DALTON TRANSACTIONS
·
2023
·Vol. 52
·期 11
·3517-3525
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IF 4
Shihui Wang,Zhoujun He,Ling Wu,Deling Wang,Ruiru Si,Xiyao Liu,Ruowen Liang
Due to their explicit structure, metal–organic frameworks (MOFs) have been supposed to be credible platforms to research the micro-mechanism of heterogeneous photocatalysis. In this study, amino-functionalized MOFs (MIL-125(Ti)–NH2 (denoted as MTi), UiO-66(Zr)–NH2 (denoted as UZr) and MIL-68(In)–NH2 (denoted as MIn)) with three different metal centers were synthesized and applied for the denitrification of simulated fuels under visible light irradiation, during which pyridine was used as a typical nitrogen-containing compound. The results showed that MTi had the best activity among the above three MOFs, and the denitrogenation rate increased to 80% after 4 h of visible light irradiation. On the grounds of the theoretical calculation of pyridine adsorption and actual activity experiments, it can be presumed that the unsaturated Ti4+ metal centers should be the key active sites. Meanwhile, the XPS and in situ infrared results verified that the coordinatively unsaturated Ti4+ sites facilitate the activation of pyridine molecules through the surface –N⋯Ti– coordination species. The coordination–photocatalysis synergism promotes the efficiency of photocatalytic performance and the corresponding mechanism is proposed.
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MOLECULES
·
2018
·Vol. 23
·期 7
·1524
·
IF 3.098
Xue-Xue Liang,Nan Wang,You-Le Qu,Li-Ye Yang,Yang-Guang Wang,Xiao-Kun Ouyang
In this study, novel composite titanium-based metal-organic framework (MOF) beads were synthesized from titanium based metal organic framework MIL-125 and chitosan (CS) and used to remove Pb(II) from wastewater. The MIL-125-CS beads were prepared by combining the titanium-based MIL-125 MOF and chitosan using a template-free solvothermal approach under ambient conditions. The surface and elemental properties of these beads were analyzed using scanning electron microscopy, Fourier transform infrared and X-ray photoelectron spectroscopies, as well as thermal gravimetric analysis. Moreover, a series of experiments designed to determine the influences of factors such as initial Pb(II) concentration, pH, reaction time and adsorption temperature was conducted. Notably, it was found that the adsorption of Pb(II) onto the MIL-125-CS beads reached equilibrium in 180 min to a level of 407.50 mg/g at ambient temperature. In addition, kinetic and equilibrium experiments provided data that were fit to the Langmuir isotherm model and pseudo-second-order kinetics. Furthermore, reusability tests showed that MIL-125-CS retained 85% of its Pb(II)-removal capacity after five reuse cycles. All in all, we believe that the developed MIL-125-CS beads are a promising adsorbent material for the remediation of environmental water polluted by heavy metal ions.Keywords:metal-organic framework;chitosan beads;adsorption;Pb(II)
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Processes
·
2024
·Vol. 12
·期 9
·1879
·
IF 2.8
Huiying Yang,Xiangchao Meng
The conversion of nitrogen (N2) and water (H2O) into NH3by photocatalysis under ambient conditions has been considered an environmentally friendly strategy. However, developing effective catalysts for N2fixation is still challenging. Herein, we report a bimetallic JH Fe, Co/TiO2derived from NH2-MIL-125(Ti) by the fast Joule heating (FJH) method for visible–light–driven catalytic N2fixation. It was found that the photocatalytic N2reduction efficiency of bimetallic FC@TiO2-JH was improved, enabling an NH3yield rate of 110.14 µmol g−1h−1without any sacrificial agents. Furthermore, the rate was higher than those of Fe@TiO2-JH and Co@TiO2-JH, suggesting that the synergistic effect between Fe and Co broke the electronic equilibrium and increased the center of its d-band, enhancing electronic feedback to the antibonding π* orbitals of N2while weakening the bonding energy of N≡N. Meanwhile, the rate was about 2.75 times higher than that of FC@TiO2-TF, which was calcined in a tube furnace. It is assumed that FJH might lead to the formation of lattice defects, leading to localized charge deficiency, enhanced carrier separation, and transport. Thus, doping of Fe and Co synergistically interacted with the defects produced from FJH, facilitating the photocatalytic reduction process. As detected, it had a greater ability to separate hole–electron pairs and transferred electrons to adsorbed N2at faster rates. Our work demonstrates a prospective strategy for designing bimetallic catalysts derived from NH2-MIL-125(Ti) for N2fixation.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2016
·
IF 8.328
Yanghe Fu,Long Sun,Huan Yang,Lai Xu,Fumin Zhang,Weidong Zhu
The Ni-doped NH 2 -MIL-125(Ti) catalyst was developed for the photocatalytic aerobic oxidation of aromatic alcohols upon visible light irradiation. The results show that different aromatic alcohols can be effectively transformed to their corresponding aldehydes with almost absolute selectivity using O 2 as the oxidant over Ni-doped NH 2 -MIL-125(Ti) upon visible light irradiation. Compared with the parent catalyst NH 2 -MIL-125(Ti), Ni-doped NH 2 -MIL-125(Ti) exhibits a significantly enhanced photocatalytic activity for the selective oxidation of aromatic alcohols. Preliminary studies indicate that the doping of Ni nanoparticles into NH 2 -MIL-125(Ti) could improve the visible-light harvesting, charge-separation, and electron-transport of the resultant catalyst, leading to the enhanced photocatalytic activity. The current work provides some guidance in the development of MOF-based photocatalysts for organic syntheses.
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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 ELECTRONIC MATERIALS
·
2025
·
IF 2.5
Li Lingyu,Ma Qian,Zhao Dongheng,Zhang Huayushuo,Li Bolong
Recently, the development of an n-pentane-sensing product has always been plagued by the lack of suitable inorganic material with good gas-sensing response and selectivity at low operating temperatures. In this work, Ti-MIL-125-induced one-dimensional tubular In 2 O 3 /TiO 2 heterostructures have been fabricated by a facile electrospinning method and a subsequent heat-treatment process. Obvious morphological evolution from a fibrous to a tubular shape with the presence of In 2 O 3 -TiO 2 heterojunctions can be adjusted by varying the added amount of the Ti-ML-125 component. Compared with pure In 2 O 3 , the optimal In 2 O 3 /TiO 2 composites exhibit a blue-shifted energy band (2.52 eV) and an increased specific surface area (227.70 m 2 /g), as well as the enhanced gas-sensing performance on various concentrations of n-pentane. For example, In 2 O 3 /TiO 2 -3% can not only display excellent long-term stability and humidity stability but also has a high response of 670–100 ppm n-pentanol at 50°C, much larger than that of pure In 2 O 3 (50) at 150°C. Significantly, In 2 O 3 /TiO 2 -3% can still reach the high response of 197–100 ppm n-pentanol at room temperature. According to density functional theory (DFT) calculations, the enhanced gas-sensing mechanism is mainly attributed to the combination of the distinctly increased surface active sites through the regulation of morphology and the introduction of effective In 2 O 3 -TiO 2 heterojunctions, which can be beneficial to improving the surface adsorption/desorption characteristics and the electron transport between n-pentanol and the sensing material interface. Graphical
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Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Yisha Zheng,Shuoling Lei,Wenjie Guo,Wenlong Xiang,Yanmei Chen,Yanhui Zhang
The high toxicity and persistence of nitroaromatic pollutants pose a serious threat to aquatic ecosystems. In this study, inert SiO 2 was employed as an "inactive enhancer" to construct core-shell MIL-125-NH 2 @ZIF-67/SiO 2 (M@Z/SiO 2 ) heterogeneous MOF catalysts via an epitaxial-wet impregnation method, enabling the efficient reduction of p -nitrophenol ( p -NP) under ambient temperature and pressure. Although SiO 2 itself lacks catalytic activity, the micro-mesoporous network it forms effectively disperses Co active sites and prevents their aggregation. The conversion rate of p -NP increased from 92.5% to 98.4% within 6 min and retained 98% activity after three consecutive cycles. Moreover, the catalyst exhibited excellent stability across a wide pH range (3-11) and in various anionic environments. Mechanistic studies revealed that the interfacial electron transfer between ZIF-67 and MIL-125-NH 2 significantly reduces the activation energy barrier of NaBH 4 . Additionally, the incorporation of SiO 2 not only enhances the mechanical stability of the composite but also optimizes pore structure and substrate mass transfer by modulating surface hydrophilicity. This work provides valuable insights for the precise design of MOF-on-MOF heterostructures and the synergistic engineering of interfacial and surface properties in environmental catalytic materials.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2025
·
IF 8.3
Jun-Qing Ye,Bin Cheng,Yunfei Bu,Jun-Feng Qian,Qian Liang,Ming-Yang He,Qun Chen
The development of high-efficiency photocatalysts for water splitting to hydrogen (H 2 ) is crucial for alleviating energy crisis and environmental problems. In this study, a novel type-II ternary heterojunction photocatalyst, CDs/NH 2 -MIL-125 (Ti)/Cu 2 O, was fabricated through the integration of NH 2 -MIL-125 (Ti) with Cu 2 O and carbon dots (CDs), exhibited excellent photocatalytic H 2 production rate of 12817.1 μmol/g/h with apparent quantum efficiency (AQE) of 17.13 % under visible light irradiation. Characterization revealed a uniform and dense structural integration with a high Brunauer-Emmett-Teller (BET) surface area of 275.9 m 2 g −1 and a suitable energy band gap of 2.18 eV. Furthermore, the heterostructures promoted efficient photo-generated carrier separation and enhanced reduction capabilities . Notably, CDs, serving as cocatalysts or electron acceptors, improved visible light utilization and electron migration, significantly boosting H 2 production. Insights from electron spin resonance (ESR) and density functional theory (DFT) calculations supported the migration mechanisms of electrons. This work presents a significant advance in photocatalytic technology for sustainable energy by designing high-performance CDs-modified heterojunction photocatalysts.
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DALTON TRANSACTIONS
·
2023
·Vol. 52
·期 35
·12244-12252
·
IF 4
Shen Yu,Zhan Liu,Jia-Min Lyu,Chun-Mu Guo,Yi-Long Wang,Zhi-Yi Hu,Yu Li,Ming-Hui Sun,Li-Hua Chen,Bao-Lian Su
The catalytic oxidative desulfurization (ODS) technique is able to remove sulfur compounds from fuels, conducive to achieving deep desulfurization for the good of the ecological environment. Ti-based metal–organic frameworks (Ti-MOFs) possessing good affinity to organic reactants and considerable numbers of Ti active sites are promising catalysts for ODS. However, current Ti-MOFs suffer from severe diffusion limitations caused by the size mismatch between sole micropores and bulky sulfur compounds, leading to poor ODS performance. Here, a facile method of intraparticle ripening without any additive is developed to obtain hierarchically meso–microporous Ti-MIL-125 single crystals (Meso-Ti-MIL-125) for the first time. Such Meso-Ti-MIL-125 shows a BET surface area of 1401 m2 g−1 and a mesoporous volume that is 1.7 times as high as that of the conventional Ti-MIL-125. Our novel Meso-Ti-MIL-125 exhibits excellent catalytic performance in the ODS of a series of bulky thiophenic sulfur compounds, completely removing benzothiophene (BT), dibenzothiophene (DBT), and 4,6-dimethyldibenzothiophene (DMDBT) from model fuels, which is, respectively, 2.4 times, 1.5 times, and 6.7 times higher than the removal achieved with conventional Ti-MIL-125. Such a facile synthetic strategy is envisioned to be applied in many kinds of crystalline materials, such as zeolites, for industrial production.
研究领域:
化学工程
·
材料科学
·
环境科学
·
催化
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Chemical Science
·
2026
·
IF 8.1
Lijun Liao,Guangquan Zhao,Ruiwen Shu,Xuepeng Wang,Jinxin Zhang,Ruting Yuan
Photocatalytic reduction of nitrate (NO3-) to ammonia (NH3) represents a sustainable route for wastewater treatment and chemical production. Metal-organic frameworks (MOFs) like MIL-125 are promising catalysts, yet their performance often decays during reaction. This study reveals that the aggregation state of Ti3+ sites in MIL-125 is a critical factor governing its photocatalytic efficiency. We demonstrate that the as-synthesized MIL-125, featuring isolated Ti3+ sites, achieves a high NH3 production rate of 738.32 μmol g-1 h-1 under full-spectrum light without sacrificial agents. Comprehensive characterization and theoretical calculations indicate that these isolated Ti3+ sites elevate the material’s conduction band and enhance NO3- adsorption, thereby lowering the energy barrier for the rate-determining step. However, prolonged photoreaction leads to linker deficiency, resulting in agglomeration of Ti3+ sites. This structural evolution causes a negative shift in the conduction band potential, impedes charge separation, and increases the reaction barrier, leading to a noticeable loss in activity over cycles. This work underscores the pivotal role of maintaining isolated metal sites for designing stable and efficient MOF-based photocatalysts for nitrogen cycling.
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JOURNAL OF POLYMER RESEARCH
·
2026
·Vol. 33
·期 8
·327
·
IF 3.5
Yu Shouwu,Yue Tingting,Chen Yifu,Tong Yuxia,Xiao Shujuan
The treatment of dye-containing oil-in-water emulsions remains challenging due to membrane fouling and limited operational stability. In this study, amino-functionalized metal-organic framework (MOF) NH 2 -MIL-125 was incorporated into polysulfone (PSF) membranes via phase inversion to fabricate mixed matrix membranes (MMMs) for oil-in-water emulsion separation and light-assisted self-cleaning. The separation test was conducted at 0.2 MPa using an as-prepared sodium dodecyl sulfate (SDS)-stabilized n-hexane-in-water emulsion containing 1.0 vol% oil. Compared with pristine PSF, the optimized PN0.5 membrane showed a decrease in water contact angle (WCA) from 67.5 ± 2.0° to 22.7 ± 2.4° and an increase in underwater oil contact angle (UWOCA) from 73.0 ± 2.3° to 140.0 ± 2.6°, confirming enhanced hydrophilicity and underwater oleophobicity. PN0.5 achieved a permeate flux of approximately 245 L·m⁻ 2 ·h⁻ 1 and a separation efficiency close to 99%. Moreover, PN0.5 maintained approximately 98% separation efficiency during a seven-day cyclic filtration test. In a separate antifouling test, the membrane exhibited a low irreversible fouling ratio of 3.79%. Under irradiation with a 300 W xenon lamp for 60 min, the NH 2 -MIL-125-containing membrane promoted methylene blue (MB) decolorization and dye-foulant removal, while the irreversible fouling ratio remained low at 3.98% for the MB-containing emulsion after light-assisted self-cleaning. These results demonstrate the potential of NH 2 -MIL-125/PSF mixed-matrix membranes for treating dye-containing oily wastewater.
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Journal of Water Process Engineering
·
2026
·
IF 6.6
Yanhua Liu,Yunpeng Luo,Geoffrey I.N. Waterhouse,Zhiming Zhang,Liangmin Yu
The rational design of charge-transfer interfaces is essential for high-performance photoelectrocatalytic (PEC) wastewater remediation. Herein, a novel ternary n-n-p heterojunction electrode, titanium dioxide/NH 2 -MIL-125(titanium)/polyaniline (TiO 2 /Ti-MOF/PANI), was successfully fabricated via a two-step hydrothermal and chemical polymerization strategy, followed by electrophoretic deposition. The optimized electrode exhibited a superior Rhodamine B (RhB) degradation efficiency of 96.1% and a total organic carbon mineralization rate of 67.19% within 70 min under visible light with a −0.8 V bias, significantly outperforming the individual photocatalytic and electrocatalytic processes. The superior performance originates from the synergistic integration of the ternary components. Ti-MOF and PANI broaden the visible-light response, promoting the generation of photogenerated electron-hole pairs under visible-light irradiation. Within this heterostructure, PANI functions as a narrow-band-gap sensitizer and p-type hole-transport layer, while n-type Ti-MOF provides a continuous pathway for rapid interfacial charge transfer. Meanwhile, n-type TiO 2 serves as a robust electron-transport backbone and offers stable surface active sites for subsequent redox reactions. The resulting n-n-p heterojunction establishes an internal electric field that, in conjunction with the applied negative bias, accelerates charge-carrier migration and accumulation at the electrode surface, thereby facilitating RhB degradation. Furthermore, PANI acts as an efficient conductive bridge, shortening electron-transport distances and reducing interfacial resistance. Mechanistic insights from radical trapping and electron spin resonance analysis confirm that •O 2 − and •OH are the predominant reactive species driving the oxidative cleavage of the xanthene chromophore. Overall, this work provides valuable design principles for multi-component PEC electrodes, offering insights into efficient environmental remediation.
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