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.
研究领域:
材料科学
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化学
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DOI
高影响因子
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.
研究领域:
材料科学
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环境科学
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DOI
PubMed
高影响因子
APPLIED ORGANOMETALLIC CHEMISTRY
·
2015
·Vol. 29
·期 9
·618-623
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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.
研究领域:
材料科学
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环境科学
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DOI
高影响因子
JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
·
2025
·Vol. 36
·期 19
·1-15
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IF 2.8
Li Zi-Yan,Li Ya-Jun,Li Wei,Wang Ze-Hong,Zhao Zhao-Ye,Zhou Ting-Ting,Huang Yi-Rui,Wu Xiang-Feng,Zhang Peng-Liang,Zhen Zi-Yan,Ci Li-Jie
In this study, a photoelectrochemical sensor for the detection of glucose was developed by combining the unique properties of NH 2 -MIL-125 and Ti 3 C 2 film. The relationship between the microstructure of the samples and their performance in glucose detection was investigated. Experimental results demonstrated a linear decrease in the differential pulse voltammetry current of the Ti 3 C 2 /NH 2 -MIL-125-3 photoelectrochemical sensor with increasing glucose concentration. Below 200 μM, the relationship between DPV current and glucose concentration was found to be: I (mA) = − 3.86667 × 10 –8 ·c g (μM) + 3.66 × 10 –4 (c g denoted as the concentration of glucose). Above 200 μM, the relationship was: I (mA) = − 4.03049 × 10 –8 ·c g (μM) + 3.68268 × 10 –4 . Density functional theory calculations were in agreement with the experimental data. The Ti 3 C 2 /NH 2 -MIL-125-3 photoelectrochemical sensor demonstrates exceptional glucose detection capability. This technology has the potential to advance the development of MXenes/MOFs-based photoelectrochemical biosensors.
研究领域:
生物传感
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材料科学
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分析化学
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DOI
高影响因子
LANGMUIR
·
2025
·
IF 3.9
Guang Lu,Lunqiu Zhang,Jiling Liang,Wei Li,Zheng Li,Xuejun Zou,Xiaodong Zhang
Herein, first, MIL-125 samples were synthesized via a hydrothermal method. Then, Ag species were doping on the surface of MIL-125 samples via the photolysis of silver nitrate. Finally, the Z-scheme MIL-125/Ag/BiOBr composite was synthesized via a directed liquid assembly method. The structure, morphology, and optical properties of the prepared samples were investigated via X-ray diffraction, scanning electron microscopy, high-resolution transmission electron microscopy, energy-dispersive X-ray spectroscopic mapping, Fourier transform infrared spectroscopy, X-ray photoelectron spectroscopy, N2 adsorption–desorption analysis, ultraviolet–visible spectroscopy, photoluminescence spectroscopy, surface photovoltage analysis, transient photocurrent response analysis, electrochemical impedance spectroscopy, and electron spin resonance analysis. Photocatalytic experiments indicated that the photocatalytic Cr6+ reduction efficiency of MIL-125/Ag/BiOBr heterojunctions was 85.7% at pH = 6, which was approximately 5.5 and 2.2 times higher than that using BiOBr and MIL-125 alone, respectively. This performance was attributed to the intimate interfacial contact between MIL-125 and BiOBr and the doping of Ag species, which increased the transfer and separation of photogenerated carriers and inhibited the recombination of electrons and holes. Furthermore, the possible photocatalytic Cr6+ reduction mechanism of the Z-scheme MIL-125/Ag/BiOBr photocatalyst was proposed.
研究领域:
材料科学
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环境科学
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DOI
PubMed
高影响因子
INORGANIC CHEMISTRY
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2025
·
IF 4.7
Xian-Yu Shen,Ya-Nan Wang,Ya-Ting Zheng,Ye Wang,Wen-Wen Dong,Jun Zhao,Dong-Sheng Li
Formaldehyde (HCHO), a crucial industrial chemical, finds extensive applications across diverse sectors, including household products, commercial materials, aviation, and medical supplies. Methane (CH4), as an abundant C1 resource, presents a promising feedstock for HCHO synthesis. However, the direct conversion of CH4 to HCHO remains challenging due to its inherent chemical inertness, characterized by low polarizability and high C–H bond dissociation energy (439 kJ mol–1), coupled with the high reactivity of intermediate products. The development of efficient strategies for selective CH4 oxidation to high-value HCHO under mild conditions is therefore of significant practical importance. In this study, we developed a series of MIL-125-NH2@FeOOH-x heterostructured photocatalysts (FM-x) through the controlled deposition of FeOOH nanoparticles on MIL-125-NH2 surfaces. Comprehensive characterization and photocatalytic evaluations reveal that the optimized FM-1 catalyst facilitates in situ H2O2 generation and subsequent decomposition into hydroxyl radicals (•OH), enabling efficient CH4 photooxidation. Remarkably, the FM-1 catalyst achieves an exceptional HCHO production rate of 197.79 μmol·gcat–1 with >99.99% selectivity in water vapor, significantly outperforming both pristine FeOOH and MIL-125-NH2 components. This work presents a promising photocatalytic system for selective CH4 conversion, offering new insights into the design of efficient catalysts for C1 chemistry.
研究领域:
化学工程
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材料科学
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环境科学
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DOI
PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2024
·
IF 12.2
Xuanhao Liang,Guangyuan Chen,Hao Zhang,Ling Zhang,Tao Duan,Lin Zhu
Ti-based MOFs exhibit ultra-high stability in radioactive waste gases containing nitrogen oxides (NO X ) and are effective in capturing radioactive iodine. In this study, NH 2 -MIL-125 was synthesized via a one-pot solvothermal method and its adsorption performance for iodine was investigated using batch adsorption experiments, the stability of materials was tested by simulating post-processing conditions. The results indicated that NH 2 -MIL-125 had a maximum iodine adsorption capacity of 1.61 g/g at 75 ℃ and reached adsorption equilibrium within 60 min, and the adsorption capacity of methyl iodine reached 776.9 mg/g. The material also exhibited excellent stability and iodine adsorption performance in the presence of NO X . After soaking in NO 2 for 24 h, its structure remained stable and the adsorption capacity for iodine remained at 231.5 mg/g. The excellent co-adsorption performance of NH 2 -MIL-125 on iodine and NO X was attributed to the synergistic effects of Ti-OH groups and amino functional groups. These findings provide a reference for the capture of radioactive iodine and also demonstrate the potential of NH 2 -MIL-125 for iodine capture during spent fuel reprocessing .
研究领域:
材料科学
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环境科学
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核能工程
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DOI
PubMed
高影响因子
Catalysts
·
2020
·Vol. 11
·期 1
·24
·
IF 3.52
Juan Du,Jiaxin Zhang,Tingyu Yang,Renming Liu,Zhiyi Li,Dandan Wang,Tong Zhou,Yucun Liu,Chunbo Liu,Guangbo Che
The BiOI/NH2-MIL-125(Ti) composite photocatalyst with excellent photocatalytic performance was prepared by the solvothermal method. For the BiOI/NH2-MIL-125(Ti) (BNMT) system, the contents of NH2-MIL-125(Ti) in BNMT-4, BNMT-5, BNMT-7, BNMT-9, and BNMT-10 were 4 wt %, 5 wt %, 7 wt %, 9 wt %, and 10 wt %, respectively. XRD, XPS, SEM, and TEM characterizations indicated that BiOI/NH2-MIL-125(Ti) was successfully prepared. Brunauer, Emmett, and Teller (BET) and UV–vis diffuse reflectance spectra photoelectrochemical analysis indicated that BNMT-9 can make the specific surface area and photo absorption region larger than BiOI. In addition, the separation efficiency of photogenerated carriers was improved, and the recombination efficiency was reduced. The degradation percentages of Rhodamine B (RhB) and p-chlorophenol (P-CP) reached 99% and 90% over BNMT-9 under visible light irradiation. Additionally, the catalysts had high stability. The results of the active spices trapping experiments test indicated that h+was the main active species. The possible degradation mechanism was proposed.Keywords:photocatalysis;BiOI;NH2-MIL-125(Ti);organic pollutants
研究领域:
材料科学
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环境科学
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DOI
高影响因子
INORGANIC CHEMISTRY
·
2023
·
IF 4.6
Jun-Qing Ye,Yan-Zi Dai,Shu-Ying Xu,Pin-Xi Wang,Zhong-Hua Sun,Jun-Feng Qian,Qian Liang,Ming-Yang He,Qun Chen
The construction of efficient photocatalysts for water splitting to enable H2 evolution is pivotal to alleviate energy issues and environmental concerns. In this work, carbon dots (CDs) were prepared by employing “green solvent” ionic liquids as carbon sources and then combined with Pt/NH2-MIL-125, resulting in the emergence of a high-efficiency photocatalyst termed CDs-Pt/NH2-MIL-125 for the first time. This composite photocatalyst exhibited outstanding photocatalytic activity in H2 production under visible light irradiation. Notably, the H2 production rate of CDs100-Pt/NH2-MIL-125 reaches up to 951.4 μmol/g/h, which was 3.1 times that of Pt/NH2-MIL-125. The characterization results indicate that CDs and Pt uniformly dispersed on the surface of NH2-MIL-125 and fabricated a synergistic compact structure, providing a high BET surface area (985 m2 g–1) and a suitable band gap. Furthermore, the distinctive embeddable-dispersed CDs and Pt, as dual cocatalyst, can harvest light and facilitate the transfer of photogenerated electrons, thereby significantly augmenting the exploitation of visible light. The plausible mechanism of photocatalytic H2 evolution over the CDs-Pt/NH2-MIL-125 catalyst was also discussed. This work introduces a promising strategy for designing high-performance CDs-MOFs-based photocatalysts, an innovative step toward achieving efficient photocatalytic water splitting for H2 production.
研究领域:
材料科学
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能源化学
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DOI
PubMed
高影响因子
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 .
研究领域:
材料科学
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能源科学
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化学工程
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DOI
高影响因子
BIOTECHNOLOGY AND BIOPROCESS ENGINEERING
·
2022
·Vol. 27
·期 1
·135-144
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IF 3.386
Wang Zichen,Liu Yang,Li Jinhong,Meng Guoqing,Zhu Daoyu,Cui Jiandong,Jia Shiru
As a series of metal organic framework (MOFs), materials of institute lavoisier frameworks (MILs) are expected to be excellent supports for enzyme immobilization due to their good water-stability and acid tolerance. However, enzyme loading on MIL-125-NH 2 is very low due to small pore size and few amino groups on the surface of the MIL-125-NH 2 . In this work, catalase (CAT) was immobilized on the MIL-125-NH 2 and amino functionalized MIL-125-NH 2 by adsorption (CAT@MIL-125-NH 2 ) and covalent binding (CAT@Amino MIL-125-NH 2 ), respectively. Compared with the CAT@MIL-125-NH 2 and free CAT, the CAT@Amino MIL-125-NH 2 displayed high activity recovery, good pH stability, stability against denaturants, and thermostability. Furthermore, activity recovery of CAT@Amino MIL-125-NH 2 was 56% higher than CAT@MIL-125-NH 2 . The CAT@Amino MIL-125-NH 2 still retained 50% residual activity for 14 days at room temperature, whereas free CAT lost activity after storage for 1 day at the same storage conditions. Furthermore, the CAT@Amino MIL-125-NH 2 maintained 62% of its initial activity after 4 consecutive uses, showing good reusability. The results showed that the amino functionalized MIL-125-NH 2 is an excellent carrier of enzyme immobilization.
研究领域:
生物化学
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材料科学
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DOI
高影响因子
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.
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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DOI
高影响因子
危险品化学品经营许可证（带存储）