ENVIRONMENTAL RESEARCH
·
2023
·
IF 8.3
Chunyan Hu,Jinke He,Jianjun Liang,Tao Lin,Qiuliang Liu
A novel photo-Fenton catalyst α-Fe 2 O 3 @g-C 3 N 4 @NH 2 -MIL-101(Fe) (FGN) with dual Z-scheme heterojunction was successfully prepared by hydrothermal method to degrade tetracycline (TC). The preparation conditions were optimized by orthogonal test, and the successful synthesis was confirmed by characterization analyses. The prepared FGN showed better light absorption performance, higher photoelectrons-holes separation efficiency, lower photoelectrons transfer resistance, and higher specific surface area and pore capacity compared with α-Fe 2 O 3 @g-C 3 N 4 and α-Fe 2 O 3 . The effects of experimental conditions on the catalytic degradation of TC were investigated. The degradation rate of 10 mg/L TC could reach 98.33% within 2 h when the dosage of FGN was 200 mg/L, and the degradation rate could remain 92.27% after 5 times of reuse. Furthermore, the XRD spectra and XPS spectra of FGN before and after reuse were compared to explore the structural stability and catalytic active sites of FGN, respectively. According to the identification of oxidation intermediates, three degradation pathways of TC were proposed. Through H 2 O 2 consumption experiment, radical-scavenging experiments, EPR results, the mechanism of the dual Z-scheme heterojunction was proved. The improved performance of FGN was attributed to the dual Z-Scheme heterojunction effectively promoting the separation of photogenerated electrons from the holes and accelerating the electrons transfer , and the increase of the specific surface area.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
FOOD CHEMISTRY
·
2024
·
IF 8.5
Yu Zou,Wanshan Wang,Fengyin Duan,Wen Yun,Hong Chen,Yiping Li,Lizhu Yang
An ultrasensitive fluorescence detection strategy of chloramphenicol (CAP) was developed based on product catalysis of tetrahedral DNA framework (TDF) and fluorescent quenching of MIL-101(Fe). The product was used to catalyze the reaction. As the concentration of catalyst increased, the reaction time was significantly shorted to 21 min which was much shorter than other isothermal amplification technologies. Moreover, the multiple fluorophores of TDF and high efficient quenching ability of MIL-101(Fe) provided better performance with a linear range for CAP detecting from 1.6 pM to 80 pM and the limit of detection (LOD) as low as 0.67 pM. In addition, it also demonstrated good specificity and resistance to interference from other related antibiotics. Importantly, this strategy exhibited satisfactory relative standard deviation and recovery results for practical application, exhibiting a favorable application prospect in CAP analysis.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Applied Nano Materials
·
2024
·
IF 5.3
Linlin Zheng,Xuechuan Lv,Yanan Chen,Bingyu Wei,Wanqing Hao,Ziyi Zhang,Jingru Yang,Ruiyu Liu,Xu Zhu,Yanli Zhou,Maotian Xu,Xiaohan Gao,Hui Dong
The iron-based metal–organic framework (NH2-MIL-101(Fe)) nanoparticles exhibited excellent conductivity, exceptional catalytic effect, sturdy stability flexible structure, etc. Consequently, it has been exploited in various applications. Herein, NH2-MIL-101(Fe) nanoparticles were successfully synthesized via the hydrothermal method and were grown in situ onto the pencil core electrode (PCE) for simultaneous determination of caffeic acid (CA) and acetaminophen (AP). The PCE decorated by NH2-MIL-101(Fe) as electrode substrate, combined with the dual effects of the excellent electrocatalytic activity of NH2-MIL-101(Fe) and the commendable electrical conductivity of PCE, the constructed sensor exhibits superior electrochemical sensing activity. The electrochemical behavior of CA and AP at the electrodes were investigated mainly by differential pulse voltammetry (DPV) and cyclic voltammetry (CV), exhibiting broad linear responses from 0.1 to 500 μM, and 0.08 to 800 μM for simultaneous detection of CA and AP, with detection limits of 29 nM and 24 nM, respectively. Moreover, the results of CA and AP in drug and human urine using this sensor were satisfactory, which proved that the sensor is feasible to simultaneously detect CA and AP.
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF MOLECULAR STRUCTURE
·
2024
·
IF 4
Shaopeng Zhang,Jie Ding,Dayong Tian,Jing Wang,Jiale Zhang,Minghua Lu
China faces severe antimony pollution due to long-term, high-intensity mining and smelting operations. Long-term exposure to Sb(III) can lead to chronic respiratory problems. Adsorption method is used to remove Sb(III) because of its simplicity, economy and high efficiency. Therefore, a novel MIL-101(Fe)-Cl/SA hydrogel with oxidation-sorption bifunctionality was developed. 1602 cm −1 and 1025 cm −1 correspond to N H and S = O indicate N-chlorosulfonamide is bonded to MIL-101(Fe)-Cl/SA. MIL-101(Fe)-Cl/SA exhibited rough and wrinkled surfaces with numerous irregular particles by SEM. The presence of O (22 %) and Cl (2 %) confirmed the incorporation of N-chlorosulfonamide and SA into MIL-101(Fe)-Cl/SA by EDS and mappings. The adsorption capacities of MIL-101(Fe)-Cl/SA were 86 mg/g at 298 K and 123.21 mg/g at 328 K by Langmuir model. Kinetic and equilibrium correspond to pseudo-second-order and Langmuir model, respectively. Adsorption was spontaneous and endothermic by thermodynamic analysis. MIL-101(Fe)-Cl/SA exhibited enhanced selectivity in solution containing various ions. Moreover, MIL-101(Fe)-Cl/SA demonstrated potential for regeneration and reuse. The removal process primarily involved oxidation, electrostatic interaction, and complexation. In summary, the capability of MIL-101(Fe)-Cl/SA to adsorb and oxidize Sb(III) underscores its promising potential in mitigating the hazards associated with Sb(III).
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
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.
✓ 已验证
产品关联
DOI
高影响因子
Journal of Water Process Engineering
·
2024
·
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.
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
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.
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Guozhen Qin,Jianfeng Zheng,Yifan Li,Yatao Yang,Xingmin Liu,Xiaojin Han,Zhanggen Huang
Mainly exposed crystal facets and controllable morphology play a key role in the final performance of the preparation of specific nanomaterials . In the present study, a metal–organic framework pyrolysis method without adding solvent modifiers was developed. By adding CO in the calcination atmosphere to change atmosphere ratio, Fe 3 O 4 nanostructures are exposed with different crystal planes and evaluated their performance in NH 3 -SCR reaction. This study proves that SCR catalytic activity of Fe 3 O 4 nanocrystals is dependent on morphology and crystal facet. Compared with materials exposed (1 0 0), catalysts with more (1 1 1) show stronger deNO x performance. The preferential exposure of Fe 3 O 4 (1 1 1) crystal facets increases the concentration of adsorbed oxygen on the catalyst, showing higher surface acidity , and enhances the interaction among NO, O 2 and catalyst, which is conducive to SCR reaction. This is supported by DFT calculations . The results present a great application prospect in preparing nanomaterials with specific crystal structures to effectively treat pollutants.
✓ 已验证
DOI
高影响因子
Journal of Environmental Sciences
·
2026
·
IF 6.5
Mengqi Zhong,Hongrui Ma,Chao Zhu,Tingting Qu,Wenjie Quan
● The differences in the adsorption mechanisms of MIL-101(Fe) for small molecular ligands, larger molecular ligands, and mixed-ligand complexes were investigated. ● The adsorption capacity of MIL-101(Fe) for TA-Cr(Ⅲ) was superior to that of other ligands, with a maximum adsorption amount reaching 183.15 mg/g. ● The adsorption competitive of TA-Cr(Ⅲ) is stronger than that of EDTA-Cr(Ⅲ) and TA-EDTA-Cr(Ⅲ) in the mixed solution. ● The order of binding affinities for different interactions was clarified by combining DFT calculations. The ubiquity of diverse organic-Cr(Ⅲ) complexes in industrial effluents poses a significant challenge to water remediation due to their high stability and complex competitive behaviors. In this study, MIL-101(Fe) was employed to decipher the differential adsorption behaviors and mechanisms of single and co-existing Cr(Ⅲ) complexes, specifically targeting natural (Tannic acid (TA)) and anthropogenic (EDTA) ligands. The experimental results revealed a distinct selective hierarchy as TA-Cr(Ⅲ) > free Cr(Ⅲ) > EDTA-Cr(Ⅲ) > TA-EDTA-Cr(Ⅲ), with values of 183.15, 134.05, 93.02, and 73.80 mg/g, respectively. Among them, TA-Cr(Ⅲ) demonstrated an extremely strong adsorption capacity. Kinetic and isotherm analyses confirmed a chemisorption-dominated process. Crucially, the competitive mechanism was elucidated by integrating spectroscopic characterization with Density Functional Theory (DFT) calculations. The results revealed that while electrostatic interactions drive the initial approach, the specific affinity of phenolic hydroxyl groups in TA towards the Fe-clusters of metal organic frameworks (MOFs), combined with strong π-π stacking interactions, provides an advantage for TA-complexes. The differences of organic-metal complexes were revealed through analysis of electrostatic potential, frontier molecular orbitals and binding energy. This work provides a fundamental understanding of ligand-dependent competitive adsorption, offering a theoretical basis for the selective removal of complexed heavy metals in realistic aquatic environments. Download: Download high-res image (308KB) Download: Download full-size image
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2026
·
IF 5.1
Yingnan Ma,Zixuan Guo,Juan Chen,Shuyan Meng,Zijian Zhang,Jihong Tian,Yanxin Hu,Yijun Fang,Yawen Zhu,Panliang Zhang
High-temperature proton exchange membranes had attracted considerable interest for electrochemical devices such as fuel cells. However, it remained challenging to simultaneously achieve high proton conductivity, effective acid retention, and robust dimensional stability. To address the limitations of conventional filler incorporation, which was insufficient to realize both efficient acid utilization and the construction of continuous proton-conduction networks, we developed a PBI-based mixed-matrix membrane (MMMs) via the in-situ growth of MIL-101(Fe). The in-situ introduced MIL-101(Fe) not only formed a well-dispersed MOFs framework with excellent interfacial compatibility, but also reconfigured the spatial distribution and physicochemical state of phosphoric acid within the membrane, transforming it from disordered accumulation into a continuous hydrogen-bonded pathway for cooperative proton transport. As the extent of MIL-101(Fe) in-situ growth increased, the acid distribution became more uniform, the proton-conduction pathways became more interconnected, the transport resistance was significantly reduced, and the conductivity was markedly enhanced. Meanwhile, the confinement effect of the MOFs channels and their interfacial nanodomains on phosphoric acid effectively suppressed acid loss and substantially improved the dimensional stability of the membrane. This study demonstrated that in-situ grown MIL-101(Fe) not only increased acid accommodation, but more importantly enabled microenvironment regulation and reconstruction of the proton-transport network, thereby providing new insight into the design of high-performance and durable high-temperature proton exchange membranes.
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2026
·
IF 6.7
Jun-Chuan Wang,Peng-Liang Zhang,Wen-Bo Zhang,Tai-Sen Zhang,Zi-Yan Zhen,Tian-Yu Wang,Xiang-Xiang Jia,Gang Yu
Modulating localized electronic structures and interfacial charge-transfer pathways in metal-organic framework (MOF)-based heterogeneous catalysts remains a critical challenge for achieving efficient and durable advanced oxidation processes. Herein, a highly crystalline S-scheme NH₂-MIL-101(Fe)@DQ-TFP (NM@DT) core-shell heterojunction was constructed through a microwave-assisted MOF-first in situ growth strategy. Distinct from conventional physical assembly, the anthraquinone-based β-ketoenamine covalent organic framework (COF) shell was integrated with the amino-functionalized MOF core through chemically coupled growth and interfacial hydrogen-bonding interactions, generating a robust core-shell interface. This intimate interfacial coupling induces spontaneous electronic redistribution and charge polarization, which are verified by X-ray photoelectron spectroscopy, ultraviolet photoelectron spectroscopy, and density functional theory calculations, thereby providing the electronic basis for an internal electric field-assisted S-scheme charge-transfer pathway. The optimized NM@DT-3 heterostructure exhibits enhanced photocatalytic tetracycline degradation performance, achieving 90.70% removal efficiency within 180 min without external H₂O₂ addition. The core-shell configuration not only promotes interfacial charge separation but also creates a spatially confined catalytic microenvironment, enabling efficient oxygen activation and reactive oxygen species evolution coupled with localized H₂O₂ activation at adjacent Fe centers. Mechanistic investigations reveal that freely diffusing hydroxyl radicals (·OH) make only a minor contribution under the tested conditions, whereas superoxide radicals (·O₂⁻), photogenerated holes (h⁺), and singlet oxygen (¹O₂) participate in TC oxidation. In this reaction network, ·O₂⁻ acts as a key intermediate linking photocatalytic O₂ reduction to both H₂O₂ formation and a proposed h⁺-mediated ¹O₂ generation pathway. The reduced reliance on conventional bulk ·OH-dependent chemistry is consistent with the retained catalytic activity of NM@DT-3 under alkaline conditions, with a TC removal efficiency of 77.74% at pH 10. Meanwhile, the chemically integrated core-shell structure effectively suppresses iron leaching, with only 0.107 mg L⁻¹ Fe released during the photocatalytic process. This work provides new insights into engineering chemically coupled MOF/COF interfaces for regulating interfacial charge migration and ROS evolution, offering an effective strategy for constructing stable photo-self-Fenton catalysts for environmental remediation.
✓ 已验证
DOI
高影响因子
CHEMICAL PAPERS
·
2022
·Vol. 76
·期 7
·4379-4392
·
IF 2.146
Zhang Huixian,Hu Xizhou,Xia Hong,Zhou Youxiang,Peng Lijun,Wu Jianyuan,Peng Xitian
Phenoxy carboxylic acid herbicides (PCAs) are widely used in agricultural production. However, due to their potential threat to human health, it is necessary to develop efficient analysis method for monitoring PCA concentration in environment and food samples. Based on dispersive micro-solid phase extraction (D-μ-SPE) with amine-functionalized metal–organic framework MIL-101(Fe)-NH 2 , a selective, sensitive, and cost-efficient method was proposed for the extraction of PCAs from environmental water and rice samples in this study. From the perspective of adsorption kinetics and isotherms, interaction mechanisms between MIL-101(Fe)-NH 2 and PCAs were investigated. Key parameters of D-μ-SPE procedure including adsorbent dosage, solution pH, ionic strength, eluting solution, and washing solutions were optimized. Using of small amount of MIL-101(Fe)-NH 2 could achieve desirable extraction effect due to its large surface area and multiple interactions with PCAs. Under the optimized D-μ-SPE conditions, calibration curves of 8 PCAs were linear within a concentration range of 0.05–5 ng/mL for water samples ( r 2 > 0.9898) and 0.5–50 ng/g for rice samples ( r 2 > 0.9879). Limits of detection of water and rice samples were as low as 0.004–0.008 ng/mL and 0.05–0.1 ng/g, respectively. The recoveries of 8 PCAs ranged from 83.0 to 109.3%. Both inter- and intra-day relative standard deviations were less than 10.3%. Our proposed method was successfully employed in actual environmental water and rice samples.
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）