APPLIED CATALYSIS A-GENERAL
·
2021
·
IF 5.706
Wentao Zhang,Kunrui Wei,Wenguang Huang,Jianghua Yang,Yonghai Gan,Shujuan Zhang
Post-synthetic modification with β -diketone has been proven as an effective strategy to improve the visible light response activities of metal-organic frameworks (MOFs). Nevertheless, the effects of the anchored-diketones on the excitonic behaviors and photocatalytic mechanisms of MOFs are still unclear. Herein, two MOFs (MIL-101 with Cr III and MIL-101 with Al III ) were employed as prototypical materials to further understand this post-synthetic modification strategy. Diketone anchoring could enhance the photocatalytic generation of singlet oxygen ( 1 O 2 ) by the two MOFs in a joint mechanism: exciton-mediated energy transfer and photosensitization. Diketone anchoring induced triplet exciton was found playing an important role in the photocatalytic generation of 1 O 2 . The photosensitization of the anchored-diketone also played a key role in the photocatalytic generation of 1 O 2 . The results here provide a useful guidance for the development of MOFs-based photocatalysts and are helpful to realize the regulation of excitonic behaviors and photocatalytic mechanisms of MOFs.
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高影响因子
Environmental Technology & Innovation
·
2022
·
IF 7.758
Zhen Jiao,Zhijia Miao,Heluan An,Qing Li,Xiangyuan Meng
Water eutrophication caused by phosphate emissions has become a serious environmental issue. In this study, we used the solvothermal method to prepare a novel Ce-doped MIL-100(Fe). Scanning electron microscope observations suggest that Ce-doped MIL-100(Fe) consisted of irregular polyhedrons in the size range of tens of micrometers. Spectroscopy results show that cerium atoms (Ce) were successfully doped into the MIL-100(Fe) frameworks. The specific surface area and pore size of the Ce-doped MIL-100(Fe) were 2.6 m 2 /g and 3.4 nm, respectively. Adsorptive kinetics indicated that the pseudo-second-order model with a high correlation coefficient of ( R 2 : 0.9950) fitted better than the pseudo first-order model with R 2 of 0.9436. The adsorptive isotherms showed that for these adsorption reactions, the Langmuir model matched much better than the Freundlich model for this adsorption. These facts suggest that adsorption is chemical sorption, which occurred on a homogeneous surface. The adsorption capacity of the Ce-doped MIL-100(Fe) was as high as 12.03 mg/g. The adsorption capacity of the Ce-doped MIL-100(Fe) depended strongly on the solution pH, ionic strength, and the coexisted ions. The study also found that the precipitation reaction and complexation interaction might be dominated in the adsorption. This study may contribute to the design of bimetal organic frameworks, and might add new insights into the removal of phosphate.
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CHEMOSPHERE
·
2021
·
IF 7.086
Jiajie Xu,Shengye Wang,Changyu Yan,Hafiz Mohammad Adeel Sharif,Bo Yang
Advanced oxidation processes based on sulfate radicals are considered as a promising approach for environmental remediation. In this study, TiO 2 @MIL-101(Fe) is successfully fabricated by a facile impregnation method and is used for sodium persulfate (SPS) activation. TiO 2 @MIL-101@SPS combines the advantages of photocatalysis and SPS activation, which shows high removal efficiency for nitrobenzene and methyl orange. In addition, the effect of multiple factors, including light source, SPS amount and catalyst amount, on nitrobenzene degradation have been investigated. Results show that the nitrobenzene degradation efficiency is up to 66.53 % while that of TOC removal is 32.21 % under 4-h visible light irradiation with 30 mg catalyst and 1.6 mM SPS. Moreover, LC-MS have been carried out to study the route of nitrobenzene degradation. Besides, ESR analysis reveals that both ● SO 4 − and ● OH radicals are generated sustainably under visible light irradiation, and more ● OH radicals can be detected owing to the synergic effect of photocatalysis and SPS activation. Interfacial charge transfer effect provides photoinduced electrons for the Fe 3+ /Fe 2+ cycle in MIL-101(Fe), which boosts the SPS activation process, resulting in high photocatalytic activity.
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Journal of Environmental Chemical Engineering
·
2025
·Vol. 14
·期 1
·120546
·
IF 7.2
JinCheng Dai,Shuyue He,Xiyu Song,Hongjuan Zhang,Ruyi Xie
The construction of heterojunction photo-Fenton catalysts to activate hydrogen peroxide for the efficient degradation of organic pollutants in water has attracted considerable attention. Herein, a CuBi 2 O 4 @MIL-53(Fe) Z-scheme heterojunction catalyst was successfully prepared by solvothermal method for tetracycline (TC) degradation. In this catalytic system, the heterogeneous photocatalytic reaction and the Fenton reaction form a strong synergistic effect in the degradation of organic pollutants through the transfer of photogenerated electrons. The results indicate that in the presence of trace concentrations of H 2 O 2 (2.60 mM), 0.20 g/L of MC-15 (with CuBi 2 O 4 accounting for 15 % of the mass of MIL-53(Fe)) exhibited the highest catalytic activity, with a TC (150 mg/L) removal rate of 94.0 % after 50 min of visible light irradiation. Interestingly, the MC-15 catalyst can still achieve a removal rate of 62.1 % of TC even under dark conditions. Furthermore, in degradation experiments, MC-15 exhibited high environmental stability and applicability in different natural water system. The excellent catalytic performance of the light/MC-15/H 2 O 2 system is attributed to the quick separation of photogenerated electron-hole pairs from Z-scheme heterojunction CuBi 2 O 4 @MIL-53(Fe) and the accelerated bimetallic ions cycle. A possible photo-Fenton catalytic mechanism of MC-15 catalyst is proposed based photoelectrochemical tests, free radical capture experiment and electron paramagnetic resonance (EPR) analysis. This study provides a reference for the development of iron-based metal-organic framework composite photo-Fenton catalysts.
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JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
·
2018
·Vol. 29
·期 14
·12045-12054
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IF 2.324
Huang Zhaohui,Chen Hui,Zhao Lei,He Xuan,Fang Wei,Du Yingying,Li Weixin,Wang Guanghui,Zhang Fuqing
With increasing concern about the problems of environmental pollution and energy, the visible light photocatalytic for dye degradation is receiving considerable attention. CdSe quantum dot (CdSe QDs) sensitized MIL-125/TiO 2 @SiO 2 biogenic hierarchical materials (CMTS) has been fabricated through dual modification of CdSe with TiO 2 and MIL-125, that is the metal–organic framework (MOF) with Ti ions as metal centers and terephthalic acid as the organic ligand. The hierarchical porous heterostructured MIL-125/TiO 2 @SiO 2 composites are firstly obtained by a biogenic-templated method using rice husk as biomorphic. CdSe QDs as sensitizer is further deposited on MIL-125/TiO 2 @SiO 2 via a dipping method. This strategy applies CdSe, MIL-125, and TiO 2 undergo a two-level heterostructure, setting a stage for efficient charge separation. In addition, CMTS possesses a hierarchical porous structure in scale from micrometer to nanometer with high BET surface area. As a result, the CMTS can efficiently adsorption target, improving light harvesting and promoting degradation of organic waste from water. Meanwhile, Rhodamine B aqueous solution can be degraded more than 98% by CMTS in 100 min under visible light irradiation.
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Applied Catalysis O: Open
·
2025
·
IF 0
Yiyin Zhu,Qibing Dong,Atif Sial,Abdelkader Labidi,Ke Zhao,Ximing Li,Junjun Wang,Chuanyi Wang
Achieving efficient ligand-metal charge transfer remains a significant challenge for constructing high-performance N 2 -fixing MOF photocatalysts. Herein, we successfully fabricated mixed-metal MIL-101(Fe/Cr) materials to achieve ligand-metal charge transfer, leading to significantly improved N 2 fixation performance. Performance test under visible light demonstrated that MIL-101(Fe/Cr) achieved nitrogen fixation activity of 125.19 μmol h −1 g −1 , which is 1.7 times greater than that of pure MIL-101(Fe). The experimental confirm that the incorporation of Cr metal enables the more favorable accumulation of photogenerated electrons at the Fe catalytic centers, attributed to increased electronic interactions and enhanced charge transfer efficiency, thus facilitating the activation process of N 2 , and consequently enhancing ammonia (NH 3 ) production. This work provides new insights into strategies for improving the ligand-metal charge transfer efficiency of MOF-based photocatalytic nitrogen fixation materials.
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RSC Advances
·
2020
·Vol. 10
·期 4
·2198-2208
·
IF 3.119
Hui Su,Jiaxin Lv,Liansheng Yang,Li Feng,Yongze Liu,Ziwen Du,Liqiu Zhang
The pollution of aromatic organophosphorus flame retardants (aromatic OPFRs) in aquatic environments has drawn great attention over the last few years. Two MIL-101-based metal–organic frameworks (Cr-MIL-101 and Fe-MIL-101-NH2) which possess ordered mesoporous cavities (2.9 and 3.4 nm) and aromatic structures were chosen and prepared to selectively adsorb a typical aromatic OPFR [triphenyl phosphate (TPhP)] from aqueous solution. Pore distribution analysis showed that Cr-MIL-101 and Fe-MIL-101-NH2 had both a mesoporous structure (2–3.5 nm) and microporous structure (1–2 nm), conducive to diffusion and adsorption of TPhP molecules. Compared with Fe-MIL-101-NH2 as well as commercial activated carbon, Cr-MIL-101 showed rapid and efficient adsorption for TPhP, and its initial sorption velocity (v0) calculated from the pseudo-second-order model was up to 568.18 μmol g−1 h−1. The adsorption equilibrium of TPhP on the Cr-MIL-101 was almost achieved within 12 h, while the equilibrium time of other adsorbents required more than 48 h. The study of selective adsorption found that Cr-MIL-101 had a higher sorption amount for aromatic OPFRs than alkyl-OPFRs and other aromatic compounds with different chemical structures. Cr-MIL-101 was able to keep a steady selective adsorption for TPhP in the presence of co-existing aromatic compounds. Based on the analysis of Kow, molecular structure and further density functional theory calculations, hydrophobic interactions may play a dominant role in the selective adsorption process of TPhP, and π–π interactions may be also involved. Cr-MIL-101 exhibits reusability and promising potential to rapidly and selectively remove aromatic OPFR in environmental remediation.
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JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2022
·Vol. 169
·期 10
·106518
·
IF 4.386
Qingxiao Zhang,Pei Han,Hui Zhang,Jixin Yao,Xinyu Wang,Dongmeng Chen,Xueqin Zuo,Qun Yang,Shaowei Jin,Guang Li
The oxygen evolution reaction (OER) is a critical process in the operation of electrochemical water splitting. Metal-organic frameworks (MOFs) are applied in the field of OER electrocatalysis because of their unique structure, but the high impedance and unstable framework during pyrolysis remain unresolved. Here, MIL-88A (iron-based MOF) was modified by hydrolysis and loading Co(OH)2 to improve the catalytic activity. The electrochemical results showed that the Co(OH)2/MIL-88A achieved the optimized performance with the current density of 10 mA cm−2 at 278 mV (vs RHE). Density functional calculations (DFT) combined with characterization tests suggest that electrons transfer from Co(OH)2 to MIL-88A at the interface of the heterostructure, leading to a larger hole electron pair density. D-band theory calculations demonstrated that the synergistic effect of MIL-88A and Co(OH)2 in heterostructure strengthens the adsorption between active sites and adsorbate. The above proofs are the source of the excellent OER performance of the Co(OH)2/MIL-88A. The finding has certain reference significance for the heterogeneous treatment of iron-based MOF catalysts.
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高影响因子
MICROCHEMICAL JOURNAL
·
2024
·
IF 4.9
Jiejun Li,Lin Li,junjie Fei,Pengcheng Zhao,Jinyao zhao,Yixi Xie
Fenitrothion (FT) is a common organophosphorus pesticide widely used in agricultural. Residues of fenitrothion in crops can adversely affect human health. In this work, modified MIL-125-Fe was prepared by changing the solvent ratios and further etching with iron nitrate, followed by high-temperature pyrolysis to obtain modified-TiO 2 /FeTiO 3 -doped nitrogen-containing carbon framework (m-TiO 2 /FeTiO 3 @NCF). The porous carbon material of m-TiO 2 /FeTiO 3 @NCF was used to modify the GCE to produce FT electrochemical sensor. Under optimized conditions, the sensor exhibited good detection performance for FT with a low LOD of 0.96 nM and a wide detection linear range of 1–9000 nM, and also exhibited good reproducibility (RSD = 2.08 %), repeatability (RSD = 1.09 %) and anti-interference performance. The sensor was successfully applied in real sample tests showing the recovery rates of 98.7 %–101.2 %. The present study provides a new idea for the rapid and accurate detection of FT.
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Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Yuhang Ren,Yu Tian,Yating Lu,Dongyu Nie,Huayi Zhu,Xia Yang
Malathion (MA) is a widely used organophosphorus pesticide globally. Developing efficient photocatalysts is crucial for eliminating MA pollution in water by photocatalytic technology. This study focuses on preparing a series of H-PDI supermolecule/NH 2 -MIL-101(Fe) (PM) materials by amidating NH 2 -MIL-101(Fe) with the more stable H-PDI supermolecule, forming a covalent O C–NH bond. Among these materials, 40 %PM (indicating a mass percentage content of 40 % H-PDI supermolecule in PM) exhibited the best performance for degradation of MA. Under simulated sunlight irradiation of a 10 mg·L 1 MA solution for 180 min, the reaction rate constants of 40 %PM were 5.95 times and 3.13 times higher than those of NH 2 -MIL-101(Fe) and H-PDI supermolecule, respectively. The enhanced performance is attributed to the formation of Z-scheme heterojunctions in the 40 %PM composite lead to fast separation of photogenerated e − and h + . Combining the results of HPLC-MS with Fukui Function, the HOMO, LUMO, and pathway of degradation of MA attracted by 1 O 2 , •OH, and h + were speculated. The pathway involves oxidation, demethylation, P-S bond breakage, decarboxylation, and final conversion to some inorganic molecules. The toxicity of the degradation byproducts were lower than that of MA estimated by Toxicity Estimation Software Tool.
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JOURNAL OF RARE EARTHS
·
2024
·
IF 5.2
Xiayu Liang,Aylin M. Deliormanlı,Qingle Zeng
A novel composite material, Poly(IL-AA)@MIL-101(Cr), combining metal-organic framework, polymeric ionic liquid and acrylic acid, was synthesized for the selective and efficient adsorption of rare earths europium(III) (Eu 3+ ). Characterization of the materials was carried out using techniques such as X-ray diffraction (XRD), Fourier transform infrared (FTIR), scanning electron microscopy-energy dispersive X-ray spectroscopy (SEM-EDS), thermogravimetric analysis (TGA) and Brunauer-Emmett-Teller (BET). The results demonstrate successful incorporation of the polymeric ionic liquid onto the material surface while preserving the crystal structure and morphology of MIL-101(Cr). Adsorption experiments were conducted to explore parameters including solution pH, initial Eu 3+ concentration, and duration, with comprehensive analyses of adsorption kinetics, isotherms, and mechanisms. Findings reveal that Poly(IL1-AA)@MIL-101(Cr), Poly(IL3-AA)@MIL-101(Cr), and Poly(IL5-AA)@MIL-101(Cr) achieve adsorption equilibrium for Eu 3+ at approximately 9 h with an equilibrium pH of 6.2. The adsorption of Eu 3+ predominantly follows a pseudo-second-order kinetic model and Langmuir isotherm adsorption model. Moreover, the prepared composite material exhibits superior adsorption selectivity for Eu 3+ over other metal ions in the mixture (K + , Mg 2+ , Ni 2+ , Co 2+ , Zn 2+ , La 3+ , and Nd 3+ ). Even after five adsorption-desorption cycles, the composite material maintains satisfactory adsorption performance.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Ziyi Zhang,Huiqing Dong,Dongxu Zhou,Kexin Tang,Yidi Ma,Tao Han,Jianqiu Lei,Shoushuang Huang,Xiaodong Zhang,Liang Tang,Ning Liu
Photocatalytic CO 2 reduction is a promising strategy to address both environmental issues and energy crisis. Defect engineering offers great potential for improving the photocatalytic performance. Herein, we report an innovative approach to introduce defects in MIL-68(In) via electron beam irradiation for the photoreduction of CO 2 into CH 4 . The irradiated X-MIL-68(In) (X mean the irradiation dose) retained the crystal structure and morphology of pristine MIL-68(In), while generating novel organic framework defects. These defects significantly improved the CO 2 photoreduction activity, with 300-MIL-68(In) achieving the highest CH 4 rate of 87.5 μmol g −1 h −1 and a CH 4 selectivity of 74.8 %. Comprehensive ex situ and in situ characterizations, combined with DFT calculations, demonstrated that defects formation in 300-MIL-68(In) accelerated the separation and transfer of photoexcited carriers, thereby driving its superior photocatalytic performance. Furthermore, In situ DRIFTS along with DFT calculations confirmed that ⁎ COOH, ⁎ CHO and ⁎ CH 2 O were key intermediates during CO 2 reduction process. This work highlights electron beam irradiation as an effective strategy for defect engineering, offering new opportunities for tuning the performance of photocatalysts.
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