CHEMICAL ENGINEERING JOURNAL
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2024
·
IF 13.3
Yiting Lv,Jinjuan Xue,Zhaoxia Chen,Jianan Qu,Kaiwen Huang,Mingxin Wang,Wei Sun
Photocatalytic production of H 2 O 2 has garnered significant attention, but the use of sacrificial reagents in H 2 O 2 photosynthesis and the subsequent limited H 2 O 2 activation efficiency would impede its practical application in water decontamination. In this work, hydrothermal carbonaceous carbon/NH 2 -MIL-101(Fe) (abbreviated as HTC-cf/NMIL-101(Fe)) heterojunction was fabricated through a solvothermal strategy, and serving as a self-sufficient photo-Fenton-like catalyst to in-situ generate and activate H 2 O 2 . Hydrothermal carbonaceous carbon derived from cost-effective waste coffee grounds, serving as a green and sustainable photocatalyst, demonstrated high H 2 O 2 production rate of 612 μmol/g/h without the need for sacrificial reagents or aeration assistance. Moreover, the excellent self-sufficient photo-Fenton activity for HTC-cf/NMIL-101(Fe) can be obtained, which ascribed to the synergistic effect of self-generated H 2 O 2 production as well as the in-situ catalytic H 2 O 2 decomposition of • OH by Fe species in NMIL-101(Fe) and photogenerated electrons. The optimized HTC-cf/NMIL-101(Fe) photocatalyst showed simultaneous improvements in both H 2 O 2 production and activation capabilities. Impressively, the effective circulation of Fe 3+ /Fe 2+ in NMIL-101(Fe), aided by photogenerated electrons, results in a 5-fold increase toward H 2 O 2 decomposition rate constant (K d ) compared to HTC-cf alone under light irradiation in open-air conditions. The enhanced charge separation and appropriate band structure of HTC-cf/NMIL-101(Fe) photocatalyst assured the high selectivity of two-electron O 2 -reduction to H 2 O 2 . HTC-cf/NMIL-101(Fe) displayed excellent photocatalytic sterilization efficiency against E. coli and S. aureus under visible light, and its sterilization application in actual water was also demonstrated. Notably, the adaptability of this system to ambient conditions, including open-air atmosphere, non-sacrificial reagents, and low leaching of Fe ions, highlights the promising practical utility of the HTC-cf/NMIL-101(Fe) photocatalyst.
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CHEMICAL ENGINEERING JOURNAL
·
2025
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IF 13.2
Tiantian Li,Zhining Huang,Mengfan Hu,Yuen Hu,Ke Quan,Man Zhou,Yao chen,Shaoju Fu
Heavy metal wastewater pollution has been a globally important and serious issue for the industrial manufacturing center. Herein, we developed a novel CAP@Ui0-66-NH 2 @PPy nanocomposite fibrous membrane, by combining the in-situ growth and oxidative polymerization technical routes, which possessed a high specific surface area and abundant amino-active sites to remove Cr (Ⅵ). Systematic characterization showed that the porous structure and in situ growth of MOF provided sites for polymerization of charged polypyrrole (PPy), resulting in the large specific surface area (78.837 m 2 /g) of CAP2@Ui0-66-NH 2 @10 %PPy. The maximum adsorption capacity was as high as 312.70 mg/g at 298 K, which was significantly better than that of CAP (CA and PVP electrostatic spinning and then washing off the PVP) nanomembranes. The adsorption process was consistent with the proposed secondary kinetic and Langmuir model, and the high adsorption capacity was maintained after five rounds of cyclic adsorptions. Through XPS analysis, the abundant amino groups on the surface of the adsorbent material were protonated, caused the electrostatic attraction and ion-exchange interaction with the anion Cr(Ⅵ). These protonated amino groups were able to reduce the toxic Cr (Ⅵ) to non-toxic Cr (Ⅲ), which was immobilized on the surface of the material through chelation. The MOF lattice achieved in-situ growth on porous CA nanofibrous membranes, which significantly enhances the mass-transfer dynamics and the membrane cycling stability, the amine-based functionalization of the UI0-66-NH 2 improved the coordination activity and increased the adsorption efficiency, and polypyrrole (PPy) conductive layer promoted the directional migration of Cr (VI) and effectively suppressed the interference of competing ions. In sum, the prepared CAP@Ui0-66-NH 2 @PPy hybrid fibrous membranes showing great potentially applicable for heavy-metal wastewater treatment.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2024
·
IF 5.8
Xiao-hu Ma,Si-yuan He,Zhe-rui Zhang,Zhe Meng
Persistent light-emitting materials (PLMs), which have the potential to store and release light energy after light irradiation, are receiving increasing attention for their role in prolonging the lifetime of photogenerated electrons for the development of photocatalysts with round-the-clock applications. In this paper, a double S-scheme Sr 2 MgSi 2 O 7 :Eu 2+ ,Dy 3+ /ZnIn 2 S 4 /UiO-66-NH 2 (SZU) heterojunction with round-the-clock catalytic activity was prepared by hydrothermal self-assembly method. The photocatalytic performance of the SZU heterojunction for RhB(MB) degradation was significantly improved compared with the pristine ZnIn 2 S 4 and UiO-66-NH 2 . The SZU heterojunction has excellent catalytic degradation performance for RhB (MB), and the removal rate of RhB (MB) reaches 72.2 % (81.7 %) after visible light irradiation for 40 (60) minutes. After the end of light, the total removal rate of RhB (MB) reached 86.7 % (96.8 %) when the catalysis continued for several hours under dark conditions, which was 14 % and 15 % higher than that under visible light irradiation, respectively. Based on the characteristics of SMS photoluminescence, combined with a large number of photocatalytic experiments, The sustained photocatalytic activity was enhanced under both daytime and darkness conditions, not only because of the production of SZU complexes, which prolonged the visible light response of ZnIn 2 S 4 , but also because of the construction of double S-scheme heterojunctions, which facilitates the light storage capacity, charge transfer, and the separation of photo-induced charge carriers and effectively promoted the photocatalytic activity of the photocatalysts. This work contributes to a deeper understanding of the design of round-the-clock photocatalysts, and provides a useful exploration for the practical application of photocatalytic technology.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Guzheng Mao,Qiqi Kan,Zhongyuan Yue,Shengui Ju,Haoli Zhou,Wanqin Jin
Pervaporation (PV) is an energy-efficient membrane technology for separating organic mixtures. Traditional polymer membranes in the PV face limitations due to a trade-off between flux and separation factor. Mixed-matrix membranes (MMMs) fabricated using solution mixing or filler modification often suffer from interfacial defects or require additional complex preparation steps. This study introduces an in situ polymerization method that incorporates UiO-66-NH 2 into the polyamide polymerization process to fabricate UiO-66-NH 2 @polyamide (PA) MMMs for methanol and dimethyl carbonate separation, which effectively resolves the interfacial defect issues while eliminating additional filler modification steps. The trade-off issue is also overcome. Results show that in situ polymerization improves UiO-66-NH 2 dispersion in the polymer matrix and strengthens polymer–filler interactions. MMMs with 5 wt% UiO-66-NH 2 loading achieved a total flux of 11.5 kg/(m 2 ·h) and a separation factor of 12.5 at 30 °C, representing a 2.32-fold and 1.46-fold improvement over pure PA membranes. These findings demonstrate the significant benefits of in situ polymerization in enhancing MMM performance and simplifying fabrication, providing an efficient strategy for industrial PV applications.
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JOURNAL OF MOLECULAR STRUCTURE
·
2024
·
IF 4
Shuangbao Li,Shuaibing Ma,Jian Li,Yongbo Yu,Zechao Wu,Yuteng Zhang,Li Jin,Julun Zong,Jianpo Zhang
Malachite green (MG), a cost-effective triphenylmethane dye known for its insecticidal and germicidal properties in aquaculture, unfortunately poses significant environmental and human health-related risks due to its mutagenic, carcinogenic, and teratogenic effects. Herein, a novel diamine-functionalized zirconium-based metal organic cage (Zr-MOC), abbreviated as ZrT-1-(NH 2 ) 2 , was synthesized through microwave-assisted method, serving as a ratiometric fluorescent sensor for the precise detection of MG in aquaculture water. When the pH value was adjusted to 3.0, the probe solution exhibited two distinct characteristic emission bands centered at 454 nm and 582 nm, upon excitation at 365 nm. With the addition of MG, the emission intensity at 582 nm was significantly quenched, whereas the fluorescence intensity at 454 nm was gradually increased. The related experimental data and DFT calculations revealed that the quenching process is predominantly governed by the inner filter effect and static quenching mechanisms. Notably, the ratiometric fluorescence probe exhibited a good linear correlation with the MG concentration within the range of 1.37–17.81 nM, boasting a remarkably low detection limit of 1.05 nM. Furthermore, the proposed ZrT-1-(NH 2 ) 2 ratiometric fluorescence probe features high recoveries (95.37–104.93 %) and low relative standard deviations (RSD<3.5 %) for the detection of trace MG in aquaculture water, indicating its feasibility and practicality for MG detection.
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FOOD CHEMISTRY
·
2024
·
IF 8.5
Yeling Han,Wenyuan Zhou,Yuhong Wu,Aiping Deng,Lei Yuan,Yajun Gao,Huaxiang Li,Zhirong Wang,Bo Wang,Guoqiang Zhu,Zhenquan Yang
In this study, a colourimetric biosensor based on bacteriophage SapYZUM13 and an aminated Mn 3 O 4 (Mn 3 O 4 -NH 2 ) nanozyme was constructed and evaluated for its ability to detect Staphylococcus aureus in food. The biosensor had a detection time of 20 min, with a detection limit of 2 × 10 1 CFU/mL and recovery rate of 92.42–106.96%, indicating its high reliability and accuracy in detecting the food pathogen . Mechanistically, SapYZUM13@Mn 3 O 4 -NH 2 exhibited oxidase-mimicking capability, producing O 2 •– free radicals which oxidise 3,3′,5,5′-tetramethylbenzidine (TMB) to yield blue-coloured oxTMB. In the presence of S. aureus , the oxidase activity decreased remarkably owing to shielding of the nanozyme active sites. Moreover, SapYZUM13@Mn 3 O 4 -NH 2 could detect viable S. aureus from various sources, likely because of the special receptor-binding proteins of SapYZUM13 adsorbing to the wall teichoic acids on the S. aureus cell surface. Thus, SapYZUM13@Mn 3 O 4 -NH 2 has broad application prospects for the detection of viable S. aureus in various foods.
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PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2020
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IF 9.038
Shi-Wen Lv,Jing-Min Liu,Ning Zhao,Chun-Yang Li,Zhi-Hao Wang,Shuo Wang
Nowadays, designing highly active photocatalysts for pollutant degradation under visible light still remains a challenging problem. Herein, a novel benzothiadiazole functionalized Co-doped MOF-based photocatalyst with electron deficient unit was first synthesized via a feasible step-by-step assembly strategy. Benzothiadiazole, as typical electron deficient group, could effectively promote the separation and transfer of photoinduced charge carriers. The implantation of Co ion could be served as an effective mediator to further facilitate the charge transfer through a Co 3+ /Co 2+ redox pathway. Interestingly, the as-synthesized Co-MIL-53-NH-BT exhibited significantly enhanced photocatalytic degradation capacity for BPA and OFX under visible light irradiation, with removal efficiency as high as 99.9 % and 99.8 % within 120 min. TOC analysis suggested that majority of contaminants had been degraded into CO 2 and H 2 O. The important parameters influencing the photocatalytic activity were investigated, and the kinetics study was also conducted. The possible degradation pathways and the possible photocatalytic mechanism were proposed. More importantly, the as-synthesized Co-MIL-53-NH-BT showed good reusability, stability as well as universal applicability. To sum up, current work not only developed an efficient and visible-light active photocatalyst for treating organic-contaminated wastewater, but also afforded some novel insight into the utilization of benzothiadiazole in MOF-based photocatalyst towards improving photocatalytic activity.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
·
IF 9.7
Chen Chen,Jianhao Qiu,Guanglu Xia,Lu Zhang,Yixin Li,Biyao Fang,Meng Liu,Jianfeng Yao
Utilizing metal–organic frameworks as templates to synthesize photocatalysts has garnered increasing attention thanks to their substantial advantages. In this study, Cu-doped ZnIn 2 S 4 with hollow tubular structures was ingeniously synthesized using MIL-68-NH 2 as a template for photocatalytic H 2 O 2 production in ambient air and pure water under visible light. The hollow tubular structures promote light penetration and reflection, furnish substantial accessible reactive sites and accelerate the diffusion of reactants and products. Cu doping notably varies the band configuration of ZnIn 2 S 4 , resulting in a narrower bandgap and a lower conduction band potential. Their cooperative effects enable a respectable H 2 O 2 production from oxygen reduction reactions. The hollow tubular ZnIn 2 S 4 and corresponding Cu-doped counterpart achieved high H 2 O 2 yields of 1153 and 1616 μmol·L −1 , respectively, 3.6 and 5.1 times-increase compared with that of ordinary ZnIn 2 S 4 prepared without MIL-68-NH 2 . This work would provide a new perspective on ZnIn 2 S 4 -based photocatalysts and provoke the study on the green synthesis of H 2 O 2 .
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Jiajun Yu,Xiao Wang,Shijie Yang,Xiaofeng Xie,Jing Sun
Ligand functionalization could effectively modulate the local electron distribution of MOFs, thus improving their performance in both the capturing and photocatalytic oxidization of various VOCs. In this work, a series of Fc-CHO/NU-X (X = 1, 2, 3, 4) were obtained through the ligand functionalization of reo -NH 2 -UiO-66 (denoted as NU) with ferrocenecarboxaldehyde (Fc-CHO) as the modifier. By altering the local charge distribution and inducing Fe-OH and cyclopentadienyl rings as new adsorption sites, Fc-CHO altered the adsorption behavior of both aromatic and oxygenated VOCs and consequently their degradation pathways. The introduction of electron-donating Fc-CHO enhanced the ligand to metal charge transfer (LMCT), accelerated the electron-hole separation and therefore promoted the effective formation of oxidative radicals, facilitating the effective oxidation of acetaldehyde. Direct charge transfer through p-p interaction enabled the ring-opening and deep oxidation of toluene. The degradation efficiencies of toluene and acetaldehyde increased from 25 % and 28 % (NU) to 80 % (Fc-CHO/NU-3) and 65 % (Fc-CHO/NU-2), respectively. Positive effects of Fc-CHO functionalization were also observed during the removal of acetaldehyde-toluene mixtures and the synergistic effect between acetaldehyde and toluene was revealed. This work provides new ideas and novel materials for the purification of in-door air pollutants.
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JOURNAL OF SEPARATION SCIENCE
·
2025
·Vol. 48
·期 7
·e70217
·
IF 2.8
Piao Liu,Changhong Li,Minqi Ou,Chang Yin,Xinyue Kang,Jun Chen,Ran Liu,Jialang Zhuang
A dispersive solid-phase extraction process was established using UiO-66-NH 2 as an adsorbent, in combination with ultra-high-performance liquid chromatography-tandem mass spectrometry (UHPLC-MS/MS) technology, and the performance of this combination for the metabolomic analysis of biological specimens was assessed. Differential metabolites in plasma samples from oral squamous cell carcinoma and hepatocellular carcinoma patients and healthy volunteers were screened, and metabolic pathway enrichment analysis was performed via pseudo-targeted metabolomics. Based on the significantly enriched metabolic pathways and related literature, 20 amino acids were selected and targeted for quantitative analysis. The key parameters for extraction recovery, including the type of liquid in the adsorption system, pH of the eluent, amount of UiO-66-NH 2 , and time of extraction and elution, were optimized based on the selected amino acids. The optimized method demonstrated a remarkable performance: correlation coefficients > 0.99, limits of detection ranging from 0.002 to 0.080 µg/mL (signal-to-noise ratio = 10), and recoveries of 63.9%–110.8% in plasma samples. Thus, via targeted metabolomics analysis, 10 amino acids (including lysine and 3-iodo-L-tyrosine) and 10 amino acids (including arginine and histidine) were determined as potential biomarkers for oral squamous cell carcinoma and hepatocellular carcinoma, respectively. Based on the above potential amino acid markers, discriminant equations for oral squamous cell carcinoma and hepatocellular carcinoma were established, respectively. Two biomarker combinations were successfully screened: lysine and 3-iodo-L-tyrosine (AUC = 0.998, sensitivity = 0.967, specificity = 1.0) for oral squamous cell carcinoma, and histidine and arginine (AUC = 0.944, sensitivity = 0.833, specificity = 0.933) for hepatocellular carcinoma. Our findings will provide new directions for cancer diagnosis.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Zhiqiang Guo,Xinmiao Wu,Juanjuan Meng,Xinxin Li,Yuan Li,Liangliang Hu
MIL-101(Fe) has received more and more attention in wastewater treatment, and how to further improve its stability and sorption capacity has become a research focus. In this study, metal Mg was used to dope MIL-101(Fe) to construct Mg@MIL-101(Fe) with bimetallic sites, which was then mixed with NH 2 -MIL-125(Ti) to successfully fabricate Mg@MIL-101(Fe)/NH 2 -MIL-125(Ti) (MOM) bis-MIL composites. MOM not only contains a large number of sorption sites but also exhibits excellent stability and reusability, realizing efficient sorption of Pb(II) from aqueous solution. In addition, the sorption performance and mechanism of Pb(II) on MOM were investigated by the characterizations of SEM, BET, TG, XRD, FTIR and XPS, as well as the kinetic and thermodynamic analyses. The sorption of Pb(II) on MOM is in accordance with the Langmuir isothermal model and pseudo-second-order kinetic model. The maximum sorption capacity of Pb(II) on MOM derived from the Langmuir model fitting is 320.941 mg·g −1 . The sorption of Pb(II) on MOM is strongly affected by pH, but not by ionic strength, which indicates that MOM has good resistance to salt interferences. The strong complexation of carboxyl, hydroxyl and amino functional groups with Pb(II) is the main sorption mechanism of Pb(II) on MOM, and electrostatic interaction and ion exchange also contribute to the sorption. In conclusion, MOM has strong practical application prospects in the treatment of Pb(II)-containing wastewater.
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高影响因子
BIOELECTROCHEMISTRY
·
2019
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IF 4.474
Shuan Zhang,Chunyan Zhang,Yilei Jia,Xiaobo Zhang,Yunhui Dong,Xinjin Li,Qing Liu,Yueyun Li,Zengdian Zhao
A sandwich-type electrochemical immunosensor was fabricated for the quantitation of alpha fetoprotein (AFP). To this end, the Au@Pt dendritic nanorods loaded with amino functionalized molybdenum selenide nanosheets (Au@Pt 41 DNRs/NH2-MoSe2 NSs) with enhanced peroxidase-like properties were selected as the secondary antibody label (Ab2) to achieve signal amplification. The as-obtained Au@Pt DNRs/NH2-MoSe2 NSs exhibited better catalytic activity toward hydrogen peroxide reduction and offered rich anchors for bioconjugation . Meanwhile, gold nanoparticles anchored on an amino functionalized graphene (Au NPs/NH2-GS) composite with admirable conductivity and biocompatibility was used as the matrix material to improve sensitivity. Under optimal conditions, amperometric current responses had a good linear relationship with the logarithm values of AFP concentration in the range 10 fg mL –1 to 200 ng mL –1 with a detection limit of 3.3 fg mL –1 (S/N = 3). Additionally, the immunosensor had excellent reproducibility, selectivity, and stability, which indicated superior performance for AFP detection compared with previous reports. The satisfactory results of human serum samples analysis showed that the designed immunosensor has potential applicability for the sensitive detection of other tumor markers.
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