NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 14
·6804-6821
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IF 3.3
Yuwen Huang,Zongxue Yu,Pingquan Wang,Shuangli Li,Qiuyue Tan,Niandan He,Qingcan Xiang
The production of abundant free radicals and the effective separation of photo-induced carriers are considered challenging by researchers for the application of photocatalytic technology in the field of wastewater purification and environmental remediation. Herein, we successfully synthesized a novel S-MIL-101(Fe)@CQD composite via multi-step synthetic routes involving a simple solvothermal synthesis method and annealing treatment process to remove both Cr6+ and dyes in wastewater. A series of characterization methods and photocatalytic property tests were performed, proving that the synthesized S-MIL-101(Fe)@CQDs exhibited higher photocatalytic activity than MIL-101(Fe), which is mainly due to the formation of an intramolecular energy level and modulation of the intrinsic electronic properties of the MOF, where the CQDs act as an electron acceptor. We proposed the underlying photocatalytic mechanism through trapping experiments of the active species. Also, we performed several typical pollutant degradation experiments and confirmed the wide applicability of this composite. In summary, this work provides new insight into the construction of modified MOFs for the efficient removal of toxic pollutants from water.
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RSC Advances
·
2024
·Vol. 14
·期 24
·16727-16735
·
IF 3.9
Huizhong Wu,Qiong Yi,Xiang Li,Yingxi Wang,Ling Li
Low catalytic efficiency and catalyst recovery are the key factors limiting the practical application of advanced oxidation processes. In this work, a core–shell magnetic nanostructure Fe3O4@MIL-101(Fe, Co) was prepared via a simple solvothermal method. The core–shell structure and magnetic recovery performance were characterized by various technologies. The results of dye degradation experiments proved that within 10 minutes, the Fe3O4@MIL-101(Fe, Co)/PMS system can degrade more than 95% of 10 mg per L Rhodamine (RhB) at an initial pH of 7, which possesses higher catalytic activity than the Fe3O4/PMS system and the MIL-101(Fe, Co)/PMS system. The effects of initial solution pH and coexisting anions in water on the degradation of RhB were further discussed. The results showed that Fe3O4@MIL-101(Fe, Co) displayed excellent degradation efficiency in a wide pH range of 3–11 and capability of resisting coexisting anions. It is worth mentioning that after five cycles, the RhB removal rate can still be maintained at over 90% after 10 minutes of reaction. Free radical quenching experiments were further studied, confirming that ˙OH and SO4−˙ were involved in the degradation of RhB, while the dominating active free radical was SO4−˙. The possible reaction mechanism of the RhB degradation process was also inferred.
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APPLIED CATALYSIS A-GENERAL
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2013
·
IF 3.41
Zhiguo Sun,Gang Li,Hai-ou Liu,Liping Liu
A series of MOF-based catalysts, metal-salen complexes incorporated into amino-functionalized MIL-101 matrices by salicylaldehyde condensing to amino group and coordinating metal ion through one pot method, have been prepared and characterized. The successful preparation of catalysts demonstrates that postsynthetic modification (PSM) is a practical and powerful route to generate MOF-based catalyst with multiple active sites. The catalytic performances of prepared catalysts were investigated via selective oxidation of cyclohexane to cyclohexanone and cyclohexanol (KA-oil) by molecular oxygen in the absence of solvent. It was found that NH 2 -MIL-101(Cr)-Sal-Co, as a typical case, behaves as cooperative catalyst for cyclohexane selective oxidation. That is, salen-Co(II) attached to framework of MOF is able to assist in the generation of new radicals from peroxides via a Haber–Weiss catalytic cycle to promote conversion of cyclohexane while framework Cr ion is able to catalyze the dehydration of intermediate product cyclohexyl hydroperoxide (CHHP) to improve KA-oil selectivity. Furthermore, this catalyst exhibits good recyclability and behaves as truely heterogeneous catalyst.
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JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL
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2015
·
IF 3.615
Huiyan Pan,Xiaohong Li,Yin Yu,Junrui Li,Jun Hu,Yejun Guan,Peng Wu
Metal organic-framework MIL-101 and inorganic mesoporous composites Al 2 O 3 @SBA-15 supported Pt catalysts, Pt/MIL-101 and Pt/Al 2 O 3 @SBA-15 catalysts, were prepared and characterized by means of X-ray diffraction (XRD), N 2 adsorption–desorption, scanning electron microscopy (SEM), transmission electron microscopy (TEM), CO chemisorption and thermo-gravimetric (TG) analysis. Pt nanoparticles were highly dispersed on both supports. In liquid-phase hydrogenation of nitrobenzene, benzaldehyde and their derivatives, the Pt/MIL-101 catalyst was superior to the Pt/Al 2 O 3 @SBA-15 catalyst in water. For liquid-phase hydrogenation of nitrobenzene with the Pt/MIL-101 catalyst, owing to high solubility of nitrobenzene in ethanol, the reaction in ethanol went much faster than that in water, furnishing a turnover frequency (TOF) in ethanol up to 18,053 h −1 , almost triple of that obtained in water under similar conditions. The highest TOF of 25,438 h −1 was obtained in ethanol for hydrogenation of 3-chloro-nitrobenzene with the Pt/MIL-101 catalyst. As for hydrogenation of benzaldehyde series, 2-fluoro-benzaldehyde and 3-fluoro-benzaldehyde gave the highest TOFs of 5146 h −1 and 3165 h −1 in water with the Pt/MIL-101 and Pt/Al 2 O 3 @SBA-15 catalysts, respectively. We deduce that surface property of MIL-101 with high hydrophobicity is helpful to enrich reactants around the Pt/MIL-101 catalyst in water, where nitrobenzene or benzaldehyde and its derivatives have a limited solubility, so that high catalytic performance was achieved with the Pt/MIL-101 catalyst in water. Of particular note is that the Pt/MIL-101 catalyst can be reused at least four times without loss in activity or selectivity.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Xinqi Luan,Xuehui Jia,Syed Jalil Shah,Jingyu Bao,Shunxiang Qin,Ruimeng Wang,Jiguang Deng,Zhongxing Zhao,Zhenxia Zhao
Low adsorption efficiency and secondary pollution release pose a bottleneck for the efficient capture of radioactive iodine vapor during nuclear utilization via adsorption. In addition, the simultaneous adsorption of iodine vapor alongside other harmful vapors in complex systems has been rarely reported. In this work, an electron/H-donating defective pore construction strategy involving MIL-101 modification via amino acids (AAs) was proposed to enhance its simultaneous adsorption efficiency for iodine and formaldehyde vapors. These defective microenvironments possessed microporous property with 11.3 Å, which not only formed strong affinity for I 2 molecules itself but also enhanced its adsorption interaction towards polyiodide anion (I 3 - and I 5 - ) through electron donation of AAs. Moreover, these adsorbed polyiodide anions and AAs-SL within the MOFs, resulting in multisite capture of FA via NH…O-H…I hydrogen bonding. The results revealed that AAs coordinated MIL-101 exhibited superior removal rate ( k 80% = 0.61–1.15 g g −1 h −1 ) for iodine vapor than that of the original MIL-101, which was 3.6–30.8 times higher that of state-of-the-art adsorbents under similar conditions. Notably, a high-capacity superior retention rate of 94.8 % was achieved for its I 2 adsorption after exposure to air for 7 days. After adsorption of iodine, AAs coordinated MIL-101 retained high FA adsorption capacity up to 9.7–12.9 mg/g, representing 75.1 %–87.7 % of the original AAs@MIL adsorption capacity for FA. This defective engineering strategy in MOFs supplied an efficient method for removing multiple harmful gases from the surrounding nuclear waste atmosphere.
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INORGANIC CHEMISTRY COMMUNICATIONS
·
2025
·
IF 5.4
Rui Zhang,Lingqiao Hu,Zixi Li,Jingjing Hao
The special layered structure and narrow band gap of BiOI semiconductors lead to a high recombination rate of photogenerated electrons and holes. Therefore, it is compounded with the porous structure of the metal–organic backbone NH 2 -MIL-101(Fe) to form heterojunctions and provide more active sites. In this paper, NH 2 -MIL-101(Fe)/BiOI composites were successfully prepared by solvothermal method, which has a high specific surface area and adjustable pore size, which is conducive to the effective separation and transport of photogenerated electrons and holes, thereby improving the photocatalytic efficiency. The results of XRD, SEM, XPS and other characterization experiments show that NH 2 -MIL-101(Fe)/BiOI composites have been successfully prepared. Secondly, ultraviolet diffuse reflectance spectroscopy (UV–vis DRS) was used to test the light absorption performance of the composites, which confirmed that the materials had a larger visible light range. Through PL, EIS confirmed that the efficiency of photogenerated electron and hole separation was further improved. In addition, the M–S curves of NH 2 -MIL-101(Fe) and BiOI were tested to calculate the valence and conduction band values of the material. Combined with the results of free radical trapping experiments, O 2 − and h + play a major role in the degradation of tetracyclines and can be degraded into CO 2 and H 2 O. The Z-type electron transfer mechanism of the composites is deduced, which can improve the separation rate of electrons and holes. In addition, the cyclic test verified that the composite material has good stability. When the tetracycline concentration was 30 mg/L, the degradation rate of the 10 % NH 2 -MIL-101(Fe)/BiOI composite reached 93.3 %. Its materials also have certain potential application value in environmental treatment, energy conversion and other fields, especially for the treatment of pollutants in water bodies.
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ACS Applied Nano Materials
·
2025
·
IF 5.5
Ai-Hui Cao,Xin-Tai Su,Min Zhang,Qi-Long Zhu
Photocatalytic water decomposition is a cost-effective way to convert sustainable solar energy into chemical energy. While semiconductor photocatalysis has generated considerable interest in photocatalytic hydrogen evolution, it is hampered by fast electron–hole complexation and suboptimal efficiency. Herein, an NH2-MIL-101(Cr)/doped-C3N4 heterojunction possessing a static internal electric field (IEF) is successfully prepared, characterized, and assessed for photocatalytic hydrogen production. The optimized photocatalytic H2 evolution rate of the resultant NH2-MIL-101(Cr)/O–C3N4 is 460 μmol g–1 h–1 under visible light, with an AQY of 2.5% at 450 nm. Spectral evidence indicates that the static IEF facilitates rapid electron transfer from NH2-MIL-101(Cr) to O–C3N4, achieving efficient photogenerated charge separation and a consequent significant enhancement in catalytic activity. This work not only presents a case of construction of an IEF through assembling NH2-MIL-101(Cr) with O–C3N4 but also deepens the insight of the rudimentary mechanisms of the static IEF in heterojunctions for photocatalytic hydrogen evolution.
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Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Yuhui Xue,Changyan Guo,Jingjing Wang,Xueli Yang,Meng Wang,Jide Wang
The overuse of antibiotics poses a serious threat to the ecosystem. In particular, antibiotic residues in the aquatic environment are particularly serious. Therefore, preparation of efficient adsorbents for removing trace antibiotic residues from the environment becomes essential. In this work, a series of magnetic porous carbon material (Fe-MPC-gly) derived from MIL-101, which was regulated by glycine, were prepared by high temperature calcination for the adsorption of trace sulfonamide antibiotics (SAs) in water. The morphology of MIL-101 was found to gradually change from a regular ortho-octahedron to an acicular spindle with the increase as the glycine content increased. The results of adsorption experiments showed that Fe-MPC-gly-2 had the best adsorption effect on SAs. In particular, the adsorption of Fe-MPC-gly-2 on SAs could reach the adsorption equilibrium in 5 min, and the maximum adsorption amounts were 50.0 mg·g −1 and 38.2 mg·g −1 for sulfameter and sulfachloropyridazine, respectively. The adsorption kinetic model was best fitted to the quasi-first-order kinetic model. The possible adsorption mechanisms were pore filling, hydrogen bonding and π-π interactions. Meanwhile, the synthetic strategy of this study provides an idea for the preparation of efficient adsorbents for antibiotics.
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APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Jiming Huang,Runqing Liu,Hangdao Qin,Fan Wu,Lei Guo,Wei Shi,Ping Xue,Sizhan Wu,Guiying Zhang,Zhengbang Wang
Developing S-scheme photocatalysts with excellent catalytic activity and convenient retrieval is highly desirable for wastewater purification. Herein, a novel S-scheme MIL-101(Fe)/WO 3 heterojunction on carbon cloth is successfully synthesized via a facile solvothermal approach. The optimized MIL-101(Fe)/WO 3 composite (MWC-1.5) has been found to be highly effective in activating peroxymonosulfate (PMS) and then degrading tetracycline hydrochloride (TC-HCl) with a 100% degradation rate when exposed to visible light (Vis) within a period of 20 min. Such MWC-1.5/PMS/Light system also shows stable cycling performance and good recyclability. The remarkable photocatalytic degradation performance is mainly attributed to the powerful intrinsic electric field that accelerates the separation of photogenerated charge carriers via the S-scheme charge transfer. Radical quenching experiments and electron paramagnetic resonance (EPR) results suggest that SO 4 – and OH are the major oxidizing substances in the photocatalytic processes. Three potential degradation pathways are deduced based on an in-depth analysis of the degradation intermediates and the degradation mechanism is also elucidated through a rational combination of the experimental studies and theoretical calculations. This novel hybrid photocatalyst system has been shown to be a promising strategy for environmental remediation, while also suggesting a feasible approach for the development of photocatalysts with both remarkable activity and stability.
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MICROCHEMICAL JOURNAL
·
2024
·
IF 4.9
Yan Chen,Xiaojuan Yang,Zhonggang Liu,Guohua Liu,Zheng Guo
Resolving the issue of poor conductivity and easy aggregation of MOFs is recognized as one important factor for their successful applications in electrochemical sensors and electrocatalysis. In this work, we propose an assembly of NH 2 -MIL-101(Fe) onto a nanoporous gold (NPG) microelectrode surface. The nanoporous gold could greatly improve the conductivity and reduce the aggregation of NH 2 -MIL-101(Fe). The proposed NH 2 -MIL-101(Fe)/NPG microelectrode was developed for the electroanalysis of ascorbic acid (AA) and uric acid (UA). It exhibited excellent electrochemical performance for the individual and simultaneous sensing of AA and UA in a 0.1 M PBS solution (pH 7.4). High sensitivities (2.03 μA μM −1 cm −2 for AA; 29.30 μA μM −1 cm −2 for UA) were achieved in the simultaneous analysis process. The improved electrochemical performance was attributed to the electrocatalytic properties and large specific surface area of NH 2 -MIL-101(Fe)/NPG, as well as the electrostatic interaction between NH 2 -MIL-101(Fe) and analytes. Moreover, the NH 2 -MIL-101(Fe)/NPG microelectrode was successfully used for the simultaneous detection of AA and UA in complicated environment (human sweat and advanced DMEM). This work shows great promise for the simultaneous detection of AA and UA and extends the applications of MOFs in electrochemical devices.
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FOOD CHEMISTRY
·
2024
·
IF 8.5
Rui Cheng,Yiqun Wan,Xuejin Mao,Hao Wan,Fan Liu,Lan Guo,Bingzhen Zhang
This work presents an efficient sorbent for plant growth regulators (PGRs) by regulating the defects of a metal–organic framework MIL-101(Cr). Using the regulated MIL-101(Cr), we developed a simple and effective method for the simultaneous determination of eleven PGRs in fresh fruit juice. The extraction conditions were optimized by an orthogonal array design. Under optimal conditions, the method showed a satisfactory limit of detection (0.1–1.2 ng/g), recovery rates (83.4–110.2 %), and precision (2.9–18.0 % for intra-day and 2.7–10.8 % for inter-day), as well as a greatly suppressed matrix effect. Notably, regulating the defects significantly enhanced the desorption of PGRs on MIL-101(Cr). The sorbent didn’t need to be destroyed to release the adsorbed PGRs and could be reused at least 6 times. Furthermore, the defects of MIL-101(Cr) and interactions between the sorbent and PGRs were studied by TGA, ATR-IR, XPS, NH 3 -TPD and UV–Vis DRS.
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PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
·
2025
·
IF 7.8
Weitao Kong,Zhongmou Liu,Jinghui Wu,Chenying Wen,Juncheng Yan,Yidi Gao,Guanqiao Li,Xianze Wang,Mingxin Huo
This study investigates the degradation of sulfamethoxazole (SMX), a widely detected and persistent antibiotic in the environment, using a novel photocatalytic system based on MIL-101(Fe) supported Mo single-atom with oxygen vacancies (Mo/Ov-MOF). Anchoring Mo single-atoms into the MOF structure enhances catalytic activity by effectively improving charge separation and reducing electron-hole recombination. The Mo/Ov-MOF efficiently activates peroxymonosulfate (PMS) under visible light, generating singlet oxygen ( 1 O 2 ) as a primary reactive species responsible for SMX degradation. Degradation experiments demonstrated that the degradation efficiency reached 96.8 % in the presence of PMS and visible light. Through quenching and trapping experiments on active species, an in-depth investigation into the source of 1 O 2 was performed, demonstrating the crucial role of holes in the rapid and selective generation of 1 O 2 under visible light. Additionally, the reusability of the Mo/Ov-MOF catalyst was confirmed, maintaining over 70 % degradation efficiency after five cycles. Toxicity assessments indicated that the degradation by-products exhibited significantly lower toxicity than the parent compound SMX, thus mitigating potential ecological risks. The mechanistic insights reveal that oxygen vacancies and Mo single-atom enhance electron transport and facilitate efficient PMS activation, ultimately leading to effective pollutant degradation. The findings underscore the potential of the Mo/Ov-MOF photocatalytic system for practical applications in wastewater treatment, particularly for removing persistent organic pollutants from aquatic environments.
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