Molecular Catalysis
·
2024
·
IF 3.9
Yuwei Liang,Chunling Hu,Peng Chen,Qi Li,Jianning Wu,Zhiyong Liu,Jichang Liu,Yanlong Tai
5-hydroxymethylfurfural (HMF) can catalyte into 2,5-diformylfuran (DFF) which had received much attention as a potential biomass resource. Here, we used a simple and effective method to construct hollow CdS quantum dot (CdS QDs)/MIL-101 heterostructures with high contact area and multiple active sites. The structure of heterostructures could improve photocatalytic activity by charge transfer, photogenerated carrier separation and the multiple refractions of light supported within the hollow-structured CdS QDs. The detailed catalytic mechanism was illustrated by trap agent experiments and electron paramagnetic resonance (EPR) spectroscopy, in which superoxide radicals (·O 2 - ) play a decisive role in the catalytic oxidation of HMF to DFF. Furthermore, the large specific surface area of MIL-101 adsorbs O 2 from the reaction system thereby accelerating the ·O 2 - formation process. Under environmental conditions, 70 % CdS QDs/MIL-101 exhibited optimal catalytic performance. Comparing with pure CdS QDs, the photocurrent enhances 1.8 times, HMF conversion is 1.5 times and DFF selectivity is 1.2 times. This work provide a useful way to improve the conversion of biomass by Z-heterostructures under ambient conditions.
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Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Yuhang Ren,Yu Tian,Yating Lu,Dongyu Nie,Huayi Zhu,Xia Yang
Malathion (MA) is a widely used organophosphorus pesticide globally. Developing efficient photocatalysts is crucial for eliminating MA pollution in water by photocatalytic technology. This study focuses on preparing a series of H-PDI supermolecule/NH 2 -MIL-101(Fe) (PM) materials by amidating NH 2 -MIL-101(Fe) with the more stable H-PDI supermolecule, forming a covalent O C–NH bond. Among these materials, 40 %PM (indicating a mass percentage content of 40 % H-PDI supermolecule in PM) exhibited the best performance for degradation of MA. Under simulated sunlight irradiation of a 10 mg·L 1 MA solution for 180 min, the reaction rate constants of 40 %PM were 5.95 times and 3.13 times higher than those of NH 2 -MIL-101(Fe) and H-PDI supermolecule, respectively. The enhanced performance is attributed to the formation of Z-scheme heterojunctions in the 40 %PM composite lead to fast separation of photogenerated e − and h + . Combining the results of HPLC-MS with Fukui Function, the HOMO, LUMO, and pathway of degradation of MA attracted by 1 O 2 , •OH, and h + were speculated. The pathway involves oxidation, demethylation, P-S bond breakage, decarboxylation, and final conversion to some inorganic molecules. The toxicity of the degradation byproducts were lower than that of MA estimated by Toxicity Estimation Software Tool.
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MICROCHEMICAL JOURNAL
·
2024
·
IF 4.9
Jiejun Li,Lin Li,junjie Fei,Pengcheng Zhao,Jinyao zhao,Yixi Xie
Fenitrothion (FT) is a common organophosphorus pesticide widely used in agricultural. Residues of fenitrothion in crops can adversely affect human health. In this work, modified MIL-125-Fe was prepared by changing the solvent ratios and further etching with iron nitrate, followed by high-temperature pyrolysis to obtain modified-TiO 2 /FeTiO 3 -doped nitrogen-containing carbon framework (m-TiO 2 /FeTiO 3 @NCF). The porous carbon material of m-TiO 2 /FeTiO 3 @NCF was used to modify the GCE to produce FT electrochemical sensor. Under optimized conditions, the sensor exhibited good detection performance for FT with a low LOD of 0.96 nM and a wide detection linear range of 1–9000 nM, and also exhibited good reproducibility (RSD = 2.08 %), repeatability (RSD = 1.09 %) and anti-interference performance. The sensor was successfully applied in real sample tests showing the recovery rates of 98.7 %–101.2 %. The present study provides a new idea for the rapid and accurate detection of FT.
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JOURNAL OF ELECTRONIC MATERIALS
·
2025
·
IF 2.5
Li Lingyu,Ma Qian,Zhao Dongheng,Zhang Huayushuo,Li Bolong
Recently, the development of an n-pentane-sensing product has always been plagued by the lack of suitable inorganic material with good gas-sensing response and selectivity at low operating temperatures. In this work, Ti-MIL-125-induced one-dimensional tubular In 2 O 3 /TiO 2 heterostructures have been fabricated by a facile electrospinning method and a subsequent heat-treatment process. Obvious morphological evolution from a fibrous to a tubular shape with the presence of In 2 O 3 -TiO 2 heterojunctions can be adjusted by varying the added amount of the Ti-ML-125 component. Compared with pure In 2 O 3 , the optimal In 2 O 3 /TiO 2 composites exhibit a blue-shifted energy band (2.52 eV) and an increased specific surface area (227.70 m 2 /g), as well as the enhanced gas-sensing performance on various concentrations of n-pentane. For example, In 2 O 3 /TiO 2 -3% can not only display excellent long-term stability and humidity stability but also has a high response of 670–100 ppm n-pentanol at 50°C, much larger than that of pure In 2 O 3 (50) at 150°C. Significantly, In 2 O 3 /TiO 2 -3% can still reach the high response of 197–100 ppm n-pentanol at room temperature. According to density functional theory (DFT) calculations, the enhanced gas-sensing mechanism is mainly attributed to the combination of the distinctly increased surface active sites through the regulation of morphology and the introduction of effective In 2 O 3 -TiO 2 heterojunctions, which can be beneficial to improving the surface adsorption/desorption characteristics and the electron transport between n-pentanol and the sensing material interface. Graphical
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Biomedical Materials
·
2024
·Vol. 19
·期 2
·025018
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IF 3.9
Antong Jiang,Teng Wang,Xiaoling Lu,Yuxiang Tian,Zihan Jiang,Bin Xu,Hanyuan Zhang,Weijun Fang
The application of both chemotherapy and ferrotherapy together has shown great potential in increasing the effectiveness of cancer treatment. To achieve such a combination, we herein have synthesized Fe3O4 core/MIL-100(Fe) shell nanocomposites (FM) that can be used for tumor chemo-ferroptosis combination therapy. In these nanocomposites, the anticancer drug 10-hydroxycamptothecin (HCPT) and iron ions could be co-delivered into tumors. On one hand, the released HCPT molecules can enter the cell nucleus and bind with DNA, resulting in induction of tumor cell apoptosis. On the other hand, the iron ions could react with H2O2 leading to the production of ROS through the Fenton reaction, thereby triggering tumor cell ferroptosis. Consequently, a superior antitumor effect was achieved through the combination of the apoptosis and ferroptosis. Additionally, the Fe3O4 core endowed FM with high performance for magnetic resonance imaging, which further provided novel avenues for imaging guidance therapy. Therefore, we anticipate that application of these nanocomposites could have great potential in the field of tumor therapy.
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Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Yisha Zheng,Shuoling Lei,Wenjie Guo,Wenlong Xiang,Yanmei Chen,Yanhui Zhang
The high toxicity and persistence of nitroaromatic pollutants pose a serious threat to aquatic ecosystems. In this study, inert SiO 2 was employed as an "inactive enhancer" to construct core-shell MIL-125-NH 2 @ZIF-67/SiO 2 (M@Z/SiO 2 ) heterogeneous MOF catalysts via an epitaxial-wet impregnation method, enabling the efficient reduction of p -nitrophenol ( p -NP) under ambient temperature and pressure. Although SiO 2 itself lacks catalytic activity, the micro-mesoporous network it forms effectively disperses Co active sites and prevents their aggregation. The conversion rate of p -NP increased from 92.5% to 98.4% within 6 min and retained 98% activity after three consecutive cycles. Moreover, the catalyst exhibited excellent stability across a wide pH range (3-11) and in various anionic environments. Mechanistic studies revealed that the interfacial electron transfer between ZIF-67 and MIL-125-NH 2 significantly reduces the activation energy barrier of NaBH 4 . Additionally, the incorporation of SiO 2 not only enhances the mechanical stability of the composite but also optimizes pore structure and substrate mass transfer by modulating surface hydrophilicity. This work provides valuable insights for the precise design of MOF-on-MOF heterostructures and the synergistic engineering of interfacial and surface properties in environmental catalytic materials.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
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IF 9.7
Ziyi Zhang,Huiqing Dong,Dongxu Zhou,Kexin Tang,Yidi Ma,Tao Han,Jianqiu Lei,Shoushuang Huang,Xiaodong Zhang,Liang Tang,Ning Liu
Photocatalytic CO 2 reduction is a promising strategy to address both environmental issues and energy crisis. Defect engineering offers great potential for improving the photocatalytic performance. Herein, we report an innovative approach to introduce defects in MIL-68(In) via electron beam irradiation for the photoreduction of CO 2 into CH 4 . The irradiated X-MIL-68(In) (X mean the irradiation dose) retained the crystal structure and morphology of pristine MIL-68(In), while generating novel organic framework defects. These defects significantly improved the CO 2 photoreduction activity, with 300-MIL-68(In) achieving the highest CH 4 rate of 87.5 μmol g −1 h −1 and a CH 4 selectivity of 74.8 %. Comprehensive ex situ and in situ characterizations, combined with DFT calculations, demonstrated that defects formation in 300-MIL-68(In) accelerated the separation and transfer of photoexcited carriers, thereby driving its superior photocatalytic performance. Furthermore, In situ DRIFTS along with DFT calculations confirmed that ⁎ COOH, ⁎ CHO and ⁎ CH 2 O were key intermediates during CO 2 reduction process. This work highlights electron beam irradiation as an effective strategy for defect engineering, offering new opportunities for tuning the performance of photocatalysts.
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MICROCHEMICAL JOURNAL
·
2025
·
IF 5.1
Lianpeng Lv,Xiaojing Kang,Lubin Hua,Zejian Du,Ruixue Sun,Yefeng Deng,Hailiang Yang,Zheng Xu,Yang Zhou,Bing Wang
Effective identification of excavated leather artifacts assumes a crucial role in the subsequent restoration and protection of the artifacts, and on a deeper level, it holds significant implications for the history and culture represented by the artifacts. Existing approaches fail to address the pain points of micro-trace detection and species identification. In this work, two-dimensional transition metal carbonitrides/carbon nanotubes (MXene/CNTs) and metal organic frameworks (MOFs) were employed as electrochemical immunosensor materials to construct and utilize a sandwich-type immunosensor for the first time to detect leather artifacts. The sensor exhibits a wide linear detection range of 10 −1 –10 3 ng/mL and an extremely low detection limit of 83 pg/mL, which can fulfill the requirements of ultra-sensitive detection. In addition, the sandwich electrochemical immunosensor demonstrates excellent specificity and stability, with the redox peak current value retaining over 95 % of the original value after 10 repeats of cyclic voltammetry (CV) and more than 85 % of the original peak current after one week of differential pulse voltammetry (DPV), with an RSD of 0.767 %. The immunosensor achieves satisfactory outcomes in both qualitative and quantitative detection when analyzing leather artifacts and micro-traces, and its performance surpasses that of existing methods. Therefore, this work not only introduces novel materials for the construction of sandwich immunosensors but also provides new concepts and approaches for archaeological detection of cultural relics.
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MICROCHEMICAL JOURNAL
·
2025
·
IF 5.1
Jing Meng,Moustafa Zahran,Ahmed S. Abou-Elyazed,Xiaolin Li
Herein, we report a novel electrochemical sensor for determining glucose in sweat, employing a graphene/metal–organic framework (MOF) as a modifier for stainless steel (SS) electrode. The MOF structures, MIL-101(Cr), MIL-101(Cr)-NO 2 , and MIL-101(Cr)-NH 2 , were hydrothermally synthesized and then characterized using X-ray diffraction (XRD), Fourier transform infrared (FT-IR) spectroscopy, N 2 adsorption/desorption isotherms, and scanning electron microscopy (SEM). XRD and SEM results proved the formation of the crystalline MIL-101(Cr) and MIL-101(Cr)-NO 2 , and the amorphous MIL-101(Cr)-NH 2 . Additionally, FT-IR and isotherms confirmed their composition and mesoporosity, respectively. The amorphous MIL-101(Cr)-NH 2 showed the best electrocatalytic activity towards glucose oxidation among the fabricated MOFs. The electrocatalytic activity was also boosted after incorporating conductive graphene. Under optimized conditions, graphene/MIL-101(Cr)-NH 2 /SS was used for glucose determination using square wave voltammetry and chronoamperometry with detection limits of 0.004 and 0.01 mM, respectively. Moreover, the modified electrode showed acceptable recovery values when it was applied to detect glucose in artificial sweat samples.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Xianyun Ma,Bowen Zhu,Zuopeng Li,Min Wang,Chang-qing Miao,Yajia Liu,Sanbing Zhang
Defect engineering is a promising approach for constructing highly efficient catalytic activity based on metal–organic frameworks (MOFs). In this study, a defective MOFs, referred to as quasi-MIL-100(Fe), was synthesized by moderate synthesis method and then careful thermal treatment at an atmosphere ranging from 150 to 450 °C, linking crystalline materials and the associated metal oxides. MIL-100(Fe) heat-treated at 250 °C (referred to as M-250) partially breaks coordination bonds, resulting in a crystalline-to-amorphous transformation, increased porosity, and elimination of ligands. Compared to pristine MIL-100(Fe), M-250 possessed more reactive sites and exhibited the highest photo-Fenton degradation of ciprofloxacin with 95.6 % removal efficiency in 90 min, despite the unfavorable photo properties for photo-Fenton performance due to the destruction of the crystal structure. Additionally, density functional theory (DFT) calculations, combined with free radical quenching and mass spectrometry analysis, elucidated the catalytic mechanism. These findings highlight the significant potential of quasi-MOFs for applications in the photo-Fenton reaction.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2025
·
IF 8.3
Jun-Qing Ye,Bin Cheng,Yunfei Bu,Jun-Feng Qian,Qian Liang,Ming-Yang He,Qun Chen
The development of high-efficiency photocatalysts for water splitting to hydrogen (H 2 ) is crucial for alleviating energy crisis and environmental problems. In this study, a novel type-II ternary heterojunction photocatalyst, CDs/NH 2 -MIL-125 (Ti)/Cu 2 O, was fabricated through the integration of NH 2 -MIL-125 (Ti) with Cu 2 O and carbon dots (CDs), exhibited excellent photocatalytic H 2 production rate of 12817.1 μmol/g/h with apparent quantum efficiency (AQE) of 17.13 % under visible light irradiation. Characterization revealed a uniform and dense structural integration with a high Brunauer-Emmett-Teller (BET) surface area of 275.9 m 2 g −1 and a suitable energy band gap of 2.18 eV. Furthermore, the heterostructures promoted efficient photo-generated carrier separation and enhanced reduction capabilities . Notably, CDs, serving as cocatalysts or electron acceptors, improved visible light utilization and electron migration, significantly boosting H 2 production. Insights from electron spin resonance (ESR) and density functional theory (DFT) calculations supported the migration mechanisms of electrons. This work presents a significant advance in photocatalytic technology for sustainable energy by designing high-performance CDs-modified heterojunction photocatalysts.
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TALANTA
·
2016
·
IF 4.035
Guobin Han,Qiaoling Zeng,Zhongwei Jiang,Tiantian Xing,Chengzhi Huang,Yuanfang Li
Matrix-assisted laser desorption/ionization time-of-flight mass spectrometry (MALDI-TOF-MS) has been proven as a useful and advanced technique in the identification of polymers and proteins. However, MALDI-TOF-MS still has the unavoidable drawback of self-signal interference with traditional organic matrices, which could suppress and overlap with the analyte signals in the low-mass region. In this work, MIL-101(Cr), a kind of metal-organic frameworks which possess high molecular weight , π-conjugated 3-D structure, coordinately unsaturated chromium sites (CUS) and strong absorption in the UV range, was employed to replace traditional organic matrices, and it was found that MIL-101(Cr) can dramatically eliminate the background peaks, showing high signal-to-noise level in the analysis of small molecules. As proof-of-concept, quercetin , daidzein , genistein and naringenin , members of flavonol family which widely exists in food and natural products , were successfully determined by utilizing MIL-101(Cr) as the surface-assisted matrix, and the detection of quercetin was sensitive with good salt tolerance and reproducibility. Under optimal conditions, the mass peak intensity exhibited good linear relationships in the range from 0.25 µg/mL-7.00 µg/mL for quercetin ( R 2 =0.996) with detection limit 2.11 ng/mL (3σ/k), making the identification of quercetin in sophora japonica successfully. With this strategy we have demonstrated the potentiality of MIL-101(Cr) nanomaterials as MALDI-MS matrix for the detection of small molecules.
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