CHEMICAL ENGINEERING JOURNAL
·
2016
·
IF 5.31
Ting Wang,Pan Zhao,Nan Lu,Hongche Chen,Conglu Zhang,Xiaohong Hou
Attractive magnetic metal-organic framework (MOF) material Fe 3 O 4 /MIL-101(Cr) (Matérial Institute Lavoisier, MIL) was synthesized by a simple reduction–precipitation method, and applied as an effective sorbent to the removal of two acid dyes, acid red 1 (AR1) and orange G (OG), in water. The novel synthetic method avoided the oxidation of Fe 2+ and made the Fe 3 O 4 /MIL-101(Cr) composite have the advantages of strong magnetism, large surface areas and excellent dispersion effect. Parameters that influenced the adsorption process, such as solution pH, adsorbent dosage, ionic strength, and so on, were investigated. Under the optimum conditions, adsorption kinetics and isotherms were determined from the obtained experimental data. The adsorption kinetics suggested the adsorption process of Fe 3 O 4 /MIL-101(Cr) toward AR1 and OG met the pseudo-second-order kinetic model. The adsorption isotherms were fitted by Langmuir, Freundlich and Dubinin–Radushkevich (D–R) isotherm models. Compared with the Freundlich and D–R models, the Langmuir isotherm model was found to be suitable to describe the equilibrium data, suggesting that the uptake of AR1 and OG by the Fe 3 O 4 /MIL-101(Cr) would be through monolayer adsorption. The thermodynamic results demonstrated that the adsorption was a spontaneous, exothermic and entropy decreased process. In addition, the Zeta potential data with pH value of AR1 and OG indicated that the electrostatic interactions between the dyes and the adsorbent might be critical to the adsorption mechanism. The used Fe 3 O 4 /MIL-101(Cr) could be regenerated by washing with NaOH solution and reused at least six times. The maximum adsorption capacities of the magnetic composite toward AR1 and OG were up to 142.9 mg g −1 and 200.0 mg g −1 , respectively. These results demonstrated that the novel composite would be an effective and easily re-usable adsorbent for AR1 and OG.
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APPLIED ORGANOMETALLIC CHEMISTRY
·
2024
·Vol. 38
·期 9
·e7614
·
IF 3.7
Qiuyun Zhang,Feiran Xie,Jialu Wang,Tianqing Wang,Jiao Lei,Weihua Li,Jingsong Cheng,Yutao Zhang
For nearly a century, the excessive discharge of organic contaminants has gradually polluted water and endangered people's health, and photocatalysis has been prominently employed to remove persistent recalcitrant organic. Here, MIL-101(Cr) was firstly employed to introduce thin-layered Bi 2 O 2 CO 3 for the formation of Bi 2 O 2 CO 3 /MIL-101(Cr) nanosheet composite, by a simple and low-temperature in-situ growth approach. The phase, morphology, optical, and surface characteristics of the fabricated composite were characterized through XRD, FTIR, SEM-EDS, N 2 adsorption–desorption, UV–Vis DRS, PL, TG, and XPS techniques, and the ability in the photocatalytic breakdown of rhodamine B (RhB) molecule under visible light was also studied. The results of characterization analysis and optical analysis exhibited that Bi 2 O 2 CO 3 /MIL-101(Cr) has large pore size, good visible light response-ability, and the heterojunction created by intercalating Bi 2 O 2 CO 3 on MIL-101(Cr). Photocatalytic studies revealed that Bi 2 O 2 CO 3 /MIL-101(Cr) had superior RhB degradation activity than pure MIL-101(Cr) and Bi 2 O 2 CO 3 , which achieved 97.1% with visible light irradiation for 20 mg/l RhB. Meanwhile, the Bi 2 O 2 CO 3 /MIL-101(Cr) composite displayed good recyclability after three cycles as revealed by XRD and FTIR analysis proving their excellent stability. This study provides feasible insight into developing novel and efficient MIL-101-based heterojunction catalysts for environmental remediation in the future.
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APPLIED ORGANOMETALLIC CHEMISTRY
·
2025
·Vol. 39
·期 3
·e70037
·
IF 0
Qiuyun Zhang,Maozhen He,Jialu Wang,Shijian He,Mei Deng,Yanhui Lei,Xiaojuan Zhang,Jingsong Cheng,Zhengjun Liu,Yutao Zhang
The construction and optimization of an effective photocatalyst for photodegradation of persistent recalcitrant organic remains challenging. In this work, MIL-101(Cr)-based nanocomposites (AgI@MCr) are proposed to be fabricated by a simple, green solvent, and room temperature in situ preparation strategy, achieving a highly efficient photocatalytic degradation of organic dye rhodamine B (RhB) molecule under visible light irradiation. Extensive characterization (XRD, FTIR, N 2 adsorption–desorption, SEM and EDS, TG, XPS, UV–vis DRS, PL, transient photocurrent, and EIS) confirmed the composite material's structure, morphology, elemental composition, and optical characteristics. Among all the prepared nanocomposites, AgI@MCr-2 demonstrates outstanding photocatalytic performance for RhB with a removal efficiency of 95.4% within 70 min, and a reaction kinetics of 0.0392 min −1 , superior to pristine AgI or MIL-101(Cr), and also shows excellent durability, retaining over 80% RhB degradation efficiency after four cycles. Remarkably, the significant enhancement is attributed to the built interfacial contact and synergistic effect between substances in the nanocomposite, high specific surface area, strong visible light–harvesting capacity, low bandgaps, and high electron–hole pair separation. In addition, a possible degradation route for the AgI@MCr nanocomposite is further proposed using various analysis techniques. This study provides valuable references for developing effective multicomponent MOF-based photocatalytic composite materials for dyeing wastewater treatment and environmental remediation.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Si Duan,Yuan Gao,Guihong Lan,Haiyan Qiu,Bo Xu,Xiangming Liu,Ming Zhang,Yusong Chen
Functionalization of ligands is an effective strategy to enhance the adsorption performance of adsorbents. In this study, MIL-101(Fe)-R (R = -H, –OH, –NH 2 , and –NO 2 ) was selected as a platform for systematically studying the impact of functionalization on the adsorption behavior of chlortetracycline (CTC). A series of characterizations were conducted on the prepared MIL-101(Fe)-R to clarify the influence of organic linkers on the microscopic morphology, pore structure, and surface functionality of the adsorbents. Additionally, the effects of different functional groups on the adsorption behavior of MIL-101(Fe)-R were compared to screen for MOFs with high efficiency in removing CTC. Experimental results showed that the maximum adsorption capacities (q m ) of MIL-101(Fe), MIL-101(Fe)–NH 2 , MIL-101(Fe)–OH, and MIL-101(Fe)–NO 2 were 418.980 mg/g, 559.854 mg/g, 187.387 mg/g, and 154.131 mg/g, respectively. Among them, MIL-101(Fe)–NH 2 exhibited a higher mass transfer rate (reaching equilibrium in 15 min). Based on apparent adsorption behavior, adsorption kinetics, isotherm and thermodynamic studies, as well as FTIR and XPS characterizations before and after adsorption, the performance modulation mechanism of MIL-101(Fe)-R in CTC adsorption was discussed in detail. Combined with density functional theory (DFT) calculations, the host–guest interaction controlling the adsorption behavior was understood at the molecular level, demonstrating the optimal binding sites of the adsorbents. This study provides guidance for the design of efficient MOF adsorbents for antibiotic wastewater treatment.
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Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Hongbin He,Bolong Liang,Shumin Lin,Yan Chen,Xin Zhang,Shu-Xuan Liang
The residues of oxytetracycline hydrochloride (OTC) in water have potential adverse effects on human health and ecological environment. Photocatalytic degradation has been widely studied in the treatment of antibiotic pollution due to its environmentally friendly and efficient characteristics. However, the band gap of traditional photocatalysts is too wide, and the recombination of photogenerated electrons and holes is serious, which has negative effects on photocatalysis . Therefore, the Z-scheme heterojunction g-C 3 N 4 @MIL-101(Fe) composite photocatalyst was synthesized by high temperature calcination combined with solvothermal method. g-C 3 N 4 @MIL-101(Fe) was characterized by XRD, FTIR , SEM, TEM and other tests. All the results showed that the compound was successful A series of photoelectric tests showed that g-C 3 N 4 @MIL-101(Fe) has a narrower band gap, stronger light absorption ability, and improved the separation rate of photogenerated electrons and holes. Under visible light irradiation, g-C 3 N 4 @MIL-101(Fe) could remove 87.68% of OTC in 300 min. g-C 3 N 4 @MIL-101(Fe) showed good potential for practical application in five real water samples and stability after six cycles. Finally, superoxide radicals and hole radicals were identified as the main reactive species in the photodegradation process. The mechanism and pathway of the photocatalytic degradation of OTC by g-C 3 N 4 @MIL-101(Fe) are proposed. This work expands the construction and application of Fe-MOF based Z-scheme heterostructure and provides a new idea for water pollution remediation.
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MOLECULES
·
2024
·Vol. 29
·期 14
·3417
·
IF 4.2
Pengfei Zhu,Zhaoxia Hu,Shouwen Chen
The development of economical catalysts that exhibit both high activity and durability for chlorinated volatile organic compounds (CVOCs) elimination remains a challenge. The oxidizing and acidic sites play a crucial role in the oxidation process of CVOCs; herein, praseodymium (Pr) was introduced into CrOx catalysts via in situ pyrolysis of MIL-101(Cr). With the decomposition of the ligand, a mixed micro-mesoporous structure was formed within the M-Cr catalyst, thereby reducing the contact resistance between catalyst active sites and the 1,2-dichloroethane molecule. Moreover, the synergistic interaction between chromium and praseodymium facilitates Oβspecies and acidic sites, significantly enhancing the low-temperature catalytic performance and durability of the M-PrCr catalyst for 1,2-dichloroethane (1,2-DCE) oxidation. The M-30PrCr catalyst possess enhanced active oxygen sites and acid sites, thereby exhibiting the highest catalytic activity and stability. This study may provide a novel and promising strategy for practical applications in the elimination of 1,2-DCE.
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PubMed
高影响因子
Journal of Water Process Engineering
·
2025
·
IF 6.7
Mei Dong,Qiguang Cao,Song Li,Kebin Li
Designing stable and efficient heterogeneous catalysts for peroxymonosulfate (PMS) activation remains a critical challenge in advanced oxidation processes. Herein, we prepared a polyvinylpyrrolidone (PVP)-modified MIL-101(Fe)@CoZn-ZIF (PVP-MCZ) core-shell nanocomposite that synergistically combined enhanced catalytic activity with exceptional stability. The PVP-MCZ catalyst achieved complete degradation of 4-nitrophenol (4-NP) (20 mg/L) within 15 min, while suppressing metal leaching (<0.5 mg/L). Comprehensive characterization (XPS, EPR) revealed a dual-pathway mechanism: (i) radical-dominated SO 4 − generation via Co 2+ /Co 3+ and Fe 2+ /Fe 3+ redox cycling, and (ii) non-radical 1 O 2 production from PMS self-decomposition. This work provides a scalable strategy to design MOF-based catalysts for sustainable water remediation.
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DALTON TRANSACTIONS
·
2025
·
IF 3.3
Yanjia Zhou,Xiao-Dong Tang,Jingjing Li,Da-Yong Qing,Hong Wang
MIL-101(Cr) and MIL-100(Fe) are both representative MIL-type Metal-Organic-Frameworks (MOFs) materials, renowned for their large specific surface areas and size-tunable characteristics, making them suitable candidates for Li+ extraction from lithium-containing solvent. By introducing -NH2 functional groups and using LiNO3 as both a template and mineralizer, the functionalized MOF materials Li/NH2/MIL-101(Cr) and Li/NH2/MIL-100(Fe) were synthesized. Following modification, their Li+ adsorption capacities were increased, reaching 43.58 and 38.22 mg/g, respectively. The dosage of mineralizer, initial Li+ concentration, adsorbent dosage, solution pH value, and temperature all have an impact on the adsorption capacity of adsorbents. In addition, through the establishment of the pseudo-first-order kinetic model, pseudo-second-order kinetic model, as well as Langmuir and Freundlich thermodynamic models, it can be known that the adsorption of the materials belonged to monolayer chemisorption, and the adsorption process was exothermic. Furthermore, both adsorbents showed good reusability, retaining over 85% of their initial adsorption capacity after four adsorption-desorption cycles, highlighting their practical applicability in lithium recovery processes. In Mg-Li mixed solution systems, both materials exhibited exceptional Li+ selectivity. At a low Mg2+/Li+ ratio of 3, the separation factor (α) exceeded 80; even at a high Mg2+/Li+ ratio of 10, α remained near 50. Additionally, in systems with coexistence of multiple interfering ions, the distribution coefficient (Kd) followed the order: Li+ ≫ Mg2+ > Ca2+ > Na+ > K+. In the mixed systems, Li/NH2/MIL-101(Cr) and Li/NH2/MIL-100(Fe) exhibited certain separation effect for Li+ against competing cations.
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INORGANIC CHEMISTRY
·
2024
·
IF 4.3
Jingyu Cai,Junjie Shi,Jian Zhang,Xiaoyu Miao,Sen Wang,Longqiang Xiao,Dan Liu,Linxi Hou
Electronic-grade isopropyl alcohol is widely utilized in the cleaning of semiconductors and microelectronic components. Removing ions like Pb2+ is crucial since the presence of impurities may cause degradation of electronics, increased failure rates, and short circuits. Membrane materials offer a number of advantages in the field of adsorption separation; however, the lack of adsorption sites results in limited adsorption capacity. In the current work, guanidino-grafted NH2-MIL-101(Fe) was incorporated into polyvinylidene fluoride (PVDF) to prepare MOF/PVDF mixed matrix membranes (NM/PVDF) for the removal of Pb2+ from isopropanol. Benefiting from the larger specific surface area and more lone electron pairs in the guanidine group, the Pb2+ adsorption capacity of the as-prepared NM/PVDF membrane was 29.4458 mg/g, which was higher than that of the NH2-MIL-101(Fe)/PVDF membrane (20.9306 mg/g) and the pure PVDF membrane (6.7324 mg/g). The NM/PVDF membrane was able to reduce the concentration of Pb2+ from 500 to 86.73 ppb. This work highlights the potential of guanidine-grafted Fe-based MOFs/PVDF membranes as adsorbents for acquisition of electronic-grade solvents.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Yanni Jiang,Zhongjuan Wang,Jianbo Huang,Feng Yan,Ye Du,Chuanshu He,Yang Liu,Gang Yao,Bo Lai
Singlet oxygen ( 1 O 2 ) is an effective reactive oxygen species in disinfection due to its long lifetime and sensitivity to bacteria. This study tried to develop a 1 O 2 dominated process for bacterial inactivation by visible light (vis) photocatalysis assisted by PMS. A novel CuS-modified MIL-101(Fe) (CSMF) photocatalyst was synthesized for the first time. Compared with MIL-101(Fe), CuS-modified MIL-101(Fe) enhanced the photocatalytic performance by increasing absorption of visible light, narrowing down the bandgap and promoting photo carrier separation efficiency. 7.5-log Gram-negative Escherichia coli (E. coli) could be inactivated by Vis/CSMF/PMS system within 40 min, showing much better performance of 3.5-log E. coli inactivated by Vis/PMS system. The Vis/CSMF/PMS system is applicable in a broad pH range from 3.0 to 9.0, remaining quite steady disinfection efficiency after regenerations of the catalyst. Quenching experiments and electron paramagnetic resonance (EPR) analysis demonstrated 1 O 2 was the dominated ROS rather than OH • and SO 4 •− . Three pathways, including photo-generated electrons (e − ) and O 2 dependent pathway, photo-generated holes (h + ) dependent pathway and CSMF enhanced PMS dissociation pathway, were evidenced to responsible for 1 O 2 formation by aeration experiments and specific 1 O 2 fluorescence probe. 1 O 2 in water attacked the bacterial cell membranes first, got inside the cell and up-regulated the level of intracellular ROS, which further led to cell membrane damage and DNA degradation so as to irreversible cell death. In addition, the developed Vis/CSMF/PMS system could also efficiently inactivate gram-positive bacteria Staphylococcus aureus and fecal coliform bacteria in practical wastewater, suggesting its wide applicability as a promising alternative to conventional disinfection process.
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Molecular Catalysis
·
2025
·
IF 4.9
Xuetong Liu,Chi Zhang,Nuoyan Li,Runfeng Li,Songlin Lei,Wei Hong,Shuguang Deng,Jun Wang
Herein, a novel and flexible self-supporting gas diffusion electrode (GDE) was fabricated, which including an electrodeposited Bi nanocomposite as a catalyst layer and MIL-101 derived porous carbon in the gas diffusion layer (GDL). Compared with the conventional fabrication of GDE electrodes, the electrodeposition approach can avoid the tedious drop-casting processes of the catalyst layer (CL). The in situ growth mode by electrodeposition can also ensure the firmly interaction between CL and current collector, thus enhancing the stability of the electrode. Meanwhile, the porous carbon derived from MIL-101 which with a high specific area is conducive for the CO 2 enrichment on the electrode, thus facilitate the reaction with high current density. Owe to the special structure, the resultant catalyst showed excellent performance for electrocatalytic CO 2 reduction reaction (CO 2 RR) with enhanced formic acid generation. Notably, at -1.37 V ( vs. RHE), a large current density of 400 mA cm -2 and a high formate Faraday efficiency (FE formate ) of 96.5 % were achieved, and the yield of formic acid reached 46.5 mmol cm -2 h -1 , which is superior to most electrocatalytic catalysts for CO 2 RR. In addition, the FE formate value remained high (>90 %) over a wide voltage window of 800 mV, and the catalyst also maintained stable operation at industrial current density for 70 h. This work provides a new strategy for the design of GDEs with novel structure to achieve high activity and durability for different electrocatalysis.
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TALANTA
·
2025
·
IF 6.1
Haotian Chen,Zimo Chen,Hanbing Yao,Yujuan Zhan,Binyu Xiao,Shuangshuang Liu,Jiayi Yan,Yifu Li,Chang Shu
Dopamine (DA) is an essential biomarker implicated in the diagnosis of neurological diseases. In this work, we designed a dual-enzyme mimetic activity MIL-101(Fe) that catalyzed specific cyclization reaction between 1,3-dihydroxynaphthalene (NR) and dopamine. As the concentration of dopamine increased, the fluorescence emission of NR at 440 nm was markedly quenched, concomitant with the emergence of a new fluorophore exhibiting enhanced emission at 480 nm and increased absorbance at 462 nm. The ratiometric fluorescence/colorimetric dual-mode detection strategy provided intrinsic self-calibration to effectively mitigate signal variations. Furthermore, a linear correlation was established for ratiometric fluorescence signal across the range of 0.25–35 μM (R 2 = 0.999), and similarly for colorimetric absorbance (R 2 = 0.999). This method provided an accurate, specific, sensitive and high-throughput detection of dopamine in human serum.
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