PHYSICAL CHEMISTRY CHEMICAL PHYSICS
·
2025
·Vol. 27
·期 8
·4278-4289
·
IF 2.9
Ziyu Li,Mei Li,Rongsheng Xu,Zhiliang Jin
The electron transfer rate in photocatalysts is one of the factors determining their hydrogen production activity. In this work, NH2-MIL-88B(Fe) (NFM) was synthesized using a one-step hydrothermal synthesis method and NFM/GDY-25 (NFMG-25) was successfully synthesized by loading graphdiyne (GDY) onto the surface of NFM. The hydrogen production performance and the mechanism of the prepared photocatalysts were systematically investigated using XRD, SEM, FT-IR, XPS, UV-Vis, PL and photoelectrochemical tests. The results showed that the hydrogen production of NFMG-25 reached 61.7 μmol in 5 hours. Photoelectrochemical and Mott–Schottky tests demonstrated that the composite catalyst exhibited high photogenerated carrier separation efficiency and single catalysts were n-type semiconductors. The conduction bands of NFM and GDY were −0.36 V and −0.56 V, respectively, while the valence bands were 1.90 V and 1.12 V. NFM acted as an electron acceptor and donor, which accelerated the transfer of the electrons, and enhanced the photocatalytic hydrogen production efficiency of the composite system. This study provides an effective method for using NFM in photocatalytic hydrogen production.
研究领域:
材料科学
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能源科学
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产品关联
DOI
PubMed
高影响因子
Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Shusu Shen,Honglin Li,Yang Shen,Renbi Bai,Ganwei Zhang
Metal organic frameworks (MOFs) possess excellent post-modification characteristics, high specific surface area, diversity of skeleton composition and pore tunability, have been increasingly applied in membrane modifications. In this work, NH 2 -MIL-88B(Fe) (NM88B) was first fixed onto polyvinylidene fluoride (PVDF) membrane by polyethyleneimine (PEI) through a vacuum-assisted self-assembly process, and the deposited NM88B was subsequently grafted with perfluoroalkyl polyethoxyacetic acid (FPEOAA) via a condensation reaction to realize the surface modifications. The modified membranes (named as N1F x ) showed improved hydrophilicity and underwater-oleophobicity. In addition, very high pure water flux (up to 9403 L‧m −2 ‧h −1 ) was obtained for the N1F x membranes due to the high porosity of introduced NM88B. In the dead-end filtration experiments of n -hexadecane-water emulsion, the optimum membrane N1F20 showed a good oil rejection rate (98.3%) and high permeation flux (667 L‧m −2 ‧h −1 ) which is approximately seven times of the pure PVDF membrane, indicating that the surface-modified membranes had excellent permeability and good separation performance. Even after four filtration cycles of oil-water emulsion, the rejection rate maintained higher than 97%, showing good reusability. Furthermore, the study found that N1F20 had certain acid and alkaline resistance and great potential for engineering applications.
研究领域:
材料科学
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环境工程
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产品关联
DOI
高影响因子
CRYSTENGCOMM
·
2025
·Vol. 27
·期 5
·678-686
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IF 2.6
Dongling Xie,Jianan Wang,Bo Huang,Yiyi Yang,Dunmin Lin,Chenggang Xu,Fengyu Xie
Rational design of viable routes to develop affordable and efficient oxygen evolution reaction (OER) catalysts is essential for advancing electrochemical water splitting, yet significant challenges remain, particularly in seawater. Here, we propose a ligand defect engineering strategy to modify the electronic structure of NH2-MIL-88B(Fe) using a monodentate ligand (acetic acid, AcOH), inducing ligand vacancies in NH2-MIL-88B(Fe) for oxygen evolution in an alkaline seawater electrolyte, thereby improving the performance of the electrocatalysts. The resulting defective MOFs (denoted as NH2-MIL-88B(Fe)-x) exhibited exceptionally high catalytic activity for OER, requiring low overpotentials of 313 and 329 mV at a current density of 100 mA cm−2 in 1 M KOH and simulated seawater (1 M KOH + 0.5 M NaCl) solutions, respectively. Experimental analyses revealed that the introduction of AcOH can modulate the d-band center of active sites in NH2-MIL-88B(Fe)-x and play a critical role in alleviating chloride ion (Cl−) corrosion, thereby enhancing catalytic stability in seawater. When directly used as an OER catalyst in an alkaline electrolyte, wind and solar power were harnessed to operate the NH2-MIL-88B(Fe)-x || Pt/C configuration to drive the electrolytic water reaction. Thus, the ligand defect strategy can be employed to design and prepare high-performance OER electrocatalysts, particularly for generating H2 through water electrolysis powered by renewable energy sources.
研究领域:
材料科学
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电化学
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能源工程
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产品关联
DOI
高影响因子
APPLIED ORGANOMETALLIC CHEMISTRY
·
2018
·Vol. 33
·期 1
·e4580
·
IF 3.581
Hongxu Guo,Baitong Niu,Xuemin Wu,Yi Zhang,Shaoming Ying
A nanostructured organic–inorganic framework, hexagonal NH 2 -MIL-88B, has been prepared through a facile one-pot reflux reaction and then it was characterized using various techniques. The as-prepared sample with high specific surface area (414 m 2 g −1 ) showed excellent adsorption for 2,4,6-trinitrophenol (TNP) in the liquid phase. Detailed studies of the adsorption kinetics, adsorption mechanism, adsorption isotherm, activation energy and various thermodynamic parameters were conducted. The adsorption mechanism of NH 2 -MIL-88B for TNP may be ascribed to hydrogen bond interaction, and the complexation between ─OH in TNP and unsaturated Fe(III) on the surface of NH 2 -MIL-88B. The maximum adsorption capacity of NH 2 -MIL-88B for TNP based on the Langmuir isotherm was 163.66 mg g −1 . The as-prepared NH 2 -MIL-88B adsorbent seems to be a promising material in practice for TNP removal from aqueous solution.
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
NANO
·
2021
·
IF 1.556
Jungang Yi,Kun Wu,Huadong Wu,Jia Guo,Linfeng Zhang,Hao Li,Jianding Li
The presence of the antibiotics in the wastewater has posed a huge risk to aquatic life and human health. It is a great significance to develop an effective technology to treat the antibiotics-containing wastewater. In this study, a series of g-C 3 N 4 /NH 2 -MIL-88B(Fe) composite photocatalysts are synthesized through a simple one-step method. The structure and optical properties of prepared photocatalysts are detected by X-ray diffraction (XRD), field emission scanning electron microscope (FESEM), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), UV–Vis absorption spectra (UV–Vis DRS), photoluminescence (PL) spectroscopy and transient photocurrent techniques, respectively. FESEM and TEM show that MOF is uniformly dispersed in petaloid g-C 3 N 4 . The uniform dispersion of Fe-MOFs in the heterojunction composites increases the specific surface area ( S BET ) of g-C 3 N 4 , which results in a great adsorption property for the nanocomposite. The capture experiment shows that • O 2 − and h + are the main active substances in ciprofloxacin (CIP) degradation. These prepared composite photocatalysts exhibit excellent CIP photodegradation activity under visibly light irradiation with an apparent rate constant of 0.0127 min − 1 (3.74 times as the rate of single component). The remarkable catalytic performance can be ascribed to the fact that the g-C 3 N 4 /NH 2 -MIL-88B(Fe) heterojunction inhibits the recombination of photoinduced electron–hole pairs and improved the visible light absorption.
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
JOURNAL OF MEMBRANE SCIENCE
·
2021
·
IF 8.742
Yixuan Gao,Siming Yan,Yi He,Yi Fan,Liyun Zhang,Jing Ma,Ruitong Hou,Li Chen,Jingyu Chen
Herein, a novel membrane with polyacrylic acid (PAA), NH 2 -MIL-88B(Fe) (NM88B), and graphene oxide (GO) was fabricated via a simple vacuum filter method equipped with the nylon membrane substrate. The composite membrane (PAA@NM88B/GO membrane) retained the laminated structure of GO, and PAA@NM88B was used as the photo-Fenton catalytic nano-filler to intercalate GO. Through a series of material characterization and membrane separation performance tests, the results showed that by introducing porous NM88B and PAA cross-linking modification, PAA@NM88B/GO membrane had excellent hydrophilicity, water flux and dye rejection performance. The flux of the PAA@NM88B/GO membrane was 68.21 L m −2 h −1 bar −1 , which is about 15 times higher than that of GO membrane. In addition, the composite membrane had a high rejection (over 97%) for methylene blue (MB), crystal violet (CV) and Congo red (CR). More importantly, PAA@NM88B/GO membrane can also be used to degrade textile wastewater in real life. The membrane can be used as a catalyst to degrade contaminants, and had a high removal of MB in 40 min (98.79%) under the synergistic effect of membrane adsorption and photocatalysis . Therefore, the results indicated that this new type of PAA@NM88B/GO membrane had potential applications in water purification and actual textile wastewater treatment .
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
JOURNAL OF MEMBRANE SCIENCE
·
2019
·
IF 7.015
Atian Xie,Jiuyun Cui,Jin Yang,Yangyang Chen,Jihui Lang,Chunxiang Li,Yongsheng Yan,Jiangdong Dai
Membrane fouling is one of the major blockages toward the further sustained development of membrane technology . In this work, PVDF/NH 2 -MIL-88B(Fe) (PVDF/NM88B) membranes were prepared for the first time via one-step simple non-solvent induced phase conversion method. The PVDF/NM88B membrane shows an excellent separation performance (above 99.4%) and permeation flux (340–1970 L m −2 h −1 bar −1 ) towards different oil/water emulsions. Moreover, PVDF/NM88B membrane exhibits excellent antifouling performance with flux recovery ratio of almost 100% attributing to hydrophilicity and high photo-Fenton activity of NM88B. In addition, the membrane with good mechanical properties and recyclability shows great application potential in wastewater treatment . This work may shine a new light on the promising photo-Fenton self-cleaning prospect of Fe-based MOFs in constructing antifouling membranes for wastewater remediation and potential applications.
研究领域:
材料科学
·
环境科学
✓ 已验证
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2019
·
IF 14.229
Ranran Yuan,Cailiang Yue,Jinli Qiu,Fuqiang Liu,Aimin Li
TiO 2 @NH 2 -MIL-88B(Fe) heterostructures (TMFe-x) were successfully synthesized and used in an efficient sunlight-driven reduction towards Cr(VI) in a neutral aqueous media. Further, the prepared TMFe-x heterostructures exhibited higher photocatalytic activity when compared with those exhibited by pure TiO 2 and NH 2 -MIL-88B(Fe) under simulated sunlight irradiation. The optical TiO 2 modification content was determined to be 10 wt.% (TMFe-b), with 98.6% Cr(VI) being converted to Cr(III) within 35 min using ammonium oxalate as the hole scavenger at pH = 7. In neutral conditions, the kinetic rate constant (0.0878 min −1 ) was five times larger than the published values. Additionally, the photocatalytic performance of TMFe-b was maintained and Fe leaching was observed to be negligible after the completion of four reaction cycles. The superior photocatalytic property can be attributed to the high photoelectron-hole separation and migration efficiency. Subsequently, TMFe-b achieved Cr(VI) reduction under neutral conditions by capturing hydrogen from the water molecules or the hole scavengers. The photoelectrons and superoxide radicals were the main active species. Furthermore, TMFe-b was able to efficiently eliminate various pollutants through photocatalytic oxidation and reduction. This study suggests a novel strategy for the preparation of environmentally stable and efficient MOF-based photocatalysts to efficiently eliminate various pollutants. Further, there is a huge potential for the practical application of this technology to water purification .
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
NEW JOURNAL OF CHEMISTRY
·
2022
·Vol. 46
·期 36
·17438-17455
·
IF 3.925
Qingcan Xiang,Zongxue Yu,Xuyang Li,Pingquan Wang,Niandan He,Yao Pang,Qiuxiang Wang,Yucheng Liu
A g-C3N4/NH2-MIL-88B(Fe)/CD@GO membrane (M2) was prepared by a simple vacuum filtration method. By embedding a Z-scheme heterojunction composite photocatalyst into graphene oxide (GO) nanosheets, not only can the water molecule transport channel be regulated, but the membrane can also be endowed with photocatalytic activity and membrane fouling is effectively alleviated. The pure water permeation flux of M2 (253.26 L m−2 h−1 bar−1) was 13 times that of the original GO membrane (18.83 L m−2 h−1 bar−1). What's more, even after 10 cycles, M2 still maintains excellent separation efficiency and flux. After six cycles, the rejection of Congo Red (CR), Malachite Green (MG) and Rhodamine B (RhB) by M2 was over 95%. At the same time, under the conditions of an extreme pH value and high salt concentration, the rejection of dye remained at the original level after six cycles. Therefore, the novel photocatalytic membrane has excellent separation performance, stability and photocatalytic activity, and can be used as a potential membrane for wastewater purification and environmental protection.
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
JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
·
2022
·Vol. 33
·期 17
·14228-14239
·
IF 2.779
Liu Jieling,Yang Jiaji,An Shuyue,Wen Meiqi,Wang Xian,Gong Rongzhou,Nie Yan
Metal-organic framework (MOF) crystals have promising applications in a number of different fields, but the growth of MOF crystals with controllable morphology and high uniformity remains a major challenge. By taking the advantage of the synergistic effects of water molecules in the mixed solvent and polyvinylpyrrolidone (PVP) surfactants, this work demonstrates an approach for the preparation of NH 2 -MIL-88B(Fe) MOF crystals with both highly customizable size and aspect ratios and high uniformity. The effects of the concentration of water in the mixed solvent and the amount of PVP surfactants on the morphology and size of the MOF crystals were investigated. The morphology and crystalline properties were characterized by scanning electron microscopy and X-ray diffraction techniques. The data showed that through controlling the concentration of water in the solvent and the amount of the PVP surfactant, the size of the MOF crystals can be tuned rather widely, over 344–5.14 μm, while the aspect ratio of the crystals can be varied widely over 1.0–7.1. Possible mechanisms for such high tunability were discussed. As an example of potential applications, the complex permeability and permittivity of MOF-derived composites (25 wt%) were measured over a wide frequency range of 2–18 GHz. The parameters were then used to evaluate the potential for electromagnetic wave absorption. The results indicate that the composite with a thickness of only 1.2 mm exhibits a “− 10 dB” absorption bandwidth of 4.1 GHz and a minimum reflection of − 20 dB. Such bandwidth and reflection properties provide inspiration for future design of lightweight, broadband electromagnetic wave absorbers from the perspective of fine morphology control.
研究领域:
材料科学
·
化学工程
·
电磁学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Yuexin Wang,Zhen Zhong,Yaseen Muhammad,Hui He,Zhongxing Zhao,Shuangxi Nie,Zhenxia Zhao
Engineering of monodentate ligands induced defects was proposed to modify NH 2 -MIL-88B(Fe) in order to promote its synergetic photo-Fenton catalytic degradation performance for acetamiprid (ACTM) as model neonicotinoid insecticides. Three monodentate ligands with different coordination groups (benzoic acid, pyrrole and pyrrole-2-carboxylic acid) were applied to in-situ induce ligand vacancies on NH 2 -MIL-88B(Fe). Effect of defect coordination mode on its photo-Fenton catalytic performance was investigated through the ACTM degradation reaction. Ligand defects on NH 2 -MIL-88B(Fe) would generate three merits: (1) it can modulate surface properties to enhance adsorption affinity towards ACTM; (2) it can introduce large amount of monodentate ligands and ligand vacancies in MOFs to promote light absorption and electron-hole separation capacity for photo-catalysis; (3) it can increase the amount of Fe Lewis acid sites to improve redox capacity of Fe 2+ /Fe 3+ for Fenton-catalysis. In this work, Pyrrole-2-carboxylic acid (Pac) was proved to introduce more monodentate ligands in MOFs and generate more ligand vacancies as well. As a result, ACTM can be easily captured by defective NH 2 -MIL-88B(Fe) and degraded by in-situ triggered oxidative reaction through the synergistic “photo-Fenton catalysis”. Performance measurements showed that Pac-MIL88(Fe) achieved 7.3 times higher adsorption rate and 5.5 times higher catalytic rate for ACTM than that of pristine MIL88(Fe). Moreover, total organic carbon (TOC) conversion reached 97.0% within only 90 min using Pac-MIL88(Fe) as photo-Fenton catalyst, showing 1.7 times higher than pristine MIL88(Fe). Thus, the in-situ fabrication of ligand defect-containing MIL88(Fe) can be foreseen of potential for designing new MOFs for wider practical applications.
研究领域:
环境科学
·
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Xiaolong Hu,Jingyu Bao,Daiwen Chen,Syed Jalil Shah,Sidra Subhan,Wenxue Gong,Wenyuan Li,Xinqi Luan,Zhongxing Zhao :,Zhenxia Zhao
In the photo-Fenton reactions, fast recombination of photoinduced electrons and holes in Fe-based metal–organic frameworks (Fe-MOFs) slows Fe(III)/Fe(II) cycle, which remains big challenge that significantly retards the overall process. Herein, NH 2 -MIL-88B(Fe) (NM88) was modified with 3,5-diaminobenzoic acid (DB) and TPB-DMTP-COF (COF-OMe) to in situ construct NM88(DB) 0.85 /COF-OMe composite that could strongly harvest the visible light for photo-Fenton degradation of sulfamerazine (SMR). With the addition of DB, electron-donating effect of NM88 was strengthened, which then promoted amino groups to react with aldehyde groups (Schiff-base), and thus highly facilitated the interfacial contact between NM88 and COF-OMe. Such modifications increased the degradation rate constants for NM88(DB) 0.85 /COF-OMe to 15.1 and 17.3 times that of NM88 and COF-OMe respectively with good reusability. Moreover, the catalyst exhibited 32–170 times higher degradation kinetics in comparison to other reported catalysts. Results showed that due to the Schiff-base reaction between NM88(DB) and COF-OMe, electron density on Fe(III) was decreased; and the photogenerated electrons of COF-OMe moved to NM88(DB) to reduce Fe(III), thus resulting in the generation of highly active Fe(II) and ·OH species. Furthermore, the main reactive species were determined to be ·OH and ·O 2 – by trapping experiments, and a possible mechanism of the degradation system followed Z-scheme charge transfer.
研究领域:
环境科学
·
材料科学
✓ 已验证
DOI
PubMed
高影响因子
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