ACS Applied Nano Materials
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2023
·
IF 5.9
Dongmei Jia,Yuejin Li,Huamin Cai,Yongzheng Duan,Jing Li,Chen Ling
Capture of heavy metal ions from aqueous solutions is a critical but challenging step in environmental treatment. In this work, NH2-MIL-101(Fe) nanoparticles were synthesized by simple solvothermal methods and applied to capture Cr(VI) anions from aqueous solutions. The results revealed that NH2-MIL-101(Fe) exhibited a high capture capacity (375.2 mg g–1) and an ultrafast capture rate (4 min reaching equilibrium). The competitive effects of coexisting ions such as Cl–, HCO3–, PO43–, Cd2+, Ca2+, and Cu2+ on Cr(VI) are very weak, suggesting that the adsorption selectivity significantly enhanced by loading amino groups on MIL-101(Fe). Density functional theory (DFT) calculation was performed to better understand the adsorption mechanism of Cr(VI), showing that the amino groups could increase the adsorption energy of Cr(VI) for enhancing the adsorption capacity. Based on powder X-ray diffraction, X-ray photoelectron spectroscopy, and DFT calculations, the Cr(VI) capture mechanism by NH2-MIL-101(Fe) nanoparticles was a combination of coordination between Fe and Cr(VI), electrostatic interaction between Cr2O72– and the protonated amino group, and reduction of Cr(VI) to Cr(III).
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RSC Advances
·
2018
·Vol. 8
·期 71
·41003-41011
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IF 2.936
Wen Bing Wu,Sun Xue,Jian Hua Chen,Xiao Li
Membrane separation technologies have great promising potential for applications in several industries. Metal–organic frameworks (MOFs), for their large surface areas, low framework densities, transition-metal ions in the skeleton and high pore volumes relative to other porous matrices, have great potential for the removal of sulfur from gasoline with high efficiency. In the present study, a novel porous membrane adsorbent MIL-101(Cr)/SA was prepared by immobilizing MIL-101(Cr) onto sodium alginate (SA) matrix, which can combine the size/shape selectivity of MIL-101(Cr) with the processability and mechanical stability of SA polymer. The physico-chemical properties of MIL-101(Cr)/SA were investigated by FT-IR, SEM, BET, XRD and EDX methods. To investigate the effects of some important factors on the adsorption behavior for thiophene, a batch of experiments were performed by changing the concentration of porogen polyethylene glycol in the MIL-101(Cr)/SA, solution temperature, initial thiophene concentration and contact time. Meanwhile, benzothiophene, thiophene and 3-methyl thiophene were used to test the selectivity of MIL-101(Cr)/SA. The MIL-101(Cr)/SA showed an excellent uptake capacity of 671 mg g−1 under the optimal adsorption conditions. Selectivity testing indicated that the uptake capacity of MIL-101(Cr)/SA follows the order of benzothiophene > thiophene > 3-methyl thiophene. Kinetics experiments indicated the pseudo-second-order model displayed good correlation with adsorption kinetics data. The Crank model showed that the intraparticle solute diffusion is the rate-controlling adsorption step. Regeneration experiment result shows that the prepared MIL-101(Cr)/SA has excellent adsorption and desorption efficiencies.
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PubMed
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NANO
·
2018
·
IF 1.1
Shipeng Yang,Siwei Peng,Chunhui Zhang,Xuwen He,Yaqi Cai
Nanoparticles of the semiconductor catalyst Cd x Zn 1 − x S were embedded into the metal organic framework MIL-101(Cr) to obtain Cd x Zn 1 − x S@MIL-101(Cr) nanocomposites. These materials not only possess high surface areas and mesopores but also show good utilization of light energy. The ultraviolet-visible diffuse reflectance patterns of Cd x Zn 1 − x S@MIL-101(Cr) nanocomposites showed that Cd 0 . 8 Zn 0 . 2 S@MIL-101(Cr) possessed good visible light response ability among the synthesized nanocomposites. The photocatalytic performance of the Cd x Zn 1 − x S@MIL-101(Cr) nanocomposites were tested via degradation and mineralization of methylene blue in neutral water solution under light irradiation using a 300W xenon lamp. As a result, using Cd 0 . 8 Zn 0 . 2 S@MIL-101(Cr) as a catalyst, 99.2% of methylene blue was mineralized within 30 min. Due to the synergistic effect of adsorption by the MIL-101(Cr) component and photocatalytic degradation provided by the Cd 0 . 8 Zn 0 . 2 S component, the Cd 0 . 8 Zn 0 . 2 S@MIL-101(Cr) catalyst displayed superior photocatalytic performance relative to Cd 0 . 8 Zn 0 . 2 S and MIL-101(Cr). Furthermore, Cd 0 . 8 Zn 0 . 2 S@MIL-101(Cr) possessed excellent stability during photodegradation and exhibited good reusability. The remarkable photocatalytic performance of Cd 0 . 8 Zn 0 . 2 S@MIL-101(Cr) is likely due to the effective transfer of electrons and holes at the heterojunction interfaces.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2019
·
IF 4.084
Guoru Li,Xiaobo He,Fengxiang Yin,Biaohua Chen,Huaqiang Yin
The development of highly efficient electrocatalysts with low cost for oxygen reduction reaction (ORR) is urgently required for metal-air batteries and fuel cells. In this work, Fe Co/MIL-101(Cr) with various molar ratios of Fe/Co as hybrid catalysts was prepared by a facile and mild impregnation method. MIL-101(Cr) increased the specific surface areas of the hybrid catalysts, thus improving the dispersion of Fe and Co species at their surfaces. The effects of Fe and Co species on ORR activity of the hybrid catalysts were investigated. It is found that the synergistic effects between the well-dispersed Fe and Co species contribute mainly to ORR activity. More specifically, Fe species exert a partial-charge-transfer-activation effect on Co ones, which reduces the charge transfer resistance and thus improves the catalytic activity . As a result, Fe Co/MIL-101(Cr) showed the excellent ORR activity, in which Co 50 Fe 50 /MIL-101(Cr) exhibited the superior ORR activity to the other prepared hybrid catalysts.
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INORGANICA CHIMICA ACTA
·
2018
·
IF 2.264
Yebin Guan,Ming Xia,Xiaohong Wang,Weicheng Cao,Alessandro Marchetti
Nano-sized NH 2 -MIL-53(Al) particles were conveniently synthesized in aqueous solution at ambient temperature with a widely applicable mixing method, and the morphology and character were examined with a series of techniques. XRD patterns and TEM images showed that the obtained NH 2 -MIL-53(Al) material possessed rod-like shape, which is different from those obtained from N, N-dimethyl formamide (DMF). This nano-sized NH 2 -MIL-53(Al) matrix displayed enhanced efficiency for adsorptive elimination of methyl blue molecules in aqueous solution.
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2019
·
IF 4.182
Qiang Wang,Congcong Wei,Dandan Li,Wenjun Guo,Dazhong Zhong,Qiang Zhao
Metal–organic frameworks (MOFs) have been widely used in the field of electrocatalysis in recent years. In most reports, an MOF is used as a sacrificial template to prepare a highly efficient electrocatalyst by calcination . Here, a series of FeNi bimetallic MIL-101 materials has been synthesized by a solvothermal method and directly applied for the oxygen evolution reaction (OER). These MOFs contain a large number of catalytically active MO 6 octahedra and exposed hydrophilic carboxyl groups, which are believed to enhance OER activity. In addition, after the introduction of Ni, the catalytic activity is significantly improved by synergy between the metals. Among the studied compositions, Fe 2 Ni-MIL-101 showed the best OER performance, requiring a low overpotential of just 237 mV to drive a current density of 20 mA cm −2 in 1 m KOH solution, corresponding to a low Tafel slope of 44.2 mV dec −1 . Moreover, the electrochemical properties remained virtually unchanged during a 40-h long-term stability test. These findings enrich the application of MOFs materials in the field of electrocatalysis.
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JOURNAL OF POROUS MATERIALS
·
2019
·Vol. 26
·期 6
·1607-1618
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IF 1.947
Hou Pengchao,Xing Guangjian,Han Dan,Zhao Yan,Zhang Gang,Wang Hao,Zhao Chang,Yu Chunna
MIL-101(Cr)/graphene aerogel (MIL-101(Cr)/GA) was synthesized using a two-step synthesis and used as a high efficient adsorbent for wastewater purification. The as-prepared MIL-101(Cr)/GA was characterized using XRD, FTIR and Raman spectroscopy, XPS and FESEM to investigate its structure, composition and morphology. MIL-101(Cr)/GA exhibited a 3D interconnected macroporous framework comprised of graphene sheets, on which MIL-101(Cr) particles were dispersed uniformly. Dyes, organic solvents and oils were used to evaluate the adsorption performance of MIL-101(Cr)/GA, which exhibited an excellent adsorption capacity for both anionic methyl orange (331.5 mg g −1 ) and cationic rhodamine B (345.7 mg g −1 ) as well as 51–101 times its own weight of various solvents/oils. In addition, the MIL-101(Cr)/GA showed superior recycling stability for dyes and a rapid adsorption rate for solvents/oils. The excellent adsorption performance was attributed to a synergistic effect between MIL-101 and the graphene aerogel. The kinetic behavior for adsorption observed for MIL-101(Cr)/GA was well-fitted by a pseudo-second-order kinetic model. It is envisaged that MIL-101(Cr)/GA will be a promising adsorbent for the removal of pollutants and wastewater purification.
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JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
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2019
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IF 3.261
Shengchao Miao,Zhenxing Zha,Ying Li,Xinxiang Geng,Jiahui Yang,Shihai Cui,Jing Yang
The novel semiconductor heterojunction of MIL-53(Fe)/BiOCl composite was first prepared through the solvothermal reaction. The prepared materials were characterized by Fourier transform infrared spectroscopy (FT-IR), X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), Brunner-Emmet-Teller (BET) and ultraviolet-visible diffuse reflectance spectroscopy (DRS). MIL-53(Fe)/BiOCl heterojunction is a kind of photoexcited materials and it accelerates the photoreactivity of BiOCl under the visible light irradiation. It was used to remove Rhodamine B (RhB) with the existence of persulfate (PS). The UV–vis spectrophotometer and the TOC detector show that the degradation rate and TOC removal efficiency of RhB (20 mg/L) are 99.5% and 69.4%within 30 min visible-light irradiation, respectively. Due to the proper band gap of material and the presence of electron acceptor, PS, the survival time of active radicals are increased. The active species h + , ·SO 4 − and ·OH are found to play the important roles during the reaction system. The possible mechanism for the RhB degradation of MIL-53(Fe)/BiOCl/PS is also proposed. Furthermore, the results of the material reusability for the degradation of RhB indicate that the MIL-53(Fe)/BiOCl has a good stability and can be used in the environmental water sample treatment.
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ENERGY & FUELS
·
2017
·
IF 3.091
Xuejiao Sun,Daofei Lv,Yongwei Chen,Ying Wu,Qihui Wu,Qibin Xia,Zhong Li
Chromium-based MIL-101 and graphite oxide (GO) composite (MIL-101@GO) was synthesized and applied for adsorption performances toward a series of aromatics (benzene, toluene, and ethylbenzene). Desorption activation energies of aromatics on this composite were evaluated based on temperature-programmed desorption (TPD) experiments. The results indicated that the aromatic uptakes on the composite increase with the carbon number at low pressure. In contrast, at high pressure, their adsorption capacities exhibit an opposite trend. The composite possesses high uptakes of the aromatics, which are approximately 1.8–6.0 times higher compared with conventional adsorbents. The desorption activation energies of the aromatics increase with the carbon number of aromatics. Additionally, the adsorption of ethylbenzene on the composite is highly reversible. More importantly, the MIL-101@GO composite exhibits enhanced thermal conductivity up to 0.369 W/mK at 303 K. The MIL-101@GO composite with high adsorption capacity, enhanced thermal conductivity, and efficient recyclability provided a promising candidate for practical applications in field of volatile organic compounds adsorption.
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Surfaces and Interfaces
·
2024
·
IF 5.7
Pengfei Zhu,Mengrong Geng,Shuang Qin,Heyang Cao,Zhenhong He,Xinhua Gao,Chuanyi Wang
The conversion of CO 2 into chemical products or fuels of great value always remains an outstanding challenge. Here, we report a heterojunction Fe@C/Ni 2 P composite catalyst obtained by preparing MIL-100(Fe) derived Fe@C confined Ni 2 P nanoparticles, which is applied to photothermal catalytic CO 2 hydrogenation with H 2 O. Without adding any sacrificial agents or co-catalysts, the optimal Fe@C/Ni 2 P sample shows higher yields for CO 2 -to-C 2 H 6 and CO 2 -to-CO yield of 5.83 μmol g −1 h −1 and 179.9 μmol g −1 h −1 than that of pristine Fe@C and Ni 2 P, respectively. The experimental results indicated that the obtained Fe@C/Ni 2 P can act as catalytic sites to adsorb, activate, and convert CO 2 under low-intensity LED light irradiation (420 nm) with a temperature of 200 ℃. The physical structure, photochemical properties and energy band structure of the Fe@C/Ni 2 P composite catalysts were investigated by XRD, XPS, FT-IR, TEM, BET, respectively. Furthermore, the reaction pathway of Fe@C/Ni 2 P photothermal catalytic CO 2 hydrogenation with H 2 O to C2 products and CO were systematically analyzed by in situ infrared spectroscopy (DRIFTS).
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JOURNAL OF MATERIALS CHEMISTRY
·
2012
·Vol. 22
·期 15
·7449-7455
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IF 5.968
Shu-Hui Huo,Xiu-Ping Yan
The adsorption of malachite green from aqueous solution on a highly porous metal–organic framework MIL-100(Fe) was studied in view of the adsorption isotherm, thermodynamics, kinetics, and regeneration of the sorbent. The adsorption isotherms of malachite green on MIL-100(Fe) followed the Freundlich model, and MIL-100(Fe) possessed heterogeneous surface caused by the presence of different functional groups on the surface. The adsorption of malachite green on MIL-100(Fe) is controlled by an entropy effect rather than an enthalpy change, and obeyed a pseudo-second-order kinetics. Analysis of the intraparticle diffusion plots revealed that more than one process affected the adsorption, and film (boundary layer) diffusion controlled the adsorption rate at the beginning. Evidence from zeta potential and X-ray photoelectron spectroscopic data showed that the adsorption of malachite green was also driven by electrostatic attraction and the interaction between the Lewis base –N(CH3)2 in malachite green and the water molecule coordinated metal sites of MIL-100(Fe). MIL-100(Fe) gave much higher adsorption capacity for malachite green than other conventional adsorbents such as activated carbon and natural zeolite. The high adsorption capacity, good solvent stability, and excellent reusability make MIL-100(Fe) attractive for the removal of MG from aqueous solution.
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Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Jiepeng Zhao,Yifei Ma,Zhaomin Tong,Mei Wang,Liantuan Xiao,Suotang Jia,Xuyuan Chen
Engineering photocatalyst crystal facets and constructing heterojunctions are effective strategies to improve photocatalytic activity. The amino-modified titanium-based metal–organic framework (MOF) NH 2 -MIL-125(Ti) (NM) has drawn extensive attention as a photocatalyst by virtue of its high specific surface area, abundant pore structure, and narrow bandgap. However, its catalytic activity is hindered by fast electron-hole recombination and limited light absorption. This study synthesizes NM with engineered crystal facets and Co 3 O 4 @NH 2 -MIL-125(Ti) (C-NM) composites with varying Co 3 O 4 loadings using a facile hydrothermal method. The impact of heterojunctions and facet design on photocatalytic CO 2 reduction under visible light is also studied. Results show that the C-NM, with exposed {111} facets and optimal Co 3 O 4 loading, demonstrates superior photocatalytic CO and CH 4 production rates of 21.64 μmol h −1 g −1 and 3.99 μmol h −1 g −1 , 2.1 and 1.6 times higher than those of NM {001} , respectively. Experimental characterization and density functional theory (DFT) analyses attribute the improved photocatalytic activity to several mechanisms. First, crystal facet modulation can optimize the active sites and specific surface area of the photocatalysts. Second, by loading the narrow-bandgap Co 3 O 4 nanoparticles, bandgap of the C-NM photocatalyst is further reduced, thereby enhancing the absorption and utilization of visible light. Finally, the NM/Co 3 O 4 heterostructure minimizes electron-hole recombination, significantly boosting CO 2 reduction efficiency.
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