SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Yong Tang,Jianhao Qiu,Dingliang Dai,Guanglu Xia,Biyao Fang,Yixin Li,Jianfeng Yao
Defect engineering is used in the development of photocatalysts and has received widespread attention for achieving efficient photocatalysis. Here, ZnIn 2 S 4 with rich sulfur vacancies (V S -ZnIn 2 S 4 ) was integrated with MIL-53-NH 2 for photocatalytic H 2 O 2 production from O 2 reduction under visible light. The sulfur vacancy could effectively promote charge separation and O 2 capture, and the heterostructure between ZnIn 2 S 4 and MIL-53-NH 2 further inhibits charge recombination, which promises highly boosted photocatalytic activities. In ambient air and pure water, V S -ZnIn 2 S 4 /MIL-53-NH 2 heterostructures exhibit superior photocatalytic H 2 O 2 production performance (705 μmol·L −1 ) relative to those of monomeric Znln 2 S 4 (78 μmol·L −1 ), V S -Znln 2 S 4 (210 μmol·L −1 ), MIL-53-NH 2 (38 μmol·L −1 ), as well as ZnIn 2 S 4 /MIL-53-NH 2 (395 μmol·L −1 ). Mechanistic studies have confirmed that the main pathway for H 2 O 2 formation on V S -ZnIn 2 S 4 /MIL-53-NH 2 is ⋅O 2 – -triggered O 2 reduction, and sulfur vacancy can adsorb and activate O 2 to facilitate the production of ⋅O 2 – . This study provides new insights into catalyst design and green synthesis of H 2 O 2 .
研究领域:
材料科学
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环境科学
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化学工程
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高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2020
·
IF 9.038
Shi-Wen Lv,Jing-Min Liu,Ning Zhao,Chun-Yang Li,Zhi-Hao Wang,Shuo Wang
Nowadays, designing highly active photocatalysts for pollutant degradation under visible light still remains a challenging problem. Herein, a novel benzothiadiazole functionalized Co-doped MOF-based photocatalyst with electron deficient unit was first synthesized via a feasible step-by-step assembly strategy. Benzothiadiazole, as typical electron deficient group, could effectively promote the separation and transfer of photoinduced charge carriers. The implantation of Co ion could be served as an effective mediator to further facilitate the charge transfer through a Co 3+ /Co 2+ redox pathway. Interestingly, the as-synthesized Co-MIL-53-NH-BT exhibited significantly enhanced photocatalytic degradation capacity for BPA and OFX under visible light irradiation, with removal efficiency as high as 99.9 % and 99.8 % within 120 min. TOC analysis suggested that majority of contaminants had been degraded into CO 2 and H 2 O. The important parameters influencing the photocatalytic activity were investigated, and the kinetics study was also conducted. The possible degradation pathways and the possible photocatalytic mechanism were proposed. More importantly, the as-synthesized Co-MIL-53-NH-BT showed good reusability, stability as well as universal applicability. To sum up, current work not only developed an efficient and visible-light active photocatalyst for treating organic-contaminated wastewater, but also afforded some novel insight into the utilization of benzothiadiazole in MOF-based photocatalyst towards improving photocatalytic activity.
研究领域:
环境科学
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材料科学
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化学
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DOI
PubMed
高影响因子
NEW JOURNAL OF CHEMISTRY
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2024
·Vol. 48
·期 21
·9702-9708
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IF 2.7
An-Xu Ma,Cai-Fang Liu,Yu-Lan Zhu,Zong-Hong Luo,Hong-Mei Zhou,Yue Zhang,Bang-Jin Wang,Jun-Hui Zhang,Sheng-Ming Xie,Li-Ming Yuan
In this work, a chiral core–shell microspheres composite, L-his-MIL-53-NH2@SiO2, was prepared through in situ growth and chiral post-modification strategies. The core–shell microspheres were applied as a novel chiral stationary phase for HPLC enantiomeric separation. Various racemates were separated on the L-his-MIL-53-NH2@SiO2 packed column using n-hexane/isopropanol as the mobile phase. The chiral column showed excellent separation efficiency for fourteen chiral compounds, including alcohols, alkanes, esters, phenols, ketones, and organic acids. The influence of injection mass and temperature on the separation performance of the chiral column were investigated. The relative standard deviations (n = 5) of the retention time and peak area by repeated separation of benzoin are 0.28% and 0.63%, respectively. The results show that the L-his-MIL-53-NH2@SiO2 packed column exhibited good reproducibility and stability. In addition, the chiral resolution ability of the L-his-MIL-53-NH2@SiO2 packed column was compared with that of a commercial chiral column (Chiralpak AD-H). The L-his-MIL-53-NH2@SiO2 packed column exhibits unique advantages in chiral separations that can be complementary to the commercial chiral column. It was demonstrated that the chiral core–shell microspheres composite L-his-MIL-53-NH2@SiO2 prepared based on in situ growth and chiral post-modification strategies has great potential for enantiomeric separation by HPLC.
研究领域:
分析化学
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材料科学
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色谱技术
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DOI
高影响因子
ChemCatChem
·
2026
·Vol. 18
·期 5
·e70662
·
IF 4.1
Mengjiao Yu,Xiong-Fei Zhang,DongEn Zhang,Jianhao Qiu,Jianfeng Yao
The development of stable, efficient catalysts for fructose conversion to 5-hydroxymethylfurfural (5-HMF) remains a challenge. While sulfonation enhances Brønsted acidity in metal–organic frameworks (MOFs), it often compromises their structural integrity. This work addresses the critical challenge by demonstrating that amino (–NH 2 ) functionalization in MIL-53(Al) acts as a stabilizer, enabling the framework to withstand direct modification with chlorosulfonic acid and facilitating the introduction of sulfonic acid groups. The resulting sulfonated catalyst, MIL-53-N/S(1), achieves an outstanding 5-HMF yield of 84.3% in a biphasic system (170°C, 6 h). This work underscores the dual role of amino functionalization in stabilizing MOFs and enabling efficient acid catalysis for biomass conversion. Graphical A strategy using amino-functionalized MIL-53(Al) was proposed, where pre-grafted –NH 2 groups facilitate effective sulfonation to create abundant –SO 3 H sites without compromising framework stability. This approach addresses the challenge between acidity and structural degradation of MOFs. Under optimized conditions, MIL-53-N/S(1) achieves an HMF yield of 84.3%, demonstrating its potential for practical biomass valorization.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2024
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IF 5.8
Yong Tang,Jianhao Qiu,Dingliang Dai,Guanglu Xia,Yixin Li,Biyao Fang,Jianfeng Yao
Sluggish charge transfer dynamics are still the key issue limiting the development of photocatalysis. In this study, CdS/ZnIn 2 S 4 /MIL-53-NH 2 ternary hierarchical heterostructures were constructed via a building block approach, where ZnIn 2 S 4 lamellae first grow on MIL-53-NH 2 followed by CdS nanoparticle deposition. The favorable interfacial compatibility and ternary heterostructures contribute to rapid and multistep spatial charge transfer, which suppresses charge recombination. Therefore, ultrahigh H 2 O 2 production of 1792 μmol·L −1 was obtained over CdS/Znln 2 S 4 /MIL-53-NH 2 composites with visible light, pure water and ambient air, which is not only higher than that of each monomer and binary heterostructure but also better than those of most reported references. Notably, the apparent quantum yield reached 4.5 % at 400 nm, and the solar-to-H 2 O 2 conversion efficiency was 0.081 % in pure water and ambient air. Additionally, H 2 O 2 generation over CdS/Znln 2 S 4 /MIL-53-NH 2 composites involves two-electron O 2 reduction with ·O 2 - as an intermediate. This work may encourage heterostructure design for efficient photocatalytic H 2 O 2 production.
研究领域:
材料科学
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光催化
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纳米技术
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化学工程
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环境科学
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高影响因子
ANALYTICA CHIMICA ACTA
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2017
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IF 4.95
Yaran Du,Xiqian Li,Haijiao Zheng,Xueju Lv,Qiong Jia
In the present work, a novel metal-organic framework (MOF) fluorescent probe was prepared by post-synthetic modification of MIL-53-NH 2 (Al) with carboxylatocalix[4]arene (CC[4]A). The introduced CC[4]A could not only enhance the fluorescence performance and the recognition ability of the probe, but also sustain the high stability under UV light and moisture conditions. A method based on the as-synthesized CC[4]A@MIL-53-NH 2 (Al) probe was established for sensing hippuric acid . The detection limit was determined to be as low as 3.7 μg mL −1 . Over the concentration range of 0.005–3 mg mL −1 , the calibration curve was obtained with a satisfactory linearity ( R 2 = 0.993). The method was successfully used for rapid and highly selective direct monitor of hippuric acid in human urine. The sensor had great potential to be used as a simple diagnostic tool for hippuric acid in human urine which is regarded as a biological index of toluene exposure.
研究领域:
化学
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材料科学
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分析化学
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环境科学
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DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2024
·
IF 13.3
Jiayi Qin,Jia Su,Hong Li,Ling Zhang,Ling Zhang,Ke Jiang
The development of novel antibacterial strategies as alternatives to antibiotics is of great significance but remains considerable challenges due to the lack of safe, effective, and broad-spectrum agents. Here, we explored the potential of a biocompatible metal–organic framework Fe-MIL-53-NH 2 (FM) for reactive oxygen species (ROS)-based antibacterial applications. However, FM was found to be catalytically inert due to the very weak reducibility of Fe 3+ toward H 2 O 2 . To address this challenge, we incorporated a small amount of Co 2+ (0.98 %) into FM (CFM), successfully activating Fenton chemistry and achieving a notable 5.5-fold improvement in Fenton activity. Density functional theory (DFT) calculations revealed that a very small amount of Co 2+ doping significantly reduces the energy barrier of the Fenton reaction by shifting the d-band center to the Fermi level and optimizing the charge density of active Co atoms. We further enhanced the antibacterial properties of CFM by modifying it with the photothermal agent polydopamine (PDA), resulting in CFMP. Through the synergistic effects of ROS and photothermal properties, CFMP exhibited remarkable antibacterial activity, with bacterial eradication rates exceeding 99 % against both E. coli and S. aureus . Moreover, in vivo experiments demonstrated the exceptional efficacy of CFMP in sterilizing S. aureus -infected wounds, while causing negligible damage to other major organs. This study not only highlights the role of atom engineering in activating Fenton reaction, but also provides rational designs for a synergistic antibacterial strategy via powerful MOFs chemistry.
研究领域:
材料科学
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纳米技术
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生物医学工程
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化学
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微生物学
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高影响因子
NANOTECHNOLOGY
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2024
·Vol. 35
·期 42
·425702
·
IF 2.9
Rui Li,Huilin Hu,Furong Xiong,Xiang Xue,Minqi Wu,Xuan Zuo,Wang Zhang,Xiangliang Pan
Efficient metal–organic frameworks (MOFs) photocatalytic bactericidal catalysts are urgently needed in water purification. Herein, a Fe-MOF (MIL-88B-NH2(V1Fe5) with promoted electron transport was achieved by vanadium (V) ions doping and V/Fe ratio optimization, showing excellent photocatalytic bactericidal activity against E. coli under visible light irradiation (99.92%). The efficient antibacterial mechanism, V as a Ti-like mediator boosting electronic transmission in MIL-88B-NH2(V1Fe5), was revealed by its band structure, transient photocurrent, electrochemical impedance spectroscopy, and scavenger quenching experiments. The enhancement of photocatalytic bactericidal performance of Fe-MOFs by V–ion-doping was confirmed by two other Fe-MOFs, MIL-53-NH2(V1Fe5) and MIL-101-NH2(V1Fe5), with the same metal ions and ligands, both of which have higher performance than the corresponding undoped MOFs. Among them, MIL-88B-NH2(V1Fe5) exhibits the highest photocatalytic bactericidal activity due to its suitable metal clusters ([M(μ3-O)] cluster) and topological structure (three-dimensional rhomboid network structure). This work demonstrated the amplification effect of V ion doping on electron transport in Fe-MOFs photocatalysts.
研究领域:
材料科学
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环境科学
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化学
·
光催化
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产品关联
DOI
PubMed
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2019
·Vol. 44
·期 4
·1245-1252
·
IF 3.069
Shi-Wen Lv,Jing-Min Liu,Ning Zhao,Chun-Yang Li,Zhi-Hao Wang,Shuo Wang
The issue of environmental pollution is currently more and more serious, and developing an effective method with universal applicability for removing various contaminants is pretty necessary. Herein, a novel photocatalyst denoted as Co-doped MIL-53-NH2(Fe : Co 4 : 1) was constructed via a feasible solvothermal method, which served as an efficient mediator to activate peroxydisulfate for degrading various organic pollutants. Results from the current work indicated that doping Co with an appropriate proportion could enhance the optical absorption intensity of MIL-53-NH2 and reduce the band gap. Furthermore, a Co ion acting as a mediator could facilitate the charge transfer through a Co3+/Co2+ redox pathway, and thereby suppress the recombination of photogenerated electron–hole pairs. More interestingly, the Co-doped MIL-53-NH2 exhibited excellent and extensive degradation abilities for various organic pollutants including bisphenol A (BPA), antibiotics and organic dyes in the presence of peroxydisulfate (PS) under visible light irradiation. It was also found that ˙OH and SO4−˙ were the major contributors to the catalytic process. Total organic carbon (TOC) analysis indicated that the majority of the contaminants were degraded into CO2 and H2O. Even in the real samples, the developed Co-doped MIL-53-NH2/PS/solar system still possessed excellent performance for the degradation of BPA. Possible photocatalytic mechanisms and the kinetics were also investigated. Besides, the Co-doped MIL-53-NH2 had good catalytic reusability and stability. To sum up, this study provides a promising approach for removing organic pollutants from wastewater.
研究领域:
环境科学
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材料科学
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化学工程
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光化学
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高影响因子
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