SOLID STATE SCIENCES
·
2021
·
IF 3.059
Cong Huang,Jun Wang,Mengjun Li,Xiaofang Lei,Qiang Wu
The construction of Z-scheme systems is a valid strategy to effectively enhance photocatalytic property in the field of photocatalysis . In the present work, a novel Z-scheme V 2 O 5 /NH 2 -MIL-101(Fe) heterojunction photocatalyst was prepared via a simple one-pot solvothermal method for the first time. The phase structure, morphology and optical property of the as-prepared V 2 O 5 /NH 2 -MIL-101(Fe) composite were carried out by a series of characterizations. The photocatalytic property of V 2 O 5 /NH 2 -MIL-101(Fe) heterojunction photocatalyst was investigated by photodegrading tetracycline (TC) under ultraviolet–visible light irradiation. The systematic studies indicate that the obtained V 2 O 5 /NH 2 -MIL-101(Fe) heterojunction photocatalyst possesses superior photocatalytic performance toward TC removal. Furthermore, a Z-scheme photocatalytic degradation mechanism for TC over V 2 O 5 /NH 2 -MIL-101(Fe) composites was proposed. The results show that Z-scheme V 2 O 5 /NH 2 -MIL-101(Fe) heterojunction photocatalyst has potential application in the treatment of TC wastewater. This research will broaden the studies of NH 2 -MIL-101(Fe)-based Z-scheme photocatalysts.
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Catalysts
·
2019
·Vol. 9
·期 11
·906
·
IF 3.444
Jieyang Yang,Zequan Zeng,Zhanggen Huang,Yan Cui
In this work, the activation effect of vacuum thermal treatment on MIL-101(Fe) (MIL: Materials of Institute Lavoisier) was investigated for the first time. It demonstrated that vacuum thermal activation could accelerate the activation of persulfate (PS) by MIL-101(Fe), and the enhancement of the catalytic capacity of MIL-101(Fe) was mainly attributed to the change in the FeII/FeIII mixed-valence center. The results of the SEM and XRD showed that vacuum thermal activation had a negligible effect on the crystal structure and particle morphology of MIL-101(Fe). Meanwhile, the higher temperature of vacuum thermal activation caused a higher relative content ratio of FeII/FeIII. A widely used azo dye, X-3B, was chosen as the probe molecule to investigate the catalytic performance of all samples. The results showed that the activated samples could remove X-3B more effectively, and the sample activated at 150 °C without regeneration could effectively activate PS to remove X-3B for at least 5 runs and approximately 900 min. This work highlights the often-overlooked activation effect of vacuum thermal treatment and provides a simple way to improve the catalytic capacity and reusability of MIL-101(Fe) which is beneficial for the application of MIL-101(Fe)/PS systems in azo dye wastewater treatment.Keywords:vacuum thermal activation;MIL-101(Fe);persulfate;azo dye
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MOLECULES
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2019
·Vol. 24
·期 20
·3718
·
IF 3.06
Mao-Long Chen,Shu-Yang Zhou,Zhou Xu,Li Ding,Yun-Hui Cheng
MIL-100(Fe, Cr) and MIL-101(Cr) were synthesized by the hydrothermal method and applied to the adsorptions of five aromatic amines from aqueous solutions. These three metal-organic frameworks (MOFs) were well characterized by powder X-ray diffraction (PXRD), scanning electron microscope (SEM), transmission electron microscope (TEM), thermogravimetric analysis (TGA) and surface area analysis. The adsorption mechanism of three MOFs and the effects of the structures of MOFs on the adsorption of aromatic amines were discussed. The results show that the cavity system and suitable hydrogen bond acceptor were important factors for the adsorption for five aromatic amines of aniline, 1-naphthalamine, o-toluidine, 2-amino-4-nitrotoluene and 2-nitroaniline: (a) the saturated adsorption capacity of aniline, 1-naphthylamine and o-toluidine on MIL-100(Fe) were 52.0, 53.4 and 49.6 mg/g, respectively, which can be attributed to the intermolecular hydrogen bond interaction and cavity system diffusion. (b) The adsorption capacity of 2-nitroaniline and 2-amino-4-nitrotoluene on MIL-101(Cr) were 54.3 and 25.0 mg/g, respectively, which can be attributed to the more suitable pore size of MIL-101(Cr) than that of MIL-100(Fe, Cr). The MOFs of MIL-100(Fe) and MIL-101(Cr) can be potential materials for removing aromatic amines from aqueous solutions.Keywords:metal-organic framework;adsorption;aromatic amines;aniline;1-naphthalamine;o-toluidine;2-amino-4-nitrotoluene;2-nitroaniline
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APPLIED CATALYSIS A-GENERAL
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2018
·
IF 4.521
Zhenzhen Lin,Mengting Luo,Yindi Zhang,Xiaoxue Wu,Yanghe Fu,Fumin Zhang,Weidong Zhu
Heterogeneous catalytic conversion of biomass-derived methyl levulinate (ML) to γ-valerolactone (GVL) is highly attractive as a sustainable route to mitigating the dependence on nonrenewable fossil resources. However, this route is limited by its low selectivity toward GVL and severe reaction conditions. Here, we present a synergistic catalytic process that offers exclusive GVL selectivity with complete ML conversion under mild conditions (80 °C, 0.5 MPa of H 2 pressure). This is achieved over a dual-functionalized catalyst of Ru nanoparticles (Ru-NPs) and Brønsted acid SO 3 H groups in a Cr-based metal-organic framework (MIL-101). The Ru-NPs served as metal sites for the hydrogenation of ML to methyl-3-hydroxyvalerate (MHV) and the acidic SO 3 H moieties promoted the cyclization of MHV to generate GVL via lactonization. In contrast, GVL production was significantly suppressed over the physically mixed congener (2.0 wt% Ru/MIL-101 + MIL-101-SO 3 H). This result demonstrates an unrivalled advantage of the dual integration of metal/acid sites in a single MOF crystal, and the relative amount of sulfonic acid groups in the catalyst can exert significant influence on the overall catalytic performances. The activation energies for the hydrogenation and lactonization steps with the developed catalyst were 29.5 and 42.1 kJ/mol, respectively, which are much lower than those observed with the traditional 5.0 wt% Ru/AC catalyst.
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CATALYSIS COMMUNICATIONS
·
2015
·
IF 3.699
Yong Liu,Shao-Yi Jia,Song-Hai Wu,Ping-Li Li,Chun-Jiang Liu,Yi-Ming Xu,Feng-Xiang Qin
Highly dispersed metallic nanoparticles immobilizing inside the pores of MIL-101(Cr) were prepared using double solvent method (DSM). The particle size of Au, Ag, Pd, and AuPd NPs were 2.9 ± 0.7 nm, 1.9 ± 0.6 nm, 2.1 ± 0.6 nm and 2.8 ± 0.7 nm, respectively. The catalytic activity determined by the reduction of p-nitrophenol by NaBH 4 to p-aminophenol of Pd and AuPd prepared by DSM is 9.6 and 8.3 times higher than that of Pd and AuPd prepared by conventional impregnation method. The structure and activity of the catalysts prepared by DSM have no significant changes after three cycles.
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TALANTA
·
2017
·
IF 4.162
Li Liang,Xinghua Wang,Ying Sun,Pinyi Ma,Xinpei Li,Huilan Piao,Yanxiao Jiang,Daqian Song
The metal-organic framework (MOF) functionalized magnetic graphene oxide/mesoporous silica composites (Fe 3 O 4 @SiO 2 -GO/MIL-101(Cr)) were synthesized and utilized as magnetic solid-phase extraction (MSPE) adsorbent for the extraction of seven triazine herbicides (terbuthylazine, secbumeton , terbumeton , atraton , atrazine , prometon and trietazine) in rice samples. Several experimental parameters, including type and volume of extraction solvent, amount of MIL-101(Cr), extraction time, volume of desorption solvent and desorption time were investigated and optimized. The limits of detection (LODs) of seven triazine herbicides obtained by using the proposed MSPE method combined with high performance liquid chromatography (HPLC) were in the range of 0.010–0.080 µg kg −1 . The recoveries of the triazine herbicides in spiked rice samples ranged from of 83.9–103.5% with the relative standard deviations lower than 8.7%. The intra and inter-day (n = 6) precisions for all triazine herbicides at the spiked level of 100.0 µg kg −1 were 1.4–5.9% and 2.6–7.8%, respectively.
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高影响因子
TALANTA
·
2017
·
IF 4.162
Xue Qian Tang,Yi Dan Zhang,Zhong Wei Jiang,Dong Mei Wang,Cheng Zhi Huang,Yuan Fang Li
In this work, Fe 3 O 4 and metal–organic framework MIL-101(Fe) composites (Fe 3 O 4 /MIL-101(Fe)) was demonstrated to possess excellent catalytic property to directly catalyze luminol chemiluminescence without extra oxidants. We utilized Fe 3 O 4 /MIL-101(Fe) to develop a ultra-sensitive quantitative analytical method for H 2 O 2 and glucose. The possible mechanism of the chemiluminescence reaction had been investigated. Under optimal conditions, the relative chemiluminescence intensity was linearly proportional to the logarithm of H 2 O 2 concentration in the range of 5–150 nM with a limit of detection of 3.7 nM (signal-to-noise ratio = 3), and glucose could be linearly detected in the range from 5 to 100 nM and the detection limit was 4.9 nM (signal-to-noise ratio = 3). Furthermore, the present approach was successfully applied to quantitative determination of H 2 O 2 in medical disinfectant and glucose in human serum samples.
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高影响因子
NEW JOURNAL OF CHEMISTRY
·
2024
·
IF 2.7
Xia Zhang,Jialong Chu,Yifang Zhang,Fei Li,Chen Wang,Tiemei Li,Jing Fan
A novel microporous iron-based MIL-101@MIL-53 Z-scheme heterojunction photocatalyst was synthesized via a one-pot solvothermal strategy. Composition, structure, morphology and optical properties of the prepared photocatalyst were characterized using XRD, SEM, FT-IR, XPS and UV-vis DRS. The formation mechanism of the iron-based MIL-101@MIL-53 Z-scheme heterojunction was proposed to be attributed to the gradual transformation from MIL-101 to MIL-53. The in situ formation of an iron-based MIL-101@MIL-53 Z-scheme heterojunction facilitated the electron transfer from MIL-53 to MIL-101. Therefore, the separation of photogenerated charge carriers was enhanced. The removal efficiency of 300 mg L−1 tetracycline hydrochloride reached 99.6% in 90 min under simulated solar light irradiation. Radical capturing experiments showed that ˙O2− was the main active substance for the degradation of tetracycline hydrochloride. This work provided strategies for development and application of iron-based MIL-101@MIL-53 Z-scheme heterojunction and efficient treatment of wastewater with a high tetracycline hydrochloride concentration.
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JOURNAL OF MEMBRANE SCIENCE
·
2025
·
IF 9
Tian Zhao,Saiqun Nie,Pengcheng Xiao,Shilin Peng,Jiayao Chen,Jiangrong Yu,Fuli Luo,Yi Chen
The formation of zinc dendrites and by-products significantly affects the cycling performance of aqueous zinc-ion batteries (AZIBs). This study presents the first application of MIL-101(Cr) as a separator material in AZIBs, investigating the impact of various MIL-101(Cr) morphologies in cellulose-based separators on battery performance. The findings demonstrate that separators incorporating spherical MIL-101(Cr) morphology considerably enhance ion conductivity and the transport rate of Zn 2+ ions while effectively inhibiting corrosion reactions and dendrite growth. Notably, the spherical MIL-101(Cr)-based separator exhibited more than double the cycle life of Zn//Zn symmetric cells compared to those made from octahedral and nano-fusion morphologies, achieving over 750 h of operation. Additionally, a Zn//MnO₂ full cells utilizing this separator achieved a remarkable capacity retention of 83.6 % after 400 cycles, with a close-to-100 % Coulombic efficiency. This research underscores the critical role of MIL-101(Cr) morphology in enhancing the performance of AZIB separators, paving the way for innovative designs in future metal-organic framework (MOF)-based separators.
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TALANTA
·
2024
·
IF 5.6
Shengyuan Zhang,Haiyan Li,Dezhi Yang,Yaling Yang
In the present research, Fe-based metal-organic frameworks (MIL-101(Fe)–NH 2 ) nanoparticles were synthesized by simple solvothermal methods and used to assay Cr(Ⅵ). The MIL-101(Fe)–NH 2 performs dual functions: the 2-aminoterephthalic acid (NH 2 -BDC) ligand endows a strong fluorescence emission, and the Fe metal nodes are able to facilitate the oxidation of 3,3′,5,5′- tetramethylbenzidine (TMB) directly, resulting in the generation of oxidized-TMB (ox-TMB). Our research results showed that reducing agents such as ascorbic acid (AA) can collapse the structures of MIL-101(Fe)–NH 2 because of the reduction of Fe 3+ by AA, resulting in release of NH 2 -BDC. In the presence of Cr(Ⅵ), the fluorescence intensity of the MIL-101(Fe)–NH 2 + AA system will be decreased due to the competitive reduction of Fe 3+ and Cr(Ⅵ). Nevertheless, Cr(Ⅵ) can significantly accelerate the oxidation of TMB by MIL-101(Fe)–NH 2 as it boosts the electron transfer rate between Fe 3+ and Fe 2+ . Therefore, a fluorescent/colorimetric dual-mode platform was developed for the detection of Cr(Ⅵ) with an extensive linear range (7.5–750 μg/L and 13.3–1000 μg/L) as well as a remarkably low detection limit (0.99 μg/L and 1.98 μg/L). This MOF with the ability to release ligands not only provides inspiration for the design of new luminescent materials, but also offers a novel and reliable solution for the detection of Cr(Ⅵ).
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INORGANIC CHEMISTRY
·
2025
·
IF 4.7
Miaomiao Chen,Huili Zhao,Han Xue,Yan Liang,Min Ji,Min Wang
B(C6F5)3-based frustrated Lewis pairs (FLPs) have made remarkable progress in metal-free catalytic reduction. However, the high affinity of B(C6F5)3 for oxygen makes it susceptible to irreversible poisoning when exposed to H2O, limiting its widespread application in reductive amination. To overcome the influence of H2O, a hydrophobic catalyst, B(C6F5)3@Rn–1-MIL-101 (n = 3, 5, 7), was developed by confining B(C6F5)3 within the nanocages of metal–organic frameworks (MOFs) modified with alkyl chains. The hydrophobic strength of the catalyst could be adjusted by varying the length of the alkyl chain. At n = 3, the alkyl chain was too short to be hydrophobic, while the excessively long alkyl chain blocked the pore channels and adversely affected the loading of B(C6F5)3 at n = 7. Only the catalyst B(C6F5)3@R4-MIL-101 synthesized at n = 5 could effectively facilitate the reductive amination of aldehydes or ketones with amines in a “wet solvent.” The strategy of combining hydrophobic MOFs with B(C6F5)3 to prepare heterogeneous catalysts for FLP catalysis not only provides a fresh avenue for investigating catalytic systems for reductive amination but also represents an innovative approach to advancing FLP chemistry.
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APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Huiyuan Cheng,Jingwei Hu,Zihan Liu,Guangping Lei,Guojun Xi,Yayun Zhang,Hantao Liu,Xuhuan Guo,Huiyun Ren
Developing novel adsorbents for CO 2 capture and separation offers an efficient approach to relieving global environmental problems. To promote CO 2 capture from flue gas, novel Cr 3 O@MIL-101(Cr) composites was synthesized through packing [Cr 3 O(HCOO) 6 (H 2 O) 3 ]NO 3 into MIL-101(Cr) cages. The resultant composite Cr 3 O@MIL-101(Cr) presents higher CO 2 uptakes at lower pressure ranges, benefiting from the increased content of unsaturated Cr(III) ions and micropores relative to MIL-101(Cr). Meanwhile, IAST selectivity for CO 2 /N 2 mixture reached 50.2 under standard temperature and pressure, outperforming most of the reported materials. Further GCMC simulations reveal that the synergistic effect of [Cr 3 O(HCOO) 6 (H 2 O) 3 ] + , NO 3 − and MIL-101 (Cr) could effectively facilitate the interactions with CO 2 molecules and hinder N 2 molecules from approaching the optimal adsorption sites. Thus the [Cr 3 O(HCOO) 6 (H 2 O) 3 ]NO 3 encapsulated MIL-101(Cr) can be recommended as a promising adsorbent for superior CO 2 /N 2 separation.
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