JOURNAL OF CATALYSIS
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2025
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IF 6.5
Qi Chen,Xingxing Huang,Cheng Liu,Yueling Chen,Jionghua Wu,Jimmy C. Yu,Ling Wu
The attainment of rapid charge mobility and effective N 2 activation is of critical importance for photocatalytic nitrogen fixation but it has always been a challenge. Such challenge may be met by the construction of a Type II MoS 2 nanoparticles/ MIL-100(Fe) heterojunction photocatalyst. The new material possesses charge migration channels that facilitate the separation of photogenerated carriers. This charge redistribution during photocatalysis is confirmed by experimental results showing a decrease of charge density on the Fe species and an increase of that on Mo. Moreover, DFT calculations show that the adsorption of N 2 and H 2 O is more likely to occur on Fe sites and Mo sites, respectively. These findings clearly suggest a drastically improved spatial isolation of reduction and oxidation sites on the photocatalyst as compared to pristine MIL-100(Fe). The optimized MoS 2 /MIL-100(Fe) exhibits a NH 4 + yield rate of 1.29 μmol·h −1 as excellent utilization of photoinduced electron-hole pairs and effective adsorption and activation of N 2 become possible. This work offers an insight on the synergy of heterojunction engineering with coordinated activation for photocatalytic ammonia synthesis.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Chiyu Wen,Chao Wang,Defang Liu,Zhuo Cheng,Jing Zhao,Hongli Zhang,Jun Wang,Guoxiang Zhu,Yongfa Zhu
Nitro-aromatic compounds constitute predominant explosive materials extensively utilized in military applications and industrial blasting operations. However, the manufacturing, consumption, and decommissioning of these explosives generate significant quantities of wastewater exhibiting both ecotoxicological hazards and explosive potential. Herein, an amino-functionalized MIL-100(Fe) (AFM) catalyst demonstrating simultaneously enhanced explosive capture and degradation is developed. The synergistic interplay of electrostatic attraction and hydrogen bonding between the amino groups of AFM and nitro groups of nitro-aromatic explosive confer exceptional binding affinity. The optimized AFM exhibits a remarkable 2,4,6-trinitrotoluene (TNT) adsorption of 14.93 mg/g, which is 3.6 times of unmodified MIL-100(Fe). In photo-Fenton reactions, the optimized AFM completely degrades TNT within 30 min, and achieves a mineralization efficiency as high as 96.7 %. Moreover, the AFM exhibits excellent stability, retaining a high TNT degradation efficiency of 97.7 % after five consecutive cycles. The currently designed AFM catalyst possessing fascinating explosive affinity and high explosive mineralization efficiency is expected to advance sustainable remediation of high-risk explosive wastewater.
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ENERGY CONVERSION AND MANAGEMENT
·
2018
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IF 6.377
Hui Li,Fengsheng Liu,Xiaoling Ma,Zhongjie Wu,Yan Li,Linhua Zhang,Shoujun Zhou,Yaxin Helian
Strontium oxide (SrO) is restricted by poor reusability and pore structure in catalyzing transesterification for biodiesel production. To address this problem, metal organic frameworks is employed as a carrier to support strontium carbonate by mechanical mixing method (MM) and in situ titration method (ST), and then calcined under inert atmosphere to obtain the catalyst of MM–SrO and ST–SrO. As a comparison, the reusability of pure SrO is compared and the homogeneous contribution of leached active sites for ST–SrO and MM–SrO are also assessed. The catalysts are characterized by TG, XRD, FTIR, EDS, Hammett indicator titration, nitrogen adsorption–desorption, and VSM. From the catalyst reusability, MM–SrO exhibits the excellent performance, where the maximum conversion of 96.19% is achieved at molar ratio of methanol to oil 12, catalyst addition 8 wt% (refer to oil), reaction temperature 65 °C within 30 min. And the conversion of 82.49% is still obtained at the third cycle, which could be easily separated from the mixture by external magnetic field after each cycle as well. In order to optimize the activation condition and investigate MM–SrO deeply, thermal characteristics of its corresponding precursor are further evaluated, where the TG experiments are conducted at heating rate of 20, 30, and 40 °C/min. and kinetic parameters are calculated through model–free method and Avrami theory, respectively.
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Desalination and Water Treatment
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2024
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IF 1
Shanshan Chen,Kang Wen,Xiaoting Zhang,Ruize Zhang,Runping Han
Metal organic frameworks are attracting scientific interest in adsorption applications owing to their large surface area and controllable pore size or shape over both microporous and mesoporous domains. Based on this, an iron(III) trimesic acid MIL-100(Fe) was facilely synthesized by hydrothermal treatment and used as adsorbent to remove neutral red (NR) from aqueous solution. MIL-100(Fe) was characterized using X-ray diffraction, scanning electron microscopy and transform infrared spectroscopy. MIL-100(Fe) was studied in view of the adsorption isotherms, thermodynamics, kinetics, and regeneration of the adsorbent. The adsorption kinetics data of NR were found to be in agreement with pseudo-second-order model. Temkin model was observed to be more suitable than Freundlich and Langmuir models in describing the adsorption isotherm. The maximum adsorption quantity was 333 mg g –1 at 313 K from Langmuir model. Thermodynamic parameters indicated that the NR adsorption process was endothermic and spontaneous. The NR-loaded MIL-100(Fe) adsorbent was regenerated and reused using pH = 2, 75% ethanol. A single-stage batch design for NR adsorption onto MIL-100(Fe) was also presented based on Temkin isotherm model equation. Based on the findings, MIL-100(Fe) is a promising adsorbent for the removal of cationic dyes from solution and thus can be used in practical application.
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JOURNAL OF SOLID STATE CHEMISTRY
·
2026
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IF 3.2
Yongwei Li,Shuting Fan,Zhihao Fang,Xiangru Zeng,Jinting Jiang,Fangfang Liu,Xuening Lun,Chengjie Li
A simple mineralizer regulation strategy is developed to tune the structure of hydrothermal MIL-100(Fe). • NaHCO 3 enhances the surface area of MIL-100 (Fe), affording superior XO adsorption performance. • Synergistic pore adsorption, hydrogen bonding, Fe 3+ coordination and π-π stacking enable efficient XO removal. Metal-organic frameworks (MOFs) are promising crystalline porous solids, whose functional properties are highly dependent on their crystallinity, defect states and pore characteristics. In this work, hydrothermal synthesis was employed to prepare MIL-100(Fe) materials modulated by three different mineralizers: sodium carbonate, acetic acid, and sodium bicarbonate; mineralizer-free pristine MIL-100(Fe) was used as the reference sample. The addition of mineralizers effectively modulates the crystal structure and porosity of MIL-100(Fe). All mineralizer-modified samples exhibit larger specific surface area compared with the pristine material. Among them, NaHCO 3 -regulated MIL-100(Fe) achieves the best adsorption performance toward xylenol orange (XO), which originates from its optimized porous structure. Adsorption experimental data fit well with the pseudo-second-order kinetic model and Langmuir isotherm model. The maximum monolayer adsorption capacity calculated by the Langmuir model reaches 155.28 mg/g, which is competitive with many reported adsorbents. Synergistic adsorption mechanisms, including pore-filling effect, hydrogen bonding, Fe 3+ complexation and π-π stacking interactions, have been elucidated. This work presents a facile mineralizer-mediated strategy for tuning the solid-state structural features of MIL-100(Fe), offering experimental insights for the structure-performance optimization of Fe-based MOF solids. Download: Download high-res image (357KB) Download: Download full-size image
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Journal of Environmental Chemical Engineering
·
2023
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IF 7.7
Yongpan Shan,Yajie Ma,Changcai Wu,Xiangliang Ren,Xianpeng Song,Dan Wang,Hongyan Hu,Xiaoyan Ma,Yan Ma
Control release of pesticides based on target plant characteristics is highly desirable for improving the effective utilization rate and reducing non-target organism risks. Here, the controlled release formulations (Cu-CS@IN@MIL-100 (Fe)) were successfully prepared by employing MIL-100 (Fe) as the carrier material, indoxacarb (IN) as the model pesticide, and chitosan (CS) as a coating to chelate copper ions by chemical crosslinking. The prepared Cu-CS@IN@MIL-100 (Fe) had an acceptable loading content (36.25 %). The introduction of CS and copper ions endowed it with sustained release properties under weak acidity conditions like cotton leaves. The laboratory bioassay experiments showed that Cu-CS@IN@MIL-100 (Fe) had practical good insecticidal activity (LC 50 = 4.936 mg/L) in controlling Helicoverpa armigera larvae. For long-term control efficacy experiments, after 14 days of application, the Cu-CS@IN@MIL-100 (Fe) treatment (73 %) mortality of Helicoverpa armigera larvae was significantly higher than the 15 % indoxacarb suspension concentrates (SC) treatment (27 %). Moreover, Cu-CS@IN@MIL-100 (Fe) had no adverse effect on cottonseed germination and the acute toxicity to Chrysopa pallens larvae was significantly lower than IN SC. Therefore, MIL-100 (Fe) could be used as an ecological safety carrier for pesticide delivery to improve IN effective utilization and reduce non-target organism risks.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Chengyu Huangfu,Shuning Yu,Bo Tong,Anni Yang,Jiafei Lyu,Xianghai Guo
MIL-100(Fe) is a kind of metal–organic frameworks (MOFs) with robust water and chemical stability. The adsorption kinetics, isotherms, thermodynamics and regeneration of MIL-100(Fe) were investigated to illustrate the process of efficient lithium adsorption. The adsorption kinetics of MIL-100(Fe) followed Pseudo-second-order model, and the lithium adsorption equilibrium was reached rapidly in 2 h. Langmuir model fit best with the adsorption isotherms, indicating chemisorption of lithium ions on MIL-100(Fe) and possibly a monolayer adsorption process. By calculating thermodynamic parameters (Δ G θ , Δ H θ and Δ S θ ), the adsorption of lithium on MIL-100(Fe) can be illustrated by a spontaneous endothermic process. The adsorption mechanism involved electrostatic interaction, impact of crystal defect sites and coordinative interactions between metal active sites and lithium ions (Fe—F‧‧‧Li). MIL-100(Fe) was regenerated for four cycles, and there was only a slightly decrease in adsorption capacity and the morphology remained stable. Combined with extremely short equilibrium time and high stability, MIL-100(Fe) can be a promising adsorbent for lithium extraction.
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ENVIRONMENTAL RESEARCH
·
2022
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IF 8.431
Mingyu Li,Yuhan Ma,Jingjing Jiang,Tianren Li,Chongjun Zhang,Zhonghui Han,Shuangshi Dong
Heterogeneous photo-Fenton technology has drawn tremendous attention for removal of recalcitrant pollutants. Fe-based metal-organic frameworks (Fe-MOFs) are regarded to be superior candidates in wastewater treatment technology . However, the central metal sites of the MOFs are coordinated with the linkers, which reduces active site exposure and decelerates H 2 O 2 activation. In this study, a series of 2, 5-dioxido-1, 4-benzenedicarboxylate (H 2 DOBDC)-functionalized MIL-100(Fe) with enhanced degradation performance was successfully constructed via solvothermal strategy. The modified MIL-100(Fe) displayed an improvement in photo-Fenton behaviors. The photocatalytic rate constant of optimized MIL-100(Fe)-1/2/3 are 2.3, 3.6 and 4.4 times higher compared with the original MIL-100(Fe). The introduced H 2 DOBDC accelerates the separation and transfer in photo-induced charges and promotes Fe(II)/Fe(III) cycle, thus improving the performance. •OH and •O 2 − are main reactive radicals in tetracycline (TCH) degradation. Dealkylation, hydroxylation, dehydration and dealdehyding are the main pathways for TCH degradation.
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高影响因子
JOURNAL OF MOLECULAR STRUCTURE
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2022
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IF 3.841
Chenyan Wu,Qianhong Shen,Suhua Zheng,Xinyu Zhang,Jiansong Sheng,Hui Yang
A novel Bi 2 Sn 2 O 7 @MIL-100(Fe) composite photocatalyst was fabricated by loading Bi 2 Sn 2 O 7 nanoparticles on the surface of mesoporous MIL-100(Fe). The structure-property relationships of such composite photocatalyst were studied. The results exhibit that the formed Bi 2 Sn 2 O 7 @MIL-100(Fe) heterojunction promote the separation of photo-generated carriers, leading to the enrichment of photo-generated electrons on MIL-100(Fe). Meanwhile, MIL-100(Fe) can provide more active sites for photocatalytic reaction due to its extraordinary specific surface area. Therefore, the Bi 2 Sn 2 O 7 @MIL-100(Fe) composite photocatalyst exhibits excellent superoxide-radical-dominated photocatalytic activity and is more propitious to degrading the contaminants such as ciprofloxacin, which can be efficiently degraded in the absence of superoxide radicals. The Bi 2 Sn 2 O 7 @MIL-100(Fe) composite reveals enhanced photocatalytic activity for degrading ciprofloxacin with rate constant (0.0143 min −1 ) 1.96 and 3.86 times higher than that of pure MIL-100(Fe) (0.0073 min −1 ) and pure Bi 2 Sn 2 O 7 (0.0037 min −1 ), respectively.
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Biomaterials Science
·
2021
·Vol. 9
·期 20
·6772-6786
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IF 6.843
Sulan Luo,Yiting Zhao,Kewei Pan,Yixian Zhou,Guilan Quan,Xinguo Wen,Xin Pan,Chuanbin Wu
The low oxygen level in tumors significantly reduces the antitumor efficacy of photodynamic therapy (PDT). The provision of O2 and monomeric hydrophobic photosensitizers (PSs) under physiological conditions would greatly help to shrink malignant tumors. We take advantage of the high porosity and multifunctionality of metal–organic frameworks (MOFs) to fabricate a simple all-in-one nanoplatform mediated by microneedle delivery to achieve synergistic O2 evolution and chemophototherapy. An iron(III)-based MOF (MIL-100(Fe)) acted not only as a vehicle for the concurrent delivery of zinc phthalocyanine (ZnPc) and doxorubicin hydrochloride (Dox), but also to supply O2 by decomposing hydrogen peroxide (H2O2) in the tumor microenvironment via a Fenton-like reaction. In vitro and in vivo experiments indicated that the nanoplatform had excellent biocompatibility and exerted enhanced anticancer effects. The encapsulated drug was sustainably released from the nanoplatform skeleton in response to acidic tumor microenvironments. Moreover, upon 660 nm light irradiation, ZnPc effectively produced reactive oxygen species (ROS) due to the reduction of hypoxia by MIL-100(Fe). A microneedle technique was adopted to directly deliver the nanoplatform into superficial tumors rather than via systemic circulation. Hence, this study provides a new strategy for more efficient chemophototherapy of hypoxic superficial tumors.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2019
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IF 6.361
Haibo Zhang,Jia Wen,Ying Fang,Siyu Zhang,Guangming Zeng
Hypothesis Modification of MIL-100(Fe) with ethanediamine (ED) is expected to improve the removal percentage of Pb(II) ions from aqueous solution. Nevertheless, the adsorption performance of ED-MIL-100(Fe) in natural waters will be affected by natural organic matter such as fulvic acids (FA). Hence, it is necessary to study the influence of FA on the physicochemical property, adsorption behavior and mechanisms of ED-MIL-100(Fe) towards the removal of Pb(II) from water. Experiments Batch adsorption experiments were conducted to compare adsorption capacity of MIL-100(Fe) and ED-MIL-100(Fe) for Pb(II). In addition, XRD , FTIR, SEM and XPS techniques were applied to investigate the characteristics, adsorption isotherms , and kinetics in the presence and absence of FA. Findings ED-MIL-100(Fe) enabled 99% removal of Pb(II) from water at or below 60 mg L −1 , whereas the MIL-100(Fe) hardly adsorbed any Pb(II). Additionally, the adsorption percentage of the Pb(II) ions (76%) outcompeted that of other metal ions (i.e. Co, Cu, Ni, Zn, and Cd) (each ≤ 25%) in the mixed solution. The negative surface charge of ED-MIL-100(Fe) was not affected by FA. Increasing FA concentration steadily increased the functional groups surrounding the ED-MIL-100(Fe) via electrical interaction, thus facilitating the Pb(II) ions adsorption.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2025
·
IF 3.9
Bolun Yu,Jun Chen,Quanzhang Liu,Shuoyang Li,Xiaohang Zhang,Bowen Liang,Zuhong Lin,Haipu Li,Jingjing Yao
The use of metal–organic framework-derived materials for removing micropollutants from water is increasing, but precise composition control remains a challenge. In this study, 14 MIL-100(Fe)-derived materials were synthesized to adsorb and remove antipyrine (ANT) from water by optimizing the heating rate, pyrolysis temperature, and activation methods. The adsorbents demonstrated excellent ANT removal performance across a pH range of 3 to 11, as well as in complex water bodies. They also exhibited easy recovery and outstanding regeneration capabilities. Under the optimized conditions (i.e., ANT content: 10 mg/L, M-600–2 dosage: 0.1 g/L, and pH: 7), M-600-10 displayed the highest adsorption capacity (23.10 mg/g for ANT) while MIL-100(Fe) had limited adsorption capability (2.56 mg/g for ANT). The adsorption process was exothermic and spontaneous, influenced by both membrane diffusion and intraparticle diffusion, and followed the Freundlich and pseudo-second-order models. Despite variations in surface areas (75.70–261.91 m2/g), total pore volumes (0.2019–0.5984 cm3/g), and average pore sizes (7.47–13.99 nm), there was no strong linear relationship with adsorption capacity (7.47–15.99 mg/g). The major components, including Fe/pyrrolic N-doped graphene (PING), Fe3C/PING, Fe3O4/PING, and PING, had calculated adsorption energies of −0.94, −2.16, −0.79, and −2.24 eV, respectively, which correlated positively with Bader charge transfer numbers. The adsorbents relied on van der Waals forces for ANT adsorption, with PING exhibiting the strongest interactions and Fe3O4/PING exhibiting the weakest. These findings enhance the theoretical understanding of derived materials and expand their application in water purification.
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