INORGANIC CHEMISTRY COMMUNICATIONS
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2019
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IF 1.795
Jianhua Liu,Yumei Wang,Hao Guo,Songjie Fan
A novel heterogeneous membrane-MIL-121/118 were successfully synthesized on the surface of macroporous glass frits by increasing the content of aluminum nitrate in the starting solution. For the gas mixtures of H 2 /CO 2 , H 2 /CH 4 and H 2 /N 2 , the membrane exhibits permselectivity towards H 2 . Specifically, the separation factors are 10.7, 8.9 and 7.5 respectively with average H 2 permeance of 7.83 × 10 −8 mol·m −2 ·s −1 ·Pa −1 . As far as we know there is no report of any heterogeneous MOF membranes and the diversity of membrane structure certainly facilitates its versatility.
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
Journal of Cleaner Production
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2021
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IF 9.297
Hong Ma,Yilin Yang,Fengyue Yin,Xiong-Fei Zhang,Jianhao Qiu,Jianfeng Yao
Metal-organic frameworks (MOFs) have been widely explored as adsorbents for heavy metal ions removal. However, the recovery and regeneration of powdery MOFs remains a huge challenge. In this work, MIL-121 (Al-based MOF) crystals were incorporated into biodegradable alginate matrix to form composite beads with enhanced recyclability and adsorption capacity . A systematic adsorption test for Cu 2+ and Cd 2+ was conducted and the optimal sample (with a MOF loading of 50 wt%) presented an adsorption capacity of 204.5 mg/g for Cu 2+ and 88.7 mg/g for Cd 2+ . Moreover, the composite beads can be regenerated effectively by hot water (80 °C). The desorption is attributed to the carboxyl-rich MIL-121, which could release massive protons (H + ) at elevated temperature. Compared with the traditional desorption using strong acids, this chemical-free thermal desorption strategy holds a great potential for adsorbent regeneration and practical wastewater treatment .
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
ACS Applied Materials & Interfaces
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2022
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IF 10.383
Ming Li,Jianhao Qiu,Jie Xu,Yuxiang Zhu,Jianfeng Yao
The oxygen vacancies could efficiently drive the photocatalytic oxidation of aromatic alcohol through the activation of reactants. However, the activation between aromatic alcohol and O2 (oxidant) over oxygen vacancies is rarely studied. Herein, the ZnIn2S4/MIL-121 heterostructure with abundant surface uncoordinated carboxyl was rationally designed for benzyl alcohol (BA) oxidation under visible light. Oxygen vacancies on catalysts were self-induced after the surface complexation between the uncoordinated carboxyl and BA molecules. Based on the reaction results, it is concluded that the oxygen vacancy activation to BA is more effective than that to O2 for BA oxidation over ZnIn2S4/MIL-121 hybrids. Specifically, when the activation fully occurs on BA (reaction in N2), an admirable conversion of 93.9% (corresponding production rate of benzaldehyde: 2348 μmol·g–1·h–1) is achieved, which is 3.4 times that of pure ZnIn2S4, whereas an inferior conversion of 45.9% is obtained in O2 due to the competition effect between O2 and BA for oxygen vacancies.
研究领域:
材料科学
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催化化学
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DOI
PubMed
高影响因子
WATER RESEARCH
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2020
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IF 9.13
Chenghan Ji,Daowen Wu,Junhe Lu,Chao Shan,Yi Ren,Ting Li,Lu Lv,Bingcai Pan,Weiming Zhang
Adsorption is a viable technology to remove trace heavy metals from wastewater, but regeneration of adsorbents in an economic and environmentally friendly manner often represents a limiting factor of its application. Compared with traditional strong acid desorption, developing a chemical-free method is of great significance to both economic and the environmental welfare. Herein, we synthesized a novel thermoresponsive absorbent, A-MIL-121, which could effectively remove trace Cu(II) (> 95 %) from a high-salinity ([Na + ]/[Cu 2+ ] = 20000) water at normal temperature. At elevated temperature, A-MIL-121 could quickly and efficiently desorb Cu(II), with over 90% desorption rate at 80°C within 3 h. Fourier transform infrared spectroscopy (FTIR) analysis revealed that two types of –COOH groups existed in the material. One was in free form and acted as the sites for Cu(II) adsorption; the other was in dimer connected by two H-bonds, which cleaved at elevated temperature. As a result, massive exchangeable protons were released to the solution, which caused the desorption of Cu(II). Similar temperature dependent adsorption-desorption behavior was also found to other heavy metals, such as Cd 2+ , Pb 2+ , Ni 2+ . No significant capacity loss was observed after 10 successive adsorption-desorption cycles. Finally, Column experiments using a real copper electroplating wastewater showed that a total of ~ 1650 mL of clean water was generated before breakthrough (Cu 2+ < 0.5 mg/L), while less than 45 mL of 80°C water was used for regeneration. This study indicates the potential of A-MIL-121 as a novel green adsorbent to address trace heavy metals in wastewater.
研究领域:
环境科学
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材料科学
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DOI
PubMed
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2021
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IF 5.316
Dingliang Dai,Jianhao Qiu,Ming Li,Jie Xu,Lu Zhang,Jianfeng Yao
A series of BiOI/MIL-121(Al) hybrid photocatalysts has been prepared by a facile hydrothermal method. Two-dimensional BiOI sheets are intimately anchored on rod-like MIL-121 due to the electrostatic and coordination effects between Bi 3+ and carboxyl. The BiOI/MIL-121(Al) hybrid exhibits favorable performances for visible-light-driven degradation of tetracycline. The degradation performance of the optimal sample BM-20 is more than twice as that of pure BiOI. Apart from the close contacts between BiOI and MIL-121, the hydrogen bond induced by carboxyl in MIL-121 promotes the adsorption of tetracycline, which is also conducive to the photocatalytic degradation process. Moreover, results show that photo-induced holes and superoxide radicals are both the main active species for the photocatalytic degradation of tetracycline over BiOI/MIL-121 composites. This work would inspire the materials design with specific functional groups for efficient (photo)catalytic reaction.
研究领域:
材料科学
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环境科学
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光催化
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DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2021
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IF 10.588
Chenghan Ji,Mujian Xu,Hang Yu,Lu Lv,Weiming Zhang
The development of heavy metal adsorbents with high selectivity has become a research hotspot due to the interference of coexisting ions (e.g., Na + , Ca 2+ ) in the actual wastewater, but the more difficult regeneration caused by high adsorption selectivity severely limits its practical applications. Herein, a carboxyl adsorbent, MIL-121, demonstrated high adsorption selectivity for heavy metals at 10,000 mg/L of Na + (removal > 99% for Cu 2+ ) as well as unexpected easy regeneration (desorption > 99%) at low H + concentration (10 −3.5 –10 −3.0 M), which is hundreds of times lower than that of ever reported selective adsorbents (> 10 −1 M H + ). X-ray photoelectron spectrometry (XPS), extended X-ray absorption fine structure (EXAFS) coupled with Density functional theory (DFT) simulation unveil that the -COOH groups in MIL-121 for heavy metals adsorption is specific inner-sphere coordination with higher binding energy (1.31 eV for Cu), and less energy required for regeneration (0.26 eV for H). Similar high selectivity and easy regeneration were also satisfied with other heavy metals (e.g., Pb 2+ , Ni 2+ ), and removal of heavy metals remained > 99% in 10 consecutive adsorption-desorption cycles. For actual copper electroplating wastewater treatment , MIL-121 could produce ~ 3600 mL clean water/g sample, outperforming 300 mL that of the benchmark commercial adsorbent D-113. This study shows the potential of MIL-121 for heavy metal wastewater treatment and provides mechanistic insight for developing adsorbents with high selective adsorption and easy regeneration.
研究领域:
环境科学
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材料科学
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DOI
PubMed
高影响因子
Catalysts
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2025
·Vol. 15
·期 10
·995
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IF 4
Tao Xu,Jinmin Chen,Yang Ma,Yuwei Pan,Hui Huang,Guangyu Wu
The increasing discharge of organic pollutants such as dyes and antibiotics poses severe threats to aquatic ecosystems and human health. Conventional wastewater treatment methods are often limited by high energy consumption, secondary pollution, or low efficiency under visible light. It is crucial to design novel photocatalysts that can simultaneously utilize visible photons and enable swift transport of photoinduced charge carriers to drive contaminant decomposition. Herein, novel BiOCl/MIL-121 composites were synthesized via a straightforward hydrothermal route. A suite of complementary microscopic and spectroscopic analyses, including SEM, TEM, XRD and XPS, were employed to elucidate the material’s composition. Furthermore, collective evidence from spectroscopic and electrochemical analyses confirms markedly improved light absorption and charge separation efficiency within the BiOCl/MIL-121 photocatalyst. The 5% BiOCl/MIL-121 composite achieved 93.7% removal of Rhodamine B in 60 min, exhibiting a high photocatalytic degradation rate. Similarly, 5% BiOCl/MIL-121 photodegraded 80.4% of tetracyclin, which was much better than that of BiOCl. A plausible interfacial charge-transfer mechanism was deduced from the band structure of the 5% BiOCl/MIL-121 composite and experimental evidence from radical scavenger studies. This study provides an effective strategy for constructing a composite photocatalyst and offers a green way for the efficient degradation of organic pollutants.
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高影响因子