CHEMISTRY AND ECOLOGY
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2024
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IF 1.3
Zhenpeng Li,Dongmei Yan,Jun Li,Ziwei Mai,Fuchuan Huang
Hexavalent chromium (Cr(VI)) is regarded as a water pollutant because of its high toxicity in aquatic environments. In this study, polyethyleneimine-functionalised NH2-MIL-101(Cr) (PEI@NH2-MIL-101(Cr)) was fabricated by a facile wet impregnation method, and its effectiveness at removing Cr(VI) from wastewater was systematically investigated. As suggested by the experimental findings, pH was a significant determinant of Cr(VI) uptake by the fabricated PEI@NH2-MIL-101(Cr). Preferable depiction of adsorption system was achievable with the Langmuir adsorption model and the pseudo-order 2 kinetic model. At 288, 298, and 308 K, the highest adsorbability values were 241.55, 310.56, and 408.16 mg g−1, respectively. Processes like electrostatic attraction, reduction and chelation helped promote the Cr(VI) elimination. SO42− ions had a relatively large impact on the Cr(VI) adsorption compared with other coexisting ions such as NO3−, Cl− and H2PO4−1. Because of its properties of high adsorption capacity and Cr(VI) detoxification, the potential of PEI@NH2-MIL-101(Cr) in the Cr(VI) elimination from wastewater appears to be promising.
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
JOURNAL OF SOLID STATE CHEMISTRY
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2022
·
IF 3.656
Lijun Guo,Feifei Li,Jianxin Liu,Rui Li,Zhuobin Yu,Qing Xi,Lulu Zhang,Yaru Li,Caimei Fan
Morphology regulation is a simple way to improve photocatalytic activity. In this work, a MIL-101(Fe) photocatalyst with cracked spindle morphology has been successfully prepared by EG pre-coordination solvothermal method . The cracking degree of MIL-101(Fe) can be regulated by adjusting pre-coordination time. The MIL-101(Fe) with the optimal uniform crack displays a best NH 3 evolution rate of 592 μmol h −1 g −1 under the visible light irradiation . Cracked MIL-101(Fe) is similar to a semi-exposed model, which can increase the number of reactive sites, improve refraction and reflection of light, and ultimately enhance the photocatalytic nitrogen fixation activity. This work developed a convenient strategy to improve the photocatalytic activity of nitrogen reduction by controlling morphology.
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
高影响因子
CANADIAN JOURNAL OF CHEMICAL ENGINEERING
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2022
·Vol. 101
·期 6
·3262-3272
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IF 2.5
Dongmei Jia,Jia Guo,Jing Li,Yongzheng Duan
The composite of CuO coated MIL-101(Fe) (CuO@MIL-101(Fe)) was successfully prepared using a one-pot hydrothermal technology. X-ray diffraction (XRD), Fourier transform infrared spectrum (FTIR), scanning electron microscopy (SEM), energy dispersive spectroscopy (EDS), Brunauer–Emmett–Teller (BET), and TG technologies were used to characterize its structural, morphological, and physicochemical properties. CuO@MIL-101(Fe) exhibited a better pH adaptivity, a faster removal ratio of 95.8% for glyphosate within 10 min at pH 7, and a higher selectivity of adsorption capacity, even reaching 231.6 and 233.5 mg g −1 with coexisting Cl − (10 mmol L −1 ) and SO 4 2− (10 mmol L −1 ). The enhanced adsorption performances of CuO@MIL-101(Fe) may be caused by Cu forming a coordination interaction with glyphosate. A possible mechanism of glyphosate removal was discussed on the basis of the FTIR and X-ray photoelectron spectroscopy (XPS) analysis. CuO@MIL-101(Fe) composite would be more favourable to capture glyphosate from 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
Materials Today Communications
·
2024
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IF 3.7
Chunlong Qiu,Haiyang Sun,Yeyang Ni,Zhenjiang Dou,Ming Xia,Zhaoyang Fei,Zhuxiu Zhang,Mifen Cui,Qing Liu,Xu Qiao
The impressive water stability demonstrated by MIL-101(Cr) highlights its considerable potential for the effective elimination of organic contaminants from wastewater. Nevertheless, the limited availability of adsorption sites within MOFs leads to an unsatisfactory capacity for tetracycline (TC) adsorption. In this case, the lanthanum modified MIL-101(Cr) porous adsorbents, termed as nLa-MIL-101(Cr), were successfully synthesized using a post-synthetic modification method. Through various characterization analyses, it was confirmed that lanthanum exists in the form of La(OH) 3 within the adsorbents, and all adsorbents also preserved the original structure as MIL-101(Cr). The results of static adsorption experiments demonstrated that, compared to the original material, the adsorption capacity of 1La-MIL-101(Cr) for TC increased by 3.5 times. Further experiments demonstrated that the adsorbent exhibits remarkable ion interference resistance and cycle stability. Finally, based on X-ray photoelectron spectroscopy, the adsorption mechanism was primarily attributed to the coordination between TC molecules and metals active site, while electrostatic interactions also played a significant role in the process. This study has developed a highly efficient adsorbent for the treatment of TC-contaminated wastewater, which reflects promising practical application prospects.
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
JOURNAL OF SOLID STATE CHEMISTRY
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2022
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IF 3.656
Lei Ma,Feifei Zhang,Kunjie Li,Yingying Zhang,Zhiqiang Song,Li Wang,Jiangfeng Yang,Jinping Li
The capture of N 2 O from CO 2 by an adsorption-based mechanism remains a significant challenge due to their similar molecular sizes and physical properties. Although substituent engineering has been widely employed for the selectivity regulation and improvement of gas mixtures in metal-organic frameworks, its effect on N 2 O/CO 2 separation has yet not been explored. Herein, four isoreticular MTN-type metal-organic frameworks (MOFs) with different substituents (-H, –NH 2 , -Br or –NO 2 ) are reported for the capture of N 2 O from a N 2 O/CO 2 mixture. As revealed by isothermal measurements, thermodynamic studies and ideal adsorbed solution theory computations, the N 2 O/CO 2 separation potential can be effectively improved by an electron-donating group (-NH 2 ), whereas electron-withdrawing groups (-NO 2 or -Br) exhibit the opposite effect. Notably, MIL-101(Cr)–NH 2 exhibits, by far, the highest ideal adsorbed solution theory equilibrium adsorption selectivity of 1.91 for 50/50 N 2 O/CO 2 . The N 2 O/N 2 separation ability of the modified materials is also studied and functionalization with a -Br group yields an improved separation potential compared to the parent MIL-101(Cr) material. The strategy of using substituents to enhance the N 2 O/CO 2 separation efficiency of MOFs could also be extended to other porous materials for chemical separation processes.
研究领域:
材料科学
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化学工程
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DOI
高影响因子
Nanomaterials
·
2023
·Vol. 13
·期 14
·2072
·
IF 5.3
Xu Zhang,Bo Tian,Zhiheng Ma,He Wang,Zhixuan Cheng,Jiaqiang Xu
As a volatile air pollutant, formaldehyde can enter people’s living environment through interior decoration, furniture and paint, causing serious harm to human health. Therefore, it is necessary to develop a sensor for the real-time detection of formaldehyde in low concentrations. According to the chemical interaction between amino groups and formaldehyde, a MIL-101(Cr) aminated-material-based formaldehyde cantilever sensor was prepared, of which ethylenediamine- functionalized MIL-101(Cr) named ED-MIL-101(Cr)) showed the best gas sensing performance. Using quasi-in situ infrared spectroscopy, ED-MIL-101(Cr) was found bound to formaldehyde through a Schiff base. The adsorption enthalpy of formaldehyde-bound ED-MIL-101(Cr) was −52.6 kJ/mol, which corresponds to weak chemical adsorption, so the material showed good selectivity. In addition, ED-MIL-101(Cr) has the most active sites, so its response value to formaldehyde is larger and it takes longer to reach saturation adsorption than bare MIL-101(Cr). Through the research on the gas sensing performance of functionalized MIL-101(Cr) material, we found that it has a strong application potential in the field of formaldehyde monitoring, and the material performance can be quantitatively and accurately evaluated through combining calculation and experimentation for understanding the gas sensing mechanism.
研究领域:
材料科学
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环境科学
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分析化学
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DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Shaoan Cheng,Yangxi Li,Zhen Yu,Yuqing Su
Adsorption can be used as a pollutant removal method to solve the increasingly serious problem of synthetic dye pollution and metal organic framework (MOF) is considered as a novel adsorbent for its unique structure. However, the high cost and high toxicity during the synthesis procedure of MOFs like MIL-101(Cr) limited their potential on the large-scale production and application. In this paper, waste PET plastic was depolymerized to prepare terephthalic acid (TPA) as an organic linker to synthesize MIL-101(Cr). Besides, Hydrofluoric acid (HF) was not added during the synthesis to avoid poisonous pollution. MIL-101(Cr) was applied to the adsorption of anionic dyes reactive red 2 (RR2) and reactive blue 19 (RB19). The batch experiments exhibited kinetic data best fitted the pseudo-first-order model (PFO) with the adsorption capacity of 662.87 (RR2) and 863.67 mg g -1 (RB19). The isotherm adsorption data fitted well with the Freundlich isotherm, indicating formation of multilayer coverage over the surface of MIL-101(Cr). The highest regeneration rate of MIL-101(Cr) at the fourth cycle was 91.18 and 91.44 % after RR2 and RB19 adsorption. X-ray photoelectron spectroscopy (XPS) technique and Fourier Transform Infrared (FTIR) spectroscopy both indicated the possible adsorption mechanism of MIL-101(Cr) toward RR2 and RB19 could be attributed to electrostatic interactions, hydrogen bonding, and the π-π stacking. This work proposed a novel method using waste plastics as raw materials to synthesize eco-friendly pollutant adsorbent, which had an enlightening effect on pollutant 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
International Journal of Refrigeration
·
2025
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IF 3.8
Shuyi Yao,Zhongbao Liu,Shijie Li,Zhipeng Qie
Improving water vapor adsorption performance at low humidity and enhancing thermal conductivity are beneficial for the performances of adsorption refrigeration materials. In this study, MIL-101(Cr) was integrated with graphene oxide (GO) and calcium chloride (CaCl₂) to develop high-performance composite adsorbents. The materials were characterized by XRD, Raman spectroscopy, nitrogen adsorption-desorption, and thermal conductivity measurements. Adsorption and desorption tests revealed that the MIL-101(Cr)/2% GO + 20% CaCl₂ composite exhibited the best performance, achieving a dynamic adsorption capacity of 0.368 g/g and a 36% increase in thermal conductivity compared to pure MIL-101(Cr). Meanwhile, the heat and mass transfer performance of the materials and the COP and SCP of the system were analyzed by modeling the adsorbent and the system under the corresponding operating conditions, and MIL-101(Cr)/2% GO + 20% CaCl₂ showed the best performance among all the samples of the present study in all these models. Furthermore, the composite demonstrated excellent stability after 50 adsorption-desorption cycles, retaining a desorption efficiency above 93%. The synergistic effects of GO and CaCl₂ significantly improved both water vapor adsorption and thermal conductivity, making this composite a promising candidate for energy-efficient adsorption refrigeration systems.
研究领域:
材料科学
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能源工程
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DOI
高影响因子
Materials
·
2022
·Vol. 15
·期 16
·5763
·
IF 3.748
Minmin Zou,Hexin Zhu,Ming Dong,Tian Zhao
As one of the most important prototypical chromium-based MOFs, MIL-101(Cr) is well-studied and widely employed in various scientific fields. However, due to its small capture window sizes and curved internal apertures, its application in large molecular removal is quite limited, and given its high stability and high synthetic temperature (>200 °C), it is difficult to achieve hierarchically porous MIL-101(Cr). In our study, hierarchically porous MIL-101(Cr) involving a high macro-/meso-/micropores ratio was designed and synthesized using acetic acid as an additive and silicon dioxide (SiO2) nanoparticles as a template. The optimal hierarchically porous MIL-101(Cr) (A-4) possessed a high specific surface area (2693 m2g−1) and an abundant macro-/mesoporous structure with the addition of SiO2of 200 mg. Compared with the control sample (A-0) with a less macro-/mesoporous structure, A-4 showed good adsorption properties for both coomassie brilliant blue R-250 (CBB, 82.1 mg g−1) and methylene blue (MB, 34.3 mg g−1) dyes, which were 1.36 times and 9.37 times higher than those of A-0. Moreover, A-4 also had good recyclability, and the removal rate of CBB was still higher than 85% after five cycles of adsorption.Keywords:MIL-101(Cr);SiO2;dye adsorption;template
研究领域:
材料科学
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环境科学
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产品关联
DOI
PubMed
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2024
·Vol. 48
·期 20
·9185-9195
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IF 2.7
Shikai Xue,Dongying Zhu,Qing Zuo,Shuangfeng Yang,Haiyan Wang,Qiujun Lu,Guoxing Yin,Guihua Ruan,Fuyou Du
A novel MIL-101(Fe)/ZnCrZr-LBMO heterojunction was successfully constructed and used for the removal of ciprofloxacin (CIP) in this work. The MIL-101(Fe)/ZnCrZr-LBMO composite exhibited significantly enhanced photocatalytic degradation activity, with reaction rates approximately 3.4 and 3.1 times faster than those observed with pristine MIL-101(Fe) and ZnCrZr-LBMO, respectively. The effect of different amounts of ZnCrZr-LBMO, sample pH, CIP concentration, inorganic cations, and anions on CIP removal was investigated, and the possible intermediates and degradation pathways of CIP were speculated. The·O2− radicals dominated CIP degradation, with minor contributions from 1O2, h+, and ·OH radicals. The composite exhibited high removal rates for CIP (94.7%), ofloxacin (86.8%), and tetracycline (96.3%), respectively, within 60 min of light irradiation, and excellent reusability, retaining over 85.1% CIP degradation rate after five cycles. Our work provides a new reference to construct highly efficient and easily recyclable MIL-101(Fe)/ZnCrZr-LBMO photocatalysts for the removal of antibiotic pollutants, promising advancements in real water treatment applications.
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
LANGMUIR
·
2024
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IF 3.7
Zeqi Wu,Feng Niu,Wenhao Yao,Siyuan Gao,Da Chen,Yuexiang Huang
The activation of an inert C(sp3)–H bond in selective oxidation of hydrocarbons under mild conditions is a critical and challenging process. Herein, we report a stable chlorine-coordinated metal–organic framework (MOF) photocatalyst, MIL-101(Fe), for efficient visible-light-driven photocatalytic selective oxidation of toluene to benzaldehyde in air under ambient conditions. Encouragingly, a benzaldehyde formation yield of 3.11 mmol·g–1·h–1 with a selectivity of 92.1% is achieved in 5 h, which is superior to most of the reported works. Based on the experimental results and characterizations, the high catalytic performance is mainly due to the promoted rate-limiting step of C(sp3)–H bond activation by a chlorine radical (Cl·) from the coordinated −Cl in the MIL-101(Fe) structure. In addition, the present photocatalyst possesses good substrate tolerance for photocatalytic selective oxidation of various toluene derivatives under optimized conditions.
研究领域:
化学
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材料科学
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环境科学
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产品关联
DOI
PubMed
高影响因子
RSC Advances
·
2022
·Vol. 12
·期 38
·24670-24680
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IF 4.036
Wei Qin,Along Yu,Xue Han,Junwei Wang,Jiayin Sun,Jianli Zhang,Yaqing Weng
With the increasing demand for rare earth elements (REEs) due to their wide application in high technology, their recovery and separation from waste sources has gradually come onto the agenda. Herein, a new kind of MIL-101-NH2 (M1N) MOF functionalized with diethanol anhydride (DGA) incorporated into a polyvinylidene fluoride (PVDF) membrane (DGA-M1N@PVDF) has been fabricated for the sorption of REEs from a simulated acid leaching solution of waste phosphor, which contains a large amount of REEs. FTIR, TGA, XRD, fluorescence spectra and XPS analysis were used to characterize the synthesized composite membrane. Batch tests were employed to determine the optimal sorption conditions for Y and Eu adsorbed on DGA-M1N@PVDF adsorbent, such as pH (1–5), content of M1N MOFs (0–40 wt%), contact time (10–180 min) and ion concentration (0–20 mg L−1). Maximum adsorption capacities for Y and Eu on DGA-M1N@PVDF reached 991.7 μg g−1 and 98.76 μg g−1 for trace REE solution, respectively. Moreover, a pseudo-second-order kinetic model accurately described the sorption process, and the plotted isothermal data indicated that the Langmuir model was more suitable than the Freundlich model for Y and Eu sorption with monolayer and chemical adsorption. Meanwhile, FTIR and XPS analyses revealed that the Y and Eu adsorption on the DGA-M1N@PVDF composite membrane was mainly caused by the N and O atoms of the –CONH or –COOH groups coordinated with metal ions. Furthermore, after five cycles, the recovery efficiency by DGA-M1N@PVDF for REEs remains above 82% and the XRD patterns were consistent with the original sample, which implied that the DGA-M1N@PVDF membrane has preferable stability, recyclability and good efficiency in REE separation from waste phosphor solutions.
研究领域:
材料科学
·
环境工程
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DOI
高影响因子
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