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Tungsten · 2024 · IF 5.6

Highly effective photocatalytic decomposition of tetracycline and reduction of Cr(VI) under visible light using Ag/polyoxometalate composite nanomaterials prepared by a mild grinding method

Lan Qing,Jin Su-Juan,Liu Ying,Jin Xiao-Li,Xie Hai-Quan,Li Yu-Zhu,Liu Ke-Cheng,Chen Li

With environmental issues gaining increasing attention, the demand for developing economical and reusable catalysts has become increasingly critical. Although precious metal catalysts are effective in photocatalytic pollutant decomposition and Cr(VI) reduction, their high price, instability, and recovery difficulty constrain their application. This study introduces an approach where Ag + ions are exchanged with cations in polyoxometalate (POM) via a mild grinding method, followed by in situ illumination under ultraviolet light to produce Ag/Ag-POM composite nanomaterials. Upon interaction with POM clusters, Ag + ions are reduced to Ag nanoparticles, which enhances visible light absorption in the composite, thereby improving its photocatalytic efficiency. Ag/Ag-POM nanomaterials obtained from this process exhibit efficient and stable catalytic performance, efficiently degrading tetracycline (TC) and reducing hexavalent chromium (Cr(VI)) under visible light (λ > 420 nm). Especially, the Ag/AgHPMo 11 V composite demonstrated superior catalytic performance, achieving degradation efficiencies of 99.9% for 40 mg·L −1 TC. Moreover, it also exhibited efficient photoreduction of Cr(VI), achieving a reduction rate of 62.81% for 80 mg·L −1 Cr(VI) in a 100 mL solution using just 10 mg of the catalyst within 40 min of visible-light exposure. This research highlights the potential of polyoxometalate-based catalysts in the photocatalytic treatment of pollutants.

研究领域: 环境科学 · 材料科学
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ENVIRONMENTAL RESEARCH · 2024 · IF 7.7

Preparation of core-shell structure Ag@TiO2 plasma photocatalysts and reduction of Cr(VI): Size dependent and LSPR effect

Jiwen Li,Yaqian Duan,Linlin Wang,Jingjun Ma

The poor light absorption and low carrier separation efficiency of Titanium dioxide (TiO 2 ) limit its further application. The introduction of plasma metal Ag have the potential to solve these drawbacks owing to its plasma resonance effect. Thus core-shell structure Ag@TiO 2 plasma photocatalysts was prepared by using facile reduction method in this work. More specifically, Ag@TiO 2 composite catalysts with different Ag loading amounts were prepared in the presence of surfactant PVP. Ag@TiO 2 demonstrates excellent light absorption performance and photoelectric separation efficiency compared with pure TiO 2 . As a result, it displays excellent performance of Cr(VI) reduction under visible light. The optimal composite catalysts Ag@TiO 2 –5P achieves exceptional visible-light-driven photocatalytic Cr(VI) reduction efficiency of 0.01416 min −1 that is 2.29 times greater than pure TiO 2 . To investigate the role of PVP, we also synthesized Ag@TiO 2 -5 without PVP. The experimental results show that although Ag@TiO 2 -5 Cr(VI) reduction performance is superior to pure TiO 2 , it significantly decreases compared with Ag@TiO 2 –5P. The results of TEM and optoelectronic testing show that agglomeration of Ag particles leads to a decrease in the photoelectric separation efficiency of Ag@TiO 2 -5. The smaller Ag particles provide more active sites and demonstrating a stronger overall local surface plasmon resonance (LSPR) effect. DMPO spin-trapping ESR spectra testing indicates that ∙O 2 − and ∙OH are the main reactive species. This research provides a potential strategy to prepare Ag-based plasma photocatalysts for environment protection.

CAS / MDL: 2226-96-2 102-71-6
研究领域: 材料科学 · 环境科学
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MOLECULES · 2024 ·Vol. 29 ·期 22 ·5418 · IF 4.2

Photocatalytic Enhancement and Recyclability in Visible-Light-Responsive 2D/2D g-C3N4/BiOI p-n Heterojunctions via a Z-Scheme Charge Transfer Mechanism

Shuo Yang,Tianna Wu,Kaiyue Li,Ping Huang,Wenhui Li,Yuquan Zhuo,Keyan Liu,Ziwen Yang,Donglai Han

With the intensification of the energy crisis and the growing concern over environmental pollution, particularly the discharge of organic dye pollutants in industrial wastewater, photocatalytic degradation of these contaminants using solar energy has emerged as an effective, eco-friendly solution. In this study, we successfully synthesized 2D/2D g-C3N4/BiOI p-n heterojunctions via a simple precipitation method and a high-temperature calcination method. The unique 2D structures of g-C3N4nanosheets (NSs) and BiOI NSs, coupled with the synergistic effect between the two materials, significantly enhanced the photocatalytic degradation performance of the heterojunctions under simulated sunlight. The band structures, as determined by Tauc curves, Mott–Schottky curves and XPS-VB analysis, revealed a Z-scheme charge transfer mechanism that efficiently reduced charge carrier recombination and improved electron–hole separation. The photocatalytic activity of 2D/2D g-C3N4/BiOI p-n heterojunctions for rhodamine B (Rh B) degradation reached 99.7% efficiency within 60 min, a 2.37-fold and 1.27-fold improvement over pristine BiOI NSs and g-C3N4NSs, respectively. Furthermore, the heterojunction exhibited excellent recyclability stability, with the degradation efficiency decreasing by only 1.2% after five cycles. Radical scavenging experiments confirmed the involvement of superoxide radicals (∙O2−) and hydroxyl radicals (∙OH) as the primary reactive species in the degradation process. This work highlights the potential of 2D/2D g-C3N4/BiOI p-n heterojunctions for efficient photocatalytic applications in environmental remediation.

研究领域: 环境科学 · 材料科学
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Microsystems & Nanoengineering · 2024 ·Vol. 10 ·期 1 ·1-13 · IF 7.3

Simultaneous photocatalytic degradation and SERS detection of tetracycline with self-sustainable and recyclable ternary PI/TiO2/Ag flexible microfibers

Han Donglai,Guo Boyang,Li Yanru,Feng Wei,Liu Keyan,Wu Tianna,Wan Yuchun,Wang Lili,Gao Ming,Liu Yang,Yang Lili,Wei Maobin,Yang Shuo

Facile and efficient photocatalysts using sunlight, as well as fast and sensitive surface-enhanced Raman spectroscopy (SERS) substrates, are urgently needed for practical degradation of tetracycline (TC). To meet these requirements, a new paradigm for PI/TiO 2 /Ag organic‒inorganic ternary flexible microfibers based on semiconducting titanium dioxide (TiO 2 ), the noble metal silver (Ag) and the conjugated polymer polyimide (PI) was developed by engineering a simple method. Under sunlight, the photocatalytic characteristics of the PI/TiO 2 /Ag flexible microfibers containing varying amounts of Ag quantum dots (QDs) were evaluated with photocatalytic degradation of TC in aqueous solution. The results demonstrated that the amount of Ag affected the photocatalytic activity. Among the tested samples, PI/TiO 2 /Ag-0.07 (93.1%) exhibited a higher photocatalytic degradation rate than PI/TiO 2 (25.7%), PI/TiO 2 /Ag-0.05 (77.7%), and PI/TiO 2 /Ag-0.09 (63.3%). This observation and evaluation conducted in the present work strongly indicated a charge transfer mechanism. Moreover, the PI/TiO 2 /Ag-0.07 flexible microfibers exhibited highly sensitive SERS detection, as demonstrated by the observation of the Raman peaks for TC even at an extremely low concentration of 10 –10 moles per liter. The excellent photocatalytic performance and SERS detection capability of the PI/TiO 2 /Ag flexible microfibers arose from the Schottky barrier formed between Ag and TiO 2 and also from the outstanding plasmonic resonance and visible light absorptivity of Ag, along with immobilization by the PI. The successful synthesis of PI/TiO 2 /Ag flexible microfibers holds significant promise for sensitive detection and efficient photocatalytic degradation of antibiotics.

研究领域: 环境科学 · 材料科学 · 分析化学
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ADVANCED FUNCTIONAL MATERIALS · 2024 · IF 18.5

Hierarchically Porous Carbon Colloidal Aerogels for Highly Efficient Flow Cells

Yinglai Hou,Zhizhi Sheng,Mengchuang Zhang,Kaifa Lin,Jie Kong,Xuetong Zhang

Electrodes with high active areas often compromise with limited ion transport kinetics in flow electrochemical devices. Herein, hierarchically porous carbon colloidal aerogels (HPCCAs) are constructed with multiscale porosities to meet the tradeoff between highly active areas and efficient mass transfer behavior. It is realized by introducing multiphase co-separation in a sol-gel transition process of aramid nanofibers/polyvinylpyrrolidone/carbon nanotubes followed by subsequent freeze-drying and carbonization. The resulting HPCCA possesses a high volumetric electrochemically accessible surface area (3.27 × 10 7 m −1 ) and excellent mass transfer efficiency, 2–3 times higher permeability than commercial Toray carbon paper and 9.86 times higher than bare aerogel. An all-vanadium single cell with HPCCAs as electrodes possesses a high energy efficiency of 83.18% under the current density of 100 mA cm −2 , which is 10–31% higher than most of the state-of-the-art carbon electrode materials including commercial carbon papers. In addition, the cell with HPCCAs shows outstanding long-term stability up to 1000 cycles. Notably, HPCCAs are applicable to more flow battery systems, such as iron/chromium (Fe/Cr), iron/vanadium (Fe/V), zinc/bromine (Zn/Br), vanadium/methylene blue (V/MB), sodium salt of flavin mononucleotide/potassium ferrocyanide (FMN-Na/K 4 [Fe(CN) 6 ]), and methyl viologen/4-hydroxy-2,2,6,6-tetramethyl-piperidin-1-oxyl (MV/4-HO-TEMPO). This work offers a new chemistry paradigm for developing advanced nanoporous aerogel materials and paves the way toward highly efficient flow electrochemical devices.

研究领域: 材料科学 · 电化学 · 储能技术
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MOLECULES · 2024 ·Vol. 29 ·期 17 ·4120 · IF 4.2

Investigation into the Synergistic Effect of the Zinc Peroxide/Peroxymonosulfate Double-Oxidation System for the Efficient Degradation of Tetracycline

Shefeng Li,Yong Zhang,Siyu Ding,Xuli Li,Wei Wang,Ningning Dong,Miaomiao Nie,Pei Chen

The increasingly severe antibiotic pollution has become one of the most critical issues. In this study, a zinc peroxide/peroxymonosulfate (ZnO2/PMS) double-oxidation system was developed for tetracycline (TC) degradation. A small amount of ZnO2(10 mg) and PMS (30 mg) could effectively degrade 82.8% of TC (100 mL, 50 mg/L), and the degradation process could be well described by the pseudo-second-order kinetic model. Meanwhile, the ZnO2/PMS double-oxidation system showed high adaptability in terms of reaction temperature (2–40 °C), initial pH value (4–12), common inorganic anions (Cl−, NO3−, SO42−and HCO3−), natural water source and organic pollutant type. The quenching experiment and electron paramagnetic resonance (EPR) characterization results confirmed that the main reactive oxygen species (ROS) was singlet oxygen (1O2). Moreover, three possible pathways of TC degradation were deduced according to the analyses of intermediates. On the basis of comparative characterization and experiment results, a synergistic activation mechanism was further proposed for the ZnO2/PMS double-oxidation system, accounting for the superior degradation performance. The released OH−and H2O2from ZnO2could activate PMS to produce major1O2and minor superoxide radicals (•O2−), respectively.

研究领域: 环境科学 · 化学工程 · 生物学
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JOURNAL OF HAZARDOUS MATERIALS · 2024 · IF 12.2

Insight on the optimized electronic structure of carbon nitride on ultrafast water treatment via photocatalytic activation of ferrate

Ningxuan Xue,Zhaobing Guo,Xinyu Gai,Yiyang Chen,Siyue He,Guanjie Lin,Fengling Liu,Shuai Zhang,Pengxiang Qiu

Ferrate (Fe(VI)) is a widely used water purifier and is easily affected by external factors. Given that the actual water environment conditions are complicated, this study designed an oxygen-doped carbon nitride (CNO) with rich electron sites to explore whether direct electron transfer promotes the degradation efficiency of Fe(VI) for pollutants under visible light. For comparison, we also prepared phosphorus-doped carbon nitride (CNP), which has electron-deficient sites and indirect electron transfer. In the CNO/Fe(VI)/light system, not only more high-valent iron and reactive oxygen species were generated, but also the pollutant degradation rate, reaction kinetics, and electron yield were significantly better than those of the CNP and CN systems, verifying the superiority of direct electron transfer. In addition, CNO showed excellent performance in both actual solar photocatalysis and continuous flow experiments. Therefore, the photocatalysis/direct electron transfer mechanism proposed provides an innovative strategy for improving the application potential of Fe(VI) in the field of pollution control and its industrialization application.

研究领域: 环境科学 · 材料科学
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ENVIRONMENTAL POLLUTION · 2024 · IF 7.6

Influence of microplastics and environmentally persistent free radicals on the ability of biochar components to promote degradation of antibiotics by activated peroxymonosulfate

Yanzhuo Zhang,Rui He,Yutai Sun,Jing Zhao,Xiaozhuan Zhang,Jiqin Wang,Alexandr V. Bildyukevich

Microplastics (MPs) in sludge can affect the ability of biochar-activated peroxymonosulfate (PMS) to degrade antibiotics. In this work, biochar was prepared by mixing sludge and polystyrene (PS) through hydrothermal carbonization (HTC) and high-temperature pyrolysis processes . The resulting biochar was used to activate PMS to degrade ofloxacin (OFX), levofloxacin (LEV), and pefloxacin (PFX). The addition of PS significantly enhanced the ability of biochar/PMS to degrade antibiotics and the levels of environmentally persistent free radicals (EPFRs, 4.59 × 10 20 spin/g) due to the decomposition of PS. The addition of PS resulted in a slight decrease in the specific surface area of biochar (2–3 m 2 /g on average), but a significant increase in the concentration of EPFRs increased the removal efficiency. The activation of PMS by biochar is dominated by free radicals, accounting for about 70%, in which SO 4 •- and •OH contribute the most and O 2 •- the least. However, 1 O 2 contributes 15–20% to the degradation of antibiotics in non-free radical processes. Overall, the process of biochar/PMS degradation of antibiotics is mainly dominated by free radicals, and the effect of non-free radicals is not obvious. Both hydrochar and pyrocarbon samples showed good hydrophilicity, and this property should improve the ability of active sites on biochar to degrade antibiotics. In the HTC process, PS can decompose during hydrochar preparation, with a maximum reduction value of 40.09%. The three-dimension excitation emission matrix fluorescence spectroscopy (3D-EEM) and total organic carbon (TOC) results show that the protein content in sludge plays a major role in reducing PS, with little effect of polysaccharide and SiO 2 . There are six to seven degradation intermediates of quinolone antibiotics, which are eventually degraded into CO 2 , H 2 O, and inorganic substances. The regeneration experiment showed good reusability of hydrochar and pyrocarbon, further demonstrating the suitability of biochar for the degradation of antibiotics.

研究领域: 环境科学 · 化学工程
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES · 2024 · IF 7.7

Nanozyme-based inulin@nanogold for adhesive and antibacterial agent with enhanced biosafety

Shiwen Zhao,Danyang Wang,Qiong Zhou,Beibei Wang,Zhao Tong,Honglei Tian,Jianke Li,Yuhuan Zhang

Nanozymes with oxidase or peroxidase-mimicking activity have emerged as a promising alternative for disinfecting resistant pathogens. However, further research and clinical applications of nanozymes are hampered by their low in vivo biosafety and biocompatibility. In this study, inulin-confined gold nanoparticles (IN@AuNP) are synthesized as an antibacterial agent via a straightforward in situ reduction of Au 3+ ions by the hydroxyl groups in inulin. The IN@AuNP exhibits both peroxidase-mimicking and oxidase-mimicking catalytic activities, of which the maximum reaction velocity ( V max ) for H 2 O 2 is 2.66 times higher than that of horseradish peroxidase. IN@AuNP can catalyze the production of reactive oxygen species (ROS), resulting in effective antibacterial behavior against both Gram-negative ( Escherichia coli ) and Gram-positive ( Staphylococcus aureus ) bacteria. Abundant hydroxyl groups retained in inulin endow the nanozyme with high adhesion to bacteria, reducing the distance between the captured bacteria and ROS, achieving an antibacterial ratio of 100 % within 1 h. Importantly, due to the natural biosafety and non-absorption of the dietary fiber inulin, as well as the inability of inulin-trapped AuNP to diffuse, the IN@AuNP exhibits high biosafety and biocompatibility under physiological conditions. This work is expected to open a new avenue for nanozymes with great clinical application value.

研究领域: 生物医学工程 · 材料科学 · 微生物学
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Journal of Environmental Chemical Engineering · 2025 · IF 7.2

Study on the dissolution of precious metals in the nitrogrn-oxygen free radical ionic liquid system

Feng Feng,Jiaying Zhang,Lu Yu,Haixin Wang,Heda Ding,Jifan Cheng,Miaolan Wang,Fangfang Chen,Jiahui Zhang,Lingling Guo,Chunshan Lu,Qunfeng Zhang,Xiaonian Li

In order to develop an efficient and environmentally friendly method for the recovery of precious metals, a functionalized ionic liquid containing free radicals (1-methyl-3-(2-oxo-2-(2,2,6,6-tetramethyl-1-oxo-4-piperidinoxy) butyl) imidazole trichloro-1-bromoaluminium salt) was designed and synthesized. This was achieved by combining 2,2,6,6-tetramethylpiperidine-1-oxyl (TEMPO), which possesses oxidizing properties, with halide ions that exhibit complexing abilities. Notably, under optimal conditions, a maximum gold dissolution rate of 100 % was attained. X-ray photoelectron spectroscopy (XPS), X-ray diffraction (XRD), and Raman spectroscopy analyses were conducted to elucidate the dissolution mechanism. Ultimately, these functionalized ionic liquids can be utilized for the dissolution of precious metals in CPU pins and waste catalysts. This study presents an effective approach for the recovery of precious metals.

研究领域: 化学 · 材料科学 · 环境科学
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WATER SCIENCE AND TECHNOLOGY · 2026 ·Vol. 93 ·期 3 ·318-331 · IF 2.6

Green preparation of pyrrhotite-activated H2O2 for tetracycline degradation: performance and mechanism

Wang Hanlin,Chu Ziyang,Li Mengxue,Chen Tianhu

View large Download slide View large Download slide Close modal Pyrrhotite (Fe 1-x S) was prepared by the pyrolysis of pyrite and the sulfidation of hematite, and subsequently used to activate H 2 O 2 for the degradation of tetracycline (TC). The pyrite-derived Fe 1-x S samples (P600 and P700) and the hematite-derived Fe 1-x S samples (S600, S700), prepared at 600 and 700 °C, respectively, were characterized using X-ray diffraction (XRD), X-ray photoelectronic spectroscopy (XRS), scanning electron microscopy (SEM) and magnetism analysis. The effects of annealing temperature, preparation method, and initial solution pH on TC degradation were systematically investigated. The results showed that the degradation of TC increased with the decrease in annealing temperature and initial solution pH. Quenching experiments and electron spin resonance (ESR) demonstrated that • OH and 1 O 2 were reactive oxygen species (ROSs) in acidic and alkaline media, respectively. Moreover, the sulfidation-derived pyrrhotite, featuring a monoclinic Fe 1-x S shell, exhibited superior catalytic performance than pyrolysis-derived pyrrhotite with a hexagonal Fe 1-x S shell. Notably, 1 O 2 was easier to produce in the P600/H 2 O 2 system. Both P600 and S600 maintained a high catalytic activity after five runs. These findings offer a novel approach for pyrrhotite preparation and promote the comprehensive utilization of pyrite and hematite. Pyrolytic pyrrhotite and sulfurized pyrrhotite were prepared by a one-step method. Sulfurized pyrrhotite exhibited superior catalytic activity than pyrolytic pyrrhotite. • OH was the dominant ROS under acidic conditions, while 1 O 2 prevailed under alkaline conditions. The magnetic pyrrhotite showed excellent reusability over five cycles.

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JOURNAL OF MOLECULAR STRUCTURE · 2025 · IF 4.7

Bromine-doped Bi2MoO6 nanosheets: synergistic effects of band structure engineering and oxygen vacancy regulation for boosting photocatalytic activity

Jiayu Gu,Mingzhou Wu,Linlin Wang,Fengling Liu,Suhao He,Minrui Ding,Yuye Yao,Neng Tao,Haitao Sha,Zhaobing Guo,Huimin Zhou,Pin Zhou,Pengxiang Qiu

Photocatalyst modification by energy level engineering is crucial for efficient free radical generation. Here, a novel strategy was employed to construct bromine-doped Bi 2 MoO 6 (BMO-Br) followed by an in-situ approach using Cetyltrimethylammonium bromide (CTAB) as the bromine (Br) precursor. The Br doping effectively modulated the energy band, increasing the oxygen vacancy concentration in Bi 2 MoO 6 . The modification significantly enhanced photoinduced charge separation and active free radical generation, leading to superior photocatalytic performance. The photocatalytic bacteriostatic and sulfamethazine (SM) degradation efficiency over BMO-Br-4 reached 100% and 70% within 60 min and 150 min, respectively. This work highlighted a facile yet effective strategy for tailoring the photocatalyst properties, demonstrating promising potential for various photocatalytic applications.

研究领域: 材料科学 · 环境科学
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