RENEWABLE ENERGY
·
2025
·
IF 9.1
Jingchuan Guo,Yan Gao,Xuankai Cao,Linxuan Li,Xin Yu,Shidan Chi,Haoyu Liu,Guohong Tian,Xudong Zhao
The technology of using electricity generated from renewable energy sources such as wind and solar power for water electrolysis to produce hydrogen has achieved high efficiency, high purity, and environmental friendliness. However, its further development is constrained by the high overpotential of the oxygen evolution reaction (OER) and the high cost of precious metal catalysts. The methanol oxidation reaction (MOR) as an alternative to OER can significantly reduce overall energy consumption and accelerate the hydrogen evolution reaction. This study innovatively utilizes the metal-organic framework (MOF) of NH₂-MIL-88(Fe) to introduce Ni doping, preparing a series of Fe x Ni y -MOF and their bimetallic carbon derivatives (Fe x Ni y /C) through solvothermal synthesis and high-temperature carbonization. Results show that FeNi₂/C exhibited excellent performance in OER, with a Tafel slope of 38.69 mV·dec⁻ 1 and an overpotential of 335 mV at 10 mA cm⁻ 2 , comparable to RuO₂. In MOR, the overpotential was 193 mV, reduced by approximately 140 mV compared to OER, with outstanding stability. The catalytic mechanism was analyzed using ion chromatography, revealing the key role of Ni doping in enhancing catalytic activity and stability. This study provides new strategies for improving the electrocatalytic hydrogen production efficiency of renewable energy and reducing the production cost of hydrogen energy.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Yadan Luo,Chenguang Li,Zhen Liu,Wei Guo,Cuizhu Sun,Shasha Zhao,Qian Wang,Yuanyuan Li,Lingyun Chen,Hao Zheng,Fengmin Li
Phthalates (PAEs) are known to pose a serious threat to the environment and human health duo to their endocrine disrupting effects, thus a great deal of effort has been made to develop destruction technologies for PAEs treatment in the water environment, such as peroxymonosulfate (PMS)-based advanced oxidation technology. Here we prepared an environmentally friendly visible light catalyzer, a heterojunction of carbonitride nanosheets (CNN) doped with NH 2 -iron metal organic frameworks (NH 2 -MIL-101(Fe)), for the activation of PMS to efficaciously remove two representative PAEs—diisobutyl phthalate (DIBP) and diethyl phthalate (DEP)—from the aquatic environment. The CNN@NH 2 -MIL-101(Fe) photocatalyst possesses an excellent visible light harvesting performance with a narrow band gap (1.66 eV), low recombination ratio of photoinduced carriers, and long charge lifetime. The pore volume and surface area of the composite material was increased compared with any single component. The optimum CNN@NH 2 -MIL-101(Fe) catalyst manifested the high performance to activate PMS to degrade DIBP and DEP under visible irradiation with maximum removal of 94.5 ± 2.2 % and 83.4 ± 0.9 %, respectively. Four main active species (•OH, O 2 − •, SO 4 − •, and h + ) were involved in PAEs photodegradation, with h + and SO 4 − • playing a key role in the degradation of DIBP, and h + in the degradation of DEP. The degradation mechanism of DIBP and DEP mainly involved the ester bond cleavage and oxidation by active species. Additionally, the CNN@NH 2 -MIL-101(Fe) heterojunction exhibited high and stable catalytic performance to activate PMS for PAEs destruction under pH 3 – 9. Therefore, this study provides a new strategy for designing and selecting environment-friendly treatment approach for the effective eradication of PAEs via a PMS-based advanced oxidation process.
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TALANTA
·
2024
·
IF 5.6
Yuting Zhou,Xiang Chen,Xianlu Lei,Meiqi Huang,Miaomiao Ma,Jian Zeng,Fuyan Zhang,Shuang Li,Qi Sun,Tao Le
Zearalenone (ZEN), a prevalent mycotoxin found in cereal crops, poses a significant threat to food safety and human health. To address this issue, there is an urgent need for rapid, sensitive, and cost-effective detection methods. In this study, we developed a novel bimodal aptasensor based on NH 2 -UiO-66@MB composites for ZEN detection. Methylene blue (MB) was encapsulated within NH 2 -UiO-66 nanoparticles to enhance fluorescence intensity, and the ZEN aptamer was attached to NH 2 -UiO-66 via Zr–O–P bonds and Coulombic forces to create a gating effect. In the presence of ZEN, the aptamer bounded to ZEN, triggering a conformational change that released MB, resulting in decreased fluorescence intensity and absorbance. Under optimal conditions, the bimodal aptasensor exhibited wide linear ranges (2.5–300 ng/mL for colorimetry and 0.125–200 ng/mL for fluorescence) and low limits of detection (1.16 ng/mL for colorimetry and 0.03 ng/mL for fluorescence). Furthermore, the aptasensor demonstrated high specificity and reproducibility, with recovery rates ranging from 97.43 % to 103.71 % in spiked cereal products. These findings highlight the potential of the developed bimodal aptasensor as a novel tool for the rapid, accurate, and cost-effective detection of ZEN in cereal products, contributing to improved food safety monitoring.
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PubMed
高影响因子
RENEWABLE ENERGY
·
2024
·
IF 9
Wenli Zhang,Jifei Liu,Hongwei Gu,Cheng Pan,Yifei Long,Qunpeng Cheng,Guozhi Fan
The metal-organic framework materials ZIF-8 and UiO-66-NH 2 , synthesized by hydrothermal methods, were characterized in detail and combined to catalyze the transfer hydrogenation of 5-hydroxymethylfurfural (5-HMF) to 2,5-di(hydroxymethyl)furan (2,5-DHMF) using isopropanol as the hydrogen source. The ZIF-8/UiO-66-NH 2 catalyst mixture exhibited abundant Lewis acid-base sites and a hierarchical multiporous structure with a large specific surface area (564.0 m 2 /g). The conversion of 5-HMF reached 98.2 %, and the selectivity and yield of 2,5-DHMF were 96.2 % and 94.5 %, respectively. The recycling performance of ZIF-8/UiO-66-NH 2 was also investigated, and the conversion of 5-HMF and selectivity of 2,5-DHMF significantly decreased to 78.4 % and 79.1 % in the second run, respectively. The loss of −NH 2 groups was found to be the main reason for the decrease in activity. However, the catalytic activity of the recovered catalyst can be almost completely restored by the addition of a small amount of fresh UiO-66-NH 2 and ZIF-8, and the conversion of 5-HMF and selectivity of 2,5-DHMF were increased to 89.4 % and 95.5 %, respectively. In the proposed reaction mechanism, Lewis acid-base sites play important roles and exhibit a synergistic catalytic effect in the selective conversion of 5-HMF to 2,5-DHMF.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2025
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IF 7.7
Jiaqi Chang,Fengsen Wang,Peng Zhang,Jiaqi Li,Xi Zhang,Fanhong Chen,Qianrui Lv
The controllable pore structures and surface functionalization characteristics of metal-organic frameworks (MOFs) provide new ideas for the development of high-performance humidity sensors. In this study, a hierarchical porous IL/UIO-66-NH 2 material with well-defined microporous-mesoporous channels was successfully synthesized. This unique porous structure results from the steric hindrance effect and competitive coordination of a carboxylic acid-functionalized ionic liquid used as the MOF precursor. By combining the Kelvin equation with Fick's law of diffusion, we revealed how the synergistic interactions within hierarchical pore structures enhance water-molecule transport dynamics, resulting in ultrafast sensor performance with response and recovery times of 0.6 s and 0.9 s, respectively. The humidity sensing mechanism was systematically investigated using electrochemical impedance spectroscopy. The sensor can accurately distinguish respiratory states and recognize short speech signals, providing a new material design strategy for wearable health monitoring devices.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Jingling Gong,Bin Xiang,Ruirui Jin,Zhaoyang Li,Weimin Liu,Jian Li
Membrane fouling is a key challenge to the sustainable operation of oil–water separation membranes. Constructing a stable hydration layer on the membrane surface as an oil-fouling resistance barrier by modulating the physicochemical structure of the membrane is one of the most effective strategies. Herein, inspired by the petal structure in nature, Cu 3 (PO 4 ) 2 and UiO-66-NH 2 particles were combined by a self-assembly strategy to construct CUP (Cu 3 (PO 4 ) 2 /UiO-66-NH 2 /PVA) composite membranes with anti-fouling capability against viscous crude oil. Benefiting from the petal structure and abundant polar groups within the membrane, the as-prepared membrane could easily combine with water molecules to form a stable hydration layer, which acted as a barrier to hinder the oil contamination of the membrane. Further, the hierarchical flower-like structure was conducive to the improvement of the emulsion breaking rate and permeation flux of oil-in-water emulsions. After 60 min continuous cross-flow separation, the obtained CUP composite membrane still remained prominent separation efficiency (99.6 %) and permeate flux (4685.96 LMH/bar). In addition, the CUP composite membranes showed outstanding resistance to acid and alkali as well as abrasion. This study provides an effective method for the advancement of high-performance membranes with high flux and anti-fouling capability in the flied of oily wastewater treatment.
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APPLIED SURFACE SCIENCE
·
2025
·
IF 6.9
Yue Wang,Wenjun Zhang,Yanjun Zhang,Meng Chen
Metal-organic frameworks (MOFs), with tunable morphologies and porous architectures, show great potential in photocatalysis. A variety of MOFs can be synthesized by changing the types of metal ions and organic ligands. However, fewer studies have explored the influence of the metal-to-ligand molar ratio on the catalytic performance of the resulting MOF-related products. In this work, capsule-shaped NH 2 -MIL-68(In)/InOOH composites were synthesized by adjusting molar ratios of In(NO 3 ) 3 to 2-aminoterephthalic acid. Time-dependent characterization revealed sequential crystallization: rod-shaped NH 2 -MIL-68(In) initially formed in the solution, followed by the in-situ growth of InOOH nanowires on its surfaces via excess indium ions, ultimately constructing a Z-scheme heterojunction. The optimized NM/InOOH (8:1) composite exhibited a larger specific surface area and extended light absorption. The Z-scheme configuration significantly promoted charge carrier separation efficiency while maintaining strong redox potentials of the photoinduced holes and electrons, thereby resulting in 5–8-fold improvement in degradation rates for four dyes (AOII, RhB, MB, and Rh6G), highlighting its broad photocatalytic applicability.
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JOURNAL OF MEMBRANE SCIENCE
·
2025
·
IF 9
Ziheng Li,Fengting Yao,Yan Dai,Xuehua Ruan,Xiaobin Jiang,Xuemei Wu,Wenji Zheng,Gaohong He
Metal-organic frameworks (MOFs) offer exceptional pore tunability for targeted separations. Moving beyond conventional defect engineering which often sacrifices selectivity for permeability, we propose to construct functionalized defects that synergistically integrate hierarchical low-resistance gas transfer pathways with tailored ultra-CO 2 -philic molecular domains. This strategy is achieved by in-situ embedding β-cyclodextrin (β-CD) as a multifunctional modulator during the crystallization of NH 2 -UiO-66 (NUiO). The macrocyclic cavities of β-CD induced structural defects cooperatively optimize the pore architecture of NH 2 -UiO-66, significantly enhancing gas permeability. Concurrently, exposed Zr 6 clusters and hydroxyl groups from β-CD enhance CO 2 adsorption capacity. Furthermore, defect-induced incomplete coordination promotes hydrogen bonding between the β-CD@NUiO and Pebax, improving interfacial compatibility for MMMs. The prepared β-CD 20 @NUiO MMM at 5 wt.% filler loading exhibits a CO 2 permeability of 125.5 Barrer and a CO 2 /N 2 selectivity of 112.4, exceeding the 2019 McKeown upper bound. The in-situ construction of defects via functional molecules transcends the limitations of single-parameter optimization for mass transfer pathways and active sites in porous materials, establishing a universal design principle for multifunctional coupled separation materials.
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ACS Sustainable Chemistry & Engineering
·
2025
·
IF 7.3
Meng Xia,Longqi Li,Xiaocong Wang,Kaihao Xu,Shuai Zhang,Chengxue Zhang
During CO2/HCO3– reduction with renewable biomass, achieving high-efficiency production of the target products is vital but challenging. In this study, an NH2– functional-group-modified MIL-53(Fe) catalyst was synthesized using a facile and efficient method. Under the action of the NH2-MIL-53(Fe) catalyst, a clear synergistic effect was exhibited on the transformation of glucose and NaHCO3 into formic acid with a high yield of 50% at a low reaction temperature (190 °C) via a three-pronged route, which mainly involved the decomposition of intermediates of glucose to gradually reduce NaHCO3 to formic acid under hydrothermal conditions. An in-depth analysis of the catalytic mechanism and density functional theory calculations demonstrated that the increased alkalinity of active sites by the NH2– functional group incorporation into the catalytic system enhanced the crucial reaction steps and reduced the activation energy of the crucial reactions, including glucose isomerization, aldehyde intermediate retro-aldol condensation, and redox of aldehyde compounds and NaHCO3 to formic acid, thereby promoting the generation of target products and suppressing side products. This study addresses the challenge of reducing NaHCO3 from renewable biomass to commercial formic acid by constructing multifunctional active sites, thus providing a new strategy for achieving carbon cycling.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Shihui Wang,Yuzhou Xia,Guiyang Yan,Meixia Chen,Xuxu Wang,Ling Wu,Ruowen Liang
Inspired by the concept of frustrated Lewis pairs (FLPs) from homogeneous catalysis, an organic supramolecular bridged metal-organic frameworks (MOFs) heterojunction, i.e., a perylene-3,4,9,10-tetracarboxylic diimide@MIL-125(Ti)-NH 2 (denoted PDI@MTi) composite is successfully fabricated via a two-step synthesis method. Experimental characterisations and theoretical calculations reveal that in the obtained “TiO 5−x -ligand-PDI” FLPs, the unsaturated Ti-O clusters function as a Lewis acid to accept photogenerated electrons, and the PDI sites act as a Lewis base to capture photogenerated holes. With the unique structure characteristics, the PDI@MTi shows excellent photocatalytic activity toward the disinfection of Staphylococcus aureus and Cr(VI) reduction, with 1.0- and 10.3-fold enhancements, respectively, compared with unadorned MTi. The synergic effects of the micro polarisation field, multiple active sites, and a C-N bonded interface contributed to photoactivity enhancement. This work demonstrates the potential of using MTi as a platform for constructing FLPs-containing heterogeneous photocatalysts and provides new strategies to control carrier separation.
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JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2024
·Vol. 171
·期 3
·037526
·
IF 3.1
Deyong Kang,Shanbao Ma,Qiaoling Zheng
Squamous cell carcinoma antigen (SCCA) is an important biomarker in the diagnose of cancer, so developing effective methods for its detection is of great significance. In the present work, a novel sandwich-like electrochemical immunosensing assay (STEM) of SCCA was constructed by preparing gold nanoparticle/reduced graphene-oxide (Au NPs/rGO) to immobilize primary antibody (PAb) of SCCA and UIO-66-NH2 MOFs structure to immobilize second antibody (SAb) and electroactive toluidine blue (Tb) probe. In this designed STEM assay, the prepared Au NPs/rGO nanohybrid offers the advantages in large surface area and conductivity as carrier, and UIO-66-NH2 provided an ideal platform to accommodate SAb and a large number of Tb molecules as signal amplifier. In the existence of SCCA, the current peaks of Tb from the formed STEM structure increase with the increase of SCCA level. After optimizing the related control factors, a wide linear range (0.01 pg ml−1 and 15.0 ng ml−1) and very low detection limit (0.003 pg ml−1) of SCCA was achieved, it's thus expected the designed STEM strategy has important applications for the detection of SCCA.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Xiaoxia Liang,Jiakang Duan,Yu Tian,Yue Han,Zewan Qin,Huixia Zhu,Yating Lu,Dongyu Nie,Yingna Guo,Xia Yang
AgCl/Ag 0 shows great promise for the removal of environmental pollutants, while its photocatalytic performance is still a great challenge on account of the agglomeration. Herein, orientational deposited and octahedral AgCl/Ag 0 were obtained by etching the UiO-66-NH 2 template for the first time. The 0.35:1–AgCl/Ag 0 exhibited outstanding efficiency in the degradation of Diazinon (DZN), which was closely 300 times than that of UiO-66-NH 2 and 0.35:1–AgCl@Ag 0 prepared without a template. Its bigger surface area provided more active sites to promote mass transfer efficiency and large amounts of •OH and 1 O 2 were fabricated to offense specific positions of DZN determined through Fukui function. Meanwhile, a high removal rate of 91.0 % was obtained after 5 recycles. Finally, the results of HPLC-MS, T.E.S.T., TOC and IC indicated all intermediates had less toxicity than DZN and were rapidly mineralized. Our work developed a new strategy for designing superb performance AgCl/Ag 0 photocatalysts.
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