JOURNAL OF HAZARDOUS MATERIALS
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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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CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Yarui Wang,Chengzhuo Yu,Sen Wang,Jin Xu,Fanglan Geng,Silong Wang,Jitao Lv,Lixia Zhao,Yawei Wang
Humic acids (HA) released during algal bloom poses a key challenge for efficient photocatalytic degradation of Microcystin-LR (MC-LR) due to their scavenging function on active species. Herein, MIL-101(Fe)/TiO 2 -P25 (M/P) was constructed to diminish the inhibitory effect of HA on the photocatalytic degradation of MC-LR. Results showed that MC-LR could be efficiently removed assigning to the photogenerated holes (h + ) and superoxide radical (O 2 •− ) oxidation under visible light irradiation, where the carboxy groups of D -glutamic acid (Glu) and methyl- D -aspartic acid (MeAsp), and Adda side chain related to MC-LR biotoxicity were selectively destroyed to achieve MC-LR detoxication. More importantly, HA exerted non-inhibitory effect on MC-LR removal by M/P. The counteracting mechanisms were studied. Firstly, the location of TiO 2 in the pore structure of MIL-101(Fe) could occupy the adsorption sites of HA, and decrease the HA adsorption on M/P. Furthermore, XPS analyses suggested the coordination of unsaturated Fe metal sites on the surface of M/P hybrids complexed with –OH and –COOH of HA, which could accelerate the electron transfer and reduce hole consumption. Thus, the inhibitory effect of HA was alleviated during photocatalytic MC-LR treatment. This work offers a possible way to remove MC-LR in an abundant HA matrix water system efficiently.
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FOOD CHEMISTRY
·
2023
·
IF 8.8
Junxue Liu,Wenyan Ma,Yufei Wang,Qinfen Gu,Qinhe Pan,Siyu Zong,Minghao Qin,Jiyang Li
Monitoring of gallic acid (GA) in food and biothiols in humans is crucial for body health. Nanozyme-mediated colorimetric strategy for evaluating them has been widely applied nowadays, however, the inferior efficient and susceptible single-signal recognition limit its further application. Herein, a sensitive biosensor was first constructed for bimodal detection of GA and biothiols based on CDs@MIL-53(Fe)-NO 2 , prepared through a facile and time-saving microwave treatment. Benefiting from the excellent fluorescent and electron transfer properties of CDs, CDs@MIL-53(Fe)-NO 2 exhibited significant enhanced blue fluorescence and oxidase-like activity, which could oxide colorless 3,3′,5,5′-tetramethylbenzidine without H 2 O 2 , and the blue product could quench the fluorescence of composite. The dual-mode assay based on such bifunctional nanozyme showed an extremely sensitivity towards GA/ l -cysteine/homocysteine with the detection limit of 62/65/124 nM and 17/16/27 nM in colorimetric/fluorescent modes, respectively. The practicability in real samples and portability based on a smartphone of the analysis has been investigated with reliable results.
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Nano Research
·
2017
·Vol. 11
·期 2
·1109-1123
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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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LUMINESCENCE
·
2025
·Vol. 40
·期 1
·e70073
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IF 3
Xuhui Zhang,Yafei Chen,Jun Ling,Jianping Li
It is of great significance to develop sensors for trace pesticide residues detection in food. Herein, an electrochemiluminescence (ECL) sensor with high sensitivity for the detection of methyl parathion (MP) was constructed by combining of the acetylcholinesterase (AChE) enzyme-inhibited reaction with tris-2,2′-bipyridyl ruthenium Ru(bpy) 3 2+ -triethylamine (TEA) system for the first time. A new ECL probe of MIL-100 loaded with Ru(bpy) 3 2+ (Ru-MIL-100) was synthesized, and then Ru-MIL-100 and AChE were immobilized on the electrode with Nafion. Triethylamine was used as a coreactant to form a Ru-MIL-100–TEA luminescence system. The hydrolysis of iodinated acetylthiocholine by AChE to generate acetic acid that consumes TEA, leading to the quenching of ECL of the Ru-MIL-100–TEA system. But MP can inhibit the activity of AChE, which leads to the decrease of the generated acetic acid and the enhancement of ECL. With the increase of the MP concentration, the ECL intensity increases. Due to the high catalytic activity of the AChE and the excellent ECL luminescence performance of the Ru-MIL-100 probe, the sensor is highly sensitive. The detection concentration range of MP was 1.0 × 10 −12 –1.0 × 10 −9 mol/L, and the detection limit was 2.07 × 10 −13 mol/L. The biosensor was applied to the determination of MP in vegetable samples.
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ELECTROPHORESIS
·
2017
·Vol. 38
·期 19
·2521-2529
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IF 2.744
Yue Liu,Jia Hu,Yan Li,Yun-Tao Shang,Jia-Qi Wang,Ye Zhang,Zhong-Liang Wang
In this work, a CE method was developed to separate five anthraquinones: aloe-emodin, rhein, emodin, chrysophanol, and physcion. The CE method used a nano-sized metal organic framework MIL-101 (nMIL-101) as pseudostationary phase (PSP) and sorbent for dispersed particle extraction (DPE). The nMIL-101 was synthesized by microwave technique and was characterized by UV-vis, TEM, Zeta potential, X-ray diffraction spectrometry and micropore physisorption. In this method, anthraquinones were adsorbed by nMIL-101 of a fast kinetics within 10 min and then separated by CE. The CE conditions were optimized considering time, pH, buffer ionic strength, and nanoparticles concentration. The optimal CE condition is using 20 mM sodium borate buffer (pH 9.1) containing 15% methanol (v/v) and 400 mg/L nMIL-101 as additives within 8 min. The LODs varied from 24 to 57 μg/L, which were lower than those previously reported. Our method has been successfully applied to determine trace anthraquinones in environmental water samples.
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MICROCHIMICA ACTA
·
2019
·Vol. 186
·期 2
·1-8
·
IF 5.479
Cheng Ting,Li Xiang,Huang Peng,Wang Han,Wang Meixia,Yang Wenming
An electrochemical and colorimetric dual-readout method is described for the determination of thrombin. A platinum nanoparticle (Pt NP) modified metal organic framework (MOF) acts as a peroxidase (POx) mimic that causes the formation of a blue product from 3,3′,5,5′-tetramethylbenzidine (TMB) and hydrogen peroxide, with an absorption maximum at 650 nm. In addition, gold nanoparticles enrich initiators that trigger the hybridization chain reaction for dual signal amplification to generate an electrochemical current typically measured at 0.31 V (from −0.5 to −0.1 V) and allow quantitation of thrombin with high sensitivity and over a wide detection range. The colorimetric and electrochemical (dual) thrombin assay produces two kinds of signals which warrants accuracy, diversity, and an option for visual inspection. The dual-channel sensor allows for the quantitative determination of thrombin with a low detection limit (0.33 fM) for the electrochemical method and 0.17 pM for the colorimetric method) and over a wide detection range (1 fM to 10 nM for electrochemical method and 0.5 pM to 1 nM for colorimetric method). The electrochemical detection limit is lower than that of colorimetry, and the linear range is wider, which is more suitable for further quantitative analysis of the target.
Schematic representation of a colorimetric and electrochemical (dual) thrombin assay based on the use of a platinum nanoparticle modified metal-organic framework for color development and hybridization chain reaction for electrochemical signal. C-TBA: complementary sequences of thrombin aptamer, TBA: thrombin aptamer, I-Au NPs: initiators enriched by gold nanoparticles, S-AuE: sensing gold electrode, RS-AuE: reacted sensing gold electrode, TB: thrombin, MB: Methylene Blue, HCR: hybridization chain reaction.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Liping Liang,Fenfen Xi,Jinhui Zhao,Gunel Imanova,Sridhar Komarneni,Jianfeng Ma
nZVI was immobilized on MIL-101(Cr), a metal–organic framework (MOF), and subsequently utilized for the removal of U(VI) from aqueous solution. This composite was also tested for its toxicity to Escherichia coli ( E. coli ). The results demonstrated that MIL-101(Cr) and nZVI had a significant synergistic effect. This composite material is excellent for removing U(VI) and the optimal ratio of MIL-101(Cr) to nZVI was found to be 1.2:1 on mass basis. Adsorption data exhibited excellent fitting to the Freundlich and pseudo-second-order kinetic models, and a maximum removal capacity of 526.32 mg/g of U(VI) was achieved by M-Fe at 298 K (pH = 6.0). The removal mechanisms were clarified by the X-ray absorption near edge structure (XANES), X-ray photoelectron spectroscopy (XPS), and extended X-ray absorption fine structure (EXAFS). Results reveled that U(VI) was mainly removed through chemisorption, forming a bidentate mononuclear edge-sharing linkage between UO 3 pyramid and iron(hydro)oxide. Through free radical quenching experiments and EPR analysis, it was indicated that the existence of reactive oxygen species (ROS) accelerates the oxidation of nZVI, generating more iron oxides or hydroxides for U(VI) adsorption, while inhibiting the reduction of U(VI) to U(IV). Furthermore, immobilized nZVI on MIL-101(Cr) mitigated the biotoxicity of Escherichia coli ( E. coli ). Direct contact played a crucial role in inactivating E. coli cells by nZVI/ E. coli system. Extracellular reactive oxygen species (ROS) played a vital role in inactivating E. coli in the M-Fe/ E. coli system where OH is the main ROS. These findings enhance our understanding of the mechanism of U(VI) removal and bactericidal effect on organisms using ZVI-based composites, which will broaden the application scope of the two materials in pollution removal, especially in radioactive decontamination.
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JOURNAL OF CHROMATOGRAPHY A
·
2024
·
IF 3.8
Tianci Lv,Fubin Liu,Mengqian Xiao,Ying Liu,Litao Wang,Guihua Gao
In this study, a novel hierarchical pore MIL-101(Cr) foam (HPF-MIL-101) was designed and prepared using the sacrificial template method with NaCl as the sacrificial template. This method involved grinding, heating, and washing the NaCl template to produce HPF-MIL-101, with PVDF as the binder and MIL-101(Cr) as the adsorbent. This preparation process is both straightforward and cost-effective, avoiding the use or generation of any organic reagents, thereby offering an environmentally sustainable approach for producing metal-organic framework (MOF) composites. The prepared HPF-MIL-101 exhibited excellent adsorption capabilities for both anionic dye (methyl orange, MO) and cationic dye (methylene blue, MB). The adsorption process followed a pseudo-second-order kinetic model and Friedrich isotherm model, indicating a multilayer adsorption. This is further supported by the Weber-Morris intraparticle diffusion model, which divided the adsorption process into three stages. Furthermore, the adsorption process was consistent with the Freundlich isotherm model, with a correlation coefficient ( r ) greater than 0.96. HPF-MIL-101 can also be used as an adsorbent for solid phase extraction (SPE). Therefore, an SPE method combined with high-performance liquid chromatography (HPLC) was developed using HPF-MIL-101 as the adsorbent to analyze five fluoroquinolones (FQs) in water samples. This analytical method showed good linearity in the range of 30–2000 ng·mL −1 , with excellent linear correlation coefficient ( r = 0.9991–0.9999), reasonable extraction recoveries ranging from 80.39 to 112.7 % (RSD ≤ 7.9 %), and low limits of detection (8–30 ng·mL −1 ). Overall, the results indicated that HPF-MIL-101 not only had a simple, environment-friendly, and pollution-free preparation process but also can be reused for enrichment and detection of trace FQs in water. Thus, HPF-MIL-101 exhibits immense application potential in environmental pollutant removal and also provides a valuable reference for the preparation and application of other MOF composites.
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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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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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