LANGMUIR
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2024
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IF 3.7
Zhuangzhi Sun,Jiawei Lin,Suwei Lu,Yuhang Li,Tingting Qi,Xiaobo Peng,Shijing Liang,Lilong Jiang
The electrochemical nitrogen reduction reaction (eNRR) has emerged as a promising strategy for green ammonia synthesis. However, it suffers unsatisfactory reaction performance owing to the low aqueous solubility of N2 in aqueous solution, the high dissociation energy of N≡N, and the unavoidable competing hydrogen evolution reaction (HER). Herein, a MIL-53(Fe)@TiO2 catalyst is designed and synthesized for highly efficient eNRR. Relative to simple MIL-53(Fe), MIL-53(Fe)@TiO2 achieves a 2-fold enhancement in the Faradaic efficiency (FE) with an improved ammonia yield rate by 76.5% at −0.1 V versus reversible hydrogen electrode (RHE). After four cycles of electrocatalysis, MIL-53(Fe)@TiO2 can maintain a good catalytic activity, while MIL-53(Fe) exhibits a significant decrease in the NH3 yield rate and FE by 79.8 and 82.3%, respectively. Benefiting from the synergetic effect between TiO2 and MIL-53(Fe) in the composites, Fe3+ ions can be greatly stabilized in MIL-53(Fe) during the eNRR process, which greatly hinders the catalyst deactivation caused by the electrochemical reduction of Fe3+ ions. Further, the charge transfer ability in the interface of composites can be improved, and thus, the eNRR activity is significantly boosted. These findings provide a promising insight into the preparation of efficient composite electrocatalysts.
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高影响因子
International Journal of Environmental Research and Public Health
·
2023
·Vol. 20
·期 5
·4571
·
IF 4.614
Shuyan Yu,Huiying Zhang,Congju Li
In this study, MIL-53(Fe) was innovatively incorporated into carbon felt (CF) by growing in-situ using the solvothermal method. MIL-53(Fe)@carbon felt (MIL-53(Fe)@CF) was prepared and used for the degradation of rhodamine B (RhB). As a new photocatalytic membrane, MIL-53(Fe)@CF photocatalytic membrane has the characteristics of high degradation efficiency and recyclability. Influence of various parameters including MIL-53(Fe)@CF loading, light, electron trapper type, and starting pH on RhB degradation were investigated. The morphology, structure, and degradation properties of MIL-53(Fe)@CF photocatalytic membrane were characterized. Corresponding reaction mechanisms were explored. The results indicated that pH at 4.5 and 1 mmol/L H2O2, 150 mg MIL-53(Fe)@CF could photocatalytically degrade 1 mg/L RhB by 98.8% within 120 min, and the reaction rate constant (k) could reach 0.03635 min−1. The clearance rate of RhB decreased by only 2.8% after three operations. MIL-53(Fe)@CF photocatalytic membrane was found to be stable.Keywords:MIL-53(Fe)@carbon felt;photocatalytic;degradation;rhodamine B
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Energies
·
2022
·Vol. 15
·期 16
·5851
·
IF 3.252
Yong Yao,Shizhu Li,Chuangting Chen,Dongchen Zheng,Zhichao Wu,Chi Yu,Shuying Pu,Fa-Qian Liu
MIL-53(Fe) was prepared and modified with benzoic acid to prepare MIL-53(Fe)-BA additive, which was used to improve the catalytic oxidation rate of sulfite, prevent the scaling of the desulfurization tower, and improve the desulfurization efficiency during the wet flue gas desulfurization (WFGD) process of power plants. MIL-53(Fe)-BA exhibits abundant Lewis acid sites because of the appearance of coordination unsaturated Fe atoms. Due to the excellent sorption capacity, Ca(OH)2was used as the main SO2desulfurizer. The composite desulfurizers were prepared by mixing MIL-53(Fe)-based additives and Ca(OH)2, and were characterized by SEM, XRD, and FT-IR. A desulfurization unit was set up at laboratory scale to study the effect of catalytic oxidation additives on sulfite oxidation and desulfurization efficiency. The results showed that the addition of MIL-53(Fe)-BA can increase the oxidation capacity of sulfite by 159%, and greatly improve the desulfurization efficiency. These composite desulfurizers broaden the adaptability of the desulfurizing system to high-sulfur coals, and provide support for improving the desulfurizing efficiency of power plants.Keywords:catalytic oxidation;oxidative desulfurization;wet flue gas desulfurization;calcium hydroxide;MIL-53(Fe);Lewis acid sites
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
IF 8.128
Linbo Luo,Sheying Dong,Hao Cui,Longhui Sun,Tinglin Huang
The ecosystems and human health were seriously threatened by hexavalent chromium (Cr(VI)) in wastewater. In this article, using the idea of the highly matched energy band structure between indium sulfide (In 2 S 3 ) and MIL-53(Fe), a Type-II heterojunction has been constructed by loading In 2 S 3 on MIL-53(Fe) microrod to overcome the fault like high recombination rates of photogenerated electron-holes of In 2 S 3 . The composite with 20:1 mass ratio of In 2 S 3 to MIL-53(Fe) (IM-2) was adopted as an optimal sample for efficient photocatalytic Cr(VI) reduction under visible light . Various characterization techniques were used to verify the characteristics of composites and delved into the structure-effect relationship between this heterojunction and its activity. Results showed that the reaction rate constants of the photoreduction process over IM-2 was ~ 4 and 26 times higher than those of pure In 2 S 3 and MIL-53(Fe), respectively, and the catalyst could maintain superior removal efficiency (88.6%) and steady crystal structure after four cycles. First-principles calculations further illustrated that the heterostructure formed between In 2 S 3 and MIL-53(Fe) could effectively accelerate the separation of photogenerated electrons and holes, thus improving the photocatalytic reduction performance. Moreover, the active species analyses revealed that the superoxide radicals and electrons were mainly involved in the reduction of Cr(VI).
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ANALYTICAL BIOCHEMISTRY
·
2019
·
IF 2.507
Ying Jiang,Qi-Meng Yang,Qiu-Ju Xu,Shi-Yu Lu,Lin-Yu Hu,Mao-Wen Xu,Ying-Shuai Liu
Biothiols play critical roles in many biological processes and their aberrant is related to a variety of syndromes. A simple and reliable colorimetric method is developed in this work for biothiols detection based on an oxidase mimic, a metal organic framework (MOF) MIL-53(Fe), and a peroxidase substrate 3,3′,5,5′-tetramethylbenzidine (TMB). In this design, MIL-53(Fe) is utilized to catalyze the conversion of TMB to a blue colored 3,3′,5,5′-tetramethylbenzidine diimine, which can be read on a spectrophotometer at 652 nm. The oxidation-induced blue color generation can be efficiently inhibited by biothiols, thus a colorimetric analytical method is proposed for biothiols detection based on the above system. Under optimal conditions, a linear relationship in a range from 1 to 100 μM and a limit of detection (LOD) at 120 nM are achieved with Cys as a model target. The developed platform is further applied to evaluate cellular biothiols in normal (RWPE-1) and cancer (LNCap) cell lines, revealing that the overall biothiols level in LNCap is much higher than that in RWPE-1. This work renders a powerful tool for identifying cancer cells in a simple manner for biomedical diagnosis associated with biothiols.
研究领域:
材料科学
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分析化学
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纳米技术
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生物医学诊断
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生物无机化学
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2023
·
IF 5.2
Shiyu Zhang,Mengru Li,Jingwen Wang,Ruonan Zhang,Xiaoyu Ma,Haisheng Tao
Metal-organic frameworks with high porosity have received much attention in environmental pollutant treatment. This study presented a simple single-pot solvent thermal method for the preparation of a bimetal-organic framework MIL-53(Fe,Ni), further used for activated peroxydisulfate to degrade rhodamine B (RhB). The morphology and structure of the sample were characterized by scanning electron microscopy, transmission electron microscopy , x-ray diffraction, photoelectron spectroscopy , fourier transform infrared spectroscopy , and thermogravimetric analysis . The results showed that MIL-53(Fe,Ni) was successfully synthesized by the simple reaction, with high thermal stability and high specific surface area. The effects of pH value, co-existing ions, temperature, humic acid and different real water samples on RhB degradation were systematically investigated. Under optimized conditions, 93.9% of RhB was degraded within 180 min, together with excellent reusability. Quenching experiments and electron paramagnetic resonance showed that both free radicals (∙OH, SO 4 ∙- and O 2 ∙- ) and non-free radicals ( 1 O 2 and direct charge transfer) were responsible for the RhB degradation. In addition, the identification of intermediates by high-resolution mass spectrometer and reaction site prediction calculations (electrostatic potential, Fukui function and molecular orbit analysis), proposing a possible degradation pathway of RhB. The work highlights the broad applications of bimetal-organic frameworks in advanced oxidation processes .
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FOOD CHEMISTRY
·
2023
·
IF 8.8
Yu-Han Sun,Liu Yang,Xian-Xian Ji,Yuan-Zhen Wang,Yu-Long Liu,Ying Fu,Fei Ye
Flusilazole is a triazole fungicide with residues that are potentially toxic to humans. It enters the human body mainly through food, although its bactericidal activity is substantial. In this study, an electrochemical sensor Fe/Fe 2 O 3 @C with a core–shell structure was constructed to efficiently detect flusilazole by annealing MIL-53(Fe) which was prepared by a simple solvothermal method. Transmission electron microscopy and scanning electron microscopy were used to characterize the apparent morphology of MIL-53(Fe) and Fe/Fe 2 O 3 @C , and their structures were further characterized by X-ray photoelectron spectroscopy, Raman spectroscopy, powder X-ray diffraction, and the mapping of elements by energy dispersive spectroscopy. The electrochemical behavior of Fe/Fe 2 O 3 @C in the detection of flusilazole was evaluated by differential pulse voltammetry under optimal conditions. The results of the study indicate that the Fe/Fe 2 O 3 @C electrochemical sensor displayed excellent detection capabilities for flusilazole, where the sensor exhibited a wide detection range from 1.00 × 10 −4 to 1.00 × 10 −12 mol/L with an incredibly low LOD of 593 fM, making it highly sensitive to trace amounts of flusilazole. Moreover, Fe/Fe 2 O 3 @C demonstrated superior reproducibility, stability, and resistance to interference, highlighting its reliability in practical applications. The sensor was also successfully utilized to quantitatively detect flusilazole in various real samples, which suggests that Fe/Fe 2 O 3 @C has broad-spectrum environmental resistance and can effectively and rapidly detect flusilazole residues in different types of food items and environmental matrices. The study also delved into the mechanism of Fe/Fe 2 O 3 @C for the detection of flusilazole, providing a deeper understanding of the functionality of this sensor. Overall, these findings emphasize the practical significance of Fe/Fe 2 O 3 @C as an electrochemical sensor, showcasing its potential for real-world applications in food safety and environmental monitoring.
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CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Xiaohan Guo,Yanfang Liu,Hongxiang Zhu,Xiaohui Yu,Feng Shi,Qinqin Liu,Qiang Liu,Ying Xu
Asp donates electrons to reprogram Fe O clusters of MIL-53(Fe). • This electronic switch redirects dominant ROS from •OH to •O 2 − . • The mechanism enables neutral-pH POD-like activity of MIL-53(Fe)@Asp. • The Asp-modified nanozyme integrates with GOX for cascade glucose sensing. MIL-53(Fe) exhibits peroxidase-like activity only under acidic conditions, limiting its biosensing applications. We overcome this by using aspartic acid (Asp) as a structure-directing agent to modify MIL-53(Fe) (MIL-53(Fe)@Asp) via hydrothermal synthesis followed by Asp coordination. Unlike conventional pH-reduction strategies, Asp modification does not alter bulk pH but induces intrinsic electronic restructuring of Fe O clusters, as confirmed by increased Fe 3+ /Fe 2+ ratio and introduction of N → Fe coordination (XPS). At pH 6.9, the TMB-based activity of MIL-53(Fe)@Asp is 27-fold higher than that of pristine MIL-53(Fe). Steady-state kinetics show favorable Km values (TMB 0.27 mM, H 2 O 2 1.38 mM) at neutral pH. Mechanistic studies (ROS identification, EPR, band structure, DFT) reveal that Asp exerts an electron-donating effect that reprograms the electron distribution of Fe O clusters, activating the otherwise inactive MIL-53(Fe) framework at neutral pH and diversifying the catalytic pathways to include a less pH-dependent •O 2 − route alongside the partially maintained •OH pathway. This pathway diversification enables efficient neutral-pH peroxidase-like catalysis, with •O 2 − as the dominant pathway. Leveraging this, we construct a cascade nanoplatform (MIL-53(Fe)@Asp@GOX) integrating glucose oxidase, which exhibits excellent cascade activity at neutral pH. The method is applied to glucose detection in blood and saliva, demonstrating good linearity, precision, selectivity, and recovery. The glucose concentrations determined by our sensor correlated well with those obtained using a commercial assay kit. Notably, the limit of detection for glucose in saliva reaches 2.08 μM, offering a promising route toward non-invasive glucose sensing. This work establishes a design principle for creating pH-adaptive catalytic microenvironments in Fe-MOFs through electronic restructuring and pathway diversification, overcoming a long-standing limitation of MIL-53(Fe) for biomedical applications. Download: Download high-res image (111KB) Download: Download full-size image
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JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
·
2020
·Vol. 31
·期 6
·4822-4835
·
IF 2.22
Zhou Nan,Tan Junjie,Li Xi,Wang Lu,Jin Chenglong,Chen Ming,Yu Zhengsong,Liang Yani,Qiu Zhidong,Li Wenlong,Dong Yulin,Xie Zhizhong,Lin Yawei,Qu Deyu,Zhang Chaocan
A series of Bi 5 O 7 I/MIL-53(Fe) (BOI/MIL- w ) composites were successfully prepared by a facile in-situ solvothermal approach. The matched energy bands enabled Bi 5 O 7 I and MIL-53(Fe) to form a Z-scheme heterojunction which resulted in an efficient separation of the photo-induced electron–hole pairs. The photocatalytic activity of BOI/MIL- w was evaluated by the degradation of Rhodamine B (RhB) in water under the visible light irradiation. Compared with Bi 5 O 7 I, photocatalytic performances of BOI/MIL- w notably boosted. When the content of added MIL-53(Fe) was 3 wt%, BOI/MIL-3 presented the highest activity with a degradation efficiency of 99.7% only after 60 min of irradiation. The reaction rate constant k could reach 0.0992 min −1 which was nearly 12.6 times as high as that of Bi 5 O 7 I. Moreover, BOI/MIL- w had a good stability and reusability, which could ensure its practical application. Trapping experiments confirmed that h + and ·O 2 − were the dominant active species during the photocatalytic process, and further demonstrated the formation of the Z-scheme heterojunction facilitated the photocatalytic performance of BOI/MIL- w .
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CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Qiong Wu,Yining Liu,Haochuan Jing,Hongbin Yu,Ying Lu,Mingxin Huo,Hongliang Huo
Special enhanced synergistic effect of ultra-small γ-Fe 2 O 3 and graphene oxide (GO) on MIL-53 (Fe) was achieved for boosting photocatalysis. Compared to traditional methods of surface coverage, the incorporation of γ-Fe 2 O 3 (average size 2–3 nm) inside MOFs particles not only increased the light absorption of catalyst, but also formed numerous micro-heterojunctions with MOFs units and thus effectively facilitated the separation of photogenerated carriers. By supplying attachment sites for MOFs crystal, the functionalized GO reduced the size of MOFs particles to 100–200 nm, meanwhile improved their dispersibility. The active sites and quantum yield of photocatalytic reaction were also intensified benefiting from the large surface area and high electronic conductivity of GO. Therefore, the novel γ-Fe 2 O 3 -MIL-53(Fe)-GO composite exhibited the highest photocatalytic activity towards norfloxacin, with a removal rate of 92.8% in 90 min. The kinetic constant was 4.49-fold higher than that using pure MIL-53 (Fe), and 1.43-time greater than that in the system of MIL-53 (Fe) and hydrogen peroxide, which usually acted as efficient electron acceptors to increase the quantum yield and final photocatalytic performance of MOFs. Based on the identified intermediates, three NOR degradation pathways including the cleavage of piperazine ring, defluorination and decarboxylation, as well as the conversion of quinolones group were proposed. Photocatalytic mechanism investigation revealed the holes and hydroxyl radicals came from the reaction of electrons with oxygen played the important role in γ-Fe 2 O 3 -MIL-53(Fe)-GO photocatalysis. Moreover, the utilization of magnetic nanoparticles improved the recovery and recyclability of ternary catalyst.
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RSC Advances
·
2015
·Vol. 5
·期 50
·40094-40102
·
IF 3.84
Zhiming Yan,Wenmin Zhang,Jia Gao,Yifen Lin,Jianrong Li,Zian Lin,Lan Zhang
The application of the metal–organic framework (MOF) MIL-53(Fe) as a novel stationary phase for reverse-phase high performance liquid chromatography (HPLC) separation of positional isomers is described for the first time. Under the optimized conditions, baseline separation of xylene, dichlorobenzene, chlorotoluene and nitroaniline isomers was achieved on the MIL-53(Fe) packed column within a short time. The retention mechanisms of these isomers on the MIL-53(Fe) packed column were discussed in detail, and a typical reverse-phase behavior can describe the results. The thermodynamic characteristics of the HPLC separation of positional isomers were also evaluated. It was confirmed that the HPLC separation of positional isomers was controlled by the Gibbs free energy change (ΔG). In addition, reverse-phase HPLC separation of the tested isomers was also carried on MIL-53(Al, Cr) packed columns to investigate the influence of the metal centre of the MIL-53 framework on their chromatographic behaviors. The results showed that the MIL-53(Fe) packed column exhibited better separation performance than the MIL-53(Al, Cr) packed columns. Moreover, the MIL-53(Fe) packed column also gave efficient HPLC separation of alkylbenzene and naphthalene, aniline compounds and polycyclic aromatic hydrocarbons (PAHs). These successful applications suggest the potential of MIL-53(Fe) as a novel stationary phase for efficient reverse-phase HPLC separation.
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ACS Applied Nano Materials
·
2024
·
IF 5.3
Baixin Liu,Xuelian Chen,Guojuan Hai,Wenwen Zhao,Kai Li,Zhicong Yuan,Xiaoyong Zhang
The design and synthesis of metal–organic frameworks (MOFs) for direct use as electrode materials are crucial for enhancing the electrocatalytic oxygen evolution reaction (OER). Herein, the ultrathin MIL-53(Fe) nanosheet arrays with enriched coordinatively unsaturated metal sites (denoted as MIL-53(Fe)/NF-B0.2-2) are obtained under the inhibition and modulation of benzoic acid (BA) ligands via a substitution-suppression process. The results confirm that this unique ultrathin structure effectively increases the electrochemical active surface areas (ECSA) and exposes the coordinatively unsaturated metal sites. More importantly, the enriched coordinatively unsaturated metal sites acting as active sites facilitate the adsorption of OH– during the OER process. Additionally, MIL-53(Fe)/NF-B0.2-2, with its optimized energy band structure, exhibits superior charge transfer ability and diffusion processes, significantly improving the reaction kinetics in alkaline electrolytes. As a result, the MIL-53(Fe)/NF-B0.2-2 electrode only requires extremely low overpotentials of 190 and 229 mV to reach current densities of 10 and 100 mA cm–2 for OER, respectively. This research not only proposes a novel strategy for designing efficient electrocatalysts but also provides insights into the structure–activity relationship, advancing the rational design of MOFs as effective electrode materials.
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