JOURNAL OF SEPARATION SCIENCE
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2016
·Vol. 39
·期 12
·2356-2364
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IF 2.741
Fuyou Du,Qun Qin,Jianchao Deng,Guihua Ruan,Xianqing Yang,Laihao Li,Jianping Li
In this work, a magnetic metal–organic framework designated as MIL-100(Fe) was prepared and applied as a magnetic solid-phase extraction sorbent for the determination of trace polycyclic aromatic hydrocarbons in environmental water samples by coupling with high-performance liquid chromatography and fluorescence detection. The magnetic microspheres exhibited large surface areas and high extraction ability, making them excellent candidates as sorbents for enrichment of trace polycyclic aromatic hydrocarbons. Under the optimized experimental conditions, good sensitivity levels were achieved with low detection limits ranging from 32 to 2110 pg/mL and good linearities with correlation coefficients higher than 0.9990 for the investigated 13 polycyclic aromatic hydrocarbons. The proposed method has been validated in the analysis of real water samples with mean recoveries in the range of 81.4–126.9% at four spiked levels and the relative standard deviations in the range of 1.3–17.0%. The magnetic MIL-100(Fe) microspheres were stable enough for 150 extractions without a significant loss of extraction performance.
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MICROCHIMICA ACTA
·
2016
·Vol. 183
·期 8
·2467-2472
·
IF 4.831
Yang Yang,Ma Xiaowei,Feng Fan,Dang Xueping,Huang Jianlin,Chen Huaixia
The article describes the synthesis of core-shell magnetic nanoparticles (MNPs) of the type Fe 3 O 4 @MIL-100 (MIL standing for Material Institut Lavoisier), and their application as sorbent for magnetic solid-phase extraction (MSPE) of triclosan. The MNPs were prepared via circular self-assembly of ferric chloride and benzenetricarboxylic acid. The functionalized MNPs were characterized by transmission electron microscopy, FTIR and thermogravimetry. Following extraction, triclosan was eluted with ammoniacal methanol and then submitted to HPLC with UV detection. The amount of magnetic microspheres, sample pH and ionic strength, adsorption time, desorption time, desorption solvent and the volume of the eluent were optimized. Under optimum conditions, the method showed good linearity in the 0.1 to 50 mg·kg −1 triclosan concentration range in toothpaste samples. Other features include (a) intra-day and inter-day relative standard deviations (RSD, for n = 4) of <5.5 %, (b) a 30 μg·kg −1 limit of detection, and (c) extraction recoveries between 90.86 % and 101.1 %. The method was successfully applied to the determination of triclosan in children’s toothpaste.
The article describes the synthesis of core-shell magnetic nanoparticles (MNPs) of the type Fe 3 O 4 @MIL-100, and their application as sorbent for magnetic solid-phase extraction (MSPE) of triclosan.
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ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Zhijian Chen,Zhenghui Ma,Guoli Fan,Feng Li
Presently, realizing high ethanol selectivity in CO2 electroreduction remains challenging due to difficult C–C coupling and fierce product competition. In this work, we report an innovative approach for improving the efficiency of Cu-based electrocatalysts in ethanol generation from electrocatalytic CO2 reduction using a crystal plane modification strategy. These novel Cu-based electrocatalysts were fabricated by electrochemically activating three-dimensional (3D) flower-like CuO micro/nanostructures grown in situ on copper foils and modifying with surfactants. It was demonstrated that the fabricated Cu-based electrocatalyst featured a predominantly exposed Cu(100) surface loaded with high-density Cu nanoparticles (NPs). The optimal Cu-based electrocatalyst displayed considerably improved CO2 electroreduction performance, with a Faraday efficiency of 37.9% for ethanol and a maximum Faraday efficiency of 68.0% for C2+ products at −1.4 V vs RHE in an H-cell, accompanied by a high current density of 69.9 mA·cm–2, much better than the particulate Cu-based electrocatalyst. It was unveiled that the Cu(100)-rich surface of nanoscale petals with abundant under-coordinated copper atoms from CuNPs was conducive to the formation and stabilization of key *CH3CHO and *OC2H5 intermediates, thereby promoting ethanol generation. This study highlighted the critical role of CuNP-loaded Cu(100) surface structures on structured Cu-based electrocatalysts in enhancing ethanol production for the CO2 electroreduction process.
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TALANTA
·
2017
·
IF 4.162
Yun Lei,Beibei Chen,Linna You,Man He,Bin Hu
Polydimethylsiloxane (PDMS)/MIL-100(Fe) coated stir bar was prepared by sol gel technique, and good preparation reproducibility was achieved with relative standard deviations (RSDs) ranging from 2.6% to 7.5% (n=7) and 3.6% to 10.8% (n=7) for bar-to-bar and batch-to-batch, respectively. Compared with commercial PDMS coated stir bar (Gerstel) and PEG coated stir bar (Gerstel), the prepared PDMS/MIL-100(Fe) stir bar showed better extraction efficiency for target triazines compounds. It also exhibited relatively fast extraction/desorption kinetics and long lifespan. Based on it, a method of PDMS/MIL-100(Fe) coated stir bar sorptive extraction (SBSE)-high performance liquid chromatography-ultraviolet detector (HPLC-UV) was developed for the determination of six triazines (simazine, atrazine , prometon , ametryn , prometryne and prebane) in environmental water samples. Several parameters affecting SBSE of six target triazines including extraction time, stirring rate, sample pH, ionic strength , desorption solvent and desorption time were investigated. Under the optimal experimental conditions, the limits of detection (LODs, S/N=3) were found to be in the range of 0.021–0.079 μg L −1 . The repeatability RSDs were in the range of 2.3–6.3% (n=7, c=0.5 μg L −1 ) and the enrichment factors (EFs) ranged from 51.1 to 102-fold (theoretical EF was 200-fold). The proposed method was applied to the analysis of target triazines in environmental water samples, with recoveries of 98.0–118% and 94.0–107% for spiked East Lake water and local pond water samples, respectively.
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TALANTA
·
2024
·
IF 5.6
Shuping Liu,Qingqing Zhang,Xiaohua Zhang,Cuicui Du,Jinhua Chen,Shihui Si
The misregulation of protein phosphatases is a key factor in the development of many human diseases, notably cancers. Here, based on a 100 MHz quartz crystal microbalance (QCM) biosensing platform, the dephosphorylation process of phosphopeptide (P-peptide) caused by protein tyrosine phosphatase 1B (PTP1B) was monitored in real time for the first time and PTP1B activity was assayed rapidly and sensitively. The QCM chip, coated with a gold (Au) film, was used to immobilized thiol-labeled single-stranded 5′-phosphate-DNAs (P-DNA) through Au–S bond. The P-peptide, specific to PTP1B, was then connected to the P-DNA via chelation between Zr 4+ and phosphate groups . When PTP1B was injected into the QCM flow cell where the P-peptide/Zr 4+ /MCH/P-DNA/Au chip was placed, the P-peptide was dephosphorylated and released from the Au chip surface, resulting in an increase in the frequency of the QCM Au chip. This allowed the real-time monitoring of the P-peptide dephosphorylation process and sensitive detection of PTP1B activity within 6 min with a linear detection range of 0.01–100 pM and a detection limit of 0.008 pM. In addition, the maximum inhibitory ratios of inhibitors were evaluated using this proposed 100 MHz QCM biosensor. The developed 100 MHz QCM biosensing platform shows immense potential for early diagnosis of diseases related to protein phosphatases and the development of drugs targeting protein phosphatases.
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JOURNAL OF CHROMATOGRAPHY A
·
2025
·
IF 4
Liangliang Peng,Yao Yao,Meiqi Li,Xingtong Ji,Jinbo Cao,Jiaming Zhang,Fusheng Zhong,Xixiang Yang,Xiaogang Hu
Zearalenone (ZEN), a mycotoxin produced by fungi of the genus Fusarium , is widely present in animal feeds and human foods, posing a serious hazard to human health. Herein, a zearalenone aptamer-functionalized magnetic metal-organic framework material (ZEN-Apt@MMIL-100(Fe)) was constructed and applied for the rapid enrichment of ZEN, coupled with high-performance liquid chromatography (HPLC) for ultrasensitive detection. By a self-templating method, magnetic MIL-100(Fe) was formed by self-assembly of sodium citrate-modified Fe 3 O 4 particles as nuclei with homobenzoic acid, which was bonded to amino-modified zearalenone nucleic acid aptamer via amide reaction to realize a specific recognition function. The magnetic dispersive solid-phase extraction and HPLC method was established using this material, with the linear range of 5 to 200 μg/L ( R 2 = 0 . 997) and the limit of detection of 2.92 μg/L. The method was applied to detect ZEN in maize and wheat samples, with spiked recoveries ranging from 81.7% to 98.2% at spiking levels of 25 μg/L, 50 μg/L, and 100 μg/L. The method is able to realize the selective and rapid enrichment and detection of trace ZEN in wheat and maize through the synergistic action of aptamer-specific recognition and magnetic MOFs, which provides a sensitive and reliable analytical strategy for food security monitoring.
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CHEMICAL ENGINEERING JOURNAL
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2025
·
IF 13.2
Xinrui Liu,Yupeng Li,Dairong Chen,Xiuling Jiao,Yuguo Xia
The selective hydrogenation of α,β-unsaturated aldehydes to unsaturated alcohols is a cornerstone of fine chemical synthesis, yet it remains a formidable challenge due to competing hydrogenation of thermodynamically favored C C bonds over kinetically sluggish C O bonds. Here, we present a PtFe dual-atom catalyst anchored on defective polymeric carbon nitride (DPCN), which achieves nearly complete conversion and exceptional selectivity toward cinnamyl alcohol (COL) under mild conditions. Particularly, the PtFe/DPCN exhibits a superior turnover frequency and achieves 99.02 % conversion of cinnamaldehyde (CAL) with 99.34 % selectivity for COL at 70 °C and 2 MPa H 2 . Kinetic studies and in-situ DRIFTS analyses reveal that this dual-atom architecture facilitates preferential C O adsorption and hydrogenation while suppressing C C activation. In addition, DFT calculations further show that the Pt-Fe dual atomic pair lowers the activation barrier by modulating the d -band center and Gibbs free energy profiles, enhancing H 2 splitting and intermediate stabilization. This work demonstrates a promising strategy for fine-tuning electronic and geometric structures via dual-atom design, offering an effective route for developing highly selective hydrogenation catalysts under industrially viable conditions.
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Acta Biomaterialia
·
2025
·
IF 9.6
Pai Wang,Heshi Liu,Lei Guo,Yixin Tang,Tianwei Lan,Rui Zhou,Huiqing Xu,Lu Wang,Xue Wang,Baiqiao Chen,Yixing Wang,Siyuan Wang,Chang Liu,Jie Chen,Caina Xu,Quan Wang,Huayu Tian
Colorectal cancer (CRC) remains a major global health burden as the third most commonly diagnosed malignancy and the second leading cause of cancer-related mortality worldwide. While combination chemotherapy and immune agonists hold potential to overcome tumor heterogeneity through multi-pathway modulation, their therapeutic efficacy remains limited by off-target drug distribution and immunosuppressive tumor microenvironment (TME). To address this, we developed a tumor-targeted chemo-immunotherapy platform by encapsulating irinotecan (CPT-11) and resiquimod (R848) in hyaluronic acid (HA) coated MIL-100(Fe) metal-organic frameworks (CRMH NPs), enabling CD44-mediated delivery and synergistic anti-tumor responses. The system enabled controlled drug release in the acidic TME, promoting immunogenic cell death (ICD), inducing the cGAS-STING pathway and activating immune cells. In vitro , CRMH NPs induced significant ICD, as evidenced by the release of damage-associated molecular patterns (DAMPs) like high mobility group box 1 (HMGB1) and calreticulin (CRT), and matured dendritic cells (DCs), which triggered by TLR7 agonist, enhancing immune responses. It also activated the cGAS-STING pathway, which could efficiently induce the targeted cells to produce type I interferon (IFN) and proinflammatory cytokines, thereby enhancing T cell activation and recruitment. In vivo , CRMH NPs significantly reduced tumor growth in CT26 mouse models, activated innate immune signaling, and increased immune cell infiltration, demonstrating superior anti-tumor effects compared to free drugs and other nanoparticle formulations. Furthermore, CRMH NPs upregulated PD-L1 expression on tumor cells, suggesting potential synergy with immune checkpoint blockade therapy. Combining CRMH NPs with anti-PD-L1 therapy enhanced anti-tumor immunity, particularly in distant tumors, highlighting a promising approach to overcoming immune evasion and achieving durable tumor regression. These findings supported CRMH NPs as a versatile and effective platform for chemo-immunotherapy in CRC. Statement of Significance Colorectal cancer (CRC) remains a major global health challenge with limited treatment efficacy due to tumor heterogeneity and immunosuppression. This study introduces a novel tumor-targeted nanoparticle platform, CRMH NPs, which co-deliver the chemotherapeutic drug irinotecan (CPT-11) and the immune agonist resiquimod (R848) using hyaluronic acid-coated MIL-100(Fe) metal-organic frameworks. CRMH NPs enhance drug delivery, induce immunogenic cell death, and activate the cGAS-STING pathway, synergizing chemotherapy and immunotherapy. Demonstrating superior tumor suppression and immune activation in preclinical models, this platform overcomes key limitations of current therapies, such as off-target effects and immune evasion. Its combination with anti-PD-L1 therapy further improves outcomes, offering a promising strategy for durable CRC treatment. This work advances nanomedicine and immuno-oncology, providing a transformative approach for cancer therapy.
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2020
·
IF 6.551
Kaibo Huang,Jiahao Liang,Jin Wang,Yuanxi Ouyang,Rui Wang,Ting Tang,Yusen Luo,Xueqin Tao,Hua Yin,Zhi Dang,Guining Lu
This study aimed to investigate the effects of nitrate on the ultraviolet (UV) treatment of simulated washing wastes containing Trion X-100 (TX-100) surfactant and 4,4′-dibromodiphenyl ether (BDE-15) pollutant. The presence of nitrate accelerated the photodegradation of BDE-15 and TX-100, because they reacted with reactive oxygen species (ROS) produced from conversion between nitrate and nitrite. Due to nitrite having a stronger radical quenching property than nitrate, nitrite hindered TX-100 decay while the photodegradation rate of BDE-15 was similar to that in the presence of nitrate. This indicated that nitrate/nitrite affected BDE-15 photodegradation by photosensitization and TX-100 loss by ROS attack. An increased TX-100 concentration increased the loss of total inorganic nitrogen possibly owing to an increase in organic nitrogen formation through TX-100 nitration reactions. At pH < 7 HOONO rapidly isomerized to NO 3 − , and at pH = 7–9 it homolyzed to ONOO − , which increased OH production to decay the BDE-15 and TX-100 and also increased NO 2 − formation. BDE-15 mainly underwent debromination, and some rearrangement, ring formation, nitration and hydroxylation products were detected, indicating that the produced OH and NO 2 attacked the BDE-15 and products. Furthermore, broken-chain, carboxylation , hydroxylation and nitro products were detected by Liquid chromatography high resolution mass spectrometry (LC-HRMS). Escherichia coli was used to assess the toxicity of washing waste containing nitrate: the presence of nitrate will increase the wastes' toxicity during UV treatment. Therefore, the presence of nitrate is deleterious to the UV treatment of washing wastes, and it is important to remove nitrates and nitrites from washing waste before UV irradiation.
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JOURNAL OF HAZARDOUS MATERIALS
·
2021
·
IF 10.588
Wenting Shen,Jiang Xu,Lizhong Zhu
Sulfidized nanoscale zerovalent iron (SNZVI) with improved reactivity and selectivity has shown great potential for environmental remediation. However, it is unclear if SNZVI could be applied for the remediation of soil washing solution, and how a soil-washing surfactant affects the reactivity and selectivity of SNZVI. Here, we assess the impact of Triton X-100 (TX-100) on the reactivity and selectivity of a sulfidized commercial NZVI toward tetrabromobisphenol A (TBBPA). While sulfidation of NZVI improved its reactivity and electron efficiency toward TBBPA, TX-100 could further improve these promoting effects, which was 8–21 and 4–7 times higher than those without TX-100, respectively, depending on TX-100 concentration. Because TX-100 could induce the solubilization of TBBPA, sorb onto the SNZVI surface, and favor the subsequent sorption and degradation of TBBPA. SNZVI performance for successive treatments of TBBPA contaminated water was also greatly improved by TX-100. Moreover, washing the TBBPA-contaminated soil with TX-100 could efficiently extract the TBBPA, and almost all of the TBBPA in the soil washing solution could be efficiently degraded by SNZVI. These results suggest that TX-100 is a good additive to SNZVI for improving its performance, and SNZVI coupled with TX-100 can be a promising technology for the remediation of TBBPA-contaminated soil.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Shan Hu,Panzhe Qiao,Xinming Liang,Guiming Ba,Xiaolong Zu,Huilin Hu,Jinhua Ye,Defa Wang
Photoreduction of CO 2 and H 2 O into fuels and value-added chemicals is a promising green technology for solar-to-chemical conversion. However, improving the conversion efficiency with regulated product selectivity is a big challenge due to the sluggish dynamic transfer and insufficient active sites. Herein, we report on Pt single atoms anchored porous C 3 N 4 nanosheet photocatalyst (Pt 1 @CN) with Pt–N 4 coordination for stable and efficient CO 2 photoreduction using H 2 O as reductant. The Pt 1 @CN exhibits an evolution rate of 84.8 μmol g −1 h −1 with nearly 100% CO selectivity, outperforming most previous C 3 N 4 -based single-atom photocatalysts. Experimental and DFT calculation results reveal that the Pt–N 4 coordinated active sites promote the photogenerated electron transfer, CO 2 adsorption/activation, *COOH generation, and *CO desorption, thus accounting for the significantly improved CO 2 photoreduction activity with ∼100% CO selectivity. This study provides a deep insight into the significant roles of single-atom active sites in enhancing the CO 2 photoreduction activity and regulating the product selectivity.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2024
·
IF 8
Siqi Wei,Renjie Li,Ling Li,Dan Huang,Li Wu,Xiandeng Hou
The development of a rapid and accurate assay for the detection of biothiols is critical for early diagnosis and prevention of diseases. Herein, we report that the preparation of photoinduced defective MIL-100-NH 2 (PID-MIL-100-NH 2 ) with oxygen vacancy defects as a surface-enhanced Raman scattering (SERS) substrate by high-energy light irradiation. The substrate exhibited excellent SERS activity to Cys, Hcy and GSH with limits of detection (LODs) as low as 30, 23 and 18 nM, respectively, notably lowering the detectable concentration by at least 10 5 times compared to the Au NP substrate. Such superior SERS activity is attributed to the energy level matching of the PID-MIL-100-NH 2 substrate and the biothiol molecules, which results in efficient multiple charge-transfer resonances, such as photoinduced charge-transfer (PICT), ground-state charge-transfer (GSCT), and exciton resonances. Making good use of the rich fingerprint information, selective identification and simultaneous quantitation of biothiols in complex biological environment can be achieved. Trace biothiols in human serum samples have been successfully determined using this method. This work provides a feasible strategy to construct efficient charge-transfer resonances, enabling high-performance direct SERS sensing of biological small molecules.
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