OPTICAL MATERIALS
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2022
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IF 3.754
Hao Hu,Jiacheng Jin,Mingchen Xu,Chengdong Xu,Yue Cheng,Weiwei Ji,Zhencen Ding,Min Shao,Yushan Wan
The present work demonstrates the synthesis of the microsphere composite photocatalyst Bi 3 O 4 Br/NH 2 -MIL-125(Ti) (BOB/NMILT) system, and the physicochemical properties of the material were analyzed by various characterization means. Further, the photocatalytic performance of the BOB/NMILT system was evaluated by degrading tetracycline (TC) under simulated sunlight. The degradation rate of TC using BOB/NMILT-5 reached 88.5% within 90 min. The degradation rate is 6.5 times and 3 times higher than that of individual catalysts NH 2 -MIL-125(Ti) (NMILT) and Bi 3 O 4 Br, respectively. The improvement in photocatalytic activity of composites mainly benefited from the construction of heterojunctions , which effectively inhibited the recombination of carriers. Importantly, the role of h + and •O 2 − was found to be significant in the reaction of TC. Cumulatively, a Z-scheme photocatalytic degradation mechanism of tetracycline on the BOB/NMILT composite system was proposed. The proposal of this system is of great significance for the future development of photocatalytic materials that can degrade tetracycline.
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CHEMICAL ENGINEERING JOURNAL
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2021
·
IF 13.273
Yangjie Fu,Kejie Zhang,Yi Zhang,Yanqing Cong,Qi Wang
Visible-light-active MR/NH 2 -MIL-125(Ti) homojunction was successfully synthesized via post-synthetic modification of NH 2 -MIL-125(Ti). A chromophore group (–MR) similar to the structure of methyl red, was introduced to partially replace the –NH 2 group. Using pure NH 2 -MIL-125(Ti) and MR-MIL-125(Ti) as control samples, the possible structural and optical changes were carefully studied. It was found that the lattice structure remained unchanged, while the specific surface area and band gap were in the order of NH 2 -MIL-125(Ti) > MR/NH 2 -MIL-125(Ti) > MR-MIL-125(Ti). Despite of these, MR/NH 2 -MIL-125(Ti) exhibited highest photocurrent response and lowest charge transfer resistance, which were associated with optimal photocatalytic performance. For the photocatalytic reduction of Cr(VI), the estimated rate constant on MR/NH 2 -MIL-125(Ti) was ca. 9 times and 3 times relative to that on NH 2 -MIL-125(Ti) and MR-MIL-125(Ti), respectively. Besides, 4.6 times rate enhancement can also be observed on the homojunction relative to physical mixture (MR/NH 2 -MIL-125(Ti)-PM). The boosted photocatalytic performance may be ascribed to promoted separation and transfer of photogenerated electron-hole pairs. The operating factors was optimized at acidic pH (2.0), lower catalyst dosage (0.1 g/L) and appropriate concentration of coexisting organics (2.0 mM) within the tested range. Furthermore, good stability both in photocatalytic performance and structure were also observed after 5 cyclic runs. Thus, this study report a facile way for the construction of visible-light-active MOFs, and provided a stable photocatalytic candidate for the disposal of Cr(VI)-containing wastewaters.
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Journal of Environmental Chemical Engineering
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2025
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IF 7.2
Jiepeng Zhao,Yifei Ma,Zhaomin Tong,Mei Wang,Liantuan Xiao,Suotang Jia,Xuyuan Chen
Engineering photocatalyst crystal facets and constructing heterojunctions are effective strategies to improve photocatalytic activity. The amino-modified titanium-based metal–organic framework (MOF) NH 2 -MIL-125(Ti) (NM) has drawn extensive attention as a photocatalyst by virtue of its high specific surface area, abundant pore structure, and narrow bandgap. However, its catalytic activity is hindered by fast electron-hole recombination and limited light absorption. This study synthesizes NM with engineered crystal facets and Co 3 O 4 @NH 2 -MIL-125(Ti) (C-NM) composites with varying Co 3 O 4 loadings using a facile hydrothermal method. The impact of heterojunctions and facet design on photocatalytic CO 2 reduction under visible light is also studied. Results show that the C-NM, with exposed {111} facets and optimal Co 3 O 4 loading, demonstrates superior photocatalytic CO and CH 4 production rates of 21.64 μmol h −1 g −1 and 3.99 μmol h −1 g −1 , 2.1 and 1.6 times higher than those of NM {001} , respectively. Experimental characterization and density functional theory (DFT) analyses attribute the improved photocatalytic activity to several mechanisms. First, crystal facet modulation can optimize the active sites and specific surface area of the photocatalysts. Second, by loading the narrow-bandgap Co 3 O 4 nanoparticles, bandgap of the C-NM photocatalyst is further reduced, thereby enhancing the absorption and utilization of visible light. Finally, the NM/Co 3 O 4 heterostructure minimizes electron-hole recombination, significantly boosting CO 2 reduction efficiency.
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Materials
·
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.
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高影响因子
APPLIED CATALYSIS A-GENERAL
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2024
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IF 4.7
Meidan Que,Yabo Wang,Ruochen Shi,Xun Sun,Jun Xu,Peihong Ma,Yanbo Sun,Jing Guan,Shengxia An
MIL-125(Ti) is well known for having stable structure, tunable electron structure, and multiple active sites, which is commonly studied in the field of photocatalysis . In this work, a series of rare earth (RE) doped MIL-125(Ti) (RE=Ce, Pr, Tm, Dy, Eu, and Sm) are prepared via the one-step hydrothermal method . Notably, Pr-MIL-125 displays a significantly enhanced catalytic performance than other RE-doped MIL-125, resulting in a maximal CO and CH 4 yield of 13.30 and 0.87 µmol·g −1 ·h −1 , respectively, which are 2.53-fold and 4.14-fold of the pristine MIL-125. The layered morphology endows Pr-MIL-125 with more active sites and facilitates the reaction of photoreduction CO 2 . Furthermore, the promoted photoactivities attributed to Pr ion dopant can act as electron transfer bridge and suppress charge recombination. This work would provide insight and guidance for designing RE-MOF based photocatalysts and enhancing the performance of photoreduction CO 2 .
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Materials Today Chemistry
·
2023
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IF 7.3
Wenlong Sheng,Fengwei Huang,Xianjun Lang
Metal–organic frameworks (MOFs) have received increasing attention for conducting miscellaneous photocatalytic reactions. Amorphous TiO 2 , despite the lack of visible light activity, can be a platform for integrating with a Ti-based MOF NH 2 -MIL-125(Ti) during hydrothermal process. Herein, amorphous TiO 2 microspheres are synthesized to enhance the activity of NH 2 -MIL-125(Ti) by integration. The morphology, porosity, and activity of NH 2 -MIL-125(Ti)/amorphous TiO 2 microspheres are systematically investigated by various methods. The photocatalyst NH 2 -MIL-125(Ti)/amorphous TiO 2 exhibits enhanced conversions, more than five times that of pristine NH 2 -MIL-125(Ti), for the selective oxidation of benzylamine. A series of optical and electrochemical characterizations are performed to clarify the mechanism for the photocatalytic selective oxidation of benzyl amines. Specifically, for NH 2 -MIL-125(Ti)/amorphous TiO 2 , visible light absorption is from NH 2 -MIL-125(Ti); and faster electron transfer to molecular oxygen is due to amorphous TiO 2 . This work shows that integrating MOFs with metal oxides can be crucial in enhancing visible light photocatalysis .
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JOURNAL OF ALLOYS AND COMPOUNDS
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2023
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IF 6.2
Hao Tu,Huihu Wang,Huang Xu,Ziguan Zhang,Guode Chen,Chenhuinan Wei,Xing Xiang,Zhixiong Xie
In this work, a series of ZnIn 2 S 4 nanosheets encapsulated NH 2 -MIL-125(Ti) heterostructures (NM-125(Ti)@ZIS) have been rationally designed and established through a facile oil bath method. The photocatalytic Cr(VI) reduction and H 2 evolution performance on NM-125(Ti)@ZIS were elaborately modulated by adjusting the mass ratio of two components, introducing S vacancy and loading cocatalysts. The experimental results demonstrate that the optimized NM-125(Ti)@ZIS heterostructure with mass ratio 3:1 of NM-125(Ti) to ZIS has an excellent Cr(VI) reduction performance in neutral solution, giving 98% reduction efficiency within 60 min. Moreover, the NM-125(Ti)@ZIS heterostructure, following the introduction of sulfur vacancies and the incorporation of Pt nanoclusters , demonstrates an optimal visible light (λ > 420 nm) hydrogen evolution rate of 4.708 mmol/g/h, which is 5.82 times greater than that of pristine ZIS. A thorough investigation of the microstructures and photoelectrochemical properties of the NM-125(Ti)@ZIS heterostructures reveals that the intimate contact interface, sulfur vacancy, and Pt nanocluster serve to effectively enhance charge separation efficiency, thereby improving the photocatalytic performance. Further analysis on the charges behavior at the interface verifies that a novel Z-scheme heterojunction has been constructed between ZnIn 2 S 4 and NH 2 -MIL-125(Ti).
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POLYHEDRON
·
2020
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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).
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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
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SEPARATION AND PURIFICATION TECHNOLOGY
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2021
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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.
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APPLIED ORGANOMETALLIC CHEMISTRY
·
2014
·Vol. 29
·期 1
·12-19
·
IF 2.017
Hongxu Guo,Fan Lin,Jianhua Chen,Feiming Li,Wen Weng
A metal–organic framework material, MIL-125(Ti), was solvothermally prepared and characterized using X-ray diffraction, scanning electron microscopy, Fourier transform infrared spectroscopy and surface area measurements. MIL-125(Ti) was then used as an adsorbent for Rhodamine B (RhB) removal in aqueous solution. The adsorption kinetics, adsorption mechanism, adsorption isotherm, activation energy and various thermodynamic parameters were studied in detail. The maximum adsorption capacity of MIL-125(Ti) for RhB was 59.92 mg g −1 . MIL-125(Ti) appears to be a promising material for RhB adsorption from aqueous solutions. Copyright © 2014 John Wiley & Sons, Ltd.
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CERAMICS INTERNATIONAL
·
2024
·
IF 5.1
Hongmin Dai,Xuan He,Xing Du,Weixin Li,Daheng Wang,Hui Chen,Wei Fang,Lei Zhao
Applying piezoelectric effect on modulating charge transport behavior was considered as one efficient strategy to make feasible charge separation in photocatalysts towards boosting hydrogen evolution performance. Here, with employing corona-poling treatment, SrTiO 3 is converted to be a piezoelectric component in the constructed type II NH 2 -MIL-125(Ti)/SrTiO 3 heterojunction . Since the piezoelectric field could tilt the band bending to a degree to be convenient for the charge transfer from SrTiO 3 to NH 2 -MIL-125(Ti), it is also favorable to offer additional active sites on SrTiO 3 to form dual reduction sites for the following piezo-photocatalytic reaction. Both the ameliorated surficial polarization and charge transfer trajectory in NH 2 -MIL-125(Ti)/SrTiO 3 type II heterojunction are devoted to the boosted hydrogen production rate for NH 2 -MIL-125(Ti)/SrTiO 3 -0.1 (NM/STO-0.1), that is up to 1562.3 μmol h −1 g −1 , 1.79 times higher than that of unpolarized NM/STO-0.1 (871.6 μmol h −1 g −1 ) and 2.35 times higher than that of NH 2 -MIL-125(Ti) (663.8 μmol h −1 g −1 ), respectively. This research reported initially the assistant of SrTiO 3 with piezoelectric feature for enhanced performance photocatalytic hydrogen evolution, which could be one prominent strategy to achieve the reasonable design of efficient photocatalytic system.
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