BIOINORGANIC CHEMISTRY AND APPLICATIONS
·
2022
·
IF 4.724
Yuqin Yang,Junjie Miao,Zhendong Yin,Weili Hao,Hongmei Shi,Ling Ma,Tiesheng Shi
Efficient extractions of trace antibiotic residues in the environment are a key factor for accurate quantification of the residues. A new nanoporous material, namely, magnetically covalent organic polymer (MCOP, Fe3O4@SiO2-NH2-COP) was synthesized in this work and was used for magnetic solid-phase extraction (MSPE). The combination of MSPE with high-performance liquid chromatography separation together with ultraviolet detection (HPLC-UV) was established as an effective method for the determination of four sulfonamide (SA) residues in surface water surrounding a cattle farm. The synthesized magnetic material was characterized by SEM, TEM, FT-IR, magnetic properties measurement system (MPMS), and nitrogen gas porosimetry. The material possessed many attractive features, such as a unique microporous structure, a larger specific surface area (137.93 m2·g−1) than bare Fe3O4 (24.84 m2·g−1), high saturation magnetization (50.5 emu·g−1), open adsorption sites, and high stability. The influencing parameters, including pH, the used amount of MCOPs, the type of eluent, adsorption solution, and desorption time, were optimized. Under the optimized conditions, the method conferred good linearity ranges (R2 ≥ 0.9990), low detection limits (S/N = 3, LOD, 0.10–0.25 μg·L−1), and satisfactory recoveries (79.7% to 92.2%). The enrichment factor (EF) for the four SAs was 34.13–38.86. The relative standard deviations of intraday (n = 5) and of interday (n = 3) were less than 4.8% and 8.9%, respectively. The equilibria between extraction and desorption for SAs could be reached within 150 s. The proposed method was sensitive and convenient for detecting SA residues in complex environmental matrices, and the successful application of the new MCOPs as an adsorbent was demonstrated.
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FUEL PROCESSING TECHNOLOGY
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2022
·
IF 8.129
Wei Ruan,Haoyun Liu,Hao Wu,Yuan Qi,Mengchang Zhou,Changsong Zhou,Zhen Zhang,Hongmin Yang
In this work, the Zr-based MOF was successfully fabricated with 4,6-Diamino-2-mercaptopyrimidine (DMP) and a novel adsorbent (Uio-DMP) was synthesized for the immobilization of Pb 2+ in aqueous medium . The morphological and structural characteristics of Uio-DMP were characterized by X-ray diffractometer (XRD), Fourier transform infrared (FT-IR), Field emission scanning electron microscopy (FE-SEM), Brunner Emmet Teller (BET), and X-ray photoelectron spectroscopy (XPS). The characterization results showed that the Uio-DMP maintained a pristine crystal structure and the sulfhydryl group was introduced to Zr-based MOF after chemical functionalization. The adsorption behavior of Uio-DMP for Pb 2+ was investigated in different conditions (solution pH, sorbent dose, Pb 2+ concentration, adsorption time, and co-existing ions). The experimental results indicated that the optimal pH was 6, the maximum adsorption capacity was 296.5 mg/g, and the Langmuir model well fitted the Pb 2+ removal process based on adsorption isotherm studies. The adsorption kinetic experiments revealed that the adsorption equilibrium could be achieved at 30 min and the adsorption process was consistent with the Pseudo-second-order model. The co-existing ions had a limited impact on Pb 2+ removal and the removal rate of 71.0% was maintained after five consecutive adsorption-desorption experiments. Furthermore, zeta potential and XPS analysis proved that the removal process of Pb 2+ over Uio-DMP was affected by electrostatic interaction , and nitrogen/sulfur atoms acting as the main adsorption sites. This study provides an insight into the removal of Pb 2+ in aqueous medium and the functionalization of adsorbents.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
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IF 8.128
Jiming Huang,Ping Xue,Sheng Wang,Shujun Han,Liguang Lin,Xuan Chen,Zhengbang Wang
Designing recyclable photocatalysts with high activity and stability has drawn considerable attention in the fields of sewage treatment. Herein, a series of heterojunctions constructed by zirconium-based metal–organic frameworks (UiO-66-NH 2 ) and tungsten trioxide (WO 3 ) is immobilized on carbon cloth via a facile solvothermal method , resulting in highly recyclable photocatalysts. Multiple characterization techniques, such as X-ray diffraction, scanning electron microscopy, transmission electron microscopy , X-ray photoelectron spectroscopy, and Fourier-transform infrared spectroscopy, verify the successful synthesis of UiO-66-NH 2 nanospheres on the surface of needlelike WO 3 modified carbon cloth. Results show that the optimal heterojunction photocatalyst exhibits excellent photocatalytic degradation efficiency for the removal of tetracycline (TC) from water, for which nearly 100% of TC is degraded within 60 min under visible light . Trapping experiments and electron spin resonance (ESR) spectra analyses demonstrate that the superoxide radicals O 2 – and photogenerated hole h + play a dominant role in the degradation process. Excellent photocatalytic activity is dominantly attributed to the effective separation of photoinduced carriers in this type-Ⅱ heterostructure system. Moreover, the possible photocatalytic oxidation degradation pathway is confirmed by analyzing intermediates using liquid chromatography mass spectrometry (LC-MS). This study offers a highly efficient strategy to design recyclable heterojunction photocatalysts for the degradation of refractory antibiotics in sewage.
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RSC Advances
·
2021
·Vol. 11
·期 33
·20439-20445
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IF 3.361
Jinhua Luo,Liping Jiang,Guihua Ruan,Chengyong Li,Fuyou Du
In this work, a metal–organic framework MIL-68(In)–NH2 incorporated high internal phase emulsion polymeric monolith (MIL-68(In)–NH2/polyHIPE) was prepared and applied as a solid phase extraction adsorbent for the extraction and detection of trace triazine herbicides in environmental water samples by coupling with HPLC-UV detection. The fabricated material showed good adsorption for simazine, prometryn, and prometon in water samples because of π–π interactions and hydrogen bonding interactions. Under optimal conditions, the maximum adsorption capacity of simazine, prometon and prometryn was 800 μg g−1, 800 μg g−1 and 6.01 mg g−1, respectively. The linearities were 10–800 ng mL−1 for simazine, prometon and prometryn. The limits of detection were 31–97 ng L−1, and the recoveries were 85.6–118.2% at four spiked levels with relative standard deviations lower than 5.0%. The method has a high sensitivity for the determination of three triazine herbicides in environmental water samples.
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JOURNAL OF HAZARDOUS MATERIALS
·
2020
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IF 9.038
Shuang Luo,Xingyan Liu,Xiangjun Wei,Min Fu,Peng Lu,Xuan Li,Yiming Jia,Qiao Ren,Youzhou He
The novel bifunctional NH 2 -MIL-125/Co(dmgH) 2 composite catalysts with several different Co(dmgH) 2 contents that can simultaneously achieve photocatalytic NO removal and hydrogen production were first prepared by a simple and convenient method. The corresponding physical and chemical properties of the composite catalysts were characterized by SEM, XRD, ESR, in situ DRIFTS, etc. The characterization results indicated that the noble-metal-free Co(dmgH) 2 , which was much cheaper and more available than most noble-metals such as Pt, could be an effective co-catalyst to accelerate the separation of photogenerated electron-hole pairs, further eventually enhancing the photocatalytic efficiency. Under visible-light irradiation for half an hour, the NO removal ratio of NH 2 -MIL-125/Co(dmgH) 2 (3 wt%) increased by 22.7 % compared with the pristine NH 2 -MIL-125 without Co(dmgH) 2 loading. In addition, it was found that Eosin Y dye-sensitized NH 2 -MIL-125/Co(dmgH) 2 (3 wt%) was capable of promoting a hydrogen generation rate of 2195 μmol g −1 h -1 under visible light, which was 12.6 times greater than the original NH 2 -MIL-125. This strategy was expected as an available way to fabricate noble-metal-free molecular complexes with metal-organic frameworks (MOFs) to enhance the photocatalytic NO removal and hydrogen production performance simultaneously.
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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.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Qing Wang,Xingyue Qian,Hui Xu,Guangyu He,Haiqun Chen
Exploring effective approach to promote more comprehensive charge transfer and efficient spatial charge separation is considered to be a prospective strategy to reinforce photocatalytic degradation activity. Herein, the oxygen vacancy modified Bi 2 WO 6 /NH 2 -MIL-68(In) Z-scheme heterojunction photocatalyst was successfully fabricated via a facile solvothermal method. The chemical structure, morphology, and optical properties of the photocatalyst were characterized in detail. The optimized Bi 2 WO 6 /NH 2 -MIL-68(In) Z-scheme heterojunction displayed the maximum photocatalytic efficiency (84.3 %) for the degradation of levofloxacin (LEV), which was significantly higher than that of pure Bi 2 WO 6 (45.1 %), oxygen vacancy modified Bi 2 WO 6 (69.4 %), and NH 2 -MIL-68(In) (49.3 %). Importantly, the high-resolution mass spectrometry (HRMS), three-dimensional excitation-emission matrix (3D EEMs) fluorescence spectra, the photo-electrochemical and photo-luminescence measurement, radical trapping test, and electron spin resonance (ESR) technique were carried out to illuminate the probable degradation pathway and mechanism of the LEV. The improved photocatalytic efficiency can be ascribed to the synergetic effect between oxygen vacancy and the Z-scheme heterojunction, which can serve as trapping centers to enhance the generation of photoexcited electrons and accelerate the charge transfer. Meanwhile, the effects of pH, photocatalyst dose, LEV concentration and different kinds of harmful organic pollutants were systematically explored from the practical application. This study offers a novel perspective for the integration of defect engineering and Z-scheme heterojunction in efficient organic pollutants degradation.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2019
·
IF 14.229
Shiyu Zhang,Meng Du,Zipeng Xing,Zhenzi Li,Kai Pan,Wei Zhou
Defective-rich and electron-rich mesoporous NH 2 -MIL-125(Ti)@ZnIn 2 S 4 /CdS hierarchical tandem heterojunctions were fabricated through two-step solvothermal and one-step hydrothermal strategies. The interface with electron enrichment can cause active interface reaction, fast transfer and separation of charge carriers and restrain the photocorrosion of CdS. ZnIn 2 S 4 , as a bridge to connect Ti-MOFs and CdS, favors the separation of charge carriers and forms tandem heterojunctions. The as-prepared photocatalyst has a relative large surface area of ∼877.0 m 2 g −1 and a narrow band gap of ∼1.84 eV, which could absorb visible light efficiently. Furthermore, it exhibits a high photocatalytic hydrogen generation rate which was increased to 2.367 mmol g −1 h −1 and the high photocatalytic degradation efficiency for 2,6-dichlorophen and 2,4,5-trichlorophenol which were 98.6% and 97.5%, respectively. Additionally, recycling text for several cycles indicates the high stability. This novel Ti-MOFs based core@shell hierarchical tandem heterojunctions may offer a new insight for fabricating high-performance heterojunctions for multi-channel charges transfer.
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EUROPEAN JOURNAL OF MEDICINAL CHEMISTRY
·
2023
·
IF 6.7
Dongliang Guan,Jian Li,Feifei Chen,Jiaqi Li,Xiaolei Bian,Yue Yu,Xinxin Feng,Lefu Lan,Wei Huang
Wide-spread use of daptomycin unavoidably resulted in the emergence of daptomycin-resistant pathogens. In the hunt for more active daptomycin derivatives through medicinal chemistry studies, we established a concise semisynthetic approach to modify the L-Kyn13 on daptomycin specifically and effectively. Here, 19 novel derivatives with certain diversity were designed and synthesized to perform a comprehensive SAR study on this underestimated position. The optimal compound, termed “hexakynomycin”, as the new generation of daptomycin-based antibiotic candidate exhibited 4->125-fold higher activity against methicillin-susceptible S. aureus (MSSA), methicillin-resistant S. aureus (MRSA), vancomycin-intermediate resistant S. aureus (VISA), and vancomycin-resistant Enterococci (VRE), including daptomycin-resistant strains, compared with that of daptomycin. Greater membrane binding capacity rendered hexakynomycin better activity and special antibiotic property. Hexakynomycin also demonstrated a better pharmacokinetic profile, good safety features and good pharmacodynamics properties. This work provided an effective modification strategy aiming at daptomycin which provided significant insights and showed great promise for the next generation of daptomycin derivatives.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2023
·Vol. 30
·期 26
·68691-68700
·
IF 5.8
Liu Yuhao,Wang Jieqi,Wang Xuyi,Chen Jiayue,Zhang Beibo,Chen Liping,Zheng Dan,Cheng Ming
It is a great challenge to develop photocatalysts for the degradation of organic pollutants in the aqueous environment, especially those with excellent catalytic performance under visible light conditions. In this work, using graphene oxide (GO) as an electron shuttle agent and carrier, a hybrid of ZIF-8/NH 2 -MIL-125(Ti) and GO (ZIF-8/NH 2 -MIL-125(Ti)/GO) was prepared by a simple two-step solvothermal method. The morphology, structure, and combination of the synthesized catalysts were studied. The results showed that graphene oxide and ZIF-8 formed an in situ load on NH 2 -MIL-125(Ti). The construction of hybrid materials significantly improved the catalytic activity of NH 2 -MIL-125(Ti) in the visible light range. The degradation activity of the synthesized catalyst was further tested with reactive red dye. The results showed that the catalyst exhibited excellent catalytic removal efficiency for active red, with a degradation rate of 99.8% within 2 h. The prepared hybrid materials have good application prospects in the field of organic pollutant treatment in water. Graphical Abstract
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Small
·
2023
·Vol. 19
·期 20
·2207198
·
IF 13.3
Jiayou Liu,Xiaoxiang Huang,Liuhu Jia,Linfeng Liu,Qianqian Nie,Zhongchao Tan,Hesheng Yu
Efficient nitric oxide (NO) removal without nitrogen dioxide (NO 2 ) emission is desired for the control of air pollution. Herein, a series of (Zr/Ti)UiO-66-NH 2 with congenetic shell–core structure, denoted as Ti-UION, are rapidly synthesized by microwave-assisted post-synthetic modification for NO removal. The optimal Ti-UION (i.e., 2.5Ti-UION) exhibits the highest activity of 80.74% without NO 2 emission with moisture, which is 21.65% greater than that of the UiO-66-NH 2 . The NO removal efficiency of 2.5Ti-UION further increases to 95.92% without photocatalyst deactivation under an anhydrous condition. This is because selectively produced NO 2 in photocatalysis is completely adsorbed into micropores, refreshing active sites for subsequent reaction. In addition, the enhanced photocatalytic activity after Ti substitution is due to the presence of Ti electron acceptor, the potential difference between the shell and core of Ti-UION crystal, and the high conductivity of Ti O units. Additionally, the improved adsorption of gas molecules not only favors NO oxidation, but also avoids the emission of NO 2 . This work provides a feasible strategy for rapid metal substitution in metal-organic frameworks and insights into enhanced NO photodegradation.
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NEW JOURNAL OF CHEMISTRY
·
2019
·Vol. 43
·期 32
·12563-12569
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IF 3.069
Huixiao Duo,Xiaofeng Lu,Shuai Wang,Licheng Wang,Yong Guo,Xiaojing Liang
Herein, a novel, fusiform-like magnetic metal–organic framework material (Fe3O4-NH2@MOF-235) was fabricated by a facile two-step solvothermal approach. Then, Fe3O4-NH2@MOF-235 was applied as an adsorbent in magnetic solid-phase extraction (MSPE) coupled with high-performance liquid chromatography (HPLC) for the simultaneous extraction and determination of five kinds of benzoylurea insecticides (flufenoxuron, chlorbenzuron, teflubenzuron, diflubenzuron and triflumuron) from honey, fruit juice and tap water samples. Moreover, potential variables influencing the MSPE efficiency were optimized. Under the optimized conditions, an excellent linearity was achieved in the range of 1.0–300.0 μg L−1 for teflubenzuron and flufenoxuron and 2.0–300.0 μg L−1 for diflubenzuron, chlorbenzuron and triflumuron, with the correlation coefficients of 0.9991–0.9995. The limits of detection for the analytes were 0.25–0.5 μg L−1, and the recoveries at three fortified concentration levels ranged from 76.45% to 90.74% for the honey samples, 79.95–95.27% for the fruit juice samples, and 84.02–99.62% for the tap water samples. The π–π stacking and hydrophobic interactions between Fe3O4-NH2@MOF-235 and the analytes played an important role in the adsorption process. Moreover, maximum adsorption could be achieved within 5 minutes with very little adsorbent for all the samples. Therefore, the magnetic Fe3O4-NH2@MOF-235 composite combined with MSPE is a convenient approach to detect benzoylurea insecticides in actual samples.
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