Catalysis Science & Technology
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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
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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
Catalysts
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2020
·Vol. 11
·期 1
·24
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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
JOURNAL OF SOLID STATE CHEMISTRY
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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
RSC Advances
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2017
·Vol. 7
·期 68
·42819-42825
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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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高影响因子
Materials
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2025
·Vol. 18
·期 6
·1343
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IF 3.2
Hangmin Xu,Hao Song,Xiaozhi Wang,Xingwang Zhu
The substantial release of industrial carbon dioxide has been identified as a key factor in the development of various environmental issues. In addressing these concerns, the utilization of photocatalytic technology for carbon reduction has garnered significant attention. The disadvantage of CO2photoreduction is the problem of product yield and selectivity. It is known that MIL-125(Ti) with a high specific surface area (SBET) possesses more active sites using Ti as a node. The calcination of MIL-125(Ti) in a reducing atmosphere has been shown to introduce oxygen vacancies (OV), thereby enhancing the material’s surface and internal pores. This process has been demonstrated to result in a significant increase in the SBETand an enhancement of the Ti3+/Ti4+ratio. The increased Ti3+centers have been found to improve the material’s reducing properties. The results demonstrate that the OV-rich MIL-125-2H material exhibits the high-performance and highly selective photoreduction in CO2.
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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DOI
PubMed
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
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2014
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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.
研究领域:
材料科学
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传感器技术
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纳米材料
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功能材料
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DOI
高影响因子
CHEMOSPHERE
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2022
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IF 8.943
Cheng Cheng,Dongyun Chen,Najun Li,Hua Li,Qingfeng Xu,Jinhui He,Jianmei Lu
This paper reports the application of NH 2 -MIL-125(Ti) modified carbon nitride C v -C 3 N 4 with carbon vacancies in the removal of NO. We performed a series of characterizations of the complex and compared various ratios with the individual components. The results of UV spectrum analysis show that the composite's range of light absorption expanded due to the modification of Ti metal–organic framework. Furthermore, the results of photocurrent and electrical impedance indicate the compound has a better ability to generate and transfer electrons . The increase in the compound's NO removal efficiency (up to 63%) indicates that MOF has a positive effect on C v -C 3 N 4 modification—a good method for photocatalysis . Moreover, the compound can promote photocatalysis in a favorable direction.
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
POLYHEDRON
·
2020
·
IF 2.343
Zhongmin Liu,Cong Wang,Yongchuan Wu,Longlong Geng,Xiuling Zhang,Dashuai Zhang,Hui Hu,Yongzheng Zhang,Xin Li,Wei Liu,Ping Na
The adsorption behavior of arsenic on adsorbent have been researched widely, but chemical adsorption of arsenic is uncommon. In this work, a kind of microporous metal-organic framework (MIL-125(Ti)) with columnar morphology and uniform size was solvothermally synthesized, and its chemical adsorption behavior and mechanism of arsenic were firstly investigated by experimental and simulation study. Remarkably, ultra-fast adsorption behavior and excellent arsenic removal capability was achieved. It takes only 20 min to rapidly remove 5 mg L −1 arsenic with 0.2 g L −1 MIL-125(Ti), which is far superior to the previously reported materials. Both experimental and simulation study results show that the adsorption of arsenic obeys a new chemical adsorption mechanism. Both As(III) and As(V) can easily replace the terephthalic acid ligand via competitive coordination and bind to the Ti active site of MIL-125(Ti). In addition, the reaction energy barriers for ligand substitution by H 2 O, As(III) and As(V) are 0.46, 0.33 and 0.15 eV, respectively, which further confirming that structure reforming of MIL-125(Ti) plays a key role for chemical adsorption. The study solves the difficulty of removing low concentration of arsenic and provides molecular-level understanding of the chemical adsorption mechanism of arsenic on MIL-125(Ti).
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
SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Guanglai Mo,Linxi Wang,Jianhong Luo
It is a challenge to achieve efficient photocatalytic activity of pure MOFs. Herein, the defective NH 2 -MIL-125(Ti) with adjustable linker vacancy level was successfully created by thermal treatment. The band gaps of samples decreased and the more Ti-O clusters on the surface of the samples can be achieved as the time of thermal treatment increased from 0 to 500 min, both of which facilitated the photocatalytic activity for the reduction of Cr(VI). Moreover, the ligands from the surface to the inside of the samples were successively decarboxylated, resulting in the declined specific surface area and the increased proportion of mesoporous and the defect level. The moderate defect level in NH 2 -MIL-125(Ti) can be obtained as the time of thermal treatment was 300 min, which facilitated the separation of photogenerated charges, contributing to the highest photocatalytic activity for reduction of Cr(VI), which was 9.2 times than that of the initial MOFs. However, the excessive linker vacancy defect level in NH 2 -MIL-125(Ti) may result in the seriously affected crystal structure and the retarded separation of photogenerated charges.
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 COORDINATION CHEMISTRY
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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.
研究领域:
材料化学
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催化化学
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高影响因子
危险品化学品经营许可证（带存储）