based MOFs. In this study, a scalable, room-temperature and aqueous synthesis of MOF-808—a Zr-MOF extensively explored as an adsorbent in both academic and industrial sectors—was reported. A rational use of water/formic acid (FA) as a green co-solvent enabled the formation of Zr 6 -cluster in an aqueous phase, thereby facilitating subsequent coordination with H 3 BTC to yield well-crystallized MOF-808. The effects of the water/FA volume ratio, the total solvent volume, and reaction time on the physicochemical properties of MOF-808 were studied. The optimized synthesis conditions (FA/water = 2.7:8.1, and reaction time = 24 h) resulted in the synthesis of MOF-808 with good hydrophilicity, excellent stability, high surface area, and weak positive charges. Moreover, this synthesis approach was successfully upscaled, yielding 11.5 g of MOF-808 at a magnification factor of 48. Notably, MOF-808-V 10.8 exhibited an impressive adsorption capacity for Congo Red (ca. 1500 mg/g) and demonstrated selective fractionation of dye mixtures, suggesting their potential application in dye wastewater treatment. This methodology is expected to provide guidance for aqueous and scalable fabrication of Zr-MOFs towards water-related environmental applications.
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
ACS Applied Materials & Interfaces
·
2019
·
IF 8.456
Wen Zhang,An Bu,Qingyuan Ji,Luofu Min,Song Zhao,Yuxin Wang,Jing Chen
We report a class of pKa-directed, precise incorporation of phosphonate ligands into a zirconium-based metal–organic framework (Zr-MOF), MOF-808, via ligand exchange. By replacing of formate ligands with methylphosphonic acid (MPA), ethanephosphonic acid (EPA), and vinylphosphonic acid (VPA), whose pKa values are slightly higher than that of the benzenetricarboxylic acid (BTC) linker in MOF-808, daughter MOFs can be synthesized without controlling the stoichiometric amounts of added MPA. The methylphosphonate MOFs (808-MPAs) demonstrate high porosities, with only small changes in the pore diameter and specific surface area when compared with the parent MOF-808. PXRD patterns and structure refinements indicate the expansion of the lattice for all MOFs after decorating with methylphosphonate ligands. The XPS spectra reveal a charge redistribution of the Zr6 node after ligand exchange. FTIR and 31P MAS NMR spectra, combined with DFT calculation, suggest that the methylphosphonate ligand is connected to the Zr6 node as CH3P(O)(OZr)(OH) species with an accessible acidic P–OH group. Besides, 808-MPAs demonstrate excellent chemical stability in concentrated HCl, concentrated HNO3, hot water, and 0.2 mol/L trifluoroacetic acid solutions. Impressively, 808-MPAs show ultrafast adsorption performance for uranyl ions using the ion-exchange property of P–OH sites in their cavity environment, with an equilibrium time of 10 min, much quicker than the previous adsorbents. The present study demonstrates a series of important proof-of-concept examples of the pKa-directed Zr-MOFs with tunable phosphonate-terminated ligands, which can extend to other phosphonate-functionalized Zr-based framework platforms in the near future.
研究领域:
材料科学
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环境科学
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化学工程
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产品关联
DOI
PubMed
高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2022
·Vol. 29
·期 26
·39427-39440
·
IF 5.19
Wang Cheng,Li Airong,Ma Yuling,Qing Shenglan
Due to the increasingly serious environmental problems caused by the combustion of sulfides in fuel, deep desulfurization of fuel became particularly urgent. Herein, the catalyst (PMA@MOF-808) of the Zr-based metal–organic framework (MOF-808) encapsulating phosphomolybdic acid (PMA) was prepared via a one-pot hydrothermal method. Besides, the formate ions of PMA@MOF-808 were removed by posttreatment with methanol, resulting in formate-free PMA@MOF-808-H catalysts with unsaturated open metal sites. The as-synthesized catalysts were systematically characterized by XRD, FT-IR, SEM, BET, TGA, 1 H NMR and XPS. The catalysts were also applied in catalytic oxidation desulfurization of fuel. The results indicated that the introduction of PMA and the removal of formate ions can improve the desulfurization performance of catalysts. Formate-free 0.2-PMA@MOF-808-H catalyst can reach 100% desulfurization rate for DBT. Besides, the kinetic properties were studied, and the apparent activation energy was 29.34 kJ/mol. Graphical abstract
研究领域:
材料科学
·
环境科学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF ENVIRONMENTAL MANAGEMENT
·
2025
·
IF 8.4
Xiao-Jun Dai,Yi-Ting Chen,Wen-Ge Zhang,Shu-Xuan Li,Wen-Rui Zhang,Xiang-Hua Qi,Chun-Hui Gong,Peng Wang,Man-Li He,Yi Yang
Radioactive iodine (I 2 ) is a potential risk to environmental safety and human health. The design of efficient and stable functional materials for I 2 capture remains a challenge. In this work, a simple in-situ impregnation method is used to load Ionic Liquid (IL)-[C 2 mim][Tf 2 N] into the pores of MOF-808, named IL@MOF. IL@MOF exhibit excellent I 2 removal performance (2.61 g/g), which is 1.75 and 21.75 times higher than that of MOF-808 and [C 2 mim][Tf 2 N], respectively. This is attributed to the excellent pore structure of MOF-808 and the abundant heteroatom adsorption sites of IL. After modification with hydrophobic IL, IL@MOF exhibit good adsorption performance in high humidity environment. I 2 is retained within IL@MOF in the forms of I 3 − (85 %) and I 2 (15 %). The formation of I 3 − is attributed to charge transfer between the unsaturated site, the heteroatom (N, O, S, F) adsorption site and I 2 within IL@MOF. In addition, the adsorption sites on the IL@MOF surface and adsorption energy are investigated by Density Functional Theory (DFT). Finally, this study provides ideas and guidance for designing MOF-based composites for the effective immobilization of radioiodine.
研究领域:
环境科学
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材料科学
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核工程
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化学工程
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物理化学
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产品关联
DOI
PubMed
高影响因子
SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
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2021
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IF 4.098
Xiaoting Zhang,Ying Li,Lei Zhang
Dyes detection remains a serious task because of their high toxicity. In present work, designed Eu 3+ functionalized Zr-metal-organic framework (Eu 3+ @Zr-MOF-808) as fluorescent probe was constructed via post-synthetic modification (PSM) for rapid monitoring four most commonly used dyes (malachite green (MG), brilliant green (BG), alizarin red S (ARS), indigo red (IDR)). Systematic exploring on the sensing mechanism reveals that fluorescence resonance energy transfer (FRET) for BG, MG and IDR and inner filter effect (IFE) for ARS contribute to the realization of the fluorescence quenching process. It exhibits excellent sensing performances with low limit of detection (LOD) of 32, 58, 77 and 133 nM for BG, IDR, MG and ARS, respectively. The as-constructed Eu 3+ @Zr-MOF-808 was demonstrated to be a highly sensitive probe for screening of MG in fish pond and IDR in printing wastewater with satisfying results. Moreover, a portable test reagent bottle has been developed for visual on-site screening of sample containing dyes with naked eyes under UV light. This is the first attempt to construct the Eu 3+ @Zr-MOF-808 probe for sensing multiple dyes in real samples and demonstrates promising applications in water quality monitoring.
研究领域:
环境科学
·
分析化学
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产品关联
DOI
PubMed
高影响因子
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