JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
·
2025
·Vol. 36
·期 30
·1-21
·
IF 2.8
Yang Minjie,Zou Congyang,Ji Yufeng,Liu Ruijie,Xu Ying
A novel MIL-101(Fe)/Bi₂S₃ Z-scheme heterojunction with a metal–organic framework (MOF) structure was synthesized via a solvothermal method. Compared with pristine MIL-101(Fe) and pristine Bi₂S₃, this composite exhibits a significant breakthrough in degradation performance toward rhodamine B (RhB) and tetracycline hydrochloride (TCH). Specifically, it achieves a degradation efficiency of 95.7% for 20 mg/L TCH within 120 min and 98.6% for 40 mg/L RhB within 90 min.Characterizations including X-ray diffraction (XRD), scanning electron microscopy (SEM), ultraviolet–visible diffuse reflectance spectroscopy (UV–Vis DRS), and electrochemical impedance spectroscopy (EIS) confirm that the MOF structure of MIL-101(Fe) provides a stable support matrix for Bi₂S₃. Moreover, the construction of the Z-scheme heterojunction can effectively suppress the recombination of photogenerated electron–hole pairs while retaining the strongly oxidizing hydroxyl radicals (・OH) and strongly reducing superoxide radicals (・O₂⁻). More importantly, after five recycling cycles, the degradation efficiencies of the composite for TCH and RhB remain at 86.8% and 88.6%, respectively, with no obvious damage to its crystal structure after cycling. This demonstrates superior structural stability and reusability compared to most reported MOF-based photo-Fenton catalysts.
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Materials Today Chemistry
·
2026
·
IF 7.4
Yu Xia,Aiping Wang,Qiao Hu,Guangming Han,Kaidi Gao,Yangyang Gao,Ruize Wang,Yongqi Wang,Jianfeng Yao
A well-designed Fe-N dual sites amino-functionalized (MIL-101(Fe)-NH 2 ) separator is fabricated. • The unsaturated Fe sites in the MOF act as strong anionphilic modifiers to adsorb PF 6 − . • The polar -NH 2 groups act as Lewis's base sites to enhance electrolyte wettability. • The synergistic Fe-N sites induce the formation of a stable solid electrolyte interphase. • This separator can regulate lithium deposition and enable high-performance lithium metal batteries. Lithium-based batteries utilizing metallic lithium anodes have attracted widespread research interest due to their exceptional theoretical energy density. However, the growth of dendritic lithium structures, unstable solid electrolyte interphase (SEI) and associated safety concerns pose substantial obstacles to their commercial application. Traditional polypropylene (PP) separators suffer from poor electrolyte affinity and electrochemical inertness, causing heterogeneous Li + distribution and severe interfacial polarization. Herein, an amino-functionalized MIL-101(Fe)-modified PP separator is successfully developed to regulate Li deposition through the synergistic effects of Fe-N dual active sites. The unsaturated Fe sites in the MOF act as strong anionphilic modifiers to adsorb PF 6 − and suppress anion migration; the polar -NH 2 groups act as Lewis's base sites to enhance electrolyte wettability and accelerate ion transport. These synergistic Fe-N sites induce the in-situ formation of a stable LiF/Li 3 N-rich and flexible inorganic-organic hybrid SEI, preventing the penetration of dendritic lithium. Electrochemical testing reveals that the Li|Li symmetric cells achieve more than 650 h of uniform lithium deposition and also stable cycling at elevated temperatures. Furthermore, the LiFePO 4 |Li cells and the LiFe 0.5 Mn 0.5 PO 4 |Li cells employing this modified separator demonstrate superior cycling stability and enhanced rate capability. Modifying separators with functionalized metal-organic frameworks (MOFs) presents a plausible strategy to improve the performance of electrochemical batteries, contributing to an in-depth discussion of the application of MOFs in lithium battery technology. Amino-functionalized separators (PP@MIL-101-NH 2 ) are successfully designed to regulate ion transport for high-performance lithium metal batteries. The unsaturated Fe sites in the MOF act as strong anionphilic modifiers to adsorb PF 6 − ; the polar -NH 2 groups act as Lewis's base sites to enhance electrolyte wettability. Synergistic Fe-N sites induce the formation of a stable LiF/Li 3 N-rich solid electrolyte interphase, preventing the penetration of dendritic lithium. Download: Download high-res image (365KB) Download: Download full-size image
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Applied Materials Today
·
2026
·
IF 7
Madiha Rafiq,Dan Liao,Changkun Liu
Ternary g-C 3 N 4 /Ti 3 C 2 T x /MIL-101(Fe) photocatalyst was constructed via in situ assembly. • Ti 3 C 2 T x promotes interfacial charge separation and accelerates electron transfer. • Rapid in situ H 2 O 2 generation enables an oxidant-free visible-light photo-Fenton process. • CTF achieves efficient, broad-spectrum degradation of dyes and PPCPs. Visible-light photo-Fenton oxidation represents a promising strategy for removing dyes and pharmaceuticals/personal care products (PPCPs), which are persistent water contaminants. However, its broader application is constrained by challenges such as inefficient charge separation and dependence on externally added hydrogen peroxide (H 2 O 2 ). In this study, a ternary g-C 3 N 4 /Ti 3 C 2 T x /MIL-101(Fe) photocatalyst was synthesized via the in-situ growth of MIL-101(Fe) on g-C 3 N 4 /Ti 3 C 2 T x , enabling efficient visible-light-driven, zero-external H 2 O 2 -added photo-Fenton degradation of organic pollutants. The hybrid system exhibits significantly enhanced oxygen activation and interfacial electron-transfer capability, with in situ H 2 O 2 generation rates about three times higher than those of pristine g-C 3 N 4 . Under visible-light irradiation, the composite continuously produces reactive oxygen species ( ∙ O 2 - , and ∙ OH) at substantially higher levels than g-C 3 N 4 and g-C 3 N 4 /MIL-101(Fe), indicating promoted charge separation and faster interfacial electron transfer. As a result, the catalyst enables broad-spectrum pollutant removal within 60 min, achieving degradation efficiencies of 99.78% (methylene blue), 99.49% (rhodamine B), 88.27% (tribromophenol), 61.50% (doxycycline hydrochloride), and 78.98% (levofloxacin). Overall, rapid in situ H 2 O 2 formation, coupled with efficient ROS generation, enables high-performance pollutant degradation without the need for external oxidant dosing, providing a green strategy for degrading dyes and PPCPs under visible light. Download: Download high-res image (174KB) Download: Download full-size image A ternary g-C 3 N 4 /Ti 3 C 2 T x /MIL-101(Fe) photocatalyst enables visible-light-driven, oxidant-free photo-Fenton degradation of dyes and PPCPs through MXene-promoted charge separation and rapid in situ H 2 O 2 generation. The self-generated H 2 O 2 activates Fe 3+ /Fe 2+ cycling to continuously produce h + , ∙O 2 - , and ∙OH, achieving efficient pollutant mineralization.
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ACS Omega
·
2023
·
IF 4.1
Qiyue Zhang,Aori Qileng,Jiale Li,Yiran Cao,Weipeng Liu,Yingju Liu
Organic dyes can produce harmful effects on the water environment, such as affecting the growth of aquatic organisms, reducing the transparency of water bodies, and causing eutrophication of water bodies, so it is necessary to mitigate the hazards of organic dyes. In this study, a metal–organic framework [NH2-MIL-101(Fe)] was synthesized by the solvothermal method as a carrier for the in situ uniform deposition of AgCl nanoparticles on its surface, which was successfully used for both adsorption and degradation of Congo red. Adsorption results showed that the adsorption kinetics conformed to the proposed secondary adsorption kinetics equation with a maximum adsorption capacity of 248.4 mg·g–1. Furthermore, the degradation results indicated that with the aid of sodium borohydride as a reducing agent, the degradation of Congo red followed pseudo-first-order kinetics with a degradation rate of 0.077 min–1, and the complete degradation of Congo red was finished within 18 min. Therefore, AgCl/NH2-MIL-101(Fe) may find a potential application in the removal of dyes from wastewater.
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PubMed
高影响因子
CHEMOSPHERE
·
2022
·
IF 8.943
Lu Zheng,Yifan Gu,Baolv Hua,Jiarui Fu,Fengting Li
Metal-organic frameworks have been investigated in Fenton-like catalysis for tetracycline hydrochloride degradation, a widely used antibiotic which threatens the growth and health of creatures. However, powder phase and absence of large pores limit the materials’ degradation performance and application. In this work, a hierarchical macro-meso-microporous composite melamine sponge@MIL-101-Fe-NH 2 was firstly designed and constructed. While the micropores provided plenty of active sites to generate reactive oxygen species , the macropores and mesopores accelerated mass transfer. Besides, MIL-101-Fe-NH 2 particles dispersed on melamine sponge individually, exposing more catalytic sites and avoiding inactivation caused by aggregation compared to powder catalysts. Its catalysis performance for tetracycline hydrochloride degradation was evaluated through changing various influence factors like H 2 O 2 concentration, catalyst amount, pH and coexisting ions. Different from the preference of homogenous Fenton catalysts for pH 2–4, the composite displayed the most effective degradation at a subacid environment closer to nature with 77.24% in 30 min. Owing to the synergistic effect of hierarchical porous structure and monodispersed nanoparticles , the composite exhibited faster reaction rate and longer persistence compared to powder MIL-101-Fe-NH 2 . Easy recycling and less ion leaching made it advantages for practical application. •OH, •O 2 − and 1 O 2 active species contributed together to the degradation and two main possible degradation pathways were put forward based on 35 detected intermediates.
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CELLULOSE
·
2022
·Vol. 30
·期 2
·1171-1191
·
IF 6.123
Tu Chao,Sun Zenghui,Huang Fei,Wu Ziwei,Chen Hang
The photocatalytic process is an energy-saving and high-efficiency wastewater treatment technology. In this work, a simple in-situ hydrothermal method was used to prepare a photocatalytic material based on waste loofah with high efficiency, reusability and excellent heterostructure to improve the photodegradation efficiency. The prepared MoS 2 @MIL-101(Fe)@Carboxylated loofah composite material was characterized by scanning electron microscope (SEM), electrochemical impedance spectroscopy (EIS), UV–Vis diffuse reflection spectroscopy (UV–vis DRS), X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FTIR), and transient photocurrent (TPC). The composite material demonstrated high adsorption capacity for hydrochloride (TC) and methylene blue (MB) and photocatalytic capacity under visible-light irradiation at room temperature which were attributed to the porous structure, strong visible-light absorption, and low recombination velocity of electron–hole pairs due to the heterojunctions. The loofah sponge used as a substrate can provide a means for powder catalyst recovery and waste cellulose recycling. Meanwhile, the photocatalyst proved excellent stability in the MB degradation experiment and could be reused for four cycles.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Ziyi Xiao,Rui Wu,Tingting Shu,Yingxi Wang,Ling Li
In order to further improve the catalytic performance of MIL-101, cobalt-doped MIL-101(Fe,Co) was synthesized by solvothermal method. By adjusting the ratio of cobalt doping, the MIL-101(Fe,Co 20% ) with the best catalytic activity was obtained. The activation performance of MIL-101(Fe,Co 20% ) for peroxymonosulfate (PMS) was studied using Rhodamine B (RhB) as a pollutant model. The experimental results proved MIL-101(Fe,Co 20% ) with much better catalytic performance than MIL-101(Fe), which can degrade more than 99% of RhB within 15 min. The effects of initial solution pH and coexisting anions in water on the degradation of RhB were further discussed. The results showed that MIL-101(Fe,Co 20% ) was with excellent stability and degradation efficiency can still keep above 90% after five cycles. The free radical quenching experiments were further studied to explore the degradation mechanism. It can be concluded that SO 4 - · was the main active free radical for the degradation of RhB. The possible intermediate products in the degradation process of RhB were analyzed by LC-MS. Combined with the comparison of XPS before and after the reaction, the possible reaction mechanism of RhB degradation process was inferred.
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CHEMICAL PAPERS
·
2017
·Vol. 72
·期 1
·235-250
·
IF 1.258
Duan Mei-Juan,Guan Ze-yu,Ma Yong-Wen,Wan Jin-Quan,Wang Yan,Qu Yan-Fei
In this work, effective and novel heterogeneous catalysts of Metal–organic framework MIL-101(Fe) doped with cobalt (Co 2+ ) or copper (Cu 2+ ) have been synthesized by post-synthesis method, namely Co–MIL-101(Fe) and Cu–MIL-101(Fe). The initial and metal-doped samples were tested to activate persulfate (PS) for removal of Acid Orange 7 (AO7) in water. The surface of samples were characterized using X-ray diffraction, Fourier transform infrared spectroscopy, Raman spectroscopy, N 2 adsorption, scanning electron microscopy and transmission electron microscopy. The addition of Cu 2+ and Co 2+ could alter structure characteristics of MIL-101(Fe) in crystal structure and morphology. The unusual octahedron morphology of MIL-101(Fe) turned to be irregular, disorder and a rod-like morphology was shaped. What is more, Co doping caused greater changes in structure characteristics in comparison with Cu doping. The alteration was reflected in the catalytic capacity of PS activation. An interesting note was that, whether Co or Cu doping, metal-doped MIL-101(Fe) greatly improved the PS activation as compared to unmodified MIL-101(Fe). The removal rate of AO7 was about 66, 92, 98% in MIL-101(Fe)/PS, 6%wtCu–MIL-101(Fe)/PS and 6%wtCo–MIL-101(Fe)/PS system, respectively. Some results also suggested the performance of Co–MIL-101(Fe) was superior to that of Cu–MIL-101(Fe). Additionally, a series of parameters were designed to achieve maximum capacity of PS activation. Such an enhancement in activity may be attributed to the main reasons: the new active sites created by metal additives; an increase in number of active Fe sites produced by Co and Cu doping which results in alteration of morphology and structure of catalysts.
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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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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2016
·Vol. 23
·期 15
·15218-15226
·
IF 2.76
Yue Xinxin,Guo Weilin,Li Xianghui,Zhou Haihong,Wang Ruiqin
In this study, a novel core-shell Fe 3 O 4 @MIL-101 (MIL stands for Materials of Institute Lavoisier) composite was successfully synthesized by hydrothermal method and was fully characterized by X-ray diffraction, transmission electron microscopy, Fourier-transform infrared spectra, and X-ray photoelectron spectroscopy. The composite was introduced as a catalyst to generate powerful radicals from persulfate for the removal of Acid Orange 7 in an aqueous solution. Effects of the central metal ions of MIL-101, amino group content of MIL-101, and pH were evaluated in batch experiments. It was found that both hydroxyl and sulfate radicals were generated; importantly, sulfate radicals were speculated to serve as the dominant active species in the catalytic oxidation of Acid Orange 7. In addition, a possible mechanism was proposed. This study provides new physical insights for the rational design of advanced metal-organic frameworks (MOF)-based catalysts for improved environmental remediation.
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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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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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