NEW JOURNAL OF CHEMISTRY
·
2022
·Vol. 46
·期 24
·11840-11850
·
IF 3.925
Dongying Zhu,Zhujun Huang,Haiyan Wang,Qiujun Lu,Guihua Ruan,Chenxi Zhao,Fuyou Du
The fabrication of sustainable and reusable photocatalyst materials is urgent and desirable for the removal of emerging pharmaceutical pollutants (EPPs) in environmental water samples. In this work, we described the fabrication of electrospun nitrogen-rich carbon nitrides/MIL-101(Fe)/poly(acrylonitrile-co-maleic acid) nanofibers (E-spun g-C3N5/MIL-101(Fe)/PANCMA NFs) by using electrospinning dispersion solutions of g-C3N5/MIL-101(Fe) and PANCMA, as well as their applications as sustainable and reusable photocatalysts toward a model EPP carbamazepine degradation under light irradiation. The E-spun g-C3N5/MIL-101(Fe)/PANCMA NFs exhibited the highest carbamazepine degradation efficiency of 94.2% within 40 min. The O2˙−, ˙OH, and h+ reactive species all participated in the photodegradation process, and some degradation byproducts of carbamazepine were identified by liquid chromatography-mass spectrometry. Importantly, the electrospun photocatalyst possessed high reusability (at least 15 consecutive runs) and wide applications in the degradation of other EPPs (such as tetracycline and ciprofloxacin), which suggested the great potential of the electrospun photocatalytical nanofibers in the EPPs removal.
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高影响因子
ACS Applied Nano Materials
·
2021
·
IF 5.097
Jianqiu Gong,Weiwei Zhang,Tapas Sen,Yichen Yu,Yuchen Liu,Jinlong Zhang,Lingzhi Wang
Photocatalysis is a promising technology to treat dilute phenol–Cr(VI) mixture, where photoinduced electrons are commonly thought of as the main active species for Cr(VI) reduction. However, it generally depends on the surface adsorption to achieve efficient electron transfer. Meanwhile, the possible contribution of reductive quinone derivatives oxidized from phenol to Cr(VI) reduction has been rarely explored. The key is to explicitly understand the relation between the phenol oxidation pathway and Cr(VI) reduction. Herein, Ag/AgCl/MIL-101(Fe) prepared by directly loading Ag nanoparticles on MIL-101(Fe) was applied to the joint treatment of phenol and Cr(VI). The role of quinone derivatives in reducing Cr(VI) was revealed by excluding the surface adsorption. During the phenol oxidation, •OH radicals were more consumed in the initial stage for the ring opening of phenol. Meanwhile, 1O2 evolved from •O2– gradually caused the accumulation of reductive quinone intermediates, which dramatically accelerated the Cr(VI) reduction afterward. This study demonstrates the significance of controlling the evolution process of active oxygen species for the joint photocatalytic treatment of phenol–Cr(VI) mixture.
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FOOD CHEMISTRY
·
2021
·
IF 7.514
Yingpan Song,Lina He,Shuai Zhang,Xiao Liu,Kun Chen,Qiaojuan Jia,Zhihong Zhang,Miao Du
Iron-based metal-organic framework, NH 2 -MIL-101(Fe), was doped with different dosages of cobalt phthalocyanine nanoparticles (CoPc) to synthesize a series of NH 2 -MIL-101(Fe)@CoPc nanocomposites. The NH 2 -MIL-101(Fe)@CoPc nanocomposites were then employed to construct novel impedimetric aptasensors for the detection of ochratoxin A (OTA). Combining the intrinsic advantages of NH 2 -MIL-101(Fe) (highly porous structure and excellently electrochemical activity) and CoPc (good physiochemical stability and strong bioaffinity), the NH 2 -MIL-101(Fe)@CoPc nanocomposites show promising properties, which are beneficial for immobilizing OTA-targeted aptamer strands. Amongst, the developed impedimetric aptasensor based on NH 2 -MIL-101(Fe)@CoPc 6:1 , prepared using the mass ratio of NH 2 -MIL-101(Fe):CoPc of 6:1, exhibits the best amplified electrochemical signal and highest sensitivity for detecting OTA. The detection limitation is 0.063 fg·mL −1 within the OTA concentration of 0.0001–100 pg·mL −1 , accompanying with high selectivity, good reproducibility and stability, acceptable regenerability, and wide applicability in diverse real samples. Consequently, the proposed sensing strategy can be applied for detecting OTA to cope with food safety.
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NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 14
·6804-6821
·
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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高影响因子
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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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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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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高影响因子
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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JOURNAL OF SOLID STATE ELECTROCHEMISTRY
·
2024
·Vol. 28
·期 8
·2959-2971
·
IF 2.6
Gao Yali,Pang Wanyu,Chang Xile,Hu Zhiyong,Hu Tuoping,Ma Xuemei
Baicalin (Bn) is one of the flavonoids with various biological activities, and its accurate determination is of great significance to clinical medicine. The new “MOF-on-MOF” materials have a broad application prospect. ZIF-67 and MIL-101(Fe) are typical metal–organic frame (MOF) materials, which have the advantages of flexible structure, large specific surface area, large porosity, and adjustable pore size. In this paper, a disposable and sensitive Bn electrochemical sensor based on ZIF-67/MIL-101(Fe) composite modified carbon paper (CP) electrode was developed for the first time. The sensing nanomaterials were characterized by scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray diffraction spectroscopy (XRD), and X-ray photoelectron spectroscopy (XPS). Cyclic voltammetry (CV) was used to evaluate the electrochemical behavior of Bn on different modified electrodes. The results showed that ZIF-67/MIL-101(Fe)/CP exhibited a well-defined redox peak compared with bare CP, ZIF-67/CP, and MIL-101(Fe)/CP, which was attributed to the synergistic effect of ZIF-67 and MIL-101(Fe). Under optimal conditions, the electrochemical sensor was able to quantify Bn in the ranges of 0.01 ~ 3 µM and 3 ~ 6 µM with a detection limit (LOD) as low as 0.009 µM (S/N = 3). In addition, the sensor was successfully used for the quantitative analysis of Bn in Dual yellow oral liquid with reliable results.
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高影响因子
JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
·
2026
·
IF 6.2
Jie Gao,Leiyu Yang,Yijia Yao,Meiyi Wang
To mitigate the ecological risks of trifluralin (TFL) from volatilization, photolysis, and leaching, a stimuli-responsive composite, TFL/CMC-GEL/MIL-101(Fe), was developed by encapsulating MIL-101(Fe) within a carboxymethyl cellulose–gelatin semi-interpenetrating hydrogel. The composite enhanced light stability of TFL by 1.5 times, reduced leaching by 17.8%, and extended soil retention beyond 14 days, minimizing groundwater contamination. In addition, the herbicidal activity of TFL/CMC-GEL/MIL-101(Fe) against Portulaca oleracea L. and Setaria viridis (L.) P. Beauv. were 95% and 94%, respectively, which was equivalent to TFL technical. Meanwhile, this herbicidal delivery system markedly enhanced crop safety, with rice seed germination rising from 13% under TFL technical alone to 36%. The dual-network design enables on-demand herbicide release by integrating MIL-101(Fe)-mediated protection with hydrogel-based stimuli responsiveness, effectively mitigating herbicide migration in the environment and offering a sustainable plant protection platform.
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高影响因子
CHEMOSPHERE
·
2021
·
IF 7.086
Peipei Huang,Lili Yao,Qing Chang,Yunhan Sha,Guodong Jiang,Shenghua Zhang,Zhe Li
The slow redox rate of Fe(III)/Fe(II) couples is a rate-limiting step for Fenton-like performance of Fe-MOFs. In this study, a series of catalysts (MIL-101) with various p-phthalic acid/2-aminoterephthalic acid (H 2 BDC/NH 2 –H 2 BDC) molar ratios were prepared using a simple and mild chemical method and applied for catalyzed degradation of bisphenol A (BPA). Interestingly, the –NH 2 modified MIL-101(Fe) can adjust Fe-Oxo node by increasing the electron density of Fe(III) in the presence of –NH 2 group with high electron density, thus forming Fe(II) in situ in MOFs. Meanwhile, the –NH 2 groups used as electron-donors can promote electron transfer , resulting in faster Fe(III)→Fe(II) half-reaction and active H 2 O 2 to continuously generate •OH radical. The BPA degradation and rate constant of Fe-BDC-NH 2 /H 2 O 2 system are 15.4-fold and 86.8-fold higher than that of Fe-BDC/H 2 O 2 system, respectively. The density functional theory (DFT) calculations showed that Fe-BDC-NH 2 possesses higher Fermi level energy (−4.88 eV) and lower activation energy barriers (0.32 eV) compared with Fe-BDC. Moreover, Fe-BDC-NH 2 showed good reusability and stability. This work offers a highly efficient and stable MOFs-based Fenton-like catalyst to rapidly degrade organic pollutants over a wide pH range for potential applications in wastewater treatment .
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高影响因子
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