FUEL
·
2024
·
IF 6.7
Wei Fu,Muhammad Kashif,Chen Cai,Jiayin Chen,Hao Zhou,Bingtao Zhao,Philippe M. Heynderickx,Yaxin Su
The hydrothermal technique was applied to prepare a new metal–organic framework, MIL-100(Fe), which was modified by ultrasonic impregnation with different wt % of copper. The results showed that the NO x conversion over 2.3Cu-MIL-100(Fe) was 100 % at 275 °C and maintained at ≥ 85 %, with N 2 selectivity ≥ 90 % in the temperature range of 275–400 °C and high SO 2 resistance. An increase in the Cu content up to 2.3 wt% showed the highest surface area (1206 m 2 /g) observed in N 2 adsorption–desorption. The results show that the introduction of Cu increased the oxygen vacancies on the catalyst surface. Electron transfer and a synergistic effect were observed between Cu and Fe. The shift of the reduction peaks to lower temperatures after the addition of Cu confirmed that Cu improved the reducibility of the catalysts. The 2.3Cu-MIL-100(Fe) exhibited the highest Lewis content (44.97 μmol/g), which functions as an active site for the selective catalytic reduction (SCR) reaction. By precisely controlling the acid-base properties of the catalyst, the specificity for the desired products can be increased in complicated reaction systems, especially in hydrocarbon-SCR technology.
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ACS Applied Materials & Interfaces
·
2022
·
IF 10.383
Mingxiong Lin,Yifei Luo,Tingshi Zhang,Xiaoxin Shen,Zanyong Zhuang,Yan Yu
This work disclosed the trade-off effect of two metal sites, which display distinct, key functionalities in naturally occurring and artificial catalysts for developing an advanced CO2 reduction system. To exploit the metal–organic frameworks (MOFs) as advanced catalysts, we prepared a series of Prussian blue analogues (FeNix PBAs) of tunable Ni/Fe molar ratio without changing the oxidation state of Fe and Ni for use as a photocatalyst in the CO2 reduction reaction (CRR). The FeNi0.66 PBA gives a superior CO yield rate (14.28 mmol·g–1·h–1) with nearly 100% CO selectivity, but the PBA would be basically CRR-inactive without either Ni or Fe. Experimental and calculation studies demonstrate that Fe and Ni display distinct functionalities. Specifically, Fe is an efficient mediator that boosts the electron transfer both from the photosensitizer to FeNix PBA and from FeNix PBA to CO2, and Ni serves as the active site for CO2 adsorption and reduction. Intriguingly, when there is already sufficient Ni in the catalyst, further increase of the Ni content gives marginal gains in the CO2 adsorption affinity that cannot offset the weakened electron transfer due to the Ni excess. The findings can help advance the design of bimetallic MOF catalysts that mimic naturally occurring bimetallic catalysts.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2015
·
IF 4.097
Dongfang Wang,Yingchang Ke,Di Guo,Hongxu Guo,Jianhua Chen,Wen Weng
A metal-organic frameworks (MOFs), cauliflower-like MIL-100(Cr), has been facilely prepared through simple reflux method for the first time and characterized by XRD, FT-IR, SEM and XPS. The MOFs was found to be useful for the simultaneous and selective electrochemical detection of microgram Cd(II), Pb(II), Cu(II), and Hg(II) in aqueous solution. The detection was performed by the square wave anodic stripping voltammetry (SWASV). The MIL-100(Cr) modified electrode showed an excellent selectivity and stability for Cd 2+ , Pb 2+ , Cu 2+ , Hg 2+ determinations. The electrochemical properties and applications of the modified electrode were studied. Operational parameters such as pH, deposition potential and deposition time were optimized for the purpose of determination of traces of metal ions .
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ANALYTICA CHIMICA ACTA
·
2022
·
IF 6.911
Ruiming Chen,Shu Xing,Tingting Hu,Yiming Li,Jianbin Chen,Qingfen Niu,Tianduo Li
A new ICT type D-π-A structured chemosensor DTB derived from a bithiophene-benzothiazole derivative has been synthesized. Sensor DTB showed a colorimetric and fluorometric dual-signaling response to hypochlorite (ClO − ) in EtOH/HEPES solution (1/99, V/V, pH = 7.4, nearly 100% aqueous solution). Sensor DTB exhibited well specificity, high sensitivity and rapidity (<1 min) for ClO − with a detection limit of 25 nM. Sensor DTB features remarkable color changes and significant fluorescence “turn-on” response ( ca. 45 fold) after treating with ClO − . Comprehensive analyses by 1 H NMR, TLC , FTIR, HRMS , UV–vis, fluorescence and DFT illustrated that ClO − reacted with the C C bond of DTB , generating fluorophore 2T-CHO , leading to strong blue fluorescence. Interestingly, DTB loaded colorimetric test strips were established for rapid and real-time visual detection of ClO − . Furthermore, the DTB was successfully applied to quantitatively and sensitively detect ClO − in 84 disinfectant, bio-fluids (human serum and urine) and actual water samples. Importantly, the biocompatible DTB has been employed for visualizing and bioimaging ClO − in mung bean sprouts, Arabidopsis , live cells and zebrafish. These investigations demonstrate that DTB has great potentials for detecting ClO − in various biosystems and environments. This work would offer a new idea for developing multifunctional sensors with better performance for chemo/biosensors.
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CHEMISTRY-A EUROPEAN JOURNAL
·
2022
·Vol. 28
·期 68
·e202201985
·
IF 5.02
Hao Zhang,Jixiang Ji,Fa Guo,Zhurui Shen
Graphical The mechanism for alkali-treated photocatalyst in CO 2 photoreduction is studied, especially for demonstrating the role of OH − and metal cations in detail for highly selective production of CO. DFT calculations confirmed that K ions enhance the charge density of nearby atoms to stabilize CO* groups and reduce the reaction energy barrier, inducing the switch of CH 4 to CO. In this work, the modulation of activity and selectivity via photoreduction of carbon dioxide under simulated sunlight was achieved by treating P25 and P25/Pt NPs with KOH. It found that KOH treatment could significantly improve the overall conversion efficiency and switch the selectivity for CO. Photoelectric characterizations and CO 2 -TPD demonstrated that the synergistic effect of K + and OH - accelerated the separation and migration of photogenerated charges, and also improved CO 2 adsorption level. Significantly, the K ions could act as active sites for CO 2 adsorption and further activation. In situ FTIR measurements and DFT calculations confirmed that K + enhanced the charge density of adjacent atoms and stabilize CO* groups, reducing the reaction energy barrier and inducing the switching of original CH 4 to CO, which played a selective regulatory role. This study provides insights into the photocatalytic activity and selectivity of alkali-treated photocatalysts and facilitates the design of efficient and product-specific photocatalysis.
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RSC Advances
·
2026
·Vol. 16
·期 6
·5501-5514
·
IF 4.6
Lian Yu,Baozi Lu,Zhen Liang,Dabin Wang,Jiarui Lu,Fengyi Wei,Cunzhen Liang
The slow rate of the Fe3+/Fe2+ cycle has decreased the efficiency of photo-Fenton technology for wastewater treatment. Here, a novel GO/MIL-100(Fe)@Fe3O4 heterostructure was constructed by growing Fe3O4 nanoparticles and MIL-100(Fe) onto GO, thus accelerating the Fe3+/Fe2+ cycle and improving catalytic activity, and it was used as a heterogeneous photo-Fenton catalyst for ERY degradation. The catalyst was fully characterized by TEM, XRD, Raman spectroscopy, XPS, N2 adsorption–desorption and UV-vis DRS. The influences of initial solution pH, H2O2 concentration and catalyst dosage on ERY degradation were investigated. Under optimal conditions (initial pH of 4.03, 10.0 mM H2O2, 0.1 g L−1 catalyst), the GO/MIL-100(Fe)@Fe3O4 + H2O2 + vis system removed 97.3% of ERY (0.1 mmol L−1) within 60 min, and the pseudo-first-order rate constant was 0.0575 min−1. Furthermore, the catalyst showed favorable stability, maintaining excellent catalytic activity even after 4 cycles. A possible degradation mechanism of ERY was proposed based on the results of characterization, ERY degradation, and reactive species analysis. Fe3O4, MIL-100(Fe) and GO in the catalyst showed synergistic effects; the photo-induced electrons from MIL-100(Fe) could be immediately transferred to Fe3O4, promoting Fe3+ reduction to Fe2+ in the photo-Fenton reaction. GO in the catalyst could promote electron transfer from MIL-100(Fe) and organics to Fe3O4, significantly promoting the Fe3+/Fe2+ cycle.
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Catalysis Science & Technology
·
2026
·
IF 4.2
Tao Liu,Zhenjie Xu,Guangming Zhou,Simiao Yu,Jie Liu,Jian Ke,Gang Lu
Chemical excess sludge, containing viruses, heavy metals, polycyclic aromatic hydrocarbons, and other components, exhibits high toxicity, making its safe disposal an urgent issue. In this work, MIL-100 (Materials of Institut Lavoisier – 100(iron)) was synthesized using 1,3,5-benzenetricarboxylic acid and iron extracted from excess sludge. Additionally, titanium dioxide was loaded onto MIL-100 via an impregnation–calcination method to form T@MIL-100, and their visible-light-driven photocatalytic activities for methylene blue (MB) degradation were evaluated. The results showed that the synthesized MIL-100 exhibited excellent photocatalytic performance for MB degradation, with a degradation efficiency of 92.44% and a corresponding kinetic constant (kobs) of 0.97612 h−1. The degradation efficiency of MB over 1%T@MIL-100 was enhanced to 98.42%, and the kobs value increased to 1.39943 h−1. Quenching experiments further revealed the catalytic mechanism: h+ was the dominant active species in the MIL-100 system, while ·O2− and h+ primarily contributed to MB degradation in the T@MIL-100 system. This study provides a low-cost, efficient, and sustainable approach to convert excess sludge into functional metal–organic frameworks (MOFs) and further load TiO2. This strategy not only promotes the recycling of residual iron in excess sludge to significantly reduce catalyst costs, but also enhances photocatalytic degradation performance, offering an excellent functional material for MB removal.
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MICROCHEMICAL JOURNAL
·
2026
·
IF 5.2
Peng Du,Wei Gao,Zhaohui Huang,Chuqi Jiang,Jiahui Zhang,Dongjun Lv,Luyang Liang,Ling Yin,Xiaolei Zhang,Hongbo Zhang,Huiting Wu
Three-level ET cascade relieves bottleneck. • TMB: 5.8x act., 24.2x eff.. • GSH sensing + redox disruption (depletion/ROS). Nanozyme efficiency is fundamentally constrained by interfacial electron transfer (ET) bottlenecks, yet most strategies overlook the rational design of ET pathways. Herein, a ternary NiMo 6 @MIL-100(Fe)/g-C 3 N 4 nanozyme featuring a hierarchical three-level ET cascade was reported: TMB substrates are preconcentrated onto g-C 3 N 4 via π–π stacking (Level I); electrons transfer from g-C 3 N 4 to Fe 3+ nodes of MIL-100(Fe) through interfacial Fe O C bonds (Level II); and finally cascade into the encapsulated NiMo 6 cluster for H 2 O 2 activation and •OH generation (Level III). This design yields higher activity than binary (1.8-fold) and pristine counterparts (5.8-fold), with a 24.2-fold enhancement in catalytic efficiency for TMB. By leveraging glutathione (GSH) as a specific electron cascade interceptor, a colorimetric assay achieves a detection limit of 0.36 μM with excellent selectivity over structurally similar thiols. Beyond sensing, the same cascade efficiently depletes GSH and induces intracellular ROS bursts in HepG2 cells, disrupting tumor redox homeostasis and highlighting its therapeutic potential and establishing a mechanism-driven paradigm for biosensing and cancer therapy. A hierarchical three-level ET cascade transforms electron bottlenecks into a superhighway for GSH sensing and tumor redox therapy. Download: Download high-res image (274KB) Download: Download full-size image
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Materials Today Communications
·
2022
·
IF 3.662
Tao Wei,Zhimeng Wang,Mi Zhang,Qi Zhang,Jiahao Lu,Yanyan Zhou,Cheng Sun,Zidong Yu,Yu Wang,Man Qiao,Sai Qin
As a common filler in polymer electrolytes , Metal-organic frameworks (MOFs) has been studied extensively in recent years. In this study, we propose a novel solid composite electrolytes (SCEs) based on PEO/LiTFSI/a-MIL-100 (Fe)/PVDF by using a straightforward solution-casting method. Unactivated and activated MIL-100 (Fe) (a-MIL-100 (Fe)) as the fillers were compared, and the interactions of functional groups of unactivated MIL-100 (Fe) and a-MIL-100 (Fe) with anions of electrolyte salts through Lewis acid-base interaction are studied with density functional theory (DFT) calculations. The influences of different a-MIL-100 (Fe) contents on electrochemical performances were also examined. The Li/SCEs/LiFePO 4 cell displayed high average discharge capacities of 161.8 mAh g −1 , 166.8 mAh g −1 , 158.9 mAh g −1 , 146.2 mAh g −1 and 92.6 mAh g −1 at the rate of 0.1, 0.2, 0.5, 1 and 2 C at 60 ℃, respectively, without liquid electrolytes. This work might provide new insight into the role of activated MOFs fillers in polymer electrolytes.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2020
·
IF 3.573
Xing-Zhe Guo,Shuai-Shuai Han,Ji-Min Yang,Xiao-Meng Wang,Shui-Sheng Chen,Shuai Quan
We herein report that the morphology, size, and surface charge status of MIL-100(Fe) micro/nanoparticles can be tailored by adding a coordination modulator (HF or tetramethylammonium hydroxide) to the reaction system. Interestingly, the adsorption capacities of low-crystallinity MIL-100(Fe) and MIL-100(Fe)-TMA toward Congo red (CR) and acid chrome blue K (AC) were found to be significantly larger than that of the high-crystallinity MIL-100(Fe)-HF adsorbent, whereas there was little difference in the adsorption capacities of the three MIL-100(Fe) toward methyl orange (MO) and methylene blue (MB). The adsorption uptake of MIL-100-(Fe)-TMA toward the anionic dyes (CR, AC, and MO) was found to be highest, whereas the adsorption uptake of MIL-100(Fe) toward the cationic dye (MB) was the highest owing to different adsorption mechanisms. This adsorption behavior could be rationalized based on the morphological characteristics and crystal structure defects, zeta potential, and pore volume of MIL-100(Fe) and the adsorption characteristics and molecular structure of the dye. It was revealed that the adsorption performance of MIL-100(Fe) micro/nanoparticles is governed by the synergistic interplay between electrostatic, hydrophobic, and π–π stacking interactions, pore volume, crystal structure defects, and steric hindrance of the adsorbent.
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ANALYST
·
2023
·Vol. 148
·期 12
·2725-2731
·
IF 4.2
Yuhan Ji,Yupu Wei,Jinghui Shen,Jinlong Zhuo,Mingqi Xu,Yunliang Wang,Jingquan Sha
To improve the peroxidase-like activities of metal–organic frameworks (MOFs) as nanozymes, a ternary MIL-100(Fe)@PMo12@3DGO nanocomposite was designed and fabricated by encapsulating Keggin-type H3PMo12O40 (PMo12) with fast and reversible multi-electron redox processes and an electron-rich structure into MIL-100(Fe), then being covered by three-dimensional graphene (3DGO) with higher conductivity, larger surface area, higher porosity, and better chemical stability. As a consequence, the as-prepared MIL-100(Fe)@PMo12@3DGO nanocomposite exhibits excellent peroxidase-like activities, namely, the lowest limit of detection (0.14 μM) in the range of 1–100 μM for glucose to date, to the best of our knowledge, attributed to the individual and synergistic effects of H3PMo12O40, 3DGO and MIL-100(Fe).
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Nanotechnology Reviews
·
2023
·Vol. 12
·期 1
·
IF 7.4
Ke Chen,Xudong Yang,Rui Hao,Minghui Shao,Xiaoyong Yang,Xiuze Li,Yuxuan Li,Juzhe Liu,Sai Zhang
Activation of peroxymonosulfate (PMS) to degrade persistent organic contaminants has received increasing attention in wastewater purification. In this study, Cu 2 O catalysts with different exposed crystal facets were prepared, characterized, and evaluated for acetaminophen (ACE) degradation through PMS activation. The experimental results showed that cubic Cu 2 O with {100} facets exhibited remarkable activity on ACE removal by PMS activation in wide pH range of 3–11. DFT calculations indicated that Cu 2 O-{100} displayed higher electron transfer efficiency and PMS adsorption ability, further improving PMS activation. The radicals quenching experiments and electron paramagnetic resonance (EPR) results illustrated that singlet oxygen ( 1 O 2 ) was dominant reactive oxidative species (ROSs) during oxidation reactions and the relevant generation pathways were distinctly elucidated. Finally, the possible PMS activation mechanisms were discussed for ACE degradation in a wide pH range. This study will provide new insights to disclose PMS-based advanced oxidation processes (AOPs), and offer a new approach for wastewater purification by non-radical reactions.
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