SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Si Duan,Yuan Gao,Guihong Lan,Haiyan Qiu,Bo Xu,Zhuang Xie,Songsong Xue,Tianxiong Ou
The widespread use of chlortetracycline hydrochloride (CTC) inevitably poses a potential threat to human health and the biological system, and its environmental pollution and ecotoxicological effects cannot be ignored. Herein, we adopted an in-situ growth method to immobilize the powder form of MIL-100(Fe) adsorbent into low-cost chitosan (CS) matrix for the CTC removal. Metal hydroxide (or metal oxide)/CS beads from the acid-dissolved/alkali-solidified self-sphering shaping method were employed as the substrates for MIL-100(Fe) immobilization, allowing it grow uniformly and stably. Notably, this strategy not only reduced the loss in the separation and regeneration process of powdery MIL-100(Fe), but also improved the adsorption capacity of the CS. Isotherm and kinetic studies showed that the Freundlich and PSO models can describe the experimental data better, respectively, and the maximum adsorption capacity of Langmuir can reach 578.03 mg g −1 . Further, the performance of MIL-100@CS-2 composite beads was thoroughly explored by batch experiments and response surface methodology (RSM) to obtain the optimized operating conditions with the highest CTC removal rate. By combining the density functional theory (DFT) calculation with experimental analysis, the adsorption mechanisms of pore filling, hydrogen bonding , electrostatic interaction , π-π EDA interaction, and hydrophilic interaction were proposed. This work provides a reliable basis for the development of shaping adsorbents and has potential application prospects in the treatment of wastewater containing antibiotics.
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Nano Research
·
2015
·Vol. 8
·期 10
·3237-3249
·
IF 7.01
Liang Ruowen,Jing Fenfen,Shen Lijuan,Qin Na,Wu Ling
Proper design and preparation of high-performance and stable dual functional photocatalytic materials remains a significant objective of research. In this work, highly dispersed noble-metal nanoparticles (Au, Pd, Pt) were immobilized on MIL-100(Fe) (denoted M@MIL-100(Fe)) using a facile room-temperature photodeposition technique. The resulting M@MIL-100(Fe) (M = Au, Pd, and Pt) nanocomposites exhibited enhanced photoactivities toward photocatalytic degradation of methyl orange (MO) and reduction of heavy-metal Cr(VI) ions under visible-light irradiation (λ ≥ 420 nm) compared with blank-MIL-100(Fe). Combining these results with photoelectrochemical analyses revealed that noble-metal deposition can effectively improve the charge-separation efficiency of MIL-100(Fe) under visible-light irradiation. This phenomenon in turn leads to the enhancement of visible-light-driven photoactivity of M@MIL-100(Fe) toward photocatalytic redox reactions. In particular, the Pt@MIL-100(Fe) with an average Pt particle size of 2 nm exhibited remarkably enhanced photoactivities compared with those of M@MIL-100(Fe) (M = Au and Pd), which can be attributed to the integrative effect of the enhanced light absorption intensity and more efficient separation of the photogenerated charge carrier. In addition, possible photocatalytic reaction mechanisms are also proposed.
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MICROCHEMICAL JOURNAL
·
2022
·
IF 5.304
Mingchun Lv,Da-Wen Sun,Hongbin Pu,Haofan Zhu
Recyclable surface-enhanced Raman scattering (SERS) substrates are beneficial to cost reduction and environmental protection and have always been a research topic with great interest. Herein, a core–shell-satellite structured SERS substrate Fe 3 O 4 @MIL-100(Fe)@Ag nanoparticles (FMAs) was developed, possessing versatile functionalities of adsorption, detection, degradation and recovery. Results showed that the MIL-100(Fe) with peroxidase-like activity as shell catalyzed H 2 O 2 to generate ·OH degraded pollutants within 5 min to achieve substrate cleaning, making FMAs recyclable for at least 5 times to sequentially detect different cationic dyes with high sensitivity, having low detection limits as low as 15.24 ng/L, 387.87 ng/L and 0.71 ng/g for crystal violet in deionized water, aquaculture water and tilapia, respectively. FMAs also showed good uniformity, reproducibility and stability, with a relative standard deviation value of 5.58 % between substrates and about 78.60 % SERS activity remained after 20 d storage at 4 °C. This FMAs substrate thus has great potential for selective detection of trace cationic dyes in food or other fields.
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ENVIRONMENTAL POLLUTION
·
2024
·
IF 7.6
Hiba Shaghaleh,Yousef Alhaj Hamoud,Qin Sun
Hydrogel adsorbents are promising tools for reducing heavy metals' bioavailability in contaminated soil. However, their practical feasibility remains limited by the low stability, inefficient removal efficiency, and potential secondary pollution. Optimizing the adsorption operation and the functional properties of hydrogel adsorbents could eliminate this method's drawbacks. Herein, three innovative in-situ remediation strategies for Pb/Cu-contaminated soil were adopted based on the concept of novel TEMPO-cellulose (TO-NFCs)/lignin/acrylamide@MIL-100(Fe) nanocomposite hydrogel adsorbent (NCLMH). Characteristic analyses revealed ideal Pb/Cu adsorption mechanisms by swelling, complexation, electrical attraction, and ion exchange via carboxyl/hydroxyl/carbonyl groups and unsaturated Fe(III) sites on ANCMH besides FeOOH formation. The highest maximum theoretical adsorption capacities of Pb(II) and Cu(II) on ANCMH were 416.39 and 133.98 mg/g, under pH 6.5, governed by pseudo-second-order/Freundlich models. Greenhouse pot experiments with contaminated soils amended with two-depth layers of 0.5% NCLMHs (SA@NCLMH) displayed a decline in Pb and Cu bioavailability up to 85.9% and 74.5% within 45 d. Soil column studies simulating continuous water soil flushing coupled with NCLMH layers, instead of conventional extractant fluids, and connected to NCLMH-sand column as purification unit (CF@NCLMH) achieved higher removal rates for Pb, and Cu of 89.5% and 77.2% within 24 h. Alternatively, conducting multiple-pulse soil flushing mode (MF@NCLMH) gained the highest Pb and Cu removal of 96.5% and 85.4%, as the water flushing-stop flux events allowed adequate water movement/residence period, promoting Pb/Cu desorption-adsorption from soil to NCLMH. Also, the NCLMH-sand column conducting and easy separation of the stable/reusable NCLMHs prevented the potential secondary pollution. Interestingly, the three remediated soils reached the corresponding regulation of the permissible limits for Pb and Cu residential scenarios in medium-to-heavily agricultural polluted soils, alleviating the Pb/Cu bioaccumulation and phytotoxicity symptoms in cultivated wheat, especially after MF@NCLMH treatment. This study introduces promising alternative remediation strategies with high sustainability and feasibility in acidic-to-neutral heavy metal-contaminated agricultural soil.
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JOURNAL OF FOOD SCIENCE
·
2024
·
IF 3.2
Juan Du,Zongshuang Li,Jiangli Guo,Kaidong Du,Zhijian Chen,Yanhong Bai
In this study, a pretreatment method based on a magnetic capture probe for the rapid isolation and enrichment of bacteria from raw pork was developed. The chitosan immobilized Fe 3 O 4 @MIL-100(Fe) was prepared as a capture probe for total bacterial counts through the electrostatic interaction of positively charged chitosan and the negatively charged substances on the surface of bacteria. The interference of matrix in pork samples on this method was studied and removed by differential centrifugation. The results showed the capture probe had a great selectivity binding and magnetic separation properties for the tested six common bacteria in pork. Under the optimal conditions, the capture efficiency of the bacteria (10 5 CFU mL −1 ) from pork surface samples was all above 90%. The capture efficiency of the bacteria in a homogenate system was greatly decreased due to the interference of sarcoplasmic protein and myofibrillar protein in pork. The matrix effect was mitigated by a differential centrifugation method, and the capture efficiency of all six bacteria was >80%. The developed magnetic separation method took 40 min and showed good isolation and enrichment properties of bacteria. Thus, the proposed method is expected to provide a simple, convenient, and time-saving pretreatment method for the detection of total bacterial counts in pork.
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MICROCHIMICA ACTA
·
2021
·Vol. 188
·期 2
·1-9
·
IF 5.833
Senosy Ibrahim Abdelhai,Zhang Xin-Zhong,Lu Zhi-Heng,Guan Xiao-Yu,Yang Zhong-Hua,Li Jian-Hong,Guo Hao-Ming,Abdelrahman Talat Mahmoud,Mmby Mohamed,Gbiliy Asmaa
Fe 3 O 4 @MIL-100 (Fe)/PEI are used for the first time as an adsorbent material for the extraction of pesticide residues (epoxiconazole, flusilazole, tebuconazole, and triadimefon) from food matrices. The adsorbent proposed (Fe 3 O 4 @MIL-100(Fe)/PEI) was characterized by X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FT-IR), transmission electron microscopy (TEM), field emission scanning electron microscopy (FE-SEM), thermogravimetric (TG) analysis, and vibrating sample magnetometer (VSM) techniques to evaluate the properties of the sorbent. Then, the Fe 3 O 4 @MIL-100 (Fe)/PEI was employed for the quantification of the four triazole fungicides in fruits and vegetables (apple, orange, tomato, cabbage, and cucumber) using HPLC-UV for separation and detection. During the extraction process, the main parameters such as amount of adsorbent, extraction time, pH value, ionic strength, eluting solvent, and eluting volume were optimized. Under the optimum conditions, good linearity of this method was observed for all analytes, with correlation coefficients ( R 2 ) ≥ 0.9908. The limits of detection (LODs) ranged from 0.021–3.04 μg kg −1 . The extraction recoveries of the four triazole fungicides varied from 73.9 to 109.4% with relative standard deviations (RSD) in the range 0.5 to 6.2%. Compared with other MOFs, the modification of Fe 3 O 4 @MIL-100 (Fe) with PEI shows high efficient adsorption due to the combined benefits of MIL-100 (Fe) and PEI. The material is easily synthesized, has good stability, and is of low cost.
Graphical abstract
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CARBOHYDRATE POLYMERS
·
2019
·
IF 6.044
Chao Duan,Chaoran Liu,Xin Meng,Kun Gao,Wanli Lu,Yanling Zhang,Lei Dai,Wei Zhao,Chuanyin Xiong,Wenliang Wang,Yishan Liu,Yonghao Ni
3D Hydrogel is one of the most popular adsorbents for water remediation due to its excellent concentration/ adsorption capacity. However, it remains a challenge to use the hydrogel alone for treating complex wastewater. In this work, we designed and fabricated a versatile bio-based hybrid hydrogel consisting of Ag NPs@ MIL-100(Fe) photocatalysts and guar gum (GG) via facile blending and self-crosslinking. The hybrid hydrogel integrated with multifunctions of dye adsorption and degradation, oil/water separation and antibacterial properties, thus enabling its applications in complex wastewater remediation process. The presence of Ag nanoparticles (Ag NPs) not only enhanced the photocatalytic activity of MIL-100(Fe), but also imparted the antibacterial activity of Ag NPs@MIL-100(Fe)/ GG hydrogel. Particularly, the bio-based GG hydrogel scaffold showed excellent injectable, remodeling, and self-healing properties, which enabled an effective oil/water separation ability (silicone oil, cyclohexane and canola oil) and facilitated the recyclability/sustainability of the nano-photocatalyst powders. This novel multifunctional 3D hybrid hydrogel provides new opportunities for wastewater remediation purpose.
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Nano Research
·
2017
·Vol. 11
·期 2
·1109-1123
·
IF 7.354
Liang Ruowen,Huang Renkun,Ying Shaoming,Wang Xuxu,Yan Guiyang,Wu Ling
A simple, facile in situ reduction approach is reported for the synthesis of Pd-nanoparticle-decorated phosphotungstic acid (PTA)-MIL-100(Fe) nanocomposites (Pd-H 3 PW 12 O 40 -MIL-100(Fe), denoted Pd-PTA-MIL-100(Fe)). During the in situ synthesis, PTA is encapsulated into the matrix of MIL-100(Fe) and serves as a UV-switchable reducing agent, resulting in highly dispersed Pd NPs. Using the photocatalytic degradation of pharmaceuticals and personal care products as model reactions, the ternary Pd-PTA-MIL-100(Fe) hybrids exhibited enhanced photocatalytic activity compared with their foundation matrices, the binary PTA-MIL-100(Fe) nanocomposite. Based on photoelectrochemical analyses, the improved photocatalytic performance can be attributed to the well-known electronic conductivity of the Pd NPs, the fast electron transport of PTA, the intense visible-light absorption of MIL-100(Fe), and the matched energy levels of the three components: MIL-100(Fe), PTA, and Pd NPs. Importantly, almost no Fe and W ions were leached from the samples during the reaction, demonstrating the photostability of the Pd-PTA-MIL-100(Fe) composite. In addition, possible photocatalytic reactions mechanisms have also been investigated.
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FOOD CHEMISTRY
·
2021
·
IF 7.514
Manlu Wang,Juan He,Jin Luo,Jing Hu,Xiandeng Hou
The determination of inorganic arsenic species in real samples can be particularly challenging due to their trace levels and the interferences arising from sample matrix. Normally, the speciation analysis necessitates chromatographic separation. Herein, we report a novel method for the ultrasensitive detection and non-chromatographic speciation of inorganic arsenic by inductively coupled plasma mass spectrometry (ICP-MS), utilizing CdS/MIL-100(Fe) composites as an adsorbent and photocatalyst. The synthesized CdS/MIL-100(Fe) could completely adsorb As(V) and As(III) within 5 and 105 min, respectively. Following filtration and re-suspension in formic acid, the adsorbed As(III)/As(V) were reduced to arsine (AsH 3 ) under UV irradiation and swept to ICP-MS for detection. The limits of detection were found to be 1.7 ng L −1 (without preconcentration) and 0.11 ng L −1 (after 20-fold preconcentration). The method was successfully applied to the determination of trace inorganic arsenic in various food and water samples.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Jiandong Guo,Husheng Jia,Aiqin Zhang,Zhen Pei,Man Luo,Jinbo Xue,Qianqian Shen,Xuguang Liu,Bingshe Xu
Iron-based MOFs have been considered as the candidate for Fenton-like reagents owing to their open pore size and uniformly dispersed Fe active centers. However, the strong coordination of metal ions with organic ligands greatly reduces the exposed active sites of most iron-based MOFs, thus reducing Lewis acid sites and limiting the activation efficiency of H 2 O 2 . At the same time, low Fe 3+ /Fe 2+ cycle efficiency also restricts H 2 O 2 activation efficiency. Hence, in this work, a series of MIL-100 (Fe) containing mixed valence coordinatively unsaturated metal site (CUS) with different Fe 2+ /Fe 3+ ratios was synthesized by heat treatment and used for tetracycline hydrochloride (TC-HCL) degradation with the assistance of visible light. Interestingly, accelerated Fe 3+ /Fe 2+ cycle was observed with the aid of visible light. Among the prepared samples, CUS-MIL-250 prepared under vacuum at 250℃ has superior degradation performance, primarily owing to its large specific surface area and pore volume, improved visible light absorption, and the introduction of more Fe 2+ CUS. Meanwhile, compared with Fenton-like system and photocatalytic system, the CUS-MIL-250/H 2 O 2 /Vis system, with effective separation of photogenerated electrons and holes, demonstrates a synergistic effect to generate more reactive oxidation species, thereby improving the degradation efficiency. In addition, the catalyst shows good stability and recyclability.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2015
·
IF 7.435
Ruowen Liang,Shuiguang Luo,Fenfen Jing,Lijuan Shen,Na Qin,Ling Wu
The effective treatment of pharmaceutical and personal care products (PPCPs) contained wastewater remains a significant but challenging task for the environmental restoration. In this work, a novel Pd@MIL-100(Fe) nanocomposite has been successfully fabricated via a facile alcohol reduction approach. The resulting Pd@MIL-100(Fe) has exhibited superior photoactivity toward degradation of three typical PPCPs, that is theophylline, ibuprofen and bisphenol A, under visible light irradiation ( λ ≥ 420 nm). Its photoactivity is also much higher than that of original-MIL-100(Fe). Combining with photoelectrochemical analyses, it could be revealed that the introduction of Pd NPs would minimize the recombination of photogenerated electron–hole pairs, thereby improving the photocatalytic performance. Furthermore, the effects of different kinds of metals, the loading amount of noble-metal, the pH value of reaction solution and initial concentration of hydrogen peroxide on the photocatalytic degradation activities have been measured in detail. In addition, a possible photocatalytic reaction mechanism has been investigated. This work has not only represented the first example of using the MOFs photocatalysts to remove the aqueous PPCPs, but also offered useful information on the fabrication of efficient MOF photocatalysts for environmental restoration.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2026
·
IF 9.6
Siqi Liu,Shanshan Cheng,Zhimeng Liu,Miaomiao Zheng,Hongyuan Wang,Supakorn Boonyuen,Hongyi Gao,Ge Wang
Reactive oxygen species (ROS)-mediated sterilization typically relies on continuous light irradiation or exogenous H 2 O 2 addition, limiting their practical utility under dark or resource-limited conditions. Herein, we rationally design an S-scheme MIL-100(Fe)/Zn 3 In 2 S 6 heterojunction (M 5 Z 1 –1@ZIS2) by in-situ growing Zn-doped MIL-100(Fe) on Zn 3 In 2 S 6 , achieving synergistic light-harvesting and ROS self-supply capabilities. The incorporation of Zn 3 In 2 S 6 enhances electron density around Fe 2+ sites while modulating Fe 3+ states, significantly improving O₂ activation and H 2 O 2 affinity. This unique electronic regulation enables the heterojunction to generate superoxide radical(·O₂ − )-dominated ROS even in the dark. Notably, visible-light pretreatment induces active In sites in Zn 3 In 2 S 6 to produce H 2 O 2 , which accumulates and sustains the FeII/FeIII redox cycle in the absence of light, driving continuous hydroxyl radical(·OH)-dominated ROS generation. Combined characterizations including X-ray photoelectron spectroscopy (XPS) and Electron Paramagnetic Resonance (EPR) confirm H₂O₂-mediated Fe 2+ regeneration and ROS persistence. The M 5 Z 1 –1@ZIS2 heterojunction exhibits exceptional antibacterial performance, achieving ≥99.9% inactivation of Escherichia coli ( E. coli ) within 1.5 h in the dark and 40 min under visible light. This work provides a strategy for designing self-sustaining catalytic systems that leverage light-driven H₂O₂ supply to enable day-night ROS functionality. Furthermore, M 5 Z 1 –1@ZIS2 loaded on polyvinylidene fluoride (PVDF) film can achieve an efficiency of over 99% for particulate matter (PM) pollutants at the wind speeds of 1.5 m/s and 0.5 m/s and reach a maximum adsorption efficiency of 99.5% for formaldehyde within 19 min, highlighting its potential for all-weather air purification via ROS-mediated environmental remediation.
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