Catalysis Science & Technology
·
2023
·Vol. 13
·期 15
·4525-4533
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IF 5
Qiuyu Zhang,Yajie Chen,Xinyan Yu,Yuejia Yin,Yaxin Ru,Guohui Tian
Fabricating photocatalysts with customizable structure and composition using different metal–organic framework (MOF) building blocks has intriguing implications in chemistry and material science, but it is challenging to do so. Here, a two-step synthetic strategy was designed to prepare MIL-125(Ti)@TiO2 hollow nanodiscs decorated with Co3S4 nanoparticles for CO2 photoreduction. The Co-based zeolite imidazolium ester backbone (ZIF-67) nanolayer was first loaded on the prepared MIL-125(Ti) nanodiscs to form core@shell MIL-125(Ti)@ZIF-67 nanodiscs. The following sulfidation process under solvothermal condition led to the production of MIL-125(Ti)@TiO2 hollow nanodiscs decorated with Co3S4 nanoparticles (MIL-125(Ti)@TiO2\Co3S4). This ternary hybrid catalyst with hollow nanodisc structure possessed a significantly enhanced charge separation efficiency and visible light absorption, along with offering a huge number of active sites. Considering the above advantages, the CO2 photoreduction activity of the optimized MIL-125(Ti)@TiO2\Co3S4 catalyst was significantly increased when compared to single-component catalysts (MIL-125(Ti), TiO2, and Co3S4) and binary hybrid catalysts (MIL-125(Ti)@TiO2 and TiO2\Co3S4) under simulated sunlight irradiation. CO is the main product with a productivity of 587.50 μmol g−1 h−1, which is almost seven times higher than that of pure MIL-125(Ti). The potential photocatalytic mechanism of the hybrid photocatalyst has also been demonstrated. This study presents a simple and effective technique for fabricating MOF-based hybrid catalysts for photocatalytic applications.
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APPLIED ORGANOMETALLIC CHEMISTRY
·
2015
·Vol. 29
·期 9
·618-623
·
IF 2.248
Hongxu Guo,Di Guo,Zishan Zheng,Wen Weng,Jianhua Chen
Ag nanoparticle (NP)-decorated MIL-125(Ti) microspheres (Ag@MIL-125(Ti)) were firstly fabricated via a facile hydrothermal and following photo-reduction method. The photocatalysts were characterized using X-ray diffraction, scanning and transmission electron microscopies, X-ray photoelectron spectroscopy and UV–visible diffuse reflectance spectroscopy. The characterization results indicated that Ag NPs were dispersed on the surface of MIL-125(Ti) microspheres, and the Ag NPs had a uniform diameter of about 40 nm. The composites exhibited excellent visible-light absorption, due to the modification with the Ag NPs. The photocatalytic activity for the visible-light-promoted degradation of Rhodamine B was improved through the optimization of the amount of Ag loaded as a co-catalyst, this amount being determined as 3 wt%. Additionally, studies performed using radical scavengers indicated that O 2 − and e − served as the main reactive species. The catalyst can be reused at least five times without significant loss of its catalytic activity. Furthermore, a photocatalytic mechanism for degradation of organics over Ag@MIL-125(Ti) is also proposed. Copyright © 2015 John Wiley & Sons, Ltd.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2014
·
IF 3.84
Ying Zhang,Bo Fu,Kuixue Liu,Yupeng Zhang,Xu Li,Shanpeng Wen,Yu Chen,Shengping Ruan
FeCl 3 -NH 2 -MIL-125(Ti) with different FeCl 3 content was prepared and characterized by XRD , SEM and XPS . The humidity sensing properties of FeCl 3 -NH 2 -MIL-125(Ti) have been investigated. Compared with NH 2 -MIL-125(Ti), FeCl 3 -NH 2 -MIL-125(Ti) was more effective in the humidity sensing. The optimal mixing ratio was FeCl 3 -NH 2 -MIL-125(Ti) (8 wt%), which exhibited the best linearity. The impedance of FeCl 3 -NH 2 -MIL-125(Ti) (8 wt%) decreases by almost three orders of magnitude in the range of 11%-95% RH. The response time and recovery time of the humidity sensor by FeCl 3 -NH 2 -MIL-125(Ti) (8 wt%) are 11 s and 86 s respectively. These results indicate the potential application of FeCl 3 -NH 2 -MIL-125(Ti) in humidity sensors.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2024
·
IF 4.9
Qian Wang,Tingting Wang,Yongwei Huang,Liang Cheng,Ting Yang,Yali Ma
The modulation of the crystal phase structure can change the band gap and chemisorbed oxygen content of the metal oxide semiconductors (MOSs) materials, thereby optimizing the gas sensing properties of the material. Herein, the effect of TiO 2 with different crystal phase structures derived from MIL-125 (Ti) calcined at different temperatures on the gas-sensitive properties of acetone is investigated. The study indicates that despite anatase TiO 2 -400 (derived from MIL-125 (Ti) under calcination at 400℃) having a large specific surface area and abundant oxygen vacancies, rutile TiO 2 -700 (derived from MIL-125 (Ti) under calcination at 700℃) exhibits superior gas sensitive performance with the high sensitivity, good selectivity, fast response times, and an ultra-low detection limit (200 ppb) for acetone (biomarker of diabetes). In-depth discussion shows that the excellent sensing performance can be attributed to the regulation of the crystal phase structure of TiO 2 that is favorable for narrowing of band gap, the increase of chemisorbed oxygen content and adsorption energy of acetone molecules. In addition, TiO 2 -700 has excellent properties for diabetes detection in simulation. Our findings help to understand the effect of the crystal phase structure of the material on gas sensitive performance, paving the way for designing excellent TiO 2 -based gas sensors.
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JOURNAL OF SOLID STATE CHEMISTRY
·
2024
·
IF 3.2
Ziqiang Zhang,Zhengfeng Shen,Chuanyu Zhu,Yunfang Wang,Yawen Wang,Caimei Fan,Rui Li,Jianxin Liu
Producing hydrogen from organic/inorganic hydrides is an innovative clean energy alternative to fossil fuels , addressing the increasing energy demands. Here, we first propose coupled photocatalytic water hydrogen production and N,N-dimethylformamide (DMF, C 3 H 7 NO) dehydrogenation technology to obtain high value-added H 2 and N,N-dimethylcarbamic acid (C 3 H 7 NO 2 ). ZnIn 2 S 4 @MIL-125(Ti) nanoheterostructures were synthesized using a simple solvothermal method and resulting in a photocatalytic H 2 production rate of 2.135 mmol h −1 g −1 (apparent quantum efficiency at 380 nm was 2.6 %) which is 2.77 times higher than pure ZnIn 2 S 4 . Liquid-phase mass spectrometry indicates that the DMF oxidation activity of ZIS@MIL heterojunction is double pure ZnIn 2 S 4 and only microcrystalline CO 2 is produced. Isotopes indicate that the production pathway of H 2 results from the coupling of the –CHO bond in DMF and the –H in water. The improved photocatalytic activity of the ZnIn 2 S 4 @MIL-125(Ti) heterostructure is attributed to facilitating efficient charge carrier transfer and separation and DMF depletion of holes accelerates electron transfer .
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Cheng Liu,Qi Chen,Yueling Chen,Jimmy C. Yu,Jionghua Wu,Ling Wu
Photocatalysis, which uses sunlight, N 2 and H 2 O to produce NH 3 , is a more sustainable approach to N 2 fixation than the Haber-Bosch process. However, its efficiency is severely limited by the difficulty of activating N N bonds. This work presents metal (M = Cu, Fe, V)-substituted MIL-125(Ti) (MIL-(MTi)) for photocatalytic N 2 fixation without using any sacrificial agents. Structural characterizations reveal that the active sites including oxygen vacancies (OV) and Ti 3+ species are formed by the resulting crystal distortion due to the partial substitution of Ti 4+ by other metal ions (Cu + , Fe 2+ , V 3+ ) in MIL-125(Ti). MIL-(CuTi) possesses a larger number of OV and Ti 3+ compared to MIL-(FeTi) and MIL-(VTi) due to the larger valence difference between Cu + and Ti 4+ . These active sites not only promote the adsorption and activation of N 2 and H 2 O, but also facilitate the photogenerated charge mobility. Photogenerated holes oxidize H 2 O to produce O 2 and H + . Photogenerated electrons reduce N 2 activated on Ti 3+ sites by combining with H + to form NH 4 + . Therefore, MIL-(CuTi) shows the highest NH 4 + production rate 46.5 µmol·h −1 ·g −1 , which is much higher than that (1.2 µmol·h −1 ·g −1 ) of the pristine MIL-125(Ti). This work provides a new insight into rational design for artificial N 2 fixation systems by the construction of the active site.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Mazhar Khan,Zeeshan Akmal,Muhammad Mubashir Khan,Muhammad Tayyab,Seemal Mansoor,Muhammad Adnan Zeb,Amir Zeeshan,Ziwei Ye,Jinlong Zhang,Shiqun Wu,Lingzhi Wang
Metal-organic framework (MOF) based heterojunctions offer a promising strategy for CO 2 photoreduction, contributing to carbon neutrality and environmental remediation. However, the precise design and control of these heterostructures remain critical challenges. Herein, we report the precise construction of a heterostructure by integrating 2D ZnIn 2 S 4 nanosheets with NH 2 -MIL-125(Ti) for efficient CO 2 photoreduction in a sacrificial agent-free environment. A comprehensive investigation demonstrates robust interfacial interactions and work function differences between NH 2 -MIL-125(Ti) and ZnIn 2 S 4 , facilitating the formation of an interfacial electric field and enabling the construction of an S-scheme heterojunction. The directional migration of photogenerated charge carriers effectively suppresses their recombination, retaining the strong oxidative and reductive potential of the heterostructure components. In-situ infrared spectroscopy provides concrete evidence that the S-scheme heterojunction significantly enhances the formation of key intermediates, which are crucial for CO generation. The optimized NMT-5@ZIS achieves a CO yield of 17.30 umol g -1 h −1 without sacrificial agents, representing 8.6 and 6.6-fold improvements over pristine NH 2 -MIL-125(Ti) and ZnIn 2 S 4 , respectively. This work bestows an innovative insight into the construction of MOF-based S-scheme heterojunctions, opening new avenues for practical applications in energy storage and photocatalysis.
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SOLID STATE SCIENCES
·
2026
·
IF 3.3
Yubo Zhou,Zan Li,Junchao Yin,Liangmin Yu
Photocatalytic degradation of antibiotics in high-salinity seawater remains challenging due to salt ion interference and limited visible-light utilization. In this study, we developed a defect-rich titanium-based metal–organic framework (MIL-125(HAC)) through acetic acid modulation via a solvothermal method. The optimized MIL-125(HAC)-3 photocatalyst exhibited remarkable tetracycline (TC) degradation efficiency in seawater, reaching 90.9% after 60 min of visible-light irradiation (compared with 90.0% in deionized water) and maintaining over 85% efficiency after five cycles. This demonstrates its robust resistance to salt ion interference. Additionally, the degradation rate constant of MIL-125(HAC)-3 in seawater (0.0283 min −1 ) was 25 times higher than that of commercial TiO 2 , highlighting its superior photocatalytic performance. The enhanced performance is attributed to the introduction of acetic acid, which induced a rich mesoporous defect structure, facilitating selective TC adsorption and significantly broadening the visible light response range. Free radical trapping experiments and electron paramagnetic resonance (EPR) spectroscopy further revealed that superoxide radicals (•O 2 − ) and holes (h + ) serve as the primary active species in the degradation process. This work offers a scalable and effective strategy for designing marine-tolerant photocatalysts to remediate antibiotic pollution.
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JOURNAL OF COORDINATION CHEMISTRY
·
2023
·
IF 1.9
Jinyan Tan,Na Zhang,Ling Wang,Liduo Chen,Cuiqin Li,Jun Wang
Metal-organic framework MIL-125(Ti)-NH2 was prepared and coordinated with salicylaldehyde and NiCl2·6H2O to create a heterogeneous catalyst for ethylene polymerization. The structure of the products was characterized by a variety of physical methods, such as Fourier transform infrared spectroscopy (FT-IR), X-ray diffraction (XRD), scanning electron microscopy (SEM), inductively coupled plasma mass spectrometry (ICP-MS), and nitrogen adsorption-desorption. The catalytic performance of MIL-125(Ti)-NH2-Sal-Ni was also investigated. The results showed that the reaction temperature, Al/Ni molar ratio, and ethylene pressure influenced on the catalytic activity and product selectivity. Under optimal reaction conditions, the catalytic activity of MIL-125(Ti)-NH2-Sal-Ni for ethylene oligomerization could reach 5.90 × 104 g·(mol Ni·h)−1 using cyclohexane as the solvent and MAO as the co-catalyst; the main products were C4 and C6. In addition, MIL-125(Ti)-NH2-Sal-Ni had good catalytic stability and recycling, which could be reused at least twice without significant loss of activity. Moreover, based on the evaluation of catalytic performance, the catalytic ethylene oligomerization mechanism of MIL-125(Ti)-NH2-Sal-Ni was also deduced.
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RSC Advances
·
2017
·Vol. 7
·期 68
·42819-42825
·
IF 3.108
Yanghe Fu,Huan Yang,Rongfei Du,Gaomei Tu,Chunhui Xu,Fumin Zhang,Maohong Fan,Weidong Zhu
Co-doped NH2-MIL-125(Ti) catalysts [Co/NH2-MIL-125(Ti)] are developed for the photocatalytic reduction of CO2 upon visible-light irradiation. Compared with NH2-MIL-125(Ti), Co/NH2-MIL-125(Ti) exhibits a significantly enhanced activity in CO2 reduction, due to the fact that the doping of Co nanoparticles onto NH2-MIL-125(Ti) can promote the visible-light harvesting and electron transfer. In addition, when benzylic alcohols as electron donors, instead of triethanolamine (TEOA) which is often used as a sacrificial agent, are added into the reaction system, Co/NH2-MIL-125(Ti) can simultaneously catalyze CO2 reduction to formic acid (HCOOH) and the selective oxidation of the benzylic alcohols to the corresponding aldehydes, making the proposed process more economical and environment-friendly.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Yong Li,Xinyue Yang,Mengyao Wang,Deyun Yue,Jun Wu,Haojie Song
The pollutants present in wastewater can cause structural damage to evaporators, thereby reducing their evaporation efficiency and hindering the application of solar-driven water evaporation technologies. Here, the TiO 2 -based evaporator (CPM-Air) with highly efficient photodegradation and solar-powered water evaporation performance for simultaneous freshwater production and decontamination was prepared by pyrolysis NH 2 -MIL-125(Ti) grown on the surface of Carbon Felt (CF). The evaporation rate of CPM-Air evaporator reached 2.21 kg m -2 h −1 under 1.0 kW/m 2 , and high solar-vapor conversion efficiency of 102.20 %. Meanwhile, the Anatase TiO 2 obtained by carbonized NH 2 -MIL-125 (Ti) has more active sites for removal pollutants. CF as the catalytic promoter to accelerate electron transport, and improve the photogenerated electron-hole separation efficiency. The photothermal-photocatalytic synergy removal efficiency of high concentration (50 mg/L) CIP was 2 times higher than photocatalytic only. In addition, the CPM-Air evaporator has high water evaporation rate in different harsh environments, the 99.9 % of metal ions removal and excellent salt resistance. More importantly, the growth experiments on soybean indicated that the products of photothermal-photocatalytic synergy degradation CIP of CPM-Air evaporator was non-biotoxic. This study provides valuable insights into the potential of photothermal-photocatalytic synergy for sustainable water production.
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COMPOSITES PART B-ENGINEERING
·
2026
·
IF 14
Liang Zhou,Muhaiminul Islam Shakil,Jingyi He,Xiyue Zhang,Hongbo Wang
Metal-organic framework (MOF)-derived carbon materials exhibit significant advantages for microwave absorption applications, owing to their high electrical conductivity, structural tunability, and abundant intrinsic defects and heterogeneous interfaces. However, achieving an optimal balance between magnetic and dielectric losses remains challenging for most magnetic metal-based MOFs-derived absorbers. In this study, MIL-125(Ti) was prepared as a template, and TiO 2 @C-x composites were synthesized via a two-step pyrolysis method. Experimental results demonstrate that the pyrolysis temperature significantly affects the graphitization degree of the carbon matrix and the formation of TiO 2 nanoparticles, thereby playing a dominant role in the dielectric and microwave absorption properties of the investigated MIL-125(Ti)-derived core-shell TiO 2 @C composites. Notably, the TiO 2 @C-700 composite delivers an effective absorption bandwidth of 3.2 GHz in 9.2-12.4 GHz at a thickness of 2.01 mm. Therefore, the MIL-125(Ti)-derived TiO 2 @C composites fabricated in this study establish a viable and nonmagnetic strategy for designing tunable, lightweight, and high-performance MOF-derived microwave absorbers.
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