JOURNAL OF HAZARDOUS MATERIALS
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2017
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IF 6.065
Songjian Zhao,Jian Mei,Haomiao Xu,Wei Liu,Zan Qu,Yong Cui,Naiqiang Yan
Metal-organic frameworks (MOFs) adsorbent Mil-101(Cr) was introduced for the removal of elemental mercury from sintering flue gas. Physical and chemical characterization of the adsorbents showed that MIL-101(Cr) had the largest BET surface area, high thermal stability and oxidation capacity. Hg 0 removal performance analysis indicated that the Hg 0 removal efficiency of MIL-101(Cr) increased with the increasing temperature and oxygen content. Besides, MIL-101(Cr) had the highest Hg 0 removal performance compared with Cu-BTC, UiO-66 and activated carbon, which can reach about 88% at 250 °C. The XPS and Hg-TPD methods were used to analyze the Hg 0 removal mechanism; the results show that Hg 0 was first adsorbed on the surface of Mil-101(Cr), and then oxidized by the open metal site Cr 3+ . The generated Hg 2+ was then combined surface adsorbed oxygen of adsorbent to form HgO, and the open metal site Cr 2+ was oxidized to Cr 3+ by surface active oxygen again. Furthermore, MIL-101(Cr) had good chemical and thermal stability.
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JOURNAL OF SEPARATION SCIENCE
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2018
·Vol. 41
·期 9
·2046-2055
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IF 2.415
Yulan Deng,Ruiqi Zhang,Di Li,Peng Sun,Ping Su,Yi Yang
Here, we describe a simple one-pot solvothermal method for synthesizing MIL-101(Fe)@polydopamine@Fe 3 O 4 composites from polydopamine-modified Fe 3 O 4 particles. The composite was used as a magnetic adsorbent to rapidly extract sulfonylurea herbicides. The herbicides were then analyzed by high-performance liquid chromatography. The best possible extraction efficiencies were achieved by optimizing the most important extraction parameters, including desorption conditions, extraction time, adsorbent dose, salt concentration, and the pH of the solution. Good linearity was found (correlation coefficients >0.9991) over the herbicide concentration range 1–150 μg/L using the optimal conditions. The limits of detection (the concentrations giving signal/noise ratios of 3) were low, at 0.12–0.34 μg/L, and repeatability was good (the relative standard deviations were <4.8%, n = 6). The method was used successfully to determine four sulfonylurea herbicides in environmental water and vegetable samples, giving satisfactory recoveries of 87.1–108.9%. The extraction efficiency achieved using MIL-101(Fe)@polydopamine@Fe 3 O 4 was compared with the extraction efficiencies achieved using other magnetic composites (polydopamine@Fe 3 O 4 , Hong Kong University of Science and Technology (HKUST)-1@polydopamine@Fe 3 O 4 , and MIL-100(Fe)@polydopamine@Fe 3 O 4 ). The results showed that the magnetic MIL-101(Fe)@polydopamine@Fe 3 O 4 composites have great potential for the extraction of trace sulfonylurea herbicides from various sample types.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2024
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IF 20.2
Jianxin Zhu,Haiyang Liu,Haijun Chen,Xiuyi Hua,Deming Dong,Dapeng Liang,Zhiyong Guo,Na Zheng
Low degradation efficiency and significant transition metal leaching are two challenges in persulfate activation systems based on metal-organic frameworks (MOFs) for organic pollutant degradation. Here, the challenges were solved by designing and synthesizing a micron-sized core-shell material, γ-Al 2 O 3 -C-MIL-100(Fe) (γACM), by coating the γ-Al 2 O 3 core with carbon (γ-Al 2 O 3 -C) and futher modifying with MIL-100(Fe). Testing γACM with sulfamethazine (SMZ) demonstrated its outstanding peroxydisulfate (PDS) activation, achieving 92.5 % SMZ removal within 20 min at a low oxidant/pollutant ratio. Fe leaching from γACM was effectively inhibited, with only 3.59 % Fe lost after three recycles. The system showed adaptability across a wide pH range, and usability in sewage effluent, indicating promise for practical application. The hydrophobicity of γ-Al 2 O 3 -C, the coordinatively unsaturated sites in MIL-100(Fe), and the strong bounding of MIL-100(Fe) on γ-Al 2 O 3 -C ensured the effective SMZ gather, PDS activation, and Fe stability respectively, which led to the excellent performances of γACM.
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ANALYST
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2012
·Vol. 137
·期 15
·3445-3451
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IF 4.23
Shu-Hui Huo,Xiu-Ping Yan
The unusual properties such as high surface area, good thermal stability, uniform structured nanoscale cavities and the availability of in-pore functionality and outer-surface modification make metal–organic frameworks (MOFs) attractive for diverse analytical applications. However, integration of MOFs with magnets for magnetic solid-phase extraction for analytical application has not been attempted so far. Here we show a facile magnetization of MOF MIL-101(Cr) for rapid magnetic solid-phase extraction of polycyclic aromatic hydrocarbons (PAHs) from environmental water samples. MIL-101 is attractive as a sorbent for solid-phase extraction of pollutants in aqueous solution due to its high surface area, large pores, accessible coordinative unsaturated sites, and excellent chemical and solvent stability. In situ magnetization of MIL-101 microcrystals as well as magnetic solid-phase extraction of PAHs was achieved simultaneously by simply mixing MIL-101 and silica-coated Fe3O4 microparticles in a sample solution under sonication. Such MOF-based magnetic solid-phase extraction in combination with high-performance liquid chromatography gave the detection limits of 2.8–27.2 ng L−1 and quantitation limits of 6.3–87.7 ng L−1 for the PAHs. The relative standard deviations for intra- and inter-day analyses were in the range of 3.1–8.7% and 6.1–8.5%, respectively. The results showed that hydrophobic and π–π interactions between the PAHs and the framework terephthalic acid molecules, and the π-complexation between PAHs and the Lewis acid sites in the pores of MIL-101 play a significant role in the adsorption of PAHs.
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JOURNAL OF PHYSICAL CHEMISTRY B
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2024
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IF 2.8
Hong-Jie Zhang,Xue-Bin Shang,Xu-Ran Wang,Chen-Xi Zhang,Qing-Lun Wang
SCPEEK@MOF proton exchange membranes, where SCPEEK is sulfinyl chloride polyether ether ketone and MOF is a metal–organic framework, were prepared by doping Fe-MIL-101-NH2 into polymers. The amino group in the MOF and the -SOCl2 group in thionyl chloride polyether ether ketone cross-link to form a covalent bond through the Hinsberg reaction, and the prepared composite membrane has stronger stability than other electrostatic interactions and simple physical doping composite membranes. The formation of covalent bonds improves the water absorption of the composite membrane, which makes it easy for water molecules to form hydrogen bonds. Moreover, SPEEK as a proton conductive polymer and the synergy of MOFs improve the proton conductivity of composite membranes. The composite membranes were characterized by Fourier transform infrared spectroscopy, powder X-ray diffraction, scanning electron microscopy, and atomic force microscopy. The swelling rate, water absorption, mechanical stability, ion exchange capacity, and proton conductivity of the pure sulfonated polyether ether ketone (SPEEK) membrane were compared with those of the mechanically doped SPEEK/MOF membrane and the composite membrane SCPEEK@MOF doped with different ratios of Fe-MIL-101-NH2, and all of the SCPEEK@MOF showed superior performance. When the Fe-MIL-101-NH2 loading rate of the composite membrane is 2%, the proton conductivity of the composite membrane can reach 0.202 S cm–1 at 363 K and a 98% relative humidity, which is much higher than that of the SPEEK/MOF membrane obtained by simple physical doping under the same conditions.
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Journal of Water Process Engineering
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2024
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IF 6.3
Mei Dong,Kuilong Liu,Guoqiang Song,Guiping Ma
In this study, MOF-on-MOF hybrids were successfully synthesized by interfacial growth method using CoZn-ZIF as guest MOF and MIL-101(Fe) as host MOF, and then employed as heterogeneous catalysts to activate peroxymonosulfate (PMS) in the degradation of dyes. The hybrids exhibited different morphologies depending on the Co/Zn ratios (10/0, 10/2, 10/10, and 2/10), all of which displayed exceptional catalytic performance. Notably, the hybrid with a Co/Zn ratio of 10/2 showed the highest degradation rate of MB, reaching 100 % removal within 3 min with a k obs value of 452.75 Lg −1 min −1 based on the pseudo-second-order kinetic model. Through EPR characterization and scavenging experiments, it was determined that the degradation of dyes occurred through a combination of radical (SO 4 •-, •OH)and non-radical ( 1 O 2 ) pathways, with 1 O 2 and SO 4 •- playing prominent roles. Various factors such as Co/Zn ratio, catalyst dosage, PMS concentration, initial pH, temperature, and MB solution concentration were systematically investigated to understand their influence on the catalytic performance. Furthermore, the influence of inorganic ions, humic acid (HA), and the reusability and stability of the catalyst was evaluated, demonstrating its potential for practical applications. Overall, this research provides valuable insights into the design and application of MOF-based catalysts for environmental remediation processes.
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Molecular Catalysis
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2024
·
IF 3.9
Pushuang Xing,Cong Li,Yixin Chen,Rong-Lan Zhang
PMoV 2 was encapsulated in four MOFs (MIL-101, HKUST-1, UiO-67, ZIF-8) with different cavity sizes and window sizes using a hydrothermal synthesis method. Then, a layer of mesoporous silica was coated on the surface of the MOFs to obtain four designed three-layer encapsulated catalysts 30%PMoV 2 @MOF@mSiO 2 . The physicochemical properties of the catalysts were characterized through various characterization methods, and the influence of different MOF window sizes of the four catalysts on the removal rate of four thiophene sulfides was investigated. The optimal reaction conditions were also explored for the optimal catalyst. The results indicate that under simulated fuel of 2400 ppm, 30%PMoV 2 @UiO-67@mSiO 2 owns the highest catalytic activity. Under optimal conditions, the total removal rate of four thiophene compounds was 91.52 %, and after ten cycles, the efficiency could still reach 86.24 %. This is attributed to the sufficient cavity size of UiO-67, which provides assurance for the loading of PMoV 2 and the large window size, making it possible for the smooth reaction between sulfides and PMoV 2 .
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CHEMICAL ENGINEERING JOURNAL
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2024
·
IF 13.3
Yadan Luo,Chenguang Li,Zhen Liu,Wei Guo,Cuizhu Sun,Shasha Zhao,Qian Wang,Yuanyuan Li,Lingyun Chen,Hao Zheng,Fengmin Li
Phthalates (PAEs) are known to pose a serious threat to the environment and human health duo to their endocrine disrupting effects, thus a great deal of effort has been made to develop destruction technologies for PAEs treatment in the water environment, such as peroxymonosulfate (PMS)-based advanced oxidation technology. Here we prepared an environmentally friendly visible light catalyzer, a heterojunction of carbonitride nanosheets (CNN) doped with NH 2 -iron metal organic frameworks (NH 2 -MIL-101(Fe)), for the activation of PMS to efficaciously remove two representative PAEs—diisobutyl phthalate (DIBP) and diethyl phthalate (DEP)—from the aquatic environment. The CNN@NH 2 -MIL-101(Fe) photocatalyst possesses an excellent visible light harvesting performance with a narrow band gap (1.66 eV), low recombination ratio of photoinduced carriers, and long charge lifetime. The pore volume and surface area of the composite material was increased compared with any single component. The optimum CNN@NH 2 -MIL-101(Fe) catalyst manifested the high performance to activate PMS to degrade DIBP and DEP under visible irradiation with maximum removal of 94.5 ± 2.2 % and 83.4 ± 0.9 %, respectively. Four main active species (•OH, O 2 − •, SO 4 − •, and h + ) were involved in PAEs photodegradation, with h + and SO 4 − • playing a key role in the degradation of DIBP, and h + in the degradation of DEP. The degradation mechanism of DIBP and DEP mainly involved the ester bond cleavage and oxidation by active species. Additionally, the CNN@NH 2 -MIL-101(Fe) heterojunction exhibited high and stable catalytic performance to activate PMS for PAEs destruction under pH 3 – 9. Therefore, this study provides a new strategy for designing and selecting environment-friendly treatment approach for the effective eradication of PAEs via a PMS-based advanced oxidation process.
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ACS Sustainable Chemistry & Engineering
·
2025
·
IF 7.3
Meng Xia,Longqi Li,Xiaocong Wang,Kaihao Xu,Shuai Zhang,Chengxue Zhang
During CO2/HCO3– reduction with renewable biomass, achieving high-efficiency production of the target products is vital but challenging. In this study, an NH2– functional-group-modified MIL-53(Fe) catalyst was synthesized using a facile and efficient method. Under the action of the NH2-MIL-53(Fe) catalyst, a clear synergistic effect was exhibited on the transformation of glucose and NaHCO3 into formic acid with a high yield of 50% at a low reaction temperature (190 °C) via a three-pronged route, which mainly involved the decomposition of intermediates of glucose to gradually reduce NaHCO3 to formic acid under hydrothermal conditions. An in-depth analysis of the catalytic mechanism and density functional theory calculations demonstrated that the increased alkalinity of active sites by the NH2– functional group incorporation into the catalytic system enhanced the crucial reaction steps and reduced the activation energy of the crucial reactions, including glucose isomerization, aldehyde intermediate retro-aldol condensation, and redox of aldehyde compounds and NaHCO3 to formic acid, thereby promoting the generation of target products and suppressing side products. This study addresses the challenge of reducing NaHCO3 from renewable biomass to commercial formic acid by constructing multifunctional active sites, thus providing a new strategy for achieving carbon cycling.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
·
IF 8.1
Chunru Sun,Min Xiao,Jianghao Tian,Huixian Zhang
A polysulfone/metal–organic framework (MOF) based photocatalytic nanofiltration membrane is proposed in this study. Interfacial polymerization (IP) is the universal method of preparing nanofiltration (NF) membranes. In this work, the (TFN) membranes were synthesized with an in-situ interfacial synthetic method to incorporate BiOCl/MIL-101(Fe)@PDA(BMP) into the polyamide (PA) selective layer. Five distinct BMP loadings (0, 0.05, 0.1, 0.15, and 0.2 wt%) were established to examine the impact of additional BMP on the physicochemical characteristics of the produced TFN membranes. Under the irradiation of a xenon lamp with a power of 300 W, the water flux of M3 at a pressure of 0.6 MPa was 277.14 L m -2 h -1 . Furthermore, the BSA-based antifouling tests demonstrated the membrane’s outstanding antifouling capabilities, with a flux recovery rate reaching 94.08 %. The optimal membrane maintained a high and stable retention of tetracycline for 12 h. The interfacial synthesis of MOF/PA offers a new approach to the fabrication of photocatalytic NF membranes.
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APPLIED SURFACE SCIENCE
·
2025
·
IF 6.9
Yue Wang,Wenjun Zhang,Yanjun Zhang,Meng Chen
Metal-organic frameworks (MOFs), with tunable morphologies and porous architectures, show great potential in photocatalysis. A variety of MOFs can be synthesized by changing the types of metal ions and organic ligands. However, fewer studies have explored the influence of the metal-to-ligand molar ratio on the catalytic performance of the resulting MOF-related products. In this work, capsule-shaped NH 2 -MIL-68(In)/InOOH composites were synthesized by adjusting molar ratios of In(NO 3 ) 3 to 2-aminoterephthalic acid. Time-dependent characterization revealed sequential crystallization: rod-shaped NH 2 -MIL-68(In) initially formed in the solution, followed by the in-situ growth of InOOH nanowires on its surfaces via excess indium ions, ultimately constructing a Z-scheme heterojunction. The optimized NM/InOOH (8:1) composite exhibited a larger specific surface area and extended light absorption. The Z-scheme configuration significantly promoted charge carrier separation efficiency while maintaining strong redox potentials of the photoinduced holes and electrons, thereby resulting in 5–8-fold improvement in degradation rates for four dyes (AOII, RhB, MB, and Rh6G), highlighting its broad photocatalytic applicability.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Fanjian Meng,Yongrui Li,Chenshuai Han,Zhaorui Zhang,Xiaohui Yan,Minghui Yang
Highly-sensitive NO 2 gas sensors based on metal oxide semiconductors (MOS) are promising but often limited by poor sensing-recovery characteristics and high operating temperatures. Herein, we address these challenges by combining Zn doping modification with mild visible light activation, effectively tuning the electronic and chemical properties of MIL-68(In)-derived In 2 O 3 nanotubes (NTs), providing an advanced approach to realize rapid recovery towards sub-ppm NO 2 at room temperature (RT). The optimized 5 at% Zn-doped In 2 O 3 (Zn x In 2-x O 3 (x = 0.10)) NTs achieves an exceptional response of 15,257 toward 10 ppm NO 2 under dark condition and a rapid 4 s recovery under visible light irradiation at RT. Additionally, the sensor exhibits superior NO 2 selectivity, excellent reproducibility and long-term stability over 36 days. The enhanced sensing performance is driven by the mesoporous frameworks which enhance free electrons transfer in the modulated energy-level structure and introduce abundant photo-induced holes via visible light irradiation at the sensing-recovery stage. This work offers new insights into surface chemistry modulation in MOS nanomaterials, advancing the development of cost-effective and low-energy-consumption room-temperature NO 2 sensors.
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