COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2023
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IF 5.2
Guang-Yu Cui,Wei Zhang,Ji-Min Yang
Metal−organic framework (MOF)@graphene oxide (GO) composite materials possess the advantages of both GO and MOFs, and thus, they can be employed as effective dye adsorbents. This paper proposes a simple strategy for the preparation of MIL-101 @GO composite materials to effectively adsorb anionic dyes (Congo red, o-cresolsulfonphthalein, methyl orange, and acid chrome blue K) by adding GO to MIL-101 to form a nano-packed structure. The maximum adsorption uptakes of MIL-101 @GO were 2734.9, 484.5, and 1762.8 mg g –1 for Congo red, o-cresolsulfonphthalein, and methyl orange, respectively. These values significantly exceed the corresponding values of the original MIL-101 because of additional factors that promoted adsorption, namely hydrogen bonding and the presence of agglomerate pores. Only the maximum adsorption uptake for acid chrome blue K was lower than that of MIL-101, because of steric hindrance . Our analysis showed that the adsorption behavior of MIL-101 @GO toward Congo red, o-cresolsulfonphthalein, and methyl orange is governed by a synergistic interplay of hydrogen bonding, electrostatic interactions, π–π interactions, the adsorption space, and agglomerate pores in the composite, whereas the adsorption behavior toward acid chrome blue K is mainly limited by steric hindrance. Understanding these interactions may contribute to the development of improved sustainable composite adsorbents.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Liyan Chen,Meng Rong,Jiemiao Yu,Qiyu Meng,Shan Ni,Xia Wu,Li Wang,Huifang Xing,Huizhou Liu,Liangrong Yang
Due to the biotoxicity and ecological hazards of 2,4-toluene diamine (TDA) and 4,4′-methylene dianiline (MDA), it is the key process for upcycling polyurethane (PU) waste to remove them from the PU bio-hydrolysate with high selectivity and efficiency. Herein, MIL-53 series metal–organic frameworks (MOFs) were prepared and applied to remove aromatic diamines. Besides, the effects of their different structural units on the adsorption performance were investigated. Among the three metal nodes (Cr 3+ , Al 3+ , Fe 3+ ) of MIL-53, MIL-53(Al) demonstrated the highest adsorption capacities upon TDA (4.17 mmol/g) and MDA (2.00 mmol/g) due to its more μ 2 -OH sites and higher porosity. Compared with MIL-53(Al), DUT-4 and DUT-5 owned longer linkers but exhibited inferior aromatic diamine adsorption performance, which was ascribed to the more appropriate pore size and more μ 2 -OH sites of MIL-53(Al). Notably, MIL-53(Al) exhibited excellent selectivity towards aromatic diamines, while the removal efficiency reached over 90 %. In addition, spectral analysis before and after adsorption revealed the mechanism, which involved host–guest interactions, H-bonding interactions, and π-π stacking. The results indicate the great potential of applying the optimal MIL-53(Al) as an alternative adsorbent for removing hazardous aromatic diamines from the PU bio-hydrolysate.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2018
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IF 11.698
Munir Ahmad,Shuo Chen,Fei Ye,Xie Quan,Shahzad Afzal,Hongtao Yu,Xueyang Zhao
Metal-organic frameworks (MOFs) have received significant interest as a promising photocatalyst for environmental remediation due to its high surface area and porous nature. The small pores (<2 nm) in microporous MOFs help the adsorption of small molecules but limits diffusion and accessing of bigger molecules from MOF cavities, thus preventing their applications in some situation. The aim of this work is to fabricate mesoporous MOF composite with larger pore sizes (>2 nm) and open pore cavities that can provide right pathways for ingoing and outgoing of molecules during catalysis. Herein, we successfully report stable mesoporous MIL-100(Fe) loaded with ZnO NS by an in situ self-assembly method. The prepared samples were characterized by Brunauer–Emmett–Teller (BET) and N 2 adsorption-desorption isotherm to study their surface area and porosity. The catalytic performance of mesoporous MIL-100(Fe) was approximately 2–3 order of magnitude more than that of microporous MIL-100(Fe). Such higher catalytic activity in mesoporous MIL-100(Fe) can be ascribed to its mesocellular structure which can improve the molecular diffusion and accessibility inside MOF channels. The charge separation efficiency and photo-Fenton activity of mesoporous MIL-100(Fe) can further be increased by introduction of certain amount of ZnO NS and H 2 O 2 . Moreover, the as synthesized sample shows higher photo-Fenton degradation efficiency at lower pH value with certain amount of H 2 O 2 . Lastly, the possible catalytic mechanism has been tentatively proposed. This study not only used for the pollutants degradation but also provide useful platform for the application of mesoporous MOFs as an efficient photo-Fenton activity to various other fields.
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CHEMICAL ENGINEERING JOURNAL
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2019
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IF 8.355
Jichi Zhang,Hongsen Zhang,Qi Liu,Dalei Song,Rumin Li,Peili Liu,Jun Wang
Hollow metal-organic frameworks (MOFs) have attracted wide interest because of their unique core-shell structure. As a novel uranium adsorbent, diaminomaleonitrile (DAMN) functionalized double-shelled hollow (DSHM) metal-organic framework of chromium(III) terephthalate was prepared by a post-synthetic method of grafting amino group onto coordinatively unsaturated sites (CUS). TEM, XRD, nitrogen sorption and FT-IR spectrometry were used to characterize the obtained DAMN functionalized hollow MOF. The maximum capacity of uranium adsorption is 601 mg g −1 , which exceeds all known functionalized MIL-101 uranium adsorption materials. The optimal adsorption pH is 8 which is close to the pH of seawater. Furthermore, the high selectivity of uranium and high adsorption rate in simulated seawater provide a promising prospect to introduce DSHM-DAMN for the extraction of uranium from seawater. In this work, we first applied hollow MOF for uranium adsorption, which greatly improves the uranium adsorption performance of MOF materials; we also explored the practical application of hollow MOF materials.
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NEW JOURNAL OF CHEMISTRY
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2019
·Vol. 43
·期 24
·9725-9731
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IF 3.069
Suresh Mutyala,Sobhy M. Yakout,Shebl S. Ibrahim,Madhavi Jonnalagadda,Harisekhar Mitta
Iron metal–organic framework, MIL-100(Fe) was prepared by a hydrothermal method and used as a support to incorporate diethylenetriamine (DETA) for the study of CO2 adsorption and separation of CO2/N2. All synthesized adsorbents were characterized by PXRD, N2 adsorption–desorption isotherms, FT-IR, TGA, SEM, and elemental analysis. Structural characterization results have revealed that the structure of MIL-100(Fe) was not changed by the incorporation of diethylenetriamine. The CO2 adsorption capacities were 29 cm3 g−1 and 41 cm3 g−1 at 298 K, 1 bar for MIL-100(Fe) and DETA–MIL-100(Fe), respectively. Adsorption of CO2 on DETA–MIL-100(Fe) was higher than that on MIL-100(Fe). The enhancement was due to the presence of amine groups which could form ammonium carbamate by interaction with CO2. Similarly, the N2 adsorption capacities were 3 cm3 g−1 and 0.9 cm3 g−1 at 298 K, 1 bar for MIL-100(Fe) and DETA–MIL-100(Fe), respectively. The decrease in N2 adsorption capacity was due to the decrease in surface area. The selectivity of CO2/N2 on DETA–MIL-100(Fe) was four times higher than that on MIL-100(Fe). The heat of CO2 adsorption was 74.2 kJ mol−1 at low coverage of CO2 on DETA–MIL-100(Fe) and the CO2 adsorption capacity was constant in each adsorption cycle over the same adsorbent.
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POLYHEDRON
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2019
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IF 2.284
Ning Tian,Yifang Dai,Qing Liu,Wei Dai
A general synthetic strategy for HS-Fe 3 O 4 @MIL-53(Al) adsorbent has been developed in this work. The composite material exhibits an efficient capture performance for rubidium ion due to sulfhydryl group and magnetic Fe 3 O 4 doped in its porous cavity. The results of X-ray diffraction, scanning electron microscopy, Fourier transform infrared spectroscopy, and N 2 adsorption–desorption proved that the HS-Fe 3 O 4 was immobilized in the composite material. High Rb + uptake capacity over the HS-Fe 3 O 4 @MIL-53(Al) is attributed to the exchange of acidic protons between the sulfhydryl group and the Rb + . The pseudo-second-order and Freundlich model could make a good description of the adsorption process. The Rb + sorption selectivity was moderately influenced by any co-ions effect (K + , Na + and Cs + ) due to HS-Fe 3 O 4 doped. These results reveal that our novel composite material might be a promising industrial adsorbent for Rb + capture.
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APPLIED ORGANOMETALLIC CHEMISTRY
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2018
·Vol. 32
·期 4
·e4285
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IF 3.581
Zhiquan Yang,Jie Ding,Jinna Feng,Chong He,Ying Li,Xiaowen Tong,Xiaojun Niu,Hongguo Zhang
Because of their desired features, including very specific surface areas and designable framework architecture together with their possibility to be functionalized, Metal Framework (MOF) is a promising platform for supporting varied materials in respect of catalytic applications in water treatment. In this work, a novel visible-light-responsive photocatalyst that comprised BiVO 4 together with MIL-125(Ti), was synthesized by a two-step hydrothermal approach. The characterization of as-obtained samples as performed by X-ray diffraction, scanning electron microscopy, high resolution transmission electron microscopy, Fourier transform infrared spectroscope, X-ray photoelectron spectroscopy and ultraviolet-visible diffuse reflection spectra. Rhodamine B was selected being a target for the evaluation of the photocatalytic function of as-developed photocatalyst. The photocatalytic reaction parameters, for example, the content of BiVO 4 as well as initial concentration of Rhodamine B was researched. The composite photocatalyst possessing Bi:Ti molar ratio of 3:2 brought to light the fact that the greatest photocatalytic activity had the ability to degrade 92% of Rhodamine B in 180 min. In addition to that, the BiVO 4 /MIL-125(Ti) composite could keep its photocatalytic activity during the recycling test. The phenomenon of disintegration of the photo-generated charges in the BiVO 4 /MIL-125(Ti) composite was brought to discussion as well.
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RSC Advances
·
2018
·Vol. 8
·期 49
·27623-27630
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IF 2.936
Xiaoli Huang,Qi Hu,Lei Gao,Qirui Hao,Peng Wang,Dongli Qin
A metal–organic framework, MIL-101(Cr), was used to adsorb sulfamethoxazole (SMZ) in water and activated persulfate (PS) oxidation was investigated to regenerate SMZ-saturated MIL-101(Cr). Adsorption and oxidation were combined in this study. MIL-101(Cr) was characterized by SEM, BET, XPS and FT-IR analyses. Effects of various operating parameters on adsorption efficiency were studied. The dosages of persulfate for SMZ desorption and oxidation were investigated. The results showed that the recommended pH was 6–8 for SMZ adsorption and optimum MIL-101(Cr) dosage was 0.1 g L−1. SMZ adsorption by MIL-101(Cr) was a spontaneous process and nearly exothermic. Saturation adsorption capacity was achieved in 180 s and the adsorption followed the pseudo-second-order model. The maximum adsorption amount of MIL-101(Cr) to SMZ was 181.82 mg g−1 (Langmuir). MIL-101(Cr) also showed good adsorption capacities for sulfachloropyridazine (SCP), sulfamonomethoxine (SMM), and sulfadimethoxine (SDM). Persulfate was helpful for SMZ desorption from the surface of saturated MIL-101(Cr) and sufficient persulfate could simultaneously oxidize the SMZ. XPS analysis showed that the structure of MIL-101(Cr) was stable after the persulfate oxidation process. Regenerated MIL-101(Cr) had the same level of adsorption capacity as fresh MIL-101(Cr). An adsorption–oxidation combined process may be set up based on the results. This study provides basic data for the deep treatment of organic micropollutants in urban water bodies.
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Catalysts
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2018
·Vol. 8
·期 9
·394
·
IF 3.465
Tian Zhao,Ming Dong,Ling Yang,Yuejun Liu
Nowadays, the controllable synthesis of stable hierarchical metal–organic frameworks (MOFs) is very important for practical applications, especially in catalysis. Herein, a well-known chromium–benzenedicarboxylate metal–organic framework, MIL-101(Cr), with a stable hierarchical structure, was produced by using phenylphosphonic acid (PPOA) as a modulator via the hydrothermal method. The presence of phenylphosphonic acid could create structural defects and generate larger mesopores. The synthesized hierarchical MIL-101(Cr) possesses relatively good porosity, and the larger mesopores had widths of 4–10 nm. The hierarchical MIL-101(Cr) showed significant improvement for catalytic activity in the oxidation of indene. Further, the presence of a hierarchical structure could largely enhance large dye molecule uptake properties by impregnating.Keywords:MIL-101(Cr);phenylphosphonic acid;hierarchical;enhanced catalytic activity;large molecule uptake
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MICROCHIMICA ACTA
·
2016
·Vol. 183
·期 7
·2235-2240
·
IF 4.831
Yang Xiaoqing,Xia Yan
Mass spectrometry (MS) is the most powerful tool in phosphoproteomics research. However, phosphopeptides usually are present in low concentrations and their preconcentration therefore is highly desired. We describe a two-step method for the synthesis of a metal organic framework of the type MIL-101(Cr) that is modified with urea (then designated as MIL-101(Cr)-UR 2 ). It possesses large surface area, good solvent stability and high affinity for some phosphates. Due to the presence of modified urea functions, this material allows for selective and effective enrichment of phosphorylated peptides. It was successfully applied to the enrichment of phosphopeptides from non-fat-milk. The method was applied to the detection of phosphopeptides in a tryptic digest of β-casein where is showed a detection sensitivity as low as 10 −10 M.
A two step method was designed to synthesis MIL-101(Cr)-UR 2 and the prepared green solid was successfully applied to recognize phosphopeptides. (Amino functionalized metal-organic framework (MOF-NH 2 ); urea modified metal-organic framework (MOF-UR 2 ); matrix-assisted laser desorption/ionization time of flight mass spectrometry (MALDI-TOF MS))
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Journal of Energy Chemistry
·
2016
·
IF 2.322
Xiaofang Liu,Hu Li,Hu Pan,Heng Zhang,Shan Huang,Kaili Yang,Wei Xue,Song Yang
In this work, a series of MIL-101-SO 3 H( x ) polymeric materials were prepared and further used for the first time as efficient heterogeneous catalysts for the conversion of fructose-based carbohydrates into 5-ethoxymethylfurfural (EMF) in a renewable mixed solvent system consisting of ethanol and tetrahydrofuran (THF). The influence of –SO 3 H content on the acidity as well as on the catalytic activity of the porous coordination polymers in EMF production was also studied. High EMF yields of 67.7% and 54.2% could be successively obtained from fructose and inulin in the presence of MIL-101-SO 3 H (100) at 130 °C for 15 h. The catalyst could be reused for five times without significant loss of its activity and the recovery process was facile and simple. This work provides a new platform by application of porous coordination polymers (PCPs) for the production of the potential liquid fuel molecule EMF from biomass in a sustainable solvent system.
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JOURNAL OF HAZARDOUS MATERIALS
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2015
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IF 4.529
Xubiao Luo,Tingting Shen,Lin Ding,Weiping Zhong,Jianfeng Luo,Shenglian Luo
A novel thymine-functionalized MIL-101 (MIL-101-Thymine) material was synthesized using a post-synthesis method to remove mercury at a high efficiency. MIL-101-Thymine was successfully prepared in this work and was confirmed by several characterization methods, such as 13 C nuclear magnetic resonance, X-ray diffraction, and infrared spectroscopy. The Hg 2+ adsorption agreed well with the Langmuir model, and the maximum adsorption capacity was 51.27 mg/g. The adsorption rate fit with the pseudo-second-order kinetic model. Furthermore, MIL-101-Thymine exhibited excellent selectivity towards Hg 2+ over other cations, and the maximum value of the selective coefficient reached 947.34; this result is very likely due to the highly selective interactions of T-Hg 2+ –T in MIL-101-Thymine. The result of X-ray photoelectron spectroscopy also showed that Hg 2+ was coordinated with the N of thymine in MIL-101-Thymine. Moreover, the results of the thermogravimetric analysis and adsorption experiments showed that the Hg atom was two-coordinated with the thymine group. MIL-101-Thymine was used to remove trace Hg 2+ in real water samples, and satisfactory recoveries were obtained.
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