Surfaces and Interfaces
·
2024
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IF 5.7
Qian Cheng,Xiaohan Liu,Chuhan Huang,Hongman Sun,Fazle Subhan,Xinyi Zhou,Yuankai Liu,JiaHui Yang,Qi Li,Youhe Wang,Zifeng Yan
Recently, there has been a growing interest in the fundamental understanding of the mechanism of how MIL-101(Fe)/g-C 3 N 4 heterojunctions facilitate the occurrence of photocatalytic nitrogen fixation reactions, especially the electron transfer mechanism has attained increasing attention in photocatalysis. Herein, we implemented a "triple win scenario" strategy to fabricate the S-scheme MIL-101(Fe)/g-C 3 N 4 heterojunction through a straightforward solvothermal process. The MC-6 heterojunction minimizes the recombination of photogenerated carriers, enhances light utilization efficiency, and activates the N≡N bond, thus boosting photocatalytic nitrogen fixation efficiency. The transition metal iron activates the N≡N bond, while S-scheme heterojunctions reduce the photogenerated carrier recombination. In addition, the decrease in band gap (E g ) leads to an increase in visible light utilization efficiency. ISIXPS proved the mechanism of interelectron transfer of MIL-101(Fe)/g-C 3 N 4 heterojunction under illumination. Upon the creation of the heterojunction, electrons migrate from g-C 3 N 4 to MIL-101(Fe), establishing an inherent electric field due to the disparate Fermi levels between the two materials. The electrons (e - ) on the g-C 3 N 4 CB with a more negative reduction potential and the holes ( h + ) on the MIL-101(Fe) VB are retained, which increased the redox capacity to a great extent required for the reduction of N 2 to NH 3 . The ammonia production efficiency of MC-6 photocatalyst was 160 µmol g cat -1 h -1 , representing an 8-fold and 2.8-fold improvement over pristine g-C 3 N 4 (20 µmol g cat -1 h -1 ) and MIL-101(Fe) (57 µmol g cat -1 h -1 ), respectively.
研究领域:
材料科学
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环境科学
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化学
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DOI
高影响因子
ChemElectroChem
·
2018
·Vol. 5
·期 19
·2893-2901
·
IF 4.446
Jianxia Gu,Xiangdang Yin,Xiangjie Bo,Liping Guo
Graphical With a sense of selectivity : the metal-organic framework/reduced graphene oxide composite MIL-101(Cr)/rGO is prepared via a simple hydrothermal method. The electrochemical sensor based on the composite shows low detection limits and wide linearity ranges for the determination of metronidazole, Cd 2+ and Pb 2+ , and shows excellent selectivity, reproducibility and stability. In this work, a Cr-based MOF (MIL-101(Cr))/reduced grapheme oxide(rGO) electrocatalyst was prepared through a one-pot hydrothermal method. The obtained composite was characterized via scanning electron microscopy, transmission electron microscopy, X-ray diffraction and other standard techniques. Electrochemical methods were adopted to study the electrocatalytic ability of the composite. The results imply that, compared to the single components, it exhibits higher electrocatalytic activity for the reduction of metronidazole and stripping of Cd 2+ and Pb 2+ . Optimizing the ratio of MIL-101(Cr) and rGO, an electrochemical sensor was prepared using MIL-101(Cr)/rGO-20 and used for detection of metronidazole, Cd 2+ and Pb 2+ , respectively. The linear range for metronidazole can be divided in two parts, i. e. from 0.5 to 200 μM and from 200 to 900 μM. The limit of detection is 0.24 μM (S/N=3, n=10). Likewise, it also exhibits a wide linear range from 0.05 to 6.0 μM for the detection of Cd 2+ and Pb 2+ . The corresponding detection limits are found to be 5.2 nM and 3.0 nM (S/N=3, n=10), respectively. The proposed sensor also possesses superb selectivity, reproducibility, stability and can be applied to detect real samples with desired recovery rates. In addition, the possible reduction mechanism of metronidazole and adsorption mechanism of Cd 2+ and Pb 2+ were further discussed simply in this work.
研究领域:
材料科学
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电化学
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分析化学
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DOI
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2022
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IF 5.518
Tuckyun Cheang,Wenbin Huang,Weiping Li,Siyu Ren,Haihui Wen,Ting Zhou,Yongcheng Zhang,Weihao Lin
Exploring efficient adsorbent for heavy metals remediation from wastewater and contaminated soil is a pursuing issue. Robust functionalized metal-organic frameworks (MOFs) represent one of burgeoning scavengers because of their tunable structural topology , designable functionalities and extraordinary affinity for heavy metal ions . In this present work, we report a facile and versatile strategy to synthesize a series of carboxyl-functionalized MIL-101(Fe) derivatives by microwaving a solution of organic ligands with varying carboxyl number and Fe 3+ ions. The resulting MIL-101(Fe) derivatives were characterized using various techniques including scanning electron microscope (SEM), powder X-ray diffraction, Fourier transformed infrared, Brunauer–Emmett–Teller specific surface area and X-ray photoelectron spectroscopy. The intrinsically carboxyl-rich characteristic and large surface area of MIL-101-(COOH) 2 afford fast adsorption kinetics (< 15 min) and high saturation capacity (467.6 mg/g) for Pb(II). Strikingly, it can efficiently capture Pb(II) possessing impressive adsorption efficiencies (> 90%) over a wide pH range of 4.5–11.0. Moreover, the resulting MIL-101-(COOH) 2 simultaneously exhibited high affinity toward different types of heavy metal ions, including borderline Lewis acid (Pb(II), Cu(II) and Ni(II)), soft Lewis acid (Cd(II) and Hg(II)) and hard Lewis acid (Eu(III) and Cr(III)). Such impressive treatment for Pb(II)-contaminated lead-acid battery industrial wastewater (more than 96.7%) can be attributed to the coordination arising from abundant carboxyl groups in the pores of MIL architecture with target heavy metal ions. Significantly, these findings validate the exceptional potential of carboxyl-functionalized MIL-101(Fe) derivatives in the application of heavy metal ions remediation.
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
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2024
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IF 8.1
Yanyan Xing,Mengke Tian,Ruoman Ji,Ting Wang,Xiaohong Hou
The immobilization of bovine serum albumin (BSA) with high efficiency, good reproducibility and stability for chiral separation has attracted much attention in the medicinal field. BSA was immobilized into MIL-101(Cr) by three ways for efficient chiral separation in this research. MIL-101(Cr)@BSA was firstly prepared by adsorption, NH 2 -MIL-101(Cr) ⊂ BSA by direct bonding, and NH 2 -MIL-101(Cr) ⊂ Glu ⊂ BSA by glutaraldehyde crosslinking bonding. Compared to the other two materials, NH 2 -MIL-101(Cr) ⊂ BSA as a new enantioselective separator, with the most BSA loading rate of 437.6 mg g −1 exhibited excellent chiral separation performances and succeeded in realizing a complete chiral separation of racemic 1–phenylethanol within 14 s. It was found that the NH 2 -MIL-101(Cr) ⊂ BSA was more strongly bound to R -1-phenylethanol and the ee value could reach 100 % when the material was added in three batches. The different interactions between BSA and racemates mainly including hydrogen bonding, hydrophobic interaction and π-π interaction were revealed by the molecular docking studies, especially hydrogen bonding, accounting for the observed selective chiral recognition capacity of racemic 1–phenylethanol of NH 2 -MIL-101(Cr) ⊂ BSA. Moreover, both of NH 2 -MIL-101(Cr) ⊂ BSA and NH 2 -MIL-101(Cr) ⊂ Glu ⊂ BSA showed excellent stability and reusability. This combination of theory and experiment provided a clearer basis for other researchers to have different requirements for protein immobilization, and provided new ideas and methods for the development of chiral selectors.
研究领域:
生物化学
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材料科学
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医药工程
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DOI
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2023
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IF 5.2
Shiyu Zhang,Qiuyu Qiao,Yangfeng Wen,Kena Ren,Xiaoyu Ma,Haisheng Tao
A novel composite of acetic acid-modulated AC-NH 2 -MIL-101(Fe) was prepared by mild chemistry . The catalyst was characterized by scanning electron microscopy (SEM), X-ray diffraction (XRD), thermogravimetric analysis (TGA), Fourier transform infrared spectroscopy (FTIR), Brunaure-Emmett-Teller (BET) and X-ray photoelectron spectroscopy (XPS). Acetic acid can control the crystal size, so that the catalyst had a large specific surface area (99.35 m 2 ·g −1 ) and pore size (0.13 cm 3 ·g −1 ), the adsorption amount of Rhodamine B (RhB) up to 446.965 mg·g −1 , after the addition of peroxydisulfate (PDS), the catalytic degradation efficiency of RhB was as high as 99.7%. Electronic paramagnetic resonance spectrometer (EPR) and quenching experiments showed that the catalytic process may involve radical (·OH, SO 4 -· and O 2 ·- ) and non-radical ( 1 O 2 ) processes, in which the contribution of 1 O 2 to degradation reached 63.55% and played a major role.
研究领域:
材料科学
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环境科学
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产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Ruimeng Wang,Xinqi Luan,Jingyu Bao,Yaseen Muhammad,Syed Jalil Shah,Guanchen Wang,Jing Li,Guoyou Lin,Hongbing Ji,Zhenxia Zhao
High capacity adsorption of volatile organic compounds (VOCs) in high humidity environment is a crux but challenge for atmospheric VOCs governance. In this work, tubular carbonized N-doped polymers (TCNP) were implanted into MIL-101 via N-Cr-O interface self-assembly, enabling high adsorption for vapor toluene in high humidity. Through mechanical ball milling and carbonization, Cr ions were preloaded on TCNP to form highly dispersed 3–5 nm Cr-N crystallite as anchors for growing MIL-101(Cr/Cu). Newly constructed smaller micropores of 6.8 Å with aromatic rings/N sites at the interface and doped Cu ions in MOF framework synergistically enhanced π-π conjugation and electrostatic interaction for C 7 H 8 molecules. This endowed [TCNP 5 /MIL(Cr/Cu)] N-Cr 2.9 times higher toluene uptake (6.34 mmol/g) at low vapor pressure ( P / P 0 = 0.02) and 1.9 times diffusivity under high humidity (60% RH) than that of MIL-101(Cr) at 298 K. The adsorption breakthrough curves for vaporous toluene showed that TCNP@MIL-101(Cr/Cu) exhibited outstandingly higher adsorption equilibrium capacity (2.7 mmol/g) under 80% RH, corresponding to approximately 2–10 times than those of reported state-of-the-art adsorbents under similar conditions. This study provided a novel interface construction strategy for hydrophobic MOF composites, which supplied deeper understanding for VOCs adsorption and promoted MOFs practical application in VOCs capture under humid environment.
研究领域:
材料科学
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环境科学
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产品关联
DOI
高影响因子
ACS ES&T Engineering
·
2023
·
IF 7.1
Junna Yan,Mengyu Ma,Keyi Liu,Yang Bao,Feihu Li
Efficient removal and recovery of phosphorus (P) from wastewater is critical for addressing both phosphate rock depletion and eutrophication-related deterioration of surface water quality. Herein, we present a promising platform approach integrating cerium-doped NH2-MIL-101(Fe) with melamine sponge (MS) scaffolds for rapid and high-efficiency recovery of P from wastewater. The as-prepared MIL-101@sponge composites (denoted as MIL-101@CS, MIL-101@PVDF, and MIL-101@SDBS, respectively) are featured by flexibility and stability according to many characterization techniques. Batch adsorption of P over these composite adsorbents indicates that these MIL-101@sponge composites exhibit a maximum adsorption capacity (e.g., 253.66 mg g–1 for MIL-101@CS) at the optimum pH of 6.0 and that adsorption equilibrium can be attained within 150 min and well described by the pseudo-second-order kinetic model. In addition, these composites show a high selectivity for P over carbonate and other common monovalent anions under environmentally relevant conditions. The results of desorption and recycling tests indicate that MIL-101@CS retains good adsorption and desorption efficiency even in a much short operating time (i.e., 5 min), which allows such a composite to be applied in enriching and recovering P efficiently from wastewater via a rapid adsorption/desorption operation. Moreover, the high feasibility of MIL-101@CS in actual scenarios was validated by efficiently enriching the P from a sludge dewatering liquid. Furthermore, the main mechanisms for P adsorption are elucidated from various microstructural characterizations. Overall, this work presents a strategy of integrating MIL-101 with sponge scaffolds for rapidly and efficiently recovering P from wastewater, which may be potentially extended to the recovery of other value-added elements of interest from waste streams.
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2023
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IF 5.2
Guang-Yu Cui,Wei Zhang,Ji-Min Yang
Metal−organic framework (MOF)@graphene oxide (GO) composite materials possess the advantages of both GO and MOFs, and thus, they can be employed as effective dye adsorbents. This paper proposes a simple strategy for the preparation of MIL-101 @GO composite materials to effectively adsorb anionic dyes (Congo red, o-cresolsulfonphthalein, methyl orange, and acid chrome blue K) by adding GO to MIL-101 to form a nano-packed structure. The maximum adsorption uptakes of MIL-101 @GO were 2734.9, 484.5, and 1762.8 mg g –1 for Congo red, o-cresolsulfonphthalein, and methyl orange, respectively. These values significantly exceed the corresponding values of the original MIL-101 because of additional factors that promoted adsorption, namely hydrogen bonding and the presence of agglomerate pores. Only the maximum adsorption uptake for acid chrome blue K was lower than that of MIL-101, because of steric hindrance . Our analysis showed that the adsorption behavior of MIL-101 @GO toward Congo red, o-cresolsulfonphthalein, and methyl orange is governed by a synergistic interplay of hydrogen bonding, electrostatic interactions, π–π interactions, the adsorption space, and agglomerate pores in the composite, whereas the adsorption behavior toward acid chrome blue K is mainly limited by steric hindrance. Understanding these interactions may contribute to the development of improved sustainable composite adsorbents.
研究领域:
材料科学
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环境科学
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产品关联
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2015
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IF 4.529
Xubiao Luo,Tingting Shen,Lin Ding,Weiping Zhong,Jianfeng Luo,Shenglian Luo
A novel thymine-functionalized MIL-101 (MIL-101-Thymine) material was synthesized using a post-synthesis method to remove mercury at a high efficiency. MIL-101-Thymine was successfully prepared in this work and was confirmed by several characterization methods, such as 13 C nuclear magnetic resonance, X-ray diffraction, and infrared spectroscopy. The Hg 2+ adsorption agreed well with the Langmuir model, and the maximum adsorption capacity was 51.27 mg/g. The adsorption rate fit with the pseudo-second-order kinetic model. Furthermore, MIL-101-Thymine exhibited excellent selectivity towards Hg 2+ over other cations, and the maximum value of the selective coefficient reached 947.34; this result is very likely due to the highly selective interactions of T-Hg 2+ –T in MIL-101-Thymine. The result of X-ray photoelectron spectroscopy also showed that Hg 2+ was coordinated with the N of thymine in MIL-101-Thymine. Moreover, the results of the thermogravimetric analysis and adsorption experiments showed that the Hg atom was two-coordinated with the thymine group. MIL-101-Thymine was used to remove trace Hg 2+ in real water samples, and satisfactory recoveries were obtained.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ENERGY & FUELS
·
2017
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IF 3.091
Xuejiao Sun,Daofei Lv,Yongwei Chen,Ying Wu,Qihui Wu,Qibin Xia,Zhong Li
Chromium-based MIL-101 and graphite oxide (GO) composite (MIL-101@GO) was synthesized and applied for adsorption performances toward a series of aromatics (benzene, toluene, and ethylbenzene). Desorption activation energies of aromatics on this composite were evaluated based on temperature-programmed desorption (TPD) experiments. The results indicated that the aromatic uptakes on the composite increase with the carbon number at low pressure. In contrast, at high pressure, their adsorption capacities exhibit an opposite trend. The composite possesses high uptakes of the aromatics, which are approximately 1.8–6.0 times higher compared with conventional adsorbents. The desorption activation energies of the aromatics increase with the carbon number of aromatics. Additionally, the adsorption of ethylbenzene on the composite is highly reversible. More importantly, the MIL-101@GO composite exhibits enhanced thermal conductivity up to 0.369 W/mK at 303 K. The MIL-101@GO composite with high adsorption capacity, enhanced thermal conductivity, and efficient recyclability provided a promising candidate for practical applications in field of volatile organic compounds adsorption.
研究领域:
材料科学
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环境科学
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产品关联
DOI
高影响因子
CATALYSIS LETTERS
·
2021
·Vol. 151
·期 9
·2560-2569
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IF 3.186
Han Jishu,Wang Ying,Liu Ying,Bai Jiayu,Zhao Ruiyang,Wang Lei
In this paper, novel CdSe/NH 2 -MIL-101(Cr) nanocomposites for photocatalytic hydrogen production were synthesized. When the prepared NH 2 -MIL-101(Cr) MOFs were modified with CdSe QDs, the photocatalytic hydrogen production amount was significantly increased and reached to 17,664 μmol g −1 in 7 h. The formation of CdSe/NH 2 -MIL-101(Cr) nanocomposites enhanced the light absorption intensity, broadened the visible light absorption range, promoted the transfer of photogenerated electrons and inhibited the recombination of photogenerated electron–hole pairs, then effectively improved the photocatalytic hydrogen production performance. In addition, the CdSe/NH 2 -MIL-101(Cr) nanocomposites exhibited high cycle stability, which was beneficial to the practical application in photocatalytic hydrogen production. Graphic Abstract
研究领域:
材料科学
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环境科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2019
·
IF 14.229
Quan Huo,Xiaoran Qi,Jianshu Li,Gongquan Liu,Yao Ning,Xubiao Zhang,Boyu Zhang,Yanfei Fu,Suyan Liu
A series of direct Z-scheme α-Fe 2 O 3 /MIL-101(Cr) hybrids were successfully prepared through a facile hydrothermal method in this work. And, the materials were characterized by some technologies including X-ray diffraction (XRD), scanning electron microscopy (SEM), energy-dispersive X-ray spectroscopy (EDX), transmission electron microscopy (TEM), Fourier-transform infrared spectroscopy (FT-IR), X-ray photoelectron spectroscopy (XPS), N 2 adsorption-desorption, photoluminescence (PL) spectroscopy, Ultraviolet-visible (UV–vis) diffuse reflectance spectroscopy (DRS) and electron spin resonance (ESR). The photocatalytic activities of the hybrids were evaluated by degradation of carbamazepine (CBZ) under visible light irradiation. It is found that 100% of CBZ was able to be removed after 180 min irradiation over the optimum α-Fe 2 O 3 (0.3)/MIL-101(Cr) hybrid. The superior activity was engendered from good textural properties and the formation of a direct Z-scheme heterojunction in the hybrid. The decomposition process of CBZ and the formation of intermediate products were analyzed through liquid chromatography-tandem mass spectrometry (LC–MS) and a possible photodegradation pathway of the CBZ was proposed. Also, the possible mechanism for the photodegradation process was provided to illustrate the excellent performance. The work has paved a new way for the application of MOF materials in the design of efficient Z-scheme system for organic pollution degradation in wastewater.
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
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