APPLIED SURFACE SCIENCE
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2020
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IF 6.182
Zhihui Lu,Xuefang Cao,Hong Wei,Wenting Huo,Qiquan Wang,Kebin Li
Metal organic frameworks (MOFs) have shown a great potential to act as heterogeneous Fenton-like catalysts. However, the lower catalytic efficiency and reaction rate are limiting their practical applications. Herein, a facile and efficient strategy was studied to boost the catalytic oxidation performance of MIL-68(Fe)-mediated Fenton-like process with the addition of a minor amount of bisulfite. The factors affecting the catalytic oxidation capacity of the MIL-68(Fe)/HSO 3 − /H 2 O 2 system were investigated using methyl orange (MO) as model pollutant. Under the optimal condition, the degradation rate of MO could be increased by 11.5 times compared to that in MIL-68(Fe)/H 2 O 2 system, and the total organic carbon (TOC) removal in 120 min reached 46.8%. The MIL-68(Fe)/HSO 3 − /H 2 O 2 system also displayed a wide applicable pH range. Besides MO, other organic contaminants such as acid red 18 (AR18), rhodamine B (RhB), methylene blue (MB), xylenol orange (XO) and tetracycline hydrochloride (TC) could be effectively degraded in the MIL-68(Fe)/HSO 3 − /H 2 O 2 system as well. The quenching tests and electron paramagnetic resonance (EPR) spectrometry confirmed that OH, SO 4 − , HO 2 , and 1 O 2 were the main reactive species for MO degradation in the MIL-68(Fe)/HSO 3 − /H 2 O 2 system. The coumarin fluorometry further disclosed that much more hydroxyl radicals were generated in the MIL-68(Fe)/HSO 3 − /H 2 O 2 system than in MIL-68(Fe)/H 2 O 2 system. Cyclic voltammetry analysis, on the other hand, indicated that the presence of HSO 3 − facilitated the Fe(III)/Fe(II) cycle in the MIL-68(Fe)/HSO 3 − /H 2 O 2 system. Based on these results, the enhancement mechanism of the Fenton-like MIL-68(Fe)/HSO 3 − /H 2 O 2 system was proposed. Finally, the cyclic experiments manifested the MIL-68(Fe)/HSO 3 − /H 2 O 2 system had good stability and reusability. This study suggests that the addition of bisulfite being an excellent approach to construct the Fe-MOFs mediated Fenton systems for eliminating organic contaminants in water with high efficiency.
研究领域:
环境科学
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催化化学
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水处理技术
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Ruowen Liang,Zhoujun He,Yi Lu,Guiyang Yan,Ling Wu
Although both step-scheme (S-scheme) heterojunction and metal–organic framework (MOF) photocatalysts have been intensively studied, few efforts have been devoted to combining them to establish high-performance MOF-based S-scheme photocatalysts. In this work, binary Ag@MIL-68(Fe) (Ag@MFe) hybrids were first fabricated by decorating Ag nanoparticles (Ag NPs) onto MIL-68(Fe), an Fe-based MOF. Owing to the high specific surface area of MIL-68(Fe), the plasmonic Ag NPs were uniformly distributed on its surface. Then, AgBr particles were deposited on the Ag@MFe hybrids via precipitation to form the final ternary sandwich-like hierarchical AgBr-Ag@MFe photocatalyst. The 30 %AgBr-1.5 %Ag@MFe sample exhibited excellent photocatalytic performance for the degradation of rhodamine B under visible light irradiation ( λ ≥ 420 nm), with an effectiveness 9.2 and 2.1 times higher than those of the original MIL-68(Fe) and binary 1.5 %Ag@MFe hybrid, respectively. Furthermore, 30 %AgBr-1.5 %Ag@MFe performed as a high-efficiency bifunctional photocatalyst towards the detoxification of water contaminants (mixture of a dye and Cr(VI)). The significantly enhanced photoactivity was attributed to the effective spatial separation of photogenerated electron–hole pairs via S-scheme charge transfer. Moreover, the plasmonic Ag NPs assembled into the contact interface of AgBr and MIL-68(Fe) enhanced the vectorial interfacial electron transfer. The formation of an S-scheme heterojunction was supported by X-ray photoelectron spectroscopy and electron spin resonance studies. This novel bifunctional AgBr-Ag@MIL-68(Fe) hybrid photocatalyst system not only provides new opportunities for environmental remediation but also highlights a promising strategy to construct high-efficiency S-scheme photocatalysts.
研究领域:
材料科学
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环境科学
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光催化技术
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DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2017
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IF 9.446
Fenfen Jing,Ruowen Liang,Jinhua Xiong,Rui Chen,Shiying Zhang,Yanhua Li,Ling Wu
A highly effective Iron Metal-Framework photocatalyst (MIL-68(Fe)) has been successfully prepared via a facile solvothermal method under acidic condition. The UV–vis diffuse reflectance spectrum reveals that the absorption edge of MIL-68(Fe) is 440 nm. The flat-band potential of MIL-68(Fe) is −0.6 V vs. NHE at pH = 6.8, which is more negative than the redox potential of Cr(VI)/Cr(III) (+0.51 V, pH = 6.8). Consequently, it is thermodynamically permissible for the transformation of photogenerated electrons to the Cr(VI) to produce Cr(III). Moreover, MIL-68(Fe) could perform as an efficient photocatalyst towards the reduction of Cr(VI) aqueous with a wide pH range. After 5 min of visible light illumination (λ > 420 nm), almost 100% Cr(VI) can convert to Cr(III) with (NH 4 ) 2 C 2 O 4 as a scavenger (pH = 3), which is also higher than that of N-doped TiO 2 (50%) and ZnO (7.6%) under identical conditions. Furthermore, MIL-68(Fe) is proved to perform as a highly efficient photocatalyst for remove of different aqueous contaminant with malachite green (MG) as a scavenger. Finally, a possible reaction mechanism has also been investigated in detail.
研究领域:
环境科学
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材料科学
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DOI
高影响因子
OPTICS EXPRESS
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2022
·Vol. 30
·期 8
·12409-12419
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IF 3.833
Le Zheng,Chen Wei,Hongrong Zhou,Fanxi Sun,Ang Gao,Dongsheng Wang,Dongsheng Wang,Yong Liu
Pulsed lasers operating in the mid-infrared are of great importance for numerous applications in spectroscopy, medical surgery, laser processing, and communications. In spite of recent advances with mid-infrared gain platforms, the lack of a capable pulse generation mechanism hinders the development of compact mid-infrared pulsed laser source. Here we show that MIL-68(Al) and MIL-68(Fe), which are aluminum- and iron- based metal-organic frameworks (MOFs) with ordered atoms distribution and periodic mesoporous structure, constitute exceptional optical switches for the mid-infrared. We fabricated the MIL-68(Al) and MIL-68(Fe) via hydrothermal method and prepared reflection-type MIL-68(Al)- and MIL-68(Fe)- saturable absorber mirrors (SAMs). By employing the as-prepared SAMs in the laser cavities, we achieved high-power nanosecond Q-switched fiber lasers at 2.8 µm. Especially, the average output power and pulse duration of the MIL-68(Al) Q-switched fiber laser reached 809.1 mW and 567 ns, respectively. To the best of our knowledge, this is the first time to demonstrate that MIL-68(M) can be efficient optical switches for 3-µm mid-IR laser pulses generation. Our findings reveal that MIL-68(M) is promising saturable absorber for compact and high-performance mid-infrared pulsed lasers.
研究领域:
光学
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材料科学
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DOI
PubMed
高影响因子
Nature Communications
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2026
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IF 18.1
Lv Guoliang,Zhang Linjuan,Luo Yuanyuan,Zhu Jianqiu,Wu Jilong,Qin Li,Zhang Yanlin,Zhang Zheng,Tan Pengwei,Duan Guotao
Simultaneously achieving chemiresistive gas sensors with high selectivity, sensitivity, and stability remains a significant challenge. In this study, inspired by the H 2 S-specific catalytic enzymes in biological systems, we construct an amorphous unsaturated-ligand MIL-68(Fe) 3D MOF via in situ thermal induction. Without the introduction of extrinsic catalytic or conductive components, this MOF modification strategy creates unsaturated Fe atoms within the framework itself. These atoms function dually as catalytic and conductive sites, thereby overcoming the inherent low conductivity of conventional 3D MOFs and enabling the direct construction of chemiresistive sensor for room-temperature molecular olfactory sensing. The targeted water-adsorption-coordinated catalytic mechanism bypasses the limitations of traditional oxygen adsorption processes to achieve unprecedented comprehensive performance, including fingerprint-level selectivity (against 29 interfering gases), superior sensitivity coefficient (~83/ppm), ultra-low measured lower limit (1 ppb), rapid gas sensing response/recovery characteristics (~30 s/73 s), and excellent long-term stability at room temperature.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2026
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IF 9.1
Yufei Chen,Luyao Li,Ying Wang,Siqi Wan,Conghui Liu,Xingang Kong,Jianfeng Huang,Changqing Liu,Wenjie Huang,Lixiong Yin
Solar-driven photocatalytic hydrogen evolution represents a promising strategy, yet constructing photocatalysts that simultaneously deliver high activity and efficient visible-light utilization remains challenging. In this work, an Fe-ion-doped metal–organic framework, MIL-68(Fe), was synthesized and employed as substrate template for in-situ growth of ZnIn₂S₄ nanosheets. Subsequent one-pot synthesis yielded hollow tubular MIL-68(Fe)/ZnIn₂S₄ composite uniformly coated with ZnIn₂S₄ nanosheets, effectively mitigating severe stacking inherent to pure ZnIn₂S₄. Characterization confirmed successful Fe-ion doping, which significantly enhanced visible-light absorption. The optimal composite achieved photocatalytic hydrogen evolution rate of 10.04 mmol·g −1 ·h −1 , representing 9.84-fold enhancement over pristine ZnIn₂S₄. Density functional theory calculations revealed that interfacial Fe O and in O bonds facilitate built-in electric field formation within [ZnS₄] layers, confirming successful S-scheme heterojunction construction. This unique structure preserves photogenerated charge carriers with stronger redox potentials, thereby substantially boosting overall photocatalytic activity. This study offers novel approach for photocatalyst modification and demonstrates synergistic combination of ion doping with S-scheme heterojunction engineering as highly promising research direction
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高影响因子
JOURNAL OF MOLECULAR LIQUIDS
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2023
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IF 6
Cheng Peng,Xinyu Chen,Yu Yang,Feiyang Luo,Xuehui He,Yan Yu,Qiao Deng,Tianding Hu,Shaoyun Shan,Yunfei Zhi,Lihong Jiang,Hongying Su
The development of advanced strategy to activate persulfate for wastewater treatment is an ever-hot research topic. Herein, a high-performance composite catalyst MIL-68(Fe)/CuBi 2 O 4 (30 %) (M-CBO-30) was prepared by in-situ synthesizing MIL-68(Fe) in the CuBi 2 O 4 . The catalytic performances of M-CBO-30 as heterogeneous catalyst to activate PDS for the Rhodamine B (RhB) degradation were systematically studied. It was shown that the M-CBO-30/PDS system presented an ultrahigh RhB degradation efficiency which could remove 100 % RhB within 5 min only using 0.4 g L − 1 catalyst and 0.4 mM PDS. In addition, the M-CBO-30 could remove RhB at a wide pH range (2–10). One should note that the M-CBO-30 exhibited outstanding reusability which afforded high degradation efficiency after 5 successive recycles. And the catalyst structure remained still after being used for 5 catalytic cycles. Heavy metal ions leaching experiment indicated that Cu 2+ leaching concentration of M-CBO-30 was far lower than that of the city water criterion in Europe. The RhB degradation mechanism by M-CBO-30/PDS system was proposed based on the result of electrochemical experiment, radical quenching test, electron paramagnetic resonance and XPS analysis. The RhB degradation was attributed to the oxidization of reactive oxygen species (i.e., SO 4 •− , •OH and 1 O 2 ). The synergistic effect of redox cycle of surface Fe, Bi and Cu were responsible for the high-efficient PDS activation. The excellent recyclability, outstanding structural stability, wide pH application range, less heavy metal leaching and superhigh RhB degradation efficiency highlights the light application prospect of M-CBO-30 in SR-AOPs-driven RhB decontamination.
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高影响因子
ACS Catalysis
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2015
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IF 9.312
Dengke Wang,Mengtao Wang,Zhaohui Li
Phenol is one of the most important chemicals in industry. One-step selective benzene hydroxylation is an attractive yet challenging method for phenol production, especially when such a reaction can be driven by solar energy. Herein, we reported that a highly selective benzene hydroxylation to phenol can be achieved over two Fe-based metal–organic frameworks [MIL-100(Fe) and MIL-68(Fe)] under visible light irradiations using hydrogen peroxide (H2O2) as an oxidant. An optimal benzene conversion of 30.6% was achieved with a H2O2:benzene ratio of 3:4 over MIL-100(Fe) after 24 h irradiations. ESR results and the kinetic studies suggested that a successful coupling of the photocatalysis of Fe–O clusters in Fe-based metal–organic frameworks (MOFs) with a Fenton-like route is involved in this benzene hydroxylation process. The comparison of the reaction over MIL-100(Fe) and MIL-68(Fe) reveals that the structure of MOFs significantly influences the photocatalytic efficiency. Because the composition and the structure of MOFs are highly tunable, this study highlights the great potential of using Fe-based MOFs for photocatalytic benzene hydroxylation to form phenol, which may result in an economical, sustainable, and thus green process for phenol production.
研究领域:
化学工程
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材料科学
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环境化学
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光化学
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DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2017
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IF 9.446
Ruowen Liang,Fenfen Jing,Guiyang Yan,Ling Wu
Visible-light-initiated organic transformations have received much attention because of low cost, relative safety, and environmental friendliness. In this work, a series of CdS-decorated MIL-68(Fe) nanocomposites (CdS-M68 NCs) have been prepared via a facile room-temperature photodeposition technique in a controlled manner. Importantly, the CdS-M68 NCs exhibit remarkably enhanced photoactivity toward selective reduction of 4-nitroaniline (4-NA) to p -phenylenediamine (PPD) in water under visible light irradiation (λ ≥ 420 nm) as compared to bare CdS and MIL-68(Fe), giving a 4-NA conversion of ∼100% after irradiation for 8 min. The significantly enhanced photoactivity is attributed to the integrated factors of the effective transportation of the photogenerated electron-hole pairs and the enhanced visible light absorption intensity. Combining with trapping experiments and ESR analysis, it could be revealed that the photoexcited electrons and CO 2− radicals should be the main active species in the present system. In addition, a possible photocatalytic reduction mechanism has been investigated.
研究领域:
材料科学
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环境科学
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）